:•:•:*:
S8:
:•:•:•:•:'
i;$
ORP/CSD-75-1K3
ORPCSD751V3
PROCEEDINGS OF PUBLIC HEARINGS:
PLUTONIUM AND THE OTHER
TRANSURANIUM ELEMENTS
1
1
ii|
II
•: :•:•:•:•:•:
11
§IP
i
1
VOLUME 3
ADDITIONAL MATERIAL*
U.S. ENVIRONMENTAL PROTECTION AGENCY
Office of Radiation Programs
-------
-------
PROCEEDINGS OF PUBLIC HEARINGS:
PLUTONIUM AND THE OTHER
TRANSURANIUM ELEMENTS
VOLUME 3
ADDITIONAL MATERIALS RECEIVED
U.S. ENVIRONMENTAL PROTECTION AGENCY
Office of Radiation Programs
Criteria and Standards Division
Washington, D.C. 20460
-------
CONTENTS
page
Environmental Protection Agency
Hearing Announcement 1
Federal Register Notices 2
National Audubon Society, letter 5
Bruce W. von Zellen, letter 6
Catherine Quigg, letter and article 7
Atlantic County Citizens Council on
Environmental, letter 13
Colorado Department of Health, letter 14
Linda Header, letter 17
Freihofer et. al, letters 18
Natural Resources Defense Council,
letter and articles 31
Biophysical Society, letter and article 232
J. W. Healy, letter and articles 255
Elmer Glueck, letter 383
National Radiological Protection Board,
letter and article 384
Chester R. Richmond, letter 439
Annette Cottrell, letter 445
L. R. Anspaugh, letter and article 446
Frederick Forscher, letter 467
William Lipton, letters and article 468
General Electric, letter 490
-------
(FRL 364-2]
PLUTONIUM AND THE TRANSURANIUM
ELEMENTS
Public Hearing
In the September 23, 1974 issue of the
FEDERAL REGISTER, 38 FR 24098, the En-
vironmental Protection Agency published
a notice of Intent to evaluate the en-
vironmental Impact of Plutonium and
the other transuranium elements' and
to consider whether new guidelines or
standards under the authorities of this
Agency are needed to assure adequate
protection of the general ambient en-
vironment and of the public health from
potential contamination of the environ-
ment by radionuclides of the trans-
uranium elements. This notice requested
information from interested parties rele-
vant to the development of standards
and guidelines.
In accordance with the above request,
the Office of Radiation Programs of the
Environmental Protection Agency will
hold public hearings beginning on De-
cember 10, 1974, at 9:30 ajn. In the OSA
Auditorium, 18th & F Streets, NW.,
Washington, D.C. Further hearings will
be held in other locations if deemed ad-
visable. Announcement of such hearings
will be made in the FEDERAL REGISTER.
The Office of Radiation Programs will
consider the information derived from
these hearings, along with other avail-
able information, in determining the
adequacy of current guidelines for plu-
tonium and tlte other transuranium ele-
ments and in developing any new stand-
ards deemed necessary. Specific infor-
mation is desired Lc the following cate-
gories:
(1) General: to includa considerations
of general concern, including the public
and social Implications of Plutonium
utilization, and the factors involved in
balancing of costs vs. benefits.
(2) Doslmetry, Health, and Environ-
mental Effects: to include consideration
of available data concerning conversion
of ambient concentrations to exposure
data, on the health effects of Plutonium
exposure in humans and animals, as well
as of other possible adverse environ-
mental effects. Discussions of research
needs are also desired.
(3) Environmental Levels and Path-
Wai's: to Include consideration of avail-
able monitoring data, of the precision.
accuracy and completeness of available
data, of theoretical models developed to
predict transport through the ecosystem,
and of experimental verification of such
models.
<4> Applications Using Plutonium: to
include consideration of current and
projected uses of Plutonium and other
transuranium elements, the estimated
quantities in each such application, and
the magnitude of possible releases to the
environment.
(5) Control and Cleanup Technology:
to include consideration of currently
available or near-t»np projected engi-
neered safeguard devices and installa-
tions to minimize and restrict releases to
the environment and of technology avail-
able to restore contaminated areas, but
not to Include waste storage facilities.
A detailed agenda and schedule will be
made available on request from the Of-
fice of Radiation Programs on December
6.1974.
The entire proceeding will be open to
the public, and attendance by Interested
persons Is encouraged. Persons wishing
to make a statement at the hearing will
be afforded an opportunity to do so. In
addition, written comments as requested
In the FEDERAL REGISTER notice of Sep-
tember 23, 1974, (39 FR 34098) will con-
tinue to be received. The following
procedures and requirements shall apply
to the hearing:
(a) The hearings will be conducted in-
formally. Technical rules of evidence will
not apply. Discovery and cross-examina-
tion of participants will not be permitted.
(b) A Hearing Panel, to be appointed
by the Deputy Assistant Administrator
for Radiation Programs and consisting
of a Chairman and three or more tech-
nical experts In the field of radiation
protection, will conduct the hearings.
(c) The Chairman of the hearing
panel is empowered to conduct the
meeting in a manner that in his Judg-
ment will facilitate the orderly conduct
of business, to schedule presentations by
participants, and to exclude material
which is Irrelevant, extraneous, or repe-
titious.
(d) Persons wishing to present an oral
statement shall give written notice to
the Director, Criteria and Standards Di-
vision (AW-560), Office of Radiation
Programs. U.S. Environmental Protec-
tion Agency, Washington,-D.C. 20460, no
later than November 23. 1974, In order
to be placed on tlte agenda Such notice
shall Include the name, address and af-
filiation (if any) of the participant, the
amount of time required, and a reason-
ably detailed summary of the statement
to be presented at the hearing. The time
allotment for such oral statements shall
be at the discretion of the Chairman,
but shall not ordinarily exceed 20
minutes.
(e) Persons wishing to submit written
statements regarding the agenda items
may do so either in advance or during
the hearings. K practicable, at least 20
copies should be provided. Such persons
may also request an opportunity to pre-
sent an oral statement to accordance
with paragraph (d) abo above. The time al-
lotment for such panel discussions shall
be at the discretion of the Chairman,
but shall not ordinarily exceed 60 min-
utes.
003
(g> Requests at the time of the hear-
ings for the opportunity to make oral
statements, with no previous notice shall
be ruled on by the Chairman of the
Hearing Panel, who Is empowered to ap-
portion the time available, but nqt or-
dinarily to exceed 6 minutes.
(h) Questions may be propounded only
by members of the Hearing Panel or Its
consultants. At the discretion of the
Chairman, a procedure may be made
available for submission of pertinent
questions f torn other persons to partici-
pants.
(1) Seating for the public will be avail-
able on first-come, first-served basis.
(]) The use of still, motion picture, and
television cameras, the physical installa-
tion and presence of which will not in-
terfere with the conduct of the meeting,
will be permitted both before and after
the hearing and during any recess. The
use of such equipment will not, however,
be allowed while the hearing is In ses-
sion.
(k) A transcript of the hearing will be
made and a copy of the transcript, to-
gether with copies of all documents pre-
sented at the hearing, will constitute the
record of the hearing. A copy of the
transcript of the hearing will be avail-
able for public Inspection and copying
within 30 days after conclusion of the
hearings at the UJ3. Environmental Pro-
tection Agency Freedom of Information
Office, 2nd Floor, West Tower, 401 M
Street, SW., Washington, D.C. 20460.
Dated: October 17,1974.
Room Snmow,
Assistant Administrator
for Air and Waste Management.
[PB Doc.74-24733 Piled 10-2S-T4;8:« am)
FEDERAL UGIJTEI, VOL. 39, NO. 207—THURSDAY, OCTOBER 24, 1974
-------
005
REGIONAL
REPRESENTATIVE
ARIZONA•COLORADO
IDAHO•MONTANA
UTAH* WYOMING
NATIONAL AUDUBON SOCIETY
P. O. BOX 3232 • BOULDER, COLORADO 80303 • (303) 499-0219
October 31, 1974
Mr. W. D. Rowe, Ph.D.
Deputy Asst. Administrator, Radiation Programs
United States Environmental Protection Agency
Washington, D. C. 20460
RE: Plutonium and the transuranium elements
Dear Mr. Rowe,
I would like to make one brief statement for the upcoming
hearing.
Could not the great majority of problems related to the
storing, handling, transporting, etc. of the referenced
elements be eliminated by reducing the volume (mass) of these
elements which reactors are now generating as waste?
Specifically, I am referring to a transmutation process whereby
waste plutonium is bombarded creating lighter and shorter
lived isotopes. Nuclear scientists insist this is technically
possible though a paucity of funding appears as the main
obstacle.
Sincerely,
'"^
Robert K. Turner
RKT.lbp
cc: Mr. John Quarles, Acting Administrator of EPA
AMERICANS COMMITTED TO CONSERVATION
-------
: Mr. Gordon Hurley, Ph.D.
Chief, Environmental Standards Bureau
U.S. Environmental Protection Agency.
Washington, B.C. 20lj.60
PROM: Catherine T. Quigg (Mrs.)
Vice president
Pollution & Environmental Problems, Inc.
5U. S. Brockway
Palatine, Illinois 60067
SUBJECT: PLUTONIUM
As a representative of Pollution & Environmental Problems, Inc.,
with members in the north and northwest suburbs of Chicago, I
urge your consideration of the awesome dangers to the general
population from the proliferation of plutoniura in our environment.
For compelling evidence against plutonium, one need only look to
the Atomic Energy Commission's own laboratories.
"Plutonium is toxic beyond human experience," according to
Donald Geesaman of the AES's Lawrence Radiation Laboratory at
Livermore, California. He warned it was "demonstrably carcinogenic
to animals in microgram quantities" stating that an injection of
a millionth of a gram has caused cancer in mice and dogs. Moreover,
he said, "our transition to plutonium as a major energy source
will inextricably involve our society with the large-scale commercial
production of a substance that is a suitable nuclear explosive."
Gessaman estimated that by the year 2000 annual production of plutonium
would exceed 100 tons. Can such Quantities be protected from
internal subversion? Gessaman thinks not. He has stated that
-------
012 -5-
becorre s widespread, the possibility must be faced, of awful accidents,
either accidental or deliberate, that will cnuse wfde regions of our
earth be becor* s forever uninhabitable."
We should heed Dr. Watson's ominous words now - and ban the fast
breeder - before it bans us from this earth.
-------
ATLANTIC November 6, 1974 013
COUNTY
CITIZENS
COUNCIL ON
ENVIRONMENT 2 Old Turnpike ° Pleasantvllie, N. J. 08232 « Phone (609) 646-6604
Mr. W. D. Rowe, Ph.D.
Deputy Assistant Administrator
Radiation Programs
U.S. Environmental Protection Agency
Washington, D.C. 20^60
Dear Mr. Rowe:
The Atlantic County Citizens Council on Environment hereby
registers a request that Atlantic City, New Jersey be considered
one of the cities at which the Environmental Protection Agency
hearings on the impact of transuranium elements be held. The
nation's first offshore floating nuclear power plant Is planned
to be located 2.8 miles off the Atlantic County shore near here*
A county referendum this week resulted in an overwhelming vote
against a nuclear power plant being located off our shores*
The ACCCE is a non profit non funded citizens organization
of several hundred members including associate organizations
membership* The primary Interest Is the environment of Atlantic
county* 'iliis Council, along with the City of Brlgantine, N.J.
and the Atlantic County Board of Chosen Freeholders, Is an of-
ficial intervenor in Atomic Energy Commission hearings on the
offshore nuclear power plant held here In Atlantic City and in
Washington, D. C. The AEG hearings held here are heavily at-
tended by concerned citizens and officials from this area*
One of our major concerns is the deleterious effects of
transuranium elements or materials.
-------
014
COLORADO DEPARTMENT OF HEALTH
4210 EAST 11TH AVENUE • DENVER, COLORADO 80220 • PHONE 388-6111
Edward G. Dreyfus, M.D.S, M.P.H. Executive Director
November 8, 1974
Dr. W. D. Rowe
Deputy Assistant Administrator
for Radiation Programs
United States Environmental
Protection Agency
Washington, D.C. 20460
Dear Mr. Rowe:
Reference is made to your announcement of October 25, 1974, concerning
hearings on the environmental impact of releases of plutonium and other
transuranium elements.
Because of the location of the USAEC's Rocky Flat Plant, upwind from
a large metropolitan area, we have considerable interest in the proposed
hearings. There being no federal or. international standards for plutonium
in soil, the Colorado Department of Health held an open hearing in Denver
on February 14, 1973. On March 21, 1973, the Colorado Board of Health
established a standard for plutonium in soil, a copy Off which is enclosed
for your information.
It is presumed that most organizations and individuals; who participated
in the 1973 hearing would desire to present their opinions in a hearing
that might result in the establishment of federal standards. Therefore,
we recommend that you schedule a hearing in Denver, preferably early in
January 1975.
A spokesman for the Colorado Department of Health will present the Depart-
ment's opinion on this subject. We request that 30 minutes be allowed
for our presentation.
Sincerely,
Albert J. Haz^, Director
Occupational & Radiological
Health Division
AJH/lc
Enclosure: (1) Plutonium Standard
-------
015
JOHN P. MOORE
TTORNEY GENERAL
(Hulurulbo
DEPARTMENT OF LAW
Of THE ATTOnNEY GENERAL
104 STATE CAPITOL
DENVER, COLORADO 80203
April 6, 1973
JOHN E. BUSH
DEPUTY ATTORNEY GENERAL
Dr. Roy L. Cleere
Director
Department of Health
4210 East llth Avenue
Denver, Colorado 80220
RE: Permissible Levels of Radioactive
Material in Uncontrolled Areas
(Plutonium)
Dear Doctor Cleere:
Pursuant to the request of Mr. Alfred L Capra, we
have examined the Amendment to* the above-captioned rules
and regulations which were adopted by the State Board of
Health on March 21, 1973, to become effective May 1, 1973.
Pursuant to Section 3-16-2, C.R.S 1963 (1967 and
1969 Perm. Cum. Supp.), you are hereby advised that it is the
opinion of this office that said rules and regulations are
constitutional and within the authority granted to the State
Board of Health by the legislature.
You are further advised that your office must file
two copies of this letter of approval along with two copies
of said rules and regulations with the Secretary of State's
office.
Very truly yours,
JPM:WT:ms
JjOHN P. MOORE
ttorney General
-------
016
AMENDMENT TO THE
State of Colorado Rules and Regulations Pertaining to Radiation
Control
Subpart RH 4.21 is added:
RH 4.21 Permissible Levels of Radioactive Material in Uncontrolled
4.21.1 Plutonium. Contamination of the soil in excess of 2.0
disintegrations per minute of Plutonium per gram of dry
soil or square centimeter of surface area (0.01 microcurie
plutonium per sqaare meter) presents a sufficient hazard
to the public health to require the utilization of special
techniques of construction upon property so contaminated.
Evaluation of proposed control techniques shall be avail-
able from the Department of Health upon request.
Adopted: Colorado State Board of Health
March 21, 1973
Effective: May 1, 1973
-------
017
93 Main street
Byfield, Ma. 01922
November 11, 1974
Dear Sir(s)
I'm writing on behalf of your article on the EPA
setting Plutonium standards. My opinion is I don't think
that any plutonium what so ever should be let out of the
Nuclear power plants, because when the plutonium gets into
the soil it is then carried along by water which is later
evaporated into the atmosphere and when it is inhaled it
causes instant death. It has these effects on animals as
well as people and does not stop killing until 24,000
years after it is released. A small amount of plutonium
about the size of a folf-ball could kill a city the size
of Pittsburg. Everytime this little amount of plutonium
is released it adds up and we'll all be wiped out before
we ever got a chance to use this type of energy. I feel
this very strongly. Thank-you.
Sincerely,
Tlead&r
-------
018
FREIHOFER, COOK, HECHT, OOSTERHOUSE & DEBOER, p. c.
ATTORNEYS AT LAW
860 UNION BANK BUILDING
0W«;"VF"o«°r" ORAND «AP'DS, M.CH.OAN 40SO2
DAVID M. HECHT TELEPHONE (Olfi) 454-9321 F"D N' SEARL
DONALD r. OOSTERMOUSE EDWARD C.McCOBB
ROBERT J.DtBOER
OLCN V. BORRE
ROBERT P. COOPER
PHILIP M. IDEMA
PETER w. BT.KETEE November 13, 1974
PETER R.TOLLEY
JAMCS E. McCOBB
OEOROE C.PAWLOW8KI
WILLIAM J. FIBHER,III
JANCT T. NEFF
STUART r. CHENEY
MARK H.VERWYS
Director, Criteria and Standards
Division (AW-560)
Office of Radiation Programs
Environmental Protection Agency
Washington, D.C. 20460
Dear Sir:
This letter is written on behalf of West Michigan Environmental
Action Council, Inc., 822 Cherry Street, S.E., Grand Rapids, Michigan
49506 CWMEAC) , and responds to a letter WMEAC has received dated
October 25, 1974, together with two attached Federal Register notices
entitled Plutonium and the Transuranium Elements , over the signature
of W. D. Rowe, Ph.D., Deputy Assistant Administrator for Radiation
Programs (AW-558) .
Pursuant to the requests set forth in the letter, this is to
notify you that WMEAC desires to submit a written statement at the
hearings which you contemplate for plutonium and the transuranium
elements. WMEAC is unable to make an oral presentation due to limited
funds, and, therefore, no time for an oral presentation is requested
at this time .
WMEAC intends to file its written statement prior to the
public hearing scheduled for Washington, D.C., on December 10, 1974.
WMEAC would appreciate being notified of the schedule of hearings
and the agenda for other cities.
WMEAC 's statement will set forth its viewpoints as they per-
tain to the problems of plutonium and the environment, and the state-
ment will be limited both in length and in scope. WMEAC, in conjunc-
tion with other organizations, may submit additional technical comments.
Very truly yours,
FREIHOFER, COOK, HECHT,
OOSTERHOUSE & DE -BOER, P.C.
Peter W. Steketee
PWS/jmc
-------
019
FREIHOFER, COOK, HECHT, OOSTERHOUSE & DEBOER, p. c.
WA
FEH
OEORGE R.COOK
DAVID M. HECHT
DONALD F. OOSTERHOUSE
ROBERT J. DcBOER
BRUCE A.BARNHART
ROBERT P. COOPER
PHILIP M. IOEMA
JAMES E. MeCOBB
OEORGE E.PAWLOWSKI
WILLIAM J. FISHER, III
JAMES B. FLICKINOER
JANET T. NEFF
STUART F. CHENEY
MARK H. VERWYS
LYNWOOD P. VANDEN BOSCH
ATTORNEYS AT LAW
OSO UNION BANK BUILDING
GRAND RAPIDS, MICHIGAN -485O2
TELEPHONE (OIO) 454-83ZI
OF COUNSEL:
FRED N. SEARL
EDWARD C.McCOBB
December 12, 1974
Dr. William A. Mills, Director
Criteria and Standards Division CAW-560)
U.S. Environmental Protection Agency
Washington, D.C. 20460
Dear Dr. Mills:
This letter relates to EPA's hearings on Plutonium and the
Transuranium Elements. Please refer to my letter to you dated
November 13, 1974, and to your response to me of November 26, 1974.
This letter is submitted on behalf of West Michigan Environmental
Action Council, Inc., 822 Cherry Street, S.E., Grand Rapids,
Michigan 49506 ("WMEAC"), and is intended to be WMEAC's written
statement for submission at the hearings. It is my understanding
that the hearing record will be kept open for several weeks after
December 10, 1974, and, consequently, I would appreciate it if
you would include this statement of WMEAC in the hearing record.
As I indicated in my letter of November 13, 1974, this
statement does not address any technical points relating to plu-
tonium and the transuranium elements. Instead, for our technical
comments we rely on the submissions of the Natural Resources
Defense Council, Inc,
Also, EPA's October 17, 1974, public notice requested in-
formation on "contamination of the environment by radionuclides
of the transuranium elements", apparently suggesting that EPA would
not be concerned in these hearings with the full range of the
hazards raised potentially by plutonium. In other words, EPA
appears to us to be primarily concerned in these hearings with the
public health problems (that is, with the radiation protection
problems, including the "hot particles" question) posed by plu-
tonium rather than with the nuclear safety, nuclear proliferation,
safeguards and civil liberties issues, even though all of these
issues are interrelated. On this assumption, we will limit our
comments to the public health issues. However, for a truly excellent
review of the broader implications of plutoniiam, we refer you to an
article by Speth, Tamplin and Cochran entitled, Plutonium Recycle;
-------
020
Dr. William A. Mills, Director
December 12, 1974
Page 2
FREIHOFER,COOK, HECHT,
OOSTERHOUSE & DsBOER, P. C.
The Fateful Step, November, 1974, Bulletin of the Atomic Scientists,
a copy of which is enclosed for your convenience.
Turning, then, to the public health issues posed by plutonium,
WMEAC will try to outline as clearly and briefly as it can those
considerations which it considers to be of primary importance:
Although it may be possible still for more light to be thrown
on the subject at this time, WMEAC believes that the exchange of
technical views which has taken place recently between NRDC scientists
and the AEC on the "hot particle" issue has brought the disputed
technical questions, as well as the resulting political, legal and
moral questions, into clear focus.
Specifically, we are referring to the NRDC report of Tamplin
and Cochran, Radiation Standards for Hot Particles, A Report on the
Inadequacy of Existing Radiation Protection Standards Related to
Internal Exposure of Man to Insoluble Particles of Plutonium and
Other Alpha-Emitting Hot Particles, February 14, 1974; to the AEC's
response by Blair, Richmond and Wachholz, A Radiolpgical Assessment
of the Spatial Distribution of Radiation Dose from Inhaled Plutonium,
WASH 1320, September, 1974; to the NRDC Comments on WASH 1327, Draft
Generic Environmental Impact Statement on Mixed Oxide Fuels (GESMO),
Re; The Hot Particle Discussion in Volume 3, Chapter IV, Section J.I.
and Section J, Appendix D, Pages IV J-7, IV J(D)-1 to 41, September,
1974, Tamplin and Cochran; and to the NRDC rebuttal to WASH-1320,
The Hot Particle Issue; A Critique of WASH 1320 as it Relates to the
Hot Particle Hypothesis, November, 1974, Tamplin and Cochran.
Tamplin and Cochran state the hot particle thesis as follows
in their November, 1974, rebuttal of WASH 1320 (p. 5):
"If a particle deposited in the deep respiratory
tissue is of such activity as to expose the surrounding
lung tissue to a dose of at least 1000 rem in 1 year,
this particle represents a unique carcinogenic risk.
The biological data suggest that such a particle may
have a cancer risk equal to 1/2000."
WASH 1320 discusses a number of animal experiments which, it
claims, rebut the hot particle thesis. However, we believe that
Tamplin and Cochran have shown that WASH 1320 is not successful in
disproving the hot particle thesis. Their November, 1974, rebuttal
of WASH 1320 succinctly states the public health consequences of WASH
1320's failure (pp. 28-29):
"... Thus, these experiments do not set aside
the hot particle hypothesis. Rather, they suggest
additional experiments involving longer lived animals
to determine whether this histological change progresses
-------
•THE || • •
bulletin
OF THE ATOMIC SCIENTISTS
023
(Reprinted by permission of the Bulletin of the Atomic Scientists
and the authors. Copyright (c) by the Educational Foundation for
Nuclear Science.)" .
Plutonium Recycle:
The Fateful Step
Impending move to reprocess fuel would escalate the risks of nuclear power
/ fear that when the history of this century is
written, that the greatest debacle of our nation
will be seen not to be our tragic involvement in
Southeast Asia but our creation of vast armadas
of plutonium, whose safe containment will rep-
resent a major precondition for human survival,
not for a few decades or hundreds of years, but
for thousands of years more than human civili-
zation has so far existed.
James D. Watson
Nobel Laureate, Medicine
J. GUSTAVE SPETH, ARTHUR R. TAMPLIN
and THOMAS B. COCHRAN
The Atomic Energy Commission, if unchecked, is
about to sow the seeds of a national crisis. The Com-
mission now proposes to authorize the nuclear power
industry to proceed to use plutonium as fuel in com-
mercial nuclear reactors around the country. The re-
sult of a decision approving this commercial use of
plutonium will be the creation of a large civilian plu-
tonium industry and a dramatic escalation in the
risks posed by nuclear power.
This decision to launch what the AEC calls the
plutonium economy is the conclusion of the AEC's
recently released draft environmental impact state-
ment for plutonium recycle: the recycling of plutoni-
um as fuel in the present generation of light water
reactors [1,2]. The final version of the impact state-
ment, which is expected to confirm the decision to
authorize plutonium recycle, is due in a few months.
Plutonium is virtually unknown in nature; the en-
tire present-day inventory is man-made, produced in
nuclear reactors. Plutonium-239, the principal iso-
tope of this element, has a half-life of 24,000 years,
J. Gustave Speth (attorney), Arthur R. Tamplin
(biophysicist) and Thomas B. Cochran (nuclear
physicist) are on the staff of the Natural Resources
Defense Council in Washington, D. C. Dr. Tamplin
is on leave of absence from the Lawrence Livermore
Laboratory of the University of California.
hence its radioactivity is undiminished within human
time scales. It is perhaps the most toxic substance
known. One millionth of a gram has been shown ca-
pable of producing cancer in animals [3]. Plutonium
is also the material from which nuclear weapons are
made. An amount the size of a softball is enough
for a nuclear explosive capable of mass destruction.
Scientists now widely recognize that the design and
manufacture of a crude nuclear explosive is no longer
a difficult task technically, the only real obstacle
being the availability of the plutonium itself [4].
We believe that the commercialization of plutoni-
um will place an intolerable strain on our society
and its institutions. Our unrelenting nuclear tech-
nology has presented us with a possible new fuel
which we are asked to accept because of its potential
commercial value. But our technology has again out-
stripped our institutions, which are not prepared or
suited to deal with plutonium. Those who have asked
what changes in our institutions will be necessary to
accommodate plutonium have come away from that
enquiry profoundly concerned. And the AEC's en-
vironmental impact statement does not allay these
concerns. It reinforces them.
The AEC concedes that the problems of plutonium
toxicity and nuclear theft are far from solved and in-
dicates that they may not be for some years. Yet it
concludes, inexplicably, that we should proceed.
Whether stemming from blind faith in the technol-
ogy it has fostered or from callous promotion of the
bureaucratic and industrial interests of the nuclear
power complex, the AEC's proposal cannot be justi-
fied in light of what we know and, just as important,
what we do not know.
The fuel now used in present-day reactors, the
light water reactors, is uranium which has been en-
riched; the uranium-235 content is increased from
0.7 percent present in natural uranium to, about 3
or 4 percent. Uranium-235 is a fissionable isotope of
uranium, the remainder being non-fissile uranium-
238. Unlike plutonium, uranium fuel is not extreme-
ly toxic, and it is not sufficiently rich in uranium-235
to be fashioned into nuclear weapons. The uranium
NOVEMBER 1974 VOLUME XXX
NUMBER 9
15
-------
028
The keeping of police dossiers will not be limited
to nuclear industry personnel. The New York Times
reported August 11 that Texas state police maintain
files on nuclear power plant opponents. How much
more government investigation into the private lives
of individuals can be tolerated by a free society? Se-
curity and surveillance procedures at best infringe
upon the privacy of families and their friends. At
worst, they are the instruments of repression and
reprisal.
A second AEC safeguards proposal is the creation
of a federal police force for the protection of plutoni-
um plants and shipments. The draft impact state-
ment for plutonium recycle justifies such a federal
force in the following terms:
A federal security system would he less apt to have the
variations in staff and capability that would he en-
countered in use of private security guards. In addition,
it should be noted that the consequences of a successful
theft or diversion of plutonium would undoubtedly
have nationwide impacts and could best he handled by
Federal authorities; certainly, with Federal participa-
tion, there is the potential for a larger force, more ef-
fective weapons, and better communications [2, chap 5,
p. 42].
How large would such a force be? What standards
should govern and restrain its operations? The Wash-
ington Post reported in October 1973 that the AEC
issued shoot-to-kill orders to personnel directing the
production, shipment and storage of atomic weapons
at the height of the Yom Kippur War.
Once a significant theft of plutonium or other wea-
pons material has occurred, how will it be recovered?
To prevent traffic in heroin, police have asked for no-
knock search laws. This infringes upon one of our
most cherished freedoms. To live with plutonium we
may have to abandon this freedom along with others.
In the presence of nuclear blackmail threats, the in-
stitution of martial law seems inevitable. It has been
said that the widespread availability of weapons ma-
terial and terrorists targets in the nuclear fuel cycle
will radically alter the power balance between large
and small social units (De Nike [16]). It should be
added that the threatened society will undoubtedly
attempt to redress that balance through sophisticat-
ed and drastic police action.
In sum, to accommodate plutonium we shall have
to move toward a more intimidated society with
greatly reduced freedoms. In this respect the follow-
ing passage from the report of the distinguished in-
ternational group of scientists attending the 23rd
Pugwash Conference on Science and World Affairs
is instructive:
The problem of theft of nuclear material by internal
groups of individuals intent on sabotage, terrorism or
blackmail was agreed to be a very serious one, although
there was some sentiment expressed that the possibility
of such activity was much smaller in socialist states.
We believe that sentiment to be true. It is also ap-
parent that that is the direction in which we must
move to accommodate the nuclear industry. After
having spent billions of dollars for our nuclear de-
terrent, our civilian nuclear industry might well ac-
complish that which our defense system is trying to
prevent.
Alvin Weinberg is one of the few persons closely
associated with the nuclear power complex who has
looked carefully at the political and regulatory insti-
tutions that will be necessary to support a plutonium-
based nuclear power economy, and his views on this
subject merit close attention [19]. Weinberg's basic
premise is that nuclear power will place unprecedent-
ed strains on our society. In an unpublished paper
circulated prior to a conference in June 1973 at the
Woodrow Wilson International Center for Scholars
in Washington, D.C., Weinberg set out his views on
the type of new institutions required to cope with
the plutonium economy:
One suggestion (proposed by Sidney Siegel) that is
relevant to the situation in the United States would be
to establish a national corporation patterned after
COMSAT to take charge of the generation of nuclear
electricity. Such an organization would have technical
resources that must exceed those available to even a
large utility: and a high order of technical expertise in
operating reactors and their sub-systems is essential to
ensuring the continued integrity of these devices. [Here
Dr. Weinberg suggests nationalization of the industry.]
Each country now has its own AEC that sets stand-
ards or, in some cases, actually monitors or operates re-
actors. Perhaps this will be sufficient forever. Yet no
government has lasted continuously for 1,000 years:
only the Catholic. Church has survived more or less con-
tinuously for 2,000 years or so. Our commitment to nu-
clear energy is assumed to last in perpetuity—can we
think of a national entity that possesses the resiliency
to remain alive for even a single half-life of plutonium-
239? A permanent cadre of experts that will retain its
continuity over immensely long times hardly seems
feasible if the cadre is a national body.
It may be that an International Authority, operating
as an agent of the United Nations, could become the
focus for this cadre of expertise. The experts themselves
would remain under national auspices, but they would
be part of a worldwide community of experts who are
held together, are monitored, and are given long-term
stability by the International Authority. The Catholic
Church is the best example of what I have in mind:
a central authority that proclaims and to a degree en-
jorces doctrine, maintains its own long-term social sta-
bility, and has connections to every country's own Cath-
olic Church. (Emphasis added.)
These are far-reaching concepts presented by
Weinberg. The basic question they pose is: Will the
plutonium economy raise socio-political problems of
such magnitude that their resolution will be unac-
ceptable to society? In attempting to do the impos-
sible—live with plutonium—we may create the in-
tolerable.
Super-Human Requirements
The commercialization of plutonium will bring
with it a major escalation of the risks and problems
already associated with nuclear power. Plutonium
will further strain the already weakened regulatory
fabric of the nuclear industry.
Hannes Alfven, Nobel laureate in physics, has de-
scribed the regulatory imperatives applicable to the
nuclear industry:
Fission energy is safe only if a number of critical de-
vices work as they should, if a number of people in key
20
-------
033
BEFORE THE
ENVIRONMENTAL PROTECTION AGENCY
AND
ATOMIC ENERGY COMMISSION
In the Matter of
RADIATION PROTECTION STANDARDS ) EPA Docket No.
AS THEY APPLY TO HOT PARTICLES ) AEC Docket No. RM
PETITION TO AMEND
RADIATION PROTECTION
STANDARDS AS THEY
APPLY TO HOT PARTICLES
The NATURAL RESOURCES DEFENSE COUNCIL, INC. ("NRDC"),
on its own behalf and on behalf of its members hereby, petitions
the Environmental Protection Agency and the Atomic Energy
Commission to amend their radiation protection standards as
they apply to insoluble particles of plutonium and other
alpha-emitting hot particles as more fully described in the
Report prepared by Arthur R. Tamplin, Ph.D. and Thomas B.
Cochran, Ph.D., entitled Radiation Standards for Hot Particles/
submitted herewith. This request is filed pursuant to 5 U.S.C.
/
S 553(e) and 10 CFR § 2.802.
-------
034
-2-
Identification of Petitioner
Petitioner NATURAL RESOURCES DEFENSE COUNCIL, INC. ("NRDC")
is a non-profit, membership corporation organized under the laws
of the State of Nev; York. NRDC is a charitable organization
exempt from taxation under Section 501(c)(3) of the Internal
Revenue Code. NRDC's principal office and-place of business
is located at 15 West 44th Street, New York, New York. It main-
tains other offices at 1710 N Street, N. W., Washington, D. C.,
and at 664 Hamilton Avenue, Palo Alto, California. NRDC has a
nationwide membership composed of scientists, lawyers, educators,
and other citizens dedicated to the defense and preservation of
the human environment and the natural resources of the United
States. Other persons support NRDC's objectives by financial
contributions and personal efforts. • . •
The objectives of NRDC include:
(a) to maintain and enhance environmental quality;
(b) to monitor federal departments and regulatory
• agencies to ensure that environmental values are fully
considered in decisionmaking, and, in particular, to
ensure that federal statutes designed to protect and
enhance the environment are fully and properly imple-
mented;
-------
035
-3-
/
(c) to improve federal agency decisionmaking which
affects the environment by commenting, furnishing
information, and initiating and participating in
administrative proceedings;
(d) to select and undertake environmental lawsuits
which have a potential for establishing widely'appli-
cable precedent for saving or reclaiming some important
aspect of our national endowment, and, in particular,
which require federal agencies to meet legal obliga-
tions established in federal statutes designed to
protect and enhance the environment; and
(e) to provide a central, national focus for scientists,
lawyers, and educators, and concerned citizens in an
effort to make our courts and administrative .agencies
effective instruments of environmental protection.
In pursuit of its objectives, NRDC has been involved in
many proceedings involving the Environmental Protection Agency
and the Atomic Energy Commission.
-------
036
-4-
Petitioner's Interests in the Proceeding
NRDC's basic interest in the captioned proceeding is to
ensure that the public and radiation worker are adequately
protected from exposure to hot particle radiation by estab-
lishing radiation standards governing permissible exposure to
hot particles which carry a risk comparable to existing radia-
•tion standards governing uniform exposure to whole body radia-
tion. It is the view of NRDC that the present radiation
standards when applied to hot particles are too high by a
factor of 115,000. Each of NRDC's individual numbers is a
potential victim of exposure to hot particles. As an organiza-
tion NRDC is dedicated to preservation of the public health
and safety as part of its responsibility to maintain and
• enhance the environment. ••„,•
-------
037
-5-
Supporting Statement
Attached to this Petition is a Report prepared by Arthur
R. Tamplin, Ph.D. and Thomas B. Cochran, Ph.D. entitled Radia-
tion Standards for Hot Particles, dated February 14, 1974.
This Report and the documents referenced therein provide the
principal support for and elaboration of this Petition. The
hot particle problem underlying this Petition can be briefly
summarized as follows:
The existing biological evidence indicates that exposure
to airborne hot particles of plutonium at the levels permitted
by existing guidelines is extremely likely, indeed almost
certain, to lead to lung cancer in the exposed individuals.
Such exposures have occurred at the AEC's plutonium facility
at Rocky Flats, Colorado. Moreover, it has been shown that the
environment around the Rocky Flats facility has also been
contaminated with plutonium from the facility. As a consequence
some members, of the general public have also been exposed to
this material.
-------
-6-
These exposures involved minute particles^ of plutonivim
oxide (PuC^) . These particles can become lodged in the deep
respiratory tissue where/ because they are insoluble, they
remain fixed forayear or longer. During this time/ they
subject the surrounding lung tissue to an intense radiation
dose. For this reason they are called hot particles — that
is/ radiologically intense. While a single particle of Pu-239
oxide (one-millionth of a meter in diameter) in the lung of
an average man will deliver a dose of only 0.3 mrem per year
when averaged over the entire lung, the dosage to the tissue
actually irradiated (65 ug)* is 4,000,000 mrem per year
(4,000 rem per year). By comparison the same tissue would re-
f • •
ceive a dose of only 90 mrem due to natural 'background radia-
tion. This highly non-uniform hot particle irradiation poses
a unique cancer risk. • For the purposes of establishing
radiation exposure standards for hot particles, the risk of
cancer from a single hot particle in the lung should be con-
sidered equal to one chance in 2,000. As a result, Petitioner
"proposes that, when hot particles are involved, the existing
radiation standards governing plutonium exposure' should be
reduced by a factor of 115,000.
A ug is one-millionth of a gram.
-------
039
-7-
Proposcd Action
The action requested by Petitioner is detailed in Chapter VII
t • '
of the attached Report and summarized in Chapter VIII. The
Report, for the sake of clarity, is written with reference to
the hot particle formed from plutonium-23S. However, the
discussion in the Report and the standards sought to be estab-
lished are intended to be applicable to all radionuclidss or
mixtures thereof capable of forming hot particles.
As the Report and subsequent discussion on jurisdiction
indicate, several of the actions sought here are at least
partially within the jurisdiction of both EPA and the AEC.
Other proposals are apparently exclusively within AEC juris-
diction. It is not our purpose to postpone resolution of
this problem by jurisdictional squabbles. We jointly petition
both agencies in order to underscore our intent that between
them we believe the requested action must be taken. Each pro-
posal in the Petition should be deemed addressed to the agency
which will most quickly implement the recommendation.
-------
-8-
Jurisdiction
This Petition is addressed jointly to the Environmental
Protection Agency and the Atomic Energy Commission. Under the
Reorganization Plan No. 3 of. 1970, Sections 2 (a) (3) (ii) (C) ,
2(a)(6) and 2 (a) (7) , 42 U.S.C. § 4321, the Environmental Pro-
tection Agency became responsible for a broad range of regula-
tions related to radiation protection. Most significantly,
EPA is required to establish standards which are to be "generally
applicable. .. for the protection of the general environment
from radioactive materials-". Section 2 (a) (6). Three of the
standards proposed in the Report limit off-site exposures to
hot particles and are intended for the protection of the general
environment. "Two of these seek to establish the maximum per-
missible concentrations in air (MPCa) and on land (MPSC)
*_/
respectively. The third standard limits- the maximum per-
missible exposure resulting from nuclear facility accidents.
^/ Both of these standards are derived from the recommended
maximum permissible lung particle burden (MPLPS), which should
also be established as a standard.
-------
041
••9-
Pursuant to the provisions of the Atomic Energy Act of
1954, 42 U.S.C. §§ 2013(d), 2133(d), and 2201(b), the-AEG is
mandated to develop regulations and take other actions needed
to protect the health and safety of the public. The AEG has
adopted radiation standards which establish maximum permissible
concentration of plutonium-239 in air (see 10 CFR Part 20)
and has established limits for radiation exposure due to reactor
accidents (see 10 CFR Part 100). These standards fail to
address the hot particle problem or provide limitations which
will protect exposed persons from the risk of lung cancer
attendant upon exposure to hot particles, as described more
fully in the accompanying Report. The AEC's radiation pro-
.tection standards in these two areas are thus inadequate and
insufficient. They fail to implement the agency's mandate to
protect the health and safety of the public.
*7In 10 CFR Parts 20, 30, 31, 40, 50, 70, 71, 73, 100, and
115, the AEG regulates in whole or i'n part activities which
include the reprocessing and storage of nuclear wastes, plutonium
enrichment, transportation and storage of plutonium and other
activities from which the normal or accidental release of hot
particles could occur. None of th^se regulations have their
own limitations applicable to hot particle releases, although
Section 115.30 docs make Part 20 and Part 100 applicable to
all activities licensed under Part 115. It is Petitioner's
position that the AEG should provide specific regulations imple-
menting the recommendations and underlying principles of the
Report filed herewith for each relevant stage of the nuclear
fuel cycle.
-------
'042
-10-
In two areas relevant to the Petition, the AEG may have
exclusive jurisdiction. -First, the AEG must establish and
enforce provisions for occupational exposure to radiation.
42 U.S.C. §§ 2133, 2201(b) and (p); 29 U.S.C. § 653 (b) (1);
- 10 CFR Part 19 and S§ 20.101 et. seq. Specific limits for
worker exposure to hot particles are recommended in the
Report. These limits are consistent with the risks inherent
in the existing levels adopted for uniform whole body ex-
posure. Second, the AEG has now recognized the principle
that all radioactive releases should be kep as far below
permissible levels as is practicable. Thus, the AEG should,
after adoption of the standards recommended here, move
quickly to limit further hot particle releases to as low
as practicable levels. . '"'V '
-------
043
-ii-
Time for Action
We believe that matters of importance to the public
health and safety require prompt action. The matters we
raise here are based on data generally known and available
to both agencies for some.time. Allowing a reasonable period
for public comment we recommend that the standards requested
be set within six months.
.Pending and Proposed Action
We request that all approvals for construction or opera-
tion of any facilities for the handling, processing or re-
processing of plutonium or other radionuclides or mixtures
thereof capable of forming hot particles or for use of such
radionuclides be held in abeyance until final resolution of
the matters raised by this Petition. As to projects already
using or processing such radionuclides, we request that no
increase in the quantity of such radionuclides processed or
used be approved until final resolution of the matters raised
by this Petition.
-------
044'
-12-
Conclusion
The requested'action represents minimum steps which'must
be taken to protect the public from the dangers of hot particle
releases. Further actions consistent with and in furtherance
of the Report submitted herewith, including the adoption of
additional standards and guidelines, should be considered by
EPA and the AEC to assure that the public is provided the full
protection to which it is entitled.
Respectfully submitted,
Anthony Z. Roisnan
BERLIN, R'OISMAN & KESSLER
1712: N Street, N. W.
Washington, D. C. 20036
(202KJ23-9070
(A-t
J. Gustave Spoth
NATURAL RESOURCES DEFENSE COUNCIL
1710 N Street, N. W.
Washington, D. C. 20036
(202) 783-5710
Attorneys for Petitioner
February 14, 1974 -.
-------
045
Natural Resources Defense Council, Inc.
1710 N STREET. N.W.
WASHINGTON, D.C 20036
202 783-J710
Pah Alu Of a Ne
-------
Dr. William D. Rowe
046 July 19, 1974
Page Two ' .
I would appreciate hearing from you regarding these matters
at your earliest convenience.
Sincerely,
J.G. Speth
ccs L. Manning Muntzing
Peter W. Steketee
Carrie Dickerson
Ilene Younghein
-------
047
UNITED STATES ENVIRONMENTAL PROTECTION AGENCY
WASHINGTON. D.C. 20460
AUG 121974
f • *
Mr. J. G. Speth
Natural Resources Defense Council, Inc.
1710 N Street, N.W.
Washington, D.C. 20036
Dear Mr. Speth:
Thank you for your July 19 letter in which you requested
responses to several questions regarding our proposed information
hearings in order to obtain information on the environmental impact
of transuranium elements and to consider whether new or additional
guidelines or standards are needed. We will respond to your
questions in the order presented.
Since our proposed hearings are of a legislative nature for
information gathering purposes only, we do not intend to allow for
'discovery or cross-examination.
We consider the issues raised by the NRDC petition and the
information contained therein to be important sources of data on
the overall problem of the potential environmental impact of the
transuranium elements. Therefore, for these particular hearings,
we would hope that NRDC would want to introduce the material into
the proceedings so that the hearing record would be as complete as
possible. Regarding the manner in which EPA treats the NRDC peti-
tion, it will, of course, receive specific attention; however,
information gained at our proposed hearing may affect the ultimate
decision.
As regards to a suggested or possible jurisdictional problem
between AEG and EPA over the various rules and standards requested
in the NRDC petition, we see none. AEC has the authority, under
the Atomic Energy Act of 1954, as amended, arid under the general
--..idaiica approved by the President of the Federal Radiation Council's
(i'RC) mandate "to encourage the maintenance of radiation doses as
far below the guides as practicable," to establish regulations for
controlling occupational exposures, and for specifying effluent
limits for its activities. However, EPA through the President's
Reorganization Plan No. 3 of 1970 now has the FRC authority and it
tuay consider revision of the basic FRC radiation protection guides
and recommend to the President guidance for Federal agencies to
-------
048,
cover occupational radiation standards. Also, EPA has the authority
to establish generally applicable environmental standards for the
protection of the general environment from radioactive materials.
This includes transuranium elements as well as others. As a result
of our proposed' hearings and the information obtained therein, we
will then decide if additional guidance or standards are required.
We have not decided as yet who will chair the proposed hearings
or the actual format to be followed. These are matters that are
currently receiving serious attention by the ORP staff and a decision
should be made by the Agency within the next several weeks. We do
not envisage AEC having any role in the hearings different from any
other agency, public group, or individual who may wish to present
information. We plan to make a serious and honest effort to obtain
expressions of thought from all interested persons during the
hearings. Therefore, we will publicize on a wide-scale the fact
that we will hold such hearings so that no one will be denied an
opportunity to present information. At the same time, we may be
restricted by time elements or some other unforeseen circumstances;
however, no one individual, group, or agency will be permitted to
take an unreasonable amount of the hearing time. In summary, we are
attempting, through these proposed hearings, to obtain all pertinent
information and do this with an appropriate balance and perspective.
If you would care to meet with me to discuss further any of
these comments or any other suggestions you may have on our proposed
hearings, please let me know.
Sincerely yours,
W. D. Rowe, Ph.D.
Deputy Assistant Administrator
for Radiation Programs (AW-558)
-------
049
Natural Resources Defense Council, Inc.
1710 N STREET, N.W.
WASHINGTON, D.C. 20036
202 783-5710
Pah Aim Of a Ntw Yer
664 HAMILTON AVENUE " • 15 WEST 44ih STRE
PALO ALTO. CALIF. 94301 ' NEW YORK. N.Y. 1C
413 327-1080 _ , ' ' 212 869-OUO
August 19, 1974
Dr. William D. Rowe
Deputy Assistant Administrator
Office of Radiation Programs
U.S. Environmental Protection Agency
401 M Street, S.W.
Washington, D.C. 20460
Re: NRDC Petition Regarding Radiation Standards for
Hot Particles ' '
Dear Dr. Rowe:
I have received your letter of August 12 in which you state
that "Since our proposed hearings are of a legislative nature for
information gathering purposes only, we do not intend to allow
for discovery or cross-examination." Naturally, we are disappointed
in this decision and urge that you reconsider it.
It is not completely accurate to say that the forthcoming
hearings are "for information gathering purposes only." A more
basic purpose of these hearings, at least the portion of them
responsive to our petition, is to provide a basis for formal rule-
making determinations which could have profound impacts on the
health and safety of all future generations. 'It is imperative in
this proceeding that every effort be made to probe the expertise
and competence of witnesses, to establish as fully as possible the
facts as best they are known, and to ventilate completely differ-
ences in expert opinion, thus establishing the often implicit bases
for these opinions. Cross-examination and other adjudicatory pro-
cedures have long been recognized as essential to these purposes.
Should EPA or any other federal agency arrogate to itself the full
responsibility for the course and outcome of these critical hearings
by denying to public groups the opportunity to make an effective
presentation?
If it becomes necessary for us to challenge the EPA or AEC
disposition of our petition regarding hot particles, we will be
forced to raise in such a proceeding any inadequacies in the
-------
I'JU Dr. William D. Rowe
August 19, 1974
Page Two
procedural rights accorded us at the agency level, including,
for example, the denial of the right to cross-examination.
Sincerely,
J.G. Speth
cc: Edson Case
-------
Natural Resources Defense Council, Inc.
BOARD OF TRUSTEES
Stephen P. Duggan, E.q.
Dr. Dean E. Abrahamson
Mr.'. Louis Auchinclos!
Bofil I. Bitlkct. Esq.
Dr. Rene ]. Dubos
Df. Joshua Lcderberg
Anthony Mazzocchi
Michael Mclntosh
John B. Oakci
Dr. Gilford B. Pinchot
John R. Robinson, Esq.
Laurance Rockefeller
J. WUlard Roosevelt
David Sive. Esq.
Dr. George M. WoodweU
Edwin M. Zimmerman, Esq.
1710 N STREET, N.W.
WASHINGTON, D.C. 20036
202 /83O710
The Hot Particle issue:
-f UTACU
OI WASH
•. Tjolat-oc +-/->
3S Xt Relates tO
Hot Particle Hypothesis
«"» rer* O^rrt
u ^^^ 4^ STREET
NEW YORK. N.Y. 10036
212 869-0130
ral.AK,Offi«
f^ HAMILTON AVENUE
PALO ALTO. CALIF. 94301
4^3 327-1080
by
Arthur R. Tamplin
Thomas B. Cochran
November 1974
"A Radiobiological Assessment of the Spatial Distribution
of Radiation Dose from Inhaled Plutonium," WASH 1320,
U* S. Atomic Energy Commission [September 1974].
-------
052
I. Background
On February 14, 1974, the Natural Resources Defense Council
(NRDC) petitioned the Atomic Energy Commission (AEC) and the
Environmental Protection Agency (EPA) to amend their radiation
protection standards applicable to "hot particles" of plutonium
' and other actinides where hot particles were defined more fully
in an accompanying report. The report (referred to herein as
the Tamplin-Cochran Report) concluded that the existing radiation
protection standards are grossly inadequate to protect workers
and the public from the high cancer risk posed by exposure to
the atmospheric release of plutonium particulates from the
nuclear power and weapons industries. The report recommended
(and the petition requested) that the current standards be
made more restrictive by a factor of 115,000. In the petition
NRDC indicated that matters of importance to the public health
and safety such as this require prompt action. Allowing a
reasonable period for public comment NRDC recommended that the
proposed standards be set within six months (by August 14, 1974).
On March 15, 1974, the AEC released its Draft of the Liquid
Metal Fast Breeder Reactor Program Environmental Impact State-
ment (DRAFT LMFBR EIS). This statement contained a 15-page
discussion of the hot particle problem.2 This discussion, based
I/ Tamplin, A. R. and T. B. Cochran, "Radiation Standards for
Hot Particles," Natural Resources Defense Council, Washington,
D. C., 14 February, 1974.
2/ DRAFT LMFBR EIS, Vol. II, Part 2, Section 4.G.5, pp. 4.G-89
to 4.G-105, March 1974.
-------
053
on an earlier report by John W. Healy (referred to herein as
the Healy Report) of Los Alamos Scientific Laboratory, was
used as justification for ignoring the approach taken in the
Tamplin-Cochran Report for estimating the lung cancer incidence
associated with the inhalation of plutonium particulates (hot
particles) and using instead the assumption of uniform lung
exposure even where hot particles are concerned.
On March 28, 1974, the AEG gave notice in the Federal
Register (39 Fed. Reg. 11450) of NRDC's filing of its petition
and requested public comments by May 28, 1974.
On April 16, 1974, NRDC submitted to the AEG a critique
of the hot particle discussion in the DRAFT LMFBR EIS. Since
the hot particle discussion in the DRAFT LMFBR EIS drew heavily
from the Healy Report (much of it reproduced verbatim) , the
NRDC comments were a critique of the Healy Report itself.
On August 5,_ 1974, the AEG announced that it was releasing
a draft Generic Environmental Statement on Mixed Oxide Fuel
(DRAFT GESMO) , i.e., recycled plutonium in light water reactors.
NRDC in a letter of February 21, 1974, had requested that the
AEC give in this generic environmental statement a full and candid
3/ Healy, J. W., "Contamination Limits for Real and Personal
Property," Los Alamos Scientific Laboratory, Los Alamos, New
Mexico, LA-5482-PR, January 1974.
4/ NRDC Comments on WASH 1535, Draft Environmental Impact
Statement, Liquid Metal Fast Breeder Reactor Program, Re: Volume
II, Part 2, Section 4.G.5, Particle Lung Dose Effects, pp. 4.G-89
to 4.G-105, 6 May 1974.
-------
054 - 3-
discussion of the recommendations and supporting evidence presented
in the NRDC petition and accompanying report.
In the DRAFT GESMO, just as in the DRAFT LMFBR EIS, the
uniform exposure assumption was used to calculate the lung
cancer risk from hot particle exposures. The first paragraph
of the following quote from the DRAFT GESMO gives the justifica-
tion for this assumption. The two remaining paragraphs describe
the AEC's treatment of the NRDC petition and the Tamplin-Cochran
Report in the DRAFT GESMO.
Over the past 30 years concern has arisen from time to
time_about the possibility that radioactivity concentrated
in discrete particles might be more potent when in contact
with living tissue than the same activity diffusely
distributed through the same tissue (hot particle
hypothesis). Numerous studies to investigate this
hypothesis provide evidence that present standards
have been esrisiJ.ls-.hed on a sound basis. 2 The standards
setting bodies have not set different limits for these
two types of exposure to radioactivity. Diffuse radiation
of tissues is used to calculate dose. Hence this approach,
that is diffuse irradiation of tissues, has been used
. in the preparation of this statement.
The AEC has been asked by the Natural Resources Defense
Council, Inc. (NRDC) to consider the "hot particle"
hypothesis in this generic environmental statement on
the use of mixed oxide fuel. Appendix D presents key
elements of a report by Arthur R. Tamplin and Thomas B.
Cochran-3 submitted by NRDC as well as selections from
a report by J. W. Healy.2 The Healy study is a broad
review of investigations on this subject and generally
supports the prevailing position of the standards setting
bodies.
The Natural Resources Defense Council, Inc. has raised
again the question of the effect of "hot particles"
in a petition filed with the Atomic Energy Commission,
requesting that a reduced limit be imposed upon the
concentration of plutonium in air for particles of a
specified high activity. This matter is being given
careful consideration in a separate proceeding.->
S/ DRAFT GESMO,p. IV J-7.
-------
~4~ 055
NRDC filed its petition requesting the reduction in the
Plutonium standards with the agencies charged with the responsi-
bility. In its first official statement on this issue subse-
quent to the NRDC petition, the AEC presented in the DRAFT
LMFBR EIS an argument based on the Healy Report. NRDC responded
with a critique (NRDC's comments on the DRAFT LMFBR EIS), setting
aside the Healy Report by rebutting each of the points raised
in the DRAFT LMFBR EIS and showing why the references cited do
not support the hypothesis that hot particles can be analyzed
in the same manner as uniform organ exposures, either for pur-
I
poses of estimating carcinogenic risks or for establishing
radiation standards. Four months after submitting those comments,
we were presented with the second AEC pronouncement on the hot
particle issue (DRAFT GESMO). Here, the AEC used as justification
the original Healy Report and made no reference to NRDC's
comments. There was absolutely no justification for this
aberrant behavior by the AEC.
We are now presented with the third pronouncement on this
subject by the AEC in the report by Bair, Richmond and Wachholz
(referred to herein as the BRW Report). As we shall show in
our critique, it is for the most part an elaboration on the Healy
report. Moreover, this report also fails to acknowledge and
discuss our comments on the Healy Report submitted some six months
6/ Bair, W. J., C. R. Richmond and B. W. Wachholz, A Radio-
biological Assessment of the Spatial Distribution of Radiation
Dose from Inhaled Plutonium, WASH-1320, USAEC, September 1974.
-------
056 - 5 -
ago on April 16, 1974, relative to the DRAFT LMFBR EIS. In
this respect, it is also significant to note that on May 22-24,
1974, the AEC sponsored a symposium on the biological effects
of plutonium at Los Alamos, New Mexico. Attendance was by
invitation. The authors, Bair, Richmond and Wachholz were
invited but we were not invited. When we submitted our report
and petition to the AEC, we had hoped that this would lead to
a dialogue that would serve to resolve this important issue.
However, it appears that the AEC refuses to engage in this
dialogue either face-to-face or in writing. It appears to us
that the simplest elements of professional responsibility would
require that they respond to our refutation of their arguments
rather than continually raising the same arguments in successive
publications. To this end, we again respond to their arguments.
We begin by reviewing the principal elements of the hot particle
hypothesis.
II. The Hot Particle Hypothesis
The "hot particle hypothesis" is relatively simple.
With respect to alpha-emitting particles in the lung, it is:
If a particle deposited in the deep respiratory tissue
is of such activity as to expose the surrounding
lung tissue to a dose of at least 1000 rem in 1 year,
this particle represents a unique carcinogenic risk.
The biological data suggest that such a particle may
have a cancer risk equal to 1/2000.
This hypothesis implies that if a particle exposes the
surrounding lung tissue to a dosage greater than 1000 rem in 1
year, the cancer risk is still 1/2000. (This of course causes
a larger particle to be less effective on a per uCi basis,
-------
-6- 057
but not on a per particle basis.) The hypothesis implies nothing
about particles that expose the tissue to less than 1000 rem
in one year.
The basic support for the hypothesis derives from a number
of experiments wherein a small volume of tissue was exposed to
high dosage. In these experiments cancer was the almost inevitable
result. Although it is not explicitly stated, these experiments
are relevant to the following NCRP criteria:
(206) Simplifications in practice hinge largely on
reporting a single representative protection dose for a
•limiting organ system even when the actual irradiation
is grossly non-uniform. The representative dose is
taken as the highest that can be obtained by averaging
over a prescribed significant volume. The implication
of this concept, or at least the convention that is
followed, is that any redistribution of.a given dose . -
within such a volume does not materially alter the
.radiation response. It is usually assumed that the "sig-
nificant volume" should be of the order of one cubic
centimeter. This will be grossly conservative.
(207) There will be some cases in which selection of
.a significant volume is inappropriate. Most notably
these will include cases where the radiation agent is
an alpha particle emitter deposited in thin sheets. As
an example, the deposition of radon daughter products
on the bronchioepithelial lining of the lungs is a
case in which the effective radiation field is virtually
two-dimensional only. In such cases, one may plausibly
consider a significant area of tissue surface, perhaps
equally arbitrarily taken as one square centimeter.
Realistic modeling of such cases suggests a much smaller
region as the reasonable effective target.7
The hypothesis is essentially an extension of"these criteria.
The quantitative parameters in the hypothesis are derived from
a series of experiments conducted by Dr. Roy C. Albert on rat
7/ NCRP Report No. 39, Basic Radiation Protection Criteria,
NCRP Publications, Washington, D. C., January 15, 1971.
-------
058 - 7 -
8—10
skin. In these experiments, Dr. Albert observed that the
radiation induced cancers were remarkably correlated with the
disruption of a critical architectural unit of the skin, the
hair follicle. The cancers were induced in the rough proportion
of 1 cancer per 2000 atrophied hair follicles when the dosages
exceeded some 1000 rem.
The hot particle hypothesis thus suggests that if these
skin experiments were performed with small particles, each
capable of disrupting a single hair follicle, the observed cancer
induction would correspond to one cancer per 2000 particles.
So far as the lung is concerned, the hypothesis contains
the corollary that the lung also has such a critical architectural
unit that can be disrupted by a single particle and that this
also presents a cancer risk of 1/2000.
The potential hazard of a single hot particle embedded
in the tissue of humans is illustrated by the observation of
Lushbaugh and Langham. They excised a nodule that developed
8/ Albert, R. E., F. J. Burns, and R. D. 'Heimbach, "The effect
of penetration depth of electron radiation on skin tumor forma-
tion in the rat," Radiation Res. 30, 1967, pp. 515-524.
9_/ Albert, R. E., F. J. Burns, and R. D. Heimbach, "Skin damage
and tumor formation from grid and sieve patterns of electron
and beta radiation in the rat," Radiation Res. 30, 1967, pp. 525-
540.
10/ Albert, R. E., F. J. Burns, and R. D. Heimbach, "The
association between chronic radiation damage of the hair follicles
and tumor formation in the rat," Radiation Res. 30, 1967,
pp. 590-599.
ll/ Lushbaugh, C. C. and J. Langham, "A dermal lesion from
Implanted plutonium," Archives of Dermatology 86, October 1962,
pp. 121-124.
-------
" 8" 059
- * •
around a Pu-239 particle imbedded in the palm of a machinist.
Commenting on the histological examination of the lesion, the
authors state:
The autoradiographs showed precise confinement
of alpha-tracks to the area of maximum damage
and their penetration into the basal areas of the
epidermis, where epithelial changes typical of
ionizing radiation exposure were present. The
cause and effect relationship of these findings,
therefore, seemed obvious. Although the lesion
was minute, the changes in it were severe. Their
similarity to known precancerous epidermal_cyto-
logic changes, of course, raised the question of
the ultimate fate of such a lesion should it be
allowed to exist without surgical intervention....12
Considering the above observations, it would be surprising
indeed if a physician would not suggest surgical intervention
in a case where a patient had a few such imbedded particles.
We feel that this lesion alone should cause one to be very
cautious in estimating the hazard of hot particles.
That such lesions can develop in lung tissue is supported
by the observations of Richmond, et al., on the lesions induced
in experiments wherein hot particles were introduced into blood
vessels of the lungs of rats:
Such a lesion with collagenous degeneration and
subsequent liquefaction, due to the large local dose
of radiation at a high dose rate, has been reported
by Lushbaugh et al., (9) whose description of a plutonium
lesion found In the dermis is very similar to that
observed for plutonium in the lung.13
12/ Ibid., p. 463.
13/ Richmond, C. R. , et al_._, "Biological response to small
discrete highly radioactive sources," Health Physics,18, 1970,
p. 406.
-------
060
The above represents the distilled essences of the Tamplin-
Cochran Report which was an extension of some earlier publica-
14
tions of Professor Donald Geesaman. It is important to
restate that the hypothesis suggests that the disruption of
a critical architectural unit of a tissue is a significant
carcinogenic event.
The actual killing of cells and the development of a
fibrotic lesion surrounding the hot particle is the suggested
mechanism of carcinogenesis. As Geesaman stated:
Summing up, intense radiation exposure of mammalian
skin and lung tissue commonly results in cancers.
Tissue injury and disturbance are a primary con-
sequence of intense radiation insult, and are observed
in association with carcinogenesis. Albert has
exhibited a simple proportionality between skin
carcinomas and atrophied hair follicles. No general
description of precarcinogenic injury exists, but
in a crude sense the available observations are
compatible with the idea of an injury-mediated
carcinogenesis. Cancer is a frequent instability
of tissue. Since tissue is more than an aggregate
of cells, and has a structural and functional unity
of its own; it would not be surprising if some
disrupted local integrity, a disturbed ordering,
comprises a primary pathway of carcinogenesis. The
induction of sarcomas with inert discs of Mylar.
cellophane, Teflon and Millipore (Brues, et al.x')
is indicative that such a mechanism exists. Pre-
sumably mitotic sterilization is an important factor
in any carcinogenesis mediated by radiation-induced
tissue injury. The functional relation of this factor
in the carcinogenic response may be quite different
from a linearity in the surviving mitotic fraction.
14/ Geesaman, D. P., An Analysis of the Carcinogenic Risk
from an Insoluble Alpha-Emitting Aerosol Deposited in Deep
Respiratory Tissue, UCRL-50387 and UCRL-50387 Addendum,
Lawrence Livermore Laboratory, Livermore, California, 1S68.
-------
- 10 - 061
While regrettably unquantitative, the hypothesis of
an injury-mediated carcinogenesis is suggestively
descriptive. If the respiratory zone of the lung
contains a structure analogous to the rat hair
follicle, and if a radioactive particulate deposited
in the respiratory zone has the capacity to disrupt
one or more of these structures and create a pre-
cancerous lesion, then cancer risks of the order of
10~3 to 10""^ per particle can be expected. 15,16
The lesion excised by Lusbaugh and Langham from human
1 &
palmar tissue and the observation by Richmond, et al., that
similar lesions are produced in the lung by hot particles
strongly argue that a comparable sensitive structure is present
in the lung and other tissues. Thus, the uncertainties in the
hot particle hypothesis involve these quantitative parameters:
a) Is the risk of cancer per disrupted tissue mass
comparable to that per disrupted hair follicle?
b) Is a particle capable of irradiating the surrounding
tissue mass at the rate of 1000 rem/year sufficient
to produce such a lesion?
The thrust of the NRDC petition to modify the plutonium
exposure standards is that, until these uncertainties are
resolved, the prudent public health principle is to accept the'
hot particle hypothesis rather than the less conservative
hypothesis that average organ dose from hot particles provides
15/ Geesaman, D. P., UCRL-50387 Addendum, op. cit., pp. 6-7.
16/ Brues, e_t al. , refers to Brues, A. M. , H. Auerbach,
G. M. De Roche, and D. Brube, "Mechanisms of carcinogenesis,"
Argonne National Laboratory, Biological and Medical Research
Division Annual Report for 1967, ANL-7409, 1967, pp. 151-155.
17/ Lushbaugh, C. R. and J. Langham, op. cit.
18/ Richmond, C. R. , e_t al., op. cit.
-------
062
- ii -
a reasonable basis for protection. The implication is, of course,
that while the evidence discussed in the Tamplin-Cochran Report
supports the hot particle hypothesis there is no substantial
body of scientific evidence that can reject the hypothesis. The
purpose of this report is to demonstrate that the evidence is
also not to be found in the BRW Report.
III. Points of Analytical Confusion
Before reviewing the BRW Report in detail the following
general observations are presented in order to draw clear
distinctions among several analytical approaches or concepts
that appear to be the source of some confusion to analysts
addressing the hot particle issue. These approaches are:
(1) The assignment of a risk per hot particle, independent over
a range of particle sizes and activities; (2) the comparison
of the risk associated with a fixed amount of activity (or
absorbed dose) when spread uniformly over tissue with the risk
when the same activity (or absorbed dose) is spread non-uniformly
over the same tissue; (3) the concept of "wasted radiation"
and/or "overkill." It is essential that these three approaches
or concepts and their relationships (or distinguishing features)
1)6 clearly understood before judging the relevance of experimental
data to the hot particle issue. We begin by reviewing each
approach or concept and then examine their relationships of (2)
and (3) to (1).
-------
- 12 -
063
(1) Risk Per Hot Particle —'The assignment of a risk
per hot particle is based on a hypothesis that when the radiation
dose to the irradiated tissue mass surrounding a radioactive par-
ticle is sufficient to disturb a critical architectural unit of
the tissue, such a disrupted tissue mass poses a unique carcin-
ogenic risk. A value is assigned for the tumor risk associated
with the disrupted tissue. Since for small particles there is
a one to one correspondence between the disrupted architectural
unit and the associated radioactive particle, this tumor risk
is the risk per particle. In the Tamplin-Cochran Report, a lower
limit on the radiation dose (and therefore alpha activity) to
disrupt the architecture was assigned (1000 rem to the irradiated
tissue) and used to define a hot particle. No opinion was
offered with respect to the appropriate risk function for doses
(or activities) below this cutoff value. In the lung there is
an upper limit on the size of particles that are deposited in
the deep respiratory tissue. Hence, in the lung there is a
"window" on the hot particle size and activity. In analyzing
experimental data vis-a-vis the hot particle hypothesis the
relevant parameter is the tumor risk per hot particle.
(2) Uniform Versus Non-Uniform Exposure — Present radia-
tion standards are based on (i.e., establish limiting values
for) the concept of radiation dose equivalent (units of rem) to
the whole body and certain critical organs. In the calculation
of the rem dose a "dose distribution factor" is assigned in order
that the risk associated with a non-uniform distribution of a
given type of radiation exposure to the critical organ is
-------
064
consistent with uniform exposure by the same type of radiation.
Consistent with this approach experiments have been designed
and analyzed to assess the difference between uniform and non-
uniform distributions of dose to critical organs. For internal
alpha-emitters the absorbed dose (in rads) to a critical organ
is proportional to the total activity in the organ.19 Hence,
tumors per microcurie has been the primary parameter used
when comparing tumor risk for uniform versus non-uniform dose
distributions.
(3) Wasted Radiation — The concept of "wasted radiation"
or "overkill" has been invoked to describe that fraction of the
radiation which kills cells, where these dead cells are assumed
not to contribute to tumor production. For example, the dose rate
in the immediate vicinity of a single alpha-emitting particle
in the lung (or other tissue) can be high enough (given a
sufficient particle activity) such that even a limited residence
time in the tissue will result in the death of cells within
a given radius. Since such cells can not reproduce it has
been hypothesized that they would not lead to cancer.20 An
alternative hypothesis, consistant with the hot particle
hypothesis, is that the presence of dead cells, cellular pro-
ducts or fibrosis may be required for tumor production.
19/ This is also generally true for beta-emitters.
20/ The concept of "wasted radiation" also has been invoked
to describe the radiation dose during the period from the in-
ception of initial malignancy until detection or death. The
concepts of overkill and wasted radiation have been used inter-
changeably.
-------
065
In order to demonstrate the relationships among the three
approaches and concepts described above it is useful to analyze
some hypothetical experiments. We do this below:
Tumors/pCi or Tumors/Particle — Suppose one ran a series
of related experiments involving hot particles in tissue where
the tissue mass and the total activity were held constant across
experiments (e.g./ the same number of lungs exposed to 12 nano-
curies total activity in each experiment), and the experiments
differed only in the number of particles and the activity per par-
ticle. Consistent with the hot particle hypothesis (one tumor per
2000 hot particles) suppose one observed a tumor incidence given
below in the second column from the right.
Experiment
1
.2
3
4
Number
of Hot
Particles
6000
4000
2000
200
Activity per
Particle (pCi)
2
3
6
60
Number of
Tumors
Observed
3
2
1
0
Tumors
per nCi
0.25
0.17
0.08
0.00
From the observed number of tumors and the total activity (12
nCi), the tumors per nanocurie are calculated in the last column.
Holding the total activity and tissue mass as constant while
increasing the number of particles tends to make the exposure more
uniform. Hence the results, when analyzed on a tumor per
nanocurie basis (the last column), appear consistent with the
view that uniform exposure carries a higher risk than non-uniform
exposure. But these same experimental results are exactly
consistent with the hot particle hypothesis. What does this
tell us? First, it clearly demonstrates that an analysis of
-------
066
an experiment, or series of experiments, on a tumor per nanocurie
or microcurie basis, the results of which appear consistent
with the concept that uniform exposure carries a higher tumor
risk than non-uniform exposure, is not in itself a refutation
of the hot particle hypothesis. In fact, if the hot particle
hypothesis is correct, an analysis based on tumor per microcurie
is irrelevant. One can just as easily design a series of
experiments consistent with the hot particle hypothesis, which
when analyzed on a tumor per microcurie basis suggests the
opposite, that is, uniform exposure carries a smaller risk than
non-uniform exposure, as is the case with respect to the two
experiments below.
Experiment
1
2
Number of
Particles
6000
4000
Total
Activity
(nCi)
12
6
Number of
Tumors
Observed
3
2
Tumors
per nCi
0.25
0.33
Again, if the hot particle hypothesis is correct, the analysis
based on tumors per microcurie would be irrelevant. If tumor
production depends on the number of disrupted architectural
units independent of particle activity (over a range of activities) ,
analyzing the data on a tumor per microcurie basis clearly
makes no sense. One would not expect, a_ priori, a correlation
between tumors per microcurie and numbers of particles (uniformity
of dose). To the contrary one should not be surprised to see
conflicting experimental results (i.e., some experiments suggesting
uniform exposure carries a higher risk and other experiments
-------
- 16 -
067
* ' * • *
suggesting the opposite). The relevant parameter to judge the
hot particle hypothesis is tumors per hot particle/ not tumors
per microcurie.
At this point we might add that in addressing the hot
particle issue, an analysis based on tumors per microcurie
(or tumors per rad), where the radiation exposure is from other
than hot particles (and therefore a different carcinogenic res-
ponse mechanism may be controlling), is also irrelevant and is
simply a compounding of mistakes.
We do not imply that comparisons of the risks associated
with .uniform and non-uniform exposure serves no useful purpose.
Consider, for example, radium-226 and plutonium-239 which are
both alpha-emitters and both bone seekers, that is both are
preferentially deposited in the skeleton. The cancer risk per
microcurie deposited in the skeleton (or per rad) is about
five times,higher for plutonium than radium. This suggests
that plutonium is preferentially deposite'd in tissue more
sensitive to the development of bone cancer, and that in calcu-
lating the dose equivalent (rem) to the-skeleton due to plu-
tonium the use of a dose distribution factor of 5 is appropriate.
However, this clearly has no relevance to the hot particle
hypothesis which is an entirely different effect, aside from
the fact that the distribution factor for plutonium in the bone
is based on soluble plutonium and not hot particles.
Hot Particles and Wasted Radiation — Turning next to the
concept of wasted radiation, suppose one were to implant one hot
particle of alpha activity in a critical organ such as the lung.
Under the hot particle hypothesis it would carry a tumor risk
-------
068
- 17 -
equal to the assigned risk per particle, one in 2000. As long as
the particle activity remained above the cutoff limit defining a
hot particle, changing the activity, for example doubling it,
would not change the lung tumor risk. If the activity and there-
fore the radiation dose were doubled without a change in the tumor
risk, one could invoke'the concept of "wasted radiation" or "over-
kill." At least one-half the activity (more than one-half if
the particle activity were greater than twice the minimum defining
a hot particle) would be "wasted." The hot particle hypothesis is
consistent with the concept of "wasted radiation." But more
important, the concept of "wasted radiation" is clearly irrele-
vant in judging the validity of the hot particle hypothesis. •
What is important, is the assessment of the risk per particle
over the range of particle sizes defining hot particles. The
relevant parameter in this assessment is again, the tumor risk
per hot particle.
1V- Page by Page Critique of the BRW Report
In this section we will present a page by page critique
of the BRW Report. To avoid confusion we will use.their method
for bibliographic citation. Their bibliography is reproduced
at the end of this section.
Page 1. "Summary and Conclusions." We will comment on
the conclusions in this section as we review the related material
in the main text of the report, only noting here that the con-
r
elusions are without merit.
-------
- 18 - 069
Page 3. "I. Statement of the Problem." We generally
agree with this statement of the problem, noting only that the
hot particle hypothesis is based on damage to a critical
architectural unit as opposed to individual cells. The
discussion here is essentially the same as the discussion
on pp. 15-17 of the Tamplin-Cochran Report and Table I in
the BRW Report is comparable to Table III in the Tamplin-
Cochran Report.
Pages 5-7. "II. Background." This is a general discussion
of consideration of irradiation from radioactive materials in
particulate form by several organizations concerned with radiation
protection, including the ICRP, NCRP and National Academy of. •
Sciences—National Research Council (NAS-NRC) . The thrust of
this discussion is that (1) non-uniformity of dose has been
recognized, been of interest, and periodically reviewed since
the early days of the Manhattan Project, and (2) organizations
with responsibility for recommending radiation standards, such
as ICRP, NCRP and NAS-NRC, have never recommended a change
from the current practice of basing radiation standards on the
mean dose to organ. While the hot particle problem is well
recognized in the biological community, and while we agree with
the observations above, we do not believe the conclusion reached
on page 7 by the authors of the BRW Report is appropriate,
namely:
The fact that these organizations have not changed or
recommended changes in the procedures used for calcu-
lating dose to the lung as the result of their deli-
berations is an implication of implicit guidance on
this particular problem.
-------
070
- 19 -
To the contrary, had these organizations intended that this
conclusion be drawn, they would have made it explicit. In
its Publication 9, the ICRP (1966) states (p. 4):
...In the meantime there is no clear evidence to
show whether, with a given mean absorbed dose, the
biological risk associated with a non-homogeneous
distribution is greater or less than the risk re-
sulting from a more diffuse distribution of that
dose in the lung.
And the NCRP (1971) offers the similar statement (pp. 79-80):
(210) The NCRP has arbitrarily used 10 percent
of the volume of the organ as the significant volume
for irradiation of the gonads. There are some
cases in which choice of a significant volume or
area is virtually meaningless. For example, if a
single particle of radioactive material fixed in
either lung or lymph node may be carcinogenic, the
averaging of dose either over the lung or even over
one cubic centimeter may have little to do with this
case.
The appropriate interpretation of these remarks by the ICRP
and NCRP is that there is no guidance as to the risk for
non-homogeneous exposure in the lung. The intent of these
remarks is to call attention to exceptions to the general rule,
rather than to implicitly advocate averaging the dose over the
critical organ when the dose is grossly non-uliiform.
Page 7. With regard to the quotation from the ICRP Task
Group in Publication 14 (ICRP 1969), it is not at all clear that
the Task Group reviewed Geesaman's work before preparing
this ICRP report. Moreover, while the opinion of the Task
Group may be worth noting, it is important to note that it is
only an opinion and is totally unsupported in ICRP Publication
14. Considering this in 1974, it is significant that in the
intervening 5 years since the issuance of Publication 14,
-------
- 20 -
071
adequate support for that opinion has not been forthcoming and
as we demonstrate here is not to be found in the BRW Report.
Quite the contrary, the analysis of Geesaman and the Tamplin-
Cochran Report have emerged to support the opposite. The BRW
Report states that new data tend to support the ICRP Task Group's
opinion. With this, as we show in this critique, we totally i
disagree.
Pages 9-23. "III. Animal Studies." .'-... -
Pages 9,10. "A. Retention of Plutonium in Lung"
This section discusses the long retention time of PuO
in human lung. There is no controversy here.
Pages 10-12. "B. Spatial Distribution of Plutonium Within Lung"
This section, while attempting to indicate that Pu particles
in the lower respiratory region are not static, does admit on
page 12 that autoradiographic evidence demonstrates that such
particles are immobilized in scar tissue and possibly in Type
I alveolar epithelial cells. The long residence time of Pu
particles in the lung suggests that such immobilization must
occur.
Pages 12-23. "C. Pulmonary Neoplasia"
These pages present the animal data on Pu induced lung
cancers. The data on both soluble and insoluble Pu compounds
are presented. It is only those experiments that involve in-
soluble alpha-emitting hot particles that are of interest here.
Of those experiments discussed here, it is only those involving
Pu02 that are pertinent. Since these experiments are recanted
in the subsequent section of the BRW Report, we will briefly
discuss only a few of them here.
-------
072
- 21 -
Page 13. Mention is made here of an experiment (Bair,
et al., 1962) wherein 800 mice were subjected to inhalation
of 0.1 to 2 nCi per gram of lung. At time of death, these
animals had retained only 0.1 to 10 pCi in their lung. Moreover,
the report states that since so few autopsies were performed,
the lung tumor incidence is unknown. In other words, this
experiment is of little value to the hot particle problem.
The beagle dog experiment (Park, e_t al. , 1972) (Park
and Bair, 1974) did involve Pu hot particles. However, as we
indicated in the Tamplin-Cochran Report, since the tumor inci-
dence was essentially 100%, this experiment does little to
resolve the uncertainties in the hot particle hypothesis.
Page 15. The Pu-238 experiment by Sanders (1973) in-
volved Pu02 derived from crushed microspheres. However, Sanders
indicates that this material was "soluble" in his experiment and
that the irradiation was uniform. The observed rapid clearance
from the lungs supports this contention.
The baboon studies (Metivier, et al., 1972) relates to
hot particles but at quite large particle concentrations which,
as in the beagle experiment, makes it difficult to draw in-
ference relative to lower concentrations.
Pages 16-23. "D. Experiments of Special Relevance to Non-
Uniform Dose Distribution"
Page 16. This page is a confusing discussion of "wasted
radiation" and "overkill." As we stated in the previous section
of this critique, the hot particle hypothesis designates a
-------
- 22 -
073
minimum particle activity—one that delivers a dose of 1000 rem/year
to the irradiated tissue. Such a particle is suggested to have
a chance of producing cancer equal to 1/2000. Particles with
greater activity have the same chance, hence the concept of
"overkill" or "wasted radiation" is included in the hot particle
hypothesis.
This page also contains the following sentence and footnote:
For a single radioactive particle of 239 PuO, in the
lung (or other tissue), the dose rate near the particle_
can be high enough to cause the death of all cells within
a given radius even if the residence time of the particle
is short. Such cells will 'not^be able to reproduce and
subsequently result in cancer.
*The presence of dead cells, cellular products or
fiTarosis may be required before a cellular trans-
formation can express itself as a cancer. However,
this concept has not been generally accepted.
This same statement and footnote appeared in both the
Healy Report and the Draft EIS for the LMFBR with the significant
exception of the last sentence in the footnote. Even if this last
sentence were true, which we doubt, it is irrelevant because
matters of science are not determined by public opinion polls.
Nevertheless, we are curious concerning the method employed
by the authors of the BRW Report to establish this conclusion.
We have previously indicated that the hot particle hypo-
thesis implies an injury-mediated mechanism of carcinogenesis
as the footnote suggests (see pp. 9-10). There is no need to
repeat that discussion here. However, we submit that lesion
discussed by Lushbaugh and Langham (1962) is by itself so
-------
074
23 -
incriminating of hot particles that we are amazed that the
authors of the BRW Report are so reluctant to acknowledge the
potential hazard of such particles.
It is, however, obvious that this reluctance led to confusion
on their part. For example, the paragraph, from which the
above quote was extracted, ends on page 17 with this statement:
The relevant parameter is tumors per microcurie
because the basic question is how the risk from hot
particles compares with the risk from uniformly dis-
tributed radiation doses.
In the previous section of this critique we demonstrated
that the test of the hot particle hypothesis must be on the basis
of tumors per particle not tumors per microcurie simply because
particles can contain more than the minimum activity (and hence,
be "wasteful" on a per jaCi basis) . If the AEC had chosen to
engage in a dialogue with us, this simple but fundamental matter
could have been resolved and much of the extraneous material
in this BRW Report could have been eliminated (if not the entire
report).
Page 17. This page contains the following paragraph:
Two approaches have been used in skin experiments.
The first was to determine whether isolated small
areas of irradiated skin gave the same yield of
tumors per unit as large-area skin irradiations.
The focal irradiation pattern with low LET radiation,
electrons (Albert et al., 1967b), was less efficient
than the large area exposure in producing tumors.
However, with high LET radiation (protons) there was
no difference (Burns, et al., 1972). If these
results can be extrapolated to alpha radiation,
they suggest that the risk from particulate sources
is no greater than from uniformly distributed sources.
Apparently the authors of this paragraph do not understand the pur-
pose and significance of the experiment by Burns, et al., (1972)
-------
. 075
and this is reflected in the last sentence which makes no sense.
The purpose of the experiment by Burns, et al., was to deter-
mine the basis for the lower tumor producing efficiency of electrons
where the irradiation was performed in a sieve pattern. Since the
electrons are highly scattered, the focal radiation dose was un-
certain. With the relatively non-scattering protons, the sieve
'pattern produced the same number of tumors per area irradiated.
These experiments demonstrate that if 24 cm2 of rat skin
are irradiated to 1000 rem, one tumor will develop per animal.
If you irradiated 12 cm2 to 1000 rem, one tumor will develop
per two animals; 6 cm2 should produce one tumor per four animals
and so on. Moreover, the data strongly suggest that as the
area irradiated is reduced to that corresponding to a single
hair follicle, one tumor will develop per 2000 animals.
The next paragraph discusses the experiments of Albert,
et al., and ends with the following discussion:
A plausible explanation for the experimental results
is that each follicle has a population of stem cells
at a depth of 0.3 mm that are concerned with the pro-
duction of sebaceous cells and hair. . These stem cells
apparently constitute the most sensitive potential
oncogenic cell population to ionizing radiation in
the rat skin since all the tumors were mainly of hair
follicle origin (Albert, et al., 1969). Neoplastic
transformation of a significant number of these target
cells required large radiation doses which in turn
killed most of the target cells and thus caused fol-
licle atrophy.
This is a possible explanation but it does not set aside
the hot particle hypothesis. The killing of cells and the
consequent disruption of the tissue may well be sufficient by
itself for such "neoplastic transformation." The induction of
-------
- 25 -
076
tumors with mylar film and millipore•filters by Brues, et al.,21
would support this as would the precancerous cytological changes
observed around the lesion excised by Lushbaugh and Langham (1962)
and around the microspheres in rat lungs by Richmond, e_t al. ,
(1970).
Page 18. This page goes on to discuss other skin tumor
experiments and the first column ends by stating that the evi-
dence does not support the hot particle hypothesis as detailed in
the Tamplin-Cochran Report. We offer the above paragraph and
this entire critique as refutation of that contention.
The experiments of Richmond, e_t al. , (1970) are discussed.
This discussion, however, fails to note that Richmond, e_t al. ,
stated that the lesions observed in the rat lungs following
exposure to these hot microspheres were similar to that observed
by Lushbaugh and Langham (1962) in human palmar tissue.
Page 19. The experiment of Passonneau (1952) is mentioned
here. It was also discussed on page 17. This experiment is
simply a variation of the experiments of Albert, e_t al. , (1967a,
1967c, 1969).
Pages 19-20. These pages discuss the experiments of
Richmond with Sullivan and Voelz as reported in:
Richmond, C. R. and G. L. Voelz (eds.)
LA-4923-PR, pp. 18-34 (April 1972),
LA-5227-PR, pp. 1-11 (March 1973),
.and Richmond, C. R. and Sullivan, E. M. (eds.)
LA-5633-PR, pp. 1-9 (May 1974).
21/ Brues, A., et al., op. cit.
-------
- 26 -
077
- •
These are a series of progress reports on experiments
wherein raicrospheres of 239Pu02 and 238Pu02 incorporated in
Zr02 particles (10 p diameter) are injected into the jugular vein
of hamsters. These particles lodge in the capillary network of
the lung.
The BRW Report suggests that these experiments are a
strong argument against the hot particle hypothesis. We shall
show that while the experiments raise some questions concerning
the quantitative parameter in the hot particle hypothesis, they
also support the hypothesis. .
In the initial experiment 2000 particles per animal were
Injected according to the following dosage schedule (60 animals
per dosage level).
Isotope Level pCi/particle nCi/animal
Pu-239
1
2
2A
3
3A
4
5
6
0.07
0.22
0.42
0.91
1.60
4.30
13.30
59.40
0.14
0.44
0.84
1.82
3.20
8.60
26.60
119.00
Pu-238
Only two lung tumors developed in the experiments and they
occurred in the level 2A exposure group. However, the latest pro-
gress report (LA-5633-PR) mentions histological changes occurring
in the lungs of long term animals (15-20 months) in the 4-6 ex-
posure levels. Concerning these changes, Richmond and Sullivan
(1974, p. 7) stated:
There has been no increase in frank tumors observed
within the past year; however, the epithelial changes
described above could be considered as precursors of
peripheral adenomas.
-------
- 27 -
078
This suggests an incipient carcinogenic response to the particles
but the life span of the rats and hamsters is too short for the
development of a frank tumor.
Similar histological changes were observed in rats in-
jected with these microspheres by Richmond, et al., (1970) who
pointed to the similarity of these particle induced lesions in
the rat lung to that observed by Lushbaugh and Langham (1962) in
human palmar tissue.
For reference, in the beagle dog experiment lung tumors
developed (in all animals that survived 1600 days) some 5 to 11
years after the initial alveolar deposition of 3 to 50 nCi/gram
of bloodless lung (Park and Bair, 1972). The exposures were
by inhalation, not injection.
On a nCi/gram basis, the beagle exposures would correspond
to exposure levels 3 and above in the Richmond experiments.
But the medium activity per particle in the beagle experiment
corresponds to those in exposure levels 1 and 2 in the Richmond
experiments which suggests that with longer exposure periods,
lower activity particles (corresponding to levels 1 and 2)
can produce the histological changes observed in the rat and
hamster lung and in human palmar tissue. At the same time,
since the beagle exposures involved a spectrum of particle sizes,
it must be conceded that the carcinogenic response in the beagles
could have been elicited by the larger, higher activity particles.
In either case, the beagle dog data suggest that the
induction time for the hot particle mechanism of carcinogenesis
exceeds the life span of the hamster by some three years or more.
-------
- 28 -
079
Thus, the absence of a large carcinogenic response in the
hamsters does not set aside the hot particle hypothesis.
The Richmond experiments point out one of the uncertainties
in our quantification of the hot particle hypothesis but they do
not resolve it. We suggest that a lower limit for a hot particle
be one that contain'sufficient radioactivity to'deliver "an aver-
age dose of 1000 rem/year to the exposed tissue. For an alpha-
emitting hot particle, this limit corresponds to 0.07 pCi. In
LA-5633-PR the authors state with respect to this histological
change (p. 7), "This lesion has been observed almost entirely
in the higher activity levels (levels 4-6 and in animals given
relatively small number's of spheres (2000-6000)." A level 4
particle contained 4.3 pCi, some 60 times our limiting activity.
But, at the same time, had these experiments been performed
with animals that have longer life spans, it is quite possible
that 'these histological changes would have developed around
particles containing our suggested limiting activity.
Nevertheless, a 60 fold increase in activity requires
only a .4 fold increase in particle diameter—for Pu-239, a change
from 0.6 p. to 2.4 >A; for Pu-238, a change from 0.09 M to 0.36 p.
and for high burn-up nuclear fuel, a change from 0.4 ji to. 1.6 p.
These particles are still in the range that permits deposition
in the lower respiratory zone. Thus, these experiments do not
set aside the hot particle hypothesis. Rather they suggest
additional experiments involving longer lived animals to determine
whether this histological change progresses into frank tumors .
and whether lower activity particles also produce these changes.
-------
080
If an experiment comparable to these with hamsters
were initiated with beagles, it would serve to resolve these
uncertainties. Such an experiment would take some 15 years to
complete. In the meantime, we propose that prudent public health
practice dictates that exposure standards should be established
on the basis of the hot particle hypothesis.
The experiments of Little, et al., (1970a, 1970b, 1973}
are said to add significance to the microsphere experiments.
As we show subsequently, the experiments of Little, et al.,
involved uniform exposure to Po-210 at high dosage (above 8000
rem). These experiments therefore do not involve hot particles
and there is no a priori reason for assuming that they involve
the same carcinogenic mechanism as hot particles.
Pages 20-21. The experiments of Shubert, e_t al. , (1971)
and Brooks, et al., (1974) are discussed here. These experiments
made a determination of the frequency of chromosomal aberrations
in liver cells following uniform and particulate irradiation.
It is important to note that a causal relationship between
chromosomal aberrations and subsequent cancer development is
only a hypothesis. Moreover, as we have stated previously,
the actual killing of cells and the subsequent disruption of
the normal tissue architecture may well be the carcinogenic
mechanism for hot particles. Thus, these experiments are of
little value in resolving this issue.
Pages 21-22. The experiments of Little, e_t al. , (1970a,
1970b, 1973) and Grossman, e_t al., (1971) are discussed here.
In these experiments hamsters were exposed to Po-210 lung doses
-------
- 30 -
081
ranging from 8,000 to 20,000 rem. In some experiments the Po
was absorbed on hematite particles. However, calculations
demonstrate that the activity per particle ranged from 10~4
to ID'3 pCi22 and, consequently, that these were not hot particles.
Therefore, the conclusion of Little, ejt al. , (1973) quoted on
page 22 is not relevant to the hot particle issue.
We note in passing, however, the nature of the experiments
was that the entire lung was irradiated to very high dosage
although there was some aggregation of particles. A large car-
cinogenic response was initiated in each exposure group. The
preliminary data reported here indicate that the life span of
the hamster is longer when the dosages are this high and the
Po-210 is on particles. However, it is not sufficient to demon-
strate a reduction in overall tumor response. Like the beagle
experiments, the carcinogenic response in these experiments
appears to be saturated because of the high dosage delivered to
the whole lung of a major fraction thereof. No conclusions
can be drawn relative to lower doses nor relative to hot particles.
With respect to lower dosages, the work of Sanders (1973)
• demonstrates a large tumor incidence in rats at a dosage of 320
" rems.
Pages 22-23. These pages discuss the experiments of
Cember, et_ al. The major thrust of the Cember article deals
with 144Ce particles in the lung. The 144Ce was introduced
admixed with stable Ce as either CeF3 or CeCl3 in particles of
about 1 u in diameter (0.5 u3) . 144Ce emits a beta particle
22/ NRDC Comments on WASH 1535, op. cit., p. 39.
-------
082 " 31 "
of 0.275 MeV and its daughter product Pr emits a beta of
3 MeV. The rate of energy loss for these beta particles in
tissue is about 0.2 Kev/u compared to some 94 Kev/u for plutonium
alpha particles.
This difference in energy loss per micron indicates that
144
the activity of the Ce emitters would have to be some 500 times
that of the 39Pu in order to deposit the same energy in the
tissue irradiated by 239Pu alpha particles. Moreover, since the
QF for alpha particles is 10, the 144Ce particles must have an
activity (10) x (500) or 5,000 times that of a 239PuO_ particle
to qualify as a hot particle. Since the limiting activity of
a 239Pu02 particle is 0.07 pCi, a hot particle.of 144CeCl3
would have to contain more than 350 pCi. After correcting for
the half-life of 144Ce (288 days) a hot particle would have to
contain some 500 pCi.
The geometric mean diameter of the particles in these
experiments was 1 micron. The highest exposure group received
50 pCi of 144Ce in 30 ug of CeF . Allowing a density of
6 g/cm3 for the CeF3/ the beta-activity per particle of 1 u
diameter is only 5 pCi. In other words, these experiments did
not involve hot particles as defined above. The carcinogenesis
observed in these Cember experiments, which was considerable,
was related to high total and rather uniform organ dosage (1,000-
30,000 rad).
Page 23. Here the experiments of Sanders (1973) and
Moskalev (1972) are discussed. Large carcinogenic responses were
observed in the lungs of rats at doses of 100 to 500 rem
-------
083
using "soluble" Pu compounds. One conclusion that is justified
by the results of these studies is that the exposure standards
for plutonium may be much too high (at least 100 times too high)
even when hot particles are not involved. The results of Sanders
; indicate .#iat .a,' uniform dose of 15. remdpubled .the natural j-nci- ......
dence of lung cancer in the exposed rats. A worker is allowed
this dose each year and a member of the population could accumu-
late this dose in 10 years.
One further point could be made concerning the study of
Sanders. It is not at all clear from the description given in
the reference that the exposures did not involve a few hundred
hot particles. If this were so, these particles could have
been partly responsible for the observed cancers.
The preliminary studies by Lafuma (1974) do not appear tc
be published and we have no copy of the seminar given in France.
Indications are, however, that it is not different from the
experiments discussed above. .
Again we offer the above and this entire critique as
refutation of the conclusion reached in the last paragraph of
this section.
Pages 25-29. "IV. Human Experience."
This chapter of the BRW Report discusses the exposure of
humans to Pu. The major thrust of the chapter involves workers
from the Manhattan Project and from the Rocky Flats plutonium
facility in Colorado. We discuss these in the Tamplin-Cochran
Report but the authors of the BRW Report overlooked or ignored the
salient features of our discussion.
-------
- 33 -
084
Pages 25-26. The Manhattan workers are discussed on these
pages. On pages 38 to 40 of the Tamplin-Cochran Report, based
upon information from Hempelmann, et al., (1973a, 1973b) we cal-
culated that the exposures of these workers did not involve hot
particles. The authors of the BRW Report inexplicably ignored
• : this discussion and made the unjustifiable assumption that the
particles here corresponded to those associated with a fire at the
Rocky Flats plutonium facility. As a consequence, the discussion
of expected cancers on page 26 is without merit.
Pages 26-27. The discussion of chromosome aberrations
has no relevance to the hot particle problem.
Pages 27-28. The exposure of employees of the Rocky
Flats plutonium facility in October 1965 is discussed here. In
the Tamplin-Cochran Report we pointed out that the induction period
in man for hot particle carcinogenesis is unknown. In the beagle
dog experiment (Park and Bair, 1972) it was 11 years before the
dog with the lowest burden developed lung aancer. Thus, although
no cancers have developed in the Rocky Flats workers at this time
(9 years post exposure) the possibility exists that a number
of cancers will appear in the next 10-15 years.
Page 28. The lesion excised by Lushbaugh and Langham (1962)
is discussed here. To the extent that a lesion with changes
similar "to known precancerous epidermal cytologic changes,"
that raise the question of its fate without surgical intervention
differs from a precancerous lesion, we were remiss in the
Tamplin-Cochran Report.
-------
- 34 -
085
Page 29. As we indicated in the Tamplin-Cochran Report,
the Pu in fallout did not occur in hot particles and hence,
fallout Pu is irrelevant to the issue.
Pages 31-35. "V. Theoretical Consideration."
At the outset, it is important to .note-that one hypothesis
cannot be used to set aside another. Each hypothesis must
stand alone with respect to supporting experimental data.
Pages 31-33. "A. Dosimetry." This is general informa-
tion about which there is little controversy.
Pages 33-35. "3. Models for Dosimetry and Tumor Proba-
bility. " We agree with the concluding remarks of this section.
The models discussed here relate tumor probability to cellular .
radiation dose. Depending upon the assumption, they can give
a variety of tumor probabilities.
We would simply add that the lesion excised by Lushbaugh
and Langham (1962) coupled with the observations of similar
lesions induced in the lungs of rats and hamsters should be
sufficient to cause anyone to be skeptical of a tumor induction
model which indicates a low tumor probability for a hot particle.
Pages 35-39. "B. Radiation Carcinogenesis Relative to
Spatial Distribution of Dose."
In the first paragraph of this section, the authors state
that-one should use experimental data, "meager as it is," rather
than models based upon other organ systems. They indicate
that this is "particularly true" when rat skin data are used
to.infer human lung effects. It is doubtful whether anyone would
disagree with this. However, in the case of hot particles,
-------
- 35 -
086
the experimental data are not only meager, they are very dis-
quieting. Since this is a public health matter of importance
and not just an academic exercise, prudence dictates that
exposure standards should be based upon supportable and conser-
vative hypotheses.
Pages 35-36. The next few paragraphs discuss the concept
of "wasted" radiation as it relates to the hypothesis of linear
dose-effect response. When uniform irradiation is employed
cancer induction is generally shown to be directly propor-
tional to the dose from low doses up to a few hundred rad.
. The linear hypothesis relates these observations to cellular
effects that result from single-track ionizing events. But even
with uniform irradiation as one proceeds to higher dosages
the response curve changes; for example, the curve steepens
or the effects plateau and often decline. Obviously this indi-
cates that other phenomena are becoming dominant. The hot par-
ticle hypothesis relates to such a different phenomenon (an
injury-mediated mechanism of carcinogenesis). As such, it is
• not intended to be consistent with the linear hypothesis.
The mechanism of radiation carcinogenesis is not under-
stood even in the range of the linear hypothesis. This is
evident in the next several paragraphs of this section of
the BRW Report. Actually much of the discussion here is sup-
portive of an injury-mediated mechanism wherein the altered
tissue architecture creates a milieu highly favorable to tumor
development; for example, the quote of Mayneord (1968).
-------
087
Page 36. The discussion of contact inhibition as it
related to normal or "transformed" cells is again consistent
with the hot particle hypothesis. It is the disturbed tissue
architecture that can disrupt the normal contact inhibition.
As we mentioned earlier in this critique, the induction of
cancer by mylar film and millipore filters in the experiments
*5 "5
of Brues, et al., supports such a mechanism. J
The paragraph that begins, "Thus, both acute and late..."
is purely speculative and is no more supported by the previous
discussion than is the hot particle hypothesis.
Pages 36-38. The following ten paragraphs in this section
are .actually a discussion of an injury-mediated mechanism of
carcinogenesis.
Page 38. This is followed by the paragraph,
At present there is no compelling reason to believe
that the critical structure or volume required for
radiation-induced promotion of cancer .arising from
cancer-potential cells of hair follicles is limited
to the hair follicle. There is also no cogent evi-
dence that the lung has analagous discrete susceptible
architectural units with critical tissue volume as
small as the sphere of alpha particle range from
an isolated "hot particle."
We would propose that there is also no compelling reason for
not believing it and that prudent public health practice dic-
tates that such a critical structure should be assumed in
establishing exposure standards for hot particles.
Pages 38-39. The next two paragraphs are speculative
and are followed by the paragraph:
23/ Brues, A., et al., op. cit.
-------
088 " 37 "
Considering the amount of human data available for
carcinogenic risk estimates, and the variability
and uncertainty concerning dosimetric factors (e.g.,
relevant doses, differences in spatial and temporal
dose distribution, etc.)/ it has thus far been re-
garded as necessary to select single values of
quantities that characterize the exposure of an
organ or that organ in a group of individuals.
Mean accumulated tissue dose is the only criterion
that can be used practically at present until
adequate knowledge of more relevant criteria
becomes available. Furthermore, when the energy
is deposited non-uniformly and its influence in
the exposed organ or a group of individuals is
not.known, the non-uniformity cannot be dealt
. with until more adequate data are available. The
linear (proportional) hypothesis is the only one
that normally permits the use of mean dose as the
significant dose factor for conditions of non-
uniform exposure and exposure rate in an organ
or' among individuals, the purposes of estimating
risk or setting dose limits in the absence of
adequate data on distribution of dose and dose
rates.
While this paragraph may have been offered as an explanation
for, or even as an excuse for, the present radiation exposure
standards, we fail to see how it justifies the standards in
the future. So far as hot particles are concerned, we have
submitted a supportable hypothesis to supplant the linear
hypothesis in establishing hot particle exposure standards.
The standards are a practical problem of the moment and should
be established on the basis of conservative and supportable
hypothesis today. It is irresponsible to leave the health of
workers and the public in jeopardy while awaiting more definitive
data.
The remaining paragraph is a speculative attempt to set
aside the hot particle hypothesis. In this respect, it is
interesting to note that this section of the report failed to
-------
- 38 -
089
recant the observations of Lushbaugh.and Langham (1962) wherein
a 'precancerous' lesion was induced in the palm of a mechanic
by a single plutonium hot particle. Nor did it discuss the
observations of Richmond, ejt al. , (1970) , Richmond and Voelz
(1972, 1973) or Richmond and Sullivan (1974) that similar
lesions were induced in the lungs of rats and hamsters by plu-
tonium hot particles. These are observations, not speculation,
and they support the hot particle hypothesis.
Pages 39-40. "C. Assessment of Experimental Animal Data."
This section begins with a discussion of a probit trans-
formation of experimental data on animals relating lung cancer
and radiation dosage to which the authors correctly ascribe no
statistical validity. Nevertheless, so far as the Pu or other
alpha data are concerned there Is little that is related to hot
particles and that which is, such as the beagle data (Park and
Bair, 1972), represents a saturated response. The Pu-238
experiments of Sanders (1972) also demonstrate a saturated
response at a level of 40 rad or 400 rem. Moreover,- Sanders
indicates that Pu was soluble in his experiment.
In the second paragraph they indicate that these plots
demonstrate a RBE of about 10 for alpha radiation in accord
with radiobiological experience. In the third paragraph, they
make an assumption concerning the non-uniform distribution of
the alpha irradiation and transpose the alpha curve in accord
with this assumption. Considering the nature of the alpha
experiments (their particle size, solubility, and saturation
effects) there is no justification for this assumption and
transformation. For example, Sanders states that his irradiation
was uniform.
-------
090 _ 39 _
We see little merit to this entire discussion and the
conclusions in the 5th and 6th paragraphs that result from it
are entirely unjustified.
Page 41. The final 5 paragraphs in the BRW Report discuss
a number of animal experiments that supposedly are contrary
to the hot particle hypothesis. The first involves the results
of Laskin, e_t al. , (1963) wherein Ru-106 pellets were implanted
in the bronchi of rats. The results indicated a tumor incidence
\
of 7.3% in animals exposed to a few thousand rads with the
incidence rising to 66% in those exposed to 10 rads. This
dose was calculated as that delivered to the basal layer of
the epithelium. One can readily show that this experiment
is consistent with the hot particle hypothesis.
The pellets were some 5000 p in length. They would there-
fore be expected to produce lesions larger than the 200 to
300 u lesions observed around hot particles. The result
demonstrated a 7% tumor incidence in the 103 rad range with one
tumor occurring in an animal exposed to 1400 rad. Thus, the
cancer risk associated with this much larger lesion at a dose
of some 1000 rad was roughly 1/10 or some 200 times greater
than that which we assigned to the smaller lesion around a hot
particle. This is entirely consistent with the hot particle
hypothesis including the 1000 rem/year activity limit. More-
over, the incidence rose to 66% at higher dosage. The data
of Richmond and Voelz (1972, 1973) and Richmond and Sullivan
'(1974) with Pu microspheres demonstrated that these lesions
-------
- 4o - 091
develop more rapidly as the particle activity is increased.
This suggests that if a sufficient induction period were allowed,
the incidence for the large pellet-produced lesion could be
unity. Again, this is consistent with the hot particle hypo-
thesis.
The remaining experiments discussed here involved Co-60
implants in a variety of animal species (Warren and Gates,
1968) and whole body x-irradiation of rats (Koletsky and
Gustafson, 1955, and Castaneva, et al. , 1968). Concerning
these experiments, the BRW Report authors state:
Data in figure V-4 for five species of animals
given 6^Co wire implanted in their lungs show lung
tumor incidences ranging from about 8 to 40%, in
all but one instance, for total doses of 10^-10^
.rad to either the entire lung or to the esophagus.
It is of interest that the entire lung is irradiated,
including any and all possible "critical architectural
units," at high dose rates, yet the tumor incidence
is not unity. Also of interest is the similar response
shown for the several species used with the possible
exception of the rat lung, the highest cancer incidence
point. The observation of tumor incidences well
below unity is true also for the whole-body exposures
to X-irradiation in which the entire lungs and body
of rats received doses near 10^ rad.
All of these experiments involved whole body exposure at
fairly high dosage. These exposures elicited a generalized
carcinogenic response and a significant life shortening effect.
Since lung cancer was competing with this overall response, it
is incredible that the authors of the BRW Report expected the
lung cancer incidence could have reached 100%.
In the Co-60 experiments, the life shortening effect
amounted to 80% in all strains and species except for rabbits
-------
092
which died earlier. At the same time, 33% of the animals
developed cancer in one or more of the three tissues studied:
lung, bone, and esophagus. If all tissues had been studied
the cancer incidence would have been higher. Nevertheless,
in the rat, lung cancer had a competitive edge and reached an
incidence of 75%. In the X-ray study of Koletsky and Gustafson
(1955) the life shortening approached 50% and the incidence of
malignant neoplasms was 35% at a whole body dosage of 660 rad.
In the control group the incidence was 8%. The Castaneva,
et al., (1968) results showed a malignant tumor incidence of
100% and a 20% life shortening even at a dosage of 430 rad.
The control rats in these experiments had a 30% malignant tumor
incidence. These experiments are typical of many such experi-
ments and show the overall response to whole body radiation.
The relationship to the hot particle problem, if any, is
obscure and remote. There is no a_ priori reason to believe
that the same carcinogenic mechanism is involved.
V. Summary and Conclusion
The Tamplin-Cochran Report presented a hot particle hypothe-
sis based on an injury-mediated mechanism of carcinogenic response.
In order to assist in setting radiation protection standards we
proposed quantative values for 1) the minimum activity defining
a hot particle and 2) the carcinogenic risk per hot particle.
The ".hot particle hypothesis" is relatively simple. With respect
to alpha-emitting particles in the lung, it is:
-------
- 42 - 093
If a particle deposited in the deep respiratory tissue
is of such activity as to expose the surrounding
lung tissue to a dose of a_t least 1000 rem in 1 year,
this particle represents a unique carcinogenic risk.
The biological data suggest that such a particle may
have a cancer risk equal to 1/2000.
The BRW Report has been offered as a refutation of the
hot particle hypothesis quantitatively presented in the Tamplin-
Cochran Report. The BRW Report cites numerous experimental
studies, most of which are not relevant to the hot particle
issue. Those which are relevant we have shown to be consistant
with our hot particle hypothesis. Thus, the BRW Report is
not in any way a refutation of the hot particle hypothesis.
While it must be recognized that there are uncertainties
with respect to the quantitative values we have chosen, until those
uncertainties can be resolved by appropriate experimental data,
it is incumbant upon the AEC and EPA to adopt radiation pro-
tection standards comparable to those in the Tamplin-Cochran
Report. Furthermore, we submit that these more restrictive
standards should be quickly promulgated because it is irrespon-
sible to leave the health of the public and workers in jeopardy
while awaiting more definitive data.
-------
094
VI. BIBLIOGRAPHY
Albert, R. E., (19G2), "The Tumorigenic Action of
Beta Radiation on the Rat Skin," Progress Report
TID-15118.
Albert, R. E., Burns, F. J., and Bennett, P., (1972),
"Radiation-Induced Hair-Follicle Damage and Tumor
Formation in Mouse and Rat Skin," J. Nat. Cancer
Inst, !,!>: 1131.
Albert, R. E., Burns, F. J., and Heimbach, R. D.,
(1967a), "The Effect of Penetration Depth of Electron
Radiation on Skin Tumor Formation in the Rat," Ra-
diat. Res. SO: 515.
Albert, R. E., Burns, F. J., and Heimbach, R. D.,
(19C7b), "Skin Damage and Tumor Formation from
Grid and Sieve Patterns of Electron and Beta Radia-
tion in the Rat," Radiat. Res. SO: 525.
Albert, R. E., Burrs, F. J., and Heimbach, R. D.,
(19fi7c), "The Association Between Chronic Radiation
Damage of the Hair Follicles and Tumor Formation in
the Rat," Radiat. Res. 30: 590.
Albert, R. E., Newman, W., and Altshuler, B.,
(19G1), "The Dose-Response Relationships of Beta-
Ray-Induced Skin Tumors in the Rat," Radiat. Res.
15: 410.
Albert, R. E., Phillips, M. E., Bennett, P., Burns, F.,
and Heimbach, R., (19d9), "The Morphology and
Growth Characteristics of Radiation-Induced Epithelial
Skin Tumors in the Rat," Cancer Res 2.9; G58.
Archer, V. E. and Lundin, F. E., (1967), "Radiogenic
Lung Cancer in Man: Exposure—Effect Relationship,"
Ens-iron. Res. 1: 370.
Bair, W. J., (I960), "Radioisotope Toxicity: from
Pulmonary Absorption," In: Radioisotopes in the Bio-
sphere (It. S. Caldecott and L. A. Snyder, eds.), 431,
])u!)l. by (he Center for Continuation Study, University
of Minnesota, Minneapolis.
Bair, W. J., (1974), "Toxicology of Plutonium," In:
Advances in Radiation Biology, Volume 4, (J. T. Lett,
H. Adler and M. Zelle, eds.), Academic Press.
Hair, \V. J., (in press), "Considerations in Assessing
the Potential Harm to Populations Kxposod to Low
Levels of Plutonium in Air," In: Seminar on Radiolog-
irnl Safety Evaluation of Population Doses and Appli-
cation of Radiological Safety Standards to Man and
the Environment (L. A. Self, ed.), IAEA-SM-184/14,
Portoroz. Yugoslavia.
Rair, W. J., Hallou, J. E., Park, J. F., and Sanders,
C. L., (1973), "Plutonium in Soft Tissues with Empha-
sis on the Respiratory Tract," In: Handbook of Exper-
imental Pharmacology (II. C. Hodge, J. N. Stannard
and J. B. Hursh, eds.), Springer-Verlag, Berlin.
Bair, W. J. and McClanahan, B. J., (1961), "Pluto-
nium Inhalation Studies II. Excretion and Transloca-
tion of Inhaled -'"'PuOz Dust," Arch. Environ. Health
2: 648.
Bair, W. .J., Wiggins, A. D., and Temple, L. A.,
(1962), "The Effect of Inhaled Pu«»02 °n the Life
Span of Mice," Health Phys. 8: 659.
Bair, W. J. and Willavd, D. H., (]961), "Plutonium
Inhalation Studies III. Effect of Particle Size and
Total Dose on Retention and Translocation," HW-
68645.
Ballou, J. E. and Park, J. F., (1972), "Disposition of
Ingested, Injected and Inhaled 5:lllPu Citrate and
=i»Pu Nitrate," Pacific Northwest Laboratory Annual
Report for 1971 to the USAEC, Division of Biology
and Medicine, BNWL-1650, Vol. 1, part 1: 146.
Bennett, B. G., (1974), "Fallout 23"Pu Dose to Man,"
In: Fallout Program Quarterly Summary Report,
Health and Safety Laboratory, U. S. Atomic Energy
Commission Report HASL-278.
Brooks, A. L., Mewhinney, J. A., and McClellan, R.
0., (1972), "The In Vivo Cytogenetic Effects of "2Cf
in Liver and Bone Marrow of the Chinese Hamster,"
Health Phys. 22; 701.
Brooks, A. L., Retherford, J. C., and McClellan, R.
O., (1974), "The Effect of "9Pu02 Particle Number
and Size on the Frequency and Distribution of Chro-
mosome Aberrations in the Liver of the Chinese Ham-
ster," Radiat. Res. (in press).
Brandon, W. F., Bistline, R. W., Bloom, A. D., and
Archer, P. G., (1973), "Preliminary Findings: Chromo-
somes of Plutonium Workers," Mutat. Res. 21: 211
(abstract).
Buldakov, L. A., Lyubchansky, E. R., Moskalev, Y.
I., and Nifatov, A. P., (1969), In "Problemy Toksikolo-
gii Plutoniya," Atom Publications, Moscow (translated
as "Problems of Plutonium Toxicology," U. S. Atomic
Energy Commission LF-lr-<11, 1970).
Fiulilakov, L. A. and Lyubchansky, E. R., (J970),
"Experimental Basis for Maximum Allowable Load
(MAL) and Pu-239 in the Human Organism, and
Maximum Allowable Concentration (MAC) of Pu-239
in Air at Work Locations," Original source unknown,
Report ANL-trans-8li<1, Argonne National Laboratory,
Argonne, Illinois, (Translated from a Russian Report).
Burk, R. R., (1906), "Growth Inhibitor of Hamster
Fibroblast Cells," Nature 212: 1261.
Burnet, Sir M. B., (1964), "Immunological Factors
in the Process of Carcinogencsis," Brit. Med. Bull. 20:
154.
43
-------
Burns, F. J., Albert. R. E., Bennett, P., and Sinclair,
I. P., (1!)72), "Tumor Incidence in Rat Skin After
Proton Irradiation in a Sieve Pattern," Radial. Res.
.1": 181.
Burns. F. '.).. Albert, R. E., and Heimbach, R. D.,
(l!Xi8), "The RBE for Skin Tumors and Hair Follicle
Damage in the Rat Following irradiation with Alpha
1'artirli's and Electrons," Radial. Res. .Hi: 225.
Burns, F. J., Albert, R. E., Sinclair, I. P. and Ben-
nett. P., (I!i7.%), "The Effect of Fractionation on
Tumor Induction and Hair Follicle Damage in Rat
Skin," Radiat. Res. SJ: 235.
Burn.-, F. J.. Sinclair, I. P.. and Albert, R. E.,
(1973a), "The Oncogenic Response of Anagen Phase
Rat Skin to Electron Radiation of Various Penetra-
tions," Pror. Amer. Ass. Cancer Res. 11: 88 (abstract).
Burrows. H. and Horning, E., (1953), "Oestrogens
and N'eoplasia," Blackwell, Oxford.
Campbell, E. E., Milligan. M. F., Moss, W. D.,
Schulte, H. F., and Mclnroy, J. F., (1973), "Plutonium
in Autopsy Tissue," Los Alamos Scientific Laboratory
Report LA-4875.
Carrnno, A. V. and Heddle, J. A., (1974), "The
Fate of Chromosome Aberrations," J. Theor. Biol. (in
press).
Casarett. G. W., (19(55), "Experimental Radiation
C'arcinofii'iH'sis," Progr. Exp. Tumor Res. /•.• 49.
Casarett, G. W., (1973a), "Pathogenesis of Radionu-
clide-Induced Tumors," In: Radionuclide Carcinogene-
sis (C. L. Sanders, 11. H. Busch, J. E. Ballon, and
D. I). Mahlum, eds.), COXF-720505: 1, AEC Sympo-
sium Series 29, I". S. Atomic Energy Commission, Office
of Information Services, Springfield, Virginia.
Casaretl. G. W., (1973b), "Possible Effects of Rela-
tively Low Levels of Radiation," Current Problems in
Radiology j: 1.
Casarett, L. J. and Milley, P. S., (1964), "Alveolar
Reactivity Following Inhalation of Particles," Health
Phys. in: KHir..
Castanera, T. J., Jones, D. C., Kimeldorf, D. J. and
Rosen, V. J., (1968), "The Influence of Whole-Body ;
Exposure to X-Rays or Neutrons on the Life-Span
Distribution of Tumors Among Male Rats," Cancer
Res. .',«: 170.
Cember. H., (1063), "Further Studies on Lung Can-
cers from '"CeF.:." Health Phys. !>: ~>3!>.
Cember, H., (1964a). "Radiogenic Lung Cancer," In:
Progr. Kxp. Tumor Res. Vol. 4 (F. Hamburger, ed.),
2-M, Hafner Publishing Co., Inc.. New York.
Cember, H., (1964b), "Empirical Establishment of
Cancer-Associated Dose to the Lung from "4Ce,"
Health Phys. lit; 1177.
Cember, H., Hatch, R. F., Watson, J. A., and Grucci,
T. B., (1955), "Pulmonary Effects from Radioactive
Barium Sulfate Dust," AMA Arch. Indust. Health U:
628.
Cember, H. and Stemmer, K.. (IDfi'l), "Lung Cancer
from Radioactive Cerium Chloride," Health Phys. ID:
43.
Cember, H. and Watson. J. A.. (19.~>8a), "Carcino-
genic Effects of ""Sr Beads Implanted in the Lungs of
Rats," American Ind. Hyg. J. Hi: o'i.
Comber, H. and Watson, J. A., (19u8b), "Broncho-
095
genie Carcinoma from Radioactive Barium Sulfate,
AMA Arch. Ind. Health 17: 230.
Cember, H., Watson, J. A., and Spritzer, A. A.,
(19.r)9), "Bronchogenic Carcinoma from Radioactive
Cerium Fluoride," AMA Arch. Indust. Health 19: 14.
Clarke, W. J. and Bair, W. J., (1964), "Plutonium
Inhalation Studies: VI. Pathologic Effects of Inhaled
Plutonium Particles in DORS," Health Phys. JO: 391.
Clarke, W. J., Park, J-. F., and Bair, W. J., (I960),
"Plutonium Particle-Induced Neoplasia of the Canine
Lung. II. Histopathology and Conclusions," 345, In:
Lung Tumours in Animals, (Lucio Severi, ed.), Uni-
versity of Perugia, Perugia, Italy.
Coleman. J. R. and Perez, L. J., Jr., (1969), "Con-
sideration of a Tumor Probability Function and Mi-
cro-Dosimelry for the Lower Pulmonary
Compartment," Nuclear Utility Services Report NUS-
fi.")4, Rockville, Maryland.
Pavies, C. N.,. (1961), "A Formalized Anatomy of
the Human Respiratory Tract," In: Inhaled Particles
and Vapours, (C. N. Davies, ed.), 82, Pergamon Press,
London.
Dean, P. X. and Langham, W. H., (19G9), "Tumori-
genicity of Small Highly Radioactive Particles,"
Health Phys. Id: 79.
Dolphin, G. W., (1971), "Biological Problems in the
Radiological Protection of Workers Exposed to "»Pu,"
Health Phys. -20: 549.
Erokhin, R. A., Koshurnikova, N. A., Lemberg, V.
K., Nifatov, A. P., and Puzyrev, A. A., (1971), In:
"Remote Aftereffects of Radiation Damage," (Y. I.
Moskalev, ed.), 315, Atomizdat, Moscow (Translated in
AEC-tr-7387, 344).
Ettinger, H. J., Elder, J. C., and Gonzales, M.,
(1973), "Performance of Multiple HEPA Filters
Against Plutonium Aerosols," Los Alamos Scientific
Laboratory Report LA-5349-PR.
Geesaman, D. P., (1968), "An Analysis of the Car-
cinogenic Risk from an Insoluble Alpha-Emitting Aero-
sol Deposited in Deep Respiratory Tissue," USAEC
Documents UCRL-50387 and UCRL-50387 Addendum.
Gillette, R., (1974), "Plutonium and the 'Hot Parti-
cle Problem1: Environmental Group Proposes a Dra-
conian Answer," Science ix.l: 834.
Grossman, B. N., Little, J. B:, and O'Toole, W. F.(
(1971), "Role of Carrier Particles in the Induction of
Bronchial Cancer in Hamsters by Polonium-210 Alpha
Radiation," Radial. Res. -!?.• 253 (abstract).
Harley, N. H. and Pasternack, B. S., (in press),
"Experimental Absorption Applied to Lung Dose from
Plutonium-^")),'1 Health Phys.
Mealy, J. W., (1974), "Contamination Limits for
Real and Porsonal Property," Los Alamos Scientific
Laboratory Report Xo. LA-5482-PR.
HeimliMch, R. It., Burns, F. J., and Albert, R. E.,
(If'fiiM, "An Evaluation by Alpha Particle Bragg Peak
Radiation of the Critical Depth in the Rat Skin for
Tumor Induction," Radial. Res. .,'fl.- 332.
Hempelmann, L. H., Langham, W. H., Richmond, C.
R., and Voelz, G. L., (1973a), "Manhattan Project Plu-
tonium Workers: A Twenty-Seven Year Follow-up
Study of Si-looted Cases," Health Phys. 2."i: 4fil; see also
Los Alamos Scientific Laboratory report LA-5148-MS
(1973).
44
-------
096
Hempelniunn, L. H., Richmond, C. R., and Voelx, G.
L., (1973b), "A Twenty-Seven Year Study of Selected
Los Alamos Plutonium Workers," Los Alamos Scien-
tific Laboratory report LA-E148-MS.
Howard, E. B., (1970), "The Morphology of Experi-
mental Lung Tumors in Beagle Dogs," In: Morphology
of Experimental Respiratory Carcinogenesis (P. Net-
tesheim, M. G. Hanna, Jr., and J. W. Deatherajre, Jr.,
eds.), CONF-700501: 147, AEC Symposium Series No.
21, U. S. Atomic Energy Commission, Office of Infor-
mation Services, Springfield, Va.
ICRU Report 19, (1971), "Radiation Quantities and
Units," International Commission on Radiation Units
and Measurements, Washington, D.C.
International Commission on Radiological Protection,
(1966), "Recommendations of the International Com-
mission on Radiological Protection (Adopted Septem-
ber 17, 1965)," ICKP Publication 9, Pergamon Press,
Oxford.
International Commission on Radiological Protection,
(19(19), "Radioscnsitivily and Spatial Distribution of
Dose, Reports Prepared by Two Task Groups of Com-
mittee 1 of the International Commission on Radiologi-
cal Protection," ICRP Publication 14, Pergamon Press,
Oxford.
Kochctkova, T. A. and Avrunina, G., (1957), "Veran-
derungen in den Lungen und in andereri Organen
bee intratrachealev Eim'uhrung einiger Radioisotope,"
Arch. Gewerbepathol. Gewerbehy. 1C: 24.
Kochetkova, T. A., Avrunina, G. A., and Sagaidak-
Chernyak, N. D., (1963), "Experimental Lung Cancer
Induced with Radioactive Compounds P:1-, Au1!" and
Fe19," Acta Unio. Intern. Contra Cancrum 19: 684.
(Cited in Morken, D. A., (1955), University of Roches-
ter Report UR-379).
Koletsky, S. and Gustafson, G. E., (1955), "Whole-
Body Radiation as Carcinogenic Agent," Cancer Res.
15: 100.
Koshurnikova, N. A.. Lemberg, V. K., and Lyub-
chansky, E. R., (1971), In: "Remote Aftereffects of
Radiation Damage," (Y. I. Moskalev, cd.), 305, Atom-
izdat, Moscow. (Translated in AEC-tr-7387, 334).
Koshurnikova, N. A., Lemberg, V. K., Nifatov, A.
P., and Puzyrev, A. A., (1968), "Pneumosclerosis in
Rat Following Intratracheal Introduction of Soluble
Pu-^'Compounds," Gig. Tr. Prof. Zabol. 11: 27.
Kurshakova, N. N. and Ivanov, A. E., (1962), "A
Model of Experimental Lung Cancer Caused by In-
tratrachcal Introduction of Radioactive Cerium," Bull.
Exp. Biol. Mml. /!.',: 7S7.
Lafuma, J., 70a), "Respiratory Carcinogenesis in Hamsters In-
duced by Polonium-210- Alpha Radiation and Benzo-
(ex ) Pyrene," In: Morphology of Experimental Respira-
tory Carcinogenesis, (P. Nettesheim, M. G. Hanna, Jr.,
and J. W. Deatherage, Jr., eds.), CONF-700501: 383,
AEC Symposium Series No. 21, U. S. Atomic Energy
Commission, Office of Information Services, Spring-
field, Va.
Little, J. B., Grossman, B. N., and O'Toole, W. F.,
(l!)70b), "Induction of Bronchial Cancer in Hamsters
by Polonium-210 Alpha Radiation," Radiat. Res. 1,3:
261 (abstract).
Little, J. B., Grossman, B. N., and O'Toole, W. F.,
(197S), "Factors Influencing the Induction of Lung
Cancer in Hamsters by Intratracheal Administration
of -''"Po," In: Radionuclide Carcinogenesis, (C. L.
Sanders, R. H. Busch, J. E. Ballou, and D. D. Mahlum,
eds.), CONF-720505: 119, AEC Symposium Series No.
29, U. S. Atomic Energy Commission, Office of Infor-
mation Services, Springfield, Va.
Lundin, F. E., Wagoner, J. K., and Archer, V. E.,
(1071). "Radon Daughter Exposure and Respiratory
Cancer Quantitative and Temporal Aspects," National
Institute for Occupational Safety and Health/National
Institute for Environmental Health Sciences, Joint
Monograph No. 1, Public Health Service, U. S. Dept.
of Health, Education and Welfare.
Lushbaujih, C. C., Cloutier, R. J., Humason, G., Lang-
ham, J., and Giizuk, S., (1967), "Histopatholgic Study
of Inlradornml Plutonium Metal Deposits: Their Con-
jectured Fate," Ann. N.Y. Acad. Sri. 1l,r,: 7!)1.
l.uslil.autrh. ('. '.'. and Langham, J., (1H02), "A Der-
mal Lesion from Implanted Plutonium," Arch. Derma-
tol. XH: 461.
Mann, J. R. and Kirchner, R. A., (1967), "Evalua-
tion of Lung Burden Following Acute Inhalation
Exposure to Highly Insoluble PuO2," Health Phys. 13:
877.
Marshall, J. H. and Finkel, M. P., (1959), "Auto-
radiographic Dosimetry of Mouse Bones Containing
Ca'-V Sr"1, and Ra=-"," Argonne National Laboratory
Report ANL-6104: 48.
Marshall, J. H. and Finkel, M. P., (1960), "Autora-
dioirraphic Dosimetry of Mouse Bones Containing Ca45,
45
-------
Sr"0, and Ra"r', II. The Sensitive Region in the Induc-
tion of Osteogenic Sarcomas," Argonne National Labo-
ratory Report ANL-fil99: 44.
Mayneord, W. V., (1968), "Radiation Carcinogene-
sis," Brit. J. Radiol. 41: 241.
Mayneord, W. V. and Clarke, R. H., (1974), "A
Mathematical Investigation Into the Carcinogenic
Risks Associated with Particulate Sources of Activ-
ity," Central Electricity Generating Board,
RD/B/N2878, London, England.
McKay, L. R., Brooks, A. L., and McClcllan, R. O.,
(1972), "The Retention, Distribution, Dose and Cytoge-
netic Effects of -"Am Citrate in the Chinese Ham-
ster," Health Phys. 21: <>33.
McMurtrie, G. E. (Secretary), (1950), "Permissible
Doses Conference held at Chalk River, Ontario (Sept.,
1949)," Report RH-10, May.
Mercer, T. T., (1967), "On the Role of Particle Size
in the Dissolution of Lung Burdens," Health Phys.
l.i: 1211.
Metivier, H., Nolibe, D., Masse, R., and Lafuma, J.,
(1972). "Cancers Provoquoes chez le Singe Babouin
(Papio papio) par Inhalation de PuO'j," C. R. Acad.
Sci (Paris), 275: 3009 (translated by Howath, A. A.,
LF-tr-80).
Morrow, P. E., Bates, D. V., Fish, B. R., Hatch, T.
F., and Mercer, T. T., (1966), "Deposition and Reten-
tion Models for Internal Dosimetry of the Human Res-
piratory Tract," Health Phys. 12: 173.
Morrow, P. E. and Casarett, L. J., (1061), "An Ex-
perimental Study of the Deposition and Retention of a
Plutonium-23!) Dioxide Aerosol," In: Inhaled Particles
and Vapors, (C. N. Davies, ed.), Pergamon Press,
London.
Moskalev, Y. I., (1972), "-:'"Pu: Problems of its
Biological Effect," Health Phys. 22: 723.
Moss, W. D., Hyatt, E. C., and Schulte, H. F.,
(19(U), "Particle Size Studies on Plutonium Aerosols,"
Health Phys. 5: 212.
NAS-NRC Subcommittee on Inhalation Hazards,
Committee on Pathologic Effects of Atomic Radiation,
(lilfiln), "Effects of Inhaled Radioactive Particles,"
Publication 848, U. S. National Academy of Sciences-
National Research Council, Washington, D.C.
NAS-NRC Subcommittee on Internal Emitters, Com-
mittee on Pathological Effects of Atomic Radiation,
(19(>lb), "Internal Emitters," Publication 883, U. S.
National Academy of Sciences-National Research
Council, Washington, D.C.
NAS-NRC Report of the Advisory Committee on the
Biological Effects of Ionizing Radiations, (11)72) "The
Effects on Populations of Exposure to Low Levels of
Ionizing Radiation." N'atimial Ae.-idemy "f Scienccs-
Nuli'inal 1'esearrh Council, Washington, D.C'.
National Council on Radiation Protection and Meas-
urements, (1971), "Basic Radiation Protection Cri-
teria," NCUP Report No. 39, Wiisbingl.ni, D.C.
Nelson, I. C., Held, K. R., Fuqua, P. A., and Ma-
hony, T. D., (1972), "Plutonium in Autopsy Tissue
Samples," Health Phys. 22: 925.
N'orcross, J. A, and Newton, C. E.. Jr., (1972), "U.S.
Transuranium Registry: A Progress Report," Health
Phys.' 22, 887.
Park, J. F. and Bair, W. J., (1072), Personal Com-
munication (referenced in Bair, W. J., 1974).
097
Park, J. F. and Bair, W. J., (197-1), Personal Commu-
nication.
Park, J. F., Bair, W. J., and Busch, R. H., (1972),
"Progress in Beagle Dog Studies with Transuranium
Elements at Battelle-Northwest," Health Phys. 22: 803.
Park, J. F., Catt, D. L., Dagle, G. E., Hackett, P.
L., Olson, R. J., Powers, G. J., and Ragan, H. A.,
(1974), "Late Effects of Inhaled ""PuOz in Dogs," Pa-
cific Northwest Laboratory Annual Report for 1973 to
the USAEC Division of Biomedical and Environmental
Research, BNWL-1850, Part I.
Passonneau, J. V., Brues, A. M., Hamilton, K. A.,
and Kisieleski, W. E., (1952), "Carcinogenic Effects of
Diffuse and Point Source Beta Irradiation on Rat
Skin: Final Summary," USAEC Document ANL-4932:
31.
Raahe, 0. G., In Preparation.
Rashevsky, N., (1948), "Outline of a Mathematical
Approach to the Cancer Problem," In: Mathematical
Biophysics, University of Chicago Press, Chicago.
Richmond, C. R., Holland, L. M., Drake, G. A., and
Wilson, J. S., (1974), "Biological Response to Small
Discrete Highly Radioactive Sources, III. Effects of
Surgically Implanted ^"PuO, and "9Pu33-PR.
Richmond, C. R. and Voelz, G. L., (eds.), (1972),
Annual Report of the Biological and Medical Research
Group (H-1) to the USAKC, Division of Biology and
Medicine, Los Alamos Scientific Laboratory Report
LA-4923-PR.
Richmond, C. R. and Voelz, G. L., (eds.), (1973),
Annual Report of the Biological and Medical Research
Group (H-4) of the LASL Health Division for 1972 to
the USAEC, Division of Biomedical and Environmental
Research, Los Alamos Scientific Laboratory Report
LA-.r,227-PR.
Rnssi, H. H., (19<>7), "Energy Distribution in the
Absorption of Radiation," Adv. in Biol. and Med. Res.
// / 27, Academic Press, New York.
Sanders, C. L., (1%9), "The Distribution of Inhaled
PUitonium-2.'i!> Dioxide Particles Within Pulmonary
Macrophages," Arch. Environ. Health IX: 904.
Sanders, C. L., (1072), "Deposition Patterns and the
Toxicity of Transuranium Elements in Lung," Health
Phys. 22: <>07.
Sanders, C. L., (1973), "Carcinogenicity of Inhaled
Plutonium-238 in the Rat," Radiat. Res. Sfi: 540.
Sanders, C. L., (1974),'"Clearance of PuOj from Me-
diastinal Lymph Nodes," Pacific Northwest Laboratory
Annual Report for 1973 to the USAEC, Division of
Rinmedical and Environmental Research, BNWL-1850,
Part I.
46
-------
098
Sanders, C. L., (in press), "Effects of PuO^ Particles
Deposited in the Lung Following Intraperitoneal Injec-
tion," Health Phys.
Sanders. C. I., and Adee, R. R., (19K8), "Phagocyto-
sis of Inhaled Plutonium Oxide—-:'"Pu Particles by
Pulmonary Macropliagcs," Science ir,2: 918.
Sanders. C. L. and Adee, R. R., (1970). "Ultrastruc-
tural Localization of Inhaled -wPuO; Particles in Al-
veolar Epithelium and Macrophages," Health Phys.
JV.-293.
Sanders. C. I.., Adee. R. R., and Jackson, T. A.,
(1971 i, 'Tine Structure of Alveolar Areas in the Lung
Following Inhalation of =""PuO= Particles," Arch. En-
viron. Health 22: 525.
Sanders. C. L. and Dionne, P. X.. (1970), "Distribu-
tion of Alpha Energy in Alveoli Following Deposition
of -•••'PuO; Particles." Pacific Northwest Laboratory-
Annual Report for I!)fi8 to the USAEC, Division of
Biology and Medicine, BXWI.-1050. Part 1: 3.10.
Sanders. C. L. and Park. J. F.. (1972), "Pulmonary
Distribution of Alpha Dose from -1'-PuO: and Induc-
tion of Neoplasia in Rats and Dogs," In: Inhaled
Particles. (C. X. Davies. ed.>. Vol. Ill: 489, Pergamon
Press. London.
Sanders. C. L.. Thompson. R. C.. and Bair, W. J.,
(1970). "Lung Cancer: Dose Response Studies with
Radionuclides," In: Inhalation Carcinogenesis. (M. G.
Hanna. Jr.. P. Xettesheim. and J. R. Gilbert, eds.),
CONF-691001: 285. AEC Symposium, Series Xo. 18. U.
S. Atomic Energy Commission, Office of Information
Sei-vices. Springfield. Va.
Schubert, J. J., Fried, F., Rosenthal. M. W., and
Lindenbaum, A.. (1901), "Tissue Distribution of Mon-
omeric and Polymeric Plutonium as Modified by a Che-
lating Agent." Radial. Res. 15: 220.
Shorter, U. G.. <197Hi. "Ceil Kinetics of Respiratory
Tissues. Both Xormal and Stimulated." In: Morphol-
ogy of Experimental Respiratory Carc'inogonesis, (P.
Xette.-heim. M. G. Hanna, Jr., and J. \V. Deatherage.
Jr.. eds.), CONF-7f»i501: 45. AEC Symposium Se-
ries No. 21. U. S. Atomic 'Energy Commission, Office
of Information Services, Springfield, Va.
Sivak, A. and Van 1'uuren. B. L.. (1970), "A Cell
Culture System for the Assessment of Tumor-Promot-
ing Activity," J. Nat. Cancer Inst. 4i: 1091.
Stoker, M., (1964), "Regulation of Growth and Orien-
tation in Hamster Cells Transformed by Polyoma
Virus," Virology 2j : 105.
Stoker. M., (19(17), "Contact and Short-Range Inter-
actions Affecting Growth of Animal Cells in Culture,"
Current Topics in Developmental Biology, (A. A. Mos-
cona and A. Mouroy, eds.), Vol. II: 108, Academic
Press, New YorfT.
Tamplin. A. R. and Cochran, T. B., (1974), "Radia-
tion Standards for Hot Particles: A Report on the In-
adequacy of Existing Radiation Protection Standards
Rflated to Internal Exposure of Man to Insoluble Par-
ticles of Plutonium and Other Alpha-Emitting Hot
Particles." Natural Resources Defense Council report,
Washington, D. C.
Tempi", L. A., Marks. S., and Bair, \V. J., (I960),
"Tumors in Mice After Pulmonary Deposition of Radio-
active Particles." Int. J. Radial. Biol. 2: 143.
Temple, L. A., Willard, D. H., Marks, S., and Bair,
\V. J.. (I!i59). "Induction of Lung Tumors by Radioac-
tive particles." Nature 1S-1: 408.
Thomas, J. M. and Bair. W. J., (submitted for pub-
lication), "An Analysis of Experimental Data on Car-
cinogenic Effects of Inhaled Radiomiclides."
Thomas. R. L., Scott, J. K., and Chiffelle, T. L.,
(1972). "Metabolism and Toxicity of Inhaled 1MCe in
Rats." Radial. Res. J,0: 589.
Wager, R. W.. Dockum, X. L., Temple, L. A., and
Willnrd. D. H.. (1956), Biology Research Annual Report
for l:i55. HW-115HO, Hanford Atomic Products Opera-
tion, Richland. Washington.
Warren, S. and Gates, O.. (1968). "Cancers Induced
in Different Species by Continuous Gamma Radiation,"
Arch. Environ. Health 17: 697.
Walters, R. L. and Lebel, J. I.., (1972). "Progress
in th<> Beagle Studies at Colorado State University,"
Health Phys. ->;>: 811.
Weibd. E. R., (19G3), "Morphometry of the Human
Lung," Springer-Verlag, Berlin.
Zalmanzon, Y. E. and Chutkin, O. A., (1971), "Radia-
tion Absorbed Dose in the Lungs from Radioactive
Aerosols," translated from the Russian by The Ralph
McElroy Co.. Custom Division. 2102 Rio Grande Street,
Austin, Texas 78705.
GPO C82-C8 4
47
-------
-------
TABLE OF CONTENTS
101
I Introduction 1
II Plutonium Use and Public Health 3
III Existing Standards for Plutonium Exposure 6
IV Calculating the Dose Due to Insoluble Alpha-Emitters . . n
A The Dose Equivalent 11
B Modifying Factors 13
C The Hot Particle Problem 18
V Biological Data Related to the Cancer Risk from
Insoluble Plutonium Exposure 21
A The Geesaman Hypothesis 22
B Related Human Experience 26
C Related Lung Experiments 29
VI Critical Particle Activity 32
A Exposure at Rocky Flats 34
B Manhattan Project Workers 38
C Weapons Test Fallout 41
VII Exposure Standards for Hot Particles 41
A Occupational Exposure 42
B Exposure of the General Public 44
C Exposure from Accidental Releases 46
D Surface Contamination 48
E As Low as Practicable Hearings 50
VIII Summary of Recommendations 51
Appendix A Radiation Standards Setting Organizations and
Their Roles
Appendix B Statement Submitted to Attorneys for Mr. Edward Gleason
Glossary
-------
- 7 -
irradiated by internal sources; that is, by radionuclides
incorporated in body tissues. These radionuclides gain
entrance into the body through inhalation or through con-
taminated food or water. Once inside they behave like their
non-radioactive counterparts. Radioactive iodine, for example,
accumulates in the thyroid gland in the same fashion as
stable iodine, and radioactive strontium or calcium accumulate
in the bone similar to their naturally occurring non-radio-
active counterparts. The radioactive iodine will thus deliver
a dosage to the thyroid gland that is many times larger than
that to the other organs or to the whole body, and the
radioactive strontium and calcium will mainly irradiate the
bone.
Because of the uneven distribution of radionuclides
in the body organs, radiation exposure standards have been
developed not just for the whole body, but also for individual
organs. In this report we will be referring to the maximum
permissible whole body and lung doses.
Largely as a matter of convenience, secondary or derived
radiation standards have been developed. These secondary
standards, which limit radionuclide concentrations or organ
burdens, are often more easily employed than the primary dose
standards. We shall examine two secondary standards in this
109
-------
110
- 8 -
report; the maximum permissible lung burden (MPLB) and the
maximum permissible concentration in air (MPCa). The MPLB
is the total amount of a given radionuclide in the lung of
an average size man that will result in the lung being
irradiated at the maximum permissible lung dose (MPLD).
The MPCa is the concentration in air that will result in
an average adult male obtaining a MPLB and hence a MPLD by
breathing the air.
It is important to recognize that the MPLD is the
primary standard; it applies to all radionuclides and
radiation sources. The MPLB and the MPCa are derived standards
and are specific for a radionuclide. These derived standards
are related to the biological properties of a radionuclide
and to the form of radiation it emits.
Table I lists the existing exposure standards for em-
ployees of the nuclear industry that apply to Pu-239 in insoluble
form. The MPLD of 15 rem/yr is included in the recommendations
of the International Commission on Radiological Protection
g
(ICRP), the National Council on Radiation Protection and
Measurements (NCRP)9, and the Federal Radiation Council
8/ ICRP Publication 9, Recommendations of the International
Commission on Radiological Protection (Adopted September 17," 1966)
Pergamon Press, New York, 1966, p. 14.
9_/ NCRP Report No. 39, Basic Radiation Protection Criteria,
NCRP Publications, Washington, D. C., Jan. 15, 1971, p. 106.
-------
- 9 -
(FRC)10. The MPCa is included in the ICRP recommendations
and is also an AEC radiation standard . Of the standards
in Table I only the MPCa is designated in the AEC regulations.
However, this MPCa corresponds to that tabulated in ICRP
Publication 213 which is derived on the basis of the MPLD
listed in Table I. The MPLE is also derived on the basis of
the MPLD14. The MPLB is not. included in either the recommenda-
tions of ICRP, NCRP, the guidelines of FRC, or the AEC
regulations. In summary, in Table I the MPCa (designated
in AEC regulations) is consistant with the MPLD and MPLB. In
Table I the MPLD applies to all forms of ionizing radiation.
The MPLB and MPCa apply specifically to Pu-239 in insoluble
form15.
Ill
lO/ FRC Report No. 1, Op_. cit. , p. 38. The FRC has been
abolished and its duties transferred to EPA.
ll/ ICRP Publication 2, Report of Committee II on Permissible
Dose for Internal Radiation,. Pergamon Press, New York, 1960.
[Appeared in Health Physics, Vol. 3, Pergamon Press, June I960.]
12/ 10 CFR 20, Appendix B.
13/ ICRP Publication 2, Op. cit.
1_4/ Mann, J.R. and A.R. Kirchner , "Evaluation of Lung Burden
Fc:;.:,>'ing Acute Inhalation of Highly Insoluble Pu02," Health
Physics, Vol. 13, 1967, pp. 877-882.
15/ The MPLB could apply to most other alpha-emitting
rad-'.onuclidas with long half-lives, since the alpha particle
energies do not differ appreciably from the Pu-239 alpha
energy.
-------
112
- io -
TABLE I
Existing Occupational Exposure Guidelines
that Apply to Pu-239 in Insoluble Form*
MPLD (ICRP, NCRP, FRC) 15 rem/yr
MPLB 0.016 uCi
MPCa (ICRP, AEC) 4xlO~13- uCi/ml
*Note: See Glossary for definitions of symbols.
The exposure guidelines for Pu-239 that apply to non-
occupational exposure of the general public are tabulated in
Table II. Two guidelines are applied here. One is for the
limiting exposure to an individual and the other is for the
average exposure of a population sample. These two guidelines
differ by a factor of 3. The ICRP recommendations include only
the guidelines for individuals. The MPLD values within the
parentheses in Table II correspond to the latest recommendation
16
of the NCRP . These latest recommendations of the NCRP
have not, at this time, been incorporated into either the
AEC or EPA regulations.
16_/ NCRP Report No. 39, Op_. cit. , p. 95.
-------
113
- ii -
TABLE II
Existing Exposure Guidelines for Non-Occupational Exposure
that Apply to Pu-239 in Insoluble Form*
Individual Population Average
MPLD 1.5 (0.5) rem/yr 0.5 (0.17) rem/yr
(ICRP, NCRP, FRC)
MPLB 0.0016 (0.0005) uCi 0.0005 (0.00017) uCi
MPC 10"12 (3xlO-l3) uCi/ml 3xlO"13 (10"13) uCi/ml
(ICRP, AEC)
* The MPLD values in parentheses refer to the latest
recommendations of the NCRP. The MPLB and MPCa values in
parentheses correspond to the new NCRP dose recommendations.
IV. Calculating the Dose Due to Insoluble Alpha-Emitters
The purpose of this section is to examine the assumptions
in the radiation standards above that are inappropriate when
applied to insoluble alpha-emitting particulates such as
aerosols of Pu02- The assumptions are introduced through a
review of basic definitions of radiation dose and the factors
used to calculate the dose.
A. The Dose Equivalent
When an X-ray or the radiation emitted by a radionuclide
passes through tissue it transfers energy to the cells in
-------
114 - 12 -
these tissues. This energy produces chemical changes in
the molecule of the cells; for example, such a chemical
change could be a mutation in a gene. The radiation dose
is actually a measure of the energy transferred to or
absorbed by the tissue. The basic unit of dose is the
rad (one rad represents the absorption of 100 ergs of
energy per gram of material).
In addition to X-rays, radionuclides emit gamma rays
(high energy X-rays), beta particles (electrons), and alpha
particles (helium nuclei). In radiobiological experiments,
it was determined that, while these various types of radiation
produced the same biological effects, such as cancer, the
magnitude of the effect was not the same per rad. For
example, it was found that 100 rad of alpha radiation would
produce roughly 10 times as many cancers as 100 rad of
X-rays. Moreover, it was found that because of the special
way in which Pu-239 deposits in the bone, its alpha particles
were 5 times more effective in producing bone cancer than the
alpha particles from radium . To account, for these differences
in the magnitude of the observed effects at the same absorbed
dose in rad, the maximum permissible dose limits are given
in rem rather than rad.
The MPLD is given in rem in Tables I and II. The
17/ ICRP Publication 11, "A Review of the Radiosensitivity of
the Tissues in Bone," Pergamon Press, New York, N. Y., 1967, p. 21,
-------
115
- 13 -
18
rem is the unit of Dose Equivalent (DE) . The DE is obtained
by multiplying the absorbed dose in rad by modifying factors
to correct for these observed differences in the magnitude
of the effect. As a consequence, the magnitude of the
effect will be the same for a given DE regardless of the
nature of the radiation or the manner of radiation.
B. Modifying Factors
At the present time, two modifying factors are employed.
One is the Quality Factor (QF) which accounts for differences
in producing biological effects among various forms of
radiation. The other is the Distribution Factor (DF)
which accounts for the modification of the biological effects
when a radionuclide is nonuniformly distributed in an organ.
For example, the DE for X-ray to bone tissue is determined
by using QF=1 and DF=1, while that for Pu-239 in the bone is
determined by using a QF=10 (to account for the greater
effectiveness of alpha particle irradiation) and a DF=5
19
(to account for the peculiar distribution of Pu in the bone)
A DE=50 rem from X-rays or Pu-239 would thus induce the same
number of cancers in bone but the absorbed dose from the X-rays
would be 50 rad while that from Pu-239 would be only 1 rad.
18/ NCRP Report No. 39, Op_. cit. , p. 81.
19/ ICRP Publication 11, Op. cit., p. 21,
-------
116
- 14 -
In obtaining the derived values in Tables I and II,
MPLB and MPCa for Pu-239, a QF=10 was employed. This QF
implies, as mentioned above, that the particles of Pu-239,
which emit alpha particle radiation, are 10 times more effective
in inducing cancer than X-rays. Although the irradiation of
tissue by insoluble plutonium particles is highly nonuniform,
no DF value has been assigned to these particles and hence, a
DF=1 was employed in determining the derived values in Tables I
and II. Ideally, the DF should be determined by the ratio
of the observed effects in an organ following uniform and
nonuniform radiation of the tissue with the same radionuclide;
for example:
DF _ Number of cancers (nonuniform irradiation)
Number of cancers (uniform irradiation)
Since direct experimental data are not available, it is
necessary to derive the DF for insoluble Pu-239 particles from
collateral data. In a subsequent section, we shall present
the biological evidence that strongly suggests that a DF=1
grossly underestimates the DE for insoluble particulates of
Pu-239 and, consequently, that the derived standards, MPLB
and MPCa for this radionuclide, are greatly in error.20
In fact, it will be shown that the biological data strongly
suggests that for such particles one should use a DF=115,000.
20/ This applies as well to other alpha-emitting actinides
in insoluble particulate form.
-------
- 15 -
117
Before turning to the biological data it is appropriate to
discuss first the radiation field around a particle of Pu02
and thereby define the fundamental questions that need to be
answered by the collateral data from radiobiological studies.
The unique form of tissue irradiation displayed by
insoluble particles of Pu-239 occurs because, when Pu-239
decays, it emits an alpha particle with an energy of 5.1 MeV.
This particle has a range (produces biological damage) of only
some 40-45 u (0.004 cm) in human tissue. In other words,
a Pu-239 particle in tissue will only irradiate a volume of
tissue enclosed in a sphere of 45 u radius. As one moves in-
ward from the surface of this sphere, the radiation intensity
increases geometrically. About half of the alpha particle
energy is dissipated at 20 u (that is, with a volume that
is 1/8 the total volume). This means that the average dose
delivered in the first 20 u is 8 times that delivered in the
remaining 20 u. The first column of Table III describes
the radiation field around such a particle in soft tissue;
e.g., the skin. Since the lung is a spongy tissue with a large
air volume, the range of alpha particles is longer in the
lung and consequently the mass of irradiated tissue is larger.
Professor Donald Geesaman made a detailed analysis of plutonium
-------
118
- 16 -
particle irradiation of deep respiratory tissue21. The
last two columns in Table III describe the radiation field
around such a particle in the lung using Geesaman's lung
22
model . The dose rate to the entire organ is given in
column 2 of Table III.for comparison. From Table III it is
significant to note that with an assumed DF=1, the lung
dose from the same particle varies by more than 8 orders of
magnitude depending on whether one averages the dose over
the entire lung or calculates it on the basis of the tissue
exposed.
TABLE III
Radiation Dose Rate Due to a Pu-239 Particle
23,
(1 u in diameter, 0.28 pCi )
Mass of
Tissue
Dose Rate
(rem/yr)
Soft
Tissue
Irradiated
0 .4 ug
730,000
Entire
Organ
1000 g27
0.0003
Lung
Tissue 5
Irradiated
65 ug
4000
Closest 26
20 Alveoli
19 ug
11,000
21/ Geesaman, Donald P., An Analysis of the Carcinogenic Risk
from an Insoluble Alpha-Emitting Aerosol Deposited in Deep
Respiratory Tissue, UCRL-50387 and UCRL-50387 Addendum,
Lawrence Livermore Laboratory, Livermore, Calif., 1968.
-------
- 17 -
It would take 53,000 particles of the size illustrated
in Table III to reach the MPLB of 0.016 uCi which results
in 15 rem/yr to the entire (1000 g) lung. However, as
Table III indicates, these particles would irradiate only
3.4 g of this 1000 g to the lung, but at a dose rate of
28
4000 rem/yr . Thus, as Table III indicates, these particles
result in an intense but highly localized irradiation. A
fundamental question is, then: is this intense but localized
irradiation more or less carcinogenic than uniform
irradiation? Alternatively, is the DF for this particular form
of irradiation equal to, greater than, or less than one? In
the remainder of this section, we review the guidance, or
more appropriately lack of guidance, for dealing with this
hot particle problem.
119
22/ Geesaman, Donald P., UCRL-50387, pp. 8, 15.
23/ Langham, Wright H., The Problem of Large Area Plutonium
Contamination, U. S. Dept. of H. E. W., Public Health
Services, Seminar Paper No. 002, Dec. 6, 1968, p. 7.
24/ Long, A.B., "Plutonium Inhalation: The Burden of
Negligible Consequence," Nuclear News, June 1971, p. 71.
25/ Geesaman, Donald P., UCRL-50387, pp. 8, 15. Based on
Geesaman's model for a lung at one-half maximum inflation.
Geesaman estimates a total of 68 alveoli at risk, each
8xlO~6 cm3 in volume, and deep respiratory zone tissue density
of 0.12 g/cm3.
26/ See footnote 23.
27/ Based on a lung mass of a standard man = 1000 g.
28/ This assumes that the radiation field of the 53,000
particles do not overlap.
-------
120
C. The Hot Particle Problem
It is important to recognize that the ICRP has given
no guidance with respect to nonuniform irradiation of the lung
by insoluble alpha-emitters such as insoluble plutonium
particles. In its Publication 9, the ICRP states:
...In the meantime there is no clear evidence to show
whether, with a given mean absorbed dose, the biological
risk associated with a non-homogeneous distribution is
greater or less than the risk resulting from a more
diffuse distribution of that dose in the lung.29
In effect, the ICRP is saying that there is no guidance as
to the risk for non-homogeneous exposure in the lung, hence
the MPCa and the MPLB are meaningless for insoluble plutonium
particles.
The NCRP offers the following and similar statement
with respect to these particles:
(210) The NCRP has arbitrarily used 10 percent of
the volume of the organ as the significant volume for
irradiation of the gonads. There are some cases in
which choice of a significant volume or area is
virtually meaningless. For example, if a single
particle of radioactive material fixed in either lung
or lymph node may be carcinogenic, the averaging
of dose either over the lung or even over one cubic
centimeter may have little to do with this case.30
This hot particle problem is also well recognized in
the biological community. The following is extracted from a
29/ ICRP Publication 9, Op. cit., p. 4.
30/ NCRP Report No. 39, Op. cit., pp. 79-80
-------
- 19 -
paper by Professor Donald P. Geesaman:
So there is a hot particle problem with pluton-
ium in the lung, and the hot particle problem is not
understood, and there is no guidance as to the risk.
I don't think there is any controversy about that.
Let me quote to you from Dr. K. Z. Morgan's testimony
in January of this year before the Joint Committee on
Atomic Energy, U.S. Congress, [a] Dr. K. Z. Morgan
is one of the United States' two members to the main
Committee of the International Commission on Radio-
logical Protection; he has been a member of the com-
mittee longer than anyone; and he is director of
Health Physics Division at Oak Ridge National Labora-
tory. I quote: "There are many things about radiation
exposure we do not understand, and there will continue
to be uncertainties until health physics can provide
a coherent theory of radiation damage. This is why
some of the basic research studies of the USAEC are so
important. D. P. Geesaman and Tamplin have pointed
out recently the problems of plutonium-239 particles
and the uncertainty of the risk to a man who carries
such a particle of high specific activity in his lungs."
At the same hearing, in response to the committee's
inquiry about priorities in basic research on the bio-
logical effects of radiation, Dr. M. Eisenbud, then
Director of the New York City Environmental Protection
Administration, in part replied, "For some reason or
other the particle problem has not come upon us in
quite a little while, but it probably will one of these
days. We are not much further along on the basic
question of whether a given amount of energy delivered
to a progressively smaller and smaller volume of tissue
is better or worse for the recipient. This is another
way of asking the question of how you calculate the dose
when you inhale a single particle." [b] He was
correct; the problem has come up again.
121
laj Morgan, K. Z., "Radiation Standards for Reactor Siting,"
in Environmental Effects of Producing Electrical Power
Phase 2. Testimony presented at Hearings before the Joint
Committee on Atomic Energy, 91st Congress, 1970.
Washington, D. C. , u. S. Government Printing Office.
[b] Eisenbud, M. Panel Discussion. In: Environmental Effects
of Producing Electrical Power, Phase 2. Testimony presented
at Hearings before the Joint Committee on Atomic Energy,
91st Congress, 1970. Washington, D. C., U. S. Government
Printing Office.
-------
- 20 -
122
In the context of his comment it is interesting to
refer to the National Academy of Sciences, National
Research Council report of 1961 on the Effects of
Inhaled Radioactive Particles, [c] The first
sentence reads, "The potential hazard due to air-
borne radioactive particulates is probably the least
understood of the hazards associated with atomic
weapons tests, production of radioelements, and the
expanding use of nuclear energy for power production."
A decade later that statement is still valid. Finally
let me quote Drs. Sanders, Thompson, and Bair from a
paper given by them last October, [d] Dr. Bair and
his colleagues have done the most relevant plutonium
oxide inhalation experiments. "Nonuniform irradiation
of the lung from deposited radioactive particulates is
clearly more carcinogenic than uniform exposure (on a
total-lung dose basis), and alpha-irradiation is more
carcinogenic than beta-irradiation. The doses required
for a substantial tumor incidence, are very high, how-
ever, if measured in proximity to the particle; and,
again, there are no data to establish the low-incidence
end of a dose-effect curve. And there is no general
theory, or data on which to base a theory, which would
permit extrapolation of the high incidence portion of
the curve into the low incidence region." I agree and
I suggest that in such a circumstance it is appropriate
to view the standards with extreme caution.31
[c] U. S. NAS-NRC Subcommittee, Effects of Inhaled Radioactive
Particles. Report of the Subcommittee on Inhalation
Hazards. Committee on Pathologic Effects of Atomic
Radiation. National Academy of Sciences - National
Research Council, Washington, D. C. 1961. Publication
848. NAS-NRC/PUB-848, 1961.
[d] Sanders, C.L., R.C. Thompson, and W.J. Bair, "Lung
Cancer: Dose Response Studies with Radionuclides."
In: Inhalation Carcinogenesis. Proceedings of a Biology
Division, Oak Ridge National Laboratory, conference held
in Gatlinburg, Tennessee, October 8-11, 1969. M.G.
Hanna, Jr., P. Nettesheim, and J.R. Gilbert, eds. ,
U. S. Atomic Energy Commission Symposium Series 18, 1970.
pp. 285-303. (CONF-691001).
31/ Geesaman, Donald P., "Plutonium and Public Health,"
Lawrence Livermore Laboratory, Calif., GT-121-70, April 19, 1970,
reproduced in Underground Uses of Nuclear Energy, Part 2, Hearings
before the Subcommittee on Air and Water Pollution of the
Committee on Public Works, U. S. Senate, 91st Congress, 2nd Session
August 5, 1970, pp. 1530-1532.
-------
123
To these comments, referenced by Geesaman, can be added
the comments of Dr. A. B. Long:
"... there is an urgent need to dispell the sense of
security and certainty that the present limits for
the maximum permissible lung burden and the maximum
permissible air concentration bring . . . the public
should be informed of the uncertainties that exist
o 2
in these limits.
V . Biological Data Related to Cancer Risk from Insoluble
Plutonium Particles
We have shown that insoluble alpha-emitting particles
result in intense but localized radiation. They can irradiate
at very high doses without being organism- or organ fatal.
We said that the available biological data strongly suggests
that a DF=1 grossly underestimates the DE for insoluble
particulates of Pu-239, and consequently, the derived standards
MPLB and MPCa for this radionuclide are greatly in error.
We now turn to the experiments involving cancer induction
by intense local exposure, since these are especially
relevant in judging whether or not insoluble alpha-emitting
particles constitute a unique risk. Geesaman collected
and analyzed the pertinent experiments, and what follows
32/ Long, A.B., Qp_. cit. , p. 73,
-------
124
is essentially a review of his analysis , which has become
known as the "Geesaman hypothesis."
A The Geesaman Hypothesis
Dr. Roy E. Albert and co-workers performed a number of
14 — 36
experiments on the induction of cancer in rat skin
Albert's study of radiation-induced carcinoma in rat skin
gives some quantitative description of a high-dose car-
cinogenic situation. A skin area of 24 cm^ was exposed
to electron radiation with various depths of maximum penetra-
tion. The dose response curves are reproduced in Figure 1.
In all cases the response at sufficiently high doses (1000-
3000 rem) was large,~~1-5 tumors per rat by 80 weeks post
exposure. It was noted by Albert that when the dose was
normalized to a skin depth of 0.27 milimeters, the three
response curves became continuous (See Figure 2). Since this
33/ Geesaman, D.P., UCRL-50387 Addendum, Op. cit.
34/ Albert, R.E., F.J. Burns, and R.D. Heimbach, "The
effect of penetration depth of electron radiation on skin
tumor formation in the rat," Radiation Res. 30, 1967, pp. 515-524.
35/ Albert, R.E., F.J. Burns, and R.D. Heimbach, "Skin damage
and tumor formation from grid and sieve patterns of electron
and beta radiation in the rat," Radiation Res. 30, 1967, pp. 525-540
36/ Albert, R.E., F.J. Burns, and R.D. Heimbach, "The
association between chronic radiation damage of the hair
follicles and tumor formation in the rat," Radiation Res. 30,
1967, pp. 590-599.
-------
125
depth is near the base of the hair follicle which comprises
the deepest reservoir of epithelial cells of the germinal
layer, it was suggestive that this might be a critical
region in the observed carcinogenesis. The suggestion gained
significance from the observations that most of the tumors
are similar to hair follicles, and that in the non-ulcerogenic
dose range the number of tumors per rat was in nearly constant
ratio (1/2000-1/4000) with the number of atrophied hair
follicles. Thus the carcinogenesis in this experiment
was remarkably correlated with the dose to and specific
damage of a particular skin structure. When exposures were
made with stripe and sieve patterns of roughly 1 mm scale,
geometrical effects were observed: most notably the cancer
induction in the sieve geometry was suppressed at doses of
1700 rad but not at doses of 2300 rad. The reduction, however,
was again consistent with the reduction in damage as characterized
by atrophied hair follicles.
To summarize this important experiment, a high incidence
of cancer was observed after intense local doses of radiation,
and the carcinogenesis was proportional to the damage or
disordering of a critical architectural unit of the tissue,
the hair follicles.
-------
126
- 24 -
—I—i—I—1 T-
* 0 .36 mm
• 0.75 mm
• 1 .40 mm
o 1 .65 mm (suppl. data)
t; 4
o.
2
1
0
I I I 1 i
0123456
Surface dose — krod
Fig. 1. Tumor incidence with respect to
surface dose at 80 weeks for three
penetration depths of electrons.
8
7
6
o 5
a. 4
| 3
2
1
T
T
* 0.36mm
" 0.75 mm
• 1 .40 mm
° 1 .65 mm (suppl . data)
J I
I
012 34 56 78
Dose at 0.27 mm — krad
Fig. .2. Tumor incidence with respect to
the dose at a depth of 0.27 mm in
the skin at 80 weeks for three
penetration depths of electrons.
Source of Figures: Albert, R. E., et al., Radiation Res. 30,
Op. cit. , pp. 515-524, Figures 5 and 7; reproduced in
Geesaman, UCRL-50387 Addendum, Op. cit., p. 2.
-------
- 25 -
Others have observed carcinomas and sarcdmas in rats
and mice after intense exposure of the skin to ionizing radia-
37-43
tion. . Cancer induction is generally a frequent event
in these experiments. Even at elevated doses, such as
12,000 rad of 1 MeV electrons, Boag and Glucksmann induced
""5 sarcomas/100 cm2 in rats
A few results for rabbits, sheep, and swine were
obtained at Hanford ." -1. Despite the small number of animals
127
3_7/ Withers, H.R. , "The dose-survival relationship for
irradiation of epithelial cells of mouse skin," Brit. J.
Radiol. 4p_, 1967, pp. 187-194.
38/ • Hulse, E.V., "Tumours of the skin of mice and other
delayed effects of external beta irradiation of mice using
90sr and 32P,- Brit. J. Cancer 1£, 1962, pp. 72-86.
39/ Boag, J.W. and A. Glucksmann, "Production of cancers in
rats by the local application of Beta-rays and of chemical
carcinogens," Progress in Radiobiology, J.S. Mitchell,
B.E. Holmes, and C.L. Smith, eds. Proceedings of the Fourth
International Conference on Radiobiology held in Cambridge,
14-17 August 1955. Edinburgh, Oliver and Boyd, 1956, pp. 476-479.
40/ George, L.A. and L.K. Bustad, "Gross effects of beta rays
on the skin," Hanford Atomic Products Operation, Biology
Research Annual Report for 1956, HW-47500, 1957, pp. 135-141.
41/ George, L.A. II, R.L. Pershing, S. Marks, and L.K.
Bustad, "Cutaneous fibrosarcoma in a rabbit following beta
irradiation," Hanford Atomic Products Operation, Biology
Research Annual Report for 1959, HW-65500, 1960, pp. 68-69.
42/ Ragan, H.A., W;J. Clarke and L.K. Bustad, "Late effects
of skin irradiation," Battelle-Northwest Laboratory Annual
Report for 1965 in the Biological Sciences, BNWL-280, 1956,pp. 13-14
4_3/ Karagianes, M.T. , E.B. Howard and J.L. Palotay, Battelle-
Northwest Laboratory Annual Report for 1967 to the USAEC Division
of Biology and Medicine, Vol. I, Biological Sciences, BNWL-714,
1968, pp. 1.10-1.11
-------
128
- 26 -
involved, surface doses of 16,000 rad from a P32 plaque
induced an average of 1 cancer/animal which is indicative
that larger mammals are similarly susceptible to skin cancer
after intense radiation insult. Again, these gross obser-
vations demonstrate that enhanced tumor incidence does occur
after very high doses.
Intense localized radiation of the subcutaneous and
intraperitoneal tissue of animals by Pu-239 has also been
shown to cause a high frequency of cancer induction^3-45_
Now what are these experiments trying to tell us?
Certainly a reasonable interpretation of these experimental
results is: when a critical architectural unit of a tissue
(e.g., a hair follicle) is irradiated at a sufficiently high
dosage, the chance of it becoming cancerous is approximately
10~3 to 10~4. This has become known as the "Geesaman
hypothesis."
B Related Human Experience
Since the above experiments relate to cancer induction
in animals, it is pertinent to ask whether man is more or less
44/ Sanders, C.L. and T.A. Jackson, "Induction of Mesotheliomas
and Sarcomas From 'Hot Spots' of Pu02 Activity," Health Physics,
Vol. 22, No. 6, June 1972, pp. 755-759.
45/ Lisco, Herman, et al, "Carcinogenic Properties of
Radioactive Fission Products and of Plutonium," Radiology,
Vol. 49, No. 3, Sept. 1947, pp. 361-363.
-------
- 27 -
sensitive to such intense localized radiation. C. C.
Lushbauqh reported on a lesion that developed as the result
of residual Pu-239 from a puncture wound . The particle
contained 0.08 ug (0.005 uCi) of Pu-239. Commenting on
the histological examination of the lesion, the authors
state, "The autoradiographs showed precise confinement of
alpha-tracks to the area of maximum damage and their
penetration into the basal areas of the epidermis, where
epithelial changes typical of ionizing radiation exposure were
present. The cause and effect relationship of these findings,
therefore, seemed obvious. Although the lesion was minute,
the changes in it were severe. Their similarity to known
precancerous epidermal cytologic changes, of course, raised
the question of the ultimate fate of such a lesion should it
be allowed to exist without surgical intervention..." In
this case, less than 0.1 ug of Pu-239 produced precancerous
changes in human tissue. The dose to the surrounding tissue
was very intense. There is every reason to believe that a
smaller quantity of Pu-239 would have produced similar changes.
This precancerous lesion indicates that a single Pu-239
particle irradiates a significant (critical) volume of tissue
and is capable of inducing cancer. The Lushbaugh study was
129
46/ Lushbaugh, c.C. and J. Langham, Op. cit. , pp. 461-464
-------
130
- 28 -
published in 1962. At that time the total number of puncture
wounds in man was less than 1,000 . The treatment of such
wounds was excision so that the total number of wounds dis-
playing residual contamination by plutonium particles was
certainly less than 1,000. Therefore, this wound data would
suggest that insoluble plutonium particles could offer a risk
of cancer induction in man that is even greater than 1/1000
per particle. In other words, when a critical unit of tissue
is irradiated, man may be more susceptible to cancer than the
Albert data as analyzed by Geesaman would suggest.
A second case of plutonium particle induced cancer is
that of Mr. Edward Gleason. He was not associated with
the nuclear industry but was a freight handler who unloaded,
rotated and reloaded a crate that was contaminated by the
leaking carboy of Pu-239 solution which it contained. He
subsequently developed an infiltrating soft tissue sarcoma
on the left palm which eventually resulted in his death.
Although this case is not as clear cut as the case of the
plutonium worker, there is an overwhelming medical probability
that his cancer was induced by nlutonium. Mr. Gleason's
unfortunate contact with Pu-239 lead to a lawsuit,
47/ Vanderbeck, J.W., "Plutonium in Puncture Wounds," HW-66172,
Hanford Laboratories Operation, July 25, 1960.
-------
- 29 - 131
Edward Gleason, et al v. NUMEC. This suit was eventually
settled out-of-court. A discussion of the evidence in this
case by one of the authors is presented in the Appendix B
of this report.
These two cases, drawn from the relatively small number
of individuals so contaminated, strongly suggest that Pu-239
particles offer a unique carcinogenic risk. They indicate
that a single particle is capable of delivering an intense
radiation dose to a critical volume of tissue and that this
disruptively irradiated tissue, like an atrophied hair follicle,
has a high probability (maybe as high as 1/1000) of becoming
cancerous.
C . Related Lung Experiments
The skin experiments with animals are remarkable in that
a highly disruptive dose of radiation to a small portion of
repairable mammalian tissue produced frequent carcinogenesis.
The chance of producing one cancer per animal is essentially
unity. It is reasonable to expect that a comparable
development could occur in lung tissue. While a number of
radioactive substances have been used to induce lung cancers
in mice and rats , it is difficult to derive any characteriza-
tion of carcinogenesis from these experiments.
48/ Cember, H., "Radiogenic lung cancer," Progress in
Experimental Tumor Research, F. Homburger, ed. New York,
Hafner Publishing Company, Inc., Vol. 4, 1964, pp. 251-303.
-------
132
- 30 -
The work of Laskin, et al, though not specifically
involving deep respiratory tissue, does demonstrate a source
49
intensity-response curve for lung tissue . A Ru-106
cylindrical source was implanted in the bronchi of rats, and
cancers were observed to arise from the bronchial epithelium.
The response curve indicates a substantial response (7 percent)
even at 0.008 uCi burden, and a slow, approximately logarithmic
increase of tumor incidence over three orders of magnitude
in the source intensity. Corresponding first-year doses to
adjacent bronchial epithelium varied from 10^ rad to 106 rad
Animals were followed until death and it was observed that
the tumor incidence generally increased with the dose accumulated
at death. The lowest accumulated dose associated with a
cancer was 1400 rad. For an accumulated dose of the order of
10^ rad the incidence was approximately two-thirds. Cember
fortified glass beads (0.3 u diameter) with several microcuries
of Sr-90 , and single beads were implanted in the lungs of
rats. Tumors were observed in 7 of 23 animals. In a second
experiment Cember exposed rat lungs to Ce-144 particles. For
49/ Laskin, S., M. Kuschner, N. Nelson, B. Altshuler, J.H.
Harley and M. Daniels, "Carcinoma of the lung in rats exposed
to the beta-radiation of intra-bronchial rutheniumlOS pellets.
1. Dose response relationships," J. Natl. Cancer Inst. 31,
1963, pp. 219-231.
50/ Altshuler, B., "Dosimetry from a Ru106-coated platinum
pellet," Radiation Res. 9, 1958, pp. 626-632.
-------
133
a burden range of 0.5 uCi to 50 uCi the observed tumor incidence
fluctuated between 0.04 and 0.3 .
All of these lung experiments involved intense exposures
and a significant level of carcinogenesis . Severe damage
and disruption of tissue were associated with the exposures.
The most relevant lung experiment is Bair's Pu^39o2
inhalation study with beagles . Exposure was to
particulates of 0.25 u or 0.5 u median diameter; burdens were
in the uCi range. Twenty of the 21 dogs that survived more
than 1600 days post exposure had lung cancer. Many of these
cancers were multicentric in origin. The cancers again
appeared in conjunction with severe lung injury. Since the
natural incidence of the disease is small, it appears that
at this level of exposure the induction of lung cancer is a
certainty during the normal beagle life span. At the same
5_1/ Cember, H., Op. cit.
52/ Bair, W.J., J.F. Park, and W.J. Clarke, "Long-term
study of inhaled plutonium in dogs," Battelie Memorial Institute
(Richland), AFWL-TR-65-214, 1966 (AD-631 690).
53/ Park, J.F., W.J. Clarke and W.J. Bair, "Chronic effects
of inhaled 239puo2 in beagles," Battelle-Northwest Laboratory
Annual Report for 1967 to the USAEC Division of Biology and
Medicine, Vol. I, Biological Sciences, BNWL-714, 1968,
pp. 3.3-3.4.
54/ Park, J.F., e_t al, "Progress in Beagle Dog Studies with
Transuranium Elements at Battelle-Northwest," Health Physics,
Vol. 22, No. 6, June 1972, pp. 803-810.
-------
134 - 32 -
time, since the pathological response is saturated in this
experiment, it is inappropriate to draw any inference about
the magnitude of the response at smaller burdens. The smallest
burden (at death) in a dog showing lung cancer was 0.2 uCi.
Presumably this would correspond to a particle burden of
about 107 particles. Burdens-which are smaller by orders of
magnitude may still induce a substantial incidence of cancer.
Indeed, the cancer risk may, as for skin and soft tissues,
correspond to a risk per particle in the neighborhood of
1/1000 to 1/10,000.
VI . Critical Particle Activity
Not all particles would be expected to result in these
high cancer probabilities. As the particle size or specific
activity per particle is reduced so is the dosage to the
surrounding tissue. Indeed, at sufficiently small particle
size or specific activity, one would expect the radiation
insult to behave similar to uniform irradiation. The study
of Albert on induction of cancer in rat skin indicates a
precipitous change in the dose response curve as the dosage
exceeds 1,000 rem . (See Figure 2). This suggests that a
particular level of tissue damage must occur before this
unique carcinogenic response occurs. The experiments of
55/ Albert, R.E. , e_t al, Radiation Res. 30_, Op. cit. , pp. 515-524,
Figure 7; reproduced in Geesaman, UGRL-50387 Addendum, Op. cit.,
p. 2.
-------
- 33 -
Laskin, e_t al, indicate a significant carcinogenic response
in the lung at 1400 rem, suggesting a comparable sensitivity
of lunq tissue •. Geesaman indicates that the tissue repair
time in the lung is of the order of one year . It therefore
seems appropriate, but not necessarily conservative, to accept
as guidance that this enhanced cancer risk occurs when particles
irradiate the surrounding lung tissue at a dose rate of 1000
rem/yr or more.
135
TABLE IV
Particle Activity and Size to Give a Dose of
58
1000 rem/year to the Surrounding Lung Tissue
Particle
Activity
(pCi)
3/4 max inflated (138 alveoli) 0.14
1/2 max inflated ( 68 alveoli) 0.07
Closest 20 alveoli 0.02
Particle Diameter (u)
239PuO, 238Pu02
0.8 0.12
0.6 0.09
0.4 0.06
59
56/ Laskin, et al, Op. cit.
5_7/ Geesaman, Donald P., UCRL-503.87, Op_. cit., p.-1.1.
5_8_/ Ibid
59/ Based upon specific activity given by Langham, W.H.,
Op. cit., p. 7.
-------
136
- 34 -
As seen from Table IV, using Geesaman's lung model, a
particle with an alpha activity between 0.02 pCi and 0.14 pCi
is required to give a dose of 1000 rem/yr to irradiated lung
tissue. For purposes of establishing a maximum permissible
lung particle burden we will use 0.07 pCi from long half-
lived (greater than one year) isotopes as the limiting
alpha activity to qualify as a hot particle. Thus, throughout
the remainder of this report, hot particle will imply a particle
with at least this limiting alpha activity which is insoluble
in lung tissue.
A. Exposures at Rocky Flats
The AEC has a plutonium facility associated with its
nuclear weapons program at Rocky Flats, Colorado. This
facility is operated under contract to the AEC by the Dow
Chemical Company. The employees, the environment and undoubtedly
the surrounding population have been contaminated with plutonium
particles as a result of the operation of this plant.
It is, therefore, pertinent here to examine the information
60/ Mann, J.R. and A.R. Kirchnev, Op. cit.
61/ Poet, S.E. and E.A. Kartell, "Plutonium-239 and
Americium-241 in the Denver Area," Health Physics, Vol. 23,
1972, pp. 537-549.
62/ Richmond, Chet, Transcript of Plutonium Information
Meeting of the Advisory Committee on Reactor Safeguards,
Los Alamos, N. Mex., 5 January 1974, pp. 319-320.
-------
- 35 - 137
available on the exposure of employees of the Rocky Flats
facility and to relate this to the hot particle problem.
J. R. Mann and R. A. Kirchner discuss the exposures that
resulted from a plutonium fire at Rocky Flats on 15 October
1965. Some 400 employees were working in the room at the
time the fire occurred. These employees were subsequently
placed in a whole body counter to determine their lung burdens
of Pu-239. However, Mann and Kirchner reported only on those
25 employees who were exposed above the MPLB of 0.016 uCi.
Table V presents the information on the exposure of
these 25 employees. Utilizing the other information presented
by Mann and Kirchner , we have also estimated in Table V
the fraction of the lung burden activity (uCi) associated
with hot particles and the number of hot particles that this
represents.
63/ Mann, J.R. and R.A. Kirchner, Op. cit,
-------
138
- 36 -
TABLE V
Rocky Flats Exposure*
Number of
Cases
1
1
1
19
Total Lung
Burden (uCi)
0.272
0.160
0.111
0.064
0.024
Hot Particles
Lung Burden (uCi)
0.033
0.019
0.013
0.008
0.003
Number of
Hot Particles
137,000
79,000
54,000
33,000
12,500
* Mann and Kirchner presented the lung burdens as number
of MPLB. These have been converted to uCi in column two
using MPLB=0.016 uCi. (/or the groups with 3 and 19 cases,
we selected the midpoi- - of the reported range.) The hot
particle burden in co.umn three was estimated by multiplying
the total burden by 0.17, the fraction of the activity on
particles above 0.6 u, and 0.70, the fraction of initial
deposited activit-; that was involved in long term retention in
the lung. Baser1 on particle size data reported by Mann and
Kirchner, we estimate the average hot particle activity is
about 0.24 pCi. The numbers of hot particles in the last column
were obtained by dividing the hot particle burdens in column
three by the- average hot particle activity (0.24 pCi) .
Mlowing a risk of cancer equal to 1/2000 per hot
pa:. Licle, suggests that the individuals whose exposures are
:.resented in Table V stand a very high chance of developing
lung cancer — the probability is essentially unity. In
this respect, it is significant to note that in the experiments
-------
139
- 37 -
reported by Park, e_t al, the beagle dog with the smallest
64
lung burden, i.e., 0.2 uCi, developed lung cancer. The
highest burden in Table V is comparable to the lowest
beagle exposure; the lowest exposure in Table V, the 19
cases with lung burdens in the 0.024 uCi range are only an
order of magnitude less than the lowest beagle exposure.
We would suggest that this is potentially a serious situation.
As of this time, none of these individuals has developed
65
lung cancer. However, it is only 9 years since the exposure
and there is good reason to suggest that the latent period
(the time between exposure and the development of cancer)
is much longer than this. In the beagle dog experiments,
the lowest lung burden was associated with a latent period
of 11 years. The latent period may be longer in man and
particularly at these lower dosages and the small number of
cases involved. Therefore, while these exposed individuals
will be expected to supply pertinent data relative to this
hot particle cancer risk over the next 10 to 20 years,
these exposures give us no information at this time that would
warrant modifying the risk per particle or the critical
particle activity.
64/ Park, J.F., e_t al, Health Physics, Op. cit. p. 805,
65/ Richmond, Chet, Op. cit., p. 320.
-------
140
B . Manhattan Project Workers
Another study of human respiratory exposure to plutonium
relates to 25 young men exposed to plutonium during the
66
Manhattan Project. The latest examination of this group
found them to be free of lung cancer although the report
states, "The bronchial cells of several subjects showed
moderate to marked metaplastic changes, but the significance
of these changes is not clear." Such metaplastic changes are
a possible indicator for detecting incipient or actual lung
cancer. In one case the report indicates that the subject
was a heavy smoker (3 packs/day) and undoubtedly this con-
tributed to the changes. Nevertheless, these findings
suggest that lung cancer may become manifest in some of
these subjects in the future. Indeed, one would not be
surprised to find one lung cancer even in such a group of
non-exposed subjects. During the latest examination of these
workers, in vivo measurement of the plutonium lung burdens
were conducted with these results:
An average MDA for a 2000-sec counting time is
about 7 nCi if one uses the 95% confidence level.67
For the 68% confidence level and a similar counting
time, the comparable value is about 3.5 nCi.
66/ Hemplemann, L.H., et_ al, "Manhattan Project Plutonium
Workers; A Twenty-Seven Year Follow-Up Study of Selected Cases,
67/ MDA refers to the minimum detectable amount.
-------
141
Positive counts were obtained for 14 of 21 persons
measured. These counts suggested chest burdens ranging
from 3 to about 10 nCi. However, in no case did the
estimated chest burden exceed the MDA at the 95% con-
fidence level. Seven of the 14 subjects with positive
chest counts had estimated chest burdens of 7 nCi or
greater and may be considered (at the 68% level of
confidence) to have statistically significant chest
burdens of from 7 to 10 nCi.68
Since the plutonium is still in the lung cavity, 27 years
post-exposure, it is correct to assume that it was initially
c q
in the insoluble form and hence pertinent here. At the time
of this measurement, however, most of the material would be
expected to be in the lymph nodes. Nevertheless, we could
estimate the initial particle burden in these subjects from
these data if we knew the initial particle size at the time
of contamination. This particle size data is unavailable.
The nature of the contaminating events suggest that the
particle size might have been somewhat larger than those that
result from plutonium fires where most of the respirable
activity resides on particles in the size range of 0.1 u to
0.5 u in diameter. Much of the contamination of the
68/ Hemplemann, L.H., Op. cit., p. 474.
69/ ICRP Publication 19, The Metabolism of Compounds of
Plutonium and Other Actnides, Pergamon Press, New York, 1972, p. 7
70/ Mann, J.R. and A.R. Kirchner , Op. cit. , p. 880.
-------
142
- 40 -
Manhattan workers resulted from aspiration of droplets of
liquid solutions of plutonium into the air wherein much larger
particle sizes would result. At the same time, the activity
of the plutonium in the particle would be considerably less
than that for a particle of PuC>2 • For example, it is stated
that 14 of the 25 subjects with measurable body burdens of
plutonium worked in the recovery operation and that this
occurred when working with solutions containing 1-40 g/liter
of plutonyl nitrate to which ^2^2 was being added with
vigorous stirring in an open hood. This resulted in con-
siderable fizzing and the discharge of droplets into the
air outside the hood. A droplet 1 u in diameter (0.5 u^)
from the solution with the highest concentration (40 g/liter)
would therefore contain only 6x10"^ pCi compared with a
0.07 pCi particle of Pu02 (a specific activity that is
lower by a factor of 100). In other words, the particles
involved in this study do not qualify as hot particles.
They are delivering dosages lower than 1000 rem/yr to the
71/ Recall from Table IV that a 0.07 pCi, the limiting
activity for a hot particle, would give a dose of 1000 rem/yr
to the surrounding tissue in a lung inflated to 1/2 maximum.
72/ Of the particles of 'an inhaled aerosol that are deposited
in the deep respiratory zone of the lung, virtually all are
less than 5 u in diameter [Geesaman, UCRL-50387, Op. cit. , p. 3]
A 5 u droplet from the 40 g/liter solution would correspond
roughly to the limiting activity of a hot particle.
-------
143
- 41 -
surrounding tissue (roughly 10 rem/yr).
C Weapons Test Fallout
Another source of human contamination that is suggested
as being pertinent to this problem is the plutonium in the
fallout from nuclear weapon tests. The plutonium from
weapon tests is incorporated in or deposited on particles
that contain other materials and, like that for the Manhattan
workers, the specific activity in these particles is much
smaller than that in hot particles.
VII Exposure Standards for Hot Particles
Thus the existing biological evidence strongly suggests
that an insoluble particle of Pu-239 deposited in deep
respiratory tissue represents a risk of cancer induction
between 1/1000 and 1/10,000. Prudent public health practices
should assess the risk associated with environmental plu-
tonium and establish exposure guidelines on the basis of
these probabilities.
The existing standards for uniform radiation exposure
of the whole body or lung can be used as the basis for
establishing particle exposure standards by equating the
risk of cancer induction between the two types of exposure
(uniform vs. grossly non-uniform). The most recent
assessment of the risk associated with uniform irradiation of
-------
144
- 42 -
man was performed by the NAS-MRC Advisory Committee on the
Biological Effects of Radiation. Their report, published in
1972, is referred to as the BEIR Report.73
A. Occupational Exposure
The existing occupational exposure standard for uniform
whole body irradiation is 5 rem/yr and for the lung, 15 rem/yr.
the BEIR Report estimates that exposure of the whole body
of an individual to 5 rem/yr would lead to a cancer risk
between 4.5x10 and 2.3xlO~3/yr. Their best estimate is
-3 75
10 /yr. Their estimate of the risk of cancer to the
individual from a lung exposure of the 15 rem/yr is 3xlO~5/yr.76
Allowing a risk of cancer induction between 1/1000 and
1/10,000 per particle, Table V presents the maximim permissible
lung particle burdens (MPLPB) that result in risks comparable
to these uniform radiation standards for occupational exposure.
The MPLPB values in Table V represent a very substantial
reduction in the MPLB. A hot particle of Pu-239 at the lower
limit activity contains only 0.07 pCi while the MPLB for
occupational exposure is 1.6xl04 pCi. Thus the
TV NAS-NRC, "The Effects on Populations of Exposure to
Low Levels of Ionizing Radiation," (BEIR Report), NAS-NRC,
Washington, D. C. , Nov. 1972.
74/ Ibid, p. 91.
75_/ Ibid, p. 91.
p. 156.
-------
145
- 43 -
TABLE V
Occupational Exposure Guidance for Insoluble Alpha Emitters,
Maximum Permissible Lung Particle Burden (MPLPB)
Cancer risk due to 5 rem/yr Assumed Risk in Particle
whole body exposure ?b
4.
10
2.
5xlO~4
~3 (best estimate)
3xlO~3
1/1000
0.45
1.
2.3
1/2000
0.9
2.
4.6
1/10,000
4.5
10.
23.
largest MPLPB in Table V, 23 particles, represent a
reduction of the existing MPLB and MPCa by a factor of
10,000. It is recommended here that the best estimate of
the effects of uniform exposure by the BEIR Committee be used
together with a risk of cancer induction of 1/2000 per hot
particle in determining the MPLPB for insoluble alpha-
emitting radionuclides in hot particles. This is a somewhat
arbitrary compromise and is not the most conservative value
that could be recommended. Thus, the recommended MPLPB
for occupational exposure from hot particles of alpha-
77/ The number of particles required to give a cancer risk
equal to that from uniform radiation.
78/ Source: BEIR Report, Op. cit. , p. 91. The MPLPB
corresponding to a lung cancer risk of 3xlO~5 due to 15 rem/yr
lung dose [BEIR Report, Op. cit., p. 156] are 0.03, 0.06
and 0.3 for assumed particle risks of 1/1000, 1/2000 and
1/10,000 respectively.
-------
146
- 44 -
emitting radionuclides in the deep respiratory zone is 2
particles. This corresponds to a MPLB of 0.14 pCi and repre-
sents a reduction of 115,000 in the existing MPLB. This
implies that the DF for hot particles is 115,000. Moreover,
it requires a reduction of the MPCa for Pu-239 by 115,000 to
a value of 3.5xlO~16 uCi/ml unless it is determined that
the plutonium is not in hot particles.
B- Exposure of the General Public
As indicated in Table II, the MPLB for non-occupational
exposure (members of the public) is tenfold less than that
for occupational exposure. Such an exposure limit for a hot
particle would be 0.2 particles. Exposure at this level
implies that on the average one out of five individuals
would be contaminated by a particle and the other four would
not. Obviously the exposed invididuals would be assuming a
disproportionate fraction of the risk. In fact, since an
individual is exposed to whole particles, any non-occupational
exposure to hot particles would be an overexposure. This
condition does not meet the recommendations and admonitions
of the FRC, ICRP and NCRP.
under certain conditions, such as widespread radioactive
contamination of the environment, the only data avail-
able may be related to average contamination or exposure
levels. Under these circumstances, it is necessary to
make assumptions concerning the relationship between
-------
-45- 147
average and maximum doses. The Federal Radiation
Council suggests the use of the arbitrary assumption
that the majority of individuals do not vary from the
average by a factor greater than three. Thus, we
recommend the use of 0.17 rem for yearly whole-body
exposure of average population groups. (It is noted
that this guide is also in essential agreement with
current recommendations of the NCRP and the ICRP.)
It is critical that this guide be applied with reason
and judgment. Especially, it is noted that the use
of the average figure, as a substitute for evidence
concerning the dose to individuals, is permissible
only when there is a probability of appreciable homo-
geneity concerning the distribution of the dose within
the population included in the average. "
Strict adherence to these guidelines implies that
the ambient air standard should be zero particles.^0
While a variety of suggestions could be proposed, we recommend
a slight deviation from these guidelines and the acceptance
of the disproportionate risk implicit in the 0.2 particle
standard. This is a workable solution since best estimates
of lung burdens can be fractional quantities. Thus, we
recommend that the MPLPB for members of the public be 0.2
hot particles, and the average lung burden for members of the
public be 0.07 hot particles, a factor of 3 less than the
maximum.
79/ FRC Report No. 1, Op. cit., p. 27.
80/ Had we based the standard on a 1/10,000 risk per
particle (See Table V), the MPLPB would have been one
particle and this problem would not exist.
-------
148
- 46 -
The MPLPB=0.2 particles implies that the existing MPCa
for non-occupational exposure to Pu-239 should also be reduced
by a factor of 115,000 to a value of 9xlO~18 uCi/ml unless it
is determined that the plutonium is not in hot particles.
C. Exp_gsure from Accidental Releases
There are no direct statements by standard-setting organi-
zations regarding an "acceptable" exposure associated with
release of radioactivity in an accident.81 For purposes of
evaluating sites for nuclear reactors, establishing site
boundaries, and preparing safety analysis reports, however,
the AEC has adopted specific criteria. The reactor site
boundary (surrounding the exclusion area) must meet the following
criteria (10 CFR 100.11(a)(1)):
(1) An exclusion area of such size that an
individual located at any point on its boundary
for two hours immediately following onset of the
postulated fission product release would not
receive a total radiation dose to the whole body
in excess of 25 rem2 or a total radiation dose
in excess of 300 rem2 to the thyroid from iodine
exposure.
81/ Fish, B.R., G.W. Keilhalte, W.S. Snyder, and S.D. Swisher,
Chapter 7 of early draft version of B.R. Fish, e_t al, "Calcu-
lation of Doses Due to Accidental Released Plutonium from an
LMFBR," ORNL-NSIC-74 (Nov. 1972), p. 128. This chapter was
deleted from the final version at the direction of AEC-Division
of Reactor Development and Technology because it was judged to
be not directly applicable to the objective of the study, and
the information base from which it was developed was already
available in other documents. AEC-DRDT further stated that it
was not removed because of the quality of the work.
-------
149
- 47 -
2
The whole body dose of 25 rem referred to
above corresponds numerically to the once in a
lifetime accidental or emergency dose for radia-
tion workers which, according to NCRP recommenda-
tions may be disregarded in the determination of
their radiation exposure status (see NBS Handbook
69 dated June 5, 1959). However, neither its use
nor that of the 300 rem value for thyroid exposure
as set forth in these site criteria guides are
intended to imply that these numbers constitute
acceptable limits for emergency doses to the public
under accident conditions. Rather, this 25 rem
whole body value and the 300 rem thyroid value
have been set forth in these guides as reference
values, which can be used in the evaluation of
reactor sites with respect to potential reactor
accidents of exceedingly low probability of
occurrence, and low risk of public exposure to
radiation.
Fish, et al, made the following comments regarding the
applicability of these criteria to the case of plutonium
release. These comments are also applicable to hot particle
case.
First, the wording of sections 100.11(a)(1)
clearly limits the application to the irradiation of
the whole body and the thyroid; no other organ or tissue
is mentioned or implied. Furthermore, only fission
products in general and iodine in particular are
identified as reference substances. Finally, footnote (2)
states unequivocally that the guides are not to be
considered as acceptable limits for emergency doses
to the public under accident conditions.82
Without addressing whether the guideline values,
25 rem to the whole body and 300 rem to the thyroid, should
82/ Ibid, p. 129.
-------
150
- 48 -
be considered as acceptable limits, or whether design basis
accidents that are currently evaluated under these criteria
are "of exceedingly low probability of occurrence," we
recommend that 10 CFR 100.11(a) (1) be modified as follows in
order to establish a hot particle standard that is equivalent
to the risk associated with 25 rem whole body irradiation:
(1) An exclusion area of such size that an
individual located at any point on its boundary
for two hours immediately following onset of the
postulated fission product or other radionuclide
release would not receive a total radiation dose
to the whole body in excess of 25 rem2 or a total
radiation dose in excess of 300 rem2 to the
thyroid from iodine exposure, or receive a lung
particle burden in excess of 10 hot particles.3
2
(Unchanged from original text)
A hot particle is a particle that contains
sufficient activity to deliver at least 1000 rem/yr
to the surrounding lung tissue. For isotopes
having half-lives greater than one year, this would
correspond to particles containing at least 0.07
pCi of alpha activity.
We also recommend that similar criteria be established
limiting hot particle releases for nuclear facilities not
now covered under 10 CFR 100.
D. Surface Contamination
Hot particles deposited on land surfaces can be
resuspended into the air by any number of means, including
wind, automobile traffic, human or animal movements, Following
-------
- 49 -
151
an accident wherein surfaces are contaminated with hot
particles, it is necessary to have a standard to apply to
decontamination measures.
The number of particles that can be resuspended from
surfaces has been the subject of a number of experiments.
These experiments have usually resulted in the determination
of a resuspension factor (RF). The RF is defined by:
RF (m-l) = concentration in air (uCi/m3)
concentration on surface(uCi/m2)
R. L. Kathren has reviewed the data obtained on RF
8 3
values. He indicates that, "reported [RF] values for plutonium
and its compounds range over 11 orders of magnitude." This
11 orders corresponds to values between 10"1 to 10~H rrT1.
Kathren indicates that, "an RF of 10~4 rrT1, although
conservative is appropriate."84 Langham indicates that a
member of the Danish scientific team used an RF=10~3 m~l
during the Thule deliberation.85 We would recommend that
j83/ Kathren, R.L., "Towards interim acceptable surface con-
tamination levels for environmental Pu02," BNWL-SA-1510, Battelle
Northwest Laboratory, Richland, Washington, April 1968, pp. 3-4.
84/ Ibid, p. 4.
85/ Langham, Wright H. , Op_. cit. , p. 5. The Thule Delibera-
tions refer to the deliberations following the accidental
crash of a B-52 bomber carrying nuclear weapons near Thule
Air Force Base in Greenland. The high explosives in the
weapons detonated and dispersed the plutonium.
-------
152
- 50 -
the value selected by Kathren be used when the RF is unknown
to determine the ambient ground contamination standard.
Applying an RF=10~4 m"1 to the ambient MPCa standard
recommended in the previous section, we obtain a maximum per-
missible surface contamination (MPSC) level for hot particles
of 9xlO~8 uCi/m2. This is roughly 1 hot particle/m2.
In areas where an RF greater or less than 1CT4 m~l could
be shown to apply, the MPSC could be altered appropriately.
E. As Low as Practicable Hearings
It is to be understood that the above recommendations
do not represent endorsement on our part of the risk
inherent in the existing radiation protection guidelines
upon which these recommendations are based. Rather, we offer
the admonition that the exposures should be kept as far
below these guidelines as is practicable. Therefore, we
further recommend that these guidelines be incorporated
into the existing regulations without delay and that the
appropriate agency or agencies convene hearings to determine
for the regulations what constitutes as low as practicable
limits for exposure to hot particles.
86/ This value is derived as follows: The recommended MPCa
for hot particles is 9x10-18 uCi/ml which corresponds to
9xlO~12 uCi/m3. The maximum ground contamination level, using
RF=10-4 m"1, is 9x10-12/10-4 = 9x10-8 uCi/m2.
-------
153
Summary of Recommendations
The following recommendations apply to alpha-emitting
hot particles where a hot particle is defined as a particle
that contains sufficient activity to deliver at least 1000
rem/yr to the surrounding lung tissue. For isotopes having
half-lives greater than one year, this would correspond to
particles containing at least 0.07 pCi of alpha activity.87
It is recommended that:
1. For occupational exposure
MPLPB = 2 hot particles
MPCa for Pu-239 = 3.5xlO~16 uCi/ml88
2. For non-occupational exposure
MPLPB =0.2 hot particles
MPCa for Pu-239 = 9x10-18 uCi/ml89
87/ These particulates would consist of compounds of Pu and
the other actnides which fall into Class Y material in the ICRP
Task Group Lung Model. These materials would be retained for
years in the lung. See for example, ICRP Publication 19, Op. cit. ,
p. 6. Since only particles in the size range of 5 u and below~In"
diameter would be deposited in the deep respiratory tissue, this
in effect sets an upper limit for the particle size of interest
here. If the half-life is less than or close to 1 year the limit
of 0.07 pCi can be adjusted upward through appropriate calculations,
88/ This MPCa applies for particles containing 0.07 pCi of
Pu-239. For particles containing more than 0.07 pCi the
MPCa could be increased proportionately. For particles
containing less than 0.07 pCi the existing MPCa-4xlO-H pCi/ml
would apply. The MPCa for hot particles of other isotopes
and mixtures of isotopes should be established on a similar
basis with consideration given to the half-life of the isotope.
89/ Ibid.
-------
154
- 52 -
3. For accidental releases exposure (10 CFR 100.11(a)(1))
MPLPB (2 hours exposure) = 10 hot particles
4. For unrestricted areas
/ 9 90
MPSC = 1 hot particle/m^
5. Hearings should be convened to determine as low as
practicable regulations.
90/ This value is meant for guidance with respect to
decontamination of an unrestricted area that has been con-
taminated with hot particles. In areas where an RF greater or
less than 10~4 nT1 could be shown to apply, the MPSC could be
altered appropriately.
-------
155
APPENDIX A
Radiation Standards Setting Organizations
and Their Roles
The organization which recommends basic radiation cri-
teria and standards at the international level is the
International Commission on Radiological Protection (ICRP).
It was established in 1928 under the auspices of the Second
International Congress of Radiology. During the early
period and until 1950, the ICRP was concerned primarily with
recommendations designed to provide protection to members
of the medical profession in their diagnostic and thera-
peutic use of X-rays and gamma radiation from radium.
However, since the advent of atomic energy, and radiation
uses on a large scale, it has extended its efforts to include
studies of radiation protection matters covering the whole
gamut of radiation applications. It works together with its
sister commission, the International Commission on Radiation
Units Measurements (ICRU), and relies on the ICRU for back-
ground knowledge on radiation measurements.
The National Council on Radiation Protection and
Measurements (NCRP) was organized in 1929, a year after the
ICRP, as a combined effort of several radiation protection
committees in the United States to consolidate their
scattered efforts and to present a unified voice at meetings
of the ICRP.l The ICRP and NCRP are private groups whose
recommendations are purely advisory.
In 1934 the NCRP adopted the simple level of 0.1
roentgen per day, measured in air as the tolerance dose. In
1940, it recommended a permissible body burden of 0.1 micro-
gram for ingested radium. The latter standard, still in
effect today, corresponds to an average dose to the skeleton
of about 30 rem/yr or a dose to the critical endosteal tissue
out to a distance of 5-10 microns of about 10 rem/yr.
I/ Initially the NCRP was known as the Advisory Committee
on X-rays and Radium Protection; in 1946 the name was changed
to the National Committee on Radiation Protection and Measure-
ments, and in 1964 it received a Federal charter and took
its present name.
-------
156
- A2 -
In 1949, the maximum permissible dose for radiation
was lowered to 0.3 roentgen per week. It was lowered again
in 1957 to 5 rem/yr as the permissible dose for radiation
workers. This standard is still in effect.
The AEC has also played a significant role in setting
radiation standards. However, the AEC's regulatory authority
over materials was, and still is, limited by the Atomic Energy
Act of 1954, as amended, to source, by-product, and special
nuclear material. Before the Federal Radiation Council
(FRC) was formed, the AEC, when setting radiation standards,
generally followed closely the recommendations of the NCRP,
which in turn paralleled the ICRP recommendations.
In 1959, after the advent of the atomic age had aroused
public fears over fallout from nuclear weapons, the U. S.
government, because of uncertainty of government influence
over radiation protection standards, organized the FRC.
It was authorized by Congress to "...advise the President
with respect to radiation matters directly or indirectly
affecting health, including guidance for all federal agencies
in the formulation of radiation standards and in establishment
and execution of programs in cooperation with the states..."2
The final authority with respect to radiation standards rested
not with the FRC but with the President. Such a subordinate
agency as the AEC, for example, had to make its rules, e.g.,
those governing licensed reactors, compatible with the overall
guides developed by the FRC.
Tnroughout the 1950's the ICRP and NCRP continued to
revise and refine the basic recommendations concerning
permissible radiation exposure standards. Standards were
recommended for some non-occupational groups and for the whole
population. Maximum permissible body burdens and maximum
permissible concentrations of radionuclides in the air and in
water were recommended as secondary standards. Most of these
recommendations were incorporated by the FRC and the AEC.
In 1970 the FRC was abolished and its duties were transferred
to the EPA. Since that time, the setting of population
exposure standards has resided in EPA. Population standards,
2/ FRC Report No. 1, Background Material for the Development
of Radiation Protection Standards, Government Printing Office,
Washington, D. C., May 13, 1960, p. 1.
-------
-------
159
APPENDIX B
Statement Submitted to Attorneys for Mr. Edward Gleason
Re: Edward Gleason, et al vs. NUMEC
by: Arthur R. Tamplin
The following is my analysis of the origin of Mr. Edward
Gleason"s soft tissue sarcoma that ultimately resulted in his
death and of the Consultation Report, submitted by Dr. Niel
Wald, dated Jan. 29, 1973.
Mr. Gleason unloaded, rotated, and loaded a crate con-
taining a leaking carbov of plutonium-239 (Pu-239) solution.
This could not have occured without contaminating the palmar
surface of his left hand, which was bare. The question is:
did this Pu-239 contamination cause Mr. Gleason to develop a
sarcoma? Since radiation induced cancers are identical with
those that occur spontaneously, it is necessary to consider
the relative chances that the cancer was spontaneous or Pu-239
induced.
The United States Vital Statistics, record a death rate
for malignant neoplasms (other than melanoma) of the skin in
the upper extremity of less than one per million per year. Since
synovial sarcoma is a rare form that often metastasizes and
hence has a poor prognosis, its occurrence rate is certainly
less than the total skin cancer death rate of one per million
per year. Thus it is highly unlikely that anyone who handled
this crate would spontaneously develop this sarcoma on the
contaminated hand (less than one chance in a million).
Now let us consider what the chances are of the develop-
ment of cancer as a result of plutonium contamination of the
skin. Experimental data from plutonium contaminated animals
demonstrate that injection of 1 microgram of Pu-239 into the skin
of rats promptly produced cancer in up to 5% of the animals
(Exhibit 1). The particular tumors are fibrosarcomas.
Now the analysis done by LASL indicated that the Pu-239
concentration was about 160 micrograms per milliliter. This
is reason to suspect, since the volume of liquid was reduced,
the Pu was actually more concentrated in 1963. But setting that
aside, one drop would be expected to contain between 8 and
16 micrograms of Pu-239. One-one hundredth of a milliliter
(a very small amount of liquid) would have been sufficient to
-------
-------
-------
171
Introduction
The draft comments prepared by the Biophysical Society contain
a summary by Jane and Richard Setlow, the coordinators of the STAIS
Committee on the "Hot Particle Problem," followed by the individual
comments of the five committee members. The summary and individual
comments are reviewed separately below.
Summary Comments by Jane and Richard Setlow
The summary prepared by Drs. Jane and RicJhard Setlow indicates
the hot particle problem is a valid and serious one. Two of the
reviewers felt that the standards should be macde more restrictive.
There was only one reviewer who stated that there was no reason to
change the standard. Except for the latter, most reviewers felt .
that more -information was needed to establish such a standard on a
firm basis.
We agree that the available data are not adequate to firmly
establish the quantitative parameters in our hypothesis. At the
same time, we feel the available data fully support the hypothesis
qualitatively. In our report, "Radiation Standards for Hot Particles,"
we cited the ICRP and NCRP reservations relative to hot particles.
Both this report and "The Hot Particle Issue,"2 our critique of
WASH-1320, present evidence that suggests that hot particles offer
a unique carcinogenic risk. This possibility is acknowledged in
I/ Tamplin, Arthur R. and Thomas B. Cochran, "Radiation Standards
for Hot Particles," Natural Resources Defense Council, Washington,
D. C. (14 February 1974).
2/ Tamplin, Arthur R. and Thomas B. Cochran, "The Hot Particle
Issue: A Critique of WASH 1320 as it Relates to the Hot Particle
Hypothesis," Natural Resources Defense Council, Washington, D. C.,
(November 1974).
-------
172 -
the NCRP and ICRP reservations. In other words, there is evidence
that suggests that existing exposure standards are not adequate
when hot particles are involved. However, to modify these standards,
a quantitative estimate of the risk is required. That was the major
purpose of our original hot particle report. We petitioned for a
modification of the existing standards because there is a present
need to protect the workers in ~ and the public from — a rapidly
growing plutonium oxide fuel industry. If plutonium were to be
banned, like cyclamates, we could await more definitive data, but
right now it appears that the nuclear industry is going' ahead with
its plans.
In attempting to assess our assignment of quantitative values
to the .hypothesis, it is unfortunate that two of the reviewers3
attempt to set aside one hypothesis with another. This can only be
done with experimental data. Instead of focusing on whether the
available data support or contradict our hypothesis, these reviewers
proposed totally different hypotheses and estimated quantitative risks
based on these different hypotheses. Even' if we assume these alter-
nate hypotheses are developed more rigorously and are equally
plausible, they still would be only hypotheses and could not be
used to set aside ours. Our hypothesis, for which we find support
and no contradictory evidence, at present gives a higher risk per
particle than the alternate hypotheses. Confronted with different
estimates of risk from two or more hypotheses that cannot be set
aside, we feel that it would be worthwhile for the committee to
express its opinion as to the approach that should be followed in
Drs. M. L. Randolph and Arthur Cole.
-------
173
•
establishing public health standards in such situations.. Should
the public and workers assume the risk, should the substance be
banned, or should the industry be required to develop the technology
to reduce the exposure to a level suggested as prudent by the existing
but incomplete data? What principle should apply to the practice
of public health and safety in such cases?
Comments by M. L. Randolph
A. Overall Views —
We will comment on the conclusions in this section as we
review the related material in the subsequent sections.
B. Major Technical Considerations —
Page 2, 11 1: Our conviction is found in other experimental
evidence detailed in "Radiation Standards for Hot Particles" and
"The Hot Particle Issue," our critique of WASH-1320 which we have
submitted to the Biophysical Society committee. Perhaps some confu-
sion could have been avoided had we carefully delineated the exper-
imental evidence that supports the hypothesis qualitatively from the
evidence used to quantify the hypothesis in order to establish
•
radiation standards.
Page 2, last 11, beginning 1) (p. 22-26): Albert observed a
nearly constant ratio of tumors per atrophied hair.follicle in the
range (1/2000 to 1/4000). Geesaman, based on the observations of
Albert, e_t al., but allowing for a more liberal margin for error,
used somewhat larger (order of magnitude) limits of uncertainty on
the tumor risk probability, i.e., 10~3 to 10~4. since we had to
quantify this risk in order to recommend a standard, we selected
•the median between 0.001 and 0.0001, namely 0.0005, or 1/2000.
-------
174
On the next page (p. 3) Randolph states,
"I don't understand how the number of hair
follicles damaged by large area electron irradia-
tion relates to the volume irradiated by a hot
particle . . . One way to estimate the hazard
of one micron hot particle would be to assume
induction proportional to the volume irradiated."
It is clear that Randolph does not understand our (actually
Geesaman's) hypothesis qualitatively, and therefore does not appre-
ciate why the Albert experiments were used to quantify the hypothesis.
We will attempt to rephrase the basic hypothesis avoiding the use of
the term "critical architectural unit" which may be the source of
some confusion.
Qualitatively, the hypothesis is:
When a critical tissue mass is irradiated
at a sufficiently high dose, the probability . •
of tumor production is high.
A corollary to this is:
When a critical tissue mass in the lung is
irradiated by an immobile particle of sufficient . ,
alpha activity the probability of a lesion developing
approaches unity, and the probability of this lesion
developing into a tumor is high.
In order to quantify this hypothesis, we turned to the available
biological data to obtain a) the risk of tumor development once
the critical tissue structure has been altered through radiation
exposure at high doses, and b) the critical particle activity
(or local tissue dose) to significantly alter the tissue structure
(or with respect to the corollary, produce a lesion in the lung).
There is considerable experimental evidence to support the
hypothesis and the corollary qualitatively. However,the only good
biological data which quantifies a) the tumor risk per altered
tissue structure, is the Albert data. The altered tissue structure
-------
175
(or "critical architectural unit") in this case is the hair follicle,
and the probability of the tumor production once this alteration
has taken place is on the order of 1/2000. The same Albert data,
and the experiments of Laskin (see discussion on pp. 32-33 of
"Radiation Standards for Hot Particles") support the choice of
1000 rem/year to the local tissue as the quantitative value for
b) the critical particle activity. The Richmond experiments (see
our critique of WASH-1320, pp. 25-29) suggest equivocally that the
critical activity may be somewhat higher for particles in the lung.
These experiments point out one of the uncertainties in our quantifi-
cation of the hypothesis.
Randolph's statement on page 3, "one way to estimate the hazard
of a one micron hot particle would be to assume tumor induction
proportional to the volume irradiated," is a hypothesis clearly
"distinct from our hypothesis. This" "Randolph Hypothesis" is a
simplified and probably not a new variation of several tumor pro-
duction models based.on cells at risk. One hypothesis, however,
^
can not set aside another. This can only be done with experimental
data and we find no data that are inconsistent with our hypothesis.
In his second major conclusion on page 1 under "A. Overall
Views," Randolph questions the relevance of the Albert, et al.,
comments that no skin tumors were observed with protons, alpha
particles, or low energy (0.3 MeV) electrons. These observations
simply reflect the fact 'that these radiation sources did not pene- .
trate the skin sufficiently to disrupt the hair follicle.
N . •
Also, on page 1, where Randolph uses the Scottish verdict
"not proven," we would substitute "not set aside," This in turn
-------
176
raises the question: What conservative radiation protection criteria
should be adopted to protect the health of worker and the public?
We would suggest that the prudent public healtlh principle is to
accept the hot particle hypothesis, rather tham some less conserva-
tive hypothesis, and that our recommended standards provide a
reasonable basis for protection.
Page 3, beginning:
2) (p. 25-26) : These ^2p plaque experiments support our
hypothesis qualitatively, namely, a high tumor risk is observed when
a small volume of tissue is irradiated at a high dose.
3) (p. 27-28) : The Lushbaugh observation lends strong
support for the hypothesis qualitatively. While the statistics are
obviously poor, this observation is consistent with the quantitative
assignment of risk derived from the Albert data and suggests that
the hot particle tumor risk that we assigned may even be low.
4) (p. 27-28): While Mr. Gleason's case is equivocal
it is also consistent with the hypothesis qualitatively.
5) (p. 30): The work of Laskin, et al. , supports the
hypothesis qualitatively, and supports the quantitative choice of
the minimum critical particle activity as that capable of delivering
1000 rem/year to the tissue at risk (see also p. 39 of our critique
of WASH-1320 — on line 10 of page 39 "10 rads" should read 106 rads) .
Page 4, beginning:
6) (p. 31-32) : With respect to the beagle experiments
by Bair, et_ al. , we see no vjalid basis for assuming "a linear tumor
to radioactivity incidence," below 100% incidence at about 0.3 uCi
exposure. As we discuss in our hot particle report, the response
-------
-7-
177
in Hair's experiments was saturated and it is impossible to draw
any conclusions with respect to lower exposures.
7) (p. 34-37): No one knows the latent period for
carcinogenic response to hot particles in human lungs. It could be
20 to 30 years. .It is difficult, we submit, to document non-existent
information. We did point out (on p. 37 of our hot particle report)
however, that in the experiments reported by Park, et al._, the beagle
with the smallest lung burden (o.2 uCi) developed lung cancer after an
11 year latent period. The highest Rocky Flats worker exposure
(9 years ago) is comparable to the lowest beagle exposure.
8) (p. 38-40): We support the suggestion that an attempt
be made to reconstruct the Manhattan contamination experiments
(sans human lungs) in order to obtain more information about these
exposures.
C. Minor Technical Considerations.---—'- -
239
1. We find no reference to the activity of a one micron J Pu02
(or 238puo2) particle on page 7. Pu-238 has the 89 year half-life.
Langham ["The Problem of Large Area Plutonium Contamination,"0
U. S. Department of HEW, Public Health Services, Seminar Paper No.
002, Dec. 6, 1968, p. 7] lists the activity of 238pUQ2 and 239puQ2
particles as a function of particle diameter. The activity of a one
micron 238puQ2 particle is given as 8.0 X 10~2 nCi. It is not clear
whether these values are measured, or calculated. In either event,
assuming Langham's value, and 17.47 curies/gin for Pu-238, the
density of Pu-238 in a 1 u, particle of 238pUQ2 would be slightly
~s
less than 10 gm/cm3.
2. AEC and EPA regulations do include and delineate standards
-------
178
-8-
for both workers and the population. Whether they do so clearly is
arguable.
3. DF is defined in "Basic Radiation Protection Criteria,"
NCRP Report No. 39, p. 84.
4. P. 16. We stand corrected. Assuming some particles in
the lung are lodged in areas where they see essentially solid
tissue out to 45 i\ in any direction, we could have used the soft
tissue dose rate value instead of a lung model and obtained
(73 x 104) / (3 x 10~4) = 2 x 109, or more than 9 orders of magnitude.
5. The correct number is 57,000. The 53,000 was obtained
(with one too many significant digits) from (16 x 10~9) / (3 x 10~13).
6. P. 24-26. As we noted on p. 5 above, one hypothesis can
not be used to set aside another, and we find no data that conflicts
with ours.
7. The epithelial cell repair time was used in determining
the minimum hot particle activity. This is another of the
quantitative uncertainties. The discussion on pp. 25-29 of our
critique of WASH-1320 is pertinent to this issue.
8. P. 33. Both the Lushbaugh observation and the Richmond
experiments involved dose rates from particles considerably higher
than 5000 rem/year. The point is the hot particle can cause
severe but highly localized tissue disruption. It is this disrupted
tissue mass that we suggest carries a high tumor risk. Above a
certain value the total dosage is irrelevant.
9. No comment required.
10. Particle retention and movement is discussed on pp. 9-12
of WASH-1320. On p. 20 of our critique of WASH-1320 we note that
-------
-9-
179
while plutonium particles in the lower respiratory region are not
static, auto-radiographic evidence demonstrates that such particles
are immobilized in scar tissue and possibly in Type I alveolar
epithelial cells. The long residence time of plutonium particles in
the lung suggests that such immobilization must occur.
D. Appendix. Tentative Estimate of Maximum Permissible Lung
Burden —
Here, Randolph makes a first cut at quantifying a hypothesis
based on tumor risk as a function of dose averaged over the entire
lung. Referring again back to page 5, one hypothesis can not be
used to set aside another hypothesis. We see no data that contra-
dicts our hypothesis. It is interesting to note, however, the
quantitative results of Randolph's hypothesis are extremely sensi-
tive to differences in specific activity (238Pu vs. 239Pu). In
this regard, had Randolph (at the top of p. 6) noted that a one
micron 238pUQ2 particle gives a dose of 7 x 10~3 rad/year (instead
of 2.7 x 10~5 for 239pu02), ne would have obtained 2.5 particles
versus our 2 particles, instead of 600. - :
i
Comments by Louis Hempelmann
Most of the points raised by Hempelmann are discussed in
"The Hot Particle Issue," our critique of WASH-1320. .
We had no intention of being misleading, nor do we feel that
we were so in the three instances cited by Hempelmann.
x
1.- Our report, "Radiation Standards for Hot Particles," was
issued on February 14, 1974. We had no way of knowing that in
-------
-10-
November, Bair would author the WASH-1320 report. Moreover, our <
critique of WASH-1320 indicated that the conclusions reached in
WASH-1320 are not justified so far as hot particles are concerned.
2. We stated in our hot particle report that the Gleason case
was not clear cut. In Appendix B of that report we included the.
basis for the conclusion that the strong possibility that Gleason's
cancer was caused by plutonium. We see no sound reason for con-
cluding that several days after the incident, Mr. Gleason would
surely remember having had a sliver puncture in his hand. This would
not have had to be a gaping wound as Hempelmann seems to imply.
3. The discussion of the lesion excised by Lushbaugh and
Langham indicates that the plutonium particle produced a lesion that
was highly suggestive of an incipient carcinogenic response to a
single plutonium particle imbedded in soft tissue.
Concerning the assumptions that Hempelmann can not agree with
or understand:
1..and 2. The purpose of our report was to develop radiation
protection standards for hot particles. To do this it is essential
to develop quantitative risk estimates. This work of Albert supplied
the only available data on the risk of tumor development as a func-
tion of a disordered tissue mass. Rather than make a completely
arbitrary assumption concerning the risk per particle we chose the
value derived from this biological observation. We pointed out in our
critique of WASH-1320 (see pp. 10 and 25-29) that these quantitative
values are uncertain. At ^the same time, it is impossible to set
standards without quantitative values.
So far as the architectural structure goes, the lesion of
Lushbaugh and Langham and the lesions observed around microspheres
-------
-11-
181
in the lungs of rats and hamsters (see our critique of WASH-1320,
i
pp. 10 and 25-29) suggest that particles placed at random in
tissue are capable of inducing a lesion with neoplastic changes
similar to precancerous cytological changes.
3. We feel'that our discussion of the Rocky Flats workers is
valid. It is possible that, if the sample size were as large as
the number of exposed uranium miners, some cancers would have
appeared already.
4. As we indicated in our hot particle report, the nature of
the contaminating events at Los Alamos were described in an article
by Hempelmann. The particles (droplets) were aspirated from
solutions. As a consequence for the range of concentrations given
by Hempelmann the particle size would have had to exceed 5 u, in
diameter for the most concentrated solution in order to constitute
hot particles. The so-called sophisticated calculations of Anderson
relate to particles above 0.6 u. in diameter or a factor of 10
smaller. The reconstruction of these contaminating events, the
measurements of the particle size and activity, and the behavior of
the inhaled fraction in animals would be a worthwhile experiment.
We have discussed this "good experimental evidence" in our
critique of WASH-1320 and have shown this evidence to be either
irrelevant to the hot particle hypothesis or supportive of it on
the following pages of our critique:
1. Pages 23-25. This experiment was similar to those of Albert
wherein the beads corresponded to his sieve patterns.
2. Pages 29-30. These did not involve hot particles.
3. Pages 10 and 25-29. These experiments are supportive.
-------
182 -12-
4. Pages 30-31. Specifically the BaS04 did not involve hot
particles and induced few tumors. The Sr-90 beads (one per animal)
induced 7 malignancies in 23 rats. While the dose from the beads
(0.3 mm in diameter, 244 nCi) was from a localized source, it
irradiated the entire lung. Nevertheless, if one chooses to call
these hot particles, the cancer risk was about 1/3 instead of
1/2000 per particle as we propose.
Comments by Andrew M. Rauth
Page 1, 11 2: This discussion presents an inadequate synopsis
of our report. The discussion under "B. Modifying Factors"
(beginning p. 13) in "Radiation Standards for Hot Particles," was
meant to serve as background information, namely, a review of basic.
definitions of radiation dose and factors used to calculate dose.
In subsequent sections of the report..we estimate a risk per hot
particle and the critical particle activity (p. 32). We then
recommended radiation standards in terms of hot particle lung
burdens which were comparable in risk to the uniform whole body
exposure. It is not necessary to go back and calculate what this
implies in terms of the Distribution Factor (DF). Calculating the
DP is simply an interesting academic exercise. Note that the factor
of 115,000 assumes the lung burden consists of hot particles of
minimum activity. The DF would be. smaller for hot particles with
higher activities. Clearly, the concept of DF is not particularly
useful if the risk is defined on a per particle, rather than a per
/
microcurie (or per unit dose) basis. '
It is inappropriate to say the "DF is based primarily on the '
two experimental pieces of information, the work of Albert and
-------
-13-
183
coworkers cited on pages 22-24 on electron irradiation of rat skin
and the work of Bair on Pu239Q2." The basic qualitative support
for the hot particle hypothesis derives from a number of experiments
wherein small volumes of tissue have been exposed to high doses and
where cancer was> the almost inevitable .result* The experiments by
Albert and Bair (and their coworkers) are but -two of many such
experiments. On the other hand, the quantitative parameters in our
hypothesis (as summarized on p. 5 of our critique of WASH-1320) are
derived from the Albert experiments but not ttoose by Bair. The
quantitative parameters we assigned are supported by other experimental
observations, e.g., Laskin, et al., (Reference 56 in our report),
Lushbaugh's observation (pp. 27-28 in our repo;rt) , and the experiments
of Richmond, e_t al. , (pp. 25-29 in our critiqute of WASH-1320) .
1 3: It is stated that:
"The authors [Tamplin and Cochran] nuake no comments
on the Albert data on the facts that
1) This is a microscopic tissue irradiation
(24 cm2) in a single acute dose.
.2) Not only does the tumor incidence go up at
1000 rads, but it also goes down at doses.; above
2000 rads."
First, it is important to recognize that out O'.f necessity most
radiation standards are based on results from acute, as opposed to
chronic, exposures. Concerning the second poi.nt, at doses above
2000 rads, one is undoubtedly witnessing one o-r more competing
mechanisms. As one moves to higher doses the
-------
-14-
184
can produce this local tissue disruption without being tissue
fatal.
The remainder of this paragraph through the first full para-
graph on page 2 contains observations with which we agree. We do
not share, however, Rauth's conclusions, drawn from what he admits
are "superficial considerations."
Comments by Arthur Cole
Concerning Cole's specific points:
"P. 26. The 'critical architectural unit" is
an attractive and simplified hypothesis. However,
little evidence is available to support it."
We would suggest there is ample evidence to support this
hypothesis qualitatively, although there is much less experimental
data from which the hypothesis can be quantified. As demonstrated
in our critique of WASH-1320, most of what has been offered as
conflicting evidence is not relevant to the hot particle issue.
The relevant data support the hypothesis.
"P. 27-28. The Lushbaugh study of one
observed lesion in 1000 puncture wounds provides
no statistical basis for estimating a tumor
induction probability."
Our ho't particle risk estimate was derived from the Albert data.
The Lushbaugh observation is consistent with this risk estimate of
one tumor per 2000 hot particles. This causal observation by
Lushbaugh would suggest that if a comprehensive search had been
undertaken other lesions may have been found. While the observed
lesion had not progressed into a tumor, the concern that it might
was sufficient to have it excised.
"P. 41. Section VII ..."
-------
185
Cole offers two alternative models for estimating the hot
particle risk, the first based on Albert's data and the second
based on Bair's data. As we have stated previously one hypothesis
can not be used to set aside another. This can only be done with
experimental data.
It is perhaps worth noting that Cole's first model is similar to
the concept of prescribing a significant volume or significant
area following NCRP criteria [NCRP Report No. 39, Criteria 206 and 207],
as discussed in our critique of WASH-1320 (p. 6) .
With respect to the second model Bair's data are not useful
for quantifying the hot particle tumor risk, other than establishing
a lower limit on the risk per hot particle in the range of 10~6
to 10~7. Cole assumed "a reasonable large probability (approaching
unity) would still occur for only 106 hot particles per dog . . .".
Cole could have assumed 105, 10^ . ".and calculated a higher risk.
We share Cole's opinion that on the basis of Bair's data alone, the
permissible exposure.levels should be lowered.
3
Concerning Cole's final comments, while more experimental work
is needed, we submit that our more restrictive standards should be
quickly promulgated because it is irresponsible to leave the health
of the public and workers in jeopardy while awaiting more
definitive data.
Comments by Doris J. Dugas
We are in essential agreement with most of Dugas1 comments here.
However, they exemplify an approach to this problem that we find
quite frustrating, as we discussed in our summary remarks.
Standards are required to protect workers and the public from
-------
186
Plutonium exposure. To adopt standards, a quantitative estimate of
the risk is required. In the absence of complete data, this risk
assessment must be made on the basis of available data.
The only biological observations that we were able to find that
allowed an estimate of the risk of cancer given a disrupted tissue
mass was the rat skin data. Granted this is uncertain, what is
a better value? If the use of plutonium were to be banned pending
more definitive data, the public and workers would be protected.
But this is apparently not the case. So we selected this approach
to quantification because it was an observed biological relationship.
As we stated in the summary comments, it would be worthwhile for the
committee to propose their approach to this dilemma.
With respect to Dugas1 comments on Section V-A, p. 22, the above
comments would apply. Moreover, the lesion excised by Lushbaugh and
Langhara and the lesions and cellular changes observed around micro-
spheres in the lungs of rats suggest that any tissue mass may be the
equivalent of a critical volume when hot particles are involved.
(See our critique of WASH-1320, pp. 9-10 and 25-29).
The above is also relevant to Dugas1 comments on V-B, p. 26 and
V-C, p. 29.
As Dugas indicates, VI, p. 32, the epithelial repair time is
used to determine the hot particle minimum activity. This is one of
the quantitative uncertainties. Our discussion on pages 25-29 of the
WASH-1320 critique are pertinent to this issue. If the epithelial
turnover time is shorter, the particle activity should be higher.
With respect to,Dugas' comments on VI-A, p. 42, the lung seems to
be the organ at risk, not the lymph nodes. Although the lymph nodes
-------
I. INTRODUCTION j g -.
On February 14, 1974, the Natural Resources Defense Council
(NRDC) petitioned the Atomic Energy Commission (AEC) and the
Environmental Protection Agency (EPA) to amend their radiation
protection standards applicable to "hot particles" of plutonium
and other actinides where hot particles were defined more fully
in an accompanying report. The report (referred to herein as
the Hot Particles Report) concluded that the existing radiation
protection standards are grossly inadequate to protect workers
and the public from the high cancer risk posed by exposure to
the atmospheric release of plutonium particulates from the nuclear
power and weapons industries. The report recommended (and the
petition requested) that the current standards be made more
restrictive by a factor of 115,000 where hot particles are concerned.
In the petition NRDC indicated that matters of importance to the
public health and safety such as this require prompt action. Allow-
ing a reasonable period for public comment NRDC recommended that the
proposed standards be set within six months (by August 14, 1974).
We have requested that EPA hold adjudicatory type hearings on
0 — *5
this matter so that the issues could be properly joined.^ J Instead
EPA held these hearings with a panel format that developed a record
which tends to obfuscate the issues. In the first place it is
apparent from the transcript of the hearings on December 10 (pages
1-142 to 1-144) that certain members of the hearing panel were not
informed as to the purpose of the hearings as detailed in the Federal
Register. Moreover, so far as the hot particle issue is concerned,
-/Tamplin, A. R. and T. B. Cochran, "Radiation Standards for Hot
Particles," Natural Resources Defense Council, Washington, D.C.,
14 February, 1974.
2/
- Letter from J. G. Speth to Dr. William D. Rowe, dated July 19, 1974
I/
Letter from J. G. Speth to Dr. William D. Rowe, dated August 19,
1974.
-------
192
it is evident from the transcript of the hearings of December
10 (pages 1-148 and 1-149) that the EPA had not ascertained
that all members of the panel were prepared to discuss this issue.
All of the material which we submitted to the AEC as well as
the material prepared by the AEC was available to EPA and should
have been reviewed by the panel prior to the hearings. In short,
we feel these hearings have only served to reenforce the need for
the adjudicatory hearing which we requested.
The purpose of this report is to clarify the issues related
to the hot particle problem which the hearing record tends to
confuse. We shall first discuss the qualitative aspects of hot
particle hypothesis and then its quantitative aspects. This will
be followed by a discussion of the points raised by Dr. Edward P.
Radford, Jr. during the hearings. These discussions
will demonstrate that no information capable of rejecting the hot
particle hypothesis was presented in the course of the EPA hearing.
In fact, together with the hot particle hazard, the recommendations
of Dr. Karl Z. Morgan based on a different approach indicate that
overall the transuranic standards should be made substantially more
restrictive.
II. The Hot Particle Hypothesis
The "hot particle hypothesis" is relatively simple.
Qualitatively, the hypothesis is:
When a critical tissue mass is irradiated
at a sufficiently high dose, the probability
of tumor production is high.
A corollary to this is:
When a critical tissue mass in the lung is
irradiated by an immobile particle of sufficient
alpha activity the probability of a lesion develop-
ing approaches unity, and the probability of this
lesion developing into a tumor is high.
-------
193
-3-
In order to quantify this hypothesis, we turned to the available
biological data to obtain a) the risk of tumor development once
the critical tissue structure has been altered through radiation
exposure at high doses, and b) the critical particle activity
(or local tissue dose) to significantly alter the tissue structure
(or with respect to the corollary, produce a lesion in the lung).
In the Hot Particle Report, with respect to alpha-emitting
particles in the lung, the hypothesis was quantified on the basis
of the available biological data:
If a particle deposited in the deep respiratory
tissue is of such activity as to expose the
surrounding lung tissue to a dose of a± least
1000 rem in 1 year, this particle represents a
unique carcinogenic risk. The biological data
suggest that such a particle may have a cancer
risk equal to 1/2000.
This hypothesis implies that if a particle exposes the sur-
rounding lung tissue to a dosage greater than 1000 rem in 1 year,
the cancer risk is still 1/2000. (This, of course, causes a large
particle to be less effective on a per pCi basis, but not on a per
particle basis.) The hypothesis implies nothing about particles
that expose the tissue to less than 1000 rem in one year.
In the Hot Particle Report we indicated that much of the
basic support for the hypothesis derives from a number of experi-
ments wherein in a small volume of tissue was exposed to high
dosage. In these experiments cancer was a frequent, almost
inevitable, result. One series of experiments that was discussed
-------
-4-
194
in some detail were those conducted by Dr. Roy C. Albert on
rat skin. ~ In these experiments, Dr. Albert observed that
the radiation induced cancers were remarkably correlated with
the disruption of an architectural unit of the skin, the hair
follicle. The cancers were induced in the rough proportion of
1 cancer per 2000 atrophied hair follicles when the dosages
exceeded some 1000 rem.
The hot particle hypothesis thus suggests that if these
skin experiments were performed with small particles, each cap-
able of disrupting a single hair follicle, the observed cancer
induction would correspond to one cancer per 2000 particles.
A< Qualitative Aspects
In the Hot Particle Report we indicated that there was
qualitative support for the hypothesis in terms of two experi-
mental observations related to hot particles embedded in tissue.
Since publication of the Hot Particle Report an additional report
on hot particles in hamster lungs has been published. We shall
discuss each in turn.
The potential hazard of a single hot particle embedded in
human tissue is illustrated by the observation of Lushbaugh
v
Albert, R. E., F. J. Burns, and R. D. Heimbach, "The effect of
penetration depth of electron radiation on skin tumor formation in
the rat," Radiation Res. 30, 1967, pp. 515-524.
5/
Albert, R. E., F. J. Burns, and R. D. Heimbach, "Skin damage and
tumor formation from grid and sieve patterns of electron and beta
radiation in the rat," Radiation Res. 30, 1967, pp. 525-540.
i/
Albert, R. E., F. J. Burns, and R. D. Heimbach, "The association
between chronic radiation damage of the hair follicles and tumor
formation in. the rat," Radiation Res. 30, 1967, pp. 590-599.
-------
195
and Langham.7 They excised a nodule that developed around a
Pu-239 particle imbedded in the palm of a machinist. Commenting
on the histological examination of the lesion, the authors state:
The autoradiographs showed precise confinement of
alpha-tracks to the area of maximum damage and their
penetration into the basal areas of the epidermis,
where epithelial changes typical of ionizing radia-
tion exposure were present. The cause and effect
relationship of these findings, therefore, seemed
obvious. Although the lesion was minute, the changes
in it were severe. Their similarity to known pre-
cancerous epidermal cytologic changes, of course,
raised the question of the ultimate fate of such a
lesion should it be allowed to exist without surgical
intervention ....
Considering the above observations, it would be surprising indeed
if a physician would not suggest surgical intervention in a case
where a patient had a few such imbedded particles. We feel that
this lesion alone should cause one to be very cautious in estimat-
ing the hazard of hot particles.
That such lesions can develop in lung tissue is supported by
the observations of Richmond, e_t al. , on the lesions induced in
experiments wherein hot particles were introduced into blood
vessels of the lungs of rats:
Such a lesion with collagenous degeneration and
subsequent liquefaction, due to the large local dose
of radiation at a high dose rate, has been reported
by Lushbaugh e_t al. , whose description of a plutonium
lesion found Tn the dermis is very similar to that
observed for plutonium in the lung.
y
Lushbaugh, C. C. and J. Langham, "A dermal lesion from implanted
plutonium," Archives of Dermatology 86, October 1962, pp. 121-124.
i/
Ibid., p. 462.
I/
Richmond, C. R., et al., "Biological response to small discrete
highly radioactive sources," Health Physics 18, 1970, p. 406.
-------
196
Richmond and co-workers continued these experiments with
hamsters and the following appears in their latest progress
report (Particular attention is drawn to the last sentence) :
Most of the animals placed on study early in the
program have reached the end of their normal life
span without developing significant pulmonary lesions.
During the past few months, we have observed some
histological changes in the lungs of very long-term
animals (15-20 months). In these animals, an extension
of bronchiolar epithelium into the alveolar ducts .and
alveoli has occurred. In some cases, the alveoli are
lined with cubiodal or columnar epithelial cells
(Fig. 1) . This lesion has been observed almost entirely
in the higher activity levels (levels 4-6) and in ani-
mals given relatively small numbers of spheres
(2000-6000) . An interesting recent observation has
been given larger numbers of spheres of approximately
60,000. This group of animals has been exposed only
about 6 months. A consistent observation of this lesion
after drastically different induction times could lead
to speculation that the amount of tissue irradiated is
an important element in timing of the tumorigenic response.
There has been no increase in frank tumors observed within
the past year; however, the epithelial changes described
above could be considered as precursors of peripheral
adenomas . ^-0
The particle activity in these hamster experiments was con-
siderably lower than that associated with the excised palmar
lesion and the lesions in the rat experiments. The particle
activity from the excised palmar lesion was 5 nCi and those in the
rats experiment were 40 nCi and greater. The level 4 particles
in the hamster experiment contained only 4.3 pCi and level 6 con-
tained 60 pCi. The initial lesions observed surrounding these
lower activity particles were called granulomas measuring
10/
Richmond, p. R. and Sullivan, E. M., (eds.), Annual Report
of the Biomedical and Environmental Research Program of the LASL
Health Division for 1973, Los Alamos Scientific Laboratory Report
LA-5633-PR, May 1974, p.7.
-------
-7-
197
200-500*1 in diameter (about the same size as the excised palmar
lesion).
It is of importance to compare the description of the lesion
in the hamsters wherein there is an extension of the bronchiolar
epithelium into the alveoli. This is a suggested mechanism for
12
the histogenesis of bronchiolo-alveolar carcinomas. Moreover,
the description of the hamster lesions indicated that, in some
cases, the alveoli are lined with cubiodal or columnar epithelial
cells. Such lining cells are a histological feature of bronchiolo-
alveolar carcinoma. •* We see no reason for being complacent
about these lesions.
These experiments strongly support the proposal that a single
particle embedded in tissue is capable of eliciting a carcinogenic
response. The killing of cells and the development of a lesion sur-
rounding the particle is the suggested mechanism of carcinogenesis
(an injury mediated mechanism). It appears reasonable to propose
that the mechanism is similar to that involved in the experiments
of Brues et al, wherein sarcomas developed in the fibrous capsule
that forms adjacent to a film of plastic and other inert materials,
several months after they were implanted subcutaneous in rodents.
ii/
Richmond, C. R. and Voelz, G. L.,(eds.), Annual Report of the
Biomedical and Environmental Research Program of the LASL Health
Division for 1971, Los Alamos Scientific Laboratory Report,
LA-4923-PR, April 1972, p. 31.
ii/
Evans, Winston R., Histological Appearance of Tumors, Second
Edition, Williams and Wilkins Company, Baltimore, Maryland, 1966,
pp. 1112-1113.
IV
Ibid, p. 1111.
li/
Brues, A. M., Auerbach, H., De Roche, G.M., and Brube, D.,
"Mechanisms of carcinogenesis," Argonne National Laboratory,
Biological and Medical Research Division Annual Report for 1967,
ANL-7409, 1967, pp. 151-155.
-------
-8-
198
The association of lung tumor with peripherally situated scars
is discussed in cancer textbooks:
It is known, for example, that scars in lung
tissue marking injuries received years before
increase susceptibility of the involved cells
to cancer development.15
It is reasonable to propose that these lesions disrupt the local
tissue architecture and thereby interfere with the normal bio-
chemical and physical communication between the cells that control
processes such as contact inhibition which are responsible for
maintaining tissue stability. They thus create an area with an
increased cancer risk.
While we have here stressed the formation of the lesion
surrounding the hot particle, it is important to recognize .that
many of the cells on the periphery of the lesion are the progeny
of cells that received radiation damage during the forma-
tion of the lesion. This is implied in the Lushbaugh and Langham
quotation on page 5 above. This added effect of radiation damage
will be of particular importance for reactor fuels. In this case,
the plutonium will be contaminated with beta emitting isotopes that,
because of the longer range of beta particles in tissue, will sub-
ject the cells surrounding the lesion to appreciable radiation dosage.
Although no tumors appeared in association with the micro-
spheres in the animal experiments, the description of the lesions
is suggestive of an incipient tumorogenic response. Richmond, et
a_l, state that they could be considered as precursors of peripheral
adenomas and their description is consistent with that of developing
15/
Cowdry, E. V., Etiology and Prevention Of Cancer In Man,
Appleton-Century-Crofts, New York, N.Y., 1968, p. 137.
-------
~~ 199
bronchiole-alveolar carcinoma. It is reasonable to propose
that the induction period for a frank tumor by this
mechanism is longer than the life span of rats and hamsters. We
submit that the lesions observed around these particles are suf-
ficient to indicate that radiation protection standards should
limit the exposure of human lungs to very few hot particles.
B. Quantitative Aspects
The hot particle hypothesis as presented above
contains two quantitative parameters. The first is the risk of
cancer associated with a particle produced lesion and the second
is the particle activity that constitutes a hot particle capable
of producing such a lesion. We shall discuss each in turn.
1. Cancer risk per particle produced lesion
In our Hot Particle Report we assumed a cancer risk of
1/2,000 per particle produced lesion. This value was derived
from the tumor risk per atrophied hair follicle in the experiments
of Albert, et aJL. (see page 4 ) . To our knowledge this is the only
biological data that quantitatively relates the radiation induced
disruption of a tissue mass to cancer production. As we indicated
in our Hot Particle Report, this risk estimate is not necessarily
conservative. One could argue that the descriptions of the particle
produced lesion cited above suggest a greater risk. We can see
no justification for assignment of a lower risk. While we have
been criticized for using rat skin data to estimate the risk in
human lungs, we have not seen any suggestion for a better approach
that is based upon available biological data.
:niti.-i-: :
-------
-10-
200
2. The hot particle activity
In our original Hot Particle Report we selected 1,000
rem/year as the local tissue dose for setting the minimum activity
for a hot particle. The 1,000 rem was derived from the experi-
ments of Albert, et al, and Laskin, et al., wherein 1,000 rem
was the lowest dosage associated with a carcinogenic response. The
one year was based upon the apparent epithelial cell turnover
time in the lung. This method of defining the minimum activity
for a hot particle carried considerable uncertainty and was so
criticized.
Since the publication of the Hot Particle Report, three
reports have appeared which present experimental data
that allow a more direct determination of the minimum particle
activity without resorting to tissue dosage or turnover time.
We shall discuss these reports beginning with the one
that suggests the largest limiting particle activity and ending
with the smallest.
a. Richmond and Sullivan*6 This report is the latest
progress report on the microsphere experiments with hamsters
at LASL. As the quotation on page 6 above indicates, lesions
were observed almost entirely in the activity levels 4 and
above. The particles in level 4 contained 4.3 pCi/particle.
It is also indicated that lesions were observed in association
with particles from level 3 (0.9 pCi/particle). However, this
occurred in animals given 60,000 spheres and the lesions may
have been associated with clumping on aggregates of particles.
16/ Richmond, E. R. and Sullivan, E. M., pp. cit.
-------
-11-
201
This experiment thus suggests a range for the limiting activity
of 0.9 - 4.3 pCi/particle with the lower limit somewhat tentative.
These experiments, at this time, represent the only
direct observation of particle produced lesion and serve to
establish the upper limit for the minimum particle activity.
Had the life span of the animals been longer, it is quite possible
that lesionswould have developed around particles of lower activity
Thus, the minimum particle activity is most likely below 4.3
pCi/particles. This 4.3 pCi represents a 60 fold increase in
the minimum particle activity relative to the 0.07 pCi (based on
1000 rem/year to beal tissue) adopted in the Hot Particle Report.
Nevertheless, a 60 fold increase in activity requires
only a 4 fold increase in particle diameter—for Pu-239, a
change from 0.6 u to 2.4 u; for Pu-238, a change from 0.09 p
to 0.36 n and for high burn-up nuclear fuel, a change from
0.4 p. to 1.6 ju. These particles are still in the range that
permits deposition in the lower respiratory zone. In other
words, even when using this upper limit value, the nuclear
industry has a potential hot particle problem.
b. Mclnroy, et al.17 This report presents a particle size
analysis of plutonium particles in a tracheobronchial lymph
node of a Los Alamos plutonium worker. Another study of human
respiratory exposure to plutonium relates to 25 workers exposed
to plutonium at Los Alamos during the Manhattan Project.18 The
IT/ Mclnroy, James F., et_ a_l. , "Studies of Plutonium in
Human Tracheobronchial Lymph Nodes," Los Alamos Scientific
Laboratory Preprint, LA-UR-741454, 1974.
IB/ Hempleinann, L. H. , et al, "Manhattan Project Plutonium
Workers; A Twenty-Seven Year Fo.llow-Up Study of Selected Cases,"
Health Physics, Vol. 25, Nov. 1973, pp. 461-479.
-------
292
""' latest examination of this group found, them to be free of
lung cancer although the report states, "The bronchial cells
of several subjects showed moderate to marked metaplastic
changes, but the significance of these changes is not clear."
If these 25 workers combined retained a total of 2,000 hot
particles then the chance of none of them developing lung
cancer would be about 0.3 (assuming a tumor risk per particle
of 1/2,000). Thus, the particle size distribution given by
Mclnroy, et al., can be used to obtain a limiting particle
size that would correspond to some 2,000 hot particles retained
in the 25 workers.
Healy, et al., estimates that, the initial burden in
these workers was about 10 pCi.1^ Table I presents the
particle size distribution given by Mclnroy, et al., wherein
the incremental activity in a size range was determined by
multiplying the incremental activity fraction by the total
activity (10y pCi). The particle number was then obtained
by dividing the incremental activity by the activity per
particle.
Inspection of Table I indicates that for these workers
to contain only 2,000 particles a minimum activity somewhat
larger than 0.8 pCi/particle is required. There is considerable
uncertainty attached to this estimate (see discussion in Letter
to Mr. Robert B. Minoque attached as Appendix A to this
submission). For one thing the autoradiographic sizing technique
tends to overestimate the large particle fraction and hence,
19/ Healy, I. W., et al., "A Review of the Natural Resources
Defense Council Petition Concerning Limits for Insoluble Alpha
Emitters," Los Alamo:; Scientific Laboratory Report, LA-5810-MS.
Nov. 1974, p.15.
-------
-13-
203
TABLE I
Estimated Particle Size Distribution For
The Manhattan Project^ Workers
(Assumes a total lung burden of 10 pCi for the 25 workers)
Diameter .
Particle
u
<0.1
0.
0.
0.
0.
0.
1.
} _l_ t
1 -
3 -
5 -
7 -
9 -
1 -
.3
0.
0.
0.
0.
1.
1.
Incremental
Activity Fraction
3
5
7
9
1
3
0
0
0
0
0
0
0
0
.12
.58
.23
.056
.011
.002
.0009
.0001
Incremental
Activity
1.2X10
5.8X10
2.3X10
5.6X10
1.1X10
6
c.
\J
6
5
5
2X1 04
9X10
1X10
3
3
gCi/p article
-4
3X10
-3
9X10
4.1X10"2
-1
1.1X10
-1
2.4X10
4.3X10~1
7X10"1
)>1.0
Number
of particle:
6
5
4
4
1
<
4X10
.4X10
.6X10
5X10
.7X10
.7X10
.3X10
3
; ioj
9
8
7
6
5
4
4
-------
204
the limiting activity. Another is that this lymph node particle
size distribution may not adequately represent the lung burden
of the individual from which it was obtained. In this regard, the
exposure of this Los Alamos worker may not be representative
of the 25 Manhattan Workers. An examination of the corresponding
lung tissue is underway and this may be quite helpful. (See
letter from Mclnroy to Cochran attached as Appendix B to this
submission). Finally, assuming it is inappropriate to apply
this distribution to the Manhattan Workers and instead applying
it only to the individual from which it was obtained (see Appendix
A) leads to a minimum activity to constitute a hot particle of
0.14 pCi/particle.
-------
-14" 205
c. Rocky Flats Fire?0 The approach used above can also be
applied to the individuals contaminated during the October
1965 , fire at Rocky Flats. This will again give an upper
estimate of the minimum activity since, as we discussed in
the Hot Particle Report, lung cancer may develop in these
individuals over the next 15 or so years.
Mann and Kirchner report that the MMD for the particles
21
in this incident was 0.32 u with a standard deviation of 1.83.
The data they present indicates that the combined lung burden
r 22
of 25 exposed workers was 1.2 X 10° pCi. Table II was con-
structed using these data and the same approach as used above
for the Manhattan Workers.
Inspection of Table II indicates that for the Rocky Flats
Workers to contain only 2,000 hot particles, the minimum
activity to constitute a hot particle would have to be some 1.6
pCi/particle. If, however, the minimum particle activity were
only 1 pCi/particle, Table II would suggest that around 3 lung
cancers could be anticipated in the next 15 or so years (using a
risk per particle of 1/2,000).
20/ Mann, J. R. and A. R. Kirchner, "Evaluation of Lung Burden
Following Acute Inhalation of Highly Insoluble PuOp," Health
Physics, Vol. 13, 1967, pp. 877-882.
21/ Ibid, p. 881.
22/ Ibid, p. 880. (When a range in lung burdens was given,
we used the midpoint)
-------
-15-
206
'TABLE II
•Estimated Particle Size Distribution For
The Rocky Flats Workers
(Uses a total lung burden of 1.2 X 106 pCi)
Diameter Incremental Incremental Number of
u Activity Fraction Activi t-.v tr>ri ^ nr-i/P^T--)--; ^i ,= D=V.I--; ~-i ~~
0.6 -
0.7 -
0.8 -
0.9 -
1.0 -
1.2 -
1.4 -
1.6 -
1.8 -
0.7
0.8
0.9
1.0
1.2
1.4
1.6
1.8
2.0
0.05
0.033
0.022
0.017
0.014
0.007
0.004
0.0016
0.001
6.0X104
4.0X104
2.6xi04
2.0X104
1.7X104
8.4X103
4.8X103
1.9X103
1.2X103
0.09
0.14
0.20
0.28
0.44
0.72
1.15
1.62
2.24
*. «— j- v-*. j_ ^ -t1^* j_ t; o
6.7X105
2.9X105
1.3X105
7.1X104
3.9X104
1.2X104
4.2X103
1.2X103
5.4X102
-------
207
This possibility cannot be ruled out at the present time.
d. Sanders and Dagle23 This report presents preliminary results
of a continuation of experiments wherein Sanders induced a large
incidence of lung cancer in rats following exposure to low doses
of soluble Pu-238. Of particular interest in these new experi-
ments are three exposure groups involving insoluble particles in
which no lung cancers have appeared. One of these groups was
exposed to 238Pu02 and we shall analyze it because it will be
the most critical with respect to particle size and activity.
There were 60 rats in this group who were exposed to an
average of 160 pCi of 238Pu02 as measured one day after inhala-
tion of particles with a CMD ranging between 0.1 and 0.3 u.
The report indicates that 23 of the 60 rats have died so far
with no evidence of lung cancer (571 days past exposure).
We shall use the midpoint of the CMD range. A CMD of
0.2 ]U corresponds to a MMD of 0.3 u. The distribution of
particle sizes about the median was not given. We shall there-
fore arbitrarily assume the particle size distribution obtained
at Rocky Flats (MMD = 0.32 p, c"= 1.83) . Table III presents
the particle distribution on this basis for a total exposure
of 9,600 pCi to the 60 rats.
Inspection of Table III suggests that we can draw no
inferences from this experiment at this time. Above 0.1 ju.
there are only 5,000 particles leading to an expectation of
only 2 cancers (assuming a risk of 1/2,000 per particle). If
no cancers appear this experiment, this would only suggest a,
minimum particle activity of around 0.6 pCi/particle. We say
23/ Sanders, C. L., and G. E. Dagle, "Studies of Pulmonary
Carcinogenesis In Rodents Following Inhalation of Transuvanic
Compounds, Pacific Northwest Laboratories, Biology Dept., Preprint
-------
-I/-
208
TABLE III
Estimated Particle Size Distribution For
Rats Exposed to 238PuO2
(Total exposure for 60 rats = 9,600 pCi)
Particle
.Diameter Incremental Incremental
u Activity Fraction ActivJtv (pr-i
CO.
0.
0.
0.
0.
0.
0.
1
1 -
2 —
3 -
4 -
5 -
6 -
0
0
0
0
0
0
.2
.3
.4
.5
.6
.7
0
0
0
0
0
0
0
.02
.20
.24
.18
.12
.09
.05
192
1,920
2,300
1,730
1,150
865
480
) pCi/Partic
0.08
0.64
2.2
5.1
10
18
28
Number of
:le Particles
2,400
3,000
1,060
340
115
48
17
-------
209
only suggests because with only 5,000 particles the chance of
no cancers appearing would be 0.08 which is not generally con-
sidered statistically significant. Furthermore, as stated above,
the particle size distribution is unknown and must be assumed
somewhat arbitrarily.
Table IV presents a similar analysis for a group of
60 rats exposed to 12,000 pCi of 239Pu02. Inspection of
Table IV indicates that if no tumors appear in this group, it
would be suggestive of a minimum particle activity of 0.14 pCi./
particle (assuming a risk of 1/2,000 per particle).
It must be recognized that the above analysis is quite
tentative not only because the particle size distribution is
speculative, but also because more than half of the rats were
still living when these interim results were reported. Moreover,
as with the hamsters, the life span of the rats may compromise
the induction period for hot particle mediated carcenogenesis.
Minimum hot particle activity. We are now in a position
to summarize estimates of the minimum hot particle activity. As
stated earlier, our initial definition of the minimum hot particle
activity was based upon the dose to surrounding tissue which was
quite uncertain. The experimental results above allow assessment
of this parameter without resort to dose calculations. These
observations and analysis lead to the following estimates of
the minimum activities:
Minimum Activity
pCi/particle Experimental Basis
0.9 - 4.J Observation of particle produced lesions
1.6 Rocky Flats Workers
0.8 Manhattan Workers
0.6 238PuO2 in rats
0.14 239PuC>2 in rats and (in Appendix) from
lymph node
0.07 1,000 rem/year
-------
-19-
210
TABLE IV
Estimated Particle Size Distribution For
Rats Exposed To 239puO2 (Total exposure
For 60 rats = 12,000 pCi)
Particle
Diameter
F
0.6-0.7
0.7-0.8
0.8-0.9
0.9-1.0
1.0-1.2
1.2-1.4
1.4-1.6
Incremental Incremental
Activity Fraction Activity (pCi)
600
395
263
204
163
84
48
pCi/particle
0.09
0.14
0.20
0.28
0.44
0.72
1.15
Number
Partic
6650
2820
1315
730
37
117
42
-------
-20-
211
These activity values range over a factor of 60 but
the diameter varies by only the cube route, or a factor of 4.
Particle produced lesions which could be considered as precursors
of peripheral adenomas were observed around the 4.3 pCi particles,
Hence, it would be fortuitous if this value did not overestimate
the minimum activity.
Until more experiment data becomes available we would
choose a conservative approach to selecting the minimum activity.
Consequently, we can see little justification for assuming a
minimum activity greater than 0.6 pCi/particle and we believe it
prudent to select a lower value as we have previously proposed.
-------
-21-
212
III. The Sensitive Tissue
In his statements and questions during the December 10
and 11, 1974, hearings, Dr. Radford implied (and attempted to
solicit concurence) that hot particles can only be expected to
induce cancer in man in the more proximal bronchi because in
man this is the sensitive tissue. We cannot agree with this and
as the transcript (pages 2-262 to 2-268) indicates, Dr. Bair did
not concur.
While the predominant lung tumor in man is bronchiogenic,
bronchiole-alveolar carcinomas also occur. It would appear that
because of genetic factors, influenced by the prevalent carcinogens,
the more proximal bronchi are the most sensitive tissue. Never-
theless, we submit that alpha-emitting hot particles represent a
new and unique carcinogenic agent. As such, we see no a priori
reason for doubting that, as in animals, bronchiole-alveolar
carcinoma will be induced in man by PuC>2 deposited in the peripheral
regions of the lungs.
Along with Dr. Little, Dr. Radford has presented evidence
demonstrating that Po-210 in cigarette smoke concentrates in the
segmental bifurcation.24 Dr. Edward A. Kartell has proposed that
the Po-210 is contained in insoluble particulates which accumulate
at these bifurcations. ^ As a consequence the dose to the local
tissue is several rem/year. This is suggested as the carcinogenic
mechanisms related to cigarettes.
24/ Little, J. B. and Radford, E. P., Science, 155, 1967 pp. 606-
607.
25/ Kartell, Edward A., Nature, 249, May 17, 1974, pp. 215 - 217.
-------
-22-
213
The Po-210 particles involved have 2 orders of magnitude less
activity than hot particles. The mechanism involves continuous
exposure at "low" dose rates while the hot particle hypothesis
involves a significantly higher dose rate that is capable of
producing a tissue disruptive lesion around the particle. Because
of the particle size distribution, exposure to PuG>2 aerosols could
involve both mechanisms. As a consequence, the risk could be
larger than that estimated by each hypothesis independently.
IV. PuOp Exposure Standards
In our petition and Hot Particle Report, we concluded that,
consistent with the whole body exposure standard of 5 rem/year,
the alpha-emitting hot particle standard should be 2 particles
in the human lung. Using the estimated minimum hot particle
activity of 0.07 pCi, this resulted in the suggested reduction of
the MPLB by 115,000. However, as we stated in our Hot Particle
Report, this factor of 115,000 would apply only when it was not
determined that the activity was not on hot particles. Using the
particle size distribution determined for the Rocky Flats fire,
and allowing only 2 particles above 0.07 pCi would still have
required a reduction of the MPLB by a factor 16,000.
Table V presents the particle size distribution (using the
Rocky Flats statistics) for high burnup Pu fuel that would be used
in Pu recycle in LWR's or in the LMFBR. This table serves to
illustrate the nature of the problem associated with hot particle
exposure standards in the nuclear reactor industry. As we indi-
cated above, we can see little justification for selecting a
-------
214
-23-
TABLE V
Estimated Particle Size Distribution For
High Burnup Pu Fuel (0.2 Ci/g)(Assuming
a Lung Burden Of 16,000 pCi)
Particle Incremental
Diameter Activity Fraction
p
0.6-0.7
0.7-0.8
0.8-0.9
0.9-1.0
1.0-1.2
1.2-1.4
1.4-1.6
1.6-1.8
1.8-2.0
0.05
0.033
0.022
0.017
0.014
0.007
0.004
0.0016
0.0001
Incremental
Activity (pCi)
800
530
350
272
224
112
64
26
16
pCi/particles
0.32
0.47
.66
0.91
1.58
2.49
4.10
5.30
7.30
Number of
Particles
2500
1100
530
300
142
45
15
5
2
-------
-24-
215
minimum hot particle activity greater than 0.6 pCi/particle.
Inspection of Table V indicates that a 2 particle limit at 0.6
pCi/particle would still require a reduction of the MPLB by
a factor approaching 2000.
A 1000 fold reduction would cause the MPLB for occupational
exposure to be only 16 pCi and as such would be far below the
limits of detectability. But that appears to be the situation
with plutonium. Dr. Morgan, at the December 10th hearings,
recommended a reduction in the whole body burden by about a factor
of 400 based on other considerations; namely, exposure to the bone.
It appears that commensurate with other radiation protection
standards, if you can detect Pu in the human body, a significant
overexposure has already occurred. This, we propose, is the con-
clusion to be drawn from the record of the EPA hearings in
Washington, D.C. and Denver, Colorado.
Since acceptable levels of Pu in humans are below detectable
levels, it is apparent that the exposure standards can be enforced
only by enforcing strict compliance to design specifications and
operational procedures that have the objective of zero release.
We submit that compliance with adequate design specifications
and operational procedures is the only way to effectively meet
.any exposure standard and we suspect that it was quite effective
at the Army's bacteriological warfare laboratory where zero
release was an objective.
-------
216,
Natural Resources Defense Com.jll, Inc.
BOARD OF TRUSTEES
S^p!itn P. D"B!>'""
CVialrmcn
Jamu Marshall
Vi-e Chairmen
Dr. George M. \Voodwell
Vice Chairman
Dr. Dean E. Abnihamsorc
Mrs. l.ouis Authindoss
Boris I. ilittkcr
Frederick A. Collins, Jr.
Dr. Rene J. Dubus
Janics B. Frankcl
Robert W.Gilmorc
Lady Jackson, U.B.E.
Hamilton Kcan
J>r. josliua l.cdcrbcrg
Auljiony M.-u/occbi
Piui N. McCloskey, Jr.
Micuacl Mclnlosh
ZUcanor llo'iucs NcirJon
Ov.-cn Olpin
Kra.nk.lin H. Parker
Dr. Gidord B. I'incliot
Cbarlri B. Rangcl
Juhn R. Robinson
Laurancc Kockcfclicr
}. Willard Roosevelt
\Vhitticy North Seymour, Jr.
David Sive
Uratiir^ Abl^ou Di^-mri
John II. Adams
Executive Director
917 15X11 STR.EET, N.W.
WASHINGTON, D.C. 20005
sos 737-5000
February 4, 1975
New York Office
15 WEST 4/}T!I STREET
NEW YORK, N.Y. 10036
gig 869-0150
Western Office
664 HAMILTON AVENUE
PALO ALTO, CALIF. 94^0]
Appendix A
Mr. Robert B. Minogue
Acting Director • .
Standards Development • . . '
Nuclear Regulatory Commission
1717 H Street, N. W.' .-•-'•'
Washington,- D. C.
Dear Mr. Minogue: . " •
We are writing in response to a suggestion at the
meeting of January 9, 1975, that it would be useful if we
provided written comments on two issues discussed in "A
Review of the Natural Resources Defense Council Petition
Concerning Limits for Insoluble Alpha Emitters," J. W. Healy,
C. R. Richmond and C. E. Anderson, LASL, LA-5810-MS,
November, 1974. These issues to be addressed are:
(a) The discussion beginning on page 4, "B,
Limitations on the Usefulness of Radiation Dose" with par-
ticular emphasis on the statement,
"It is for these reasons that most scientists
have refrained from using dose calculations,
such as those given earlier, to arrive at con-
clusions as to the effect of radioactive parti-
cles but have preferred to depend upon experi-
mental evidence which bears more directly on
the actual conditions."
-------
Mr. Robert B. Minogue . - .. - 217
Page 2 .
February 4, 1975
(b) The statement on page 15, ; .
•"* '
"In a recent study Mclnroy et al., 37
measured the distribution of plutonium
particle size in a lymph node of a deceased
' worker by the autoradiographic technique.
Although this individual was exposed at a
later time than those discussed above, it is
of interest that these estimates also in-
: dicated that 15% of the plutonium was in
particles larger than 0.07 pCi."
We do not agree with the first part of the
statement from page 4. Most scientists who have considered
the particle problem have used dose calculations to arrive
at the conclusion that particle irradiation is unique and that
its consequences may be significantly different from uniform
irradiation.
At the same time, we agree that it is preferable
to use experimental data that bear directly on the problem
when estimating the .risk from particle irradiation. In
fact, in responding to criticisms of our Hot Particle
Report, such as WASH-1320, much of our effort was directed
toward demonstrating that most of the cited experiments
were not relev^nt to hot particles.
... . , -. . f
We would suggest that the most pertinent observation
involve the lesion excised from the palm of a mechanic
by Lushbaugh and Langham and the microsphere experiments
conducted by Richmond, et al. These experiments strongly
suggest that a single hot particle embedded in tissue is
capable of eliciting a tumorgenic response. Richmond, e_t al,
described the lesions induced in the lung of hamsters as
precursors of peripheral adenomas. We submit that these
observations alone are sufficient to indicate that every
effort should be made to prevent such particles from being
deposited in human lungs. They strongly suggest that a
single hot particle represents a significant hazard and
-------
Mr. Robert B. Minogue
Page 3
February 4, 1975
that the radiation protection standards should certainly
limit the exposures to very few particles.
This, however, leaves xis with the problem of what
constitutes a hot particle. In the subsequent discussion
of the statement on page 15, we address this issue and define
the hot particle from experimental data without the use
of dose calculations .
With respect to the statement on page 15 , the
unpublished paper by Mclnroy , et al. , reports new and
potentially significant data that were not available when
we wrote, "Radiation Standards for Hot Particles." Our
analysis of these data and their implication with respect
to the proposed hot particle standards is given below.
The following data were presented for Case 7-138,
•the metal fabrication worker who died of a crushed chest in
1973, twenty six years after his first exposure.
Lymph Node activity (12 nodes)
Mean concentration 770 + 493 pCi/g Pu-23S
- . . • 80+43 pCi/g Am-241
I •
Maximum concentration 1800 pCi/g
(node #11)
0*30
Distribution of ^PuC^ particles (in node #6) :
Mass median diameter MMD =0.3 urn
Geometric std. deviation Ug = 1.6
Count median diameter CMD = 0 . 2 /am
Based on these data (and Mclnroy, et al.'s, Table 5 and
Figure 2) we find that 7 percent (as opposed to 15% re-
. ported by Healy, et al.) of the lymph node activity was
^estimated to be on hot particles. This represents a sub
stantial number of hot particles by our definition (ac-
tivity >,0.07 pCi) .
-------
219
Mr. Robert B. Minogue _ . . ,
Page 4 . '••••'
February 4, 1975 • , ;. : .
239
The measured distribution of Pu°2 Particles
size is given in Mclnroy, et al.'s Table 5. For particle
diameters larger than 0.6 join (corresponding to 0.07 pCi)
the following data are presented:
Dia Midpoint Incremental Activity Activity Particle
Fraction pCi/particle pCi/node per node
0.6 '...': •'.•- •'••••••" • • • • . • ' • •
0.7 0.056 0.11 37 340
0.8 -. •• .. - • .' '•:. :•':•,:•••
0.9 0.011 0.24 7 29
1.0
1.1 0.002 0.43 1 2
.1.2 .' • ' • : : -.; ' :..' : ,\ ..
Total activity in sample (node #6) =657 pCi.
Assuming the total mass of the tracheobronchial lymph nodes
is 15 grams, the total number of hot particles (activity
>0.07 pCi) in the lymph nodes is
(15g) (770 gCi) (340 +29+2) particles = 6500 hot particles.
g 657 pCi
This probably overstates the number of hot particles in the
lymph nodes for the following reasons: (a) smaller particles
tend to aggregate into larger particles in lymph tissue
(See WASH-1320, pp. 10-12 ) , (b) according to Mclnroy
(private communication v;ith TBC , Jan. 20, 1975) aggregates
(particularly with respect to the larger particles) were
observed and reported as single particles (the experimental
design of the particle size measurements, because of
aggregation, tended to maximize the estimate of large
particles) , and (c) because one is looking at a plane
view, it is difficult using the audioradiographic technique
to distinguish star track coming from two point sources at
different depths but along the same line of view. Paul
-------
220
Mr. Robert B. Minogue
Page 5
February 4, 1975
Morrow pointed out to one of us (TBC private communication,
Jan. 20,. 1975) that the audiographic technique is not very
reliable for particle sizes below about 0.5 urn to 1.0 um
because of the difficulty in distinguishing individual
particles. In other words, aggregates of particles would
appear as point sources below this size range. In addition,
there is a sizable (64 percent) statistical uncertainty
in the 770 pCi/g estimate, and the lymph nodes analyzed
may not be representative of the total tracheobronchial
lymph node mass. , -
It is possible to make a crude estimate of the
lung burden based on the lymph node concentration, or
burden at death. We have done this using the ICRP lung
model (ICRP Publication 19, p.6) for lack of better data.
In our case the ICRP model is simplified to
Source
(S)
•D 1
Region of
Lu.nq(P)
f
T
_JT 1
— •• ~ — —Ujy mp
-------
Mr. Robert B. Minogue
Page 6 '
February 4, 1975
We have assumed the rate at deposition of activity in the
pulmonary region , is constant throughout the 26 year
exposure period to simplify the calculation, i.e. S(t) « R.
This yields
- e
For t = 26 yr, the time of death
'' '• L(26) =12
R = 17 nCi/yr ': - ~;
P(26) X 2R ^34 nCi ^
There is considerable uncertainty in these values for a
number of reasons reviewed on pp. 5-9 of ICRP Publication 19.
The parameters are for a class of compounds as opposed to
Pu02. Retention may be a strong function of particle size.
The biological half-lives are not known within a factor of
5;Tl/2 = 500d raaY represent anything between lOOd and 10,000c.
The ICRP model parameters are not consistent with uranium
miner exposure data. It should also be noted that the
calculated pulmonary and lymph node burdens are higher than
the 33 nCi of 239Pu based on urine assay (Mclnroy, et al. , p. 3
and that the exposure was surely not uniform over the 26"
year period, but probably highest "during the early years of
laboratory operation (1945 - 1955) before improved industrial
hygiene and health physics requirements reduced signif icantly
the air levels of plutonium in the laboratories and the
workers were provided with more efficient personal respiratorv
protection" (Mclnroy, et al . , p. 5.).
-------
Mr. Robert B. Minogue
Page 7
February 4, 1975
Nevertheless, assuming a pulmonary burden of 34
nCi and the particle size distribution in the lung is the
same as the measured distribution in the lymph node, the
number of particles greater than 0.07 pCi (o'.6 pm dia) is
(34 nCi)(371 particles)(1Q3 pCi/nCi) = 20,000 hot particles
657 pCi
The probability of cancer induction at a risk of 1/2000
per particle would be essentially unity.
Assuming a minimum activity to constitute a hot
^article is 0.14 pCi, corresponding to a 0.8 urn diameter
PuO2 particle, the number of hot particles'in the pul-.
inonary region would be
134)(31) x 103 = 1600 particles.
; 657 .
The tumor risk would be about 0.5. . •
• There is an obvious need for a careful particle
size analysis of the lung tissue available from Case 7-138,
and a pathological examination to determine whether lesions
are associated with the larger particles. Dr. Mclnrov
has informed one of us that an examination of the lung
tissue is underway.
It can be argued that it is premature to modify
the proposed hot particle standard ["Radiation Standards fc~
Hot^Particles"] by shifting the minimum hot particle activif,
until the lung data is available. However, our original
choice of the minimum hot particle activity carried conside--
uncertainty (See "A Critique of the Biophysical Society's
DRAFT Comments on "Radiation Standards for Hot Particles "
pp.4-6). The choice of 1000 rem/year to the local tissu- as
the cut off defining a hot particle was based on the choice
of (a) 1000 rein supported by the experiments by Albert, et
aJU , and Lackin, et_ al_. , (b) one year as the tissue repair
-------
• ' '" : - : ' ' •'':;; •'•.'. • •'•• '•••-'•" • :'—'-. 223
Mr. Robert B. Minogue ... ; - ; : •
Page 8 • . . -__ . . •'••••.... -..' ^ /'.'-: ,:.'':''v-..^.;'•''''••. ,:;;''-. :/.••.. • "
February 4, 1975 • - ._ ,';-''';.,•'';• .:••'•';• •:;-\: :.vv':'/^-:'. ••';\-i.'>--'.."••:'.''.•'.•'
time in the lung/ and (c) the Geesaman lung model
assuming- the lung was inflated to 1/2 maximum.
The combined uncertainty associated with these
assumptions is more than a factor of two. Had the lymph
node data been available to us at the time we prepared our
report we would have used these data in establishing the
minimum (or critical) hot particle activity. We therefore
propose increasing the minimum hot particle activity by a
factor of two to 0.14 pCi. This new value should of course
be re-examined as in light of any new data, particularly
the Case 7-138 lung data when it becomes available.
One of the criticisms of our report raised by
Dr.'Gamertsfelder, and others, is the arbitrariness or
uncertainty in the choice of 1000 rem/yr to the local tissue
as the definition of the critical particle activity. We
1 can avoid the use of dose or dose rate altogether in
defining the critical particle activity by basing the cut
off on the observations by Lushbaugh, et a1., the hamster
experiments of Richmond, et al., and the lymph node study
by Mclnroy, et al. LushbaugET et a^L. reported a lesion
in palmer tissue that developed~~around a particle containing
0.08 ug (5nCi) of Pu-239. Richmond, et a1. observed lesions
in the lungs of hamsters around particles containing 4.3 pCi.
Moving down further in activity, we postulate on the basis.
of the study of Mclnroy, et al. that lesions probably did not
occur around particles less than about 0.14 pCi, otherwise
Case 7-138 probably should have developed cancer according
to the hot particle hypothesis. On the basis of these data
it seems logical to select a critical particle activity
between 0.14 pCi/particle and 4.3 pCi/particle. We would
suggest a value close to 0.14 pCi/particles to be conservative
and because of the limitations of the Richmond, et al.
experiments set forth on pp.25-28 of our critique of WASK-1320
namely, that had these experiments been performed with
that have longer life spans, it is quite possible that
lesions would have developed around particles of lower
-------
224 Mr< Robert 3- Mihogue
Page 9
February 4, 1975
activity. Notice we have avoided the use of dose
altogether.
Finally, as we stated earlier, the observations
of Lushbaugh and Langham along with those of Richmond,
gt- al. , strongly suggest that a single hot particle
represents a significant hazard and that the standards
should limit exposures to very few particles. Moreover,
the direct observation by Ri chmoiid, et ail, of lesions
induced by particles containing 4.3 pCi~ciearly demonstrates
that there is a hot particle problem associated with the
nuclear industry. Particles with this activity are
within the size range that can be deposited in the deep
respiratory tissue. In other words, there is experimental
evidence that bears directly on this problem and that
evidence indicates the need for more restrictive standards
when hot particles are involved.
If you wish to discuss these, or other issues
further, don't hesitate to call us.
" • Sincerely,
Thomas B. Cochrari
Arthur R. Tamulin
cc: Dr. William A. Mills
_ Dr. W. D. Rowe
-------
UNIVERSITY OF CALIFORNIA
LOS ALAMOS SCIENTIFIC LABORATORY
(CONTRACT W-7405-ENO-36)
P. O. Box 1663
Los ALAMOS, NEW MEXICO 87544
225
IN REPLY
REFER TO: H-5-75-165
MAIL STOP. 486
Appendix B
February 10, 1975
Thomas Cochran, Ph.D.
National Resources Defense Council
1710 Nth Street, N.W.
Washington, D. C. 20036
Dear Dr. Cochran:
In reference to our recent telephone conversation concerning the
particle size distribution of Pu07 in the tracheobronchial lymph nodes
of a former employee of Los Alamos" Scientific Laboratory ("Studies of
Plutonium in Human Tracheobronchial Lymph Nodes", LA-UR-74-1454), I
checked with the person that had counted the tracks associated with the
"stars" in our autoradiographs about the possible presence of clusters
of particles. He did not find many stars in which he was able to dis-
tinguish more than one center from which the tracks originated. However,
it is my feeling that there is no way in which we could identify whether
the tracks were formed from the decay of plutonium in a single particle or
a cluster of small particles. The bast we can say is that if a group of
small particles was counted as a single particle, the size estimate was of
this larger, composite diameter. This means that our estimate of the
activity median diameter of 0.32 urn may be on the high side as counting
any aggregate cf particles as a single particle tends to maximize the es-
timate of the size distribution.
I am very interested in your calculation of the lung burden from
the lymph node concentrations. My,estimate of plutoniurn in the lung, based
upon the average concentration of 239pu -;n eight transverse sections, taken
from the superior lobe of the right lung, was 36 ^ 19 nCi. The variance is
quite large due to the variation in the distribution of the particles
throughout the lung. The estimate, however, is remarkably close to your
calculated value of 34 nCi. This may be fortuitous but I will be able to
Improve our estimation as we continue to analyze sections from this lung.
As regards our plans for continued study of this autopsy case, I have
discussed with our pathologist the possibility of examining sections of
lung tissue for lesions that could be associated with the presence of
plutonium and, at the same time, attempt to measure the particle size
distribution within the lung, using the same techniques used with the lymph
nodes. We have decided to attempt this, although there are several serious
problems that are evident, For example, our lung specimen was inflated with
dry nitrogen, shortly after the autopsy, to a configuration approximating the
natural shape it would have in the thoracic cavity/ This was frozen in this
form and has since been used in studies with our lung counter to compare the
in vivo and in vitro measurements of plutonium and americium present The sec-
tioning, mounting and staining of tissue that has been frozen presents some
AN EQUAL OPPORTUNITY EMPLOYER
-------
LOS ALAMOS SCIENTIFIC LABORATORY
UNIVTRStTY OF CALIFORNIA
LOS ALAMOS. NEW MEXICO O7S44
226
TO: Ihomas Cochran, Ph.D. -2- DATE: February 10, 1975
problems when attempting a histological examination due to the disruption
of structure by freezing and to the dehydration that has occurred during storage
I will be happy to keep you informed as to our progress. If you have
additional questions and/or suggestions, please write or call me at
505-667-4709,
Sincerely,
James F. Kclnroy
Tissue Section Leader
Industrial Hygiene Group
mlg
-------
UNIVERSITY OF OREGON
227
INSTITUTE OK
MOLECULAR BIOLOGY
EUGENE, OREGON 974°5
telephone (code 503) 6X6-5151
December 5, 1974
Dr. William Rowe
Office of Radiation Program
Environmental Protection Agency
Washington, B.C. 20460 •
Dear Dr. Rowe: !
Enclosed please find a series of reports and documents which
have been assembled in connection with a study of the radiation
standards for "hot particles" problem which was undertaken by the
Science and Technology Information and Advice Service (STAIS) of
The Biophysical Society, which was undertaken at the request of
the Center for Science in the Public Interest, as outlined in
the covering memorandum. Further details on the origin of the
study, and the procedures followed in carrying it out, are pre-
sented in the enclosed documents. I understand that the EPA is
currently undertaking a review of this problem, and I send you the
enclosures in the hope that they may be helpful to you in the course
of this review.
Please let me know if we can help in any other way.
Sincerely yours,
Peter H. von Hippel
Editor, STAIS and Past-President,
The Biophysical Society
PHvH:bm
Enclosures
-------
r
ilOPHYSICAL
10CIETY
Institute of Molecular Biology
University of Oregon
Eugene, Oregon 97403
303-686-5151
•resilient
Dr. Peter H. von Hippel
Umiuertity of Oregon
'mtdent-Elec!
Dr. Andrew Szent-Gyorgyi
Jtrandeu University
tcretary
Dr. Margaret O. Dayhoff
national Btomfdtcol Research Foundation
Vvnsurer
Dr. John B. Wolff
Httional Institutes of Health
ffovember 25, 1974
MEMORANDUM
"To: Whom It May Concern
From: Peter H. von Hippel, Editor, The Biophysical Society
•Science and Technology Advice and Information
Service; and Past-President, The Biophysical
Society.
-Subject: Enclosed STAIS Report on Radiation Protection Standards for
-Hot Particles of Plutonium and Other Actinides.
At the request of the Center for Science in the Public Interest,
fthe STAIS group of the Biophysical Society undertook a study on the problem
of Radiation Standards for Hot Particles. Information about the Biophysical
Society's Science and Technology Advice and Information Service, as well
as the procedures and ground rules under which we conduct studies, are
-attached.
As indicated in the enclosures, a committee of experts in various
fields relevant to the problem under consideration was put together,
-and their efforts were coordinated by Drs. Jane and Richard Setlow of the
Brookhaven National Laboratory. The committee members names and addresses
are listed on an attached sheet. As indicated in the summary provided
by Drs. Setlow, the committee did not actually meet, but each member was
provided a copy of the Natural Resources Defense Council petition, and
the Tamplin-Cochran report, which formed the basis for the request for
a STAIS study by the Center for Science in the Public Interest. Each
member of the committee was asked to evaluate the information contained
in the petition and report, and the literature on which these documents
•vere based, and to submit a written report to the Drs. Setlow on comple-
tion. Since each committee member went about this assignment in a differ-
ent way, and from a somewhat different point-of-view, we have felt it
appropriate to submit a summary of their findings, together with their
Individual reports, rather than trying to assemble an integrated report
at this point. The committee members have specifically asked me to point
out that their individual reports represent more individual "impressions"
following perusal of the available literature (though by people expert
in the field), than definitive studies. For this reason we would also
-------
229
The Biophysical Society -2- November 25, 1974
like to designate the present report as a draft version, and would welcome
comments of other individuals knowledgeable in the field who might wish
to comment upon, or differ with, some of the conclusions our experts have
reached. Such comments should be sent to me (or Drs. Jane or Richard
Setlow), and we will pass them on to the individual or individuals on the
committee most competent to assess them. Such comments, together with
the responses of the committee members, could then form a part of the
final record of these deliberations.
*
In addition to sending this report to the requesting group, we have
also sent copies to various other agencies and groups involved with current
studies on this problem, including: the Atomic Energy Conmission, the
Environmental Protection Agency, the General Accounting Office, the Natural
Resources Defense Council, and the National Academy of Sciences. -We hope.., -^ v
that these groups will find these statements useful in putting together
their own reports on this problem.
In conclusion, I would like to add some personal comments which seem
to me to be implicit in the attached reports. First, the main reason this
body cf experts was unable to reach a single definitive conclusion is, of.
-course, that really adequate experimental data do not exist. Thus, all
studies on this subject are of necessity somewhat subjective, since they
•must be based on rather difficult extrapolations of only marginally rele-
vant experimental work. In this connection, we might: wish that more di-
rectly relevant studies had been launched by the Atomic Energy Commission
some years ago, so at this stage there would be better data to go or..
Also, I think it is important to point'out that the National Resources
Defense Council has performed a very useful public service in calling our
-attention to the possible inadequacy of the present radiation protection
standards, since, regardless of whether the present standards are ulti-
mately found to be adequate or not, they had obviously not been formulated
vith the "hot particle" problem in mind. Our contribution to this has
been to make our best unbiased attempt to estimate the validity of the
present standards, based only on the relatively scant experimental infor-
mation available. Based on these studies and others, the nation's policy
makers will ultimately have to find the appropriate balance between health
hazards to society, and the energy requirements of the nation. . •
-------
230
THE BIOPHYSICAL SOC IETY
SCIENCE AND TECHNOLOGY ADVICE AND INFORMATION SERVICE
The Biophysical Society, a professional organization of about 2500 members
engaged ™ research and teaching in various scientific disciplines at or near the
interfaces between biology, physics, chemistry, mathematics and medicine, is
pleased to announce the availability of a Science and Technology Advice and
Information Service (STAIS). - - , &-•• • ,
The concept of such a service arose becawse many members of our Society have
expressed a desire to utilize their scientific and technical training on a part-time
basis to help with the various problems facing governmental agencies (at the federal,
state and local levels) and public Interest groups 1n formulating and Implementing
policy and programs which have scientific and technological components. To this
end the Society has surveyed Its membership and developed a Roster of Interested
members who are able and willing to participate.
Agencies .or groups requiring such assistance are Invited to write or call the
Office of the Secretary of the Biophysical Society for further information, or to
receive an "Advice Request Form". Specific questions, or requests for advice, can
also be directed to any of the members of the STAIS Editorial Board.
The ground rules under which STAIS will operate are as follows:
"The basic purpose of the Science Advisory Service of the Biophysical Society
1s to contribute to the improvement of conditions of society. For example, a
project in connection with which advice 1s solicited might be designed: to relieve
suffering and prolong life; to improve the environment by reducing pollution of
the air or water, or by protecting natural resources; or to help provide needed
facilities for people which improve or maintain the quality of life." The Editorial
Board of STAIS will retain the right to reject a request which, in its opinion and
after suitable investigation, does not seem to meet these general criteria. It
is expected that advice will not be provided in confidence, and both the designated
advisory group and the EditonaT Board will retain (and generally exercise) the
option of making the results of investigations public if such results are of public
concern. The Biophysical Society will take no official responsibility for the
advice given, nor should that advice be construed as representing the position of
the Biophysical Society on the question at issue. The only role the Society as such
will play in STAIS is to maintain the Roster and the Editorial Board, and to put
groups requesting advice in contact with the appropriate advisors. The Biophysical
Society is a non-profit organization, and the only charges to the group seeking
advice will be to cover costs.
-------
For further Information, please contact:
Peter H. von Hlppel, Editor
S.T.A.I.S.
Institute of Molecular Biology
University of Oregon
Eugene, Oregon 97403
503-686-515.1 " '. ". '
Michael Beer, Associate Editor
S.T.A.I.S.
Department of Biophysics
Johns Hopkins University.
Baltimore, Maryland 21218
301-366-3300 •x597 . ... .
Frederic M. Richards, Associate Editor
S.T.A.I.S.
Department of Molecular Biophysics
Yale University
New Haven, Connecticut 06520
203-436-2032
Andrew G. Szent-Gyorgyl, Assoc. Editor
S.T.A.I.S.
Department of- Biology
Brandeis University
Waltham, Massachusetts 02154
617-647-27S8
Margaret 0. Dayhoff, Secretary
The Biophysical Society
National Biomedical Research Foundation
Georgetown University Medical Center
3900 Reservoir Road, N. W.
Washington, D. C. 20007
-------
232
Members of STAIS Committee
on the "Hot Particle Problem"
Coordinators:
Drs. Jane and. Richard Setlow
Brookhaven National Laboratory ..
Associated Universities', Inc. '
Upton, Long Island, New York 11973
Members:
Dr. Arthur Cole
Department of Physics
M.D. Anderson Hospital
6723 Bentner
Houston, Texas 77025
Dr. Louis Herapelmann
Strong-Memorial Hospital
260 Crittenden Blvd.
Rochester, New York 14620
Dr. Malcolm L. Randolph
Biology Division
P. 0. Box Y
Oak Ridge National Laboratory
Oak Ridge, Tennessee 37830
Dr. Andrew M. Rauth
Physics Division
Ontario Cancer Institute
500 Sherbourne Street
Toronto 5, Ontario, Canada
Dr. Richard P. Spencer
Department of Nuclear Medicine
School of Medicine
University of Connecticut Health Center
Farmington, Connecticut 06105
-------
RADIATION STANDARDS FOR HOT PARTICLES
(Summary by Jane and Richard Setlow, Committee Coordinators) OQQ
Summary of the reports of five committee members asked by the Biophysical Society
to evaluate the present radiation protection standards for hot particles of
plutonium and other actinides.
The group has not met to discuss the problem since the individual members
have perused the relevant literature. Each member wrote an independent evaluation
and these have been summarized by the coordinators, R. B. Setlow and J. K. Setlow,
as follows.
1. The problem raised by the Natural Resources Defense Council petition
of'what -should be the maximum permissible lung burden (MPLB) of hot particles, is
a valid and serious one. However; the-call -for a decrease in MPLB by 10 is
exaggerated. More animal and epidemiological data are needed for a truly adequate
estimate of what should be the radiation protection standard. A crucial piece
of missing information concerns the distribution of particle sizes involved in the
Manhattan district accident. Twenty-five individuals followed for almost 30 years
have no lung cancer from 3-10 nCi of plutonium in the chest. Calculations in the
Tamplin and Cochran report accompanying the petition indicated that the particles
were too small to be effective. Other calculations resulted in the opposite con-
clusion. One of the reviewers suggested an experimental reenactment of this accident
(without humans present) for the purpose of measuring particle size.
The lung burdens of 25 Rocky Flats workers exposed to plutonium fires
range from one to ten times the present MPLB. No lung cancer has been detected •
in any of these individuals after nine years. Since there is evidence that the
latent period for cancer induction after a large exposure may be as short as this,
these data again suggest that the factor of 10 is too large.
2« The reviewers who looked into the quantitative aspects of the Taaplin-
Cochran report all concluded that it contained exaggerations and lack of adequate
reasoning (a,b,c). -This report includes interpretation of the data of others,
sometimes at variance with the authors' own interpretation. Two of the reviewers
used existing published animal data and several biological models to estimate the
probability of cancer induction in the human lung from hot particles. They con-
clude that the existing MPLB should probably be decreased by some factor between
40 and 10 , but that this figure at present can only be tentative, because of the
paucity of data. Another reviewer finds no reason to alter current standards.
a) The single instance of a hand sarcoma following plutonium contamination
Is inadequate for a quantitative argument, especially since there was no evidence
that the plutonium penetrated the skin.
b) The single instance of supposed precancerous changes in the neighbor-
hood of a puncture wound involving plutonium, later excised, is also not suitable
for a quantitative argument, especially since there was another similar but un-
excised case in which no cancer developed in 30 years.
c) The use of the data of Albert e_t al^ on rat skin tumors induced by fast
electrons to estimate the risk from hot particles seems unjustified on four grounds.
(i) The rat ,data involved a single dose, whereas the lung irradiation being con-
sidered is chronic. (ii) Tamplin and Cochran do not cite data showing that non-
uniform irradiation by beta and alpha particles is less effective than uniform
radiation. (iii) Previous experiments cited by the Albert group showed no tumor
production by 0.3 MeV electrons, external alpha particles and protons. (iv) The
hair follicle seems to be the sensitive structure for radiation-induced cancer in
the skin. No similar structure has been identified in the lung, nor is there any
estimate of the probability of a hot particle being close to such a structure.
(Albert, Burns and Heimbach, Rad_. Res. 30: 514, 525, 590 U967]).
-------
234
•August 27, 1974
>1.L. Randolph1; Appraisal of "Radiation Standards for Hot Particles",
Beport of A.H. Tanplin and T.B. Cochrea, February 14 1974
"' " "* • . V * . .' •
. A. OVKRALL VIK-TS • • ..-'•.
• I have chosen to evaluate primarily tho report "Radiation Standards for'• •
Hoi Particles", Feb. 34, 1974, of Tnnnlin and Cochrsn, end the biological and
theoretical evidence they directly refer to, rather than the ncre general
problem of rvaxisnm permissible *-^I\L lung burden end the foundations on which
it does snd/or should rest because tho more limited rroblea is easier to
consider and SOCKS tho scientific basis on which to decide the irsediate
question of whether or not the Biophysical Society should support the petition
of the Natural Resources Defense Council to ASC and EPA. Other arguments «uch
as that of Myers (Health Physics 22 (1972) 90$) might wen influence a nore
thorough appraisal of the general problen.
This appraisal is organized as follows: A) Overall views B) Major
technical considerations C) Minor (?) technical considerations D) Appendix.'
Tentative estimate of Eaxiiaua perrissible lung burdens.
V.y raj or conclusions regarding Tairplin and Cochin's report and Geessran's
•vork vhich furnishes the backbone for their report ar*e:
1. The authors are to be contended for their accroach to radiation hazards
that standards should be based on specific, rather" taan overly broad, hazards;
-for the analysis of the dose fros hot particles, and (perhaps) for their conserva-
tive approach that the crucial parameter for tu=or induction by hot particles
iS the nir:ber of particles of damaging size in the Isng rather than the gross
dose. Unfortunately their work has not yet been published in the open literature
(to ry knowledge}. ~" ' '
2. The quantitative arguments (asi I understand tben) that Tarsplin and Cochran
advance in support of their proposed reduction of rexirrua pemissible lung
• burden by a factor of 1CK at best warrant the Scottish verdict a:.'ot proven".
The main trouble seecs to be loose interpretation of the biological results
e.g., use of Albert et al's (Had. Res. 30 (1967) 515,, 525 and 590) data on
skin cancers produced by penetrating electrons in thSr-fsce of -lh&-m*~tt?&i',~i\^.-~{ -~
consents that no skin tuners were observed with protons,"alpha particles or
low energy electrons. Eight sets of biological data ^adduced by Tanplin and
Cochran are discussed under heading "B. Major technical considerations."
3. Data jcore directly applicable can be expected ±zi about 10 years when" the "
latent period jnfor detection of cancers in the Rocky Tlats workers is over and
are cor.plete.
conditions for the
particle size distri-
bution might promptly provide useful information.
5. 1 have been told that "professionals" .— i.e., the ICRP and the European
Radiation Research Society — have official cornnittee;s looking into the hazards
of hot particles. If so, I wonder how ouch effort ve? aaateurs, except Hespelsann,
should put forth.
• 6. Results of rery^tentative appraisals (D. Appendix of this report) of
lung turor risks based on data cojrpiled by Bair suggpst that the naxirrja
permissible lung burden should bo^reduced by a factoir of 40 to Itf* instead of the
factor of 105 suggested by Tanpliu End Cochran.
-------
: 235
Randolph ' . •
B. MAJOR TECHNICAL CONSIDERATIONS
As I understand it, Tnrplin and Cochron's conclusions stem almost completely
fror. their conviction thnt^krborno l/.m diameter psrticle of ^PuC2 has a
high r-obability of beinr deposited in the deep respiratory zone (D.-xZ) of a
human lung and thereafter imposes o risk of 0.001 to 0.0001 that a tumor will
be produced (vrithin perhaps 20 years).
This conviction is founded primarily on three bases:
1) the work of Mann and Kirchner (Health Physics 13_> 877 (Wb7)) on the percent
of inhaled PuO? aerosol deposited in the pulmonary region;
2) P.P. Goesnnan's theoretical analysis (UC/'.L-50387, 1968) fror: lung geometry,
aloha particle ranee, etc., of energy deposition for such hot particles;
3) from considerations by Geesaman (UCRL-50387, Addendum, 19b8) and by
Tamplin and Cochran of seven biologicar'experimenT.3".
The first two physical bases seem to depend on rather straightforward
analyses. In the work of ^snn and Kirchner the probability of deposition of
aerosol is derived for the special case of Pu02 in terms of particle size,
vhereas other more general repots (e.g., IbRP Task Group on Lung Dynamics,
Health Physics 12 (1966) 173; Dix and Dobry. Health Fnysics 22, (1972) 569;
- find Craig et al, Health Physics 22 (1972) 845) are in terms ofeerodjciarsic
-diameters". _ In the first approximation of spherical particles the aerodynamic
diameter *» I( particle density c^T~Tl7f5~ X (physical diameter). Taking this
factor into account various results seem in reasonable agreement, although^ at
very snail diameters (smaller than of concern to us) Kann and Kirchner find
less deposition than do othgjrs. Geesanan's ingenious approximate treatment
of the otherwise intractable geometrical problem of dose from hot particles
in the DRZ seems reasonable if his picture of the human- lung structure is
correct. (Although I am not an expert on this, my superficial checking
revealed no discrepancies.) Some other lesser (?) details related to the
•physical dose calculations are given in Section C.
i • —-
Of a large literature (e.g.^tangham compiled 1500 references on Pu
toxicity) possibly pertinent to the problem, I have attempted to evaluate only
8 main instances mentioned by Templin and Cochran. Obviously, the best
scientific evidence would be results from a large number of human lung exposures
to chronic aijQia particle irradiation under well known conditions. The 8 cases
ere:
(p. 22-26). The work of Albert, Burns and Heimbach (Had. Res. 30. (1967)
525 and 590) on skin tumors and atrophied hair follicles in rats caused
by fast electron irradiation of up to 7 k~g4g fi^er 24 cmVrat. Up to 5 tumors/rat
at 80 weeks post-irradiation were observed, and regardless of incident electron
energy continuous dose response curves were found when the dose was taken as that
at 0.27 mm depth*. 'Furthermore, they observed that the ratio of tumors/rat to
atrophied hair 'follicles was nearly constant — 1/2000 to 1/4000. This ratio
SOOES , but is not explicitly stated, to have been taken as a principal basis
ror Tamplin and Cochran1s interpretation (p. 26) "when a critical architectural
unit of a tissue U.g., a hair follicle) is irradiated at a sufficiently high
Incidentally, the shape of Albert et al's dosa curve suggests that ix night be
fit by something of the forn: tumors/rat •• (ADn) e~a , representing .ajnulti-hit
(n *A to 6?) tumor gonorotion and an exponential ooll killing. " —
-------
236 ' - , , K
nandolph
dosage, the chance of it becoming concorous is approximately 10"^ to 10~^."
By a loj-'c- not clonr to no, by pnr;o 36 (if not sooner) this soeir.n to bo cone
"a rick of cancer equal to 1/2000 per hot porticle". Specifically, I don't
•understand how the mm dor or' hair follicles damaged by large area electron
irradiation relates.to tho volume irrndiatod by a hot particle and would
think r~°taconists °f theno expocuro limits should make this point clear. One
vay to estimate trie hazard of a 1 micron hot pnrticle would bo annicrw tunor
induction proportional to the volume irrodioted. Thus from the electron
experiment we hove no more than (5 turcors)/(24. era2 X 0.07 en average electron
range) = 3 tunors/cm . '-'or hot particles thon.wo expect 3 (tunors/cia3) X
(65 x 10~0 f^/pnrticle X 1 cnry/m) =~ 2 x 10~A tunora/particle. This is a
poor calculation (i.e., ovorentimnto of tumors) DOCBUOO it oanunoo the
maximum radio:j_onsitivity ht all skin depths and doses. Albert et al
concluded that o.-z6ne;'of maximum sonaitivjtv exists at a depth or around 270
jXn depth. This is 6 times tho range of O'Pu alpha particles in tissue.
Albert et al (Rad. Res. 30 (1967) 515) also mention that previous experiments
vith 0.3 MeV electrons (range perhaps 80^a), with external alpha particles,
and vith protons with range of about 170/-in,did not produce tumors. Kence
one wonders why Albert et al's data were used to estimate alpha particle
hazards quantitatively.
_22) (p. 25-26). Tsrcplin and.Cochran cite experiments in which 16 krad froa
P plaques induced an average of one skin tunor/animal. Again we have the-
problem of how to relate the effect of a relatively large area beta particle
irradiation to that from a hot particle.
3) (p. 27-23)7 Turicture" wound involving 0.08/.g or 5 r.Ci ^^Pu reported bv
Lushbaugh and J. Langharn (reference obscure) who are quoted by Tamplin and
Cochran as: "Although the lesion was minute, the changes in it were severe.
Their similarity (italics added by KLR) to known precancerous epidermal cytc-
logic changes, of course, raised the question of the ultimate fate of such a
lesion should it be allowed to exist without surgical intervention . . . ".
Jj^plin and Cochran rephrase this as: "In this case>J,e3s than 0.1JU. of
Pu produced (italics added by KLH) preeencerous changes in human tissue";
then say et the tine (about I960?) there were (known?) less than 1000 puncture.
vounds and conclude "... this wound data would suggest that insoluble
plutoniun particles could offer a risk of cancer induction in man that is"~ —
greater than 0.001 per particle." I would ignore this case for attempts at
quantitation of lung cancers produced by a single hot particle because: (a) it
is uncertain if even precancerous tissue was present; (b) statistics based
on but one case are inherently poor; (c) this case involves skin rather thaa
lung cancer and is not quite an external irradiation; and (d) this case
involved 5 nCi of ^->"Pu which is more tnan JXT tines that of a standard hot
particle.
4.) (p. 27-28). Mr. Gleason's possible -^Pu-induced skin cancer. Again the
vagaries of the case isuch as cited for example 3 and the lack of independent
evidence of how much ^"Pu got where into the skin or flesh by what mechanisa)
Bake this unsuitable for quantitative appraisal.
5) (p. 30). Work of Larkin et al (J. Nat. C£ncer Inst. 21 (1963) 219)
intrabronchial tunora in rats caused by exposure to beta particles from
-------
Aflndolph •
is refe^~ed to by Tamplin and Cochran but there seems no quantitative use of
these'data to relate them to tho risk associated with a single hot particle.
6) (p. 31-^2). The work of Park, Bnir and Bunch (Health Physics 22 (19/2)
803) on lir<- turors in beadles produced by inhnlation ol 0.^5 to 0.^ median
dia-eter 2~'9Pu02 particles is cited. Twenty of twenty-one dogs that survived
Kore~th»n 1600 days postexposure had pul-nonary neonlasia. The lung burdens
ranged from 0.2 to 3.3/Uli. Tamplin and Cochran noto thnt "nince the pathological
response is saturated'in this experiment, it is Inappropriate to draw any
inference about the magnitude of the response at smnllor burdens." As Tamplin
end Coch-rm point out, lung burdens, smaller by orders or magnitude, might also
rive a high tumor incidence. On the other hand, one might assume a linear
turao~ to radioactivity incidence and sny tnat sinoe those exposures end tumor
incidence both were roughly 3 orders of magnitude greater than the present
maximum permissible lung burden and BifiiK estimate of annual cancer risfC from
a 5 rem/year whole body exposure, these data support continued use of the
present standards. These lines ol reasoning are both merely speculative.
2) ' (?• 34-37)- R°cky Fla"ts fire. Twenty-five workers each received a
2^^PU09 iur.f burda'n whicn Tanrlin and Cohcran calculate as more than 104
hot pa-ticles. By their analysis each worker should suffer one or more tumors
eventually. Investigations during the 9 years since the incident reveal no
detectable tumors. Tamplin and Cochran, without citing documentation, suggest
that tne latent period between exposure and development of cancer is much
longer. (We should ask a radiation cancer expert - F.empelnenn? - if tnis is
correct.) If so, these exposures may provide valuable information in perhaps
10 VG sr s
8) (p! 38-4.0) Twenty-five Manhattan rroject workers with measurable body
burdens of Pu vhose health and lung burdens of Pu have been followed for 27
yea-s (Ker.pelmsnn, Langnam, Richmond end Voely, Health Physics 2£ (1973) 461J.
No clear cases of radiation induced lung tumors were found. Fourteen ol 21
vorKers cnecked in 1971-72 had chest (equivalent to lung?) burcens o. 3-10 nCi,
7 had 7-10 nCi. If these exposures were from l»Ajn diameter ^ruU2 particles,
each person would have more than 10* hot particles, and by Tamplin and Cochran s
estimates one would expect 5 or more tumors/person or a total of perhaps 100
tumors. Tamplin and Cochran argue that under the most frequent, circumstances
of contemination they estimate the Pu particle masses would be -0.01 that or
a standard hot particle. Hence they discard tnis evidence.
Since this could be the most direct source of information on lung tumor
induction by hot particles in numans thau we shall have for a decade, I would
think every effort should be made to use it. Should not someone (perhaps an
ASC lab?) repeat tne contamination experiments (sans human lungs!), measure the
particle size distributiona and from these estimate tne prooabie numbers of
various size particles (in pCi) in the lungs? (Particles of ^diameter
Eight classify as hot particles.) Hot particles being a few percent of the
total radioactivity or a fraction of a percent of the total number of particles
wcJjlLd give an expectation of more than one lung tumor in this population under
"^amplin and Cochran1s hypothesis.
-------
238 ..-.-..
Rnndolpn
;•;;• C. KIKOS (?) TErtSr.'ICAL CONSIDE?.ATIO::3
. '•' (nore or less in or^er of npronrnncc in Toniplin and Cochran's report)
1^ p. 7 For 1 Jim din-ioter spherical J'PuG2 porticloo, using Pill. 5
:/gm/cn and ti« 89 years, I net around j.j ratner unan 2.2 dicintc^retions/oeo.
• . 2. p. 11 I acree that AIT, nnrt/or SPA regulations should include and clearly
delineate standards for both radiation workoro and 'population at large. (I
, thought the regulations did covnr both groups.)
"• j. p. u.. I would hnvo ' thought that D?;oTiouldjiiko RES 1 be 'defined as: " ' ''
Dose of standard (uniform)rndiaiibii5
' * '
'• ,,-BPs __ _
Dose 01 test (nonuniforir.) radiation needed to produce sane effect
• •
Inis is numerically' equivalent to what Taraplin and Cochran give only for linear
•-dose chqes response.
4. p.?io, linos 7-S "nore than 8 orders of magnitude". I get (11 x 103)/(3 x 10""4)
-s-4 x 10 , or more than 7 orders 01 cagriii,ude.
5. p. 17 line 1. I get (16 x 10~9)/(2.8 x 1CT13) ^ 57,000 instead of
53,000 particles.
6. ^p. 24-2b. I would have thought one should cor.pare the nusber of cells
•at risH «ith electron irradiation versus tnose at risic with hot particle
Irradiation. "••....
7. p. 33. How reliable is Geesaman's statement that lung repair vise is
•«ii' *li« order of one year?
8. p. 33. ."He-: --"accept' as guidance that this enhanced cancer risXT occurs
-vhen particj.es irradiate the surrounding lung tissue at a dose rate of 1CCO ren/yr
or more". At sone dose level (perhaps. aoove 5000 rec/yr) cancer risk nay
•decrease (e.g. Albert et si's data) because of cell killing.
9. p. 4*S. 1 would think (a) inclusion of "of other radionuclide" at
least superficially sounds good, (b) Addition 01' lung hot particle burden
limit seems good if this really is a najor problec>^Ce) Likewise estabiisrung
-criteria for other cases of hot particle releases sdeaT^k,.
10. Kowhe-e2dg I see ncntion or („) gibility that ^PuOg particles
nay "creep" *=a ^Po is well knovrn to do from recoil as alphas are"eniv«,ed
(for Pu this rcay be snail because of much greater, half-life); (b) possible — --- v,
importance of PuO£ conoenvranion in thoracic lymph nodes.
. D. APPENDIX. TENTATIVE ESTH-IATE 0? r^XIMW: P2R;-'JSSIELE LUNU autuwi
here we use Bair's (Adv. Radiation Biology A , Lett, Adler and Zelle, Eds.,
Aeederaic Press, ly/4, p. lOp, especially p. 305) compilation of expericental
data to estiisate the tunor risk assooia^ea wi-cn hot. parxicle inhalation
sufficient to give various lung doses to experimental aninals. Replottir.g
(roughly) Bair's compilation on log-log paper we find that all the experimental
date lie below tne line "C" and all but two points below the line "R".
Equations for. these lines in terns of the probaoiiity (T) of tunors and cumula-
tive lung dose (D) are: •
Tc si D/lO2 f f or D ^r 100 rads
. ' JK 1 for D 2 100 rads
... Tr =»D/10 for D.£. 10^ redd
: • x 1 f or D ^ 103rads .
-------
l*v tnis conservative or ronson.nblo criteria tho cunulntive dono at T = 1/2000
Is either 0.0> rnnr, or u.5 rnds. Anauralnft that nil the no done a oro Bccuraulatod
over a 3 vonr period n:nl tnnt 1 Hot particle diaxuZtx. ^.ivoa n doso of 2.7 x 10~
radsAvnr" in o 1000 rT«m nun-m umc (thio value x (!):•'» 10 ) Rives Tnjr.plin and
Cochran's vnluo given' in thoir Table III), • vfe £cf 60° or 6°°° Partlcle3
versus Taraplin and Cochron's 2. • .
One micht assure that tne pronaoillty of a lunc tumor is dependent only
on the nucbcr of hot particles in the lung. '!»,„ c,,^,ulative dose (D) for
0.28 pCi^'Pu02 particles we calculate as: .
(energy, in ergsj* depodted) 1
D e» (number oi hot ptor«.icles) x - x -
(hot particle x years) (rcass of xung in gna
(rad-ga)
x (years of energy deposition) x - - • st « (2.7)Y / 100 M
(100 erg)
where N, Y, and M are the number of hot particles, years 01 tsAp^sure, and lung
nass. '.-Ie take 1 cs. "2. years for rodents and 10 years for dogs, ana tne lung
Basses as rice 0.5 gms, rats 3 cms, and dogs 100 gas. VJe then calculate 1.' fln^
replot in Fig. 2 the sane data in terras of log tunor incidence versus log N.
L^es^ extrapolation reveals that T-=*0.000$ at around 25 hot particles, which
.suggests xnat uhe maximum permissible lung burden should be reduced by a factor
of about 10^. "JJlf V°ry tentatiya conclusion is questionable on such grounds
•as: v"a) wny is sensitivity to '9Puv$il points for "bich in Fig. 2 would
.appear at less tnan lu panicle^) so different from ^yPu? (b) numbers of hot
particles should be calculated more precisely from real size estimates rather
than assuming l>tra diameters; (c) is it fair to extrapolate from mouse to rat
to dog to nan when the dog ana rodent data seem to differ by an order of
magnitude in number of particles at maxima) effect?
-------
LOGARITHMIC 46 752O
3 X S CYCLES MM>[ IN U.S.A.
Q VH 0,
o
~
10
2 3 4567891 2 3 4567891
' o) X 7?ap^ ratc
4 567891 2 34 567891 2 3 4567891
ro
/O 1
9
3
7
6
1
^,-M
-A-
zEzf
-------
*0f
o/
r
r
-H-
.„
Jj—-!-!
-rt-
••ui. <
IpT
Zu..
±±
/2V-,: i
&8£-z, [.I
i
J_._^
I -I ;
-|—}-r-
7"P—7
:I11__|Q
LL:,U,
r-pT-
"rrrj-UJ—'.
IJ H -14±
-4-
11
_LL
4-J44
-+-I-- |-
4-hl-
-4~M-
±trit
tl,
t-t
iQ
rr
:-rr
TTTT:
"T
_L_
I I
V;
f
s
9
8
v°'
I 6 8 i 9 £ f £ Z
1 68 i 9 S
16 8 i 9 S
168 i 9 S fr £ Z
168 i 9 S fr £
-------
r" \VUed f\ fcui'vpbv j D'-V i ov^i 04; \raalQ--\-('on ^JoS€ -PhOKTn in'
. I ..J- . \ " / / I 1^ C.U I n "\ ^1 IQOj <' I .
August 18, 1974
Louis Hempclffann Response to the Tamplln-Cochran Report on Radiation
Standards for Hot Particles (February 14, 1974.)
misleadinC information of the
h thnt nolr ™d his associates at
have concluded that non-uniform irradiation of tho lunr is clearly more
r^rL^M
W^-t.^^bli.hed) that co,en to the exact opposite Tonllu Ion
-2 they imply that Mr. Edward Gleanon's synovial sarcoma of the hand was the
result of Accidental plutoniur, contamination by a leaking plutoniun carboy but
I'll no evidence that the plutoniun penetrated the skin. Plutoniun could have
reached the synovial s.-.cath only by way of a deep penetrating wound which !'-
Gleason would have purely remembered. Thousands of plutonium workers have had
contair.ina.cd wounds sor.otimos incompletely excised without developing cancer
" ^ ^^ *» *«*
3. They quote the Lushb8uSh-LanRhnn paper as proof that a sinple plutoniun
particle containing 5 nCi of activity can cause cancer. The papeV actuaUy
po ints out the similarity of tho cellular reaction^ the vicinity of the particle
ana precancerous channes in epidermal tissue and raises^he Question as to ke
ultimate fate of the lesion if it were not excised. One of^the. Los Alamos workers
has had sLx nannocuries of plutoniua embedded in the skin of his'hand for 30
years without developing cancer. -^-^'
Tarnplin and Cochran nake the following assuaptions that I do not agree with
•or cannot understand:
1. They assume that the Albert data (1967) on skin cancer induced by exposure
of large areas of rat skin (up to 24 cn^) can be applied directly to snail volunes
of huEan lung irradiated by point sources. In the first place, the skin cancers
ere derived from atrophic hair follicles and there are no comparable archi-
tectural structures in human lung. The original data cannot even be applied ouanti-
tatively to Kouse skin (Albert, 1972) or to other strains of rats (Albert 1961)
"-" LOSS to hi;-in 1 ung.
iiu-lti Tho derivation of the risk value for lung cancer of 10~3 - 10"^ per single
hot particle is incomprehensible to ne, even though I have read tho passa-e at
-ist t— tiiro-,. It seems to IEO that they jump from a risk value for skin cancer
in rats of 2-4 x 10 •> per attophic hair follicle to a risk of lung cancer in
man of 10--> to 10~^ per hot particle. There is no justification of the assumption
uoth rish values are of the sarr,e order of magnitude.
3. The lung burdens of the 25 Rocky Flat workers most heavily exposed to the
T^vtoniun fires range from the presently accepted values for maximum permissible
_, juraou to ten tiroes this value. These burdens are 115,000 to 1,500,000
times larger than the permissible lung burdens recorunended by Tamplin and Cochran.
veil known that the higher the dose, the shorter tho latent period for tumor
induction. Since lung cancers have been reported in uranium minors after a
latent period of less than ten years, we would certainly expoct to find many
lung tur.ore^ resulting from the nine year exposure of Rocky Flats personnel if
the true MPLS were of the order of magnitude recommended by Taraplin and Cochran.
4. Tanplin and Cochran dismiss the data on Los Alamos pluton'ium workers with*
measurable lung burdens for 30 ysara as not pertinent to tho "hot" particlo problem
Assuning that all exposures were duo to inhalation of droplets of a plutonium
-------
Hempelmann
solution involved in one chemical operation, they make a simple calculation to
show thnt none of the inhnlod droplets contained enough plutoniura to be considered
as hot particles (more thnn 0.07 pCi). lining a much more sophisticated calculation
involving particle size distribution of plutonium particles collected under working
conditions, Los Alamos scientists estimated that each person could have inhaled
'as many as 4 x 105 hot particles (E.G. Anderson, personal communication). If the
Tenplin and Cochrnn risk valuo of 10""* were correct, we would have expected 40
lung cancers per nan. Instead no cases of cancer have occurred in the 30 years
since the inhalation of the radioactivity.
There is good 'experimental evidence that non-uniform irradiation of rat skin
by beta rays or of hamster lung by alpha rays or ret lung by beta rays is leos
carcinogenic than uniform irradiation with the same doses. Reference is made to
the following experiments :
1. Irradiation of rat skin by the same dose of beta rays from point sources of
different strength or from a uniform flat source (Fassanneau e.^ al, 1952).
2. Irradiation of hamster lung by alpha rays from polonium^ in solution or
absorbed on hematite particles (Grossman et al, 1971; Little et al, 1973).
3. Irradiation of hamster lung by alpha particles from Pu^^^ in zirconium
oxide rcicrospheres embedded in pulmonary cappillaries (Richmond et al, 1970;
E.G. Anderson , personal communication). -,,.
4. Irradiation of rat lung by beta rays from Ba SO^ in a relatively uniform
manner and from Sr' embedded in glass beads (Cember and Watson, 1958 a and b).
The results of all these studies definitely contradict the simplistic
ncdels of Geesaman ^.1965; and Dean and Langhan (1969), which assume that lucor
induction can be calculated solely on the basis of cellular radiation exposure.
In conclusion, the question of hot particles and non-uniform radiation has
been thoroughly considered on a number of occasions by committees of knowledgeable
scientists of the ICRP, NP.CP end NAS-KRC. On the basis of the evidence or
assumptions presented in the Tamplin-Cochran Report, I see no reason to modify
the current standards of radiation protection recommended by these committees.
Respectfully submitted
References not in Tamplin-Cochran Report:
Albert, R.E., Burns, F.J. and Hermback, R.P. Radiation Research 1967 30:590.
Albert, R.E., Newman, W. and Anshuler, B. Rad. Res. 1961, 15: £10.
Albert, R.E., Burns, F.J. and Bennett, P. J. Nat. Cane. Inst. 1972 £9: 1131.
Anderson, Z.C., Ha Hand, L.M., Frine, J.R. and Richmond, C.R. To be published
in the Proceedings of the Symposium on Experimental Respiratory Carcinogenesis
and Bioassays held at the Battelle Seattle Research Center, June 23-26, 1974.
Cumber, H. and Watson, J.A. Amer. Indust. Hygiene 1958a, 19: 36.
Cumber, H. and Watson, J.S. AKA Arch. Induct. Eealth 1958b, 14: 230.
Grossman, B.N., Little, J.B. and O'Toole, W.F. Rad. Res. 47: 253 (abstract).
Little, J.B., Grossman, B.N. end O'Toole, W.F. In: Radiation Carcino^er.esis
(C.L. Sanders, J.E. Ballcw and D.D. Mahlvm, Eds.) Cont. 720503: 19
AEC Symposium Series no. 29 1973
Richmond, C.R., Langhsm, J. and Stone, R.S. Health Physics 1970, 18: 401.
-------
raiments on "Radiation Standards for Hot Particles" by A.R. Tamplin and
T.B. Cochran
(Comments by Andrew M. Rauth)
My general reaction in reading this report was that it was well written
and informative. I would like to read the opinions of those workers whose
• data is cited to the final conclusion that the Maximum Permissable Lung
Particle Burden (MPLPB) be set .at 2 particles. My reservations are based
on the fact that none of the data cited is the experimental work of the
authors A.R. Tamplin or T.B. Cochran. Since this report is a synthesis and
interpretation of the work of others, it is subject to a greater possibility
of out of context statements than a single scientific presentation of the
authors' own work. The following specific points struck nne as important.
On page 13, the authors wish to calculate the dose eJjeiivalent (DE) for
239
Pu which they say is obtained by multiplying the absozfoed dose in rads
by the modifying Quality Factor (QF) for Plutonium a particles of 10 and
a Distribution Factor (DF.) which is presently taken as 1 for the lung, but
which the authors indicate should be 115^000. As far as H can see this
choice of increase in DF is based primarily on two experimental pieces of
information, the work of Albert and coworkers cited on pages 22-24 on
239
electron irradiation of rat skin, and the work of Bair on Pu 0, inhalation
in Beagles, which together are interpreted to indicate one hot particle has
a 1/1000 to 1/10,000 chance of causing cancer when trapped in the lung.
The authors make no comments on the Albert data OEI the facts that
' 2
1) this is a macroscopic tissue irradiation (24 cm ) in a single
acute dose.
2) Not only docs the tumor incidence go up at 1,000 rads, but it also
goes down at doses above 2,000 rads.
The insoluble hot particle problem the authors deal with is one of very small
(100 ydiameter) radiation fields subject to chronic rather than acute irradiation.
-------
-2-
Rauth 245
4
In addition high radiation doses to microscopic tissue areas might cause
cell sterilization as well as carcinogenic changes. In light of these
problems their paraphrase of the "Geesaman hypothesis," on p. 26 that gives
a chance of a cancerous change of 10~ to 10 for critical volume high dose
irradiation may or may not be valid. For example, radiation therapy patients
receive'large skin'doses during fractionated radiation without skin tumors • • "• '•-.-•
appearing.
030
Bair's work with Beagles and Pu 0 inhalation is also of interest in
this regard. His work (ref. 54, Park et al) is part of a whole series of
papers appearing together in Health Physics on this problem. (22, pp.533-957)
As the authors point out, the smallest bu-rden (at death) in a dog showing
lung cancer was 0.2 yCi which was estimated to be a particle burden of
about 10 particles, a very large number in relation to the proposed limits
in man. As indicated in this article (ref.54), studies were underway in
1972 on lower burdens down tc .002 jiCi which may in time £,1ve. some dose
dependence data. It is also of interest in this paper that a great deal
of concern is expressed about dosage to draining lymph nodes as well as lung.
Obviously one can argue further pros and cons on much of the data cited.
The conclusion I came to after such superficial considerations is,
1) The authors Tamplin and Cochran have delineated a potentially
important radiation protection area.
2) Like many such controversial areas, the final decision on exposure
standards should be based,in part,on the recommendations of people
actually working in the field who have first hand knowledge of the data.
3) I could support the concern implicit in the report qualitatively but
not quantitatively on the basis of the data presented. Obviously the
least risk is no exposure, but this must be balanced out by practical
benefits. No indication of the practicability of the proposed limits
-------
246 Rauth
is indicated.
4) A broader base of informed scientific support should accompany
this report before its detailed recommendations should be submitted
for serious consideration. For example, what do people whose
papers appear in the Hanford Symposium (Health Physics 22.533.1972)
•.'say-about such a proposal?' ' "•• '• ''•''• ;< •••'.' • "".
-------
2-47
REVIEW OF REPORT ON RADIATION STANDARDS FOR HOT PARTICLES
By Arthur R. Tamplin and Thomas B. Cochran
(Comments by Afthuf Cole)
i
.The authors of the report present a valid statement that hot particle
exposure guides should not be based on standards established for uniform radiation
exposures. In spite of the fact that many specific assumptions and extrapola-
tions do not appear to be justified, the data which they cite certainly
suggests that a reduction in the present standards is indicated.
TliCM-e are a number of specific points in the report that are of particular
*
interest.
• P. 26. The "critical architectural unit" is an attractive and simplifying
hypothesis. However, little evidence is available to support it. For example,
multiple insults at different sites can be invoked in carcinogcnccic.
Pp. 27-28. The Lushbaugh study of'one observed lesion in 1,000 puncture
wounds provides no statistical basis for estimating a tumor induction proba-
bility.
P. 36. The Mann and Kirchner study summarized in Table V probably repre-
sents the most critical source of human data available, and an effort should
'be made to follow up these studies, including those personnel exposed at lower
levels.
P. Vl. Section VII. To say that the existiJig evidence "strongly
suggests that a (single) hot particle represents a (cancer) risk of
-3 -U ~ ' ••
10 and 10 n, is not justified. Present available data appears to suggest
-3 -6
a possible range of between 10 and 10 .
I was curious to play with some numbers in a naive way to compare with
*•
the sort of numerology given in the report. For example, Albert's data
-------
248
Cole
-2-
(Radiat. Res. 30:515) indicates that, at the optimum induction dose of about
2
2 krads, 5 tumors were induced per 2k cm skin exposed to short range electrons.
If we assume a sensitive (critical ?) tissue thickness of 0.2 mm., this gives
0.5 g. of tissue at risk. This comes to 1 tumor induced per 10 g. of tissue
at risk (2 krad dose). A very general and poorly Justified extrapolation of
this result might be applied to lung aveoli exposure by an "ideal" hot particle
that delivers an optimum dose to comparably sensitive cells. If the pa-tide
were attached to the inner surface of an aveoli having an inner diameter of
about 150 nm (filled with air), the total tissue mass exposed to alpha
particles would be about 10"-' g., assuming a 50 fan. particle range in unit
density. Thus, Albert's data suggests that; Aveoli tumors "per ideal hot
particle = 10"^ g. sensitive tissue
10"' g. sensitive tissue per tumor
Imposing a Quality Factor of from one to ten for tumor induction by high LET
_4
a-particles gives a range for tumors induced per ideal hot particle of 10
to 10~^, which is in agreement with Geesaman's assumption. However, this
probability applies to those hot particles which deliver optimal tumorogenic
doses and which are ideally located within critical structures. Presumably,
other doses or locations would yield smaller probabilities.
Blair's data is more directly applicable to the problem, although a
different kind of extrapolation must be made. Essentially all the dogs
7
developed (multicentric) tumors after exposures of 10 hot particles and
greater. If we assume that a reasonably large probability (approaching unity)
6
would still occur for only 10 hot particles per dog and also assume a linear
induction response, then the probability for tumor induction per hot particle
-------
-3- "" 249
would be in the order of 10~ . On the basis of this experiment alone, one
would like to limit hot particles per man to 10 for occupational exposures
2
and 10 for general population exposures in order to safely restrict the chance
-3 k
for tumor induction to 10 and 10 in each category. This represents a
reduction of about 50 fold in current standards. . '.
I recently discussed the hot particle problem with Dr. Doris Dugas and
Gerry Huth at UCLA and have enclosed a letter which they had submitted to
Science in addition to Dr. Dugas1 personal review of the Tamplin-Cochran
report. I think these comments are useful and pertinent.
Final comments: It is obvious that more experimental work need be done.
A dog experiment at lower burden levels would certainly l>e "appropriate.
Particle size effects should be reevaluated. The double trauma hypothesis
of Huth and Dugas should be considered. Hopefully, the personnel exposed
to the Rocky Flats accident will be monitored. In addition, a rather simple
study of cell transformation- in cell culture induced by hot particles attached
to the culture vessel would be a useful adjunct to the animal studies.
-------
CONCERNING THE REPORT "RADIATION STANDARDS FOR HOT PARTICLES"
A,R. Tamplin and T.B. Cochran, NRDC, February 14, 1974
(Comments by Doris J. Dugas)
General Comment: The basic intention of the report is a
valid one, namely to re-evaluate the maximum permissible
lung burden for the special case of inhaled insoluble
alpha-emitting particles. However, the data presented by
this report does not adequately support the quantitative
conclusions. Specific reasons are given below.
Section V-A, p. 22 : The Geesaman hypothesis generalizes
too much from R.E. Albert's experimental data on rat skin.
While it is true that the number of tumors and number of
atrophied hairs were correlated, this does not necessarily
mean that one was causative of the other. (We do not know
what event caused the hair follicles to atrophy.) Further-
more, even if we accept the hair follicle as the "critical
structure" and the ratio of number of tumors/number of
atrophied hair follicles as a measure of tumor risk for
rat skin, how can this be applied to areas of the body
which are not hairy (such as the lung) and therefore have
none of the so-called critical structures?
-------
251
V-B, p, 26; The case of a man who had a puncture wound
contaminated with ,005 }jCi of plutonium-239 is cited,
Cytological changes suspicious of cancer were observed
near the radioactive particle. Since there were le:ss •"
than 1000 other cases of contaminated wounds at the time,
and apparently no others developed tumors, the authors
deduce that the risk of cancer from plutonium contaminated
wounds in man must be <-< QQQ, or something > .001/particle,
Obviously, with only one case reported, there is little
justification for establishing this as a statistical risk.
V-C, p. 29: The various animal experiments show that
internal radioactivity can cause cancer, but do little
to help quantify the risk per particle. From the authors'
own figures, the risk calculated from the beagle dog data
is some unknown amount greater than 1/10 . What they
should be saying, I think, is that the risk/particle is
one if_ the particle is located in the right place, and what
needs to be determined is the probability of a particle
being located in that place,
VI, p. 32: The statement that epithelial tissue repair
time in the lung in one year was not really established
by Phillip's experiment, because no damage was observed
in one year. Yet this figure is a critical part of their
-2-
-------
252
calculation of risk/particle,
VI-A, p. 42: The calculation of numbers of particles in
plutonium workers from whole body counting seems unnecessary,
especially after the statement that most particles will be
located in the lymph nodes anyway. In aggregate, the
particles may be delivering high doses to "be nodes, and
it would not matter if each particle "qualified as hot"
individually in size or activity.
Table VI, p. A3: The calculation of risk/particle assumes
three things:
1) That 1 cancer occurs ,per 1000 to 10,000 critical
structures irradiated. This is taken from Albert's data
on 3-irradiated rat skin.
2) That 1 year is the repair time for lung epithelium.
This is Geesaman's interpretation of Phillip's experiment.
3) That 1000- rem is the critical dose to tissue to
induce cancer. This is from Albert's data.
Although the author's allow a factor of 10 uncertainty in
the first assumption, I believe that there may be one or
more orders of magnitude uncertainty in each of the assumptions,
which when combined, give a tremendous uncertainty in the
final calculation of permissible burden. The author's also
-3- '
-------
253
implicitly assume that each, particle acts independently,
which seems contrary to the evidence that most of the
inhaled particles move to the tracheobronchial lymph nodes,
forming an aggregate source,
In summary then, it seems to me that the author's quan-
titative result for the maximum permissible particle burden
.as calculated from this data is highly suspect. However,
I would again emphasize that their basic tenet is sound,
;i,e, that current MPLB's which are based on average organ
doses, are not valid for inhaled radioactive particles.
Further investigations should be made to establish appropriate
standards for such particles.
-4-
-------
254
Richard P. Spencer COMMENTS ON STANDARDS FOR HOT PARTICLES
The crucial point £s summarized on page 6 of the "Petition To Amend
Radiation Protection Standards'As They Apply To Hot Particles", in that
"... the risk of cancer from a single hot particle in the lung should be
considered equal to one chance in 2,000." The entire discussion comes
down to whether non-uniform radiation to the lungs is more or less dangerous
to the recipient than uniform radiation.
A. An intense local radiation dose would likely^fciil adjacent cells.
B. Slightly more peripheral cells, damaged by the radiation, could
likely become carcinogenic. "^"•-<-.
"">--.
A human experiment to look at this, has (unfortunately) been carried out."
I am referring to the plutonium fire at Rocky Flats (October 15, 1965).
Since it has been nearly 9 years since that accident, there might be a
wealth of data on the individuals (and lung biopsies would be invaluable).
The mass of evidence, that the permissible hot particle load in the lungs
should be revised downward is impressive. We urgently need any and all data
on the individuals exposed at Rocky Flats in order to render a final view..
-------
UNIVERSITY OF CALIFORNIA
LOS ALAMOS SCIENTIFIC LABORATORY
(CONTRACT W-7405-ENO-36)
P. O. Box 1663
Lot Alamos, New Mexico 87544
IN REPLY
H November 22, 1974
REFER TO:
Dr. William A. Mills
Director, Criteria & Standards Division (HM-560)
Office of Radiation Programs, EPA
Waterside. Mall, E-635
401 M Street, S. W.
Washington, D. C. 20460
Dear Dr. Mills:
In view of the hearings to be conducted by the Office of Radia-
tion Programs of the Environmental Protection Agency to consider
whether new guidelines or standards for transuranium elements are
needed, I wanted to inform you of several items which will not be
completed in time for consideration but which may be of interest.
The first is an analysis of the report submitted by Drs. A. Tamplin
and T. Cochran in support of the NRDC petition to lower limits for
insoluble alpha emitting particles. This is now being printed and
initial copies will be available about the first week in December.
We will send you several copies as soon as they are available.
The second item is the publication of the symposium, "Plutonium -
Health Implications for Man, " which was held at Los Alamos at the
end of May. We were very pleased to have the participation of indi-
viduals from EPA and believe that the papers and discussions at that
meeting could be pertinent to your objectives. Unfortunately, the
material will not go to the publishers until about the middle of
December and it will be about five months later before it will appear
in "Health Physics." If, in the meantime, there is any of the materi.
from that symposium that would be useful to you in your deliberations
we would be happy to cooperate.
While we do not plan to present a statement at your hearings,
we do plan to have a representative present. If he can be of any
use to you, please call on him.
« Sincerely yours,
J. W. Healy
JWH/ed
AN EQUAL OPPORTUNITY EMPLOYER
-------
256 UNIVERSITY OF CALIFORNIA
LOS ALAMOS SCIENTIFIC LABORATORY
(CONTRACT W-7405-ENO-36)
P. O. Box 1663
Lot Alamo., New Mexico 87544
IN REPLY
REPER TO: H December 24, 1974
Dr. William A. Mills
Criteria and Standards Division
U. S. Environmental Protection Agency
401 M Street, S. W.
Washington, D. C. 20460
Dear Bill:
I am submitting the enclosed report, "A Proposed Interim Stand-
ard for Plutonium in Soils," LA-5483-MS, for inclusion in the record
of your hearings on plutonium. I plan to continue work in this area
and will be extremely interested in the conclusions of your hearing
panel and the actions of EPA.
I am also enclosing a copy of LA-5810-MS, "A Review of the Nat-
ural Resources Defense Council Petition Concerning Limits for In-
soluble Alpha Emitters," which Chet Richmond mentioned in his letter
of December 17, 1974.
Sincerely yours,
Hi. W. Healy
JWH/ed
Enclosures: a/s
AN EQUAL OPPORTUNITY EMPLOYER
-------
259
A PROPOSED INTERIM STANDARD FOR PLUTONIUMalN SOILS
by
J. W. Healy
ABSTRACT
Current standards for controlling health effects from plutonium in
the body are discussed. Available information on possible sources of
exposure of people living in an area where the soils are contaminated
with plutonium is analyzed to arrive at estimates of intake. From these
estimates, a recommended interim "standard for the upper limit of con-
centration of plutonium in the soils in inhabited areas is derived. The
recommendation is based upon conservative assumptions where infor-
mation is lacking and further studies should result in revision. The
subjects of resuspension, deposition velocity of particles and effec-
tiveness of radioactive particulates in producing lung cancer are dis-
cussed in appendices.
I. INTRODUCTION
Plutonium has been utilized and processed in
relatively large quantities (hundreds to thousands of
kilograms total) in several different|countries over
the past three decades. It now can be found in
small quantities in soils and oceans over the entire
world as a result of widespread dissemination from
nuclear weapons tests in the atmosphere and one
burn-up of a space nuclear power generator con-
taining S3f Pu. More localized distributions are
found in the immediate vicinity of facilities used
for processing plutonium, at the locale of several
accidents involving weapons containing plutonium,
and in remote areas which were used for safety
tests' with weapons. In each of these areas, some
measure of potential hazard is necessary to enable
adequate decisions as to future disposition of the
area or any special considerations on habitation or
land use restrictions. Thus, it is necessary to
have some indication of the degree of hazard asso-
ciated with various levels of plutonium so that such
decisions can be adequately based.
The following study was commissioned by the
Division of Operational Safety of the U. S. Atomic
Energy Commission to provide an interim or pro-
visional standard for plutonium in the soil to meet
this need. It was recognized that the problem of
establishing such a standard is very complex due
to the many potential mechanisms of exposure
from this source and that the data available for de-
tailed definition of the problem are inadequate.
However, the necessity of making decisions on
acceptable levels requires that some guidance be
made available for comparison with measurements
made in potentially contaminated areas. To an-
swer this need, it was decided to apply the infor-
mation now available and to arrive at a standard
which, while overly conservative from a hazard
-------
260
standpoint, would give some guidance in making
these decisions. At the same time, it was felt that
such a study would permit assessment of the infor-
mation available so that future research and devel-
opment programs could be more effectively aimed
at the areas of greatest uncertainty.
It is stressed that a conscious effort has been
made to err on the conservative side in view of the
many uncertainties. (In this case, the conservative
side is defined as the over-estimation of exposure
from the plutonium in the soils. ) In addition, the
V
depth of investigatipn and the conditions considered
i» H
have been limited in a number 'of possibly important
areas in an attempt to arrive at some guidance as
soon as possible. For these reasons, it is urged
that the numerical values derived herein be re-
garded as truly provisional and not be incorporated
into rules and regulations which are difficult to
change. It is anticipated that changes in the num-
bers, and perhaps the concepts, will be forthcom-
i
ing from future work.
In the derivation of the numerical guidance, we
have considered primarily considerations of health
and hazard to man. In recent years there has been
a tendency to derive such standards based upon the
practicality of achievement rather than upon effects
on health. While such standards have their rightful
place in providing control of sources of pollution,
there is a tendency to regard them as safety stan-
dards so that exceeding them becomes a matter of
great concern. It is also of importance, even on
the practicality basis, that an upper limit be clear-
ly established, as based on safety, so that one can
assure that the practical limits are, indeed, safe,
and that the additional margin of safety attained by
lower limits can be assessed in comparison to the
qosts in resources and manpower of achieving them.
With this philosophy we have not provided two stan-
dards, one for control of sources on a continuing
basis' and one for the application of countermea-
sures in an area already contaminated, although
such considerations are appropriate to any safety
program and in the application of a standard such
as the one derived here. Again, as better infor-
mation becomes available and we reach a stage
where intelligent and informed assessment of actual
risks at various levels of plutonium in the soils are
possible, such considerations will be included.
Supplemental information on several items
not covered in detail in the literature are given in
appendices. These include a model for calculating
resuspension of particulates in Appendix A, a treat-
ment of the deposition velocity for particles in Ap-
pendix B, and a discussion of the effectiveness of
radioactive particles in producing lung cancer in
Appendix C.
II. PLUTONIUM STANDARDS
A. Properties
Plutonium is not a simple material. It is a
man-made element in which the isotopic composi-
tion, and thus, the radioactive properties, vary
widely depending upon the history of its production
and any subsequent neutron exposure as a reactor
fuel or in a detonation. There is increasing evi-
dence that the metabolic behavior and, in some
situations, the gross chemical behavior may vary
with specific activity of the isotope probably be-
cause of the influence of the energy emitted as ra-
diation as well as mass effects. The isotopic com-
positions of several typical mixtures are given in
Table I.
The compositions given in Table I are illus-
trative rather than definitive with wide variations
possible, particularly in the materials used for
power fuels. The low irradiation material is rea-
sonably representative of that used in the weapons
programs of the AEC which has utilized a large
fraction of the plutonium produced in the past.
Since the isotopes of plutonium are primarily
alpha emitters with little accompanying penetrat-
ing radiations, the hazard associated with pluto-
nium is almost completely due to potential intake
into-the body. Plutonium-Z41 is a beta emitter but,
-------
TABLE I
PLUTONIUM MIXTURES
261
Isotope
236 pu
238pu
S39Pu
S40pu
:=S41Pu
242 Pu
244 Pu
Specific
Specific
Principal
Emission
a
a
a
a
p(0. 02McV)
a
a
activity1' (alpha) of
Specific
Tj1 Activity
. yi-s Ci/g
2. 85
86.4
24, 390
6, 580
13. 2
3.79x10° 3.
7,'oxlO7 1.
mixture (Ci/g)
532
17.4
0. 0614
0. 226
112
9x 10~3
9x 10~ 5
activity with 34lAm ingrowth (Ci/g)
Low
Irradiation
wt%
--
0.
93.
5.
0.
0.
0.
0.
0.
•--
0115
6
9
4
013
02
073
084
Pu Recycle
in LWR
wt%
5x 1C
2.
39.
25.
16.
. 15.
0.
1.
,-6
9
6
6
8
0
059
08
Heat3
Source
wt%
10-
80.
15.
3.
0.
14
14
4
3
87
00
72
-
* Daughter is E4lAm, an alpha emitter, with half-life of 458 years and a specific activity of 3. 24 Ci/g.
This will reach a maximum from the 241Pu in about 70 years with one gram of E41 Pu resulting in
2.91 Ci of 841Am.
again, the energy of the beta particle is low enough
that self-absorption and small penetration into the
body makes the external dose insignificant. It is
true that massive quantities of plutonium, as en-
countered in fuel fabrication plants or other facil-
ities handling large quantities of plutonium, pose
some problems in control of external exposures to
workers, particularly as the quantities of isotopes
of higher mass than 239 increase in heavily irra-
diated fuel materials. However, in the quantities
expected in soils, these external radiations are of
no significance in comparison to an internal uptake.
Thus, our concern with the properties of plutonium
is limited to those which will influence intake.
On an overview basis, plutonium is probably
not as bad an actor in the environment as rrlany
other isotopes because of its relative insolubility.
As a result, it is not taken up to any large extent in
the ecosystems so that transfer by biological mecha-
nisms is usually minimal particularly for plutonium
in soils. Although there are measurements indicat-
ing some concentration in marine organisms,3'4
none seem to indicate anything other than biological
discrimination in plants and animals on contami-
nated soils. It must be noted, however, that ex-
perience in this regard is relatively limited and
some mechanisms for biological uptake in terres-
trial situations may occur, even if only in limited
areas where the soil and biological conditions are
proper. For example, the action of natural che-
lating agents in the soils may result in compounds
which could be biologically more active. However,
with the information now available, it appears that
for purposes of this interim standard, the physical
modes of transport and intake are of the most im-
portance.
One further reservation on the behavior of a
mixture of isotopes in the environment relatels to
the eventual buildup of s41 Am. This isotope be-
gins to appear in significant quantities from241Pu
mixtures within a few months to years. While the
assumption is frequently made that all of thetrans-
uranic elements have similar metabolic behavior
(as in ICRP 2), 5 this assumption was based pri-
ma-r'ily on the need for MFC's to be used for control
purposes. The chemical properties of americium
-------
are, indeed, different from those of plutonium par-
ticularly in the tendency of plutonium to produce
insoluble polymers and one would expect the ecolog-
ical behavior to be different. Some measurements
have indicated a much higher uptake of 24lAm by
plants6 while others have shown the transfer from
plasma to milk7 to be higher than for plutonium.
Since the contaminated areas now of interest have
resulted from plutonium with low 3*JPu content,
this has not been an important consideration. As
information becpmes available, the importance of
this factor to the interim standard will he assessed.
0.
i
B. Basic Limitations on Plutonium in Humans
As a basis for the potential harm to humans
frojn the intake and deposition of plutonium we will
use the current standards as recommended by the *
NCRP and ICRP. These were basically derived for
occupational exposures and are applicable primar-
ily to adults in reasonably good health: In applica-
tion to populations they are deduced to allow for the
lower risk which should be applicable to such groups
and to provide a margin for children or ill individ-
uals. A brief review of the origin of the occupa-
tional standards is given in this section to provide
a basis for the application to population groups in
the next section. 11
It will be noted that we:have not based our
studies on estimates of the risk to individuals in
spite of the fact that this approach is advocated by
many people. Such estimates, even for low LET
radiation, require many assumptions and arebased
upon data which have a wide range of uncertainties.
As a result, the estimates reflect more the individ-
ual assumptions and interpretations than they do the
real risk. There is a wide difference between ar-
riving at a value which the evidence indicates is
"safe" without attempting to quantify this term and
in providing a quantitative, numerical value for the
risk. In the former case, the informed judgment
of people who have studied the information available
can be used. In the latter case, a mechanistic
calculation is substituted with judgments on the as-
sumptions compounding the uncertainties in the
final number. It is true that value judgments as
to "how safe is safe" are required for the non-
numerical method but the general agreement among
bodies as diverse as the NCRP,8 the ICRP, 9 and
i~
the Federal Radiation Council10 would indicate a
remarkable similarity in such value judgments in
spite of the differences in objectives and composi-
tion of these groups. In the case of alpha emitters,
^\rch as plutonium, we would also note that the un-
•'•'-'• .''•'"'•.•" ' . -^ ••,.'
certainty in the risk estimates may be greater than
for low LET radiation because of the uncertain RBE
'
to be applied and the apparent lack of repair of
damage from these high LET radiations. (Note
that the rem should not be applied in such risk es-
timates since this unit is defined for use in radia-
tion protection and uses the Quality Factor which
is arbitrarily assigned as based on a conservative
estimate of all effects. J11 The rem is intended
for iontrol of radiation exposures and not for es-
timates of risk.
1. Body Burden. The basic standard for plu-
tonium absorbed into the body (i. e., outside of the
lung or other site of initial deposition) is 0. 04(jCi
for occupational exposure. This value was derived
by biological comparison of the late effects when
inj-ected into animals with those of radium for
which a significant body of information on the ef-
fects in humans exists., A recent review of the
derivation of this value and its application to ob-
taining maximum permissible concentrations was
made by Langham and Healy.la The value re-
sulted from the work of Brues l3 at the Argonne
National Laboratory, in which known quantities of
both plutonium and radium were injected into ani-
mals and the comparative late damage noted. As-
a result of these experiments, it was determined
that the relative toxicity of plutonium is about 15
.times that of radium-226 on the basis of equal
injected doses (microcuries). In the rodents used,
the retention of plutonium was about 75% while that
-------
of radium was about 25%. On a retained basis, this
would lead to the conclusion that, plutonium is about
five times as toxic per microcurie; however, a largo
part of the energy delivered from radium results
from the radon daughters. In these animals the re-
tention of the radon was about 15-20% as compared
to about 50% for man. Thus, in man, the higher ra-
don retention would lead to expectation of increased
damage for the radium in comparison to the pluto-
nium. The relative toxicity of the plutonium per
microcurie retained would be expected to be lower
by about a factor of two or about 2.6 times that of
radon. Thus, for ma*rii, the maximum permissible
body burden is 0. 04 microcuries. However, on an
energy delivered basis, the energy from the pluto-
nium alpha particles is five times as toxic as that
from radium since the total energy from the radium
is about twice that of the plutonium in man. The in-
creased effectiveness of the plutonium energy has
been attributed to the fact that the plutonium is not
as uniformly distributed through the bone matrix as
radium (although radium is not uniformly distrib-
uted) tending to concentrate on the surfaces so that
a smaller portion, and perhaps more sensitive por-
tion, of the bone receives a higher insult. Similar
experiments performed at the same time with 89Sr
gave results similar to these and tl('4 increased ef-
fectiveness of these two materials on an energy de-
livered basis has been generalized to the "dose dis-
tribution factor" of five which has been applied to
all bone seekers except radium. '
The value of 0. 04|_iCi was first derived at, and
immediately following, the Chalk River Conference
in 194914 and still remains as the primary standard
for plutonium in the body. Additional studies with
dogs at the University of Utah15 have essentially
confirmed the number although the Utah results in-
dicate that the relative toxicity on an energy basis
may be closer to ten than five and have demonstrated
that other organs may have significant uptake and re-
tention of plutonium depending upon the path of ad-
ministration. In their experiments, the plutonium
263
was administered intravenously in a citrate solu-
tion and the liver appeared to be a major site of
deposition although the majority of late effects
noted seemed to be primarily involved with bone.
Studies of the effects of plutonium on animals con-
tinues and it is anticipated that some revision of
>
the 0. 04[iCi value may occur in the next few years,
but a major change, for reasons of health effects,
is not anticipated. (The qualification on health ef-
fects is necessary since there is a growing ten-
dency to base such standards on practicality of
attainment rather than potential damage. For ex-
ample, the FRC recommendations10 for the intake
of 228Ra and 90Sr are based on their conclusion
that operations can be carried out without exceed-
ing the recommended intake. In application of
these standards it is important to recognize the
basis. ) There are now some human data17 based '
on exposures of 27 individuals in I944;and 1945
(28 years). Estimates of the body burden byurine
analysis are uncertain, but the latest analysis of
the data indicates that 60-70% of the individuals
have plutonium burdens at or above the 0. 04 uCi
level with the maximum individual perhaps 5-10
times this value. Followup medical examinations
have shown no changes which could be attributed to this
plutonium. While the sample is small and the time
is relatively short in comparison to the life span of
man, these data are encouraging in that they indi-
cate no gross problem such as occurred with ra-
dium.
It should be noted that this derivation is based
directly on biological evidence of-damage and does
I
not utilize the concept of radiation dose except in-
directly in the comparison of energy delivered by
the two materials. There has been an attempt to
fit the derived value into the overall framework of
dose calculations with the result that the original
basis for the number and the meaning of the derived
numbers is not always clear. For example, in
their 1959 report on internal emitters,5 the ICRP
presented the concept as follows: "The effective
-------
264
RBE dose delivered to the bone from internal or ex-
ternal radiation during any 13 week period averaged
over the entire skeleton shall not exceed the aver-
age RBE dose to the skeleton due to a body burden
Of 0. ItiCi of aasRa (derived from a dose rate of
0. 06 rad/week, an RBE of 10 and n = 1). " In this
statement, n is the so-called dose distribution fac-
tor and corresponds to the value of five on an energy
basis derived from the reasoning described above
for plutonium. The dose rate from 0. lyCi ofaasRa
retained in the body was obtained assuming that 99%
of the radium in the body was in t'he bone, the min-
eralized portion of'the bone weighing 7000 grams
was the appropriate organ, 30% of the radon daugh-
ters were retained in the bone and a quality factor
of tfen was appropriate to describe the LET effects
of the alpha particles. In this calculation, 0.04|jCi
of plutonium in the body with 90% in the bone would
deliver an average dose rate of 0. 5 rads per year
to the mineralized portion of the bone or, with a
quality factor of ten and a dose distribution factor
of five, about 25 rems per year which, within the
accuracy of the estimate, is the same as the radium
value of 30 rems per year.
2. Lung Burden. The basic limitation to the
lung for workers is a dose equivalent rate of 15
rems per year as derived from Hie experience with
external radiation exposure and the application of
the critical organ concept first set forth by the
NCRP.l8 This translates, for a 1000 gram lung,
to a lung burden of 0. 016 |jCi of plutonium based on
the average dose to the entire lung. However, in
contrast to plutonium mobilized into the body which
is retained with great tenacity, the lung has elimi-
nation mechanisms which serve to remove plutonium
or other materials. As a result, the total dose de-
livered by a given deposit is limited by the time of
retention of the material in the lung. In addition,
the deposition of material in the lung is strongly
affected by a number of factors, the most impor-
tant of which is undoubtedly the effective particle
size. The ultimate fate of the material deposited
in the lung must be considered in relation to the
radiation dose received by other parts of the body.
These questions of intake and retention will be dis-
cussed in the next section of the report.
The applicability of a dose calculated on the
basis of the average dose to the lung (i. e. , total
energy delivered divided by the total weight of the
organ without regard to the distribution of the en-
ergy within the organ) is frequently questioned on
the basis that the plutonium particulates will pro-
duce "hot spots" where the local radiation dose far
exceeds the average. These high doses to limited
volumes of tissue are, then, presumed to consti-
tute a high risk. A recent review of the informa-
tion available on this question19 (reproduced here
as Appendix C) indicates that the experimental
data available, while not completely adequate for
low activity particles, strongly supports the find-
ing that the non-homogeneous distribution of dose
is probably less hazardous than the uniform dose.
Nearly all of the support for the increased effect
of single hot particles arises from theoretical cal-
culations of doses to individual cells with the cell
response assumed from experiments on other types
of cells in different configurations of dose distri-
bution. The evidence for cancer induction from
limited volume irradiation strongly indicates that
a calculation of the dose on the average organ basis
is conservative if the irradiation is from particu-
late sources. For this ,reason, we will use the
average organ dose throughout for the lung.
C. Application to Population Groups and Individ-
uals '
It is generally recommended that exposure of
population groups or individuals in the population
be limited to values below those recommended for
occupational workers. However, there are some
differences in the recommendations of various
groups as to the exact degree of reduction to apply.
A brief review is given to aid in choosing the lim-
its to be applied in this work.
-------
The ICRP position as of 1965 9 recommended
that the annual dose limits for members of the pub-
lic be one-tenth of the corresponding annual occupa-
tional limit with the exception that the thyroid dose
to children under the age of 16 be limited to 1. 5 rems
rather than the previously used 3. 0 rems. The oc-
cupational limit listed for "bone" is given as 30 rems
per year and for "all other organs" as 15 rems per
year. Thus, the dose limit for plutonium in the
body would be 0. 004uCl (assuming the rem is cal-
culated as given earlier) and the maximum quantity
in the lung would be 0. 0016|jCi. F\>r genetic expo-
sure, they recommenS a maximum of 5 rems in 30
years or an average for a population group of 0. 17
rems per year. However, for the somatic dose of
concern here, they state "--it is expected that the
dose limits for individuals will ensure that the num-
ber of somatic injuries that could possibly occur in
a population will remain at a low level. " From this,
it appears that they did not feel that a specific limit
for groups, based on somatic effects, was neces-
sary.
The current recommendations of the NCRP8
provide dose limitations based on somatic consid-
erations for individuals and for the average popu-
lation dose. These are given as: "The dose limit
for the critical organs (whole body)
The Federal Radiation Council has considered
the problem of population dose both with respect to
external radiation10 and the somatic dose fromra-
dium-226 ls specifically. For environmental con-
tamination they point out that there may be condi-
tions where the only data available may be related
to average contamination or exposure levels. They
then suggest the use of an arbitrary assumption
that the majority of individuals do not vary from
the average by a factor greater than three. From
this, and their recommendations of 0. 5 rem whole
body radiation for individuals, they obtain a value
-------
266
of 0. 17 rem for yearly whole body exposure of av-
erage population groups. They also warned that the
use of the average figure, as a substitute for evi-
dence concerning the dose to individuals is permis-
sible only when there is a probability of appreciable
homogeneity concerning the distribution of dose with-
in the population included. For radium, they re-
jected the use of the factor of ten between the occu-
pational exposure limit and that for the individual
in the population because of the differences in char-
acteristics of the child, the longer time for carci-
nogenesis and the difference in distribution of the
i * .
radium in the bone from an environmental accumu-
lation over a number of years and the acute type of
exposure from the worker exposures. They noted
that the dose to the skeleton from all natural causes
averaged between 0. 1 and 0. 15 rads per year while
the quantities of radium and its daughters required
to give comparable doses were about 0. 003 to 0. 005
|jgm. They also compared the natural occurrence
I
of radium in the skeleton which they quote to range
from about 0. OOljagm to some two 01 three times
this amount in most areas of the U. S. In consider-
ing the dose to the bone they state: "There is insuf-
ficient information on the relative biological effec-
tiveness of the radiation from radium to attempt a
realistic conversion of this dose in rads to the skel-
eton from radium and its decay products into rems."
They, thus, specifically reject the conversion of the
body burden into dose equivalent as a basis for de-
riving or expressing limits to the bone. In consid-
ering operations involving the release of radium to
the environs, they feel that such operations can be
carried out in such a manner that the avferage daily
intake in an exposed population group will not exceed
20 pg. They also quote that data on the average in-
take and average body burden indicate that the quan-
tity of radium in the adult skeleton does not exceed
a value of about fifty times the daily intake. They
then chose a value for the daily intake of 20 pg per
day as the radiation protection guide with an alter-
nate value for individuals in the general population
of 0. 003 )jg in the adult skeleton. For a suitable
sample of the exposed population, the average value
was set at 0. 001 ^ag in the adult skeleton. It can be
seen that the factor of fifty for the body burden of
the average individual as compared to the intake,
when applied to th,e RPG of 20pg/day intake, cor-
responds to the value for the average of the popu-
lation group, while the value for the individual is
three times this. Application of these values to the
plutonium case, again selecting a factor of five for
the dose distribution factor would indicate that one
could permit only 0. 0012pCi in the body of the in-
dividual or about 0. 0004[jCi in the adult skeletons
of a suitable sample of the population. However,
it is also noted that the value was selected on the
basis of a finding that operations could be conducted
with radium at this level but the same finding has
not been made for plutonium. The direct applica-
tion of this recommendation is therefore in doubt.
For the purposes of this document it appears
appropriate to consider an upper limit for deposi-
tion in the body of an individual in the population
of 0. 004\jd of plutonium and one-third of this val-
ue as applied to a suitable sample of the population
as defined by the FRC. This will result in an av-
erage dose rate to the mineralized portion of the
bone of 0. 03 to 0. 06 rads per year or, using a
quality factor of ten for the alpha particles and a
dose distribution factor of 5, a dose equivalent rate
of 1. 5 to 3 rems per year depending upon the frac-
tion of the plutonium deposited in bone as compared
to other organs. The lung dose will be based on a
limit of 1. 5 rems per year {0. 15 rads/year) calcu-
l
lated on the basis of an average dose to the entire
lung. As noted earlier, this method of calculation
is believed to be conservative in control of actual
damage.
III. UPTAKE AND RETENTION IN THE BODY
The application of the foregoing standards for
the maximum quantity permissible in the body is
usually done through "maximum permissible
-------
concentrations" (MFC's) for air and water to be
breathed or ingested. These are derived by con-
sidering the uptake and metabolic patterns of the
isotope in the body. Such MFC's have been given
primarily for occupational exposure and, for the
values currently in use, the models used for des-
cribing the retention and elimination are outdated.
For these reasons, we have chosen to review the
current information and arrive at independent as-
sessments of the proper intake levels appropriate
to the population exposure rather than to rely on
published MFC's. The reasons fo'tf this decision
are discussed in thiis'Hsection of the report along
with the derivation of values to be used.
A. Inhalation
The current MFC's recommended by the
NCRP3° and the ICRP5 were calculated by the use
of a simple lung model which dates conceptually
back to the Chalk River Conference in 1949. 14 This
model differentiates between '(soluble" and "insol-
uble" materials without, however, any definition of
the terms other than their assumed behavior in the
body. For soluble materials, it was assumed that
25% of the material is retained in the lung and ab-
sorbed rapidly into the bloodstream from which it
is deposited in other organs of the|pody, the re-
mainder is eliminated by exhalation or ciliary ac-
tion to the throat. For insoluble materials, it was
assumed that 25% is exhaled with 50% deposited in
the upper respiratory passages and subsequently
eliminated by ciliary action and swallowed. The
remaining 25% is deposited in the deep lung with
one-half of this eliminated from the lung and swal-
lowed within the first 24 hours. The remainder
(12. 5%) is retained in the lung with a half-life of
365 days (for plutonium) with this portion assumed
to be taken up by body fluids. Thus, on this model,
the inhalation of one microcurie of material will re-
sult in the deposition in the lung for long term re-
tention about 0. 125^jCi. In general, the components
retained for shorter times are ignored in the dose
2S7
calculations because of the relatively small dose
which they will deliver over the period of elimina-
tion. In this model, a deposit of 0. 016|_iCi in the
long term retention compartment will then deliver
15/X or 15x1 year/0.693 = 22 rems over the peri-
od of elimination. However, the material taken up
':t:
by body fluids remains to be accounted for. If one
assumes that all of this material goes to the blood-
stream and is later deposited according to the pat-
tern for soluble material, then the uptake to the
body becomes limiting .and not the lung dose. On
this basis, the MFC for insoluble material should
be about twice that of the soluble since the uptake
by the blood is considered to be only half of that of
the soluble. In practice,, the MFC for the soluble
material is about 0. 06 times that of the insoluble
because the insoluble value was calculated based
only on lung dose without consideration of this frac-
tion taken up into the body. *
However, it is known that not all of the mate-
rial retained by the lung eventually passes into the
bloodstream. Instead a major portion is taken up
by the lymph nodes which drain the lungs. This has
been demonstrated by autopsy on individuals '
who have inhaled plutonium as well as by animal
experiments. 2a In response to this, as well as to
improved information on the overall deposition and
retention of various materials, a Task Group work-
ing under the auspices of the ICRP24 has described
a more definitive lung model which provides in
some detail the variation in retention in various
parts of the lung with particle size and gives some
indication of the fate of the materials deposited in
I
various parts of the respiratory tract. Although
this lung model has not, as yet, been adopted by
the ICRP, and there apparently will be some changes
when issued, it is useful for indicating the relative
comparison between the older model used for cal-
culating current MFC's and these more refined
considerations. The model provides curves for
estimating deposition in three regions of the re-
spiratory tract depending upon the particle size.
-------
268
It then provides three clearance classes depending
upon the rate of pulmonary clearance: Class Y -
those materials retained in the lung for long peri-
ods, perhaps years; Class W - those materials with
intermediate retention on the order of weeks; and
Class D - those materials rapidly cleared. Classes
Y and D correspond to the "insoluble" and "soluble"
materials considered in the earlier lung models.
Although the Task Force, presumably because of
the lack of detailed studies of the behavior of vari-
ous compounds in the lung, implies that certain of
the chemical comppunds of plutonium may belong to
1,'j
Class D, the tendency of soluble compounds of plu-
tonium to hydrolyze in body fluids and, in some
forms, to produce colloidal polymers would indi-
cate that even the more soluble compounds should
be in Category W rather than D. This is at least,
partially confirmed by the studies at Hanford using
Beagle dogs in inhalation of the nitrate and the fluo-
ride. 23 Here pulmonary retention times of 100 to
I
200 days were observed.
A summary comparison of the lung modelused
by the ICRP in deriving the present MFC's with the
Task Force model for several particle sizes is
given in Table II along with the MFC's evaluated for
a worker exposed 168 hours per week. Although
the Task Group chose a value for the half-life in
the pulmonary region for the Class W plutonium of
38 days as based on early studies with nitrate, we
have retained their general ?0-day half-time for
this class on the basis of the studies with dogs cit-
ed earlier. In general, there are no really strik-
ing differences apparent in this comparison, al-
though the inclusion of the uptake in the £ody for
the insoluble calculation eliminates the former wide
discrepancy between the "soluble" and "insoluble"
•concept.
This discussion was presented to illustrate the
uncertainties which exist in estimating the deposi-
tion and transfer of material from the lung-. In gen-
eral, it is concluded that the MFC for soluble com-
pounds as calculated on the old lung model may be
somewhat conservative in estimating the buildup of
plutonium in the body. On the other hand, it does
not fully account for the final site of deposition since
both the injection experiments at Utah15 and the
inhalation experiments at Hanford23 indicate that
considerably less than 90% of the plutonium in the
body is in the bone with the liver (and lymph nodes)
as the major alternate sites of deposition. Since
the effects on the bone still predominate in the Utah
experiments, however, this partition means that
less energy will be deposited in bone compared to
that in the total body since the fractional bone de-
position is smaller. While some concern may be
felt for use of the insoluble MFC in some situa-
tions because of the lack of accounting for the
movement into the body, the results from the newer
lung model would indicate that the transfer from
the lung to the blood may be on the order of a fac-
tor of three to ten lower th'an was considered on
the older model so that overall buildup even at the
high'er MFC should not exceed the body burden li-
mits. However, it is noted that considerable un-
certainty exists with respect to the initial deposi-
tion in the lung because of the lack of data on par-
ticle sizes in the usual situation. This will be se-
rious only in the very small particle sizes where
the deposition will be increased. On the other
hand, even for particles of 0. 1 micron size, the
pulmonary deposition is predicted by the new mod-
el to be only 50%, a factor of two higher than was
used for the one micron particle. In view of the
many other uncertainties, including the uncertain-
ty in the dose limitation to the lung, such a factor
is of little real significance, particularly when the
conservative nature of the present MFC's is con-
sidered.
For application to the public, it is believed to
be inappropriate to use two limits based on the
"soluble" and "insoluble" concept without consid-
ering the interactions between the two. Possible
values of the MFC for an individual in the popula-
tion based on lung dose of 1. 5 rems per year as
10
-------
269
COMPARISON OF LUNG MODELS (INHALED BASIS)
Model
ICR? - 'Soluble"
ICRF- "Insoluble"
Pulmonary
Deposition
fa
25
25
Task Torcc - Class Y
0. lym . 50
1 urn 25
5ijm 12
Task Force'- Cl.'ius W
0. 1 -,jr.i 50
i uin it-' 25
5 ani
12
Long Term
Retention
12. 5
30
15
7. 5
30
15
7.5
'"'MFC's
Half-life
da
...
365
500
500
500
90
'90
90
To Blood
2.
12.
3.
2.
1.
10.
8.
10.
5
5 (' )
J \ • i
34
0
61
9
8
7
To Lymph
•i
(b)7.
. (b)3.
n \
' '•
(C)2.
(C)j
(c)o.
-
5
75
B
5
25
6
1 ^v
Lung
uCi/cc-
-
4x
S
2
.2
X
X
X
4x
9
X
...
10~
10"
10"
10"
10"
10"
1 1
12
12
i i
11
11
11
Body
Burden
uCi/cc
6x
6x
7x
Ix
Ix
Ix
10"
10"
10"
10"
10"
10"
10"
13
12
12
1 2
12
12
12
(a) For worker - 168 hour per week
(bj 10% of this transfers to blood with 500 da T1 . (included in blood)
(c) Tr.'insfcrs to blood v/ith 90 da T, . (included in bltood)
recommended by the ICRP, 0. 5 rems per year as
recommended by the NCRP or a total deposition of
0. 004jjCi in the body are given in Table III as
adapted from Table II.
Since it appears unlikely that there would be
significant airborne concentrations of the Class W
compounds in pure form from resuspension and pro-
cesses of agglomeration in the soil could result in
relatively large average particle sizes, an MFC in
air of 3x 10~l3 pCi/ml applicable to both classes
would appear to be appropriately conservative.
INHAI-A'J'JOM MTG'S FOK AN INDIVIDUAL IN THE
' MCi/ml
Class Y
0.1,
ttitakc
ill Body
B. Absorption from GI Tract
Plutonium is only slightly absorbed from the
GI tra!ct when ingested so that intake with foods or
other materials through this path is not usually
considered to be a limiting method of exposure.
In rats, chronic ingestion at low mass concentra-
tions of the nitrate resulted in an average uptake
of 0. 003% of that fed with 90% of the small fraction
which was absorbed deposited in the skeleton. 3S
It was estimated with a 90% confidence level that
the retention did not exceed 0. 01% in 99% of the
rats. A similar absorption of 0. 002% was noted
in pigs following feeding of pH2 nitrate solution.26
The MFC in drinking water of the NCRPS° and the
ICRP5 for so-called "soluble" plutonium is based
on an uptake of 0. 003%.
The uptake from the GI tract can be affected
by the presence of complexing agents, the valence
state of the plutonium and the age of the animal.
The variation with valence state and the presence
of citrate is shown in Table IV as obtained from
Thompson's review. 37 Thompson also reported
experiments by Carritt et al in which the absorp-
tion of nitrate in rats was increased from 0. 01%
-------
270
ABSORPTION OF PI.llTO?-'n!H FROM SEVERAL
SOLUTION'S FKD INTRAOASTHICALLY TO RATS
TABLK V
PLUTONIUM IN ORGANS OF ANIMALS
Type of Sohalon Fed
Plutonium Valence
Principal
Anicm pH
Mitral e
Nitrate
Nitrate-
Nitrate
Nitrate
Nitrate
Citrate
Cil [ .III:
CiU.ilc
in the
1
1
2
2
Z
4
2
2
2
absence
Iclcntltii.il ',',
(HI) (IV)
68
90 10
7 93
96
97
99
«,
85
I*'"'
of citrate to
4 Days
(VI) 5>cd
100 1,
0.
0.
0.
0.
0.
•1 0.
15 0.
V"
1
0. 3% with 5%
altcr Single
2S
006
005
0013
0017
03
7.9
4 1
sodium
citrate.
,In
. one day
old rats, the
absorption of plutoni-
Station
l-iVli\
Bone
dis/min
<-i JF CUNT/
CI Tract
Contents
dis /min
iMlNA
TED A
(;
Lung
dis/min
RE AS
Transferred to
Bone per Year
dis/min
Kangaroo Rats 1958
11D
13-2
Kancaroo
nn
13-3
Jiickrablii
13-1
13-2
13-3
Jackrabbi
11D1
11D2
13-3
13-5
7. 13
4. 30
Rats 1966
47. 05
2.72 .
ts_lM_B
126. -18
11. 68
1. 75
ts 1966
665.40
88.76
19.27
2. 34
2S52
1255
1050
170
5.5x \0^
3. 2x 10'
5712
4. 1 x 10"
1. 6x 10*
1360
781
11
0
61.
5.
57.
0.
0.
98.
8.
1.
0.
.40
. 12
.28
SO
50
36
24
25
92
92
10
22. 5
13.7
1
11. 5
1.9
6000
350
63
450
175
15
9
um from a. pH2 nitrate solution averaged 0. 25%. ',
This absorption dropped to 0. 1% at 7 days of age,
to 0. C2% at 21 days and to the adult value of about
0. 003% at 33 days of age. S7
Although these uptakes ape low in most normal
situations, they cannot automatically be dismissed
in all environmental situations. Romney et al, za
for example, report data on the plutonium content
of the lung, CI tract and bone of kangaroo rats and
jackrabbits at the Nevada Test Site where they had
been living in areas contaminated.with plutonium.
Data from the animals taken from the higher con-
tamination areas are reproduced in Table V.
At first glance, the bone values appear to be
high considering the low abso'rption of plutonium.
However, the high GI tract contents indicate the
possibility of ingestion of considerable amounts of
soil so that a large quantity of plutonium is avail-
able for transfer. In the last column we have cal-
culated the amount of plutonium which would be ex-
pected in the bone after one year considering that
the GI tract contents represent one day's intake and
0. 003% of this quantity is transferred to the bone
each day. Even ignoring any absorption from the
lung, it can be seen that, within the accuracy of
the estimate, the apparently high bone values can
(a)
Assuming GI content measurement represents one day
feeding and 0. 003% per day transferred to bone.
be accounted for on this basis. It may also be
noted that these values, even though significant,
should be of little concern in a predator food chain
because of the low uptake from the GI tract of the
predator.
The effects of unabsorbed plutonium passing
through the GI tract have been studied in acute ad-
ministrations to rats. s? A dose of 88mCi/kg of
nitrate caused death in the first day, apparently
from effects other than radiation. Doses of 56
mCi/kg did not produce'grossly evident damage.
Oxide doses as high as 230mCi/kg produced no
gross evidence of damage while 155mCi/kg pro-
duced transient histological changes in the cecum
and colon which appeared three days post adminis-
tration but not at six days. These data have indi-
cated that the alpha radiations do not penetrate to
the sensitive tissues of the GI tract with any effi-'
ciency and serve as the basis for the ICRP and
NCRP assumption that only 1% of the alpha energy
at the surface of the GI tract contents is effective
V
in producing a dose to the GI tract.
12
-------
The foregoing data would indicate that the
0. 003% absorption from the GI tract chosen for cal-
culation of the MFC's for occupational exposure is
appropriate for this use. However, for the envi-
ronmental exposure of the public in situations such
as living in a contaminated area where exposure
can be continuous, both the higher absorption by
children and the possible effects of combination of
ingestion along with foods containing various addi-
tives such as citrates, preservatives and even che-
lating agents must be considered. For the young
rat, absorption above 0. 1% was in''"the first week of
life corresponding approximately to the age of the
human baby when motility is low and the environ-
ment is relatively carefully controlled so that ac-
cess, to ingestion by routes other than foods is
small. The high uptakes with citrate occur with
high acidity and significant percentages of the plu-
tonium in the +6 valence state both of which are un- •
likely to occur with any degree of regularity under
normal conditions. Thus, it ils concluded that an
uptake about ten times larger than that used by the
ICRP for occupational exposure and about one-tenth
of the highest values noted for very young animals
or citrate complexed plutonium would be reasonable
and, at the same time, relatively conservative par-
ticularly for the relatively insoluble forms of plu-
tonium expected to occur in the environment. This
would, then, be an uptake of about 0.03% and would
apply particularly to the most susceptible group,
children between the ages of about one and ten
years.
C. Skin Absorption . .
Although the intact skin serves as an excellent
barrier against the passage of plutonium on its sur-
face, a small rate of absorption through the skin
can occur. Such rates are insignificant for most
cases of sporadic, infrequent skin contamination
but we must consider the possibility of long term
accumulation from living in a contaminated area
271
where a continued maintenance of some level of
contamination on the skin can be assumed.
Data on the absorption of plutonium nitrate
from 0. 1 N acid solution on rat skin indicates ab-
sorption rates of 2 - 30 x 10~6percent per minute
over periods of 15 minutes to one day. 9 When
applied in a mixture of tributyl phosphate and car-
bon tetrachloride with traces of nitric acid, the
initial rates were up to ten times higher, with in-
dications that higher rates were maintained through
at least five days. Human data are meager and
may indicate somewhat lower absorption rates as
could be expected from data on other materials
with several species of animals as compared to
humans.
In deriving skin contamination limits for con-
trol purposes, a rate of penetration of 10~s% per
minute was used for plutonium based upon an ex-
amination of available data. ?9 This primarily re-
lates to contamination resulting from solutions
rather, than the more insoluble particulates. How-
ever, the possible effects of agents such as lotions,
detergents, and various household chemicals have
not been examined to see if they could have a pos-
sible effect of increasing the penetration. One
would expect the plutonium in soils or the environ-
ment to be initially in the form of insoluble oxide
or firmly attached to other particles so that the
skin absorption should be lower than for the solu-
tions. In view of the uncertainty of possible effects
of other agents, however, the absorption rate of
10"5% per minute will be used as a conservative
value.
I
If we again limit the intake by absorption to
that which would result in a deposition of 0. 004
(jCi after 70 years (ignoring elimination) the rate
of absorption is 0. 35 dis/min per day or assuming
a 10" 5% per minute rate of skin absorption, one
could permit continuously over the 70-year period
some 2400 dis/min on the body. The surface area
of the body is about 1. 85m2 for an average man,
about 1. 6m2 for an average woman and about
-------
I
Li i Li 0. 25m3 for the newborn. 30 Data are not available
for the average quantity of dirt or soil carried on th
the body. Treagar31 indicates that about 1 mg/cm3
of liquid is about as much as can be held on the hu-
man skin without forming a noticeable liquid pool.
Since the skin is normally cleansed at intervals,
particularly before bedtime, and it is protected over
a major portion by clothing, an average quantity of
environmental soil of about 0. 1 mg/cnr is assumed
to be continuously present. Note again, that the
child, who is more likely to be somewhat soiled,
has a smaller surfa.ce area and, thus, for the same
deposit a smaller total quantity of dirt. Under these
assumptions, the average man would have some
1. 85 grams of dirt on his body which could contain
about 1300dis/min per gram.
This calculation assumes the dirt on the body
to contain the same concentration of plutonium as
the soil in the environs. Since one would expect
the smaller soil particles to be preferentially de-
posited on the body, a mechanism for concentra-
tion or depletion of the plutonium in the soil on the
body depending upon the relative particle size does
exist. Normally, however, one would expect the
smaller plutonium particles to'be attached to soil
particles, particularly after a residence in the en-
vironment of some significant pe"riod of time so that
this possibility of concentration may not be as sig-
nificant as it would seem, particularly with the in-
herent conservatism of the calculation.
The possibility of by-passing the skin barrier
by deposition in an injury or damaged skin also ex-
ists. The mechanism is of particular concern in
plant operations where concentrated quantities of
plutonium are handled and significant amounts, in
relation to the maximum permissible body burden,
oan be introduced into a single wound. However,
at the low concentrations expected in soils at an
acceptable level, the amount of plutonium asso-
ciated with the soils is very small. Data on absorp-
tion through cuts indicates that uptake may be 10-
100 times that noted through intact skin. 3a Thus,
for this mechanism of uptake into the body to be
equallyeffective compared to skin absorption, some
1-10% of the body must be continually abraded and
contaminated to these levels. Probably of more
significance in this case is the reduction of con-
servatism in the number derived.
IV. INTAKE IN CONTAMINATED AREAS
The problem of estimating the intake of plu-
tonium by a heteorogeneous group of people visit-
ing or living in a contaminated area is exceedingly
complex and provides the major source of uncer-
tainty in the derivation of a standard. Past investi-
gations 33> 34 have used a simplified concept of the
resuspension factor to provide estimates of the air
concentrations and the resulting inhalation. Intake
by ingestion, absorption or through ecological
chains was shown to be negligible in comparison to
the inhalation. While it appears that the general
concepts of these prior investigations are reason-
able,.^ more detailed study of the various methods
whereby air concentrations or ingestion can occur
is needed to assure that the generalized concept of
the resuspension factor, for example, covers all
of the cases.
It is noted at this point that the mechanisms of
intake to be discussed are primarily physical in
nature rather than biological as can occur in an eco-
logical chain leading to concentration in one or
more links. While the evidence is not complete
that biological accumulation may not be important
in some situations, particularly as the plutonium in
the soil ages and is possibly recycled through bio-
logical systems, it now appears that plant uptake
or uptake in higher animals is low enough that the
physical methods of direct contamination will be of
greatest interest in this problem. This complicates
the study because of the large number of possible di-
rect contamination transfer systems, marked vari-
ability with different situations and the lack of firm
experimental data all of which limit our ability to quan-
tify and rank these mechanisms inor'ior of importance.
14
-------
A. Mechanisms of Intake
The intake of plutonium from the soils can be
by a varied series of pathways, either direct or in-
direct, which are dependent upon the nature of the
contaminated area, the nature and distribution of
the contaminant and the actions of individuals in the
af ea. We have not attempted to formalize these
pathways at the present time since they need con-
siderable additional definition and data to quantify
them. As will be seen, however, there are a few
generalizations which can be used to approximate
the hazard in such situations. '
If one considers'-tne situatiop occurring in an
area where soils are contaminated and families
are living, it is immediately apparent that a rela-
tively complex description is needed. We can start
with the ambient air concentrations which will re-
sult from wind pickup. This will depend upon the
type of terrain and vegetative cover, the wind
speeds and directions with respect to the contami-
nated area, the penetration of l!he particles into any
shelter plus other variables as discussed in Appen-
dix A. This type of exposure will be relatively con-
stant in time and, given certain of the variables, can
be generally evaluated for the average concentration.
Other perturbations in the exposure conditions are
both more localized and intermitteAtl depending upon
certain actions at the time. Fpr example, mechanical
disturbance of the soils by such simple actions as
walking or digging can produce localized air-con-
centrations. These, in turn, can result in con-
tamination of the body or clothing from which addi-
tional plutonium intake can occur by ingestton, ab-
sorption through the skin, or inhalation as a result
of localized actions (i. e. , taking a dress or shirt
off over the head). Further, such a mechanism can
result in transfer of contamination to other areas,
such as the home or a vehicle, where the nature of
the surroundings is such that more intimate and
prolonged contact could result in significant intake.
A probably more important variation of the same
mechanism is that of children at play in the area.
273
This is because of their generally more active na-
ture and more intimate contact with soils during
such activities. The presence of pets in many
homes provides another mechanism for transfer of
contamination into the home with possible intake by
individuals. Of particular interest here is the lo-
calized concentration for inhalation which could t
occur by fondling or hugging the pet;
Aside from living in the area there is the ques-
tion of working. Agricultural pursuits (including
home gardening) involve considerable effort di-
rectly with the soils and disturbance of the soils by
mechanical and animal activities. It is possible
that just this type of disturbance may result in mix-
ing of the contaminant in the soil making it less
available or causing redistribution over a wider
area. Again the possibility of transfer to houses
or vehicles with more intimate contact and expo-
sure of other people exists. Other types of out
door work, such as construction, is usually for a
limited''period of time and, while soil disturbance
is large, it usually results in a high degree of mix-
ing and, frequently, burying some portion of the
contaminant in an inaccessible location.
It will be noted that we have concerned our-
selves with areas in which people are living. While
it is appropriate to consider the possibility of dif-
ferent- standards for areas with only occasional vi-
sitation, the data available on contamination trans-
fer and the long-term behavior of the plutonium are
not now adequate to provide an assessment which
would be applicable to conditions some years after
the contaminating event when habitation of the area
is possible.
Much of the effort on these mechanisms of ex-
posure for this interim standard has been devoted
to the question of resuspension and inhalation since
this still seems to be the predominant mode for
taking plutonium into the body. However, future
studies will attempt to better define and quantify
these other possibilities, and in particular the trans-
fer mechanisms, in order to remove uncertainties
15
-------
274
and to, perhaps, permit a range of values appli-
cable to different situations.
B. Ingestion
Primary methods of ingestion of plutonium
from the soils are considered to be casual inges-
tion by transfer from the hands (or other parts of
the body) to the mouth or by contamination of food
crops grown in the area. There is a definite pos-
sibility of deliberate ingestion of the soils by young
children.
V"
Data on the quantities likely to be ingested in
this manner are not available but, for the casual
ingestion, it would appear that one gram per day
would be a high estimate with 0. 1 gram per day a
more likely value. If we limit the total intake by
this mechanism so that the body burden at the end
of 70 years is 0. 004 uCi with an uptake of 0. 03%,
the 0. 1 gram per day ingestion "would lead to a soil
concentration of 5 x l(T3|jCi/g or 1 1, 000 dis/min
I
per gram.
The deliberate ingestion of soil by children is
limited to a relatively short period of time, say
one year, and is intermittent over this period. If
we assume an average of one gram per day ingested
with the limitation on accumulation during this one
year at l/70th of the maximum permitted body bur-
den, the soil concentration should not exceed 5 x
10~4 uCi/- or about 1100 dis/min per g.
In the above analysis, we,have lumped several
individual - athways of exposure into our
value of 0. 1 g of soil (or the plutonium contained
therein) ing-jstedper day. These include the intake
with foods, casual ingestion, and intake v^ith water
which may have become contaminated from runoff
fror.t the contaminated area. Data for individual
assessment of each of these mechanisms are not
adequate to trace, in any detail, the intake from
each o'
-------
C. Skin Absorption
In Section IIIC, a value of 1300 dis/min per
gram or about 6x 10~4 pCi/g was derived as a lim-
iting concentration in the soils for the possibility of
skin absorption. Again, it is believed that this val-
ue is conservative because of the relatively high
absorption rate chosen, particularly for the com-
pounds expected in the soils. It is deliberately
conservative, however, in view of the uncertainty
of the influence on the absorption rate of the various
lotions, makeups, soaps and other chemical mate-
rials used on the skin. V"
As was noted, ffeje smaller particle fraction in
the soils (or of the contaminant) is again of partic-
ular interest since this fraction will stick to the
skin.
D. Inhalation
In order to be inhaled, the particles must be-
come airborne and arrive at the vicinity of the nos-
trils. Usually, this requires I energy from an ex-
ternal source to dislodge them from their resting
place and to keep them suspended in the air for a
time period sufficient for inhalation. (Although one
can visualize a direct transfer to the air stream
entering the nostrils by "sniffing" or inhaling vig-
orously with the nostrils close to (^ contaminated
object. ) For inhalation and retention of the parti-
cles in the respiratory tract, the particle size
must be relatively small, usually considered as
less than 10|_im aerodynamic diameter. Larger
particles will deposit in the upper respiratory
tract and be eliminated from the body in a' matter
of hours to days through the GI tract. Because of
the low absorption from the GI tract and the pro-
tective layer of mucous between the contents and
the GI tract wall, this fraction is of little or no
concern for the alpha radiations from plutonium.
The fraction of the particles retained in the re-
spiratory tract increases as the particle size de-
creases with the best estimate of this factor as
given by the ICRP Task Force on Lung Dynamics.24
275
This factor has been discussed and considered in
the revised MFC to be used for this study in Sec-
tion III A.
The need for considering particle size of the
contaminant in the soil and in its transfer to the
air is of considerable importance in all of the in-
>
halation transfers. Particles of the contaminant
which are larger than the "respirable" size in the
soils are of little concern from a potential inhala-
tion hazard standpoint unless reasonably efficient
mechanisms for breaking the particles into smaller
sizes are available. Thus, in the following con-
siderations, primary emphasis is placed on the
smaller particles and mechanisms for movement
which affect the larger particles, such as salta-
tion or surface creep, are considered to be of sec-
ondary importance.
In the transfer of particles to the atmosphere
or to surfaces, the distribution of the contaminant
through the soil is an important factor. One can
visualize, for illustration, two theoretical limit-
ing conditions. The first condition prevails for an
indeterminate period of time following an initial
deposition when the material is spread over the
surfaces of the ground and other objects in a thin
layer. As time passes, the erosive effects of the
wind or runoff and the removal of the material
from the surfaces of plants by washing, growth
and decay, or from other surfaces by •winds or
rains, leads to the condition where the contami-
nant is mostly in the soils and is distributed
through a layer extending to a depth dependent
upon the time since deposition, the nature of the
]
soils, the influence of physical factors acting on
the soil (such as freezing, thawing, rainfall leach-
ing, or wind or mechanical movements resulting
in mixing) and even the biological factors such as
microbial action, burrowing animals, etc. This
is further complicated by the fact that plants and
other surfaces will intercept resuspended mater-
ials, usually diluted by the accompanying soils,
and these items will serve as sources for further
17
-------
276
resuspension. However, it can be seen that the
vulnerability of the material on the surface is much
higher in the condition representing an initial de-
posit since all of the material is in a position to be
affected by winds or other disturbance while in the
latter condition, a portion of the material has pene-
trated into the soil and its availability depends upon
the depth of penetration of any disturbance. In ad-
dition, its availability may also-be affected by any
chemical or physical reaction, such as binding of
contaminant particles to soil particles, which may
V
have occurred. In the final limiting condition, the
'•A
contaminant will be essentially uniform throughout
the soil profile and will behave much as the other
constituents of the soil in producing airborne dust
when disturbed.
The above considerations apply directly to the
airborne accident case when the deposition occurs
in a short period of time so that penetration into
the soil and binding to the soil particles does not
I
occur during the period of deposition. In the in-
dustrial situation of continuous, low level, air-
borne releases, the deposition continues over a
period of time so that these mechanisms are con-
tinuously at work and only the material deposited
recently is in the upper layer of highest suscepti-
bility and undiluted with soil particles. Another
situation of interest in the industrial area would be
that in which the contaminant is carried in a liquid,
such as the buildup of materials on sediments from
low level effluents, or the situation in an area
where higher level wastes are percolated through
the ground to remove the contaminants by adsorp-
tion on soils. In these cases, the penetration of the
contaminant into the soil layers is much greater so
that, even after drying, the contaminant is diluted
to & large extent with soil and the plutonium is as-
sociated with the normal particle sizes in the soil
although there, may be a strong tendency for asso-
ciation with the smaller particles because of the na-
ture of the ion exchange process. Another special
case is the area used for burial of solid wastes.
Here the immediate problem is controlled by cover-
ing the contaminated material with a thick layer of
clean dirt and excluding the area from use. Con-
cern with such practices stems from the possibil-
ity of later use of the area with digging into the
material, from later erosion bringing the material
to the surface, or from translocation by leaching.
Here, again, the effects of time and physical and
biological processes will result in a much more
uniform mixing of the material (particularly if Ihe
contaminated objects are biodegradable) than when
they were buried. If one could, for example, pos-
tulate complete mixing then the appropriate limits
could be based upon the total contaminant and the
total volume of the burial area.
1. Estimate from Dust Loading. The normal
dust loading of the atmosphere results, at least in
part, from the resuspension of soil particles from
the earth's surface to the air*. Thus, the quantity
of such material normally found in a given region
can be'considered to be a crude index of the resus-
pendability of the surface materials for some inde-
terminate distance upwind. (Note that in a dust
storm the material in the air at a given location .
could have originated miles upwind as, for example,
from a large area of plowed fields, so that the dust
load must be regarded as an index to the average
condition over a large area. ) If we assume that
the plutonium contamination is uniformly mixed
with the soil particles soithat the same mechanisms
which result in the resuspension of the soils are
equally effective in causing resuspension of the
plutonium, then a limiting concentration in that
part of the soil layer which is resuspended can be
estimated from the standards for particulates and
for radioactivity. We have earlier concluded that
an MFC of 3x 10~13 yCi/cc seemed appropriate for •
the exposure of an individual in the population when
applied to materials most likely to be encountered.
Tb,e Federal Secondary Standard for particulates
in the air is expressed as a geometric mean (mean
of the logarithms of the concentrations) of bO^g/m3.38
18
-------
277
The geometric mean is smallerthan the arithmetic
mean by a factor depending upon the geometric
standard deviation of the measurements. Since the
average exposure (and thus, presumably the aver-
age amount inhaled and retained) depends upon the
arithmetic mean, it is necessary to convert this
standard. Equations for this purpose are given by
Drinker and Hatch.39 Experience with most air-
borne contaminants indicate that the most likely
geometric standard deviation is about two. For
this value, the arithmetic mean concentration cor-
responding to the standard is 76|jg/m3. However
as the standard deviation increases, the mean in-
i
creases rapidly, being 116 pg/m3 for " - 3, 152
ug/m3 for a = 4, and 219|Jg/m3 for
-------
278
-10
Height - I m
Wind speed- 5m/src
100 1000
Contaminotod Area Width Upwind (rn )
10000
Fig. 1. Air concentrations at maximum point downwind from an infinite
crosswind area uniformly contaminated to
As would be expected, the concentration at a
given location is highly dependent upon its location
with respect to the contaminated areas and the wind
directions. Thus, a precise definition of the ex-
pected air concentration could only be given for a
particular location if the contamination pattern and
meteorology were well defined. Some parametric
calculations on the importance of this factor are in
progress but are not completed to the point where
they would be particularly useful in this study.
However, in view of the variations possible, we have
used a situation where the location of interest is at
the edge of a uniformly contaminated area which ex-
tends to infinity in the crosswind direction. The
wind is blowing directly over the plain toward the
sampler. The results for this calculation, using
the freshly deposited value of K/u2for zinc sul-
phide particles of 2 x l(Ta are given in Fig. 1.
Since the wind pickup is assumed to increase as
the square of the wind speed and the dispersion as
the first power of the wind speed, the concentra-
tion downwind should increase directly with the
wind speed. The value of 5m/s used in the calcu-
lation is a reasonable average for many locations.
The bands in Fig. 1 result from calculations using
various values of deposition velocities, depending
upon particle size and vegetative cover in the area.
In assessing Fig. 1, there are several uncer-
tainties and factors of conservatism that should be
borne in mind. The applicability of this calculation
20
-------
i
to the stable case is particularly questionable since
wind speeds are generally lower in this condition.
The use of the same pickup rate for this stable con-
dition as for the unstable case would seem to over-
estimate the concentration since one would expect
the pickup to be lower because of the decreased
wind turbulence. The effect of aging on the pickup
rate is uncertain. While others have assumed a de-
crease in the air concentration33'3'1 with a half-
life of 35 clays, examination of the data available
(Appendix A) does not substantiate the continued
decay at this rate. There is no cfbubt that the re-
suspension rate wiHMecrease with time, probably
rapidly at first and then at a decreasing rate. Cal-
culations on the air concentrations at one area in
Nevada (GMX) are given in Appendix A. A few mea-
surements in this area40 indicate the resuspension
rates to be significantly lower than those calculated.
This is some 20 years or so after the deposit was
laid down. An additional uncertainty is in the ef-
fect of particle size on the pickup rate. The pickup
constant was derived primarily from data using ZnS
particles. Data are not available to assess possible
changes in the rate with particle size. The question
of wind variability has not been seriously considered
since the formalized type of calculation used for
Fig. 1 tends to average the concentration over a
wide angle due to the assumption of an infinite ex-
tent in the crosswind direction. This, in turn,
tends to maximize the estimate of the air concen-
tration in the real case.
Although the uncertainties are large in this type
of estimate, it would appear that a uniform concen-
tration (or average over a large area) of about
0. 1 (jCi/m3 for material freshly deposited from the
atmosphere would be reasonably conservative in
meeting the average MFC. One would expect the
i
air concentration to decrease with time. It is be-
lieved that a decrease of a factor of ten would not
be unreasonable over the first year.
279
3, Resuspension Factor. The resuspension
factor approach has been widely used for estimating
air concentrations from surface deposits. It does
tend to give average values for the particular con-
ditions under which it is measured and a reasonable
amount of information is available for several dif-
ferent conditions. We tend to believe that it is more
useful for describing localized concentrations re-
sulting from various types of disturbances but, in
view of the paucity of other data, its use for this
problem is discussed below.
The resuspension factor is defined as the ratio
of the air concentration to the quantity of material
per unit area on the ground. If the air concentra-
tion is given in quantity per m3 and the unit area on
the ground is in m2, the resuspension factor will
have units of m"1. Outdoor measurements of this
factor have been made in arid or semiarid country
, f,
following safety tests of nuclear weapons with a few
studies in other areas using relatively small plots
seeded with known levels of radioactive materials.
Stewart41 has concluded that a representative value
for quiescent conditions outdoors is about ICT6!!!""1
while in areas of moderate activity the value may
increase to 10"5 rri"1. A review of values accumu-
lated from the literature by Mishima42 indicates
values ranging from 8xlO~l0 to SxlO"4!!!"11 under
conditions of no mechanical disturbance and from ,
1.5xlO~s to SxlO"4!*!"1 as measured under condi-
tions of vehicular or pedestrian traffic or in areas
with people working. It is noted that the minimum
values under quiescent conditions occurred from
one test using 91Y. If these values were excluded,
the range without mechanical disturbance is reduced
to 8xlO~s to 3xlO~4m~1. Langham, 3* in assess-
ing limits for a weapons accident, uses a value of
10~6m~1 with, however, an exponential decrease
with time with a half-life of 35 days, thereby im-
plying a value of 7 x 10~l0 one year after deposit
and,5x 10~l3m~l two years after deposit. Kathern33
assumes a value.of 10~4m~1 decreasing with a half-
life of 45 days. The primary evidence cited for the
Zl
-------
decrease with time is a series of air samples taken
over a period of 20 weeks in an area contaminated
by plutonium following a weapons safety test. We
do not believe this magnitude of decrease to be ap-
propriate, as is discussed in Appendix A, but do
believe that some decrease will occur over the
first year following a deposition.
It is noted that the resuspension factor is sen-
sitive to the methods used for estimating the quan-
tity of plutonium on the ground, to the location of
the sampler with respect to the contaminated area
and to the meteorological conditions at the time of
the measurement. Thus, if measurements are
made under quiescent conditions, as far as me-
chanical disturbance is concerned, the wind speed
and Aie depth of the plutonium in the soil would ap-
pear to be important factors for the particular lo-
cality. Measurement of the surface contamination
by an alpha meter will detect to depths of a few
milligrams per square centimeter (perhaps a few
hundreths of a millimeter) and may underestimate
the contamination. Sampling of the area to a depth
of two inches will include soils which will not be
affected by the surface disturbance and, if contam-
inated to the full depth, will result in an overesti-
mation of the surface quantity available for resus-
pension. While the measured factor will indicate
the probable air concentration under identical con-
ditions of plutonium distribution, these variables
plus others discussed earlier make the extrapola-
tion of the values to different areas or different
types or patterns of contamination extremely un-
certain.
However, if we use the value of lO"6™"1 as
recommended by Stewart as an overall average
value for quiescent conditions, we find that a quan-
tity of 0. 3(aCi/m2 will result in an air concentra-
tion of 3x 10~l3nCi/cc. Although mechanical dis-
turbance of the surface will result in higher con-
centrations, the time period over which such dis-
turbances will occur is usually fairly short, con-
tinued disturbance over a long period of time will
result in depletion of the resuspendable material
and the values are still within the uncertainty of the
estimate of the overall factor.
4. Mechanical Disturbance. Mechanical dis-
turbance of the soils by actions ranging from walk-
ing across an area to heavy vehicular traffic or
,/
even excavation of the area can result in increased
dust loading downwind and, presumably, increased
resuspension of contaminants contained in the soil.
Such actions can also hasten the "aging" process by
mixing the material in the upper layer of the soil
and diluting the contaminant particles with soil par-
ticles. In extreme cases, such as the presence of
heavy vehicular traffic over a given area for an ex-
tended period of time, the expected increase in re-
suspension rate will result in depletion of the con-
taminant from the particular area.
Quantitative evaluation of the potential effect •
of such mechanical disturbance requires a quanti-
tative relation between the degree of disturbance
for a particular area and the resuspension, a rea-
sonable description of the disturbance expected in
the contaminated area and the relation between
these and the location of people. As was noted
earlier, Stewart has concluded that an increase by
a factor of ten for the resuspension factor for an
area of moderate activity is reasonable. In
Mishima's tabulation, the lower end of the range
of resuspension factors is increased by about three
orders of magnitude while the upper end is in-
creased by a factor of two when areas of vehicular
or pedestrian traffic are compared to undisturbed
areas. However, in this tabulation it is difficult
to account for degree of disturbance or for the fre-
quencies with which measurements were taken
under each condition. In a rough analysis of data
obtained by Mork on air concentrations downwind
from a vehicle driven across a contaminated area
of the Nevada desert, (see Appendix A), it was con-
cluded that resuspension rates up to one hundred
times those caused by the winds could occur. It
is noted that mechanical disturbance is a mechanism
-------
whereby material from the ground can become air-
borne during conditions of maximum atmospheric
stability and minimum wind speed, thereby re-
sulting in minimum dilution downwind. At the
same time, this mechanism results in the dislodg-
ing of large numbers of soil particles so that a di-
lution of the contaminant particles with these soil
particles'occurs, making the dust calculation more
appropriate to this condition than the more conven-
tional resuspension assessment.
From the data available, it appears that me-
chanical disturbance can result iJi increased air
concentrations dowWwind over those to be expected
solely from wind actions. However, if the distur-
bance is over a short period of time, the contribu-
tion to the average concentration will be well with-
in the uncertainty in knowledge of the wind effect.
For more intense disturbances or longer duration,
the effect of mixing in the soils and/or depletion of
the source will, again, minimize the contribution
to the long term average. This is not to minimize
the possible importance of such a factor in certain
situations but, rather, it would appear that the un-
certainties in the knowledge of resuspension and
changes of resuspension with time will incorporate
the variations due to such disturbances in most sit-
uations. |1
5. Personal Contamination. A possible me-
chanism of intake by inhalation is contamination of
the skin or clothing while working or playing in a
contaminated area, followed by resuspension of
the material directly from the surface of the skin
or clothing into the breathing zone or transfer of
the contamination into the home with subsequent ex-
posure of those living there.
Data on the transfer of contamination from the
ground to the skin or clothing are very sparse so
i
that any direct calculation of the resulting intake
will produce results of limited value. However, it
has been estimated from data available in the liter-
ature29 that the inhalation from contaminated cloth-
ing or skin during normal activities could be
281
equivalent to the inhalation of the contamination
from about one cm2 per hour. If we consider the
inhalation rate to be 20m3 per day, the MPC of
3x 10"1 3 |aCi/rnl would permit the inhalation of
about 6x 10~'3 (aCi/day. If the inhalation from cloth-
ing continues over the full 24 hours at the above
rate and the clothing is continuously contaminated
to the same level throughout the day, then the
allowable skin or clothing contamination would be
about 2. 5x 10~7 |aCi/cmn or about 0. 5 to 0. 6 dis/
min per cma. li we consider an average of one
mg/cm3 (or about 20 grains total on an adult male)
to be a reasonable value for the soil transferred to
clothing and skin, the concentration would be on the
order of 500-600 dis/min per gram. (Note that the
lmg/cms here includes both clothing and skin and
not just skin as was,used earlier. ) Again, the con-
siderations of particle size and mixing of the con-
taminant with the soil discussed earlier are per-
tinent to this evaluation. It should also be noted
that the rate of intake will vary widely depending
upon clothing changes, bathing, etc., and may well
be lower at night because of the decreased physical
activity.
The possible problems encountered from the
movement of plutoniurn into the home on the cloth-
ing of workers was also examined in Reference 29.
Here it was assumed that 30% of the material
brought into the home was transferred to the home
area and that it remained in resuspendable form
•with a half-life of one .week. Resuspension rates
of 5xlO~4 per hour were used as representative of
the activity in the house with two air changes per
hour. Under these conditions and using an MPC
for air of 2x 10~14 nCi/ml it was concluded that
0. OlnCi could be brought in per day without exceed-
ing the maximum permissible limits. For the re- '
vised MPCiOf 3x 10~l3 nCi/ml used for this study.
This value for the allowable surface contamina-
tio*} is higher than that given in Reference 29 be-
cause of the reexamination of the appropriate MPC
in this study.
23
-------
282
TAULE VI
PROBABILITY OF INHALATION OF PARTICLES
Grams of Soil
Action
Changing Tire
Sweeping Bus
Sweeping Car
Driving Car for One Hour
No Ventilation
High Ventilation
Probability
of Inhaling
One Particle
3xlO~s
Sxicr*
6x10-'
6x10"'
Zx 1CTS
*2x 10- =
Cunta
to 10 =
P"
20,
7,
minaled
clis/min
pram
400
30
20
000
000
700
^Measured immediately after placing powder on floorboards.
Other value represents th.- m. an ,f two a.ld.Uo-.al d,-tr, m,,,aL,On».
it is concluded that this rate could be 0. 1 to 0.
t>.,
per day. As a comparative figfcre, if the soil con-
tamination were 1000 dis/min per gram, this would
require bringing in about 200 to 400 grams per day.
Willie this is not a physical impossibility, particu-
larly in muddy weather, this rate seems somewhat
high for most conditions.
Schwendiman43 has measured the probability
of inhalation of particles under several conditions
associated with automotive transport and cars,
using ZnS particles of about 2 |am median diameter.
A summary of these probabilities and the quantity
of soil which must be present at a contamination
level of 1000 dis/min per gram to cause the inha-
lation of 6x 1Q-8 |_[Ci (the amount which could be in-
haled in one day at the UPC of 3x lO"13 (jCi/ml)
during the given action are listed in Table VI.
These values, while for a time shorter than
the full 24 hours per day, represent measured
conditions in confined areas with relatively severe
activity. As such, they provide some indication
that the previous values estimated for the home are
not unreasonable. '
V. A PROPOSED INTERIM STANDARD
In the preceeding discussions, we have touched
on several points which are of importance in con-
sidering the.conversion of estimates of exposure to
a standard for soils. To some extent these factors
are interrelated and involve the questions of distri-
bution in the soil profile, units of measurement and
si-zes of the particles of concern.
Previous recommendations for soil limits have
been expressed in units of quantity of plutonium per
unit area (i.e., pCi,/m2 or ijg/ms ) because the pri-
mary mechanism of exposure was considered to be
resuspension in the atmosphere and inhalation.
However, this method of designation has led to un-
certainties in interpretation since the layer of soil
involved and of interest was presumably that asso-
ciated with the resuspension factor applied and this
was not defined in the studies. Thus, there was,
in these recommendations, no clear guidance as to
the depth in the soil profile to which the limit should
apply and varying sampling and measurement depths
have been used in different studies. In the assess-
ment of exposures in this paper, we have used both
the concentration in the soil'and the quantity per
unit area depending upon the type of estimate made.
The two methods of expressing the limit can be in-
terrelated if such factors as the thickness of the
soil profile of interest and the soil density can be
defined. Thus, either method can be used as a
primary unit as long as the information to permit
conversion to the other is provided.
The concentration in the soil is preferred in
this study because many of the potential mecha-
nisms of exposure are more directly related to
this quantity and the common methods of measure
ment, sampling and analysis, provide answers di-
rectly in concentration units. Even with direct
measurements of external radiation, such as with
the FIDLER, the quantity per unit area is appli-
cable only when the material is in a thin layer on
the surface. For a uniform depth profile with a
large thickness compared to the effective range of
the photons, the reading with this type of instru-
ment is proportional to the concentration in the
Soil. We have, therefore, chosen to express the
standard in units of plutonium concentration but,
also, including a specification of the thickness of
24
-------
I
the soil layer to be considered. This, of course,
has the advantage of relating the standard to the
measurements to be made in a contaminated area.
The selection of an appropriate, layer must con-
sider the mechanisms of exposure and their rela-
tive importance. For dust loading of the atmos-
phere and resuspension, the appropriate thickness
will depend upon the type of disturbance which
causes the input to the atmosphere. Similar con-
siderations also apply to the transfers to the body
since the material available for transfer must be
that to which the individual is exfSosed in the soil
layer. '. i
We have tended to consider the material at the
very surface of the ground to be limiting in the
sense that it is more available for transfer or for
resuspending. The definition of the "very surface
of the ground" is difficult since it can change with
conditions such as wind speed, turbulence or degree
of mechanical disturbance. Further, the sampling
and measurement of a thin lalyer on the ground sur-
face is difficult even on bare ground and next to im-
possible in heavily vegetated areas (such as a lawn).
However, in heavily vegetated areas the access of
people to the soils is limited so that somewhat dif-
ferent considerations will apply to exposure from
the soils. In view of the potentialLHmportance of
wind pickup and the lack of information on the
thickness of the layer actually involved in this phe-
nomenon, we have arbitrarily chosen a layer on
the order of one mm thick to serve as a standard
for the low vegetated areas. The "wording "on the
order of" is deliberately chosen to indicate that the
actual thickness cannot be specified closely be-
cause of the impossibility, in most cases, of sam-
pling a precisely defined layer with any degree of
precision. It is suggested that a reasonable inter-
pretation of this term would be a shallow scraping
of the surface layer taking into account the many
imperfections and various sizes of small objects
encountered in such a scraping. The use of a
measured area and weighing of the sample will
283
permit an estimate of the average thickness. For
vegetated areas, 'where the surface is not as readi-
ly available a thickness on the order of 5mm would
seem to be appropriate. Since the specification of
this thickness provides an averaging thickness over
which the plutonium in the soil is measured, such
'•1:
a specification would permit the averaging of a
thinner layer over the full depth and would permit
a total of up to five times .as much expressed as
quantity per unit area in the vegetated area as in
the barren area. The. decreased exposure to people
due to. the smaller access to these soils and to the
decreased pickup by the winds would appear to
more than compensate for this.
For layers deeper in the soil profile, a thicker
layer would again appear to be appropriate since
exposure would result only by mechanisms which
either remove the upper layers or mix the soils to
a significant depth. Thus, for the soils beneath
the surface, averaging over a one centimeter depth
would1! seem to meet the intent of the limitation.
Note that in the above discussion, the limit on
concentration in the soil remains constant regard-
less of the thickness of the layer with those mecha-
nisms of exposure resulting from direct contact
or transfer of the soil and plutonium to the body
not affected. The main purpose of specifying the
layer is to provide an appropriate thickness for
averaging and controlling this thickness so that
averaging over deeper depths will not result in
samples meeting the limit but still presenting a
high level at the surface for the resuspension
mechanisms.
I
The second parameter of interest is the par-
ticle size of the contaminant. For inhalation, par-
ticles larger than about tenurn aerodynamic di-
ameter "will have a very low probability of reten-
tion in the lung and the solubility of plutonium is
such that particles deposited in the upper respira-
tory tract will not be of significance in adding to
the body burden before they are eliminated. It is
noted that for plutonium oxide particles, a teh|_im
25
-------
284
aerodynamic diameter corresponds to an actual par-
ticle size of about 3 urn for spherical particles due
to the density effect. In the earlier discussions it
was noted that even for mechanisms involving
transfer to the body, fractionation toward the
smaller sizes will occur both in the dislodging of
the particles from their resting place and in the
consideration of the retention on the body. There
is, therefore, good reason for believing that the
smaller particles are of predominant importance
in all mechanisms of exposure and some recogni-
tion should be given to this in the formulation of
'. '^
the standard.
If the overwhelming and only consideration in
exposure were inhalation one could confidently use
an upper limit for the size to be considered on the
order of 5-10 (am based on the possibility of attach-
ment of plutonium to particles of low density. For
pure oxide particles, the size limit could be even
lower. There is, however, the problem of the un-
certainty in the estimates of the other mechanisms
and the possibility that they may assume some im-
portance for the somewhat larger particles if the
controlling size were based only on inhalation. In
addition, the possible problems of aggregation with
breakup under the disturbance which transfers the
material to the air must be considered. We have,
therefore, chosen an arbitrary limit of particle
sizes for these considerations of less than 100 (jm
to represent the fraction of the. soil of concern.
This corresponds to a screen in the Tyler series
of 150 mesh (actually this is 105 |jm). It is recog-
nized that normal screening will not break up some
of the aggregates which could later be broken up
and serve as a source of exposure, but the choice
of the 100 |jm size should provide sufficient conser-
vatism that such errors will not be important.
However, for considering the state of the con-
taminated area over long periods of time, one must
also consider the possibility that breakup of the par-
ticles in the normal processes of soil formation
will occur and will serve as a source of smaller
particles continuously feeding to the fraction of
interest. Although it is believed that redistribution
mechanisms over the time periods of interest for
soil formation will predominate in determing the
soil concentrations, it is proposed that the total
concentration in all particle sizes be limited to an
arbitrary value of twice the concentration in the
fraction below 100 (j.m. Since the times for soil
formation from the matrix material range from
decades to tens of decades, this limitation should
be extremely conservative.
With this background on the application of the
numbers, we are now ready to review the estimates
from the exposure mechanisms to arrive at a value
for the plutonium concentration in the defined layers
and fractions. The estimates of soil concentration
obtained earlier are summarized in Table VII for
this purpose.
In assessing these values and considering the
degree of conservatism relative to each, it was
concluded that a value on the order of 500 d/m per
gram or about 2x 10~4 |_iCi per g would be appro-
priate. The resuspension values for fresh deposits
are somewhat lower than this, but, for the long
term exposure, it is expected that the values will
increase by a factor of ten or more. Further, the
estimates were deliberately made for an unrealistic
type of area in which it would be expected that the
calculations would lead to a high air concentration.
TABLE VH
ESTIMATES OF LIMITING SOIL CONCENTRATIONS
FOR SEVERAL MECHANISMS Of EXPOSURE |
Soil Concentration
Ingestion
Casual
Deliberate
Skin Absorption
Inhalation
Dust Loading
General Rcsuspension
Fresh Deposit
Aged Deposit
Resuspensiun Factor
i Clothing
5 x 1 0" 3
5x 10T«
6xlO~*
Z. 5xlO"3
'••(, x 10" 5
*6x 10"*
Zx 10"
3x 10-'
11,000
1. 100
1,300 .
5,500
t!30
*], 300
-330
600
_
-
-
'
0. 1
1
0. 3
"
-Based on 1 mm.thckncai of soil with a density of \.bf/cm'
26
-------
TAIiLE VIII
RECOMMENDED INTERIM STANDARDS
FOR PLUTONIUM IN SOILS
In <100 urn particle
-Sjy.e Fraction
Top 0. 1 cm*
Any one
cm layer
500
2x ID'*
10000
4xlO-»
* For bare soil or areas with sparse vegetation. Where area is rea-
sonably v/ell vegetated (greater than 50-Vof the area is covered with
low vcpetalion) and a reasonable root inat exists to hold the soil, the
concentration lifted can be applied to a 0. 5 cm layer which would per-
mit up to Z^iCi/nr in this layer.
•* With I he provision ih.-it the fraction with particle sizes less than
lOOuu* is known not to exceed the limits yiven. If this is not known,
the values fur the <)00pm fraction should be applied to the total.
This standard 'for the conqentration can now be
combined with the previous discussion as to the
limits of applicability to provide the final set of
stahdards as given in Table VIII.
The resuspension mechanisms, which strongly
influence the choice of the concentration value tend
to average the pickup from wide areas so that the
presence of small areas in the general vicinity
which have higher concentrations are not of great
importance. Since the other methods of more di-
rect transfer from the soil give higher estimates
for the limiting concentration and, in themselves,
require consideration of occupancy factors and
types of human activity in the contaminated area,
it is tempting to specify that the above values are
averages over large areas and that smaller lo-
calized depositions of several times these concen-
trations could be permitted. In view of the many
uncertainties and the magnitude of the values, an
allowance of this nature is not recommended for
general use at this time. However, as additional
data are obtained it is anticipated that the standard
will be revised to include such a feature. In the
meantime, it is possible that detailed investigation
of, a particular area may provide sufficient informa-
tion for that area to permit the application of such
a concept for that area. Such investigations aimed
at a particular situation will always provide better
285
answers than a general standard of this nature and
such an approach to individual problems is entire-
ly appropriate.
REFERENCES
1. C. M. Lederer, J. M. Hollander, and I. Perl-
man, "Table of Isotopes, " Sixth Edition, John
Wiley and Sons, Inc. , New York, London, i
Sydney, 1967.
2. F. X. Has.s and A. R. Campbell, "Table for the
Ingrowth of Daughter Products from (he Decay
of Plutonium Isotopes Used in Heat Sources, "
USAEC Report MLM-1919 (Mound Laboratory)
June 12, 1972.
3. K. C. Pillai, R. C. Smith, and T. R. Folsom,
"Plutonium in the Marine Environment, "
Nature Z03, 568(1964).
4. K. M. Wong, V. F. Hodge, and T. F. Folsom,
"Concentrations of Plutonium, Cobalt, and
Silver Radionuclides in Selected Pacific Sea-
weeds," USAEC Document LA-4756 (Proceed-
ings of Environmental Plutonium Symposium
held at LASL, August 4-5, 1971) pp. 93-98,
1971.
5. International Commission on Radiological
Protection, "Report of Committee II on Per-
missible Dose for Internal Radiation,"Health
Physics, 1_, June I960.
6. J. F. Cline, "Uptake of Am-241 and Pu-239
by Plants," USAEC Document BNWL-714
(Battelle, Pacific Northwest Laboratories),
pp. 126-127 (1966).
7. R. O. McClellan, H. W. Casey, and L. K.
Bustad, "Transfer of Some Transuranic
Elements to Milk, " Health Physics, 8, 689-
694 (1962).
8. National Council on Radiation Protection and
Measurement, "Basic Radiation Protection
Criteria, " NCRP Report No. 39, NCRP Pub-
lications, Washington D. C. , January 15, 1971.
9. International Commission on Radiological Pro-
tection, "Recommendations of the International
Commission on Radiological Protection (Adopt-
ed September 17, 1965)" ICRP Publ. 9, Per-
gamon Press, Oxford (1966).
10. Federal Radiation Council, "Background Mate-
rial for the Development of Radiation Protec-
tion Standards, " Report No. 1, U.S. Dept. of
i Commerce, May 13, I960.
27
-------
28 6
11. International Commission on Radiological
Units and Measurements, "Dose Equivalent,"
Supplement to ICRU Report 19, ICRU Publica-
tions, September 1, 1973.
12. W. H. Langham and J. W. Healy, "Maximum
Permissible Body Burdens and Concentrations
of Plutonium: Biological Basis and History of
Development, " in Handbuch der exp. Pharma-
kolgie, Band XXXVI, J. N. Stannard, Ed.
Springer Verlag, Berlin, Heidelberg, New
York (In Press).
13. A.M. Brues, "Comparative Chronic Toxici-
ties of Radium and Plutonium, " Argonne Lab-
oratory Quarterly Report (February-March
and April 1951), ANL-4625, p.p. 106-134.
14. G. E. McMurtri'e:'(Secretary), "Permissible
Doses Conference, held at Chalk River,
Ontario (September 1949), Report RM-10
(May 1950).
15. *T. F. Dougherty,"Annual Report of Work in
Progress in the Internal Irradiation Program,
1971, USAEC Report COO-119-244 (University
of Utah).
16. Federal Radiation Council, "Background Mate-
rial for the Development of Radiation Protec-
tion Standards, " Report No. 2, U. S. Dept.
of Health, Education, and Welfare, Washington
D. C. , (September 1961).
17. L. H. Hempelmann, C, R. Richmond, and G. L.
Voelz, "A Twenty-Seven Year Study of Select-
ed Los Alamos Plutonium Workers, " USAEC
Document LA-5148-MS (Los Alamos Scientific
Laboratory), January 1973.
n
18. National Committee on Radiation Protection,
"Permissible Dose from External Sources of
Ionizing Radiation, " National Bureau of Stan-
dards HB 59, (September 24, 1954).
19. J.W. Healy, "Contamination Limits for Real
and Personal Property, " Progress Report
January to June 1972, USAEC Document LA-
MS'(Los Alamos Scientific Laboratory) in
preparation.
I
20. National Committee on Radiation Protection
and Measurements, "Maximum Permissible
Amounts of Radioisotopes in the Human Body
and Maximum Permissible Concentrations in
Air and Water, " NCRP Report 22, National
Bureau of Standards Handbook 69, (June 5,
1959).
21. T. L. Shipman et al, "Acute Radiation Death
Resulting from an Accidental Nuclear Criti-
cal Excursion, " J. Occ. Med. _3, 146-192
(1963) Special Supplement.
22. E. E. Campbell et al, "Plutonium in Autopsy
Tissue," USAEC Document, LA-4875 (Los
Alamos Scientific Laboratory), January 1973.
23. W. J. Bair, "Plutonium Inhalation Studies, "
USAEC Document BNWL-1221 (Pacific North-
west Laboratories, Battelle Northwest) Feb-
ruary 1970.
24. International Commission on Radiological
Protection, Task Group on Lung Dynamics;
"Deposition and Retention Models for In-
ternal Dosimetry of the Human Respiratory
Tract," Health Physics, J_2, 173-207, Feb-
ruary 1966.
25. J. Katz, H. A. Kornberg, and H. M. Parker,
"Absorption of Plutonium Fed Chronically
to Rats, " Amer. J. Roentgenol. 73, 303-308,
February 1955.
26. M\ H. Weeks, et al, "Further Studies on the
Gastrointestineal Absorption of Plutonium, "
Rad. Res. 4, 339, 1956.
27. R\C. Thompson, "Biological Factors," in:
Plutonium Handbook, a Guide to the Technol-
ogy, O. J. Wick, Ed. Gordon and Breach,
Science Publishers, New York, London,
Paris (1967).
28. E. M. Romney, H. M. Mork, and K. H. Larsen,
"Persistence of Plutonium in Soils, Plants,
and Small Mammals, " Health Physics, 19,
487-491, 1970.
29. J.W. Healy, "Surface Contamination: Decision
Levels," USAEC Document, LA-4558-MS
(Los Alamos Scientific Laboratory) September
1971.
30. A.M. Laylee, "Anatomy and Physiology of
the Skin, " in: Radiation and Skin, E. T. Wray,
Ed. AHSB (RP) R_39, 1-10, (1964).
I
31. R..T. Tregear, "Physical Functions of Skin, "
Academic Press, 1966.
32. W. D. Oakely and R. C. Thompson, "Further
Studies on Percutaneous Absorption of Plu-
tonium Solutions in Rats, " in: Biology Re-
search-Annual Report 1955, USAEC Docu-
ment HW-41500, (Hanford Atomic Products
Operation, General Electric Company) Febru-
., ary 1956.
28
-------
33. R. L. Kathern, "Towards Interim Acceptable
Surface Contamination Levels for Environ-
mental PuOs," USAEC Document BNWL-SA-
1510 (Battelle Pacific Northwest Laboratory)
April 1968.
34. W. H. Langham, "Biological Considerations of
Nonnuclear Incidents Involving Nuclear War-
heads, " USAEC Document UCRL-50639 (Law-
rence Radiation Laboratory) April 1969.
35. D. O. Wilson and J. F. Cline, "Removal of
Plutonium-239, Tungsten-185 and Lead-210
from Soils, " Nature 209, 941-942, February
26, 1966.
287
36.
37.
I
38.
J. R. Buchholz, W.H. Adams, C. W. Christen-
son, and E. B, Fowler, "Summary of a Study
of the Uptake''6\f Plutoniur^i-239 by Alfalfa from
Soils," USAEC Document LADC-12897 (Los
Alamos Scientific Laboratory) 1971.
R. O. McClellan, H. W. Casey, and L. K.
Bustad, "Transfer of Some Transuranic Ele-
ments to Milk," Health Physics .8, 689(1962). *
Environmental Protection Agency, "National
Primary and Secondary Ambient Air Quality
Standards," Federal Register 36_, 21, Janu-
ary 30, 1971.
39. P. Drinker and T. Hatch, "Industrial Dust,
Hygienic Significance, Measurement and
Control, " 2nd Ed. , McGraw-Hill Book Com-
pany, Inc. , New York, 1954.
40. P. Phelps, Lawrence Radiation Laboratory,
private communication.
41. K. Steward, '"The Resuspension of Particulate
Materials from Surface Contamination," in:
Surface Contamination, B. R. Fish, Ed. , Per-
gamon Press, pp. 151-158(1967).
42. J. Mishima, "A Review of Research on Plu-
tonium Releases During Overheating and
Fires," Hanford-Atomic Products Operation
Report HW-83668 (1964).
43. L. C. Schwendiman, "An Application of Fluo-
rescent Pigment to the Measurement of Par-
ticle Inhalation Probabilities, " USAEC Docu-
ment HW-32292 (Hanford Atomic Products
Operation, General Electric Co. ) July 1, 1954.
29
-------
288
APPENDIX A
PICKUP OF PARTICLES FROM THE GROUND AND
DOWNWIND DISPERSION-GENERAL, RESUSPENSION
Airborne concentrations resulting from par-
ticulate contaminants in the soil can be a possible
mechanism of exposure of people and animals to
the contaminant. Such airborne concentrations can
be of two general types which are distinguished by
their persistence and the nature of the investiga-
tions required to define their relative importance.
The first type is the localized concentration where
the material may be in high concentration in the
breathing zone of one or a few people usually due to
some mechanical disturbance of a contaminated
soil or object. Such a localized concentration can
result directly from the soils or by contamination
of other objects which can, then, transfer the con-
tamination to the localized breathing zone of an in-
dividual. In general, the magnitude of the concen-
tration will be a function of the contamination level
and characteristics of the contamination over a rel-
atively small area. The second type of concentra-
tion is the more general, widespread concentration
which results from the pickup of materials from the
ground to the atmosphere with dispersion downwind
over a large area and, possibly, involving many
people. Such concentrations can result from ei-
ther wind or mechanical disturbance of the soils
and are a function of the contamination levels over
a relatively wide area upwind for the wind distur-
bance and of the localized levels at the site of a
disturbance for mechanical suspension. In this
discussion, we are concerned with the second type
of concentration which we will refer to as ("general
resuspension" as opposed to the local resuspension
for the first type.
I. APPROACH
The general resuspension, along with the
localized resuspension, has been described in
terms of a resuspension factor which is defined as
the ratio of the air concentration to the level of
contamination on the ground at a given location. '
A brief reflection on the upwind source, with a po-
tentially large source area involved, will indicate
the inapplicability of this concept to the problem of
general resuspension. This is one of the chief
reasons for distinguishing between the localized
and general types of resuspension. Thus, the ma-
terial in the air at the receptor may arise from the
pickup many meters or even kilometers upwind.
Further, the source will change with the wind di-
rection or the specific area in which mechanical
disturbance occurs. •;
In order to permit estimation of air concen-
trations resulting from such a contaminated area,
a rough model based upon work done some years
ago in estimating the importance of wind pickup and
transport of larger particles with eventual impac-
tion ori the person3'4 was revised. In this model,
each element of the contaminated area is consid-
ered to be a source for airborne material with the
source strength defined by the rate at which the
contaminant enters the air with the specific dis-
turbance considered. The concentration downwind
is then estimated from the dispersion and deposi-
tion -relations developed over the past years.
In general terms, if we consider a point
source of material on the ground which is subject
to resuspension, the concentration in the air at
some distance downwind is given by Eq. (A-l).
X = KnD'D"
(A-l)
In this equation, X is the air concentration, fi is
the quantity of material on the ground in a position
where it is subject to being injected into the atmos-
phere, K is the fraction of this material which is
injected per unit time by the specific disturbance
considered, D' is the dispersion which occurs
30
-------
downwind as a result of turbulent diffusion, andD"
is the fraction of the material which is not deposited
between the point of pickup and the receptor. In at-
mospheric dispersion terms, KQ is the source term
and the remainder of the equation is conventional.
The air concentration resulting from a con-
taminated area can then be evaluated by integrat-
ing the point source equation over the area taking
into account the variations in contamination level.
D'D" dy dx
(A-Z)
In the application of Eq. '(A-Z), the disper-
sion and deposition downwind can be evaluated
from existing information resulting from micro-
meteorological studies, although the exact choice
of parameters will affect the results and the choice
is made somewhat difficult by the fact that the
source is truly a ground level source. The distri-
bution of contaminant on the ground can be mea-
sured by a number of possible techniques but,
again, there is some difficulty in defining exactly
the depth of importance and the other parameters,
such as particle size, which will be appropriate.
The primary value for which little data are avail-
able is K, the rate of resuspensi9ti under the par-
ticular conditions of interest. However, it may
also be noted that Eq. (A-2) may be used in the
study of the values of K in areas where the'other
parameters are known.
While Eq. (A-2) appears relatively simple,
it describes a number of very complicated process-
es, many of which can be described only in semi-
quantitative terms at this time. In severkl of the
areas where existing information is adequate for
other purposes, added accuracy may well be needed
to! permit a realistic and adequate description for
this use. However, we have attempted to survey
such information as is available and to apply it in
a simplified fashion in order to both illustrate the
application of the technique and to derive some
289
feeling for the sensitivity of the result to some of
the parameters.
II. DISPERSION AND DEPOSITION
A. Equations
The basic equations used for estimating the
dispersion downwind and intervening deposition
according to conventional models are well-known
and have been documented elsewhere. 5 A brief
presentation of these equations is included here
for reference and for .orientation of the user, par-
ticularly in those aspects having to do with the un-
certainty.
The dispersion in the atmosphere from a
continuous point source,by turbulent diffusion is
usually described as a Gaussian distribution of
the material in the horizontal and vertical cross-
wind direction. Thus, the concentration at a
point (x, y, z) with the origin at the source, x taken
in the downwind direction and y and z the distances
in the horizontal and vertical crosswind directions
respectively is given by:
(x, y, z)
R(Kfl)
(A-3)
In Eq. (A-3), u is the average wind speed,
R is a reflection factor to account for the presence
of the ground and a and CTZ are the lengtrfs corres-
ponding to the standard deviation of concentration
in the y and z directions. The other symbols are
as given earlier.
Deposition from such a plume will result in
depletion of the material originally airborne there-
by reducing the quantity available at the receptor.
The evaluation of the deposition rate is usually
accomplished by use of a deposition velocity, Vj ,
defined as the ratio of the rate of deposition on a
given area to the air concentration at a reference
height above the area.s The dimensions of such a
ratio are those of velocity. The product of the de-
p'b.sition velocity and the concentration gives the
absolute rate of deposition from the atmosphere at
31
-------
290
a given location. The quantity depositing between
the source and the receptor is, then:
(A-4)
D" = exp
RV,
^ u4
(A-5)
In this method cfi.accounting for deposition, a
fraction of the material in the plume is assumed to
deposit per unit of plume length and this fraction is
removed from the plume. In essence, this correc-
I
tion factor reduces the source term to allow for the
material which is lost. It is unsatisfactory in many
ways since it implies a uniform depletion through
the full height of the cloud and does not account for
the concentration gradient which will exist in the
profile above the ground because of the continual
depletion at the ground surface. An alternate ap-
proach would be to account for the rate of change
in the vertical cloud dimensions as expressed by
the change in a as a factor in bringing the material
to the layer above the ground. However, this equa-
tion will be used in this model until further develop-
ment of concepts can be made.
In order to apply these equations, relations
between the values of a , a and1 the distance from
the source must be used. A number of different
methods of expressing these correlations have been
derived by different individuals. In one of the ear-
liest methods, Sutton7 provides a relation Between
the standard deviation and distance using two addi-
tional parameters which are dependent upon the at-
mospheric stability and the turbulence. The stand-
ard deviation for both the horizontal and vertical
growth increase downwind as a power of the dis-
tance with the power changing as the atmospheric
stability changes. Pasquill5 provides a set of
curves for the growth off and az based upon a
classification of the stability and values of CTQ, the
1 0
standard deviation of the wind direction fluctuations
•which have been found to be reasonably character-
istic of these conditions. Fuquay8 uses the product
of a u where the a term is the same as in Pasquill1 s
y d
and the u is the average wind speed. In addition,
Puquay expresses the dispersion as a function of
the time of travel rather than the distance. Other
systems of classification are available but the above
indicates some of the variations. While the exper-
ience of the author indicates that the system of
Fuquay has much merit and gives about as good
correlation as can be expected, it also has the dis-
advantage that the expressions are complicated,
making integration difficult, and the information
available in most situations to evaluate
-------
X = •
RQ
u n c cz
(a-n)
exp
291
(A-7)
From the point source equation, the contribu-
tion from other configurations of the source can be
evaluated by integration. For a complex deposition
pattern which cannot be expressed as an equation,
this integration must be performed by numerical
techniques. However, there are several simple
configurations for which analytical expressions can
be derived, particularly with the Sutton method of
expressing the plume growth. These are given be-
low for the convenient, dimensionless parameter
Infinite Line Source Upwind
XG R
-
exp
(A-8)
Q' - Source contamination per unit length of line.
Gaussian Line Source Upwind ('}
(Sampler directly downwind from peak concentra-
tion, np. Material along line distributed with
standard deviation of Ameters. )
(A-lOa)
n" - source contamination per unit area.
Equation (A-lOa) is somewhat misleading in
that it provides the concentration at the ground
surface rather than at some height above the ground.
In this situation, the small area immediately up-
wind contributes strongly to the final answer while,
in practice, the material from this area may con-
tribute only slightly to a receptor at some height
because the growth in the vertical height of the
plume may be low enough in this distance so that
the material from the ground does not have a chance
to reach the receptor elevation. For an elevated
source, a numerical integration is needed for the
initial distance where exp(-zs/Czx ~ n) is less
than one with application of Eq. (A-lOa) beyond
this distance.
exp -
(A-9)
A2
Uniform Area Source - Infinite in Y
(Receptor at ground level, xi distance to nearest
boundary; KS distance to further boundary of con-
tai*ninated area. )
Xu
u .
Vd
- exp
(A-10)
-------
292 '
B. Choice of Parameters
The dispersion parameters to be used in the
foregoing equations can be obtained from the cor-
relations of past experiments on turbulent diffu-
sion. 5 These correlations are not completely sat-
isfactory in a number of respects but they do rep-
resent a body of experience which can be applied
without repeating all of the experimental work
under the specific conditions of interest in this
problem. However, we do emphasize the follow-
ing limitations on these data. In the correlations,
the data are stratified into arbitrary classifications
of stability while the'-atmosphere in its variations
acts as a continuum. Thus, some restraint is
placed on the description of the variability by the
categorization. Of probably greater importance,
there is no agreed-upon method of defining sta-
bility for the purposes of classification so that dif-
ferent investigators will use different parameters
>c;- different variations of the same parameter) in
describing the classes. This also gives rise to a
subjective interpretation of the meaning of the
classes for experimenters working in different
areas or for individuals applying the data to dif-
ferent areas. For example the term "strong in-
version" can well have a different meaning to an
individual in a flat desert country Inhere very strong
inversions can occur or to an individual in an area
where temperatures are moderate with cloud cover
a large portion of the time. In the following work,
we will see instances where different parameters
are used to describe the degree of stability for dif-
ferent parameters to be used in the equations. As
will be noted, there is no assurance that the judg-
ments made on these two different methods of ex-
pressing degree of stability represent the same
condition of the atmosphere. While this factor is
troublesome from the standpoint of logic and, to
some extent scientific accuracy, this method of
classifying the data is probably about as good as can
be done without running into an overwhelming mass
of detail and the results are undoubtedly adequate
considering the remainder of the unresolved uncer-
tainties that occur elsewhere in the problem. A
more serious problem would seem to arise from
the uncertain dependence of these parameters on
the time of sampling or the time of interest at the
receptor. Particularly for the value of J the fluc-
* y
tuations in wind direction will increase as the time
of sampling increases making the value of the cloud
spread dependent upon the time. Sutton recognized
this problem in his early work and specified his
parameters for a relatively short sampling period.7
Many of the differences between the present cor-
relations and those of Sutton are undoubtedly due
to the fact that most of the samples incorporated
in these experiments were taken for periods of 30-
60 minutes. The importance of this factor lies in
the fact that the selection of a given parameter for
the dispersion also implies a given fluctuation of
wind direction and averaging.of the downwind plume
over these fluctuations which, in turn, implies a
given time of sampling under the turbulent condi-
tions existing. Such considerations are of greatest
importance when attempts are made to derive val-
ues of the pickup rate from air concentration meas-
urements around a known source of contamination
on the ground. Related to both of these problems
is the uncertainty of the growth of the plume in the
vertical, particularly in the stable condition. While
the argument can be made that wind pickup should
not be of great importance under stable conditions
because of generally low wind speeds and turbu-
lence, this has not been demonstrated and the prob-
lem of dispersion from mechanical disturbances
occurring under these conditions still exists. As
an illustration of this problem, there are data for
very stable conditions which indicate the vertical
growth to be considerably lower than is predicted
by any of the models normally used. The value of
"z is of particular importance to these calculations
since the deposition between the source and the
reteptor is strongly dependent upon this param-
eter and the importance of the long term average
34
-------
concentration at a given elevation means that the
primary dispersion mechanism over the long period
of time is due to the vertical growth (i. e. , the hori-
zontal dispersion in the plume is averaged out by
the changes in wind direction so that the value of a
is of interest only for the short sampling period. )
In view of the above considerations, it would
seem that experiments designed to measure the
pickup from the ground should provide a direct
method of measuring the dispersion parameters and
their growth during thu time of sampling. This
could be, for example, a smoke plume or other
tracer material wlflich would give direct evidence on
i
the actual conditions at the time. Alternately, one
could use a line source of sufficient length so that
the value of CT is not important and concentrate on
t Y
the vertical dispersion, perhaps by measuring a *
profile with height. This is not to say that the con-
ventional measures of stability and wind fluctuation.
should be disregarded. Rather, these methods
should be used to supplemenlj the more conventional
meteorological data.
For calculations in this paper, we have cho-
sen a set of parameters reasonably representative
of unstable, neutral and stable conditions. These
are given in Table A-I.
The values of a and «z reselling from these
choices are compared with.those of Pasquill in
Figs. A-l and A-2.
The selection of an appropriate deposition ve-
locity is difficult because of the lack of an organized
set of information on this subject. In order to pro-
vide a method of choosing the deposition velocity in
relation to the particle size and the differing atmos-
pheric conditions, a rough model to describe the
TABLE A-I
BUTTON PARAMETERS USED
Atmospheric Condition
293
Unstable
0.2
0.45
0. 3
Neutral
0. 25
0.2
0. 1
Stable
0. 5 '
0. 3
0. 07
10
I0
Distance (m)
I0a
Fig. 'A-l. Comparison of a for Pasquill's curves
and Sutton using parameters of Table
A-I.
deposition velocity was derived as based upon cur-
rent data. This model is described in detail in
Appendix B. This work predicts that the deposi-
tion velocity will vary directly with the wind speed
for the particle sizes of interest and will also be
dependent upon the deposition surface as meas-
ured by the surface roughness parameter ZQ. It is
in the choice of this valu'e that one of the main dif-
ficulties occurs in selecting parameters which are
consistent for a given stability class since the sta-
bility classification basis for the depositionivelo-
city is the Richardson's number which can be only
indirectly related to the stability used to describe
the Sutton parameters chosen.
35
-------
294
Distance (m)
Fig. A-2. Comparison ot«z for Pasquill's curves
and Sutton using parameters of Table
A-I.
In the development of the deposition velocity
model, a constant rate of transfer of the particles
through the boundary layer to the ground was con-
sidered due to the turbulent transfer across this
boundary. The primary effect of particle size (in
sizes less than those where the gravitational forces
predominate) was considered to be in the retention
once the particles were brought to the ground.
From the data available, it appears that particles
above about 1. 5|_im will be strongly retained with
the retention dropping off with particle size. For
this reason, the reflection factor in the dispersion
equations was written as (2-f) where f is the frac-
tion of the material reaching the ground which is
retained. Thus, for a material completely re-
tained, the reflection factor becomes 1 or the con-
centration is simply due to the direct transport
from the source.
The parameters for the deposition and .re-
flection which have been chosen are given in
Table A-II.
Unstable
»0 (cm) 0. 1 2. 3
>1. Sum Particulates
TABLE A-n
DEPOSITION PARAMETERS USED
Atmospheric Condition
Neutral
0.1 2.3
Stable
0.1 2.3
Vd/u 0.0093 0.017 0.0028 0.0080 0.0046 0.0029
<0. lum Particulates
(2-f) 1.97 1.97
1.97 1.97 1.97 1.97
Vd/u 0.0003 0.0005 0.00008 0.0002 0.00001 0.00009
III. RESUSPENSION RATE MEASUREMENTS
The key to the application of a model such as
this is, now, the definition of the rate of resuspen-
sion under the conditions of interest. Unfortunate-
ly, the information available from experiments
which included the necessary meteorological data
as well as the measured distribution of activity on
the ground and the air concentrations resulting are
extremely limited and cover only a. few of the many
terrain and soil possibilities of interest. However,
in this 'section we will discuss the data available
which bear on this question in order to arrive at
the best possible answer at this time and to provide
some illustration of the application of the method.
A. General
The movement of surface grains under the
action of winds has been studied for desert sands
by Bagnold9 and for agricultural fields by Chepil1 °
with only a few of Chepil's many papers referenced
here. This work has outlined the mechanisms in-
volved in producing soil erosion and has described
the influence of a number of important factors. A
brief outline of some of these concepts whichimay
be important to resuspension on the scale of inter-
est here is given below with no attempt to make
this an exhaustive treatment.
Three chief methods of movement of soils
are given as surface creep, saltation and suspen-
sion. In surface creep, the grains move along the
surface either by the direct forces transmitted to
them by the winds or by the impact of other grains.
36
-------
In saltation, the grains rise into the air for a lim-
ited distance during which distance they gain mo-
mentum in the direction of the wind and fall back to
the ground along a diagonal path to the horizontal.
In suspension, the grains, once raised from the
ground, are small enough so that the turbulence of
the air stream keeps them suspended and will move
them to higher altitudes by turbulent diffusion. Sur-
face creep occurs at the ground surface while grains
in saltation seldom rise more than a few feet above
the ground. While these latter phenomena are of
importance in spreading an initially contaminated
area and in posBitty eroding tjhe size of the grains
so that they become capable of suspension, the re-
suspension of concern in this paper is primarily as-
sopiated with the fraction which these authors have
\
categorized as the suspended fraction since this
will be composed, at least partially, of grains with
particle size in the inhalable range.
The soil grains in the medium size range of
about 0. 1 to about 0. 5 mm are the ones affected by
saltation with grains 1 mm or greater in diameter
too large to be moved even in surface creep by or-
dinary erosive winds. Chepil10 points out that the
erosive action of the winds is primarily due to the
saltation process since the bounding particles pick
up energy from the winds duringltfhe period which
they are airborne and this energy is transmitted to
the soil particles upon impact to move the larger
ones by surface creep, to provide energy to saltate
more particles or to dislodge the smaller ones to
permit the wind to carry them away in suspension.
He has'also observed a threshold velocity in the
wind speed which will result in soil movement.
This threshold velocity is least for soil particles
of about 0. 1 to 0. 15[_im in diameter and increases
for both smaller and larger particles. At this min-
imum, the threshold velocity is about 8 to 9 miles
pe'r hour at 6 feet above the ground. For the
smaller particles, the higher threshold velocity is
attributed to the smooth character of the surface
attained and the nature of the turbulence in the air
contain^-
above the surface. However, for mixtures
ing both erosive particles and fine particles the
threshold wind velocity can be much lower than for
the fine particles alone. Chepil also points out that
the threshold velocity is not affected by surface
roughness features such as ridges.
This work on the erosive properties of winds
provides considerable insight into the forces and
problems encountered in the resuspension problem.
However, the complete applicability of the concepts
and measurements to thp problem at hand is ques-
tionable since the observations are necessarily of
a gross nature because of the interest in the move-
ment of large quantities of soil. Thus, consider-
able interest in the erosion work is attached to the
condition where the mass of soil carried by the
wind is sufficient to'change the wind profile close
to the ground because of the added momentum of the
soil carried. In some of the data for mass flow
over loamy soils, the suspension flow varies from
abovtt 30mg/cma at ground level to about 3mg/cma
at 24 inches above the ground with wind speeds of
13 to SOmph at a height of 12 inches. These flows
convert to concentrations of tenths of grams to
grams per cubic meter. This is not to say that
such conditions are not of concern in resuspension
work but that the mechanisms involved in resus-
pending the small particles of interest may be dif-
ferent from those observed in the gross erosion
studies and the frequency of occurrence of the
heavy loads in most areas is relatively small unless
there is widespread disturbance of the soil surface,
as in many agricultural practices.
There is a series of observations on the effect
of soil condition and terrain which would seem to
have some relevance to the resuspension studies.
It is indicated that particles less than 0. 005mm (S
|jm) do not exist, as such, in ordinary soils since
they become aggregated into larger particles. How-
ever, it is also noted that large quantities of non-
er"osive soil are converted to erosive material by
abrasion caused by the moving soil grains. Thus,
37
-------
296
one would expect some breakup of the aggregates
formed by the soil and a contaminant by a similar
mechanism or by mechanical disturbances. If a
surface has been undisturbed for some time, the in-
itiation of erosive movement can require a higher
velocity than for succeeding wind storms due to the
formation of a surface crust which is broken by the
erosion caused by the first high wind. When soil is
carried by saltation, it can be sorted into dunes.
This process can increase the susceptibility of the
soil to later pickup and decrease the threshold velo-
V"
city. Such increase ifi. susceptibility may be of par-
ticular importance when the succeeding wind comes
from a different direction and can, therefore, pick
up material previously deposited in an eddy behind
an obstruction. A rain storm may have an effect
in increasing the threshold velocity but it has been
observed that such effects will not persist after the
rain since a few grains in saltation will break the
surface crust.
I
It is obvious that no one resuspension rate
will be applicable to all conditions. A listing of
variables which would be expected to influence the
results "would include:
1. Particle size distribution in the soils
2. Particle size distribution^ the contami-
nant
3. Distribution of contaminant through the
soil profile
4. Moisture content of the soil
5. Chemical composition of the soil (cement-
ing and compacting)
6. Type and magnitude of vegetative cover
7. Obstacles to airflow and turbulence in-
ducers
Since all of these factors can also change with time,
in particular the moisture content, vegetative cover,
distribution of the contaminant in the soil profile
and the particle size of the contaminant through ag-
gregation, a thorough understanding of the mecha-
nisms of resuspension will require characteriza-
tion of many variables. Since powerful numerical
techniques are now available for studying hydrody-
namic problems such as this, a theoretical program
to provide some insight into the importance of such
variables would seem to be of great value. In ad-
dition to providing this insight, such a study could
provide valuable guidance in defining the types of
measurements to be required in the field.
One factor not considered above, nor in this
calculational model, is that of surface redistribu-
tion through runoff of water or movement through
the actions of the winds. - There is no doubt that
this is of considerable importance since such re-
distribution will affect not only the area covered
but the redeposition will be in places where the
susceptibility to resuspension may differ from that
in the original position. However, the complexi-
ties of this problem are beyond the scope of this
treatment and study of this will be deferred to a
later date. *
Item 3, the distribution through the soil pro-
file, is': of considerable importance in interpreting
field results. For wind pickup, for example, the
material which is deeply buried will not be in a
position where the wind forces can act on it and
should, therefore, not be included in any estimate
of the source term. Thus, samples taken to a
depth of several inches can be misleading if a sig-
nificant part of the contaminant occurs below the
surface but is included in the measurement of the
inventory and is interpreted as part of the contam-
ination of concern. It can be predicted that the
critical thickness of the contaminated layer of in-
terest will vary with the degree of disturbance
1
which causes the material to become airborne.
However, for most cases, the prediction of this
thickness is not now possible. For pickup by winds
we can speculate that this thickness may vary with •
the wind speed due, in part, to the increased size
and energy of the particles carried in saltation or
surface creep with higher wind speeds and their
consequent ability to disturb a deeper layer of soil.
Note that if this is true, the dependence of air
38
-------
297
concentration with wind speed will have a terrti not
usually considered if the contamination is deeper
than the immediate surface, (i. e. , the source term
will change due to the availability of material buried
in the ground at greater depths. ) Thus, in meas-
urements of resuspension, as well as in applying
measured rates to other areas, it is of great im-
portance to specify clearly the depth of burial of
the contaminant and to take into account differences
in the depth. Again, some theoretical studies us-
ing the numerical, hydrodynamic techniques now
available could possibly be of us'e in better delin-
eating this problem! and some of its ramifications.
Another factor which can contribute uncer-
tainty to the final result is the question of particle
size of the contaminant (and soil) and its influence
on the rate of resuspension. The work of Chepil,
discussed earlier, indicates a definite dependency
of the erosion rate on particle size distribution of
the soils with uniform, relatively small particles
requiring higher wind speeds to dislodge than het-
erogeneous mixtures of several hundred jam par-
ticles. Again, the mechanisms by which the par-
ticles are transferred to the air are of importance
but not well defined quantitatively. For non-vegetated
areas, the mechanical transfer of energy from par-
ticles in saltation or surface cr^'4p would seem to
be the primary sources of such energy. Here, the
energy available would seem to increase as the
square of the wind speed but it is not clear that this
energy would be transferred to the soil particles in
such a manner that particles of all sizes would be
dislodged in proportion to the energy. In other
words, it is not now known whether all particle
sizes will contribute to the source term in propor-
tion to their fraction in the soil at all wind speeds
or whether one would expect changes in the fraction
of different sizes airborne as the wind speed changes.
(Note that there will be a change in the upper end of
the particle size spectrum, with the number of
larger particles increasing with wind speed, simply
because the energy available will dislodge larger
particles at the higher speeds and the increased
turbulence will result in longer times of residence
in the atmosphere. The effect on the smaller, in-
halable sizes, however, is not clear. )
B. Rate of Re.suspension - Direct Experiments
•'; ~~~~
The bulk of the information available in the (.
literature on the resuspension factor is not ade-
quately documented with meteorological conditions
and extent of the contaminated area to permit deri-
vation of the rate of resuspension from the meas-
urements of the air concentrations although, as
will be seen, some estimate of the order of mag-
nitude under the conditions at the time may be de-
rived.
In the earlier papers on resuspension,3'* a
rate of resuspension was derived from experimen-
tal measurements downwind from a source of zinc
sulphide particles spread on the ground. In this
paper, an attempt was made to account for particle
size'iby inclusion in the pickup coefficient of a term
combining the particle density and area exposed to
the wind, a refinement presently not believed to be
completely applicable until more data on the effect
of particle size are available. For this reason, the
pickup coefficient in the earlier paper is not the
same as the one used in Eq. (A-l). HoweVer, a
conversion can be made by comparison of the equa-
tions. This technique was used since the pickup co-
efficient in the earlier paper was calculated using
the actual wind direction in relation to the position
of the sample in order to make a correction for an
off-center plume and these data are no longer avail-
able. From this comparison, the MMD of the zinc
sulphide particles used (7|jm) and the density of
ZnS (4. Ig/cc), the conversion from the coefficient
in the earlier work (K1) to the coefficient used in
this paper (K) becomes:
K =
K'u'
pd
= 0.035 K'us (A-ll)
39
-------
298
TABLE A-III
RATE OF WIND PICKUP OF ZnS PARTICLES
First experiment - sandy soil, sparse desert grass,
and clumps of sagebrush 0. 5 to 1 meter high.
u K
K/us
m/sec Sec~lxl09 Sec/max
2.7 90
3. 1 140
2.7 SO
0.9 130
2.7 70
2.7 40
1.8 10
Second
Course
Control
Furrowed
1
Rock
Snow fence
9.5
15
6.7
16
9. 5
18
3.9
experiment -
u
u
1 09 m/sec
1.8
2.7
2. 2
3.6
1.8
1. 3
1. 3.
K
Sec-'x 10s
60
150
60
160
26
40
40
K/us
Sec/maxl09
17
20
13
13
8. 1
24
24
prepared courses.
K
m/sec . Soc~1x 10U
5. 8
10
8.1 ,
6. 7 ''
8, 2
5.8
10
8. 1
6.7
8. 2
5.8
10
8. 1
6.7
8.2
5.8
10
8. 1
6.7
8. 2
120
2450
70
'1 310
940
350
700
920
140
240
350
3500
230
470
470
47
350
140
310 -
240 '
K/i"
Sec/m3x 10"
3. 5
25 ['
1. 1
6.7
1 14
11
7
14
3. 2
3.5
11
35
3.5
11
7
1.4
3.5
2. 1
7
3. 5
Itnn.irks
Damp
Wet
Wet then dry
Damp
Wet
Wtt then dry
Damp
Wet
Wet then dry
Damp
Wet
Wet then dry
Values of the rate of pickup for these parti-
cles as obtained from the conversion are given in
Table A-III, The value of K/u2 is included since
the total energy available in the wihd varies as the
square of the wind speed although there are other
factors, such as wind profile and turbulence which
will also affect the results.
These results are representative of the par-
ticular type of particles used as a tracer and rep-
resent the pickup a relatively short period of time
after the deposition has occurred. No significant
change was seen.in the rate of resuspension in the
one week period over which measurements were
made in the first experiment. It is of interest to
note that positive concentrations were measured at
low wind speeds, on the order of one m/s or less,
or lower than the minimum threshold velocity
given by Chepil. This may be due to the existence
of gusts with speeds much above the average but
cannot be attributed to pickup at an earlier time
•when "winds were stronger because of the short
distances involved in the experiment.
Several other experiments under field condi-
tions were examined briefly to provide an order of
magnitude estimate of the results. In most of these
experiments, the published literature is inadequate
to permit full evaluation since required details are
not given. They are reviewed, however, with as-
sumptions made us to the missing data.
Wilson et al11 report on an air sampling pro-
gram associated with the contamination of an area
following a safety test with a nuclear device con-
taining plutonium at the Nevada Test Site. Data on
the detailed contamination patterns are not given
although it is noted that samplers were located ap-
proximately northeast of ground zero at distances
of about 7500 feet (at the 10|jg/m2 contour), 2500
feet at the 100ug/ma contour1 and at about 750 feet
at the 1000f_ig/m contour. It was further noted
that ttie winds blew generally from the south dur-
ing the period of the experiment (about 60% of the
time) and that this wind direction missed the high-
est contamination areas. Because of the wide var-
iation in the air concentrations measured, only
the median concentration of the three samplers at
each of the 10 and 100|jg/m2 isopleth and the two
samplers at the 1000)jg/ms isopleth are given.
These were read from a plot in the reference.
Sampling started about 2,3 days after the contami-
nation pattern was established and continued for
20 weeks.
It was assumed, for rough estimation pur-
I
poses, that the average concentration level in the
area over which the wind blew was three times the
level at the location of the sampler and the average
distance of contamination over which the wind blew-
before reaching the sampler was equal to the dis-
tance from the sampler to ground zero. The aver-
age wind speed was taken to be two meters per sec-
ond with neutral conditions. Since particle size
analysis showed the resuspended materials to have
40
-------
299
TABLE A-IV
ROUGH ESTIMATES OF PICKUP RATE FROM NEVADA STUDY
* di s / min
630
330
330
140
31
55
220
90
150
82
35
110
68
58
1
42
65
39
52
22
av
10ug/m2
K
x 10s
Sec-1
60
__
30
30
10
3
5
20
8
10
8''\'
3
10
6
5
4
6
4
5
2
10
100|ag/m2
K/u2
xlO9
m2 /sec
20
8
8
3
0. 7
1
5
2
4 V"
2 ,
0. 8
3
2
1
1
2
0.9
1
0. 5
3|
*dis/min
1200
680
250
1200
130
620
290
95
120
600
230
310
70
35
150
200
23
130
85
95
K
xlO9
Sec-1
10
7
3
10
1
6
3
1
1
6
2
3
0. 7
0.4
2
2
0. 2
1
0.9
1
3
1000ug/m2
K/u2
x
rn2
3
2
0.
3
0
2
0
0
0
2
0
0
0
0
0
0
0
0
0
0
0
10°
/ sec
. 6
. 3
. 8
. 2
. 3
. 6
. 8
. 2
.09
. 4
. 5
.06
. 3
. 2
. 2
-,,8
*dis /min
8000
:M200
1200
1800
230
950
2500
1100
2500
1100
1000
2100
850
140 -.
650
490
1£0
200
100
180
K
xlO9
Sec-1
9
1
1
2
0. 3
1
3
1
3
1
1
2
0.9
0. 2
0. 7
0. 5
0. 2
0. 2
• 0. 1
0. 2
1
K/u
;
x 109
m2/s
2
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
'• o.
0.
0.
ec
3
3
5
06
3
7
3
7
3
3
6
2
04
2
1
05
06
0'3
05
4
'"Quantity collected in one week at a
flow rate of 17 liters per minute.
an average mass median diameter of 1. 5 to 2. 5 |_im,
the deposition velocity was assumed to be that cor-
responding to the turbulent transjfjsr velocity. The
values of the expected air concentrations for a unit
deposition levelwere calculated from Eq. (A-10) and
were corrected for the assumed two m/sec wind
speed. These results are given in Table A-IV for
the successive weeks of sampling.
T,he uncertainties in these results due to the
necessary assumptions are obvious, but it is of in-
terest that they are generally not greatly different
from those measured with the zinc sulphide parti-
cles. It is not surprising that they are lower since
th'e zinc sulphide data were obtained with short pe-
riod air samples with the wind blowing from the
source to the'sampler while these values represent
a week's sample with no correction for the fraction
of time that the wind blew across the contaminated
area. Further, there is no correction for periods
of higher wind velocity nor for differences in sta-
bility of the atmosphere which would be expected
from day to night. Soil sampling at the location of
the samplers indicated the nominal isopleths to be
high by a factor of about,four at the 10^g/m3 loca-
tion, 2. 5 at the 100jjg/m2 location and 2 at the 1000
(jg/m2 location. Use of these soil values for the
calculation would increase the resuspension factors
I
estimated by these factors. The generally lower
resuspension rates for the higher contamination
areas could be due to a number of different causes
including a greater sensitivity in these areas to a
misestimate of the effective path length of the wind
over the contaminated areas and the fraction of the
time that the wind blows over this path; shorter
crosswind dimensions so that the area is not really
infinite in the y direction as is assumed inEq. (A-10);
41
-------
300
differences in particle sizes of the contaminant with
larger particles in the more heavily contaminated
area close to ground zero; or failure of the contam-
ination to reach the five foot height of the samplers
in the shorter, more contaminated areas.
Mork12 reports on an experiment at the
Nevada Test Site in which a vehicle was driven back
and forth across a stretch of ground contaminated
with plutonium for one hour while air samples were
taken at two points 20 feet from the vehicle path and
at two points 100 feet from the vehicle path. The
V"
experiment was conducted in a region between two
i*:,
sampling points designated as number 62 and 63
which, in turn, were reported to have contamination
levels of 6. 21 x 10s dis/min per square foot and 6. 63
x 105 dis/min per square foot. The vehicle path
was 1320 feet long with the samplers located about
one-third of the distance from each end. The ex-
periment was conducted twice. The first in the day-
time was from 1138 to 1238 and the second (labeled
I
as at "night") was from 1725 to 1825. Since it is
doubtful that the nighttime inversion would have set
in by this time in the evening, both sets of data were
evaluated considering the atmosphere to be unstable.
Neither the wind direction or the wind speed
were given. It was, therefore, assumed that the
wind was blowing across the vehicle path toward
the samplers. Gummed paper deposition collectors
were included which permitted a rough estimation
of the deposition velocity to this surface by compar-
ison with the air concentration. The results of this
experiment as calculated under these assumptions
are given in Table A-V.
The deposition velocities would indicate that
larger particles were involved in most cases. The
relatively lower values of resuspension in the second
experiment may indicate that the course had under-
gone depletion or that some other factor in the con-
ditions had changed. The value of K/u2 is not esti-
mated for these data since the source term is
assumed to be more dependent upon the mechanical
disturbance than on the energy transmitted by the
TABLE A-V
MECHANICAL U1STUKBANCK RESUSPENSION
West
1138-1238
Vd (ill/ sec) 0.5
K(scc-') 160xlO-9ij ^OO
1725-1825
Vd (nVsuc) 0. 3 2
K (sec-1) 130xlO-°u IS
0.004 0.9 0.02
OOxlO-'u 3000:<10~"u ZfcOOxK
0.4
ISOxKr'u
winds. Although comparison with the values of K
from the other experiments is difficult, it does
appear that resuspension rates up to 100 times
those from the natural winds can occur from this
type of mechanical disturbance in this type of ter-
rain.
In a more recent paper by Sehmel13 the par-
ticle resuspension due to moving vehicles on an
asphalt road was measured by use of ZnSparticles'
with a mass median diameter'of about ;5 |am. These
particles were distributed uniformly over a length
of 100 feet on one lane of an asphalt highway and
cars and trucks were driven at different speeds
either on the adjacent lane (by-pass) or through
the contaminated lane. Runs were made while the
winds were perpendicular to the highway and the
fraction resuspended per pass was evaluated from
air samples and deposition samples downwind. For
purposes of this discussion, the values for the re-
suspension per pass were converted to fraction re-
suspended per second from consideration of the
wind speed of the vehicle and the 100 foot path
length. This was done to enable comparison with
previously derived resuspension rates. The data
from this work are given in Table A-VI.
As is pointed out by Sehmel, the relative con-
stancy of the ratio of the rate of pickup to the
square of the vehicle speed indicates the primary
mechanism of pickup is due to the turbulence in-
duced by the passage of the vehicle. Again, the
data indicate increased pickup rates, in this case
V
by as much as three or four orders of magnitude
over those measured from ZnS in the soils and
42
-------
301
TABLE A-VI
RESUSPENSION RATES OF ZnS PARTICLES FROM
ASPHALT ROAD BY VEHICLES
Tn i-r-» a Q-i !•»<•• ft VellicIC
1IT16 OlllCG v ^•m^-A*-
Deposition Vehicle Path
(days)
0 Car By-pass
Through
*Truck Through
V"
4 *Truck By-pass
1 1 ;,'
'
Through
5 Car Through
30 Car Through
Vehicle
Speed
(m/soc)
2.
6.
13.
22.
2.
13.
22.
2.
22,
6.
6.
13.
13.
2.
6.
6.
13.
22.
13.
13.
22.
2
7
4
4
2
4
4
2
4
7
7
4
4
2
7
7
4l
4
4
4
4
Fraction
Re suspended
per pass
4.
2.
7.
1.
1.
6.
1.
2.
6.
1.
4.
8.
8.
1.
5.
2.
1.
2.
5.
5.
2.
8 x
8 x
7 x
1 x
9 x
9 x
1 x
5 x
7 x
2 x
8 x
6 x
2 x
3 x
2 x
1 x
0 x
3 x
7 x
5 x
6 x
1(TS
io-4'
io-4
io-3
io-4
10- 3 •
lO"2
10~3
io- 3
10- 6
1Q-B
10- 5
10~5
10- 5
io-4
io-4
10- 3
io- 3
10- 5
10~6
io- 5
Fraction
Resuspended
per sec
(K)
if 3-
6.
3.
8.
1.
3.
8.
1.
4.
2.
1.
3.
3.
9.
1.
4.
4.,
1.'
2.
2.
1.
5 x
2 x
4 x
1 x
4 x
0 x
0 x
8x
9x
6x
1 X
8 x
6 x
5 x.
1 x
6 x
4 x
0 x
5 x
4 x
9 x
io-6
1Q-5
io-4
io-4
10- s
10- 3
10~3
io-4
io-3
io-6
io-s
10- B
10"6
io-7
10~4
10- s
io-4
io-3
io- B
io-6
10" 5
K
(Vehicle Speed)2
7.
1.
1.
1.
2.
1.
1.
3.
9.
5.
2.
2.
2.
1.
2.
1.
2.
2.
1.
1-
3.
0 x
4 x
9x
6 x
8 x
7 x
6 x
7 x
8 x
9x
3 x
1 x
0 x
9 x
5 x
0 x
5 x
0 x
4 x
4 x
8 x
io-7
10~6
io-6
10- fi
io-G
10"5
1Q-B
10- s
IO-6
io-8
10~8
io-7
io-7
10- 5
10~s
10~6
io-6
io-6 .
io-7
ID'8
io-8
*3/4-Ton Pickup Truck.
natural winds. The data taken at later times, how-
ever, indicate a relatively rapid decrease whether
due to fixation of the particles or prior removal is
uncertain. Sehmel does provide a rough calculation,
however, which indicates that the depletion from
such a surface with any significant traffic would be
rapid.
C. Changes With Time
It is to be expected that the susceptibility of
a contaminant to resuspension will change with time
due to factors such as agglomeration with the soil
particles; possible chemical changes of the con-
taminant; migration of the particles downward in
the surface through action of rainfall, alternate
freezing and thawing; and redistribution, perhaps
into areas protected from the winds. For materials
deposited in-an area with high mechanical distur-
bance, such as a highway, the latter factor will be
of great importance in moving the material to an
area where the disturbance is lower.
Wilson, et al11 investigated the resuspension
of plutonium in an area at the Nevada Test Site
which was contaminated during a safety test in
April 1957. Samples were taken with impactors
at a height of five feet above the ground starting
about one month after the area was contaminated
and continuing for twenty weeks. Three samplers
were placed at the nominal 10|jg/m2 contour (^-7500
feet from GZ), three at the 100|_ig/m2 contour (-^2500
feet) and two at the 1000|_ig/m2 contour (-v-750 feet).
The samples were pooled to give weekly estimates
of the concentrations at these locations. The sam-
plers were located so that the winds blew directly
over the most contaminated area only about 10% of.
the time during the period of sampling. It was noted
that: "The sampling data are too erratic to establish
half-times for the 'decay' of air concentration be-
yoind a very crude estimate. " These estimates
were obtained by plotting the median of the stations
43
-------
302
100
• Median weekly concentrations from
Wilson et al.
Individual samples, Olofson & Larson
T|/2'5wecks
10 20 30 10 50 GO
Time Since Sompling.Started (weeks)
I
Fig. A-3. "Decay" of Air Concentrations -
1000 |ag/m3.
70
10
• Medion weekly concenlrolions from
Wison ct a!.
* Individual samples,Olafson & Lorson
0.01
0
-T « 5 weeks
10 20 ' 30 40 50 GO
Time Since Sampling Started (weeks)
Fig. A-4. "Decay" of Air Concentrations -
100 ^/ma.
70
on a given isopleth. This yielded an estimate of
five weeks for the half-time of concentration decay.
During the summer of 1958, (studies of the
air concentrations were conducted at the same
site.1* The two high level locations for the loca-
tion of the samplers were quoted as being at ". . .
essentially the same location as the nominal 100
and 1000 )agm locations of Wilson et al. " The data
for these' two locations for the median of the weekly
samples from Wilson and for the individual samples
reported by Olafson and Larson are plotted in Figs.
A-3 and A-4. While the use of the week-long
sample and the median value of several samplers
tends to reduce the absolute concentration due to
wind fluctuations over this time and also tends to
reduce the statistical spread, the concentrations
reported 40 weeks after the first series raise
some questions as to the long term applicability of
the 35-week half-life. It is noted that there are
other factors which could produce a reduction in the
air concentrations such as a seasonal shifting of the
winds .resulting in a lower contaminated area up-
wind or a seasonal change in wind speed. Both of
these variables could result in a regular decrease
in air concentration with time if the change in the
winds occurred in a systematic manner.
In one other experiment, Morkls reports
data taken three feet above the ground in October
1956 and in July 1958 at Station 61 at the Nevada
Test Station. These samples were in an area con-
taminated with plutonium during December of 1955
and January of 1956. In a seven day period in 1956
series the concentrations averaged about2xlO~a
Hg/m3 with a range of about 4xlO~9 to 6x 10~8
(jg/m3. In a 20 day period in the 1958 series, the
concentrations averaged 2x 10~7 iag/m3 with a range
44
-------
in the values from 0 to 7 x 10"7 ug/m3. While,
again the wind directions and speeds may well have
differed during these two periods, there is no indi-
cation of a measurable decrease with time over a
period of some twenty months or about 85 weeks.
As was indicated, one would expect a change
with time, .but it is bolieved that the data now avail-
able are not adequate to permit the assignment of
a particular decay rate, particularly for areas of
different characteristics from the Nevada Site. In
particular, it is believed that the use of the 35-day
half-life is inappropriate since''this would indicate
that the concentrations drop rapidly and, for long
term occupancy considerations, result in exposures
estimated only for the initial period of occupancy.
A.more reasonable estimate to describe this phe-
nomenon would be to consider a drop by a factor of
ten over the first year or two with the conditions
stabilized thereafter to give relatively little de-
crease.
In view of the informdtion available on the
initial concentrations at specified locations at the
Nevada Test Site, it would appear to be reasonable
to mount a campaign to resample these locations
over a period of time and to attempt to reconstruct
the meteorological conditions for the initial sam-
ples. While the deposits have tflen disturbed by
the various activities in these areas, such a series
of samples could give some indication of the long
term decrease.
D. Dust Concentrations
•The concentrations of natural dust in the at-
mosphere arise, at least in many areas, from re-
suspension of soil grains under natural or mechan-
ical disturbance mechanisms. As such, data on
these concentrations can be used to give at least
gross indications of the importance of resuspension
in various terrains and locations. Again, such in-
formation must be interpreted with restraint, con-
sidering the differences which may exist between
the deposited contaminant and the natural soil
303
particles with little real data to interpret the effect
of particle size or the effect of depth in the soil
profile on the rate of resuspension. In addition,
calculations indicate that dust in the atmosphere
may well have originated a considerable distance
upwind and could have been resuspended under
completely different meteorological conditions.
One set of data collected by Hilst15 at the
meteorological facility at Hanford has been exam-
ined. Hero the number of dust particles per cubic
foot were measured in five size ranges by use of
cascade impactors. In one experiment, measure-
ments were made at five heights ranging from
1. 25 feet to 400 feet while in the others, the mea-
surements were made at three intervals from 0. 9
feet to 41. 3 feet. These observations show that,
in general, the dust concentrations, expressed as
mass.per unit volume, decreased rapidly with
height. However, the mass median diameter of
the particles also decreased so that the change in
concentration of the smaller particles with height
was much less pronounced and, in several cases
was not detectable.
The fractional rate of pickup from the ground
cannot be determined from these data because of
the lack of information on the source material.
However, the source term, itself, can be deter-
mined and compared to the wind speed. These
data are given in Table A-VII. Again, the ratio of
the rate of pickup, as determined from these data
assuming unstable conditions and a source upwind
approaching infinity, to the square of the wind
speed appears to be relatively constant.
E. An Example of Application
As a part of the effort of the Nevada Applied
Ecology Group to define potential problems with
plutonium contamination on the Nevada Test Site,
an extensive effort is being made to measure con-
tamination patterns, resuspension and redistribu-
tion, and the ecological behavior of the plutonium.
We have chosen the GMX area for analysis because
45
-------
TABLE A -VII
DUST CONCENTRATIONS AND ESTIMATED PICKUP RATES
0.9 - 5pm 5 - 20|_im 20 - 60 pm
Date
8/11
p. m.
5/4
a. m.
5/4
p. m.
-5/27
a. m.
5/27
p. m.
10/5
p. m.
Height
Ft
1.25
50.
100.
200.
400.
0.9
14.7
41. 3
0.9
14.7
41.3
0.9
14.7
41. 3
0,9
14. 7
41. 3
0.9
14.7
41. 3
u X
m/S #/m3
6.3 2. 3xl05
11 1.8xlOE
12 1.2xl05
12 1.4xl05
14 8.0x10*
1. 3 7.8x10*
1. 8 5. 33T10*
1,8 5.6x10*
1. 3 7. 8x 10*
1.8 6.4x 10*
2. 2 5. 6x 10*
2.1 3. 1x10*
3.6 2.0x10*
4.5 2.5x10*
2.2 5.6x10*
3. 1 4. 9x 104
3.6 4.2x10*
2.7 i.SxlO5
5.8 !.2xl05
8, 0 1, 8x 105
VD/u
Kn
Sec-1m-2
37, 000
30,000
20,000
22, 000"
13,000
2, 700
1, 900 .
2,000
2,700
2,200
2,000
2, 200
1,400
1, 800
3,600
3, 100
2,700
12, 000
8,700
12,000
= 0.013
Kn/u2
Sec-1™-3
950
770
500-
570
340 ^';
1500
1000
1100
1500
1200
1100
300
200
250
620
540
470
1700
1200
1700
X
#/m3 i
91, 000
55, 000
40, 000
41, 000
29, 000
12, 000
6,700
6,400
21, 000
6,400
6,400
5, 300
3,900
3,900
24, 000
11, 000
9, 500
26, 000
8, 600
8, 100
VD/u
Kn
15, 000
9,000
6, 600
6, 700
4,800
440
240
220
740
220
220
370 .
270
270
1,500
' 700
600
1, 900
600
570
= 0. 013
Kn/u2
Sec^nf3
380
230
170
~170
120
240
130
130
400
130
130
... ;: 50
40
40
260
120
110
260 .
80
80
VD = 0. 2m/sec
X
26, 000
9,700
6, 500
5, 200
3, 100
1, 300
210
280
2, 000
-280
320
670
320
460
2, 700
850
460
2, 90.0
1,200
1, 100
Kn
Secern2
6600
2400
1600
1300
780
260
40
60
400
60
60
140
70
90
550
170
90
600
250
220
Kn/u2
Securer3
T: no
62
42
33
-;20
150
20
30
220
30
40
20
9
13
96
30
16
80
40
30
X
2500
320
110
35
70
70
10
30
50
10
20
35
35
35
70
70
35
280
70
70
CO
0
'UN
60 - 240 |jm
Vp = 1 m/sec
Kn
Secern2
2500
320
110
35
70
70
10
'30
50
11
21
35
35
35
70
-v 70
35
280
70
70
Kn'/u2
Sec^nf 3
64
8
3
0.9
2
40
6
20'
28
6
10
5
5
5
10
10
6
40
10
10
^Ground surface damp.
-------
305
— Measured (Fidler)
Calculated
90
500
<—180°
Fig. A-5. GMXArea.
initial resuspension measurements have been
planned there and some preliminary data on ground
deposition are available. The pattern of deposition
has been measured by FIDLER surveys using the
60kev photons from the s*1Am associated with the
plutonium in June 1971.ls This pattern is given by
the solid isopleths in Fig. A75. If we assume that
the pattern is Gaussian in the cross-pattern direc-
tion with the standard deviation increasing exponen-
tially with distance from ground zero (GZ) and the
centerline deposition as given in Fig. A»-6, the iso-
pleths shown by the dotted lines in Fig. A-5 are ob-
tained. These isopleths are considered to be suf-
ficiently representative of the pattern to be usable
in the calculation of expected air concentrations or
the derivation of resuspension rates from measured
air concentrations. Although it would be desirable
to have an analytical relationship between the
position on the pattern and the peak deposition
at the centerline, none was found and the relation
in Fig. A-6 was used. For the change in standard
deviation of pattern width with distance from GZ,
the following relation was used:
a = 37. 3 exp(0.00335a)
y
(A-12)
where « is the standard deviation in meters at a
distance of a.meter from GZ.
Calculations were performed for locations on
the centerline of the pattern to take advantage of •
the symmetry so produced. The basic approach
was to calculate the expected concentration from
Gaussian line sources at various distances from
the station with the standard deviation of the pat-
tern at that distance according to Eq. (A-12). Wind
47
-------
306
directions were varied at 22. 5 deg intervals from
0 deg (wind directly up-pattern) to 180 deg (wind di-
rectly down-pattern). These directions are indi-
cated on Fig. A-5. The total concentration was then
obtained from these values by weighting according
to the centerline concentration from Fig. A-6 and
multiplying by the interval represented between the
successive line sources. Since the calculations
were performed on a Wang 600 programmable cal-
culator it was necessary to limit the number of up-
wind line sources considered to a total of 50 per
calculation. The concentration resulting from a
I*'*'
Gaussian line source wi'th a standard deviation of
A meters, a centerline deposition of Q Ci/ms and a
wind direction of 6 to the pattern centerline can be
obtainfed from:
Since the deposition pattern was measured
with the FIDLER, a relation between this mea-
surement and the quantity of plutonium in the soils
in a position to be picked up by the winds is needed.
Eberhardt and Gilbert1" have provided a statistical
summary of the data on soil analyses in this area
V-
including some preliminary correlations between
the FIDLER readings and the soil analyses. In this
study, FIDLER readings were made at given loca-
tions followed by sampling in three 5-in. circles to
a depth of three centimeters. The number of sam-
ples taken was limited and no correlation was found
for those measurements in the lower two isopleths.
However, in the >5000 c/m isopleth, six samples
showed an apparent correlation with the FIDLER
reading. These data indicated about 0. 3dis/min
of plutonium per gram of soil for each count per
minute on the FIDLER. While this correlation is
y=AA
xu (2-f) y"1 A
t— * ' i-r
K£p nCyCz y=_4A (a cosB + y sin9)
2(2-f)Vd , " y2 )
•'• (a cosO + y cosS)' + — — — >
vV Cznu , 2A2 )
1 exp
(A
{1 , /(a sinO
(a cos6 + y sin6)2"n \ C
- y cos6)2
2
y
-13)
rough and the authors warn against
the lower contamination levels, in
itx
cJ
applying it to
this preliminary
In Eq. (A-13), the angle 0 is measured between the
perpendicular to the line source and the wind direc-
tion. In practice, calculations were made sepa-
rately for the up-pattern wind direction (0-90°)and
the down-pattern (90-180°) switching the sign of
the coordinate system so that a was always 'posi-
tive.
Values of the pickup and dispersion param-
eter were calculated for stations located 150m up-
pattern from GZ; at GZ; and at 75m, 200 in, and
400m down-pattern from GZ. The values were then
normalized to a value of 1 Ci/m at the peak depo-
sition point, 6400 c/m on the FIDLER. These re-
sults are given in Figs. A-7 and A-8.
study we will accept it with the reservation that as
more data become available the correlation (as
well as the shape of the pattern) should be revised.
There is, however, no information on the
change in plutonium concentration with depth in the
soil profile or on the rnicrodistribution of pluto-
nium in the area measured by the FIDLER. Some
rough calculations indicate that the FIDLER sensi-
l
tivity for 4 1 Am decreases to about 50% of the sur-
face value for a plane source buried 8mm and to
about 10% for a plane source at a depth of 2. 5 cm.
The soil sampling procedure averages the total
quantity of plutonium over the sampling depth of
3cm. Thus, while the correlation would indicate
that there would be about 7x 10""'" Ci/m3 (assuming
a soil density of 1. 6 g/cm3) per c/m on the FIDLER,
the actual fraction of this which is effective in
48
-------
307
700C
6000
cr
_
Q
U-
500°
o 4000
0
c.
Q
3000
2000
o
1000
JL
-I001
100 200 .'300 400
Distance From GZ ( m)
500
600
700
Fig. A-6. Centerline Deposition Pattern
Area.
producing air concentrations is not known. For
these preliminary calculations, w!e will use the
above value but remember the reservations quoted.
Several air samples have been obtained in
this area during tests of the Lawrence Livermore's
high volume air sampler. l7 The sampler was lo-
cated about 250 feet (76m) north of GZ. Five sam-
ples were taken in April of 1972: two for periods of
17-19 hours and three for periods of 4-5 hours.
The resuspension rates for the three shorter sam-
ples were estimated from Fig. A-7 assuming the
peak deposition on the pattern to be 6400 c/m on the
FIDLER or 4. lx 10~s Ci/m3 . These data are given
in Table A-VIII.
For these calculations, it was assumed that
unstable atmospheric conditions existed. This
seems appropriate for the middle of the day at
this time of year. For the longer samples, which
were taken overnight, there was considerable vari-
ation in both wind direction and wind speeds with
low wind speeds occurring during the middle of the
night. In addition some ,of the data on wind speeds
are missing. An attempt to approximate the value
of K/u3 was made by using the hourly recorded
values of wind speed and direction. These results,
while very crude indicated values on the order of
10"13 to 10"14 with the lower value increasing to
about 10"13 if it were assumed that pickup occurred
only during the unstable periods with higher wind
speeds.
These resuspension rates have considerable
uncertainty, particularly with respect to the defi-
nition of the surface deposit. If, for example, it
is considered that the top millimeter of the soil is
49
-------
308
100 c
Neutral
Stable
30 60 90 120
Wind Direction From Pattern
Fig'. A-7. Concentration Integrals for Different Wind
Directions with Respect to Pattern Genterline.
150
180
50
-------
100
309
Neutral
—rt— Stable
0
30 60 90 120 150
Wind Direction From Pattern t (deg)
180
Fig. A-8. Concentration Integrals for Different Directions
with Respect to Pattern Centerline.
51
-------
310
TABLE A-VIII
ESTIMATED RESUSPENSION RATES FOR THE GMX AREA
Time of
Sample
4/19/72
1200-1600
4/27/72
1100-1600
4/20/72
0930-1400
Measured
Concentration
(Ci/m3)
3.5xlO-ls
1.4xlO~l*
1.5xlO-lD
Wind
True
350
218
220
Direction
-'Pattern
(deg)
155
18
20
Wind yu
Speed Knp K
(m/s)
3 15 .IxlO-13
4 14 IxlO-10
5 14 , IxlO-11
K/us
2x 10~13
5xlO-12
5x 10- l3
*Pattern centerline is 20 deg east of true north. Value given here is for application to the
directions used in the calculation.
the layer of importance,' and the plutonium is dis-
i
tributed uniformly through the three centimeter
sampling thickness, then the effective surface de-
posit is only l/30th of that used above and the re-
suspension rates will be increased by a factor of
30. In addition, the sampling period is relatively
long in comparison to that believed appropriate to
the dispersion coefficients used in the integrations
and these may underestimate the actual cloud
spread, again resulting in some increase in the re-
suspension rates. Even considering these factors,
however, the value of K/ua appears to be consider-
ably lower than the results quoted,earlier for fresh
deposits. Additional studies in the area will be
needed to fully explain the results afijd the relatively
large variation in K/ua from these few samples,
but it can be postulated that at least a part of the
reason for the lower values may be due to aging of
the deposit and redistribution by''particle size.
Data are not available on the influence of
mechanical disturbance in this area on the resus-
pension rate. It is noted, however, that the cal-
culation of the average concentration from the full
area involves the derivation of values for a line
source at various distances upwind with the wind
in different directions. Studies of the influence of
mechanical disturbance by people or animals walk-
ing across the a'rea or a vehicle driving across
could be made by sampling during such periods of
disturbance. Such results would be extremely
valuable in assessing the relative importance of
wind pickup and such mechanical disturbance.
Similarly no attempt has been made, as yet, to
evaluate the long term average concentration tak-
< ing into account the shifts in wind direction, speed
and atmospheric stability. It is believed, however,.
that the above method, in conjunction with the ap-
propriate meteorological measurements would re-
sult in a'.reasonable estimate.
The above example emphasizes the need for
adequate meteorological support in providing the
dispersion and deposition parameters to be applied
during experiments to assess the pickup rate.
Ideally, such measurements should be adequate to
permit a more accurate estimate of the dispersion
coefficients than has been used here and the actual
equations used should be modified to apply the most
accurate estimate of the dispersion.
REFERENCES
1. W. H. Langham, "Biological Considerations
of Nonnuclear Incidents Involving Nuclear
Warheads," USAEC Document UCRL 50639
(Lawrence Radiation Laboratory) April 196'9.
2. R. L. Kathren, "Towards Interim Acceptable
Surface Contamination Levels for Environ-
mental PuO3, " ISAEC Report BNWL-SA-
1510 (Pacific Northwest Laboratory) April
1968.
3. ... J. W. Healy, "A Preliminary Estimate of
' Wind Pickup and Impaction of Particles, "
ISAEC Document HW-35542 (HanfordAtomic
Products Operation) March 1, 1955.
52
-------
4. J. W. Healy and J. J. Fuquay, "Wind Pickup
of Radioactive Particles from the Ground, "
Znd UN Geneva Conference P/391 USA
Pergamon Press, London.
5. D. H. Slade, Ed. , "Meteorology and Atomic
Energy," 1968. TID-24190, U.S. Atomic
Energy Commission, Division of Technical
Information, July 1968.
6. A. C. Chamberlain, "Aspects of Travel and
Deposition of Aerosol and Vapor Clouds, "
Document AERE-HP/R 1361 (Harwell) 1953.
7. O. G. Sutton, "Micrometeorology, " McGraw-
Hill (1953).
8. J. J. Fuquay, Private Communication, 1957.
9. R. A. Bagnc4c|, "The Physics of BlownSands
and Desert Dunes, " Metnuen and Co. , Ltd.,
London, 1954.
10. a. W. D. Chepil, "Dynamics of Wind Ero-
) sion: I. Nature of Movement of Soil by Wind,"
Soil Science 6£ (1945), pp. 305-320. »
b.
sion: II.
Science 60 (1945),
, "Dynamics of Wind Ero-
Initiation of Soil Movement, " Soil
pp. 397-411.
"Dynamics of Wind Ero-
sion: III. The Transport Capacity of the Wind,'
SoiL Science 6£ (1945), pp. 475-480.
d.
'Conversion of Relative
Field Erodibility to Annual Soil Loss by
Wind, " Soil Science Society of America Pro-
ceedings 24^ (I960), pp. 143-145.
11, R. H. Wilson, R. G. Thomas, and J. N.
Stannard, "Biomedical and Aerosol Studies
Associated with a Field Release of Pluto-
nium, " USAEC Document WT-1511 (Univer-
sity of Rochester Atomic Energy Project)
November I960.
12. H. M. Mork, "Redistribution of Plutonium
in the Environs of the Nevada Test Site, "
USAEC Document UCLA-12-590 (UCLA
Laboratory of Nuclear Medicine and Radia- ,
tion Biology) August 1970.
13. G. A. Sehmel, "Particle Resuspension from
an Asphalt Road Caused by Car and Truck
Traffic, " Atmospheric Environment ]_, 3,
291-309, March "1973.
14. J. H. Olafson and K. R. Larson, "Pluto-
nium, Its Biology and Environmental Per-
sistence, " USAEC Document UCLA 501
(UCLA Laboratory of Nuclear Medicine and
Radiation Biology) December 1961.
15. G. R. Hilst, "Some Observations of Particle
Distribution with Height in the Lower Atmos-
phere, " Unpublished document.
16. L. L. Eberhardt and R. O. Gilbert, "Sta-
tistical Analysis of Soil Plutonium Studies,
•'_Nevada Test Site, " Pacific Northwest Lab-
.oratories Report BNWL-B-217, September
1972.
17. P. L. Phelps, Private Communication.
53
-------
312
APPENDIX B
THE VELOCITY OF DEPOSITION
The concentration downwind from a source of
airborne material depends upon the amount of ma-
terial removed from the atmosphere by natural
suspended for considerable periods of time and for
gases or vapors; and (3) retention of the receiving
surface once the material is brought into contact.
processes in the region between the source and the Thus, both the fine ^articles and the iodine vapor
receptor as well as upon the source strength and
the atmospheric mixing processes. The removal
rate varies with the physical nature of the air-
borne material, the state of the atmosphere and
the nature of the terrain involved. Two basic re-
moval mechanisms are washout or rainout, during
periods of precipitation, and dry deposition at
other times. In this treatment we will be concerned
with the dry deposition phenomena since the pur-
pose'of the study is to estimate the amount remain-
ing airborne rather than the amount deposited. In-
formation on the washout processes1'2 can be
adapted to estimate the effects of these processes
on the air concentrations during periods of preci-
pitation.
Early experience with the effluents from a
radiochemical separations plant at Hanford, as
well as experiments by Chamberlain indicated that
1311 in vapor form deposits strongly from the at-
mosphere onto surfaces.3'4 Later experiments
by Megaw and Chadwick 5 using solid fission pro-
should be brought to the ground at about the same
rate by the turbulence of the atmosphere, but the
iodine, being in a chemically reactive form is ap-
parently retained at the ground surface better than
the small particles. Such considerations permit
separation of the problem into several parts de-
pending upon the physical nature of the atmospheric
contaminant.
It has been customary to express the rate of
removal of a given material by the ratio of the rate
at which it deposits to the concentration in the at-
mosphere at the point of concern. Thus:
curies per m per sec
curies per m3
= m/sec . (B-l)
This ratio, which can be measured directly,
is referred to as the velocity of deposition since it
has the units of velocity. It is the purpose of this
appendix to explore the various factors which can
influence the velocity of deposition for particles and
ducts generated by arcing an irradiated wire showed to derive a simplified model incorporating the im-
that the deposition rate of these fine particles was
considerably lower than that for iodine vapor. The
close-in fallout from nuclear detonations consists
of large particles which have a terminal velocity
sufficiently great that they will not remain sus-
pended for any length of time but will settle from
whatever height they reach in the initial cloud
meanwhile being carried by the winds.
, This information indicates that there must be
at least three separate considerations in the dry
deposition of such material from the air: (1) grav-
ity settling for large particles; (2) transfer from
the air to the ground by the turbulent eddies in the
atmosphere for small particles which remain
portant variables so that some indication of the
variation expected with these parameters can be
derived. The model is not exhaustive in its treat-
ment of the various theories and information avail-
able since the intent is to provide an overall picture
which is commensurate with our knowledge of the
applications, particularly in regard to the influence
of this variable on the air concentrations resulting
from resuspension of particles from the ground.
I. GRAVITATIONAL SETTLING
The settling of larger particles under the in-
fluence of gravity has been studied for many years.
This rate of settling is characterized by a terminal
54
-------
313
velocity in which the force exerted by gravity is ex-
actly balanced by the aerodynamic drag from the
passage through the air. As the particle size de-
creases, the terminal velocity decreases to a point
where the turbulent eddies in the atmosphere exert
sufficient force to overcome the gravitational forces
and the particle remains suspended. For our pur-
poses a large particle can be defined as one in which
the terminal velocity predominates over the atmos-
pheric turbulence and the deposition velocity is es-
sentially equal,to the terminal velocity. Note that
this is not a definition of a particular particle size
since the eddy for
-------
314
This may be defined as the diameter of a particle of
unit density which has the same terminal velocity
as the particle of interest. This diameter will be
used throughout this paper unless a correction for
density is specifically indicated. Such an aerody-
namic diameter essentially defines the inertial be-
havior of the particle wliich is of importance in many
problems, such as sampling by particle size where
the separation is done by inertial means, consider-
ation of impaction on a surface, or even deposition
of the material in the respiratory tract. Roughcon-
V
version factors between spherical particles andpar-
f^
tides of known and definable shapes can be found in
the literature but are not considered here because
of the preliminary nature of many of the data dis-
cussfed herein and the resulting \mcertainties from
these causes.
II. TURBULENT TRANSFER
For the turbulent transfer to the ground, theo-
retical treatments have been published by Stewart,8
Owen,9 and Chamberlain.10 Fuquay in unpublished
work11 has considered the transfer of mass across
the boundary layer of the atmosphere to be equal to
the transfer of momentum and ha's evaluated the
transfer coefficient or velocity to be:
n'
(B-3)
Here, the transfer velocity is designated as V to
indicate that it is the component due to the turbu-
lent transfer, u* is the friction velocity and u^ is
the wind velocity at a reference height z. The fric-
tion velocity is the ratio of the shearing stress in
the lower layers of the atmosphere to the density,
with the shearing stress considered to be constant
with height in the surface layers of concern.
Chamberlain's expression for the resistance to
transfer in the boundary layer10 is the reciprocal
of Eq. (B-3) and he has evaluated the velocity of
deposition for submicron particles from a theoret-
ical treatment by Owen to be 0. 004u*. Markee12
indicates that the deposition velocities for iodine
with a one-meter reference height at the National
Reactor Testing Station have shown an approximate
linear relation with u* where V, = 0. OlZlu*. Since,
d
as will be seen, the friction velocity for a given at-
mospheric condition and surface is proportional to
the wind velocity at a reference height, Eq. (B-3)
reduces to the same form as these observations.
The value of u* can be evaluated from the wind
profile (change in wind velocity with height) and a
parameter representing,the nature of the surface.
For a surface in which the irregularities are large
enough so that a laminar layer submerging the ir-
regularities cannot form the flow will be turbulent
down to the surface.13 Such a condition is called
fully-rough flow and occurs for nearly all natural
surfaces at moderate or high wind speeds. Sutton, 3
for example, indicates that for a wind speed of
5m/sec at a height of two meters, only a surface
such as smooth mud flats or a large sheet of ice
would Be aerodynamically smooth. A closely cut
and well rolled lawn would be smooth for winds be-
low 1m/sec measured at two meters height but
would be rough at higher wind speeds. Note that
the wind must flow over a surface for some dis-
tance before the surface layer takes on the turbu-
lence characteristics of that surface. This means
that significant changes in the character of the tur-
bulent layer occur with changes in terrain, with
possible significant changes in the turbulence trans-
fer velocity. Where artifical surfaces, such as
paper of limited area, are used to sample deposi-
tion, it is probable that the transfer velocity is
characteristic of the terrain immediately surround-
ing the sampler with the retention characteristics
those of the sampling medium so that results from
differing terrains or samplers may not compare.
The wind profile in a neutral atmosphere and
its relation to the friction velocity has been studied
more extensively and is better characterized than
for'stable or unstable atmospheres. For a neutral
atmosphere, the wind profile is logarithmic and in
56
-------
fully rough flow can be described14 as:
u
z
u*
In*
(B-4)
In Eq. (B-4), k is the Van Karmen constant
with a value of about 0. 4, u is the wind speed at a
height z and z is a constant characteristic of the
surface. This constant arises as a constant of in-
tegration in the derivation of Eq. (B-4) and repre-
sents the height at which the flow can be extrapo-
lated to zero. It can be measured for a given sur-
face from the wina profile in a neutral atmosphere
and is reasonably independent of wind speed, al-
though in situations where the surface changes with
wi^pd speed, as in the development of waves on a
body of water or the bending of tall grasses in the
•wind, the value of z can either increase or de-
o
crease with wind speed. Deacon15 has given typ-
ical values for various surfaces along with an esti-
mate of the wind speeds above which fully rough
flow can be expected so that the treatment of Eq.
(B-4) is applicable. His plot is reproduced in Fig.
1. It may be noted that this treatment is not strict-
ly applicable to surfaces with higher roughness
features such as a forest.
With stable or unstable conditions, the loga-
rithmic wind profile no longer holds. For these
conditions. Deacon15 indicates that the change in
wind velocity with height (du/dz) provides a reason-
able fit to a power function. From this, he derives
1
u* k (1 -p)
[ft)"
-1
(B-5)
The symbols in Eq. (B-5) are the same as
those in Eq. (B-4) with the addition of p which is
the exponent in the derivative of the wind profile.
Beta is greater than one for an unstable atmos-
phere, less than one for a stable atmosphere and
one for a neutral atmosphere. It is assumed that
Neutral V =
Other V = '
k
/ z \ 1
315
z is characteristic of the terrain and is the same
o
in all stabilities so that a measure of this constant
under neutral conditions will permit application to
Eq. (B-5). The validity of this assumption has not
been definitely shown and, particularly in very
stable atmospheres, the criterion for fully rough
;/
flow may not be met and the profile may differ from
the power function.
By combining Eq. (B-3) with either Eq. (B-4)
or Eq. (B-5) we can derive a functional relationship
between V and these parameters.
(B-6)
(B-7)
The above derivation is not intended to be com-
plete for all surfaces and some corrections have
been.'omitted in the interest of simplicity. It is in-
tended to indicate the functional form of this trans-
fer with the meteorological variables under most
conditions of interest in the field. If we accept the
assumption that the transfer of mass is equal to the
transfer of momentum in this situation then the
transfer velocity will be directly proportional to the
wind speed and should vary with the stability of the
atmosphere, being greater for the unstable condi-
tion and smaller for the'Stable condition. This con-
clusion is of some importance since it indicates
that the amount of material deposited from the at-
mosphere is independent of the wind speed for a
given stability. This is because the concentration
from a point source decreases inversely with the
wind speed while the deposition increases directly
as the wind speed so that the two terms cancel.
It is also of interest that the ratio of the turbulent
transfer velocity to the wind speed is equal to the
"drag coefficient" as given by Priestley14 or one
half of the drag coefficient as given by Deacon. ls
57
-------
316
(cm)
Long gross r — ^z-—
60-70 cm Sfronfl
summer-
Downlond -•
winter-
Mown grass •
( 5cm)
Mown grass (1.5cm)*
Natural snow •
surface
Sunbaked .
sandy alluvium
Smooth snow on
prepared short -
grass area
Smooth mud flats
1
0,!
Q,Q|
.001
,1
J~
*T_
*T_
Turnip field
Wheat field
Long grass land
*~ Fallow land
^Airfield
Close cropped grass
Snow
Snow
— Cricket field
Sand
Fig. B-l. The Roughness Parameter of Various
Surfaces (After Deacon.)15
58
-------
317
1.3
We can obtain an estimate of the magnitude of
the turbulent transfer velocity for various surfaces
and the change with stability of the atmosphere by
using values of z and (3 as given in the literature.
The values of z chosen were those given bySutton
as representative but to be used as general guides
only. They may be compared with those of Deacon
as given in Fig. B-l. Deacon15 has plotted values
of p as a function of stability (expressed as the
Richardson's number) from measurements made
over a short grass surface (z = 0. 27cm) and from
observations over snow (z = 0. 2,5 cm). We will
assume, for purpo^^s of illustration, that the value
i;
of p is independent of z and use these data to esti-
mate the ratio of V to u as measured at a height of
two meters (u2). (This is equivalent to calculating
the transfer velocity for a wind speed of one meter \
per second at the reference height. ) These values,
along with the values of z are given in Table B-II. .
It may be noted that the nature of the surface
is more important in determining this transfer in
the stable case than in the unstable. Thus, for high
values of z , both the stable and unstable case are
o
within a factor of two of the neutral case while for
the low values of z the stable case transfer is
o r
lower by about a factor of twenty with the unstable
case transfer higher by only a factor of six.
The variation in the turbulent transfer velocity
is shown as a function of the stability expressed as
TABLE B-II,
CALCULATED VALUES OF V /ua
Stable Neutral , Unstable
R. = 0 08 R. =0 R. = -0. 2
Surface
P =0. 18
Very smooth 0.001 0.000049 0.0011 0.0066
Grass 0.1 0.00046 0.0028 0.0093
up to 1 cm
Thin grass 0. 7
up to 10 cm
Thick grass 2. 3
up to 10 cm
Thin grass ' 5
up to 50 cm
Thick grass 9
up to 50 cm
0.
0.
0.
0.
0014
0029
0052
0084
0.
0.
0.
0.
0050
0080
012
017
0.
0.
0.
0.
013
017
022
028
the Richardson's number in Fig. B-2 for several of
the values of z from Table B-II. The values of p
o
for this plot were again taken from Deacon's plot
and the Richardson's number is that for the layer
of air between 0. 5 and 4 meters.
III. EXPERIMENTAL DATA
Data taken on an adequately controlled basis
to permit checking of these concepts are scarce.
In many cases'the particle size or physical nature
of the contaminant is not known while in others the
wind speed or other meteorological variables are
not given. Perhaps, the most common is the use
of an isolated small area of a collection material
either at ground level or at some arbitrary distance
above the ground. The meaning of these results in
terms of the local deposition is not known since the •
area is usually not large enough to establish the full
turbulent layer over the test surface. For such sur-
faces on the ground, the final result is probably a
mixture of the characteristic ground surface in the
area and the retention characteristics of the test
specimen.
A compilation of some of the data available on
deposition are given in Table B-III separated accord-
ing to stability. A brief discussion of the data iden-
tified by the letter in the source column of the table
is given below.
A. These results come from experiments by
Chamberlain and Chadwick and Megaw and ChadwickJ0
Elemental iodine was dissolved in CC14 and sprayed
into the air. Measurements of the air concentration
at several heights and of the deposited material were
made across arcs at several distances dowriwind.
The reference wind speed given in the table is at a
height of two meters. It was assumed for the pur-
poses of the tabulation that the measurements on a
sunny day were in unstable conditions while those
on a cloudy day or at dusk were in neutral conditions.
Data are also given for the friction velocity. From
this, the estimated turbulence transfer was calcu-
lated for a wind speed at the reference height of two
59
-------
318
10
-0.4 -0.3 -0.2 -O.I 0
Richardson's Number - 0.5 to 4m
0.2
Fig. B-2. Change in Turbulent Transfer with Stability.
60
-------
Material
TABLE B-III
MEASUREMENTS OF DEPOSITION
Source Surface
319
VELOCITY
( Vd/u) x 102
Stable Atmosphere
ZnS tracer
~1 jjm MMl)
ZnS tracer
Fission Products from
Melted Fuel Element
l37Cs
lo3Ru
Zr-Nb
Ce
137 Cs
103Ru
Te
Unstable Atmosphere
1311 vapor
ZnS tracer
~I |jm MMD
Fission Products
Arc
Neutral Atmosphere
1311 vapor
1311 - melted
fuel element
C
B
E
F
Desert
Desert
0.077, 0.88
0. 85,;<0. 55, 0. 78
Sticky paper -
Water
Sand
Sticky paper -
Sticky paper -
Water
Sand
Sticky paper -
Water
Sand
Sticky paper -
Sticky paper -
Sticky paper -
Rye grass
Soil
Sticky paper -
Sticky paper -
Grass
Soil
1m
1m
1m
1m
1m
grd.
1m
^
V
grd.
1m
0. 38
0.'36
0. 12
0. 018, 0
0. 64
0. 86
0. 24
0. 44
0. 86
0. 98
0. 14
0. 054, 0
0. 14, 0.
0. 094, 0
0. 16, 0.
0.42, 0.
0. 0091
0.046, 0
0. 20, 0.
0. 11, 0.
0. 12, 0.
0. 029
.043, 0.029
. 10, 0.059
16, 0. P3, 0. 22
.052, 0. 17,
32
81
. 14, 0. 13,
078, 0.078
22, 0.02, 0. 15
31
Sticky paper - grd.
Grass
Dandelion leaf
Paper leaf
Paper - Petri dish
Desert
Grass & substrate
Filter paper
Grass
Dandelion leaf
Paper leaf
Paper - Petri dish
Sticky paper - 1m
Water
Sticky paper r> 1m
Sticky paper -'grd.
Rye grass
0. 15
0. 37, 0. 35, 0.91, 0.76
0. 25, 0. 30
0. 39, 0. 37 ,
0. 12, 0. 17, 0. 15
1. 33, 0. 94, 0. 87
1. 1, 1. 1
0.069, 0.049
0.024, 0. 018, 0. 012
0.60, 1. 03, 0. 28
0. 30, 0.078
0.61, 0. 16
0. 16, 0. 18
0. 16, 0. 12
0.26, 0.34
0. 13
0. 16
0. 81
61
-------
320
Material
Source
TABLE B-III (Continued)
Surface
(Vd/u)x 102
Rn daughters
ZnS tracer
*^1 um M^4D
Fission Products
Arc
D
C
B
Flat surface
Desert
Grass & substrate
Filter paper
0. 01 - 0. 02
0. 69, 0.47, 0. 62,
0.023
0 023-v 0. 042
0. 56
Fission Products from
Melted Fuel Element
137Cs
103Ru
Zr-Nb
I Ce
Te
Sticky paper -1m
Water
Sand
Sticky paper -1m
Water
Sand
Sticky paper -1m
Sticky paper - grd.
Sticky paper - grd.
0.009, 0.017, 0.027, 0.055
O.'Ol, 0.029
0. 012, 0. 009, 0. 055
0. 20
0. 25, 0. 30
0.055, 0.063
0. 12
0. 71
0.18
0. 22
0. 20
meters from Eq. (B-3). These values are com-
pared to the measured deposition below.
Calculated
Measured
V /u
t
0. 0085
0. 0065
0. 0087
0.0087
0. 0083
0.0076 .:
0. 0045
V,/u
d
0. 0037
0.0060
'. 0.0035
o. 0091
I'b. 0103
0.0074
0.0028
Run No.
1
2
3
4
5
6
7
B. Megaw and Chadwick5 produced a fume of fis-
sion products by an arc between an irradiated wire
and an electrode. Deposition was measured down-
wind along with the air concentration. Particles
were probably submicron in size. Chamberlain °
reports that cascade impactor samplers would in-
dicate a particle size of 0.2}jm or less if theden-
sijty of the particles was that of uranium oxide. It
was noted that the deposition velocity of strontium
from this experiment seemed to be less than that
of the other solid fission products.
C. Islitzer and Dumbauld, as reported in Ref. 16,
computed the deposition velocity for fluorescent
tracer particles of one (jm MMD from tracer ma-
terial balance measurement at the National Reactor
Test Station in Idaho over level terrain sparsely
covered with sagebrush. They noted, in particular,
a marked variation in the deposition velocity with
stability. Measurements of the deposition velocity
on flat, sand covered plates 0. 1m2 in area were
also made. In unstable conditions, these measure-
ments indicated deposition velocities over an order
of magnitude smaller than those found by the deple-
tion technique.
D. Chamberlain10 quotes Bullas as measuring
the deposition of radon decay products onto flat sur-
faces. It was estimated that over 95% of the decay
products would be attached to nuclei which Wilkening
found to be about 0. 02|jm median diameter. Bullas
found the deposition velocity to depend on the wind
velocity. For purposes of Table B-U it was assumed
that the deposition quoted with "fresh" winds oc-
curred in neutral atmospheres with wind speeds of
about 5 meters per second. It is noted that in
"calm" weather values of the deposition velocity
were as low as 0. 005 to 0. 01 cm/sec. Measure-
ments were also made by Bullas of the deposition
62
-------
321
of fission products in long range fallout with depo-
sition velocities ranging from 0,063 to 0. 16 cm/sec.
Similar observations by Stewart quoted in Ref. 10
gave a mean velocity of 0. 07 cm/sec for the fission
products. Booker is reported to have measured
the 95Zr component of long range fallout on filter
paper with an average deposition velocity of 0. 1
cm/sec. When he repeated the experiment indoors,
the deposition velocity was 0. 007 cm/sec although
the atmospheric concentration was 80% of that out-
doors. These values are not included in the table
since there is no indication of thefwind speed or
stability. I,' \
i
E. A field experiment at the National Reactor
Testing Station in Idaho was conducted for the Air-
craft Nuclear Propulsion program.17 Irradiated
uranium fuel elements were melted in a furnace at *
ground level and the resulting fission products were
measured downwind to a distance of about 3. 2km.
Andersen samplers indicated that the bulk of the
material penetrated to the backup filter. Particle
size estimates for zirconium-niobium were 1 to 5
pm and for cerium 50% from 1 to 5 (jm and 50% less
than one |jm. All others were estimated to be less
than one |am. The majority of the deposition mea-
surements were made on 13" x 13" sticky paper
mounted on a support an unspecified distance (pre-
sumably about 1 meter) above the ground. Water
trays with an area of 135 in.2 and sand trays with
an area of 161 in. a were placed at ground level and
around sagebrush. The deposition velocity at each
measurement arc was computed for the ration of the
areas under the deposition profile to the area under
the air concentration profile. This technique of fit-
ting a Gaussian curve by area strongly weights the
points in the middle of the profile and essentially
ignores the points at the tail of the curve. If there
i
were diffusion patterns leading to different deposi-
tion rates at the center and the tails of the curves,
this technique would provide an estimate primarily
of the centerline deposition. It may be noted that
the points quoted in this test for unstable conditions
are included in the neutral section of Table B-II.
This is because the wind profiles for these tests were
logarithmic and the Richardson's numbers estimated
from the data available in the report were close to
zero indicating a reasonably neutral atmosphere.
F. The second series of tests for the ANPproject
was made at the Dugway Proving Ground in Utah. l8
This is a very flat region with little vegetation or
surface roughness to induce turbulence. Techniques
were similar to the previous test except that the
sticky paper was primarily used on the ground and
patches of rye grass 8"x6" at ground level were
used for some of the tests. Most of the data were
taken for stable atmospheres although one test had
a small temperature differential between 4 and 16
m and was considered as neutral. It was concluded
that there was some indication of a change in depo-
sition, velocity with wind speed but no change with
stability. The data are variable, however, and the
range in stability was not great. This report also
indicated that the sticky paper used for the bulk of
the measurements changes retention efficiency with
the humidity of the atmosphere, thereby adding an-
other variable to the measurements.
G. Simpson19 has reported detailed measurements
of the plume depletion and horizontal and vertical
profiles of concentration following the gro,und level
release of a zinc sulfide tracer (MMD~2. 7pm) at
Hanford. The deposition velocities were calculated
from the estimated values of the exchange coeffi-
cient and the vertical concentration gradient. These
runs were made under very stable conditions with
Richardson's numbers at 1. 5 to 3m ranging from
0. 046 to 0. 223. He also reports values for'the fric-
tion velocity which lead to estimates of the ratio of
turbulent transfer velocity to wind velocity from
4.9 to 22 cm/sec per meter/sec.
The data from Tables B-II and B-III are com-
pared for the neutral atmosphere in Fig. B-3. The
terminal velocities for spherical particles with a
density of four are included for comparison. Note
that particles with a different shape or irregular
63
-------
322
10
1
0.1
0.0
n nn
'
Z = 9
O
Zo - 5.*X
_ Z =2.3
O
_ Z =0.7
O
— Z =0.1
o
I z = 0.001
i-131
V"
Vspor (Grsss)
F.P. (Rye Grass)
— Vapor (Grass)
— F.P. (Water)
— Vapor (Grass)
— F.P. (Water)
i- F.P. (Paper)
-J 1
ii
i
Particles •
1 ZnS (~1 /um)
| (Desert)
Ru
— (Paper)
Zr-Nb
', (Paper)
— ~
Fission Products
~~ (Grass)
Rn
Daughters
(-0.02 Mm)
Cs
~ (Paper)
Terminal
Velocity
(Vg)
Spheres
P = 4
12 Mm
— 6 Mm
— 3.7 Mm
— 1.2 fjm
0.3 Mm
Fig. B-3. Transfer Velocities - Neutral Atmosphere.
u - 1 rn/s
64
-------
rticles will have a lower terminal velocity.
pa
IV. RETENTION ON SURFACES
The turbulent transfer velocity places an upper
limit on the movement of the smaller particles
through the boundary layer. If the material passing
downward is retained on the surface with 100%
efficiency, then the overall velocity of deposition
must equal the turbulent transfer velocity. If, how-
ever, the particle rebounds from the surface or does
not contact it because of inertial effects, then the
retention can be less than 100% and the overall ve-
locity of deposition^'will be smaller than the turbu-
lent transfer velocity.
The iodine data over grass indicates that the
measured deposition velocity for the vapor is close
to that predicted by the turbulent transfer mecha- ,
nism. The iodine from the fission product release
may be somewhat low in its deposition on paper,
but the form of the iodine, the retention character-
istics of the sticky paper and( its elevated position
introduce uncertainties. The tracer material with
a median diameter of about one i_im similarly seems
to have a high efficiency of deposition. It is of in-
terest to note that the value of z , as obtained from
two of the logarithmic wind profiles in the first
series of release tests at NRTS, .was about 1 cm, a
value in close agreement with the deposition velo-
city measured for the same general area. Also,
the measured deposition velocity for this material
is much greater than the terminal velocity for grav-
itational settling indicating the importance of the
turbulent transfer. ,
On the other hand, the data for radon daugh-
ters and fission products produced by an electric
arc indicate deposition velocities much lower than
would be indicated by turbulent transfer but still
hi'gher than would be predicted for submicron par-
ticles in gravitational settling. A similar pattern
is shown for cesium in the ANP tests although the
ruthenium and, perhaps, the zirconium-niobium
velocities appear to be higher. These data lead to
323
the conclusion that the finer particles, while trans-
ferred according to the theory, do not remain on
the surface. Thus, the measured deposition velo-
city is lower than would be predicted. On the other
hand, materials such as iodine vapor and urn-sized
particles appear to be held with relatively high ef-
ficiency particularly on surfaces such as grass.
Possible mechanisms for retention on sur-
faces are varied and undoubtedly differ with the size
and nature of the particle. We can speculate that
absorption, adsorption, electrostatic effects, iner-
tial effects and others may all be of importance
under given conditions. In order to investigate the
possible effects of one of these mechanisms, the
inertial forces, a crude model was established and
impaction efficiency estimated under several con-
ditions. It is emphasized that these calculations
are intentionally naive and are not intended to rep-
resent reality, but simply tp illustrate one of the
possible mechanisms.
Studies of the efficiency of impaction of small
particles carried by an air stream have been made
on a theoretical basis by Langmuir 7 and on an ex-
perimental basis by several investigators. °'
Figure B-4 presents the efficiency of impaction on
a cylinder predicted by Langmuir with the results
of several experiments for comparison. This ef-
ficiency is defined as the ratio of the quantity of
material collected on the unit projected area of a
cylinder to the quantity passing through the unit
area normal to the direction of the flow. In Fig.
B-4 this efficiency is correlated to the dimension-
less parameter V u/gCwhere V is the terminal
6 o
velocity of the particle in free fall through the at-
mosphere, u is the velocity of the air stream, g is
the acceleration due to gravity and C is the diam-
eter of the cylinder upon which the particles are
impacting.
It is noted that the experimental data are in
reasonable agreement with the Langmuir prediction
except for those points below the cutoff value of the
parameter. The experimental values were obtained
65
-------
324
100
- 10
o
CL I
E •
Longmuir
O.I
• Experimental
O.OOi
0.01
O.I
10-
100
V u/gc
g
Fig. B-4. Efficiency of Impaction of Particles on Cylinders.
with aerosols of finite size distribution which means
that there were particles much larger than the
mean values used, and the measuij'^d collection at
these small sizes was undoubtedly due to the pres-
ence of the larger particles. For the further cal-
culations, the theoretical predictions of Langmuir
will be used so that the values 'bbtained will be char-
acteristic of a uniform sized aerosol.
For these calculations, particles of>density
four were chosen since this corresponds to the zinc
sulfide fluorescent tracer commonly used in meteo-
rological experimentation. Figure B-5 presents the
irripaction efficiency for various values of u/C and
particle sizes for spherical particles of density four.
From these curves the impaction efficiency for var-
ious airstream speeds of diameters of impaction
cylinders can be obtained. For example, for a one
millimeter diameter cylinder, the curve of u/C =
10* gives the efficiencies for a ten meter/second
airstream, while the curve of u/C = 103 gives the
efficiencies for a one meter/second airstream.
Conversely, for a ten meter/second airstream the
curve of u/C = 10* represents the efficiency of im-
paction on a one mm cylinder while the curve of
u/C = 103 represents the efficiency of impaction on
a ten mm cylinder.
In order to illustrate the effects of this aero-
dynamic behavior of particles, a simple calc'ula-
tional model was used in which the particles are
brought to the ground by atmospheric turbulence.
Upon reaching the ground, they are carried past
obstructions in the form of cylinders of several
diameters where they are impacted according to the
efficiencies given. Only the mechanism of impac-
tidii on cylinders was considered at this point so
that any additional mechanisms such as electrostatic
66
-------
100
325
O.I
I : 1.0
Particle Diameter (urn)
100
Fig. B-5. Impaction Efficiencies for Spheres of Density 4g/cm3
effects; impaction on surfaces other than cylinders; vary with the nature of the surface (short grass,
or, for the very small particles, diffusion to the
interceptor surface will change the picture given.
It should be noted that two wind speeds are of
importance in these calculations of the deposition
velocity. The first is the wind speed at the bound-
ary layer which determines the rate of mixing
through the boundary layer or the limiting value of
the deposition velocity. Thus, from the measure-
ments available, the mixing phenomena can account streamline intercepting the cylinder so that bnly
for a deposition velocity of about 2. 5 cm/iec in neu- those particles so exposed are represented. In
tral conditions with a wind speed of 5 meters/second. other words, no correction is made for the relative
At one meter/second the deposition velocity due to areas of the interceptor surfaces and the total flow
mixing should be about 0. 5 cm/second. The other area. Two situations are calculated. The firstuses
wind speed of importance is the speed of the air- the efficiencies directly from Fig. B-5. This assumes
stream past the impacting surfaces. This is un- that the intercepting cylinders are so placed that
doubtedly lower than the wind speed at the boundary eabjh particle is on a streamline headed toward an
layer due to surface friction effects and will probably interceptor once during the passage. The second
long grass, bushes, trees, etc. ). In the present
calculations, the speed of the airstream at the inter-
ceptor is taken to be the same as the wind speed
since detailed information to choose a better value
is not available.
The definition of the impaction efficiencies for
Fig. B-4 must be considered in the model since they
represent a fraction of the particles that are in the
67
-------
126
O.I
I 10
Particle Oiamcter(^m)
100
Fig. B-6. Calculated Deposition Velocity for
Spheres of Density 4 Impinging on
1mm Diameter Cylinders in a
Neutral Atmosphere.
assumes a passage through a number of intercep-
tors so that each particle is exposed to the chance
of capture ten times.
The values of the deposition velocity in this
idealized situation were computed from Eq. (B-8).
V , = V
(B-8)
Where V. is the velocity of deposition, V is
d e
the terminal settling velocity of the particle, f is
the efficiency of impaction, (Vt/u) is the limiting
velocity of deposition from mixing across the bound-
ary layer and u is the wind speed. Equation (B-8)
is based on a simple additive process between the
two mechanisms considered. It is doubtful that
this is valid at low particle sizes where the energy
which can be imparted to the particle by eddies in
the atmosphere is much greater than the energy
which can be dissipated in an equivalent time period
I 10
Porticle Diametor (;im)
100
Fig. B-7. Calculated Deposition Velocity for
' Spheres of Density 4 Impinging on
5mm Diameter Cylinders in a
Neutral Atmosphere.
by the simple settling of the particle.
In the case of the "multiple pass" over the
interceptors, f was evaluated by:
f = 1 - e
-f'n
(B-9)
Where f is the fraction remaining after n passes
each with an efficiency of f' in removing material.
Figure B-6 presents the velocity of deposition
calculated for both the "single-pass" and the "ten-
pass" cases for impaction on one millimeter cyl-
inders and wind speeds of 20m/sec, lOm/sec,
Bm/sec and 1m/sec. It was assumed that the at-
mosphere had neutral stability so that (Vt/u) was
BxlCT3.
Figure B-7'presents the same calculations
for.impaction on five mm diameter cylinders.
68
-------
V. DEPOSITION VELOCITY MODEL.
From these considerations we can obtain a
qualitative picture of the variation in deposition ve-
locity with particle size. With large particles, the
predominant mechanism will be gravitational set-
tling. As the particles become smaller, they will
become more likely to remain suspended by the tur-
bulent air motions and, at some size, the velocity
of settling becomes small in comparison to the tur-
bulent transfer across the boundary layer. This
transition size is a function of the stability of the
atmosphere in determining the turbulence, the wind
velocity, and the na^tore of the surface. From Fig.
B-3 the transition size for a spherical particle with
a density of 4 in a neutral atmosphere with a grass
surface and a wind speed of Im/sec, would be about
6 to 10urn. For shapes other than spherical, the t
transition size would be larger. Since the gravita-
tional settling is not affected by the wind speed while.
the turbulent transfer velocity changes proportion-
ately, the transition point occurs at larger particle
sizes at higher wind speeds. In the previous exam-
ple, but at a wind speed of lOm/sec, the transition
point would come at a particle size of 20 to 30 |jm.
Once the particles are brought to the ground, the
probability of retention on the surface is undoubt-
edly a function of the particle size.^nd the wind
speed, although definitive data are not available on
this. Variations in the retention with wind speed
could account for some of the variability in the
measured deposition velocity. 'One would expect
that the larger particles would have greater re-
tention by inertial impaction which would appear to
be the primary force responsible for these particles.
As is indicated by the data in Table B-III, the re-
tention of zinc sulfide particles of one or a few Mm
appears to be high. Thus, the possibility of a pla-
teau in the curve of measured deposition velocity
versus particle size at the value of the turbulent
transfer velocity seems probable. The length of
this plateau and the particle size at -which a signi-
ficant decrease in retention occurs will probably
.327
depend upon the stability and the wind speed, but
would seem to extend down to one micron or slightly
less. Below this value the retention will decrease,
although not as rapidly as the consideration of iner-
tial forces would indicate, since new mechanisms,
such as electrostatic attraction, will come into play
for the very small particles.
Selection of numbers for this qualitative pic-
ture is difficult and uncertain because of the lack of
detailed data. Using as a reference the turbulent
transfer velocity for z = 2.3 cm, one can calculate
the efficiency of retention for the measured deposi-
tion velocities in Table B-III. For the one (jmMMD
tracer particles at Idaho Falls, the efficiency of re-
tention is 73% for neutral conditions, 63% for unsta-
ble conditions, and 28% for stable conditions. For
the radon daughters on a flat plate the efficiency is
about 2%. For the fission products produced by the
arc and deposited on grass, the efficiency is about
3% in neutral conditions and 3. 5% in unstable con-
ditions-. The deposition of Cs on the paper, sand,
and water in the ANP tests varied from 2. 5 to 3. 4%
in neutral conditions and from 3 to 10% in stable
conditions. While the absolute magnitude of these
numbers can vary with the assumption of ZQ, the
values are consistent with a rapid decrease in re-
tention efficiency in the range of 0. 5 to 1 or 2 mi-
crons with a relatively constant retention efficiency
of about 1 to 5% at 0. 1 micron. The other values in
the ANP tests were not used here because of the in-
dications of large particle size or the possible chem-
ical reactivity of the ruthenium.
The information available obviously does not
permit a detailed functional relationship between the
particle size and efficiency of retention particularly
when differences due to changes in stability, wind
speed, and nature of the surface are included. For
purposes of estimation, we will assume that the fis-
sion products produced by the electric arc in the ex-
periments of Megaw and Chadwick11 are about 0. 1
Ijm'Vith a retention of about 3% and the one |am
tracer particles of Islitzer*3 have a retention of
69
-------
328
about 70% with a linear relation between. Below
0. 1 pm the efficiency is assumed to remain about 3%
as based on the radon daughter deposition on the
flat plate. The linear relationship was chosen as
the simplest to represent the meager data, although
it is probable that the actual relation is sigrhoidwith
the steepest drop in retention somewhere between
0. 1 and 1pm. The linear relation can be approxi-
mately represented by f = 0. 74d - 0. 04 where f is
the fractional retention and d is the particle size in
pm. Extrapolation to 100% retention would indicate
this to occur with particle sizes of about 1. 4 pm,
which is not in disagreement with the high retention
implied by Simpson's data with 2 to 3 pm particles
in stable atmospheres. At the upper end of the spec-
trum of particle sizes, it is assumed that the de-
position velocity remains constant at the value for '
the turbulent transfer until (V /u) u = V .
t g
The particle density has not been included in
the above considerations, again because of the lack
of data on its influence on retention. Most of the
experiments in Table B-III were run with particles
of density ranging from about 3 to, perhaps, 10g/cm3
so that the retentions chosen may represent reason-
ably realistic particles of concern.
From this crude model of retention and the
turbulent transfer velocities of T^le B-II, it is
possible to approximate the .deposition velocities
for various particle sizes and limited types of ter-
rain. Some of these approximations are given in
Table B-IV.
It is again emphasized that the fractional re-
tention values are particularly uncertain so that
these deposition velocities must have wide limits
of uncertainty until appropriate experimental data
and study permit better estimates.
TABLE B-IV
APPROXIMATIONS OF THE RATIO OF
DEPOSITION VELOCITY TO WIND
SPEED AT ONE METER HEIGHT
Thick Grass
Particle
Size
f
ShortGrass 10cm 50cm
zo =;>: °- * cm zo = 2. 3 cm zo = 9 cm
Neutral,
>1.
~1
M).
<0.
5pm
pm
5 pm
, 1 pm
1.
0.
0.
0.
0
7
3
03
0.
0.
. 0.
0.
0028
0020
00074
00007
Unstable-,
>1.
~1
"•0.
<0.
5pm
pm
5 pm
1 pm
1.
0.
0.
0.
0
7
3
03
0.
0.
0.
0.
0093
0065
0028
0003
Stable,
>1.
-v.1
M).
<0.
5pm
pm
5 pm
1 pm
1.
0.
0.
0.
0
7
3
03
0.
0.
0.
0.
00046
00032
00014
00001
, Ri =
0
0,
0,
0.
Ri =
0.
0.
0.
0.
0
.0080
. 0056
. 0024
, 0002
-0. 02
017
012
0051
0005
0.
0.
0,
0.
0.
0.
0.
0.
017
012
0051
0005
028
020
0084
0008
Ri = 0. 08
0.
0.
0.
0.
0029
0020
0009
00009
0.
0.
0.
0.
0084
0059
0025
0003
REFERENCES
1.
.k.
J.
En
gelr
nann,
"The
Calculation
of Pre-
cipitation Scavenging, " USAEC Report BNWL-
77 (Battelle Northwest Laboratory) July 1965.
2. A. C. Chamberlain, "Aspects of Travel and
Deposition of Aerosol and Vapor Clouds, "
AERE-HP/R 1261. (Harwell) 1953.
3. J. W. Healy, B. V. Anderson, H. V. Clukey,
and J. K. Soldat, Proc. 2nd Int. Conf. on
Peaceful Uses of Atomic Energy, 18, 309
(1958).
4. A. C. Chamberlain, "Experiments on the
Deposition of Iodine-131 Vapor onto Surfaces
from an Air Stream, " AERE-HP-R 1082
(Harwell) January 3, 1953.
5. W. J. Megaw and R. C. Chadwick, "Some
Field Experiments on the Release and Depo-
sition of Fission Products and Thoria, "
AERE-HP-M-114 (Harwell) December 1956,
(Official Use Only).
6. P. Drinker and T. Hatch, "Industrial Dust,
Hygienic Significance, Measurement and
Control, " 2nd Ed. , McGraw-Hill Book Com-
pany, Inc., New York, 1954.
7/\ C. E. Lapple, et al, "Fluid and Particle
Mechanics, " University of Delaware, Newark,
Delaware, March 1951.
70
-------
329
8. K. Stewart, "The Resuspension of Particulate
Materials from Surface Contamination, in
Surface Contamination, " B. R. Fish,- Ed.
Pergamon Press, 1967, pp. 151-158.
9. P. R. Owen, "Duet Deposition from a Turbu-
lent Airstream, in Aerodynamic Capture of
Particles, " E. G. Richardson, Ed. Perga-
mon Press, New York, I960, pp. 8-Z5.
10. A. C. Chamberlain, "Aspects of the Deposi-
tion of Radioactive and Other Gases and Par-
ticles, in Aerodynamic Capture of Particles,"
E. G. Richardson, Ed., Pergamon Press,
New York, I960, pp. 63-88.
11. J. J. Fuquay, Private Communications,
1957. -.
*i
12. E. H. Markee, Jr. , "A Parametric Study of
Gaseous Plume Depletion by Around Surface
Adsorption," Proceedings of the USAEC
Meteorological Information Meeting, Sep-
' tember 11-14, 1967, C. A. Mawson, Ed.
AECL-2787.
13. O. A. Button, "Micrometeorology," McGraw-
Hill Book Company, Inc., New York, 1953.
14. C. H. B. Priestley, "Turbulent Transfer in
the Lower Atmosphere,'" The University of
Chicago Press, 1959.
15. E. L. Deacon, "Vertical Diffusion on the
Lowest Layers of the Atmosphere, " Quarter-
ly Journal Ray. Meteorol. Soc. 75; 89-103,
1949.
16. F. A. Gifford, Jr., and D. H. Pack, "Sur-
face Deposition of Airborne Material, "
Nucl. Safety, 3, 4, 26-80, 1962.
'•I:
17. U. S. Air Force Nuclear Research Facility,
"Fission Products Field Release Test I, "
Doc. NARF-59-321, September 1959.
18. U. S. Air Force Nuclear Research Facility,
"Fission Products Field Release Test 11, "
Doc. NARF-60-10T, September I960.
19. C. L. Simpson, "Some Measurements of the
Deposition of Matter and its Relatior. to Dif-
fusion from a Continuous Point Source in a
Stable Atmosphere, " USAEC Document HW-
69292 Rev. , April ,1961.
20. H. D. Landahl and R. G. Herrman, J.
Colloid Sc. , 4_: 103, 1949.
21. W. E. Ranz and J. B. Wong, Industrial and
Engineering Chemistry, 44, 6, 1371-1381,
June 1952.
22. G. Asset and D. Pury, Arch, of Industrial
Hygiene and Occupational Medicine, 9, 4,
273-283, April 1954.
71
-------
330
APPENDIX C
PARTICULATE LUNG DOSE EFFECTS
The following discussion appeared orig-
inally in a progress report for this study.
It is reproduced here because of its impor-
tance to the subject of plutonium
standards.
Current standards for limiting lung
dose from internal emitters are based upon
a calculation of the average dose delivered
to the lung by assuming thatrthe radiation
absorption is uniform throughout the mass
of the tissue. It is knowrl that this con-
dition does not exist for most "insoluble"
radioisotopes which provide focal spots of
higH level radiation close to the particle
decreasing with distance in a pattern de-
pendent upon the type and energy of the
32
radiation. Thus, a one uCi P particle
which, if the energy were averaged over the
1000 gram lung of the standard man would
deliver a dose rate of 0.035 rads/day or a
total dose of 0.75 rads, will deliver a
dose rate of about 80,000 rads per day or
a total dose approaching 2,000,000 rads to
the tissue at 100 urn distance. Richmond,
et al., report an alpha particle dose rate
of 10 rads/hour at the surface of a 180 um
238
the surface is about 500 rads/hour. Dose
and dose rates drop off rapidly with dis-
tance from the particle so that the total
volume of tissue involved is small. Table I
illustrates the same point for the maximum
permissible lung burden of plutonium if
this lung burden is divided into uniform
particles of various sizes.
From these illustrations, the physical
conditions of such irradiation are vastly
different from the uniform distribution and
the particulate exposure results in a
relatively small number of cells irradiated
to widely differing doses. While one would
expect differences in the outcome of
irradiation of an organ by these two modes,
it is not clear on a priori basis which
would be the most damaging. For acute
effects occurring after high levels,
limiting the volume of tissue can greatly
ameliorate the outcome. However, data are
not available to indicate whether a similar
situation exists for the late effects.
It is clear that this problem is a
subclass of a more general problem in ar-
riving at radiation protection standards—
Pu particle. The photon dose rate at
TABLE
RELATION BETWEEN .PARTICLE DIAMETER, PARTICLE NUMBER, DISINTEQRATION RATE
AND NUMBER OF CELLS IRRADIATED FOR A LUNG BURDEN OF 0.016uCi 239PuO,
Diameter
(um)
0.01
0.1
1.0
Number of
Particles
5.1 x 1010
5.1 x 107
5.1 x 10
Disintegration Rate
(d-week~I-partiele~l)
Number of Cells
Irradiated3-
6.7 x 10~3
6.7
6.7 x 103
1.1 x 10
1.1 x 10
1.5 x 107
13
10
For each particle size the number of .-Cells exposed within a 10 iam alpha
particle range is estimated. The total number of cells irradiated be-
comes the product of the number of cells irradiated per particle and
the number of particles. A cell volume of 103 pm3 is assumed.
72
-------
that of nonhomogeneous dose In any organ.
In order to focus more clearly on the Im-
portant question, we have considered the
current limits for uniform radiation to be
acceptable and have, then, asked whether
there Is any evidence which Indicates that
the nonunlform radiation to an organ, such
as occurs In extreme form in the particle
problem, Is more or less damaging than the
homogeneous radiation. Thus, the focus Is
on the relative, and not the absolute ef-
fect. Further, since we assumed that no
clear-cut information was available, we
went to the literature to see if even a
tentative conclusion could be made as to
whether the preponderance of the evidence
indicated which assumption should be made.
A. Review of the Literature - J. Furchner
A large number of papers and reports on
radiation dose to the lung and subsequent
damage was reviewed. One problem with
much of the work reviewed, and particularly
that having to do with individual implanted
sources, was the lack of consistency in the
331
doslmetry. Thus, some groups expressed the
dose as the average to the lung while
others calculated the dose at some refer-
ence distance from the source. While the
original Intent of this study was to at-
tempt recalculation of the doses on a com-
mon basis, this was made difficult in some
cases by the lack of data in the published
article, the uncertainty of location of the
source and the lack of time to complete a
job of this • magnitude, particularly when
the initial appraisal indicated that the
results would be uncertain.
For each paper of interest, or poten-
tial interest, to the present study a
brief abstract emphasizing the actual data
presented was prepared. Although such ab-
stracts are of primary usefulness to those
who are familar with the original article,
they are presented below as orientation to
the data available. In each case, comments
by the abstractor are presented In paren-
theses.
1. IMPLANTED SOURCES
60 Co Warren and Gates I960 2
Mice 4-6 weeks old.. °OCo wire implanted through chest wall by trochar.
Wire dimension: 2 mm by 0.5 mm. Radioactivity 170-250 yd. Among 190 mice that
survived 9? days (time of appearance of first lung cancer) 20 had carcinoma of
the lung or bronchus. The last treated mouse died 315 days after implantation.
The doses ranged from 90,000 to 1)60.000 rep. (Trauma to the lung is unavoidable;
compare with Richmond et .al. 1970).8
60Co Warren and Gates 19683 .- 6o
Mice, rats, hamsters, guinea pigs and rabbits. Co wire, 2 mm long
by 0.5 mm were implanted by trochar through the chest wall. The activity ranged
from 70-636 uCi. Most sources were between 150-200 pCi.
Treatment Number of
Orou'p Animals
(Species)
Mice
Rats
Hamsters
Guinea Pigs
Raboits
286
20
25
20
12
Median Duration
of Exposure (days)
Lung Esophagusa
180
204
195
116
127
188
202
368
363
299
Mean Total Dose
(R x 103)
Lung Esophagus
262
353
113
510
909
115
121
170
151
250
Malignant Cancer
Incidence (%) ,
Lung Esophagus
20
75
a
25
12
15
30
2H
30
25
size increases the carcinogenic dose increases.)
(As animal
-------
332
106
Ku Laskln et al.
196 3*
106C
Rats.Hollow platinum cylinder plated with Ru implanted in bronchus.
5 mm long, 1.2 mm diameter, wall thickness 0.2 mm. Hooks on cylinder maintained
position in bronchus after implantation by trochar ana tracheotomy.
Treatment
Group
uCl on Implant
0.008
0.057
0.59
5.0
13.6
Pt. control
Ru Control
Number of
Animals
37
56
57
67
18
60
22
Median
Survival
Time'
(Days)
310
310
320
225
190
330
320
Median
Time to
Cancer
(Days)
130
100
380
325
315
Number
Survlvinj
113 days'
27
39
10
12
2,9
aTwo rats had cancer before fthis time.
bSquamous cell carcinoma.
Number
with Lung
Cancerb
2
6
15
25
20
The authors rearranged the groups on the basis of calculated doses for those animals
surviving 113 days.
Average Dose
(Rads)a
3,100
36,000
160,000
1,600,000
Number of
Animals
5
11
11
57
32
Squanous Cell
Carcinomas
Numbers %
0
3
9
33
21
o
.7.3b
21.9
57.9
65.6
apose calculated at "target" tissue taken as basal layer of the epithelium of the bronchus
in which pellet was implanted - 100 ym from pellet surface.
b One tumor at 1100 rads. (There is no mention of the incidence of respiratory Infections
or causes of earlier deaths. The considerable trauma associated with Implantation may be
a factor) .
l°6Ru, 32P Laskln et al.
Rats. Hollow platinum cylinder plated with Ru Implanted In bronchus. 5 mm long,
1.2 mm diameter, wall thickness, 0.2 mm. Hooks on cylinder maintained position In bronchus
after Implantation by trochar and tracheotomy. A single dose level of I06fju (5 yd) was
given. The animals were autopsied after spontaneous death and serial sacrifice.
Phosphorua-32 pellets were also implanted in rats by this technique.
106
Ru
Mean Time of Death
Sacrificed Spontaneous
A B
122
166
198
212
225
217
282
357
129
158
193
233
300
317
378
121
Number of
Animals
A B
10
13
10
10
16
10
9
8
9
18
10
10
13
11
9
9
Mean
(Rads
A
1.2
1.3
5.2
5.2
5.t
6.3
6.5
7.7
Dosea
x 105)
B
3.2
1.5
5.2
5.5
6.9
8.0
8.6
9.2
Cancer Incidence
(J)
A B
0
15.1
30.0
60.0
81.3
90.0
88.9
100.0
0
11.1
20.0
50.0
81.6
81.8
88.9
100.0
THo~eancers' before 158 days. Only 1 animals in 31 had lung cancers after doses of 1
Rads over 160 days. Again no mention of chronic ..respiratory Infection is made).
-------
32,
333
Treatment Group
20.0 yd
2.0 pCl
0.2 yd
Number of
Animals
18
15
15
Lung Dose
(Rads)
5
it
10
10-
Lung Cancer
56
33
0
106
'Ru data from Laskln efc al. 1963, better than
(The P dose response agrees with the
does the IobRu data In this paper).
a see note on Laskin et al. 1963 for meaning of dose calculation.
106Ru Dlvertie. Titus and Shorter 1967 .
Rats 150-200 g, Sillcone rubber pegs (2.5 mm x 1 mm) impregnated with 50um ceramic
spheres containing lo6Ru were inserted Into a bronchus via tracheotomy. Twelve control
animals had inert pegs inserted Into a bronchus. Thirteen of 16 rats receiving radio-
active pegs had squamous cell, carcinomas. None were found in controls. Ho doses
are given. ...
Duration
of
Exposure
(wit's)
yCi Dose
Inserted
Recovered
ANIMALS WITH SQUAMOUS CELL CARCINOMA
18 19 20 21 23 ?5 30 34 _3_4_ _35_ _3j5_ _J6_ _38_
15.6
11.3
14.0
10.1
10.0
7.5
13.1
10.0
8.1
6.0
14.8
9.4
12.6
7.6,
13.4
•8.1
12.6
-, 7.6
14.1
8.3
Pneumonitis was usually found
In two of the three experimentals no pegs -were recovered.
distal to the pegs.
9°Sr Altmann, Hunstein and Stutz 1961' qo
Rats. Plexiglass capsules containing * Sr were sewed to the underside of the diaphragm.
The activity range was 27-62 uCi with most values between 39 and 48 yCi.
Treatment
Group
Exposure
Time
(Months)
0-3
3 - 6
6-9
9-12
over 12
Number of
['Animals
28
21
48
36
31
Lung Tumors
Number
Carcinoma
0
2
8
30
26
0
0
0
1
1
Adenoma
0
0
0
0
1
The last two groups q.lso had nonpulmonary tumors. (There is no
clue to dose data given).
75
-------
334
8 R
*3 PuOp Richmond, Langham and Stone 1970
Rats, male, 325 g. Injection of Pu02 spheres via femoral vein. Spheres 122-200 ym
in diameter. The spheres are trapped in the capillary network of the lung. The animals
were sacrificed serially and examined hlstologically. Note this method involves no surgical
trauma to the lung.
Time of Sacrifice
(Days) 1 3 7
No. of Animals 322
2
21
2
30
6
60
10
90
5
120
9
152
6
180
7
211
6
0 o *
The surface dose rates were 10 and 10J rad/hr for the alpha and gamma radiations respec-
tively. A sphere of cellular debris and collagenous tissue surrounded the spheres. A '
footnote, added in proof, states that animals at 600 days postlnjectlon show histological
changes qualitatively similar to those seen at 90, 120, and 211 days. No tumors were found.
9°Sr Cember and Watson 19589 QO
Rats, male, 286 g. Glass beads with incorporated y Sr were implanted with a hypoder-
mic needle through the chest wall. The beads were 320± 110 um in diameter and contained
from 1.09 to 59.3,pCi. Dose data was given only for tumor bearing rats. The mortality
data for the inew Sr and saline control groups was much the same as that for the experi-
mentals and was due to injection trauma.
Dose
Rate
(Rad/day)
160
160
220
277
277
HIO
660 '
Exposure
Time
(Days)
561
1(87
561
169
515
581
333
Total
Dose i.
(Rads x 10 )
9.0
7.8
12.0
1.7
15.0
26..0
22JO
Tumor
Lymphosacoma
Squamous cell carcinoma
Squamous cell Carcinoma
Lymphosarcoma
Lymphoma
Squamous cell carcinoma
Squamous cell carcinoma
The first death occurred at 131 days and the last at 575 days post Injection.
(1 of 23 rats had squamous cell carcinomas at doses of ^105 Rads).
2. INHALATION OR INTRATRACHEAL INJECTION (Beta Emitters)
35
10 j'i
(1.15
S Cember et al. 1955
Rats, female, 125-200 g.
± 0.10 pm).
A single Intratracheal injection of
particles
Dose to >
Lung (rep)
58
3,200
21,000
Rats were killed serially in a 9 month period.
No tumors were found In any group. (The calculated
doses were delivered almost entirely during the first
month). Chronic and acute inflamatlon were common.
Treatment
Group
1.5 yd
15 yd
1,500 PCI
Controls
Number of
Animals
23
21
38
25
1
76
-------
335
fema?et3?4Vg!8l
for 10 consecutive weeks.
12,000 and 20,000 Rads .
tratracheal insufflation of 375 uCi of BaS0, once a week
Particle size 1.15 ym ± 0.40 urn. Dose estimated to be between
Treatment
Group
Colony control
Inert BaSCK
3,750 yd
Number of
Animals
24
24
Number
Surviving
10 weeks
17
16
Number .
Dead at '•'
500 days
2
10
Squamous Cell
Carcinoma
0
0
2
The 'tumors were found in rats that died at 312 and 319 days.
'('
by intratracheal injection. Particle size
1.0 vim, Std dev 1.4.
Treatment
Group
Colony control
Inert CeF,
5 yCi
15 yCi
25 yd
50 yd
Number of
Animals
20
29
27
23
28
15
Number of
Survivors
10
21
19
6
a
Days to
First Tumor
178
48
93
83
Lung Dose
(Rads)
0
0
2,400 .
5,100
10,700
21,000
Number with
Squamous
Cell Carcinoma
0
Q
1
1
7
4
aTo observation of first tumor. Severe, acute pneumonia appeared in the two high dose
Groups within several days. The first tumor appeared in 48 days. (Mortality of the
inert CeF group was not given nor was the duration of the experiment;.
1^Ce Cember 1963
- Rats, male, 283 g. c*
Particle size 1.0 urn std .dev 1.4.
,'V
c**
. . . . .
ora1' intratracheal injection.
Treatment
Group
Inert CeF,
0.5 uCi
1.0 yd
2.0 uCi
4.0 uCi
Number
of
Animals
29
41
44
34
:42
Days to
First '-Tumor
Death
528
367
620
381
Lung
Dose
(Rads)
600
1,100
2,590
4,46o
Primary
Lung
Tumors
6
4
14
Squamous Undiffer-
Cell entiated Adeno- Lymph-
Careinoma Carcinoma Carcinoma oma
0
3
2
2
11
0
3
1
1
1
0
3
3
1
2
aDose at death with first tumor. Earliest tumor at 361 days. (Kxperlment lasted at least
1,033 days. No mention of chronic pulmonary disease was made).
77
-------
336
Ill
by
Ce Cember and
Rats, male,
mouth.
Treatment
Group
Inert CeCl3
10 uCi
15 yd
30 pCi
Stemmer 1
25d g. J-
Number of
Animals
21
68
55
58
9641*
^CeCl. solution
Number of
Survivors
21
61
52
37
given
by intratracheal
Days to First Lung Dp
Lung Tumor (Rads)"
306
197
70
11,000
19,600
25,000
Injection
se Number
Lung
of
of
Tun
q
31
27
0.15 ml
Primary
lors
aTwo month survivors
bDose at death with first tumor
K P/l?§pm^tr? dlffers so"}ewhat from Cember et al. 1959, where the dose rate for
5 PCI ^CeF^ is given as 59.6 rads/day in a 1.5 g lung. Here the dose rate is given
a? ? ^co/^y/°K l ?nKgi^ Cember conslders all the data for l^Ce givenqin,Cember
et al.1959,, .Cember 1963,-^ and Cember and Stemmer I9b^ in Cember 19b1."5'"6
Cember 196115 •l6
Values give.fc,- here
Cember 1964b.l° ^
Dose
(Kads;
660
1,300
2,500
5,500
15,500
26,000
13,500
144
Ce Hahn et al. 1973.
are estimated from Pig. 39, Cember 19l6a15 and from Pig. 5,
'61a 1964b
Tumor Frequency Dose Tumor Frequency
<*) . (Hads; (%)
2.
4.
5.
9.
12.
22.
29.
1
1 rt
17
Beagles. By inhalation of
g std dev 1.5-2.3. To date 15
at 113-110 days; and 5 are dead
Initial Lung Burden
MCI/kg Total uCi
26 230
27 190
31 330
35 380
16 170
33 320
11 330
51 140
53 110
56 ' 520
65 590
66 470
66 540
68 600
96 740
120 890
180 2,000
190 1,500
190 1,700
210 1,700
Time To
Death
( Days )
. 1,185
' 1,318
916
750
'' 193
1135
410
279
273
234
246
257
186
189
171
182
173
181
143
2 ' 650 1.5
0 1,200 2.5
6 4,500 5.0
5 14,000 10.0
5 20,000 12.5
2 11,000 22.5
8 49,500 25.0
i h u
Ce fused in clay particles. vL.4-2.7 A.M.A.D.,
of 126 beagles are dead of fibrosis and pneumonitis
of pulmonary neoplasia at 750-1,318 days.
Dose to Lung
At Death (Rads)a Lung Pathology
27,000 Hemangiosarcoma
23,000 Hemangiosarcoma
36,000 Hemangiosarcoma
31,000 Hemangiosarcoma + bronchiolo-
carclnoma
48,000 Hemangiosarcoma + fibrosarcoma
Pneumonitis +f ibrosis.no tumors
ii n
n n
ii n
n n
n n ]
( n n
n it
n n
n n
n n
n n
n ii
n n
» n
n
n
n
n
n
n
n
It
It
n
II
XI
11
^Calculated by Hahn et al.
are found).
(It appears that more than 700 days must elapse before tumors
78
-------
337
Ce Kurshakova and Ivanov 1962 - ^^
Twenty rabbits 2.5 - 3.0 kg were injected with 25 Ud of CeF by piercing the
anterior wall of the trachea through the skin. The particle size was 0.025 urn. One
rabbit died of bronchopneumonia on the 3rd day. Half of the rabbits died between the
60th and 238th days of sclerosis, bronchiectasis, etc. Tumors were found in 6 of the
animals surviving to 238 days. The last tumor was found at 327 days. The doses to
the lungs at 238 and 327 days were 51.1 and 68.9 kilorads respectively. There were 5
bronchogenlc and alveolar lung cancers and one squamous cell carcinoma of the esophagus.
106Ru Temple et al. I96019
• Mice, female. J-u6Ru02 in Tween-80 was injected intratracheally.
Treatment
Group
Colony Control
Inert Ru02
3.0 viCi
1.93 vCi
I
0.15 yci
it'..:
Number cif
Animals
2i8
21
23
11
10
Days After
Administration
103-470
335-500
350
369-422
340 *
Adenomas
78
9
82
90
Number of
Malignant
Tumors
0
0
1 Bronchiolar
carcinoma
1 Bronchiolar
carcinoma
1 lympho
sarcoma
(The natural incidence of adenomas is a factor of unknown importance to 'radiation
cinogenesis) .
152-154Eu
Deitch 197Q
20
Rats female, 180-200 g. Rats were made to inhale aerosols of radio-europium chloride
for 7 h/day, 5 days/wk for 6 months. The particles were characterized only as "submi-
cronic". The lung dose varied with time and was as much as 6 x 10M rads at 720 days.
No animals were free of pulmonary pathology. Severe chronic inflammatory changes and
lung abscesses we.re present in the majority of the animals. There was a complete absence
of pulmonary neoplasia.
n
_2\a. 32P, 59Fe. 198Au Kochetkova et al. 195921
Rats. These isotopes were given by intratracheal injection. Particle size unspecified.
Treatment
Group
59Fe
1-27
40-100
100-150
Number of Beta Dose (Rads)
Animals First Day Total
52
76
30
10-20
300-700
1400-2100
500-5000
1300-15000
5400-80UO
Metaplasia of
Bronchial
Epithelium Lung Cancer
Number Months Number Months
17
20
4
6-9
2-12
1-3
11
3
6-9
6.5-18
2.5-12
00-
100-200 pCl of
in single and multiple doses produced no tumors.
79
-------
338
P Kochetkova and Avrunlna 1957 ,2
Rats - Intratracheal injection of CrJ PO^. No particle size specified.
Treatment •
Group
(MCI injected)
270
100
70
40
Number of Mean Lung
Animals Burden (yCi)
10
42
34
10
180
81.
54
38
24
2
Lung
h
,900
830
670
350
Dose (Rep)
Total
19
10
8
4
,000-46
,000-18
,000-16
,500- 7
,. Life Span
(Days)
,000
,000
,000
,400
3-32
19-65
15-395
60-451
Pathology
Metaplasia
Metaplasia
3 Squamous
Cancers
3 Squamous
Cancers
Cell
Cell
There were no ttoiors after single and multiple injections of NaCl (200-1,900 yCI).
Of 25 rats that received '320 yCi of radiogold all died in 2.5 months. Three of these
rats had squamous cell cancer. The doses were in 9,000-9,7UO rep range.
INHALATION OR INTRATRACHEAL INJECTION (^Alpha)
Temple et al .
3.
•Pu Tem
Mice (BAF) PuC>2 suspended in Tween-80 or Pluronics for injection.
0.6-0.06^m mean 0.5 pm.
Particle size
Treatment
Group
Colony Control
0.16 yCi
0.06 yCi
0.003 MCI
Number of
Animals
I
28
41
17
21
Days After Dose
Administration (Rads)
400 '
100 4,000
400 2,300
500 115
Lung Tumor
22 Adenomas
1 Bronchiolar carcinoma
2 Squamous cell carcinomas
1 Fibro sarcoma
At 400 days 78% of the colony controls had adenomas. The fibrosarcoma at the 0.003 level
was considered non-radiogenic (the use of surface active agents as vehicles for the parti-
cles is a factor of unknown importance).
210
23
Po Yuile, et al. 1967
Rats, male,exposed once to an aerosol of
metric mean 0.09Bum, geometric std dev 1.81.
210
Po as the chloride, particle size: geo-
Treatment
Group
NaCl Control
0.15 PCi
0.05 UC1
0.02 PCI .
Number of
Animals
147
119
129
132
Number of
Deaths
119
98
71
Age Range At
End (wks)
87-100
106
95-100
89-91
Lung Dose
(Rads)
0
538
202
71
Primary
Lung
Tumors
0
22
15
4
Squamous
Cell
Carcinomas
0
17 i
5
1
Dose accumulated at 280 days - little increase thereafter. The aerosol was a NaCl
solution acidified to a pH of 1. Pulmonary infection was endemic in the colony and
an epidemic of acute pneumonia occurred during the second year. The experiment was
terminated when the last high-dose animal died at the 96th week.
239
Pu Wager et al. 1955
24
Mice (BAF) female - Intratracheal injection with Tween 80. Particle size 0.05 to
0.6 urn. Of 10 mice that received 0.06 uCi of 23Spu02, 3 had squamous cell carcinoma
at 1 year post-injection.
80
-------
210
25
Po Scott and Thomas 1957
Hats.Intratracheal injection of
15 months when there were 5 survivors.
210.
339
Po nitrate solution. Experiment terminated at
Treatment
Group
10 UCi/kg
5 UCi/kg
Number of
Animals
15
15
Squampus Cell
Carcinomas
0
2
Time to Tumor
(weeks)
5, 15
All animals exhibited varying degrees of murlne pneumonia.
210
Po
Little et al. 1970
26
210,
Syrian golden hamsters. " Po adsorbed on 3 mg .of FB^OT, particles (98% < 0.75 um):
suspended in saline given in 15 consecutive weekly intratracneal injections.
Treatment
Group
Control
FejiOg only
0.2 uCi/wk
0.01 wCi/wk
Number of
Animals
6'3't
32
35
34
Number of
Deadr Animals
52
1 30
35
21
Current
Week
93
93
60
59
Tumor Bearing Animals
No. % First Tumor
0 0
0 0
32 91
10 30
15th wk
40th wk
Total Dose at
2 yr (Rads)
4,500
225
The number of animals consists of the survivors of the 15-week treatment period which
were autopsied (60 animals/group at start). The doses given are maxima-carcinogenic
doses which are less than 225 rads.
210
Po Grossman et al. 1971
27
,26
A later report on Little et al. 1970""" gives the incidence of bronchogenic tumors
as 91? and 43% in the high and low dose groups respeetively.
Syrian golden hamsters were given intratracheal injections twice weekly for 7 weeks.
The doses were given in two separate intratracheal instillations (a and b in table below),
Treatment Group
47 wk
Survivors
Tumors at 27 wk
3 mg FegOj
Saline
Saline
Saline
0
0
0
0
.2
.2
.2
.2
UCi in saline
uCi .
yCU'lon
pCi
on
3
0
.0
.3
mg
mg
Fe
Fe
2
2
0
0
3
3
2
6
28
32
210Po alone is said to be homogenously distributed in the lung.
17
9
7
3
238
28
U Leach et al. 1970
Monkeys, dogs, and rats were exposed to 003 dust (M.M.D. 1.03 urn, g std dev 2.40)
5 mg/m3' for 6 h/day, 5 days/wk. The rats, after an exposure of 1 year, showed no
pathological changes in the lung apart from pigmented macrophages in the alveoli and '
bronchi. In dogs there were no pathological changes in the lung after 5 years of exposure
and estimated radiation doses of 400 rads. Monkeys responded with a patchy hyaline
fibrosls that first appeared at 3.6 years after a dose of 500 rads. No tumors were
reported in any animals at the end of the 5 year exposure. Despite doses to the tracheo-
bronchial lymph nodes of dogs and monkeys that were on-the order of 104 rads no pathology
other than an occasional necrosis and fibrosis were reported.
81
-------
340
239
29
Pu Antonehenko et al. 1969
Rats, 140-160 g, were exposed to an aerosol (90? 0.7-1.9wm, median diameter 1 um)
of Pu citrate or ammonium plutonlum pentacarbonate. (pH 5 and 8, respectively) for 20 mln.
Lung Pathology (&)
Treatment Number of Average Life Average Life Card- Ade- Adenoma-like Epithelial
Group Animals Days Dose (rads) noma noma Structures Metaplasia
673 0 "
Controls
Citrate
1.028 uCla
0.803 pCl
0.511 MCI
218
23
12
, 9t
Carbonate
1.160 uCl
0.77t yd
0.455 PCI
23
69
64
69
124
f
i 77
78
139
3,820
3,090
2,370
7,320
3,900
2,780
2.2
4.6
3.08
8.9
4.4
12.0
9.1
8.3
73.1
9.09
13.0
61.6
alnltial deposition.(Apparently the short survival time in the higher dose groups pre-
cluded the development of the characteristic pathology).
239
Pu Buldakov et al.
30
Rats. Inhalation of soluble Pu compounds: citrate and ammonium pentacart>onate.
Treatment ,
( vc
Citrate
Ammonium-
Plutonlum-
Penta-
Carbonate
*
Group
i deposited)
0.008
0.02
0.04
0.08
0.15
0.25
0.36
0.51
0.80
1.03
0.004
0.007
0.017
0.045
0.15
0.25
0.35
0.46
Q.77
1.46
Number of
Animals
157
124
203
31
105
113
rt 39
11 90
12
20
48 ,
101
91
126
83
126 '
22
65 ,
23 '
11
Mean Survival
(Days)
635
585
515
516
464
416
221
124
63
64
571
571
584
582
481
361
217
139
78
77
Lung Dose
(Rads)
47
117
234
167
852
1,390
1.740
2,370
3,090
3,820
41
80
186
197
1,065
1,615
2,140
2,780
3,900
7,320
Lung Tumors
%
5
2.5
8.4
35.5
23.8
23.0
7.7
0
0
0
1.2
5.0
13.2
36.4
42.7
26.4
9.0
0
0
0
The tumors were squamous cell carcinomas, adenocarcinomas and hemangiomos.
the tumor Incidence at low doses and the absence of tumors at high doses.
Note
239Pu Clark et al. 196431
Dogs inhaled particles (0.5-0.65 um). At 855 days 28 were dead. There was one
lung tumor at 150 days. Six more died between 855 days and 1,446 days, of these, four
had bronchiolo-alveolar tumors. The estimated d'cises were between 9,000 and 23,000 rads,
resulting from burdens of 0.6 to 19 vCl.
82
-------
341
239Pu Park et al. 19673
Dogs inhaled particles (0.5-0.65 ym) (continued from above). Of 25 dogs dying or
sacrificed between 850 and 2,270 days, 12 had primary pulmonary tumors. The estimated
doses to the tumor bearing animals ranged between 3,100 and 13,600 rads, resulting from
terminal lung burdens of 0.5-2.7 yCi.
239Pu Park et al. 197233
Dogs inhaled Pu02 particles (0.5-0.65 um) (continued from above). Of65 dogs
exposed, 62 are dead, and 24 had pulmonary neoplasla. Between 55 and 1,600 days, 36
died of pulmonary insufficiencies (edema, fibrosis, hyperplasia etc.) 'Twenty of 21
dogs surviving 1,600 days had lung tumors. Estimated initial lung burdens were 0.2 to
3.3 uCi. At 11 years the average dose to the lungs of tumor-bearing animals was in
the 2,000-12,000 rads range.
238Pu Park et al. t,-19703'*2l8
Twelve dogs inhaled -|Pu02 particles: CMD 0.05 um GSD 1.9.
Terminal Burden Lung Burden Survival Time
) ( yCi) (% Terminal Burden) (Days)
261 92 27
167 94 30
168 93 35
112 92 56
7t ' 91 56
140. 94 61
84a i 90 Y 70
88a 90 - 76
58 91 77
44 91 Ql|
17a 80 125
25 77 180
"animals with,lung tumors: bronchiolo-alveolar carcinoma. Dose
range, all animals, 8,000 to 26,000 rads. Almost total necrosis of
tracheobronchial, mediastinal, and sternal lymph nodes.
H
238Pu C. L. Sanders 197335
Rats, female, were exposed to an aerosol of crushed 3 PuO? microspheres:
CMD 0.02, GSD 2.1. The material was considered soluble (72% ultrafilterable).
Life-time study (>1,000 days).
Treatment Number of Lung Dosea Lung Tumors Median Life
Group Animals (Rads) % Span (days)
Cbntrol 92 0 1.1 825
5 nCl° 30 9 6.6 ^ 650
18 ndb 30 1 32 23.3 675
230 ndb , 30 375 25.0 550
?• mean dose in 2 years
mean initial lung deposition
tumor incidence in the 5 nCi group was not significantly different from lung
tumor Incidence in the control group. Of the 19 pulmonary tumors found, 14 were
bronchiolo-alveolar carcinomas, 2 were mixed carcinomas and there was one epidermoid
carcinoma, one undifferentiated carcinoma and one lymphosarcoma. The author concludes:
" - that spreading the Pu dose in the lung, as .compared to concentrating in
Pu02 particles, is more carcinogenic due to the greater number of epithelial cells
'hit' by alpha emissions from Pu".
83
-------
342
241
,36
Am Thomas et al. 1972-
Dogs wer« exposed to an aerosol (AMAD 0.9 urn, GSD 1.5).
Lung Burden (yCl) Days to Lung Dose
Initial At Sacrifice Sacrifice (Rads)
31
21
26
23
2.3
1.0
0.71
0.38
12?
256
512
1,022
3,000
3,200
3,800
5,300
Lung Pathology
Inflammation
Fibrosife
Flbrosls and mineralization
Plbrosls and mineralization
of the
211
Am had left the
Doses to lung were delivered early; more than
lung by 127 days. The highest doses were delivered to the tracheobronchial
lymph nodes (3,500-17,100 Rads), but the chief pathologies were flbrosis In
the medullary areas and depletion of lymphold elements.
237Np Levdik ett*a'l. 1971
37
p ev t.
Rats were injected intratracheally with nitrate and oxalate solutions of
23'Np (pH 2-3 and 5, respectively).
Treatment
Group
Control
Nitrate
0.017
0.083
0.11
2.0
Oxalate
0.017
0.083
0.11
2.0
Number of
Animals
271
50
111
18
19
85
89
89
81
Average Life
Span(Days) *
700
660
681
685
505
615
661
619
153
Dose
(Rads)
28-
138
2,500
27
131
671
3,220
Lung Tumor Incidence (%)
Malignant Benigh
3-65
16.0
20.5
12.68
11.28
10.6
9.0
28.0
37.15
0.36
2.0
1.65
8.35
2.1
0.0
3.36
5.6
3.75
Part of the increased carcinogeniclty is attributed to the chemical toxicity of
Neptunium. ;
1. EXTERNAL IRRADIATION
.38
X-ray Koletsky and Gustafson 1955"
•220 kV, 15 ma, filters:1.0 mm Al, 0.5 mm Cu, 60 R/min.
Rats, male, 200 g were exposed to a single total dose of 660 R of whole-body
radiation. The 123 rats that survived 6 months or more were autopsied at death.
Treatment
Group
(Time of Death)
6-12 months
12-18 months
18-24 months
over 24 months
Number of
Deaths
Irrad.
16
47
29
a 1
Con.
3
6
11
13
Number
With Tumors
Irrad. Con,
7
32
29
1
One rat had primary carcinoma of th'e lung, an undifferentiated carcinoma
in the lower left lobe. The right lung had an adenocarcinoma. The time
of appearance is not given.
84
-------
343
X-ray Cember et al. 195639
100 Kv, 4 ma, filters: 1 mm Al. 61.8 R/min.
Rats, female, 270 g; equal doses on 5 consecutive days. Only the thoracic region
was exposed. The rats were rotated 4 times during each exposure.
Treatment
Group
Control
5,750
11,500
17,250
Number of
Animals
20
20
20
15
First Death
(wks)
No losses
6
3
3
Median Lethal
Time
12 months
166 days
37 days
Last Death
6 Sac.% 15 months
11 months
6 months
Tumors
2 lymphoma
1 lymphoma
1 lymphoma
The primary loci of the tumors is uncertain because of mctastases.
the most common'finding.
Broncho-pneumonia was
X-ray Maisin et
-------
344
lip
Caatanera et al. 1971 .
Male rats were given a single whole-body exposure to fast neutrons (12 Mev HT on Be).
The rats were free of epidemic respiratory infections.
Age
Treatment
Group
(months) Dose (Rads)
1
1
3
3
21
21
215
0
230
0
215 ?
0
Number of
Animals
79
40
41
11
53
24
Median Survival
Time (Days)
433
699
436
601
167
158
Primary Lung Tumors
Benign Malignant
13
5
17
0
All tumors were bronchiolar in origin. Multiple tumors were found in other organs.
X-ray DeVllliers and Gross 1966
43
135 TtV, 4 ma, filters: 2.43 mm Al. VLOO R/min.
Male Syrian golden hamsters and male rats were exposed to 5 equal doses of x-rays
delivered on 5 consecutive days. A collimated beam was directed at the chest region.
Pour portals were varied through 90° per day. Hamsters received 4,000 R, rats 3,570 R.
Rats
Time of
Sacrifice
(Months)
12
24
Hamsters
Spontaneous
Deaths
Squamous
Cell Cancer
Number of
Animals
12
11
12
12
Adenomas
Tumors
Malignant
n
1 1P-
1 Adenocarcinoma
2 - Reticulum cell sarcoma
Squamous cell carcinoma
Post Irradiation Time (weeks)
11. 12. 11. ii il Ii Ii
3 3 13 6 t 22
- - 2 - 2 1 -
18
ii
3
Fifty-seven hamsters were irradiated, all died spontaneously. Only those dying be-
tween 6 and 20 weeks (42) are listed. Pulmonary cancers were not found later than1
3 1/2 months, although 4 at 6 months and at 12 months and 13 at 24 months, whereas 7
of the eight tumors found in rats were found at 12 or 24 months.
86
-------
345
X-ray Gross et al. 1969'*''
3,000 R, 110 kV,. 6.4 ma, filters: 1.83 mm Al. 75 R/mln and 4,000 R, HO kV, 8.6 ma
filters: 1.83 mm Al. 100 R/min.
Rats and hamsters were exposed to a collimated beam of x-rftys directed at the chest
region. The animals were rotated axlally at 7 rpm during exposure which was given in
5 equal doses on 5 consecutive days. Eight weeks after exposure some animals were treated
with dimethyl benzanthracene (DMBA) and/or Jewelers rouge (Fe 0 )
Treatment Group
(Rats)
Number of
Animals
9 Month
Survivors
Adeno-
carcinoma
Squamous
Cell Carcinoma.
Flbro-
sarcoma
Undlffer-
entiated
DMBA + Fe20
Radiation only
40
40
43
37
29
42
15
7
18
DMBA + Fe203
40
40
39
39
14
16
Data for the appropriate controls are not tabulated. In the unirradiate
-------
346
B. Discussion - J. W. Healy
Prior to World War II and the Manhattan
Project, radiation exposure limits had been
derived for X-rays or radium gamma rays,
for radon in the air and for radium as an
Internal emitter.* The external limits
were based on the radiation field to which
the individual was exposed with little or
no consideration of the distribution of
radiation through the body or of the expo-
sure of specific organs.** During the Man-
hattan Project, the need for considering
radiations other than X- pr gamma, the
presence of varying energies of radiations
and the availability of a ' wide variety of
radioactive chemical species resulted in
the extrapolation of these limits to the
new! conditions through the derivation of
new concepts (such as the rem) and an
Increased sophistication in dosimetry as
applied to individual organs.
Following the war, considerable atten-
tion was given to formalizing these con-
cepts in a manner which could be used by
those responsible for guiding radiation
protection practices in the vastly in-
creased uses of radiation and radioactive
materials resulting from ,nuclear energy.
This work was carried out by the NCRP in
consultation with foreign scientists
through conferences and informal discus-
sions. In 1954, the NCRP subcommittee on
Permissible Internal Emitters published
their report -* that first expounded on the
critical organ concept which has served as
the basis for the majority of the internal
emitter limitations.* Here the critical
organs were defined on the basis of exper-
ience with external radiation. The skin
was chosen as one organ because of the pro-
duction of skin cancers, usually on the
hands from the greater exposure which they
received. The increased incidence of leu- (.
kemia in radiologists led to the designa-
tion of the blood-forming organs as one of
the more important critical organs, while
cataracts produced by high LET radiations
resulted in the lens of the eye receiving
special designation. Since leukemia was
the primary outcome from whole body radia-
tion in the experience available, it was
considered "- - - safe to assume at present
that the blood-forming organs constitute
the most critical organs".** Exposure to
the more deeply seated organs was then lim-
ited to that of the bloqd-forming organs.
In the 1954 NCRP document, the limits
for tine blood-forming organs and other or-
gans were established at 0.3 rems per week
(if received every week this would be es-
sentially 15 rems per year). This is the
limitation used by the Internal Dose Com-
mittee116 in obtaining their values for
organs other than bone. In 1957. the NCRP
again revised their recommendations for
•For an excellent review of the information
available on the effects of internal radia-
tion on humans at the time of World War II,
the reader is referred to "The Tolerance
D.ose" MDDC 1100 by S. T. Cantril and H. M.
Parker.
»«In this statement we are referring to the
official limitations adopted by the NCRP
and the ICRP. Individuals did concern
themselves with these matters in reviewing
the data available and in applying the lim-
its.
•Subcommittee 2 on Permissible Internal
Dose published its report in 1953^° listing
MFC's and maximum permissible body burdens
based on the critical organ concept. The
dose limitations were those given in the
later report of the external dose subcommit-
tee and seem to reflect the NCRP decisions
arrived at in the later report.
**Genetic considerations are not pertinent
to this review but they were not ignored.
"Prom the point of, view of genetic damage
manifestable in future generations, the gon-
ads, of course, constitute the critical
tissues 'par excellence1." However, the
contribution of occupational exposures to
the dose to the population as a whole was
not considered limiting.
***Bone limits were based upon a biological
comparison with radium.
-------
workers to lower the radiation doses to the
whole body, head and trunk, active
blood-forming organs and gonads to an av-
erage of 5 rems per year over the working
\\n
years beyond age 18. ' However, the rec-
ommended limits for Internal organs other
than thyroid, skin, and gonads remained at
15 rems per year. In the same document the
NCRP recommended levels of one-tenth of
those for workers for individuals outside
of the controlled area. The latest report
MO
of the NCRP continues the use of 15 rems
per year for organs other than red bone
marrow, skin, and gonads for 'occupational
workers, but reconAnds a limitation of 0.5
rems per year to individual organs for
members of the general public.
Thus, it can be seen that the current
limitation of 15 rems per year for the lung
of workers can be traced to the original
critical organ concept and the dose
limitations derived from early experience
with external radiation. The recent lower-
ing of the recommended limit for the lung
of individual members of the public by the
NCRP is by a factor of three and Is ex-
pressly Indicated as being "- - - based
primarily on the desire for numerical sim-
plicity in the standards and not on an
established biomedical need." At the same
time, the 1971 NCRP recommendations include
a concept of "significant volume" over
which the dose should be averaged. The
implication being that any redistribution .
of a given dose within thj.s volume would
not significantly affect the outcome. The
1971 NCRP report continues, "It is usually
assumed ' that the 'significant volume'
should be of the order of one cubic centi-
meter. This will be grossly conservative
347
under most circumstances, and in special
estimations, use of a larger volume is jus-
tified."*
Although the original decision to use
the average dose to the lung (or other or-
gans) was made in the early period of the
derivation of dose limitations, it should
-if
not be inferred that those bodies respon-
sible for such recommendations have Ignored
the subject. In the Chalk River Tri-Par-
tite Conference with, scientists from the
ho
U.S., U.K. and Canada, y the statement Is
made: "In relation to the possible patho-
logical effects of radioactive particulates
in the lungs, Dr. Hamilton pointed out that
the cells in the immediate neighborhood of
a dust particle containing 1 or 2% of plu-
tonium would be subjected to a dose of a-
vbout 400 r/day. The general opinion which
emerged from the discussion was that the
carcinogenic effect per unit volume is
probably considerably less" for the irradia-
tion of small masses of tissue than for
large.'1, The ICRP has addressed this gener-
al question of non-uniform dose periodi-
cally, usually by special groups commis-
sioned by the ICRP to study the question.
In its Publication 9 (1966),5° the ICRP
stated:
"In the case of non-homogeneous dis-
tribution of absorbed dose in the lung, an
estimate of the Dose Equivalent to the
whole lung, determined merely by the prod-
uct of QF and the mean absorbed dose, may
be greatly in error, but our full under-
standing of this problem must await further
experimental evidence. In the meantime
there is no clear evidence to show whether,
•The foregoing review has been greatly
shortened to indicate the salient points in
the derivation of the current lung limita-
tions. At the same time, it has focused on
the NCRP recommendations because of their
importance in the early days when the pres-
ent limits were first derived. The ICRP
recommendations differ In detail but follow
the s'ame general pattern. The reader with
interest in this subject Is urged to re-
view these documents for further detail.
-------
348
with a given mean absorbed dose, the
biological risk associated with a non-
homogeneous distribution Is greater or less
than the risk resulting from a more diffuse
distribution of that dose In the lung." In
Publication 11 (19&9)51 prepared by two
Task Groups of ICRP Committee 1, the Irra-
diation from radioactive particles was con-
sidered specifically. Here, it is stated:
"The problems of high local concentration
of dose are at their most severe with ra-
dioactive pai-ticulate material, in the
tissue, especially with afcpha emitters.
Here the localf.'dose can reach very high
values even though the meah tissue dose may
be very low. Certainly it cannot be as-
sumed that linearity of dose and effect
willl hold at these high doses and dose
rates. On the other hand, there may be a '
great deal of cell death, and particularly
with alpha emission, with its short and.
well-defined range, the number of affected
but viable cells may be small compared with
the number of killed cells. However, this
ratio will depend on the size and activity
of the particles, the extent to which they
aggregate, and their movement within the
tissue, and the movement of the cells past
them.
"On the basis of general considerations and
some experimental data and clinical exper-
ience the Task Group • were of the opinion
that, for late effects, the same radiation
energy absorption might well be less effec-
tive when distributed as a series of "hot
spots" than when uniformly distributed.
Thus,'with particulate radioactive sources
within a tissue, a mean tissue dose would
probably introduce a factor of' safety.
However, a severe practical problem has now
been recognized in connection with the In-
halation of plutonlum partlculates, and is
now being considered in detail by a Task
Group of Committee 1 of ICRP."
The Task groups also considered the problem
of translocation of plutonium to lymph tis-
sue and concluded:
""In the meantime, the Task Group are of the
opinion that any immediate change in the
dose limit for plutonlum on the basis of
risk of lymphoid tissue is not warranted."
The potential outcome of an inhalation
of radioactive materials can be changed by
a number of factors. If, for example, the
material is readily translocated from the
lung to other organs, the eventual damage
to these other organs may well appear ear-
lier than, 'and overwhelm any lung damage.*
Thus, in considering lung dose we are fo-
cusing primarily on those materials which
will be retained dn the lung for reasonably
long periods of time. If the quantity in
the lung is large enough, death will result
at early times due to pulmonary insuffi-
ciency resulting from an adema or destruc-
tion of functional living tissue. In prac-
tice, we are interested in low dose effects
which will occur late in life .and carcino-
genesis would seem to present the end point
of greatest interest. Life shortening has
been-'1 noted in many experiments, particu-
larly at higher levels, and is used as a
criterion of damage. The statistical un-
certainties in most experiments occasioned
by the limited numbers of animals and the
variation in death times make this a rela-
tively nonsensitive indicator, even though
the argument can be made that a finding of
no 'significant life shortening is of impor-
tance since a death is a death, regardless
of whether it is caused by a heart attack
or a cancer. However, in many experiments
in which life-shortening was not signifi-
cant , the incidence of cancer at the end of
life was significant, indicating that, radia-
tion effects did occur. As a result, the
present studies focused primarily on cancer
incidence as being the appropriate end
point.
•Of particular interest in this respect is
the recent work at Battelle Northwest?2
which indicates that certain forms of
?i3°Pu02 are rapidly translocated from the
lung to the bone when inhaled resulting in
the production of bone tumors.
90
-------
In most of the experiments there ap-
pears to be a relation between the radia-
tion dose and the time of occurrence of
malignancies in animals: In general, the
higher the dose (or in case of internal
emitters, the dose rate) the shorter the
time required for cancer production. ' This
phenomenon is frequently used to invoke the
possibility of an "effective threshold"
since the time required to permit cancer
formation following a low dose will be so
great that it exceeds the normal life span
even if the induction follows a linear re-
lation with dose. However, in interpreting
data, It must be' iborne in mind that the
opposite phenomenon will occur when the
dose or dose rate becomes too high. That
is, the animal will die from other causes
before there is time to induce cancer.
This was seen in the results from the dogs
at Hanford31»33>34 where the early deaths
were due to pulmonary insufficiency with
cancers eventually appearing only in the
animals with lower lung burdens and which
had lived most of their life span. Thus,
if radiation dose is used as a primary
parameter in investigating incidence, it is
important not only that the animals live
out their normal life span so that the full
cancer incidence develops, but that the
total dose is not so high thatl'j deaths occur
from other causes before .the cancer can de-
velop. These conflicting trends in causes
of death can result in an apparent optimal
dose for the production of malignancies.
However, even at this optimal dose, the
full expression of the malignancies possi-
ble per 'unit dose at lower values will not
occur.
Akin to this concept is that of "over-
kill" of single cells close to the parti-
ole. In the case,discussed above, the pro-
duction of early death by causes 'other than
cancer can be regarded as a result of
"wasted radiation" in interpretations based
upon the narrow concept of carcinogenesis
as an end point.* From this
doses which lead to death before cancer
appears can be considered to be overkill of
the organism since the full expression of
the carcinogenic effects is not attained.
For a single particle in the lung (or other
tissue) the dose rates at close approaches
to the particle can be high enough so that
even a relatively limited time of residence
in the tissue will result in the death of
cells within .a given radius depending upon
the activity • of the particle and the type
of radiation. Such-cells will not be able
to later reproduce and, regardless of the
degree of damage, will not lead to cancer?*
From this standpoint, therefore, one would
expect that particles which lead to such
overkill would be less hazardous than uni-
( form radiation to the overall organ since
not all of the radiation is used in attain-
ing the final end point, cancer. In fact,
such a concept would lead immediately to
the conclusion that the larger the particle
(in tGjrms of activity) the less effective
it would be in producing cancer since the
dose rates close to the particle would in-
crease as the activity increased thereby
leading to a greater fraction of radiation
wasted on dead cells. One clear cut exper-
iment possibly showing this effect was done
by Passonneau >53 using Sr-90 beads on rat
skin.. Here the same amount of activity was
used for the same area of skin but the ac-
tivity was distributed either as a uniform
flat plate, in 50 beads, in 20 beads or in
10 beads. The results given in Table II
Indicate clearly a decrease in the tumor
production efficiency as the activity was
*We have already mentioned that this is an
appropriate end-point for consideration of
dose limitation since it appears to be the
latest effect in time to occur even when
other effects are relatively ineffective In
shortening the life span.
""However, the presence of dead cells, cel-
lular products or fibrosis may be required
before a cellular transformation can express
itself as a cancer. This is an interesting
possibility which needs more study.
91.
-------
350
TABLE II
TUMOR PRODUCTION IN RAT SKIN
UPON EXPOSURE.TO FLAT PLATE AND POINT SOURCES
Source
Flat Plate
1000
Flat Plate
1500
50 beads
20i»'beads
10 beads
Activity
No.
of
Animals
28.6 uc/cm
42.9 we/cm
.,,30 yc/bead
75 yc/bead
i
150 yc/bead
71
73
58
77
74
No.
of
Tumors Relative
pep yc Efficiency
Tumors
89
27
24
16
4.94 x 10
3.10 x 10"11
2.08 x 10"11
.1.44 x 10
1.59
1.00
0.671
0.464
subdivided into more active particles. -^
Gamertsfelder, in an analysis of these
data,1 assumed a mid-lethal dose for cells
of either 1635 or 9300 rads and a probabil-
ity of tumor production increasing as the
nth power of the dose td the cell. He then
calculated the ratio of the number of tu-
mors expected relative to those produced by
the 30 bead configuration. The range of
•the experimental data is not great enough
to permit distinguishing between the curves
represented by different values of n but
within this limited range, ItJhe calculations
fit the observed trend. It is of interest
to note that these calculations indicate a
maximum in the relative efficiency of tumor
production if n is greater than 1 while if
n is equal to one, the curve approaches an
asymtote as the activity per particle gets
smaller. The value of this asymtote for
the assumed median lethal dose of ,1650 rads
is 3.2 and for 9300 rads is 2.12. Since
the condition where the activity per parti-
ble becomes very small is essentially that
of a uniform, plane source, the comparison
between this value and the value of 2.1
noted in the experiment (corrected linearly
from the 1000 uCi flat plate source data)
may be of significance. A somewhat similar
5
calculation by Langham and DeanJ but on an
absolute basis, to predict the probability
of tumor production from various sizes of
Plutonium particles, u'sed data derived by
Albert^ on the production of tumors in rat
skin-, versus dose to the cell. The results
of this calculation show a very high
probability of tumor production from most
particle sizes. However, as the authors
indicate, the paper was published to Illus-
trate the method rather than to provide re-
sults. The results of this work can be
questioned on many grounds including the
use of the data on tumors in rat skin for
lung tissue, the finding of Albert that the
sensitive cells are at the base of the fol-
licle in the rat skin and the fact that the
assumed efficiency of production of lung
cancer per cell does not conform to the
experience with humans in the production of
lung tumors from external radiations.
The results of wasted radiation in the
production of lung fibrosis at high levels
of administration of radlolsotopes or the
induction of other causes of death before
cancer can develop raises the question of
the possible effects of such wasted radia-
;tion in the particle case. Richmond, et
al.8 Investigated the effects of Pu-238
92
-------
dioxide particles lodged in the lung vas-
cular following IV injection. These parti-
cles averaged about 180 ym in diameter- and
gave average dose rates to the entire lung
of about 3.5 rems per hour with the dose
rate in the vicinity of the particle on the
order of 10 rads per hour. The longest
exposure until sacrifice was a group of 6
rats which lived to 600 days. Examination
of the lung following these exposures indi-
cated the presence of a microleison with
complete degeneration of the cells close to
the particle. However, the evidence indi-
cated that this was not simpl'y a stable
type of scar tissu* but rather that the
lesion was in a dynamic state in which the
collagen was renewed constantly with subse-
quent liquification. Within this time pe-
riod ' there was no indication of effects
which would be deleterious to ; the animal's
overall well being. It is noteworthy that
the energy delivered to the lung, if aver-
aged over the full lung would be on the
order of 2,000,000 rads, well in excess of
those doses which have been shown to
produce deaths in relatively short times
when more uniformly distributed and con-
siderably above the doses required to pro-
duce lung cancers. ' .
One of the uncertainties with such an
analysis of overkill of cells it, of course,
the possibility of movement of the parti-
cles within the lung tissue so that the
number of cells at risk becomes much great-.-
er and the doses delivered 'become smaller.
In the experiment of Richmond, et al.
quoted above, the particles were relatively
firmly held in the blood vessels and, there-
fore, were not representative of particles
"Richmond, et al.8 Indicates that Halley
has estimated the average dose to a human
lung for the same size of particle to be
3.5'rems per hour. Using an RBE of 10 for
alpha particles and considering the rat
lung to be on the order of l/500th the mass
of the human lung, the dose in 600 days
becomes:
3.5 x 500 x 21 x 600 = 2,500,000 rads.
00
8
actually deposited in the alevoli. Move-G 0 J.
ment of such particles is known to occur
through ejection with mucus and movement by
the cilia and by engulfment by macrophages.
Thus, quantitative estimates of the degree
of overkill of cells and the fraction of
radiation wasted would be uncertain since
if
such movement is difficult to model. How-
ever, it would seem that such arguments
would be of more interest in the actual
quantitative sense than in the conceptual
sense. If the particles are large enough
so that very high dose rates are encoun-
tered in the near vicinity, there still,
will be a degree of overkill and wasted ra-
diation although it may be considerably
lower than would be estimated by the static
model.
•( Additional uncertainty is added by the
possible reactions of the cells located at
the periphery of the zone of destruction
caused by the radiation." This would in-
volve cells receiving radiation doses rang-
ing fro'iji just subiethal to essentially zero.
If there is attempted repopulation of the
volumes of destruction, this could result
in rapid proliferation of these cells which
have already been damaged. This situation
would appear to be the most serious con-
tender for the production of cancer and
also one which would be the most difficult
to investigate experimentally without an
understanding of the basic mechanism of
cancer production and the response of indi-
vidual cells to these conditions in an
otherwise normal environment and surrounded
by otherwise normal cells. Information on
this possibility is limited, but some indi-
cation that it is not a predominant problem
can be obtained from the experiments of
Passonneau
53
and Richmond which did in-
volve Just such conditions in several types
of tissue.
The outstanding example of increased
carcinogenity of a deposited radioactive
material due to localization and nonuniform
dose 'distribution is plutonium in bone.
93
-------
352
,56
Here, the classical work of Brues led to
the conclusion that plutonlum Is about five
times as effective for the same energy dep-
osition as is radium, which is, in itself,
nonuniformly distributed. Studies of the
comparative deposition in bone of these two
isotopes have indicated that the radium,
being chemically similar to calcium, tends
to deposit in the mineralized portions of
the bone and eventually is distributed
through the bone mineral by remodeling or
Is covered by new layers of calcified mate-
rials. By contrast, the plutonium is de-
posited on the,bone surface in locations
where It is adjacent tq the regenerative
cells and, in remodeling of the bone tends
to redeposit on these surfaces. Thus, this
represents the case of a very nonhomogene-
ous organ where the comparative isotopq
(radium), while not uniformly distributed,
is more uniformly distributed than the plu-
tonium. Further, the plutonium is prefer-
entially deposited in the vicinity of the
regenerative cells which are presumably
more sensitive to the induction of cancer
than the mineralized bone. This situation
would seem to represent a localization of
the radiation dose at cells which present a
more sensitive target and therefore, elim-
inates some of the wasted radiation which
occurs with radium in the mineralized por-
tion of the bone. In.essence, the bone can
be regarded as composed of three regions of
differing criticality: the marrow, the
proliferating cells oft the bone surfaces
and the mineralized portion which has min-
imal metabolic activity and serves primari-
ly as a structural supporting member for
the body. In this case, the sensitive tis-
sues are the marrow and the regenerating
cells with the regenerating cells of most
Interest for plutonium as the average dose
'to the marrow from the poorly penetrating
radiations from plutonium is comparatively
low. Again, however, some significant dose
rates to the marrow on a localized basis
can be calculated. These are to a small
fraction of tne marrow falling within a few
tens of micrometers of the deposited
plutonium. The fact that leukemia is a
relatively rare outcome in experimental
animals given piutonium may serve as an
indicator that irradiation of a small por-
tion of an organ (the marrow) to a high
dose is not particularly troublesome as
long as the average dose Is low.
A similar situation may, of course,
occur, in any organ as a number of different
cell types can be present in the same organ
and any mechanism' which results in prefer-
ential irradiation of the more sensitive
cell types could, theoretically lead to the
same type of result. The high incidence of
lung tumors in uranium miners from radon in
mine atmospheres is attributed to the depo-
sition of the particulate daughters of ra-
don on the bronchi, particularly at points
of division where the turbulence in the air
strean produces increased impaction and
deposition.
''Tne estimation of the radiation dose to
the assumed critical tissue, the bronchial
epithelium, is complicated by the uncertain-
ties in the areas of deposition and the
thickness of the mucus layer which serves
to absorb some of the energy of the radon
daughters deposited on the surface. How-
ever, in a review of the dosimetry for the
C-7
Federal Radiation Council ' Parker con-
siders, with important reservations, that
one working level month corresponds to a
dose to the bronchial epithelium of 2.8
rads. The working level for exposure to
radon daughters is defined as any combina-
tion of radon daughters in one liter, of air
that will result in the ultimate emission
of 1.3 x 10 MeV of potential alpha energy.
One working level month, then, is the total
exposure resulting from working in such an
atmosphere for 170 hours. If we assume
that all of the alpha energy associated
with the daughter products is released in
the lung (i.e. all of the daughters are
deposited and none are eliminated before
94
-------
they decay) the average dose to a 10UO gram
lung would be O.'JI rads . This is undoubt-
edly a maximum estimate since some of the
daughters will be exhaled and a portion
will be eliminated by ciliary action. How-
ever, much of the activity is associated
with small particles which are deposited in
the bronchi and lower pulmonary regions
with relatively high efficiency. The lin-
ear velocity of particles moving up the
bronchi is 0.25 to 1 cm/min while in the
trachea rates can Increase to 3 cm/min.
Because the longest half-life of the radon
daughters of interest is 26.8 'minutes, it
would appear that'1 ^ a sizeable fraction of
the material deposited in the bronchi would
decay before elimination and that all of
the .material deposited below the ciliated
region would contribute their full energy.
If we apply this estimate of the average
lung dose to the estimated exposures of the
uranium miners in those exposure ranges
where the incidence of lung cancer is high,
we find that the dose td the total lung
calculated on an average organ basis is,
indeed, significant, and in the range where
animal data would indicate such an outcome
to be expected. Since there is uncer-
tainty about the actual significance of the
Increase in lung cancer at the, lower expo-
sure levels, we will not mlscuss this
phase. However, the dose levels
corresponding to the exposure ranges used
TABLE III
353
in the epidemiological
''^
assuming-
an .average dose to the lung of O.'J't rads
per WLM are listed in Table III.
•In order to permit a rapid appraisal of
the data presented in the abstracts on the
incidence of lung cancer at various dbse
levels, Pig. 1 presents a crude plot of the
data for the alpha emitters. No attempt
was made in this plot to reevaluate the dose
estimates or to correct for experiments in
which the incidence was measured before the
full life-span of the animals. The five
points at the lowest doses were the results
of the 23?Np and the 2l°Po administrations.
The human data are estimates of doses re-
ceived by a group of 37 individuals exposed
during work with plutonium and represent
periods of time ranging from 4 to 24 years
after exposure.59
AVERAGE LUNG DOSES CORRESPONDING TO LEVELS
OF EXPOSURE USED IN THE URANIUM MINER
EPIDEMIOLOGICAL STUDY
Exposure
WLM
< 120
120 - 359
360 - '839
840 - 1799
1800 - 3719
> 3720
Average Lung
Dose-Rads
< 53
53 - 158
158 - 370
370 ~ 792
792 - 1636
> 1636
An additional argument concerning the
present bases for radiation protection
,standards should be included in this dis-
cussion. As a basis for dose limitations,
it is normally assumed that the response to
a given dose is proportional to the dose
received and that there is no threshold.
While there is considerable evidence to
support the use of this assumption, there
is also evidence that the dose rate is an
important factor, at least for low LET ra-
diations, with the response decreasing as
the dose Is protracted, presumably due to
the repair of the damage in the intervening
time before the full dose is accumulated.
Acceptance of this assumption would indi-
cate that the result of a dose to a small
portion of a given tissue would be the same
*We note that the same argument cannot be
made for alpha emitters since current evi-
dence indicates that the damage from high
LET radiations is not repaired. Thus, the
assumption of linearity with dose, regard-
less of dose rate, would seem to be more
appropriate for these materials than for
the gamma or x-rays. As an aside, .we also
note that the amount of repair for gamma
radiations appears to be on the order of
90?f. If we assume no repair for the alpha
radiations, the late result (after repair
is over) would be about ten times as great
for ;.the alpha radiations as for the gamma.
This 'appears to be about the same as the
commonly accepted RBE or Quality Factor for
alpha radiations.
95
-------
354
60*
50
o
o
40
30
o
o
§ 20
o
10
DO
(91%)
HO
R9
R9
R9
D8 R7
D8
R7
R8
R7
R7
R7 R,
R9 R9
RO
R8
RO R9
10 100
. R9
i JB9 M9
Sj RSR9R9"~~F
1000 10,000
Lung Dose (Rods)
Fig. 1 A plot of the crude data for lung tumor incidence versus lung dose. Data have not
been screened for,length of exposure or accuracy of dose calculations. All doses
are expressed as the average to the lung.
Legend: M-mice; R-rats; D-dogs; H-hamsters; S-humans.
0-210Po; 7,->237Np; 8-r3lSPu; 9-239Pu.
as if the same amount : of energy were dis-
tributed over the entire tissue. We have
seen that this is not the case in some,ex-
treme situations such as; in the overkill of
cells close to a particle or the induction
of more lethal effects at high dose rates.
However, acceptance of the assumption of
linearity at the more moderate conditions
would lead 'to the conclusion that there
should be no difference in outcome regard-
'less of the distribution of the dose
throughout the tissue,, unless a critical
portion of the organ is more sensitive.
This would lead to the conclusion that non-
uniform distribution of dose could have no
greater effect than a uniform dose. Be-
cause this is based upon an assumption
which is made in an effort to be conserva-
tive and is based upon effects at relative-
ly low doses, we do not believe that this
argument is very strong. However, a con-
clusion of nonlinearity of effect could
have a major impact upon current radiations
standard setting practices unless it is
shown that such nonlinearity occurs only at
very high cell doses.
No clear cut, overall picture of the
relative effects of uniform versus focal
dose can be drawn from the present data. It
p O Q
appears, from the J PuO_ microsphere data
and the sKin experiments with Sr that, in
the extreme situation of a single, very
active particle, the focal radiation is con-
siderably less damaging. Cember concludes
96
-------
that the focal source is less damaging for
beta emitters than is the uniformly distri-
buted source. The data of Grossman, e t- al.2^
for Po on iron oxide particles indicates
a seeming decrease in the tumor incidence
as well as increased survival for the focal
sources. Saunders, as a result of his
studies with soluble ^ Pu derived from
crushed microspheres arrives at a conclu-
sion that spreading the dose more uniformly
results in an increased cancer incidence
due to the greater number of epithelial
cells Involved. This conclusion was based
on the observation of "- - df significant
incidence of tuirars in the lung and in
other tissues at radiation doses that have
not previously been shown to be carcinogen-
ic in animals". In Figure 1, it is of in-
terest to note that two of these data
points are included in the five lowest dose
points with the other points being the re-
? 37
suits of J'Np administration. In both
cases, significant numbers of tumors were
also noted in locations other than the lung
indicating a more general insult to the
entire body.
Most of the support for particulates
being more hazardous than a uniformly dis-
tributed material seems to arise from cal-
culations based upon dose .distribution
around the particles and an tlassumed re-
sponse of individual cells to this dose.
In an overall appraisal of the information
available, it does not appear that the
majority of the data support the hypothesis
that the particles are more hazardous than
the uniform dose. A reasonable case can be
made that they are less hazardous. The
conclusion of this work to date, therefore,
is that the preponderance of the evidence
indicates that the use of an average lung
dose is appropriate in limiting exposures
and (may well be conservative.
REFERENCES
355
1. Subcommittee on .Inhalation Hazards, com-
mittee on Pathologic Effects of Atomic
Radiation "Effects of Inhaled Radioac-
tive Particles," Pulication 848, Nation-
al Academy of Sciences-National Research
Council, Washington, D.C. (1961).
2. 0. Gates and .S. Warren, "The Production
of Bronchial "Carcinomas in Mice," Am. J.
Path. 36_: 653 (I960).
3. S. Warren and 0. Gates, "Cancers Induced
in Different Species by Continuous Gamma
Radiation,'" Arch. Environ. Health
17:697 (1968).
4. S. Laskin, M. Kugchner, N. Nelson, B.
"Carcinoma of the Lung in Rats Exposed
to the Beta Radiation of Intrabronchial
Ruthenium-106 Pellets," J. Nat. Cane.
Inst. 31,:219 (1963).
5. S. Laskin, M. Kuschner, B. .Altschuler
and .N. Nelson, "Tissue Reactions and
Dose Relationships in Rats Following
Intrapulmonary Beta Radiation," Health
Physics 1£:1229 (1964).
6. M. B. Divertie, J. L. Titus and R. G.
Shorter, "A Simple Method for the Pro-
duction of Experimental Squamous Cell
Carcinoma of the Lung in Rats," Am.
Rev.. Resp. Dis. 96_: 820 (1967).
7. H. W. Altmann, W. Hunstein, and E.
Stutz, "Uber Lungenveranderungen und
Lungentumoren nach Bestrahlung mit
Radioaktiven Strontium (9°Sr)," Beitr.
Pathol. Anat.' Allgem. Pathol. 12-1:145
(1961).
8. C. R. Richmond, J. Langham, and R. S.
Stone, "Biological Response to Small
Discrete Radioactive Sources - II.
Marphogenesis of Microleisons in Rat
Luogs from Intravenously Injected
238puo2 Microsphere," Health
Physics 1_8:401 (1970).
9. H. Cember and J. A. Watson, "Carcin-
ogenic Effects of Strontium-90 Beads
Implanted in the Lungs of Rats," Am.
Indust. Hyg. Assoc. J. 1£:36 (1958).
10. H. Cember, T. F. Hatch, J, A. Watson,
and T. Grucci, "Pulmonary Effects from
Radioactive Barium Sulfate Dust," AMA
Arch. Indust. Health 12_: 628 (1955).
11. H. Cember and J. A. Watson, "Broncho-
genie Carcinoma from Radioactive Barium
Sulfate," AMA Arch. Indust. Health
17:230 (1958).
97
-------
356
12. H. Cember, J. A. Watson, and A. A.
Apritzer, "Bronchiogenic Carcinoma
from Radioactive Cerium Fluoride," AMA
Arch. Indust. Health 19_:14 (1959).
13.'H. Cember, "Further Studies on Lung
Cancer from It'CeFo," Health Phys.
9_:539 (1963).
14. H. Cember and K. Stemmer, "Lung Cancer
from Radioactive Cerium Chloride,"
Health Phys. 10_:43 (1964).
15. H. Cember, "Radiogenic Lung Cancer,"
Progress in Experimental Tumor Research
v4:251 (1964).
16. H. Cember, "Empirical Establishment of
Cancer-Associated Dose £>o the Lung from
1I(4ce," Health Phys. 10_:1177 (1964).
17. F. F. Hahn, S. A. Benjamin, B. B. Bo-
ecker, T. L.- Chiffelle, C. H. Hobbs,
R. K. Jones, R. 0. McClellan, J. A.
Pickrell, and H. C. Redman, "Primary
j Pulmonary Neoplasms in Beagle Dogs Ex-
posed to Aerosols of l^Ce in Fused-
Clay Particles," J. Nat. Cane. Inst. *
5_p_:675 (1973).
18. N. N. Kurshakova and A. E. Ivanov,
"A Model of Experimental Lung Cancer
Caused by Intretracheal Introduction of
Radioactive Cerium,1' Bull. Exptl.
Biol. Med. 54:787 (1962).
19. L. A. Temple, S. Marks, and W. J. Bair,
"Tumors in Mice After Pulmonary Deposi-
tion of Radioactive Particles," Int.
J. Rad. Biol. 2_:l42 (I960).
20. H. L. Berke and D. Deitch, "Pathological
Effects in the Rat After Repetitive Ex-
posure to Europium 152-154,". Inhalation
Carcinogenesis Conf. 6.91001:429 (1970).
21. T. A. Kotehetkova,-1 G. A. Avrunina, and
N. D. Sagaidak-Chernyak, "Experimental
Lung Cancer Induced with Radioactive
Compounds 32p^ 19&AU, and 59pe," Acta.
Unio. Int. Contra Cane. 19_:684 (1963).
22. T. A. Kotchetkova and G. W. Avrunina,
"Changes in Lungs and Other Organs After
Intratracheal Dosage With Some Radio-
isotopes (2^Na, 32ps 19°Au)," Arch.
23. C. L. Yu,ile, H. L. Berke, and*T. Hull,
"Lung Cancer Following Polonium-210 In-
halation in Rats," Rad. Res. 31:760
(1967).
24. R. W. Wager, N. L. Doekum, L. A. Temple,
and D. H. Willard, "Toxicity of Radio-
active Particles - Intratraehial Injec-
tion of Radioactive Suspensions," Han-
ford Works Annual Report, 1955,
HW-4l500:6l (1956).
25-. J. K. Scott and R. Thomas, "Induction
of Pulmonary Tumors Following Intratra-
cheal Injection of Polonium-210," Univ.
of Rochester Atomic Energy Quarterly
; Report Jul-Sept. 1957:30.
26. J. B. Little, B. N. Grossman, and W. F.
O'Toole, "Respiratory Carcinogenesis
in Hamsters Induced by Polonium-210
Alpha Radiation and Benzo-(a) Pyrene.
Morphology of Experimental Respiratory
Careinoeeneais," Conf. 700501:383
(1970).
27. B. N. Grossman, J. B. Little, and W. F.
O'Toolej "Role of Carrier Particles in
the Induction of Bronchial Cancer in
Hamster's by 210po Alpha Particles,"
Rad. Res. 4J7:253 (1971).
28. L. J. Leach, E. A. Maynard, H. C.
Hodge, J. K. Scott, C. L. Yuile, G. E.
Sylvester, and H. B. Wilson, "A Five-
year Inhalation Study With Natural Ura-
nium Dioxide (UOg) Dust I. Retention
and Biologic Effect in the Monkey, Dog,
and Rat," Health Phys. 18^:599 (1970).
29. G. P. Antonchenko, N. A. Koshurnikova,
and.E. R. Lyubehansky, "Morphological
Changes in the Lungs of Rats After In-
halation of Large Doses of' Soluble Plu-
tonium-239 Compounds," Radiobiology
.i£:97 (1969).
30.'L. A. Buldokov, E. R. Lyunehansky, Yu.
I. Maskalev, and A. P. Nifatov, "The
Problems of Toxicology of Plutonium-239,"
Atom Publications Moscow (1969); also
USAEC Document LF-TR-41 (1970).
31. W. J. Clarke, J. F. Park, J. L. Palotay,
and W. J. Bair, "Bronchioloalveolar
Tumors of the Canine Lung Following In-
halation of Plutonium Particles," Am.
Rev. Resp. Dis. £0:963 (1964).
32. J. F. Park, W. J. Bair, W. J. Clarke,
and E. B. Howard, "Chronic Effects of
Inhaled Plutonium Dioxide in Dogs,"
Pacific Northwest Laboratories Annual
Report 1966 BNWL-4_80_:57 (1967).
33. J. F. Park, W. J. Bair, and R. H. Busch,
"Progress in Beagle Dog Studies With
Transuranlc Elements at Battelle North-
west," Health Phys. 22_:803 (1972).
34. J. F. Park, W. J. Bair, E. B. Howard,
and W. J. Clarke, "Chronic Effects of
Inhaled 239puo2 in Beagles," Pacific
Northwest Laboratories Annual Report
1968 BNWL-1050:'3.3 (1970).
35. C. L. Saunders, "Carcinogenicity of In-
haled Plutonium-238 from Crushed Micro-
spheres," Pacific Northwest Laborato-
ries Annual Report, 1972, Part 1
' BNWL-1750:28 (1973).
98
-------
i
36. R. G. Thomas, R. 0. McClellan, R. L.
Thomas, T. L. Chiffelle, C. H. Hobbs,
P. K. Jones, J. L. Manderly, and J. A.
Pickrell, "Metabolism, Dosimetry. 'and
Biological Effects of Inhaled 24iAm in
Beagle Dogs," Health Phys. 22:863
(1972). ~
37. T. L. Levdik; V. K. Lambert, L. A..
Buldakov, E. R. Lyubehansky, and V. M.
Pesternikov, "Biological Effectiveness
of Neptunium-237," Radiobiology 11:160
(1971). —
38. S. Koletsky and G. E. Gustafson, "Whole-
Body Radiation as a Carcinogenic Agent,"
Cancer Res. 15.: 100 (1955).
39. H. Cember, J. A. Watson, and T. Grucci,
"Pulmonary Radiation Effects as a Func-
tion of Absortte-d Energy Distribution,"
Am. Indust. Hyg. Assoc.jQuart. 17:397
(1956).
tO. J. Malsen, P. Maldague, A. Dunjic, Pham
Hong-Que, and H. Maisen, "Carcinogenic
Affect of a Single Dose of X-Rays in
the Rat," Proceedings of the Second
U.N. International Conference on the
Peaceful Uses of Atomic Energy, Geneva
(1958) Vol. 22.:134.
41. T. J. Castanera, D. C. Jones, D. J.
Kimeoldorf, and V. J. Rosen, "The In-
fluence of Whole-Body pxposure to X-Rays
or Neutrons on the Life-Span Distribu-
tion of Tumors Among Male Rats," Can-
cer Res. 2_8:170 (1968).
42. T. J. Castanera, D. C. Jones, D. J.
Kimeldorf, and V. J. Rosen, "The Ef-
fects of Age at Exposure, to a Sub-Lethal
Dose of Fast Neutrons on Tumorigenesis
in the Male Rat," Cancer Res. 31:1543
(1971). , (.| ~
43. A. J. DeVilliers and P. Gross, "Mor-
phological Changes iriduced in the Lungs
of Hamsters and Rats by External Radia-
tion (X-Rays)," Cancer 19_:1399 (1966),
44. P. Gross, E. A. Pfitzer', J. Watson, R.
deTreville, M. Kaschak, E. Tolker, and
M. A. Babycek, "Experimental Carcino-
genesls: Bronchial Intramural Adeno-
cardinomas in Rats from X-Ray Irradia-
tion of the Chest," Cancer 23:1046
(1969). ,
45. National Committee on Radiation Protec-
tion, "Permissible Dose From External
• Sources of Ionizing Radiation," Natl.
,Bur. Stds. HB 59, Sept. 24,.1954.
46. National Committee on Radiation, "Maxi-
mum Permissible Amounts of Radioisotopes
in the Human Body and Maximum Permissi-
ble Concentrations in Air and Water,"
Natl. Bur. Stds. HB 52, Mar. 20, 1953.
357
47. National Committee on Radiation Protec-
tion, "Maximum Permissible Radiation
Exposures to Man," NBS Tech. News Bui.
41, 17 (Feb. 1957).
48. National Council on Radiation Protec- ,
tion and Measurement, "Basic Radiation
Protection Criteria," NCRP Report No.
39, NCRP Publication, Washington, D.C.
'Jan. 15, 1971,..
49. G. E. McMurtrle (Secretary), "Permissi-
ble Doses Conference held at Chalk
River, Ontario (Sept. 1949)," Report
RM-10 (May 1950).
50. International Commission on Radiologi-
cal Protection, "Recommendations of the
International Commission on Radiologi-
cal Protection (Adopted September 17,
1965)," ICRP Publ. 9. Pergamon Press,
Oxford, 1966.
51. International Commission on Radiologi-
cal Protection, "RadlosensiLtivity and
Spatial Distribution of Dose, Reports
Prepared by Two Task Groups of Commit-
i tee 1 of the International Commission
on Radiological Protection," ICRP
Publ. 14 (Pergmon Prsss, Oxford, 1969.
52. J. E. Ballou, D. K. Craig, j': F. Park,
H. A. Ragan, and C. L. Sanders, Pacific
Northwest Laboratory Annual-Report for
19'7.2, Vol. 1, Part 1 BNWL-1750 Pt I,
April 1973.
53- Passonneau, et al., "Carcinogenic Ef-
fects of Diffuse and Point-Source Beta
Irradiation on Rat Skin: Final Summary,"
AEC Document ANL-4932, 1952.
54. P. N. Dean and W. H. Langham, "Tumor-
igenicity of Small Highly Radioactive
Particles," Health Phys. 16:79-84
(1969). —
55. R. E. Albert, F. J. Burns, and R. D.
Heimbach, "The Effect of Penetration
Depth of Electron Radiation on Skin
Tumor Formation in.the Rat," Rad. Res.
20.:515-524 (1967).
56. A. M. Brues, "Comparative Chronic Tox-
icities of Radium and Plutonium,"
Argonne National Laboratory Quarterly
Report (Fe., March and April 1951)'
ANL-4625,. p. 106-124.
57. Federal Radiation Council, "Guidance
for the Control of Radiation Hazards
in Uranium Mining," Report No. 8 Re-
vised, U.S. Government Printing Office,
Washington, D.C., Sept. 1967.
58. F. E. Lundln, Jr., J. K, Wagoner, and
. V. E. Archer, "Radon Daughter Exposure
...and Respiratory Cancer Quantitative and
' 'Temporal Aspects," National Inst. for
99
-------
358
Occ. Safety and Health and National 59. W. H. Langham, "Biological Consldera-
Inst. of Environ. Health Sciences, tlons of Nonnuclear Incidents Involving
Joint Monograph No. 1 (1971). Nuclear Warheads," Lawrence Radiation
Laboratory, Document UCRL-50639,
April 1969.
CM:530(260)
tt Ul OOVIRNMINT PKINTINO OffICI. 1*74 — TM-MI/1?
100
-------
LA-5810-MS
Informal Report
359
UC-41andUC-48
Reporting Date: November 1974
Issued: November 1974
it,-
A Review of the Natural Resources Defense
Council Petition Concerning Limits for
Insoluble Alpha Emitters
by
J. W. Healy
C. R. Richmond*
E. C. Anderson
I'l
'Present title and address: Associate Director for Biomedical and En-
vironmental Sciences, Oak Ridge National Laboratory, Oak Ridge,
TN 37830.
lelontlffle laboratory
of th» University of California
1 LOS ALAMOS, NIW MIXICO 17544
UNITKD tTATM
ATOMIC CNHRflV COMMIMJON
CONTRACT W-740S-BNO. >•
-------
360
In the interest of prompt distribution, this LAMS report was not
edited by the Technical Information staff.
ll
Printed in the United States of America. Available from
National Technical Information Service
U.S. Department of Commerce
5285 Port Royal Road
Springfield, VA 22151
Price: Printed Copy $4.00 Microfiche $2.25
Th* rnporl ww prepare* an na account al work ipoMOrad by th» United
Slau. &,,.,„„.„, NMh., Ih. U»Ml State .« Ih. UiuM Stow.
Momic Tiuiqr Comm.™,™!. nai an| ol Ih.u .mplo,^, .01 anr ol \h.,I
contn.clori. .ubc.mUa, ICH. ol IK.,, .mplofrM. mol~ ao, wonanlr. ••
po» ..r implinl. 01 v-»m« „„, Ugal UbJIlT of r«pcm«bd,t, lot III* oc
cur
-------
A REVIEW OF THE NATURAL RESOURCES DEFENSE COUNCIL PETITION
CONCERNING LIMITS FOR INSOLUBLE ALPHA EMITTERS
361
by
J. W. Healy, C. R. Richmond, and E. C. Anderson
The interpretations of the potential effects of insoluble alpha-emitting
particles in the lung, as described in the document supporting the Natural
Resources Defense Council petition of February 14, 1974, are reviewed in
light of present evidence. It is concluded that the theories upon which the
proposal is based are not in accord with the evidence and that the theories do
not correctly predict .the outcome of experiments actually using such particles.
I. INTRODUCTION
On February 14, 1974, the Natural Resources
Defense Council (NRDC) submitted a petition to the
U. S. Atomic Energy Commission (AEC) and the
Environmental Protection Agency (EPA) requesting
that they amend their standards as said standards
apply to insoluble particles of plutonlum and other
alpha-emitting "hot particles." (The terminology
of "hot particles" is that of the NRDC and refers
to particles which contain more than 0.07 pCi of
insoluble alpha emitters.) In support of their
petition, the NRDC included a report by Drs. Arthur
R. Tamplin and Thomas B. Cochran which provides the
basis for the proposal.
The question of the possible biological effects
from radioactive particles which ca.^\irradiate small
quantities of tissue to large physical doses has
been of interest to the scientific community and
radiation protection groups for many years. In sev-
eral studies involving large extrapolations of avail-
able data, an enhanced tumor production from numbers
3 4
of such particles has been predicted. ' However,
the tenuous nature of the evidence and the indirect
methods of arriving at the answer have, in general,
prevented these predictions from gaining acceptance
in the blomedical community, and the standards have
continued to be based upon other evidence.
In view of the current Interest in this ques-
tion and the somewhat unusual procedure of submitting
the proposal through legal channels rather than
through scientific review, It was felt that an
examination of the allegations and conclusions would
be useful in informing those concerned as to the
validity of the bases. This report, therefore, re-
views in some detail the basis for the NRDC proposal
and briefly indicates the experimental information
available on the question.
II. THE CONTENTION
While it is difficult to condense the arguments
of an author without running the risk of changing his
meaning or emphasis, we will briefly summarize in
this section, for the orientation of the reader, our
understanding of this contention. However, it is
urged that reference be made to the original doc-
2
ument to obtain their full viewpoint. It is our
impression that the following are the key technical
items upon which the petition is based.
1. The responsible standards-setting organiza-
tions, the International Commission on Radiological
Protection (ICRP) and the National Council on Radia-
tion Protection (NCRP), have1given no guidance on
the question of localized radiation dose resulting
from an alpha-emitting particle.
2. In Tamplin and Cochran's words, the Geesa-
man hypothesis indicates that "when a critical '
architectural unit of a tissue (e.g., a hair fol-
licle) is irradiated at a sufficiently high dosage,
the chance of it becoming cancerous is approximately
10 to 10 ." The Geesaman hypothesis was pub-
lished in 1968 in a Lawrence Radiation Laboratory
report (now Lawrence Livermore Laboratory) but
was never published in the open literature. In
this.'theory, Geesaman relied upon a theoretical
-------
stlgation of the dose distribution around a par-
ticle in the lung and estimated sizes above which
cell death would result in no cancer. In an adden-
dum, he used data on the induction of tumors in rat
skin and the relation of these to atrophied hair
follices as a result of radiation. Perhaps his con-
clusions can best be stated by quoting from the con-
clusions section of the addendum.
"Summing up, intense radiation exposure of
mammalian skin and lung tissue commonly results in
cancers. Tissue injury and disturbance are a pri-
mary consequence of Intense radiation insult, and
are observed in association with carcinogenesis.
Albert has exhibited a simple proportionality between
skin carcinoma and atrophied hair foillcles. No
i* ;
general description of precarcinogenic injury exists,
but in a crude sense the available observations are
compatible with the idea of an injury-mediated
carcinogenesis. Cancer is a frequent instability of
tissue. Since tissue is more than an aggregate of
cells, and has a structural and functional unity of
its own, it would not be surprising if some dis-
rupted local integrity, a disturbed ordering, com-
prises a primary pathway of carcinogenesis. The
induction of sarcomas with inertj discs of Mylar,
cellophane, Teflon, and Millipore is indicative that
such a mechanism exists. Presumably mitotic steril-
ization is an important factor in any carcinogenesis
mediated by radiation-induced tissue injury. The
functional relation of this factor to the carcinogenic
response may be quite different from a linearity in
the surviving mitotic fraction. .-,'
"While regrettably unquantitative, the hypoth-
esis of an injury-mediated carcinogenesis is sugges-
tively descriptive. If the respiratory zone of the
lung contains a structure analogous to the rat hair
follicle, and if a radioactive participate deposited
in the respiratory zone has the capacity to disrupt
one or more of these structures and create a pre-
cancerous lesion, then cancer risks of the order of
—3 -4
10 and 10 per particle can be expected for bur-
8
dens much less than 10 particles."
Again, however, the reader is urged to review
the original document to obtain the full argument.
3. In deriving present limits for alpha
emitters in the lung, Tamplin and Cochran indicate
that no factor was Included to account for the non-
uniform distribution of radiation In the lung as is
done in the ICRP and NCRP formulation of bone dosim
etry. It was pointed out that such a distribution
factor could be defined by:
DF
number of cancers (non-uniform distribution)
number of cancers (uniform distribution)
"Since direct experimental evidence are not avail-
2
able....," they chose to attempt a definition of
this factor from the Geesaman hypothesis including
the quantitative derivation of probability of can-
cer Induction derived from rat skin hair follicles.
A. As regards human data, they discuss the
case of a skin lesion from plutonium embedded in the
epidermis; a purported case of synovial sarcoma due
to contamination during handling of a carboy; the
Los Alamos cases which date back to the Manhattan
Project and are dismissed as not having received
particles of sufficient activity; and a group of
exposed Rocky Flats workers which are, again, dis-
missed on the grounds that the time since exposure
has not been long enough for cancer to develop. In
the first case, the statement of the pathologist
that "their similarity to known precancerous epi-
dermal cytological changes, of course, raised the
question of the ultimate fate of such a lesion "
seems to be interpreted as proof that cancer would
have developed. In the second case, a series of
circumstantial inferences is quoted to "prove" that
the cancer was due to plutonium.
5. Since the Geesaman hypothesis, as given in
his earlier reports, seems to have no dependence of
effect on radiation dose or amount of activity per
particle but states that the effect is due to the
number of particles, Tamplin and Cochran modify this
hypothesis by establishing a critical particle size
below which the effect will not be noted (i.e., a
threshold?). Their basis is given by the following
2
quotations:
"Not all particles would be expected to result
in these high cancer probabilities. As the particle
size or specific activity per particle is reduced so
is the dosage to the surrounding tissue. Indeed,
at sufficiently small particle size or specific ac-
tivity, one would expect the radiation insult to
behave similar to uniform irradiation. The study of
Albert on induction of cancer in rat skin indicates
a precipitous change in the dose response curve as
the dosage exceeds 1,000 rem. This suggests
-------
363
that a particular level of tissue damage must occur
before this unique carcinogenic response occurs.
The experiments of Laskln et al. indicate a signif-
icant carcinogenic response in the lung at 1400 rem,
suggesting a comparable sensitivity of lung tissue.
Geesaman indicates that the tissue repair time in
the lung is of the order of one year. It there-
fore seems appropriate, but not necessarily conser-
vative, to accept as guidance that this enhanced
cancer risk occurs when particles irradiate the sur-
rounding lung tissue at a dose rate of 1000 rem/yr
or more ...... using Ceesamun's lung model, a par-
ticle with an alpha activity between 0.02 pCi and
0.14 pCi is required to give a dosfe of 1000 rem/yr
to irradiated lung&lssue. For purposes of estab-
lishing a maximum permissible lung particle burden
we will use 0.07 pCi from long half-lived (greater
than one year) isotopes as the limiting alpha activ-
it^ to qualify as a hot particle."
Reference 55 in the above quotation is to Al-
6
8 9
bert et al.\ reference 56 to Laslcin et al.; and
reference 57 to Geesaman.
6. From their definition of a "hot particle,"
Tamplin and Cochran derived values for occupational
exposure by comparing the risk of lung cancer from
dose rates of 15 rems/yr to the lung to assumed
risks from particles of 1/1000, 1/2000, and 1/10 000
per particle. They then recommended as " ..... a some-
what arbitrary compromise and ..... not the most
conservative value ..... " the use of a risk of
1/2000 per hot particle in determining the maximum
permissible lung burden for insoluble alpha-emitting
radionuclides in hot particles. From this they
arrived at a value of 2 particles or 0.14 pCi for a
reduction in the maximum permissible lung burden by
a factor of 115 000. •,
For individual members of the public, a value
of 0.2 hot particle, while recognizing the dis-
parity in risk occasioned by a fractional number of
particles per person, Is recommended along with a
value of 0.07 hpt particle as the average lung bur-
den for members of the public. Limiting values for
soil contamination and accidents are also derived
by similar considerations.
III. PARTICLES AND RADIATION DOSE
The origin of the NRDC proposal lies in the
very non-uniform radiation dose to the tissue
surrounding a radioactive particle. For this reason,
we will initially provide some description of the
nature of this non-uniformity and the application of
the concept of radiation dose to biological problems.
A. The Radiation Dose around a Particle
The unique feature of a particulate source of
radioactive material (particularly for an alpha
•
-------
abscissa would be distance.) The calculations are
239
for a particle of 0.28 pCl of Pu In tissues of
two different densities. It is assumed that the
energy loss per unit path length is constant so that
the alpha particle deposits energy uniformly along
its path. The range in unit density tissue is taken
as 40 yrn, with the range for other tissues scaled
to the tissue density. The doses given are annual
doses averaged over the volume of tissue given.
The curve indicated as density - 1 is calculated for
unit density tissue, and the curve for density » 0.12
is for a uniform tissue having a density of 0.12, cor-
responding to the average bulk density of Geeaaman's
lung model at half Inflation. No correction was
made for the self-absorption in the particle, al-
though this should be negligible for these small
PuCK particles in comparison to the errors caused by
other assumptions. The annual doses are given both
In rads which can be converted to rams by the con-
12
ventionally used quality factor of 10. It must be
emphasized that this conversion to terns is partic-
ularly uncertain for this case, since there are no
data which can be used to assess the relative effects
of alpha radiation and the reference radiation in
this particular geometry of Irradiation.
Figure 1 is intended to indicate the wide varia-
tion in dose which can be calculated by different
assumptions of averaging volume. Even here we have
minimized the dose to individual cel,ls by plotting
the average over the volume to the fraction of the
range considered. The dose to an individual cell at
differing distances varies even more than this aver-
age. •
We have not considered in this calculation the
photon dose from x rays or infrequent gamma rays
2^8 ") ^Q
from either Pu or Pu, since the focus of the
discussion Is on alpha-particle effects. It should
be noted, however, that these photons are more pene-
trating and will result In lower doses at distances
beyond the range of the alpha particles. ,
B. Limitations on the Usefulness of Radiation Dose
Calculations such as those given In the preced-
ing section are Interesting and have been made by
various Individuals for many years. The question
remains as to their usefulness and meaning in assess-
ing a biological problem.
The primary use of radiation dose, In practice,
is as a physical parameter to be used in correlating
and extrapolating experimental data on biological
effects on an empirical basis. Thus, the present
limits for radiation exposure are based upon observa-
tions of effects in humans for whom the dose has
been estimated. There is no a priori, basis for
assigning an effect to a given dose, since our
understanding of the basic mechanisms of radiation
if
carcinogenesis and the Influence of cellular inter-
actions is completely inadequate. Thus, radiation
doses are meaningful only when related to empirical
data on the outcome. .As a corollary, the further
one extrapolates from the experimental conditions
under which the dose-effect relationship is measured,
the greater the uncertainty. Thus, predicting the
behavior of the effects on individual cells or ag-
gregates of cells in a functioning organ from in
vitro studies in cell culture is a very wide extrap-
olation which ignores the very different environment
of the cells in the organ and the potential inter-
actions which occur among cells. (Such in vitro
studies, however, are of great interest for other
reasons, such as studies of the mechanisms of damage
at the cellular level.) Similarly, extrapolating
from the effects of a partial organ Irradiation to
a full organ (or vice versa) can lead to a mis-
estimate. It is for these reasons that .nest sci-
entists have refrained from using dose calculations,
such as those given earlier, to arrive at conclu-
sions as to the effect of radioactive particles but
have preferred to depend upon experimental evidence
which bears more directly on the actual conditions.
A further factor of importance In the use of
physical dose as a correlating concept is the exact
method of expression of dose. That is, if a cor-
relation with effect is established using one method
of calculating the dose, it is not valid to apply
this correlation if another basis for dose calcula-
tion is chosen. As an illustration which, inci-
dentally, seems pertinent to the problem at hand,
Vaughan indicates that 90% of the ionization alon'g
an alpha particle track formed in unit density tis-
sue is contained in a cylinder of 0.01-ym radius
with the axis of the cylinder along the track. For
an alpha particle with 5.15-MeV initial energy, the
range is about 40 ym. The average dose to this
limited volume, therefore, is about 6 x 10 rads,
with even higher average doses for smaller radii
and at the peak of the Bragg curve. For a 1000-g
-------
organ of unit density tissue, the current occupa-
tional limit of 1.5 rads (15 reins) per year, even
assuming homogeneous distribution of the alpha
tracks, means that about 0.25 mm of tissue is ir-
radiated to doses above 4 x 10 rads, or if a dose
of 1000 rads were chosen, a volume of some 1500 mm .
Since unit density tissue was chosen for this illus-
tration, the results do not compare with those for
a particle using the Geesaman model. However, it
is clear that even a "homogeneous" distribution of
alpha radiation through a body of tissue results in
considerable non-uniformity in dose distribution.
Further, for the example chosen, one could express
the limits as 15 rems to the 1000 g of tissue or as
a limitation on t)h£ volume of tissue exceeding a
given dose. For example, no more than 0.3 mm of
tissue shall exceed 4 x 10 rems or no more than
1500 mm shall exceed 10 000 rems. Although the lat-
ter methods of expression involve numbers that are
frighteningly high in more normal context, all three
methods define the same total energy deposition.
However, note that it would be highly improper to
apply the 15-rems value to the dose along the track
just as it would be improper to apply the dose along
the track to the dose arising from an assumption of
uniform tissue distribution.
A specific point in the Tamplin-Cochran dis-
2
sertation is the use of the "distribution factor"
(DF) in calculating the dose in rems for internal
emitters and is supported by the fact that a DF of
5 is used in calculating the dose for bone. They
then indicate that a DF should lie applied to lung.
However, it must be realized that a dose calculation
was not used to arrive at the present maximum per-
14
missible body burden for plutonium. Instead, a
comparison of biological effects (primarily on bone)
was made between plutonium and radium. On the basis
of these data, it was deduced that plutonium in the
body'is 2.5 times as harmful as radium on a micro-
curie basis. Since the maximum permissible body
burden for radium had been established from studies
of humans as 0.1 uCi, the maximum permissible body
burden for plutonium was set at 0.04 uCi.
The dose considerations quoted by Tamplln and
Cochran arose in an attempt to use these experiments,
and others with strontium, to provide a physical
formulation of the results which could be used for
extrapolation to other bone-seekers. For the
365
purpose of such calculations, it was assumed that
radium was uniformly distributed in bone. Further,
it was assumed that 90%, or essentially all, of the
plutonium in the body was. in bone. Since the indi-
vidual plutonium disintegration liberated about half
of the alpha energy of one disintegration of radium
with its accompanying daughter products, the fore-
going damage ratio 'of 2.5 on a microcurie basis be-
comes 5 on an average energy-delivered (dose) basis. '
The key to this comparison lies in the assump-
tions. We know, for example, that radium is not
uniformly distributed in bone. In fact, if any-
thing, It is more non-uniformly distributed than
plutonium. However, the deposition sites are dif-
ferent from those of radium so that the plutonium
affects a different, and more sensitive, portion of
the bone. One could presumably eliminate the con-
fusion caused by the distribution factor by re-
defining the critical organ to include only the sen-
sitive portion of the bone and comparing the dose
to this region from plutonium and radium. We also
note in passing that the more, recent examination of
the distribution of plutonium in animals indicates
that .only about 40 to 50% of the plutonium is in the
bone.L If this were true in the comparison animals
(as seems likely), then the actual distribution fac-
tor for bone calculations should be 10 rather than 5.
We have introduced this rather lengthy dis-
cussion on bone dose calculations to indicate, once
again, the difficulty in applying dose calculations
and concepts derived for one use to a different prob-
lem without full understanding of what was done. In
the .above case, the salient feature is that radium
is non-uniformly deposited so that some sections of
the bone receive doses orders of magnitude greater
than others. The distribution factor is not in-
tended to indicate greater localized dose from
plutonium but, rather, that the distribution in bone
is different from that of radium on a gross basis.
C. Previous Guidance
An interesting point in the Tamplin-Cochran
document is: "It is important to recognize that the
ICRP has given no guidance with respect to non-
uniform irradiation of the lung by Insoluble alpha-
emitters such as insoluble plutonium particles."
They then quote one of many statements made by the
16
ICRP and other groups which indicate that there is
no, clear evidence as to whether the effect of the
-------
366
V ~ non-homogeneous dose is greater or less than that of
the homogeneous dose. They Interpret this statement
as: "In effect, the ICRP is saying that, there la no
guidance....." A quote from the NCRP follows con-
cerning the significant volume of tissue which con-
cludes: " For example, if a single particle of
radioactive material fixed in either lung or -lymph
node might be carcinogenic, the averaging of dose
either over the lung or even over one cubic centi-
meter may have little to do with thla case."12
While we do not feel that it la useful to quote
such bodies at length, there Is evidence that the
problem has been considered since the early days of
the derivation of limits. One of Jthe earlier stata-
17
ments arose from a fri-Partite Conference in 1949
at which scientists from tha United Kingdom, Canada,
and the United States were arriving at the conclu-
sions which ware later applied by many of thaaa same
peeple in the ICRP and NCRP recommendations I "In
relation to tha possible pathological affects of \
radioactive particles in tha lungs, Dr. Hamilton
pointed out that tha cells in the immediate neigh-
borhood of a dust particle containing 1 or 2X of
Plutonium would be subjected to a dose of about
400 r/day. Tha general opinibn which emerged from
the discussion waa that the carcinogenic effect per
unit volume is probably considerably lass for the
Irradiation of small masses of tissue than for
large." This conclusion undoubtedly affected the
practice of calculating dose aa'the average doaa to
an organ at that time and comprises definite guid-
ance on the handling of such probjlVms. However, the
matter did not rest there, since several national and
international groups continued investigation from
that time to the present, with frequent statements
as to the lack of definitive -Information. 16>18~21
However, in spite of the Indications of periodic
questioning and reviews, there has been no reviaion
in tha practlcaa which they recommended of using the
averaga organ dose as a baais for establishing
standards, 1
From tha above, it seems clear that the ICRP
and tha NCRP did furnish guidance on tha pertinent
,dose to be used for standards-setting! the use of
an average calculated dose to an organ, with full
recognition of tha non-uniform distribution of dosa
around tha particle. In spite of numerous reviews
of the question over the intervening years, they
have reiterated this guidance by not changing it.
It la difficult to support any claim of no guidance
in view of this record on the part of bodies which
have traditionally been In the forefront of recog-
nizing potential problems (i.e., genetic effects)
and providing generally conservative recommenda-
tions.
12
One recommendation of the NCRP (while per-
haps not completely applicable to the particle case
as is shown by their example situation quoted
earlier) Is of interest when combined with Geesa-
man's estimate of a particle size above which can-
c;
car would not be expected due to cell death." Tha
NCR? statement is, "Simplifications in practice
hinge largely on reporting a single representative
protection dose for a limiting organ system even
when (he actual irradiation la grossly non-uniform.
The representative dose is taken as the highest that
can be obtained by averaging over a prescribed sig-
nificant volume. The implication of this concept
is that any redistribution of a given dose '
within such a volume does not materially altar tha
radiation response. It is usually assumed that tha
'significant volume' should be of the order of one
cubic centimeter. This will be groasly conservative
under moat circumstances, and in special situations
use of a larger volume is justified." It is not
clear why the NCR? recommended a significant volume
rather than a significant maas, since this results
in averaging over a smaller mass in the lung than 'in
other tissues due to the density difference.
However, if we calculate the dose over 1 cm
of lung tissue with an average density of 0.12 g/cm
for the "hot particle" of 0.07 pCi derived by
• 2
Tamplin and Cochran, we obtain a dose of only
0.055 red or 0.55 rem per year. Thus, one would re-
quire an activity of 1.9 pCi to reach the limit of
15 rema per year for this single cubic centimeter of
tissue (or an activity of 15 pCi for a single cubic
centimeter of unit density tissue). Geesaman ,quotes
an activity for a 1-pm-diameter particle of Pu aa
60 pCi and arrives at a conclusion that " unless
tha source site, s, is smaller than or of the order
of 0.25 u the yearly flux will be lethal for all
epithelial populations in tha exposed volume. The
source sice condition will only be slightly -less
stringent for endothelial populatlona s < 0,35 y."
The Implication of tha above is that no cancer will
-------
367
develop for particles larger than those described
since the cells are killed. According to the con-
stants used by Geesaman, a 0.25-ym particle would
have an activity of about 2.5 pCi, which compares
with the 2 pCi to give 15 rems to one cubic centi-
meter of tissue. Thus, if Tamplin and Cochran had
chosen to use this available NCRP guidance along
with the Geesaman study, their conclusions would
have been considerably different,
IV. THE GEESAMAN HYPOTHESIS
The Geesaman hypothesis was published us a
Lawrence Radiation Laboratory (now Lawrence Liver-
•i11 5
more Laboratory) report in February 1968, with
an addendum in October 1968 containing the quan-
i
tltatlve estimates of cancer production. This work
has never been published In the open scientific lit-
erature but remains an unrevlewed and unrefereed
'study.
Since his conclusions eeem to be baaed pri-
marily upon the studies of follicular oncer pro-
duced in rat skin, we quote below those sections of
the report in which he uses these data with his
references and footnotes deleted.
"Albert's study of radiation-Induced carcinoma
in rat skin gives some quantitative description of
a high-dose carcinogenic situation. Since such
descriptions are rare, and since Albert's results
have implications to risk analysis In general, his
experiment is outlined here.
"A skin area of 24 cm was exposed to electron
radiation with various depths df maximum penetra-
tion In all cases the response scale at
sufficiently high doses was large, ~ 1 to 5 tumors
per rat at 80 weeks after exposure. It was noted
by Albert that when the dose was normalized to a
skin depth of 0.27 mm, the three response curves
became continuous. Since this depth is near the
base of the hair follicle which comprises the deep-
est reservoir of epithelial cells of the germinal
layer, it was. suggestive that this might be a crit-
ical region in the observed carcinogenesis, The
suggestion gained significance from the observation
that most of the tumors are similar to hair fol-
licles, and that In Che nonulcerogenic dose range
the nunibei t>£ tumors per rat was in nearly constant
ratio i":,2000 to 1/4000) with the number of atro-
phied hair follicles Thu.s che carcinogenesis
in this experiment was remarkably correlated with
the dose to and the specific damage of a particular
skin structure. When exposures were made with
stripe and sieve patterns of roughly 1-mm scale,
geometrical effects were observed; most notably the
cancer induction in the sieve geometry was sup-
pressed at doses of 1700 R, but not at doses of
2300 R. The reduction, however, was again consis-
tent with the reduction in damage as characterized
by atrophied hair follicles.
"For perspective it Is valuable to relate these
observations to cellular descriptions, Carcino-
genesis in Albert's experiment is maximum in the
neighborhood of 2000 R. It is well documented -in
vitro and to a lesser extent in vivo that the frac-
tion of mltotically competent cells as measured by
clonal formation decreases in a nearly exponential
fashion with the dose. From these results a surviv-
ing mltotic fraction of approximately 10 would be
expected in a population of germinal epithelial cells
exposed to 2000 R. Even in this pre-ulcerative dose
regime the cell population suffers severe mitotlc
injury. It is significant that Albert's dose
response curves show no simple relationship with the
surviving fraction of mltotically competent epi-
thelial cells. There is certainly no exponential
decrease of the response in the neighborhood of D^,
and, in fact, the tumorigenesls is maximum in a dose
region where the population of mltotically compe-
tent cells should be Initially depleted by about
5 orders of magnitude.
"To summarize this important experiment, a high
incidence of cancer was observed after intense local
doses of radiation, and the carcinogenesis was pro-
portional to the damage or disordering of a partic-
ular skin structure."
The reasoning leading from this Information,
plus a discussion of other experiments with high
doses and particle sources leading to the conclusion
-3 1 -4
(quoted earlier) of a cancer risk of 10 to 10
per particle, is not given but Is presumed to result
from the correlation with atrophied hair follicles
from Albert's experiments.
There is a similarity between this work and
the theory propounded by Virchow in 1863 that the
cause of cancer is chronic tissue damage. This
•'We are indebted to Dr. Roy E. Albert, New York
University, for this line of reasoning.
-------
theory was disproved by experiments which showed
that cancer can be produced by very potent sub-
stances that vary widely in their capacity to cause
cancer, whereas many agents which cause damage do
not cause cancer. Thus, while there is a frequent
association between tissue damage and cancer, there
are types of cancer and types of damage for which no
association exists.
There are several aspects of the data from the
skin experiments used by Geesaman, as well as in-
formation published later from the same series of
experiments, which should force some modification
of the proposal but are not included in the Tamplin-
Cochran document. These and their implications for
the Geesaman hypothesis 'are reviewed below.
t
A. Type of Tumor
In a 1961 paper, Albert et al. first explored
the tumors resulting from irradiation of rat skin
with Y beta rays. Two strains of rats were used
with the tumor types and frequencies as given in
Table I. They indicate the Holtzman strain to be
similar to the Sprague-Dawley strain, but the ani-
mals were considerably older (~ 40 weeks compared
to ~ 20 weeks for the Sprague-Dawley).
A variety of tumor types were obtained. In
Fig. 2, we have plotted the dose-incidence curve
34567
Sur|ac« DOM (kradc)
6 9 |0
Fig. 2.
Tumor Incidence per animal vs surface dose
of electrons: ( ) Sprague-Dawley strain;
( ) Holtzman strain; (-0-) adnexal tumors;
and (-•-) other tumors.
for both strains for the predominant tumor type
(follicle and sebaceous or "adnexal") and the sum of
all other types. The Incidences were corrected for
the unidentified tumors by assuming these to arise
in "the same proportion as the identified ones. It
is of interest to note the wide disparity between
the response curves of the adnexal tumors and those
of other types, as well as the disparity between the
curves for the two strains (whether due to strain or
age is not determined). Since the remainder of the
experiments focused upon the adnexal tumo-s, with
TABLE I
Sprague-Dawlev Strain
Initial number of rats
Epldermold carcinoma
Adnexal tumor
Connective tissue tumor
Squamous papllloma
Cysts
No pathologic examination
Total
Holtzman Strain
Initial number of Tats
Epldermoid carcinoma
Adnexal tumor
Connective tissue tumor
Squamous papilloma
Cysts
No pathologic examination
Total
8
TUMOR TYPES AND FREQUENCIES FROM IRRADIATION OF RAT SKIN
Dose (rads)
10 000
12
9
5
2
0
0
_8
24
7200
n 12
11
2
1
0
0
_5
19
7200
9
7
2
0
2
0
_3
14
4870
13
6
26
0
6
1
_8
•• 47
6000
10
6
7
0
0
0
_4
17
3750
14
5
62
1
6
2
17
93
5000
8
1
6
0
0
0
_3
10
2500
15
5
23
1
3
0
19
51
4000
11
2
11
0
0
0
_3
;'i6
1900
10
1
3
1
0
0
_0
5
2000
16
0
2
0
0
0
_0
2
1225
15
0
1
1
0
0
_2
4
1000
20
0
0
0
0
0
_0
0
950
23
0
3
0
, 0
2
_0
5
500
50
0
1
1
0
0
_1
3
470
25
0
3
1
0
1
0
5
230
24
0
1
0
0
1
_0
2
-------
data) on other types discarded, the information is
aimed at a very specific tumor type even for the
organ considered: rat skin.
B. Volume of Irradiated Tissue
As was discussed earlier, the extrapolation
from one condition of irradiation or method of ex-
pressing dose to another must be done with great
caution and a full understanding of the parameters
involved. How, then, do the conditions of the rat
skin experiments compare with those of the particle
irradiation?
The particle doses typically involve tissue
quantities of tens of micrograms (see Fig. 1). In
the rat skin experiments, areas ranging from about
5 to 30 cm2 were used with depths from about 0.4 to
about 1.5 mm. Thlis, the tissue volumes ranged from
about 0.2 to about 5 cm or, for unit density tis-
sue, 0.2 to 5 g.8'23"25 This is an extrapolation in
tissue volume on the order of 10 to 10 .
t There are several observations in the rat skin
experiments which are pertinent to the validity of
extrapolation. In one series of irradiations, expo-
sures were made through two grids which provided
1-mm-wide bars of irradiation area with one grid
masking all except a third of the area and the other
I 23
all except a sixth of the area. In addition, a
mask (sieve) with circular holes which permitted an
exposed area of a third of the uniform area was used.
From these data, it was noted that the response with
the smaller areas was lower even though the total
dose to the area (expressed in gram-rads) was in the
vicinity of the uniform dose required to produce the
maximum incidence of adnexal turiors. In other words,
the delivery of a specific., amount of energy to a
given overall area of skin resulted in fewer tumors
when the energy was delivered at higher doses but to
smaller subareas. Geesaman correctly points out that
this suppression occurred at 1700 rads but not at
2300 rads.6 However, the 2300-rads value for the
uniform irradiation is well past the dose of maximum
tumor induction, and there has been a significant
drop in the incidence for this condition. Therefore,
it is difficult to attribute this effect to other
than the oversaturation of the response. Albert et
> al. conclude from this work: "The experiments re-
ported here indicate that, in a limited dose range,
the non-uniform radiation pattern has the effect of
reducing both chronic hair follicle damage and tumor
23
formation.
369
In the studies of the association between hai
follicle damage and tumor formation, Albert et at.
noted that the damage to the hair follicles across
the irradiated area waa not uniform, with the major
damage occurring at the center of the area and con-
24
siderably lower damage at the edges. From other
data, it appears that the dose across the area was
reasonably uniform and that the effect was due to
'•J:
something other than non-uniform dose. From this
24 i
and the preceding work, Albert et al. conclude:
"Two observations indicate the importance of the
size of the ir.radiated area on the magnitude of
hair damage: (1) the follicles along the margin of
the irradiated area are relatively uninjured com-
pared to the follicles in the center of the ir-
radiated area (2) there is a suppression of
follicle damage when the irradiation is delivered
in a sieve pattern These observations strongly
suggest that the pathogenic mechanisms for the
development of both irreparable hair follicle damage
and skin tumors depend upon both the dose and the
amount of skin irradiated" (emphasis added) .
Thus, the data and conclusions in the papers
used by Geesaman to justify his work (and quoted by
TampJLin and Cochran as "biological evidence" sup-
porting their contentions) strongly suggest that
extrapolations to smaller tissue volumes may not be
legitimate.
C. Species Dependence
We have alluded earlier to the difference in
response curves for skin tumor formation occasioned
by either the strain difference or the age of the
rats used. In a paper subsequent to the Geesaman
25
proposal, Albert et al. repeated some of their
studies using mice as the experimental animal, since
it had been noted that the response of mouse skin
Is different, with relatively few tumors and most
tumors being epidermoid carcinomas rather than ad-
nexal tumors.
The results of this experiment confirmed the
previous findings that adnexal tumors, noted as the
most probable outcome in rats, were rare in mice and
that the total number of tumors produced in mice was
only 15 to 20% of those in rats for comparable con-
ditions . The lack of adnexal tumors was attributed
to the fact that the hair follicles in the mouse
are more radiosensitive than those in the rat. As a
result, little follicle atrophy is noted in the
-------
370
mouse — either the follicles remain intact or they
are destroyed.
The results of this experiment indicate clearly
the difficulties of applying results from one organ
to another. Even though skin was the target in both
cases, the differences in structure between rat skin
and mouse skin caused a completely different outcome
upon irradiation. The outcome upon comparison to a
different organ such as the lung, where follicle
structures or functions do not even exist, would
seem to make the final conclusion by Geesaman one of
sheer speculation.
D. Volume of Follicle Irradiated
In the original studies of rat skin1'response,
Albert et al. used electron beams which had an ap-
proximate linear decrease in dose with depth. >22"2^
The relation between dose at the tip of the hair
follicle, lying at a depth of about 3 mm, was estab-
lished by" noting that the tumor incidence curves for
electrons of various penetrations coincided when the
dose was expressed as the dose at a depth of
Q
0.3 mm. However, it can be noted that the entire
follicle was irradiated to this dose or greater.
To test the dependence of the effect of doses
to various portions of the follicle, Heimbach et al.
used the Bragg peak of alpha radiation produced by a
*yf
cyclotron. The energy of a 37-MeV alpha beam was
adjusted by the use of aluminum absorbers in the
experiments so that the Bragg peak fell at depths of
0.12, 0.35, and 0.55 mm; Since the Bragg peak can
produce dose rates up* to 5 times that along the
early portion of the track, this enabled investiga-
tion cf doses delivered to various parts of the
follicle. The results indicated that the response
curves coincided when the dose was expressed as
minimum close to any point along the h.air follicle.
The tumor types were identical with those found with
electrons, and there was once again a correlation
between tumors and atrophied hair follicles, with
the ratio between tumors and atrophied hair fol-
licles of about 1/9000.
From this experiment, the authors concluded
that the entire hair follicle must be irradiated to
produce tumors. The minimum penetration alpha radia-
tion used did not irradiate the lowest part of the
follicle and did not induce tumors. The authors
then suggested: "The findings reported here can be
explained on the basis that the hair follicle is
reparable from cells originating at any point along
its length, and that the capacity for such repair is
inversely related to the degree of damage sustained
by the part of the follicle minimally damaged. The
existence of a 'critical depth' in skin of about
0.3 mm which was demonstrated with electron radia-
tion can be explained on the basis that the
'I:
follicle tips, which received the minimum dose to
the follicles, were the most protected part of the
skin epithelium and, therefore, contained the crit-
ical reservoir of cells for replacing the more
superficial and more heavily irradiated cells."
Since the hair follicle is a few tenths milli-
meters long (several hundred pm) and the range of an
alpha particle is about 50 urn, these results strongly
suggest that a single alpha-emitting particle, even
if it could be placed in rat skin, would not produce
tumors. Thus, in the statement of the Geesaman
hypothesis, "If the respiratory zone of the lung
contains a structure analogous to the rat hair fol-
licle, and if a radioactive particle deposited in
the respiratory zone has the capacity to disrupt one
or more of these structures then cancer risks
of the order, of 10 to 10 per particle can be
expected." The second conditional clause does not
follow unless the first is modified to further re-
define the hypothetical structure to a size where
it will be fully irradiated by the particle (i.e.,
less than ~ 100 urn). A further necessary condition
is that such structures be located throughout the
lung with such a frequency that the particle will
irradiate one with a probability approaching unity.
This appears to be stretching an already tenuous
theory beyond the realm of credibility.
V. THE TAMPLIN-COCHRAN APPLICATION
In the Tamplin-Cochran interpretation of the
2
Geesaman work, they introduce the concept of a
"critical architectural unit" in the following pass-
age: "Now what are these experiments trying to tell
us? Certainly a reasonable interpretation of these
experimental results is: when a critical architec-
tural unit of a tissue (e.g., a hair follicle) is
irradiated at a sufficiently high dosage, the chance
of it becoming cancerous is approximately 10 to
-4
10 . This has become known £s the 'Geesaman hy-
pothesis '."
10
-------
i
There are significant differences, however, in
the statement by Geesaman and that quoted above.
Geesaman states his theory as conditional: i.e.,
"If the respiratory zone contains a structure
analogous to the rat hair follicle " Thus, in
the Tamplin-Cochran version there is a progression
from "if" to "when," with no evidence or attempt to
indicate whut this critical architectural unit may
be. Further, they imply that any hair follicle
will be a "critical architectural unit," while
Geesaman carefully refers to structures " anal-
OKOIIU t'.o the rut Imlr rolllclu," Wu liuvu noon
earlier that mouse skin hair follicles do not fit
the Geesaman description, since they are not anal-
ogous in their response.
The second part of Geesaman's conditional
statement indicates that " if a radioactive par-
ticulate deposited in the respiratory zone has the
capacity to disrupt one or more of these structures
and create a precancerous lesion " has been
changed to indicate that when the structure is
" irradiated at a sufficiently high dosage, the
chance of it becoming cancerous is approximately
_o _A o
10 to 10 ." Thus, the hypothetical statement
of the possibility of disruption and cancer forma-
tion has become, in translation, a statement of
fact.
It is of interest that Tamplin and Cochran use
the same probability of cancer formation for par-
ticles deposited in the lung that Geesaman states
for the condition that the particle actually ir-
radiates the hypothetical structure. We can deduce
from this something of the character of this sup-
posed structure. From Table III of the Tamplin-
Cochran report, the mass of tissue irradiated to
1000 rems per year around a 0.07-pCi particle is
65 yg with the lung at half-inflation. Geesaman,
for this condition and his cubical lattice lung
model', estimates the range of an alpha particle to
be between 335 and 1000 urn, depending upon the path
through the lattice. The experiments with alpha
particles and rat hair follicles indicate that the
full "analogous structure" must be irradiated,
,which can only occur if the 65 yg of tissue surrounds
the particle. Thus, we can conclude that the struc-
ture has a mass of 65 yg or less, since the probabil-
ity of the particle lodging at the center would seem
to be low. From the Tamplin-Cochran assumption that
371
the probability of cancer for a particle lodged in
the deep respiratory zone is the same as Geesaman*s
probability assuming the structure to be irradiated
and damaged, it is apparent that the number and
spacings of the structures must be assumed to be
such that each particle will irradiate one. (Other-
wise, the probability of the particle lodging close
enough to irrudlaui the structure must bo Included
In their estimates.) In a 1000-g lung, there must
be greater than 10 such structures, each of which
weighs ICHH than 65 yg. 11: uppearw from llilo Lypu
of tiHtlinuLu LluiL llif "critical an:hl lucliirul unit"
is any group of cells rathur than an identified
structure, as is implied by the comparison with the
hair follicle.
The second change in interpretation intro-
duced by Tamplin and Cochran is the minimum activity
of a particle to produce cancer. This could log-
ically follow from Geesaman's second conditional
statement concerning the ability of the radiation to
disrupt one or more of the structures. However,
the consequences of introducing such a threshold on
the radiation response when the entire lung is ir-
radiated are of interest. If one irradiates the
full lung, obviously all of the hypothetical struc-
tures will be irradiated. If one assumes the dis-
ruption of these structures to be the sole cause of
radiation-induced cancer and there were more than
1000 to 10 000 such sites in the lung, then the
incidence would remain at zero until the threshold
dose (1000 rems) was reached. The incidence would
then increase rapidly above this to 100% or greater.
If there are fewer than this number of sites (with
-3 -4
a probability of 10 to 10 of producing cancer
per site when irradiated), then obviously the prob-
ability of a particle Irradiating the site must be
included. There may be causes of radiation-induced
cancer other than the mechanism of tissue disrup-
tion. These could result in a gradual increase in
incidence below the threshold, but the response
from the architectural unit mechanism postulated
would still increase to 100% when the threshold is
exceeded. This pattern does not conform to any
known data on cancer incidence dose-effect rela-
tions for full lung irradiation.
It Is of interest that the Tamplin-Cochran
interpretations of the theory receive only minimal,
i'i[ any, justifications. For example, there is no
11
-------
372
attempt to identify the structure in the lung
responsible for the effect, nor is it explained how
one can extrapolate from the effects on a hair fol-
licle to the effects in a lung which contains no
unit even similar in function or structure to the
hair follicle and sebaceous gland of the rat skin.
Data on these tumors and their incidence, which
have appeared since the original Geesaman postula-
ticn and which throw considerable light on the
hypothesis, have been Ignored. It can only be con-
cluded that a more thorough and comprehensive study
could have changed the conclusions of the document.
VI. THE HUMAN DATA , ''
People have been dxfrosed tc plutonium during
various uses of the material over the past 30 years.
Tamplin and Cochran have chosen a few of these expe-
riences, some to discount on the basis of their
threshold theory and others to support their conten-
tion. Although we profess no special knowledge in
the field of medicine, we will analyze their conten-
tions on the basis of biological and health physics
experience.
A. The Lushbaugh Report
In 1962, Lushbaugh and Langham reported on a
lesion associated with plutonium in a wound. The
patient, while machining plutonium metal, received a
wound which was later excised. Some A years after
the accident, he noticed a nodule wh,lch, upon meas-
urement, still contained some 0.08 ug of plutonium
T
the q
leal examination of the lesion, and the quotation
appearing in the Tamplin-Cochran report arose from
this paper: "The autoradiographs showed precise
confinement of alpha tracks to the area of maximum
damage and their penetration into 'the basal areas of
the epidermis, where epithelial change! typical of
Ionizing radiation exposure were present. The cause
and effect relationship of .these findings, there-
fore, seemed obvious. Although, the lesion was.'
minute, the changes"in It were severe. Their sim-
ilarity to knaan pf»-aano»rottB epidamal .aytologio
dhangee, of course, raised the question of the ulti-
mate) fate of such a lesion should it be allowed to
exist without surgical Intervention" (emphasis
added). Following this quotation, Tamplin and
Cochran indicated Chat " less than 0,1 yg of Pu-
239 produced pre-cancerous changes In human tissue."
They refer several sentences later to "this
pre-cancerous lesion " and state that this
239
proves that a single Fu particle " ir-
radiates a significant (critical) volume of tissue
and Is capable of producing cancer." In other words,
they manage, in the space of a few sentences, to
move from " similarity to known pre-cancerous
f
epidermal cytologic changes....." and expressed un-
certainty on the part of the pathologist on the
eventual outcome to a conclusion that cancer will
result. We believe .that the uncertainty expressed
by the expert should be given proper weight in the
conclusion.
In point of fact, examination of the autoradlo-
graph In the Lushbaugh paper indicates very clearly
that the lesion contained a number of small par-
ticles, since several points of origin of alpha par-
ticle "stars" can be discerned^ Further,-' the author
Indicates the lesion containing the plutonium had a
volume of 27 x 10 cm or, for unit density tissue,
a mass of some 27 yg. Reference to Fig. 1 would
indicate that a single particle would deliver an
alpha dose to only about 0.3 Pg in unit density tis-
sue. A
In a Subsequent paper, Lushbaugh et al. de-
scribe the result of the study of 8 auc'.i lesions
resulting from plutonium in wounds in which the
plutonium had resided for periods of time ranging
from 0.5 to 8 years. They Indicate, "The lesions
were found to vary morphologically in an orderly
manner related roughly to the length of time the
plutonium had been present. All were confined to
the dermis. The size of the nodule depended on the
dispersion of the particles present rather than the
duration of the lesion. The largest nodule was about
2 mm in greatest dimension." They conclude in the
discussion, "Although this study Is based on too few
small lesions to evoke much confidence In these
retrospective interpretations, the concluaions may
be warranted that metallic plutonium implanted In
the skin In minute amounts elicits a foreign-body
reaction of granulooatous type, which after subsid-
ing In cellular activity becomes flbromatous." No
reference is made in this paper to cancerous or
similarity to pre-cancerous lesions.
These lesions are the most severe changes which
have been reported in humans as a result of pluto-
nium arid, as such, require the question of wound
12
-------
373
contamination to be taken seriously in radiation
protection programs. However, to extrapolate these
to cancers, in view of the uncertainty on outcome
expressed by the pathologist, and especially to
extrapolate to lung cancer seems to be an unjusti-
fiable step.
B. The Gleason Case
The information available to the authors on the
Gleason case is primarily that presented by
Dr. Arthur R. Tamplin in the appendix of the Tamplin-
2
Cochran document. This involves the case of an
individual who handled a crate containing a leaking
239
carboy of Pu solution and later developed a
synovial sarcoma ,4.f the left hand.
In the initial analysis of this case, Tamplin
indicates that the occurrence of this type of cancer
is less than the total skin cancer death rate, since
t)he prognosis for this type of cancer is poor. He
concludes, "Thus it is highly unlikely that anyone -
who handled this crate would spontaneously develop
this sarcoma on the contaminated hand " This,
of course, is not the question of interest, since
the a priori condition that cancer did develop is
given and the question is now whether there is evi-
dence that indicates whether the plutonium was
involved. Tamplin introduces evidence from animals
239
that injection of 1 yg of Pu into the skin of
28
rats produced fibrosarcomas in 5% of the animals.
The relevance of this information appears remote,
since these tumors were of a different type and
arose from different tissues thin1 the synovial sar-
coma. (This is similar to the extrapolation from
follicular tumors in the rat skin to lung tumors in
the humans.) We know of no evidence, nor do Tamplin
and Cochran produce any, that this type of tumor
has been produced by radiation. However, in view of
the ubiquitous nature of radiation as a carcinogenic
agent, it would appear as a definite possibility
providing that the proper critical tissue is ir-
radiated (presumably the synovial membrane or the
synoid capsule). It would appear that this would
require something other than an injection into the
, dermis. Thus, the question to be examined is
whether there is a reasonable probability that
plutonium could have penetrated to the.critical
tissue under the conditions of the purported expo-
sure .
Early in the discussion, Tamplin states:
"There is little reason to doubt that this small
amount of liquid (0.01 milliliter) or even more
found its way below the surface of Mr. Gleason's
palm" (emphasis added). It is our experience that
plutonium does not "find" its way through skin,
even though there \a water exchange across the skin.
The skin has been shown to be an excellent barrier
29
to prevent the passage of many materials, includ-
ing plutonium. Thus, some mechanism such as a
break In the skin (wound) must be postulated and of
such a depth and location that the critical tissue
Is involved.
The Incident occurred on January 8, 1963.
According to the Tamplin account, a survey was con-
ducted on Mr. Gleason's home, clothing, and auto-
mobile on January 19, 1963. The results apparently
were negative, or they would have been mentioned. It
is indicated earlier when referring to Mr. Gleason's
handling of the crate: "This could not have occurred
without contaminating the palmar surface of his left
hand, which was bare." It is difficult to see why
the contamination should preferentially go to the
left'-band. Other portions of the body and the shoes
presumably would also be susceptible. However, if a
sufficient quantity to deposit 0.1 yCi (0.01 ml of a
160-yg/ml solution) were on the left hand, experience
has indicated that such contamination transfers
rapidly to other objects, including clothing and
items handled such as tools or even the automobile
steering wheel. The fact that these surveys, even
11 days later, did not detect significant contamina-
tion would Indicate that not much was initially
present.
Tamplin further indicates that urine samples
collected subsequent to January 20 gave negative
results and, "The only thing that this demonstrates
is that no detectable level of Pu-239 was found."
Later he Indicates that negative findings in1the
feces and urine were obtained in April 1970 and,
again, dismisses the results on the grounds that
little is absorbed Into the body. The latter con-
clusion is, of course, dependent upon the type of
material used. As an illustration of a worst case,
Johnson et ol. injected plutonium oxide particles
with a count mean diameter of 7 Um subcutaneously
•Into dogs. They found that the translocation to
13
-------
374
the body occurred rapidly, with on the order of
0.25% of the plutonium recovered from other tissues.
Assuming this very low translocation of PuO. to
32
apply to the nitrate and using Langham's equations
for the excretion, we find that, for the 0.1 uCi
postulated by Tamplin, urine samples should have
indicated on the order of 0.2 disintegration per
minute in the period around January 20. This level
is easily detectable by adequate analysis. Of
greater applicability to the soluble nitrate case
is a wound described by Schofield et al. Here the
material was plutonium oxalate, and they estimated
that, without treatment, about 0.1% of the material
in the wound would have been excreted in the 10- to
20-day period and 0.085S'in the 20- to 30-day period.
For a postulated wound burden of 0.1 uCi of this
soluble material, one would expect, therefore, on
the order of 20 disintegrations per minute per day
excretion in the urine or some 200 to 1000 times the
detectable level for most analyses. The later anal-
yses are also significant in that they indicate the
lack of a source of relatively insoluble material
continually leaching into the blood.
The physical examination by Dr. Roy Albert
seems to be significant in several respects. While
the details are not given, there is no mention of a
wound or other break in the skin through which pluto-
nium could enter. Further, the solution was un-
doubtedly very acidic to retain the plutonium in
solution. Such shipments are usually made in nitric
acid. There is no indication given that the medical
examination showed any signs of acid reaction with
the skin. (Nitric acid can produce a yellow dis-
coloration even when no overt burn occurs.) In a
later conclusion, Tamplin Indicates that the deposi-
tion ".....may have occurred through a small cut or
via a sliver," One can only speculate on the size
of cut required to introduce the plutonium in a
position to irradiate the critical tissue, but it is
Important to note that the medical examinations
which presumably Included questioning of Mr. Gleason,
did not reveal any Indication of such a wound or
sliver, (Tamplin presumably is referring to a con-
taminated sliver of material other than that of the
carboy, since there is no indication that it was
broken,)
From the above evidence, we can only conclude
that the association between cancer and plutonium
is speculation. The subject did handle the carboy,
but subsequent examinations showed no contamination,
and urine and medical history provided no indication
of plutonium deposition.
C. The Los Alamos Cases
In referring to the exposures of 25 individuals
exposed to plutonium some 30 years ago during the
Manhattan Project, Tamplin and Cochran indicated
that the exposures were to Insoluble plutonium and,
hence, of interest. However, they discount this
experience on the grounds that 14 of the 25 subjects
worked in plutonium recovery operations and were
exposed to droplets of plutonyl nitrate: "A droplet
1 u in diameter (0.5 u ) would therefore contain
-4
only 6 x 10 pCi compared with a 0.07 pCi particle
of PuO,." However, no justification is given for
the assumed drop size, which appears to be very
small based on attempts to produce particles by
evaporating droplets from a nebulizer. For compar-
ison, fog has a particle size of 5 to 50 ym and
mists of 50 to 100 urn. If we assume the particles
to be the size of fog particles, then the plutonium
content would range from 0,16 to 160 pCi — well
within the, range of the definition of the "hot par-
ticle."
A summary of particle size measure-erica for
various operations using plutonium is given in Ta-
ble II.35'36
The aerosol from the Rocky Flats fire was gen-
erated by high-temperature condensation of PuO, in a
manner perhaps not unlike fume formation in the war-
time reduction processes. In addition, it is sim-
ilar to those aerosols measured at the Los Alamos
Scientific Laboratory in connection with the opera-
tions of fluorlnatlon and reduction. The lathe
operation is not typical of the wartime operations,
and the resuspension aerosol from cleanup is quite
different from the others, although this distribu-
tion undoubtedly occurred during the wartime expo-
sure. As a beet estimate of the aerosol involved
in the Los Alamos exposures, we have considered the
0.32-vim mass median diameter (HMD) with a o of
1.83 pm, along with the estimates of deposition in
these individuals.
For,* 1-um-diamater droplet containing 40 g/llter
of Z39Pu with a specific activity of 0.0614 Ci/g
but st.ill assuming unit density for the solution, we
obtainil.3 x 10"3 pCi.
14
-------
TABLE II
PARTICLE SIZE MEASUREMENTS FOR PLUTONIUM OPERATIONS
Source
Rocky Flats Fire
Fluorination of Nitrate
Reduction to Metal
Lathe Operation
Cleanup
Mass Median Diameter
JLffll
Diameter greater than 0.6 ym.
Geometrical Standard
Deviation, a (urn)
0.32
0.45
0.32
0.26
1.90
— — a
1.83
1.55 .if
1.62
1.44
1.80
375
Mass Fraction as
"Hot Particles"8
0.15
0.23
0.10
0.01
0.97
,!',' TABLE III
ESTIMATED "HOT PARTICLE" BURDENS OF LOS ALAMOS WORKERS
Diameter (ym) Incremental Mass Fraction Activity (PCi/Particl.O Activity (nCi/man) Particles (per man)
0.6 - 0.7
I
0.7 - 0.8
0.8 - 0.9
0.9 - 1.0
1.0 - 1.2
1.2 - 1.4
1.4 - 1.8
0.05
0.033
0.022
0.015
0.015
0.007
0.0057
0.09
a.14
0.20
0.28
0.44
0.72
1.34
20.0
13.2
8.8
5.9
5.9
2.8
2.3
2.22 x 10
9.4 x 104
4.3 x 104
2.2 x 104
1.4 x 10 4
3.9 x 103
1.7 x 103
The number of "hot particles" from an aerosol
of this distribution was calculated by numerical
integration in given particle siziI ranges above
0.6 ym. It was further considered that the total
of 2.5 yCi of plutonium in these 25 men was 10 yCi
at the time of exposure to allow for subsequent
elimination. On this basis, t,he total number of
particles in various size ranges is given in Ta-
ble III.
The process of pulmonary deposition would not
significantly distort the deposition in this range
since, for more than 905! of the mass range'rep-
resented, the pulmonary deposition fraction varies
only in the ranges of 0.2 to 0.32. Thus, if the
lung cancer per particle estimate of 10~3 to 10~4
given by Geesaman were valid, we would expect some
1000 to 10 000 lung cancers in this group. Exposure
has been for-30 years, so that a significant portion
of the lifetime has passed with no cancers develop-
ing.
Total
4.0 x 10
37
In a recent study, Mclnroy et at. measured
the distribution of plutonium particle size in a
lymph node of a deceased worker by the autoradio-
graphic technique. Although this individual was
exposed at a later time than those discussed above,
it is of interest that these estimates also indi-
cated that 15% of the plutonium was in particles
larger than 0.07 pCi.
D. The Rocky Flats Workers
Tamplin and Cochran discuss the 25 individuals
exposed to plutonium during a fire in 1965.35 'ihey
compare the lung burdens in these individuals with
the lung burdens in the beagles which developed lung
cancer by noting, " it is significant to note
that in the experiments reported by Park et al., the
beagle dog with the smallest lung burden, i.e.,
0.2 yCi, developed lung cancer. The highest burden
in Table V is comparable to the lowest beagle expo-
sure; the lowest exposure ...'.., the 19 cases with
lung burdens in the 0.24 uCi range, are only an
15
-------
376
order of magnitude less than the lowest beagle ex-
posure." The fact that they are, In this case,
using microcuries rather than numbers of particles
leads to the conclusion that they are referring to
radiation dose to the lung, yet they neglect to point
out the difference in size between the beagle lung
and the human lung — a factor which would make the
human dose about an order of magnitude lower than
that of the dog with a comparable burden.
It is of passing interest that the lack of can-
cer in these Rocky Flats workers is dismissed on the
grounds that only 9 years have passed, which is not
f
adequate to produce cancer. We concur In this
statement but note that1 Tamplin argues strongly for
the production of a synovial sarcoma, in spite of
the lack of evidence of exposure, in a matter of a
few years after the incident. (Times are not given
in his report, but the accident occurred in 1963
and the report of Dr. Wald, referred to by Tamplin
and Cochran, was submitted in 1973, indicating that
the cancer was well developed by this time.)
VII. EVIDENCE ON PARTICLE DOSE EpECTS
As was indicated in an earlier section, those
groups charged with providing safe limits for radia-
tion exposure have consistently utilized the average
dose to an organ as a basis for the limiting quan-
tity of radioactive material. That ,1s, the dose is
calculated as though the energy were uniformly dis-
tributed through the organ. In the earliest of
these recommendations, the opinion was undoubtedly
based upon meager direct evidence plus the know-
ledge of radiation biology of those involved, and
cautions as to the uncertainty of the procedure were
appropriate (and still are, since'full and complete
data will require some years to accumulate) . How-
ever, as evidence has accumulated, such cautions
refer to a much narrower range of uncertainty. It
is the purpose of this section of the report to
summarize briefly seme of the more pertinent informa-
tion which .can be used in assessing the question of
particle dose but is not Included in the Tamplin-
Cochran document.
Two reviews on the question of particle dose
OQ OQ *1O
have appeared in the past year. ' The first
focused on the general question of whether the non-
uniform dose distribution in an organ is more or
less hazardous than the uniform distribution (i.e.,
in Tamplln-Cochran's -appraisal, Is the distribution
factor appropriate to the partlculate situation
greater or less than one?). The conclusion, from the
evidence available at that time was " that the
preponderance of the evidence indicates that the use
of an average lung dose is appropriate in limiting
.if
exposures and may well be conservative." The second
review was a more complete examination of all of the
information available on plutonium and other iso-
topes in the lung, with emphasis on the particle
question. The conclusion of this review was similar
to that of the first. We will not, here, pursue
again all of the evidence but will provide a brief
description of some of the pertinent results. While
these experiments are selected because of the way in
which they illustrate the results, we would also
note that neither of the reviews found evidence
which indicated the particle dose to be more harmful
than the uniform dose.
Little et aZ.*0'*1 administered 21°Po (an alpha
emitter) intratracheally to hamste^rs both with and
without iron oxide. The administration with iron
produced agglomerations (effectively particles) of
the Po on the iron oxide particles, while the
administration without iron produced a nore uniform
distribution as was shown by autoradiographs.
Sanders performed experiments with inhalations of
238 239
both PuO and PuO prepared in the same manner
238
in rats. The PuO. behaved in such a manner that
it appeared to be more soluble and provided a more
homogeneous dose to the lung. Both of these exper-
iments led to the conclusion that the homogeneous
distribution is more effective in producing cancer
than the partlculate distribution (i.e., the DP for
the particulate is less than l") . Dolphin quotes
Lafuma as reporting " greater toxic effects
including cancer in rats following deposition of
curium-242 in lungs compared with equal amounts of
plutonlum-239 activity. This he attributes to the
diffuse nature of the curium deposit and the par-
tlculate nature of the plutonium, as shown by auto-
radiographs ."
In studies with beta emitters in the lung,
44
Cember concluded, " the carcinogenlclty of a
given amount of absorbed radiation energy Increases
up to a point, as the absorption of the energy IB
spread'out, both time- and space-wise. From a prac-
tical point of view, this means that, for a given
16
-------
377
total amount of absorbed energy, low-level, con-
tinuous exposure of the total lung may be more
carcinogenic than the same amount of energy de-
livered acutely to a restricted volume." Thus,
there is evidence that the same effect may be true
for beta radiations.
Current experiments at the Los Alamos Scien-
tific Laboratory provide a direct test of the Geesa-
man theory in that the particles are carried to the
lung by the bloodstream and are lodged in immobile
positions in the capillaries. Here they are in
position to irradiate the surrounding tissue in pat-
terns little, if at all, different from those ad-
ministered by inhalation or intratradically. How-
ever, they do not agglomerate or move about so that
the results can be ascribed to a fixed particle and
45
the dosimetry examined. In the first experiment,
. 238
particles of PuO. of 180-ym diameter were used
in rats. Although a lesion similar to the one de-
scribed by Lushbaugh developed, it did not affect
the well-being of the animal, and no cancers de-
veloped in 32 animals sacrificed from 120 to 400 days
after implantation or in a group of 6 animals allowed
to live out their lifetime. It is estimated that the
radiation energy from this particle, if averaged
over the lung of the latter 6 animals, would have
delivered a dose of 2 500 000 rads (or 25 000 000
rems). Such a dose to the full lung would have caused
very early death and is many orders of magnitude
above that at which increased incidence of cancer is
noted.
In an experiment currently in progress, '
uniform-sized mlcrospheres (10-urn-diameter) of ZrO_
are used with intermixed PuO to provide particles
of differing activities, and' these are introduced
into the lungs of hamsters by the above technique.
In the first study in this experiment, 8 groups of
60 animals each were injected with 2000 such par-
ticles, with the plutonium content of each particle
ranging from O.07 to 59.4 pCi. Essentially all of
animals have now died, with only two lung cancers
observed. (Three other cancers in the exposed ani-
mals occurred in organs other than the lung.) The
dose rates to the lungs of those animals, when cal-
culated as the average dose to the lung, ranged
from 13 rads per year (130 rems per year) to 12 000
rads per year (120 000 rems per year). This is a
range over which one would expect high tumor
incidence and, in fact, premature death from pul-
monary inefficiency if the material had been dis-
tributed homogeneously. Since the survival curves
of the individual groups did not differ from those
of the controls and the total tumor incidence was
low, one can only conclude that the DF for plutonium
in particulate form must be less than one. In the
continuation of this study, some 1900 hamsters have
Q / Q
received 1.6 x 10 microspheres. As of October
*
1974, the minimum time of exposure has been 50 weeks,
which is comparable to or longer than the tumor
induction times observed by Little et al. in their
210
experiments with more uniformly distributed Po.
In fact, only three lung tumors (including the two
observed in the first study) have, as yet, developed
from the microsphere exposures. While this study is
as yet incomplete, the very low tumor incidence
again indicates a low effectiveness of the particles
in inducing lung cancers as compared to more homo-
geneously distributed alpha emitters, as well as the
failure of the Geesaman hypothesis to correctly fore-
cast the results of this experiment.
VIII.: DISCUSSION
There appear to be few further conclusions
which can be drawn. The preceding review has indi-
cated that the Tamplin-Cochran conclusions are based
upon a hypothesis which requires considerable
extrapolation of the data upon which it is based.
Later evidence, of the same nature as was used in
the derivation (i.e., rat skin data), does not sup-
port the assumptions of the original model. The
Tamplin-Cochran interpretation of the model not only
fails to take into account the later evidence but
appears to present the hypothesis as fact. The
supporting evidence on human data which they present
are based upon unsupported assumptions and distor-
tions of the words of the authors they quote. Most
importantly, they fail to use or acknowledge direct
evidence on the effect of radioactive particles.
Such evidence indicates that the basic damage model
which they use overestimates badly the carcinogenic
effects of radioactive particles. We conclude,
Reference 48 indicates that " by the spring of
1974 " these exposures had been attained. The
intent was to Indicate progress to the time of prep-
aration of the paper. The administrations were
actually completed in September 1973.
17
-------
378
therefore, that the application of the average organ
dose to the establishment of limits is still appro-
priate, although experimentation to narrow existing
uncertainties on the effects of non-uniform dose
distribution should continue.
REFERENCES
1. Natural Resources Defense Council, "Petition to
Amend Radiation Protection Standards as They
Apply to Hot Particles," submitted to the U. S,
Atomic Energy Commiasion and the Environmental
Protection Agency (February 14, 1974).
2. A. R. Tamplin and I. B. Cochran, "Radiation
Standards for Hot Particles. A Report on the
Inadequacy of Existing Radiation Protection
Standards Related to Internal Exposure of Han
to Insoluble Particles of Plutonium and Other
Alpha-Emitting Hot Particles," Natural Resources
Defense Council, 1710 N Street, N. W., Washing-
ton i D. C. (February 14, 1974).
3. P. N. Dean and W. H. Langham, "Tumorigenicity of
Small Highly Radioactive Particles," Health Phys.
16, 79-84 (1969).
4. J. 8. Coleman and L. S. Perez, Jr., "Considera-
tions of a Tumor Probability Function and Micro-
Dosimetry for the Deep Lung," Part II of Final
Report of Radiological Safety ^tudies for the
SNAP Program for Safety Branch, SEPO, USAEC,
Environmental Safeguards Division, NUS Corpora-
tion report NUS-596, Rockville, Md. (1969).
5. D. P. Geesaman, "An Analysis of the Carcino-
genic Risk from an Insoluble Alpha-Emitting
Aerosol Deposited in Deep Respiratory Tissue,"
Lawrence Radiation Laboratory report UCRL-
50387 (February 9, 1968).
6. D. P. Geesaman, "An Analysis of th4 (Carcinogenic
Risk from an Insoluble Alpha-Emitting Aerosol
Deposited In Deep Respiratory Tissue: Adden-
dum," Lawrence Radiation Laboratory report UCRL-
50387 (October 9, 1968).
7. C. C. Lushbaugh and J, Langham,, "A Dermal Lesion
from Implanted Plutonium," Arch! Dermatol. 86,
461-464 (1962).
8. R. E. Albert, F. J. Burns, and R. D. Helmbach,
"The Effect of Penetration Depth of Electron
Radiation on Skin Tumor Formation in the Rat,"
Radiation Res. 30, 515-524 (1967). (
9. S. Laskin, M. Kuschner, N. Nelson, B. Altshuler,
J. H. Harley, and M. Daniels, "Carcinoma of the
Lung in Rats Exposed to the 3-Radiation of
Intrabronchial Ruthenium106 Pellets. I. Dose-
Response Relationships," J. Natl. Cancer Inst.
31, 219-231 (1963).
10.
11.
12.
13.
14.
15.
16.
17.
18.
19.
20.
E. C. Anderson and P. N. Dean, "Effects of
Internal Radiation on Living Organisms (Hot
Particle Program). Doslmetry," in Annual
Report of the Biomedical and Environmental
Research Program of the LASL Health Division,
January through December 1973, Los Alamos Sci-
entific Laboratory report LA-5633-PR (1974).
D. E. Lea, "Actions of Radiations on Living
Cells," The MacMillan Company, New York
(1947).
National Council on Radiation Protection and
Measurements, "Basic Radiation Protection Cri-
teria," NCRP Publication 39, Washington, D. C.
(January 15, 1971).
J. Vaughan, "Distribution, Excretion and
Effects of Plutonium as a Bone-Seeker," in
Handbook of Experimental Pharmacology. Uranium.
Plutonium. Transplutonic Elements (H. C. Hodge,
J. N. Stannard, and J. B. Hursh, eds.),
Springer-Verlag, New York-Heidelberg-Berlin
(1973). ;
W. H. Langham and J. W. Healy, "Maximum Permis-
sible Body Burdens and Concentrations of Pluto-
nium. Biological Basis and History of Develop-
ment," in Handbook of Experimental Pharmacology.
Uranium. Plutonium, Transplutonic Elements
(H. C. Hodge, J. N. Stannard, and J. B. Hursh,
eds.), Springer-Verlag, New York-Heidelberg-
Berlin, (1973) .
R. D. Evans, "The Effect of Skeletally De-
posited Alpha-Ray Emitters in Man," Brit. J.
Radiol. 39_, 468; 881-895 (1966).
International Commission on Radiological Protec-
tion, "Recommendations of the International
Commission on Radiological Protection (Adopted
September 17, 1965)," ICRP Publication 9,
Pergamon Press, Oxford (1966).
G. E. McMurtrie (Secretary), "Permissible Doses
Conference Held at Chalk River, Ontario (Septem-
ber 1949)," Report RM-10 (May 1950).
National Committee on Radiation Protection,
"Maximum Permissible Amounts of Radioisotopes
in the Human Body and Maximum Permissible Con-
centrations in Air and Water," National Bureau
of Standards Handbook 52, U. S. Department of
Commerce, Washington, D. C. (March 20, 1953).
International Commission on Radiological Protec-
tion, "Radiosensitivity and Spatial Distribu-
tion of Dose," ICRP Publication 14, Pergamon
Press, Oxford (1969).
Subcommittee on Inhalation Hazards, Committee
on Pathologic Effects of Atomic Radiation,
"Effects of Inhaled Radioactive Particles,"
National Academy of Sciences-National Research
Council Publication 848, Washington, D. C.
(1961).
18
-------
21.
Advisory Committee on the Biological Effects of
Ionizing Radiation, Division of Medical Sci-
ences, National Academy of Sciences-National
Research Council, "The Effects on Populations
of Exposure to Low Levels of Ionizing Radia-
tion," Washington, D. C. (November 1972).
R. E. Albert, W. Newman, and B. Altshuler,
"The Dose-Response Relationships of Beta-Ray-
Induced Skin Tumors in the Rat," Radiation Res.
15, 410-430 (1961) .
R. E. Albert, F. J. Burns, and R. D. Heimbach,
"Skin Damage and Tumor Formation from Grid and
Sieve Patterns of Electron and Beta Radiation
in the Rat," Radiation Res. 30. 525-540 (1962).
R. E. Albert, F. J. Burns, and R. D. Heimbach,
"The Association between Chronic Radiation
Damage of the Hair Follicles,' and Tumor Forma-
tion in the Rat," Radiation Res. 30, 590-599
(1967). i,", ~
i
R. E. Albert, F. J. Burns, and P. Dermott,
"Radiation-Induced Hair-Follicle Damage and
Tumor Formation in Mouse and Rat Skin," J.
Natl. Cancer lost. 49(4). 1131-1137 (1972).
R. D. Heimbach, F. J. Burns, and R. E. Albert, •
"An Evaluation by Alpha-Particle Bragg Peak
Radiation of the Critical Depth in the Rat Skin
for Tumor Induction," Radiation Res. 39, 332-
344 (1969). —
C. C. Lushbaugh, R. J. Cloutier, G. Humason,
J. Langham, and S. Guzajc, "Histopathologic
Study of Intradermal Plutonium Metal Deposits:
Their Conjectured Fate," Ann. N. Y. Acad. Sci
145, 791-797 (1967).
H. Lisco, M. P. Finkel, and A. M. Brues,
"Carcinogenic Properties of Radioactive Fission
Products and of Plutonium," Radiology 49(3)
361-363 (1974). '
29. R. T. Tregear, "Physical Functions of Skin,"
Academic Press, Inc., New Yijitk (1966).
379
22.
23.
24.
25.
I
26.
27.
28.
30.
31.
32.
W. D. Oakley and R. C,' Thompson, "Further
Studies on Percutaneous Absorption of Plutonium
Solutions in Rats," in Biology Research-Annual
Report 1955. Hanford Atomic Products Operation
report HW-41500 (February 1956).
L. J. Johnson, R. L. Walters, J. L. Lebel,
C. R. Lagerquist, and S. E. Hammond, "The Dis-
tribution of Pu and Am: Subcutaneous Admin-
istration of PuO, and the Effect of Chelation
Therapy," in Radiobiology of Plutonium (B. J.
Stover and W. S. S. Jee, eds.), J. Wi Press,
Salt Lake ,City, Utah (1972) .
W. H. Langham, S. H. Bassett, P. S. Harris,
and R. E. Carter, "Distribution and Excretion
of Plutonium Administered Intravenously to
Man," Los Alamos Scientific Laboratory report
LA-1151 (September 20, 1950).
33. G. B. Schofield, H. Howells, F. Ward, J. C.
Lynn, and G. W. Dolphin, "Assessment and
Management of a Plutonium Contaminated Wound
Case," Health Phys. 26, 541-554 (1974).
34. L. H. Hempelmann, C. R. Richmond, and G. L.
Voelz, "A Twenty-Seven Year Study of Selected
Los Alamos Plutonium Workers," Los Alamos
Scientific Laboratory report LA-5148-MS
(January 1973).
•j-
35. J. R. Mann and A. R. Kirchner, "Evaluation of
Lung Burden following Acute Inhalations of
Highly Insoluble PuO " Health Phys. 13, 877-
882 (1967). l —
36. W. D. Moss, E. C. Hyatt, and H. F. Schulte,
"Particle Size Studies on Plutonium Aerosols,"
Health Phys. 5_, 212-218 (1961).
37.
38.
39.
40.
J. F. Mclnroy, M. W. Stewart, and W. D. Moss,
"Studies of Plutonium in Human Tracheobronchial
Lymph Nodes," in Proceedings of the Conference
on Radiation and the Lymphatic System, Battelle-
Northwest Laboratories, Richland, Washington
(September 30-October 4, 1974), in press.
J. W. Healy, "A Proposed Interim Standard for
Plutonium in Soils," Los Alamos Scientific
Laboratory report LA-5483-MS (January 1974).
W. J. Bair, C. R. Richmond, and B. B. Wach-
holz, "An Assessment of "Spatial Distribution of
Radiation Dose Relative to Inhalation of Radio-
nuclides," U. S. Atomic Energy Commission
report WASH-1320 (September 1974).
J. B. Little, B. N. Grossman, and W. F. O'Toole,
"Respiratory Carcinogenesis in Hamsters Induced
by Polonium-210 Alpha Radiation and Benzo(a)-
Pyrene," in Morphology of Experimental Respi-
ratory Carcinogenesis (P. Netteshelm, M. G.
Hanna, Jr., and J. W. Deatherage, Jr., eds.),
AEC Symposium Series 21, U. S. Atomic Energy
Commission report CONF-700501 (1970), Office
of Information Services, Springfield, Va.
J. B. Little, B. N. Grossman, and W. F. O'Toole,
"Factors Influencing the Induction of Lung
Cancer in Hamsters by Intratracheal Administra-
tion of 10Po," in Radionuclide Carcinogenesis
(C. L. Sanders, R. H. Busch, J. E. Ballou, and
D. D. Mahlum, eds.),'AEC Symposium Series 29,
U. S. Atomic Energy Commission report CONF-
720505 (1973), Office of Information Services
Springfield, Va.
42. C. L. Sanders, "Carcinogenicity of Inhaled
Plutonium-238 from Crushed Microspheres,f in
Pacific Northwest Laboratories Annual Report
1972, Battelle-Northwest Laboratories report
BNWL-1750, Part 1 (1973), p. 28.
43. G. W. Dolphin, "Hot Particles," National
Radiological Protection Board, Radiological
Protection Bulletin 8, Harwell, Didcot,
Berkshire, England (July 1974).
41.
19
-------
380
A4. H. Cember, "Radiogenic Lung Cancer," Prog. Exp.
Tumor Res. 4_, 251-305, Hafner Publishing Co.,
Inc., New York (1964).
45. C. R. Richmond, J. Langham, and R. S. Stone,
"Biological Response to Small Discrete Highly
Radioactive Sources. II. Morphogenesis of
Microleaions in Rat Lungs from Intravenously.
Injected 238PuO, Microspheres," Health Phys.
18, 401-408 (1970).
46. C. R. Richmond and G. L. Voelz, eds., "Annual
Report of the Biological and Medical Research
Group (H-4) of the LASL Health Division,
January through December 1972," Los Alamos
Scientific Laboratory report LA-5227-PR (March
1973).
47. C. R. Richmond and E. M. Sullivan, eds.,
"Annual Report of the Biomedlcal and Environ-
mental Research Program of the LASL Health
Division, January through December 1973," Los
Alamos Scientific Laboratory report LA-5633-PR
(May 1974).
48. E. C. Anderson, L. M. Holland, J. R. Prine, and
C. R. Richmond, "Lung Irradiation with Static
Plutonium Microspheaes," in Experimental Lung
Cancer, Careinogenesis and Bloassays, Springer-
Verlag, New York-Heidelberg-Berlin, CONF-
740648-1 (1974), in press.
40:736(280)
20
-------
LA-5483-MS
381
INFORMAL REPORT
A Proposed Interim Standard for
Plutonium in Soils
•cientiffic laboratory
of the University of California
LOS ALAMOS, NEW MEXICO 87544
UNITED STATES
ATOMIC ENI :IGY COMMISSION
CONTRACI W-74OS-ENG. 36
-------
382
This report was prepared as an account of work sponsored by the United
States Government. Neither the United States nor the United States Atomic
Energy Commission, nor any of their employees, npr any of their contrac-
tors, subcontractors, or their employees, makes any warranty, express or im-
plied, or assumes any legal liability or responsibility for the accuracy, com-
pleteness or usefulness of any information, apparatus, product or process dis-
closed, or represents that its use would not infringe privately owned rights.
In the interest of prompt distribution, this LAMS re-
port was not edited by the Technical Information staff.
Printed in the United States of America. Available from
National Technical Information Service
U. S. Department of Commerce
5285 Port Royal Road
Springfield, Virginia 22151
Price: Printed Copy $4.00; Microfiche $1.45
-------
qp q
November 22, 1974 UOO
Office of Radiation Programs
AW 560 E.P.A.
Washington, D.C. 20460
Gentlemen:
In the recent EPA Bulletin it stated that current levels of trans-uranium
elements in the environment are very low,in the case of plutomium there is
a very small amount in the environment. That statement is certainly open to
discussion. The Natural Resource Defense Council states in its "Report
on the Risks of Plutonium Recycle" that one millionth of a gram has been
shown capable of producing cancer in animals.
The question here arises as to whether the small amount of plutonium already
in the environment is more than, equal to, or less than one millionth of »a gram.
This same NRDC reports that an amount of plutonium the size of a football
is enough for a nuclear explosion capable of mass destruction. This statement
in itself would indicate that the production of plutonium ishould be kept to
an absolute minimum.
The ABC impact statement on the assesment of plutonium concedes that the
problem of plutonium toxins and nuclear theft are far from solved and suggests
that they may never be solved in the near future and perhaps may never be solved
at all. This impact statement certainly indicates that we should halt the
further construction of nuclear reactors until a solution to this problem can
be found. This is the procedure that EPA should use for meeting emergencies.
NRDC further stated in its report that microgram quantities of plutonium in
skin wounds cause" cancer and in.rthe body it is a bone seeker where, once
deposited it can cause bone cancer. But, plutonium is most dangerous when
inhaled. This means that under a number of probvable conditions plutomium
forms aerosols of micro sized particulates which can remain suspended for a
significant time. When inhaled it deposits itself in the lung tissue and can
eventually cause lung cancer.
The AEC radiation protection standards governing the amount of plutonium to
which members of the public can be exposed are roughly 100,OOO times too lax.
Judging from these statements I would advise EPA to call as immediate halt to
all construction of any equipment which produces plutonium other than what the
Defense Department deems to be absolutly necessary for national defense. This
should be the method of preventing such releases and keeping that release to
an absolute minimum. The cost of not preventing such releases could mean our
lives.
I ..
I make an appeal to the office of radiation programs to petition the AEC and
the EPA to reduce the present maximum permissable exposure levels by 100,000.
Under the existing conditions mentioned above I can see no jestifyable reason
for either of these agencies to refuse this request.
cc:The task force against nuclear pollution ^^ tr?iy
The Environmental Defense Fund 9*/^^- /JL-JlO „ L
Citizens Altfrt
Senator Gravel
Bulletin of the Atomic Scientists
-------
384
Building 566
Horw«ll Didcot
Oxfordihire OX 11 ORQ
Choirmtm: Sir trio* Wind./" Dlr«tof;Df ASMcUon S«cr.lory,lDGRictonBl T«l«phon« Rowjtock (023 383) 600
National Radiological Protection Board H<"~" Did"»"
29th November 1974
Dr. W. A. Mills,
Director,
Criteria & Standards Division (AW-560),
Office of Radiation Programs,
US Environmental. Protection Agency,
WASHINGTON, D.C.. 20460,
U.S.A.
Dear
Suf
Thank you for the copy of the notice about
public hearings in Washington! next month. I
enclose two copies of R-29. The purpose of this
report was to draw attention! to the many
different aspects of radiological protection of
people exposed to plutoniun and as a result it
is far from definitive on any one of the
problems it reviews.
All the best,
Yours sincerely,
'2 '
,Encl. • G. W. Dolphin,
Assistant Director
(Research & Development)
-------
IMRPB-R29
O)
CM
CC
Radiological Problems in the Protection
of Persons Exposed to Plutonium
.1 '
G.W. Dolphin, H.Smith, D.S.Popplewell,
J.WSlather, N.Adams, N.LSpoor,
J.Brightwell and R.A.Bulman
National
Radiological
Protection
Board
00' . , .'•• •>;;•••-'"•;
tt Harwell; Didcot,0xon. 0X11-ORQ
' September 1974
-------
386
NATIONAL RADIOLOGICAL PROTECTION BOARD - 1974
The National Radiological Protection Board was established by the
Radiological Protection Act 1970 and is responsible for carrying out research and
development and providing information advice and services to those with respon-
sibilities for radiological protection.
i
Any questions relating to this report should be addressed to the Publications
Officer, National Radiological Protection Board, Harwell, Didcot, Oxfordshire,
England.
Further copies of this report are available from Her Majesty's Stationery
Office price 50p net.
-------
387
NRPB-R29
RADIOLOGICAL PROBLEMS IN THE PROTECTION OF PERSONS
EXPOSED TO PLUTONIUM
G.W. Dolphin, H. Smith, D.S. Popplewell, J.W. Stather,
N. Adams, N.L. Spoor, J. Sriqhtwell and R.A. Bulman
ABSTRACT
For the protection of persons exposed to plutonium isotopes and higher
actinides there are five important requirements. First it is essential to
evaluate all the appropriate data and develop basic dose standards for control
of exposure of body organs, particularly bone, liver and lung; these must
be comparable to standards for exposure to external gamma"'and X-radiation.
Secondly, from these basic standards,values for maximum permissible
concentrations in air and permissible annual intakes must be derived using
metabolic models for plutonium in humans. As part of the biological
monitoring of workers it is necessary to make assessments of the amount of
plutonium in the body either by measurement of the excretion rate of plutonium
in the urine or by external counting of gamma or X-radiations'over the chest
or contaminated wound site. For the treatment of cases of high over-exposure
therapeutic techniques should be available for accelerating the excretion or
removal of the radioactivity from the body. Finally, plans must be made to
cover the possibility of a large release of plutonium into the environment
and these should include acceptable values for ground contamination levels.
Relevant data on these five subjects are reviewed in this report.
National Radiological Protection Board,
Harwell,
Didcot,
Oxfordshire OX11 ORQ
September, 1974
HMSO 50p ISBN 0 85951 028 X
-------
q O p CONTENTS
Page No.
1. INTRODUCTION ''•' • a
2. PRODUCTION AND SOME CHEMICAL AND PHYSICAL PROPERTIES 1
3. METABOLISM . 3
3.1 Routes of entry into the body 3
3.2 Metabolism at the site of entry 3 ,
3.3 Transport of plutonium from the site of entry 3
3.4 Retention in the lung of inhaled plutonlum 4
3.5 Distribution in body tissue after intake by
inhalation or through wounds , , 5
3.6 Amount in gonads 6 .
3.7 Summary of metabolism for radiological protection
purposes
4. PLUTONIUM DISTRIBUTION IN HUMANS < 7
5. BIOLOGICAL EFFECTS 8
5.1 Bone 8
5.2 Liver ..." , 9
q
5.3 Lung
5.4 'Lymph nodes 10
5.5 Blood al
v
6. BIOLOGICAL EFFECTS IN MAN la
6.1 Health of workers exposed to plutonium H
6.2 Pathological effects , 12
S'1
7. THERAPEUTIC PROCEDURES FOR THE REMOVAL OF PLUTONIUM^FROM
THE BODY " 12
8. THE RADIOLOGICAL PROTECTION OF PEOPLE EXPOSED TO PLUTONIUM 13
8.1 Basic standards 13
8.2 'Derivation and adequacy of the basic standards 13
8.3 Derived^standards for air concentration and annual intake 17
8.4 Determination of body content from bioassay measurements 18
8.5 Dosimetric model for thoracic lymph nodes 20
-------
Page No. _
389
9. HOT PARTICLES 20
10. PLUTONIUM-238 OXIDE '••: . 22
11. PLUTONIUM IN THE ENVIRONMENT 22
11.1 Sources and chemical form 22
11.2 Routes to man 23
11.3 Aquatic environment 24
11.4 Experience at Palomares 25
11.5 Plutonium in man ' 25
12. CHEMICAL TOXICITY 26
13. SUMMARY ' . ' 27
14. SUMMARY OF NRPB RESEARCH PROGRA1-D-1ES 28
15. ACKNOWLEDGEMENTS 29
16. REFERENCES M 30
TABLES
1. Some important transuranic nuclides produced in nuclear .
reactors
2. The specific alpha activity of particles of Pu02 and
nitrate from fuel irradiated to a level of 2000 MWd/t
and unit density equivalent aerodynamic diameter of 1 urn
3. Percentage distribution of plutonlum in tissue of beagles
after: inhalation and intravenous injectionfand in rabbits
after intramuscular injection
4. Distribution of plutonium in humans as measured in
tissues obtained at autopsy
5. Chromosome aberrations found in blood lymphocytes of
individuals known to have been accidentally contaminated
with plutonium
i
6. Basic dose standards expressed both as rem in a year and
as rad in a year for organs of importance in the protection
of persons exposed to plutonium, from ICRP Pub.9 (1966)
7. Estimated values of rir;k coefficient for various types of
cancer in exposed' population groups for external "^ and oC
radiation
8. Percentage of inhaled plutonium-239 activity transferred
to blood from lung and into bone and liver, half-lives of
retention as used to calculate (KPC)a and MPAI for soluble,
Insoluble., class W and Class Y compounds
9. The variation with particle size of the number of particles
and the number of cells irradiated for a constant activity
of 0.016 pCi of plutonium-239 oxide
-------
390
FIGURES
1. Plutonium induced osteogenic sarcomas in rat
2. Plutonium induced lung cancer in experimental animals
\
-------
1. INTRODUCTION QQ7
Comprehensive reviews of the biological research done during the last «J O 1
two decades on the metabolism and effects of plutonium have been recently
published by Bair (1974), Bair and Thompson (1974), Vaughan (1973),
Bair et al. (1973) and Bair et al.V<1974). The object of this report is
to review briefly, in the context of a nuclear power programme, the problems-
of radiological protection of workers exposed to plutonium in the nuclear
power industry and environmental populations who may be exposed to plutonium
as a result of an accidental release from a nuclear establishment.
2. PRODUCTION AND SOME CHEMICAL AND PHYSICAL PROPERTIES
The production of plutonium in thermal reactors and its use as fuel in
thermal or breeder reactors are unavoidable 'if the large quantities of
uranium-238 in the earth's crust are to be used as a source of energy. The
important nuclear transformations in which plutonium isotopes and some other
actinides are,produced in thermal nuclear reactors are shown.in Table 1.
The relative amounts of these radionuclides present depends on the irradiation
of the fuel. This is proportional to the time in the reactor^and the neutron
flux density and is expressed as megawatt-days per tonne. Almost pure
plutonium-239 is produced only if the fuel is given a loV irradiation, .say
less than 1000 megawatt-days per tonne. At irradiation levels higher than
this, alpha-emitting plutonium-240 and beta-emitting plutonium-241 are produced
in significant quantities relative to plutonium-239. At the very high fuel
irradiations planned for power reactors, other alpha-emitting actinides become
important, namely americium-241 from the decay of plutonium-241, curium-242
and curium-244, as shown in the, sixth column of Table 1, whejfe the figures
have been normalised to plutonium-239. It should also be noted that the
nuclides in this table undergo spontaneous fission but the total amount of
energy emitted in this type of transition is small compared with that in the
alpha particle decay process. ^
There are two relatively short-lived plutonium isotopes, plutonium-238
<86.4 years)!which decays by alpha emission to uranlum-234 (2.5 x 10 years)
and plutonium-241 (15 years) which decays by beta emission to americium-241
(458 years) which in turn decays by alpha emission to neptunium-237
(2.2 x 106 years). The short-lived curium-242 (163 days) isotope which
accounts for most of the alpha activity in the fuel rods at the end of long
irradiation porjodc dccnyo to plutonium-?38. In nummary, an tho irradiation
pf tho fuel rods increases so isotopes of plutonium other than 239 become
more important, as do the higher actinides, americium and curium.
The chemical separation of plutonium from irradiated uranium fuel is
carried out in therUK at Windscale. The process involves dissolution of
the fuel rods in nitric acid and a separation of plutonium from uranium and ^
- 1 -
-------
392 i
fission products. Plutonium is obtained from this chemical process in the
form of^ a nitrate solution which is used to produce insoluble plutonium oxalate.
Most of this material is converted to plutonium dioxide. The chemical forms
of plutonium most likely to be released j.nto a factory working area are the
oxide, the oxalate and the nitrate, the two former as a dust and the latter
as droplets of solution. If plutonium is accidentally released into the
environment it is most likely to be as the oxide.
Plutonium dioxide is chemically very inert. The material can be dissolved
only by drastic chemical treatment with hot concentrated mineral acids
containing complexing agents or by alkali fusion. Even the most highly
polluted atmosphere is unlikely to have much chemical' effect on a plutonium
dioxide aerosol. Plutonium nitrate is water soluble and it undergoes rapid
hydrolysis to produce plutonium in an insoluble form. Atmospheric droplets
of plutonium nitrate or plutonium nitrate solution undergo hydrolysis to give
insoluble plutonium' hydroxide. The plutonium dioxide or the products of
hydrolysis of plutonium nitrate deposited on soil and vegetation will be
chemically inert.
An important physical property in radiological protection is the
radioactivity associated with respirable particles. The number of particles
with a unit density equivalent aerodynamic diameter of 1 micrometer, a
representative size for respirable particles, having a total activity of 40 nCi
is given in Table 2 for two compounds of plutonium. This value of 40 nCi
is the present maximum permissible body burden (MPBB) recommended in ICRP
Publication 2 (1959), and from the table it can be seen that this amount of
activity is contained in about 10 particles of respirable size. \
One other important physical property is that plutonium-239 emits an
L X-ray: of uranium in 4% of disintegrations with an energy of about 17 keV.
It is possible to detect these X-rays through a few centimetres of tissue and
this provides the basis for the detection an^J measurement of plutonium-239
in the lungs or in a wound. All the alpha-emitting isotopes of plutonium
also emit L X-rays in varying amounts during decay. Plutonium-241 decays to
americium-241 which emits a gamma ray with an energy of 60 keV in 40% of the
disintegrations which can be readily detected outside the body from incorporated
deposits. ' •?
J.
3. HETABOMSM
3.1 Routes of entry into the body
Plutonium may enter the body either after deposition in the lung or by
penetration through the skin. There is no evidence of entry through the
intact skin in humans; however there are records of humans being internally
•i:
t contaminated after a hand wound (Schofield et al., 1974) or acid bum
(Lister et al., 1963). The transfer of orally-ingested plutonium across the
- 2 -
-------
gut wall is very small and the ICRP bask Group on The Metabolism of Compounds OJ O
of Plutonium and Other Actinides (ICRP Publication 19, 1972) summarised the
data from animal experiments and concluded that the absorption of oxides and
similar insoluble compounds was 10~4% and for the more soluble compounds,
such as nitrates, 3 x 10~3%. However, it should be noted that in some
animal experiments special forms of plutonium may be more readily absorbed,
as in the case of an early experiment by Weeks et al. (1956) who measured
an absorption of 1.9% in rats given a plutonium compound in the hexavalent
form and at pH = 1. This represents an artificial situation because such a
compound is unlikely to be met in factories or in the environment where
plutonium dioxide or hydrolysed plutonium nitrate ape the most commonly
occurring compounds in the air.
3.2 Metabolism at the site of entry
For purposes of understanding the metabolism at the site of entry a
simple model may be used in which the plutonium is considered to form three
fractions. One fraction is rapidly formed and consists of a complex of
'monomeric plutonium stabilised by.biological anions such as bicarbonate and
citrate and by amino acids and possibly some proteins. This fraction diffuses
away from the site into body fluids and is deposited mainly in bone and liver.
The second fraction consists of colloidal or participate material. Some
colloids may be formed at the site of entry as the plutonium compounds come
into contact with the biological milieu and some plutonium compounds may enter
the body as colloids or particles. Much of this second fraction of material
will become engulfed by cells within a few hours, especially if the site of
entry is the lung (Morrow and Casarett, 1961; Sanders, 1969).' The fate of
this second fraction will depend on the physical and chemical properties of
the ^compound and the biological conditions encountered but undoubtedly some
will slowly erode away from the particles or colloids during the following
months or years, become complexed by biological anions and diffuse into body
fluids similar to the first fraction. That remaining in the cells will be
distributed in the body according to the kinetics of the cell system involved
but most will probably remain in the lymphatic system (Bair, 1974; Schofield
et al., 1974) or become trapped in reticulo-endothelial cells, exemplified by
the Kupffer cells. The cells containing plutonium will be heavily irradiated
and eventually die and the.particle will be engulfed by another cell. A third
fraction may remain almost permanently at the site of entry, particularly in the
case of wounds, and become isolated in a fibrotic region (Lushbaugh and Langham,
1962). .
3.3 Transport of plutonium from the site of entry
Experimental studies in animals on the binding of plutonium in plasma
after intravenous injection of plutonium citrate (Stevens et al., 1968) or
plutonium nitrate (Boocock and Popplewell, 196J) show that about 90% of the
plutonium is bound to transferrin, a large protein molecule which binds iron,
- 3 -
-------
i-j Q r and the remainder is bound to smaller molecul t-s, probably citrate. The same
binding pattern is found when plutonium nitrate is mixed with human serum in
vitro. Some evidence from work in the NRP13 laboratories (Loveless, 1974)
indicates that this pattern of distribution in blood may be different when
the plutonium compound is originally deposited in the lung but more
experimental work is needed to substantiate this observation. Recent
experiments at NRPB (Popplewell et al., 197.
3.4 Retention in the lung of inhaled plutonium
Inhaled plMtonium deposited in the ciliated portion of the respiratory
system, that is nasal passages, trachea, bronchi, bronchioles and terminal
bronchioles, is cleared within a few hours to the external nares or to the
throat for passage through the gut into the faeces. Some of the plutonium
dust in the activity median aerodynamic diameter (AMAD) size range below 2 or
3 microns may penetrate deep into the lungs and become deposited in the
alveoli, the non-ciliated region of the lung where gas exchange 'takes place.
• f
Particles deposited in this region are cleared very slowly by(three main
routes; transport in macrophagec on to the ciliated epithelium and up to the
throat, transport probably in colln into tha lymphatic drainage pathways of
the lung, and slow solubilisation and transfer to the blood, as described by
Mercer (1967). Sanders and Adee (1970) and Sanders et al. (1971) showed
that some of the inhaled plutonium particles in mouse lung are phagocytoscd
by type I alveolar epithelial cells. These cells appear to be radio-
resistant and to be firmly attached to the epithelium wall so that plutonium
trapped by this mechanism could remain in the lung alveoli for a long time.
-------
Watts (1974) has analysed all £he available data on the lung retention of
inhaled plutonium dioxide in large animals, namely dogs, sheep, burro and
man. She found that the retention could be represented by three exponential
terms as in the equation:-
i
„ (0.69t) _ ' (0.69t) ' (0.69t)
A exp - + B exp - + C exp -
The half-lives of the three exponential terms, 1, 30 and 500 days, are reasonably
well established from the data, although it should be noted that 1000 day half-
lives have been reported in long-term dog experiments by Park et al. (1972).
The amplitudes of the three terms, A, B and C cannot be determined from the
available data and these probably depend on the particle size distribution of
the inhaled material. A possible physiological explanation of the three
terms is that the first represents the rapid clearance of particles deposited
on the ciliated epithelium, the second represents slower clearance of particles
engulfed in free macrophages which enter the alveoli from the'blood and pass
out of the lung up the ciliated epithelium, and the third represents the long
term retention of particles in cells of the epithelium.
3.5 Distribution in body tissue after intake by inhalation or through wounds
Plutonium cleared from the lung via the lymphatic drainage system may be
retained for several, years in the thoracic lymph nodes. In beagles,the
important nodes,where the plutonium concentrates,are situated round the
trachea and bronchi at the bifurcation but in man,many lymph node chains are
found in the peripheral pulmonary tissues. Park et al. (1972) reported on
the retention in tissues of beagles1 in an experiment involving inhalation of
plutonium dioxide by nearly 100 dogs and lasting over 11 years. They found
that the accumulated amount, after 11 years, in the thoracic lymph nodes was
on average about 40% of the initial alveolar deposit which ranged from 1 to
50 pCi. This is a large amount of activity; it delivered a radiation dose
to the lung so high that it could have ai'fected the lung clearance mechanisms.
Bair and Thompson (1974) describe another experiment underway at the Battelle
Laboratories in which smaller lung deposits have been vsed arid in about 10
years it should be possible to find out whether the large deposits used in the
first experiment affect lung clearance. .'V
In the experimental work reported by Park et al. (191*2), mentioned above,
the average accumulation nftnr 11 yearn in 3 ivcr and bone was 15% and 5%
rcr.i«ctively of the initial de-posit of plutonium dioxide. For the more
soluble compounds of plutonium, such as the nitrate and citrate, the
retention in the thoracic lymph nodes of both beagles and rats is less avid
and more material ig, transported to other organs. Some data indicating
this effect in beagles are shown in Table 3. By comparison with plutonium
- 5 -
-------
rx Q c dioxide, the amount of plutonium in the thoracic lymph nodes after inhalation
of soluble compounds is very small. Furthermore, the amount reaching the
skeleton is about twice that reaching the liver. The fifth column in Table 3
shows the distribution between the skeleton and liver 4 years after intravenous
injection of plutonium citrate and the ratio of the amount in the skeleton
and liver is about the same as that found after inhalation of this compound.
In the NRPB laboratories, Stather and Howden (1974) found that the extra
pulmonary distribution in rats after pulmonary intubation of small amounts
of activity, equivalent to about five times the maximum permitted amount in
man, is the same for the three compounds of plutonium used, nitrate, citrate
and oxide. They found that the skeleton to liver ratti.o wns about 6 to 1 after
7 days. This indicates that the initial diffusible fraction of the plutonium
compound is more readily deposited in the bone than in the liver. ' However,
at longer tiroes after intake some translocation from bone to liver occurs or
there may be a direct transfer of particulate material inside cells from the
lung to the liver.
Other experimental work by Stather et al. (1974) showed that the amount
of plutonium dioxide transferred from the lung to other body organs depended
markedly on the particle size. They found that plutonium dioxide filtered
through a 25 millimicron Millipore behaved almost in the same way as the
more soluble nitrate and citrate compounds. It has been known' for decades
that particle size influences deposition in the lung and now the work of
Stather et al. shows that it also influences retention. Many years previously,
Bair and Willard (1962) had noted a more rapid removal of small particles from
beagle lungs. \ I
Experiments have been made with animals to measure the tissue distribution
after intramuscular or intradermal injection and the results of these
experiments have been summarised in ICRP Publication 19 (1972). A typical
set of values obtained by Taylor (1969) after intramuscular injection in
rabbits are shown in the last column of Table 3. Again the skeletal
accumulation is more than in the liver but 67% of the injected amount remained
at the site of injection. The amount remaining at the site will depend
markedly on the physical and chemical conditions during injection. v
3.6 Amount in gonads ,,i
Measurements of the amount transferred from blood to gonads have been
made in dogs injected with .plutonium, americium or curium in citrate solution
(Mays et al., 1974). The percentages transferred and retained for a very
long time in the gonads were 0.017 for males and 0.0012 for females. In
humans, small amounts have been measured in gonads obtained at postmortem arising
from the inhalation of plutonium in fallout (Richmond and Sullivan, 1974).
The genetic effect of these small amounts is not known; the somatic effect is
_ 6 -
-------
397
likely to be relatively negligible because the concentration is lower than
in other organs such as bone or liver.
*
3.7 Summary of metabolism for radicrlogical protection purposes
All the available data on the metabolism of compounds of plutonium and
other actinides were reviewed by a Task Group of ICRP (ICRP Publication 19,
1972). They concluded that the distribution in humans could be reasonably
represented for all compounds by a distribution from blood to bone, liver
and soft tissues plus urine of 45X,45%and 10% respectively. They also
suggested that the percentage transfer from the lurtg to blood was 12% for more
soluble and 5% for less soluble compounds. Previously the recommendation for
soluble compounds was 25% and insoluble compounds were riot transferred to
blood. Transfer from the gut to blood is taken to be 3 x 10~%and 10~ % for
soluble and insoluble compounds.
Retention is exponential with half-lives for the lung of 50 and 500 days
for soluble and insoluble compounds and 100 and 40 years for bone and liver
respectively. These latter values are independent of the compound entering
the body. V
4. PLUTONIUM DISTRIBUTION IN HUMANS
—•—•——«—————————————.— t
Data on the concentration of plutonium in human tissues are gradually
becoming available from autopsy specimens. This is a very important aspect
in the study of plutonium metabolism and every effort should be made to obtain
such data. It is noted that the US authorities have set up at Richland a
register of persons exposed to transuranic elements (Korcross and Newton, 1972).
Measurements of plutonium in human tissue obtained at post-mortem have
been reported for more than 60 persons who were exposed at work. • A summary
of the data from the 12 highest exposed persons is given in Table 4. These
cases have been selected for inclusion in the table by reference to the
measured lung> contt_nt which is over 2000 dpm/kg (900 pCi in lung) in all
cases. As the analysis for plutonium at these levels should present no
problems these data are expected to be reliable. In determining the tissue
distribution in humans the problems mainly arise from the inadequacy .qjF the
tissue samples available. Both in the UK and USA, it id' the practice to
obtain as large a sample of liver, whole lung with trachea and thoracic lymph
nodes as possible, together with a portion of bone from ribs, sternum and
vertebrae (Schofield 1974; Parker 1973). Hence, the most reliable organ
content estimates can be made for the lung and liver but in the cane of the
skeleton where non-uniform deposition among the bones may have occurred the
estimate is lens reliable. Naturally, dissection of the lymph nodes in the
pulmonary and tracheobronchial region must be done with care to avoid
extraneous tissue and to locate as many lymph nodes as possible. Nevertheless,
— 7 —
-------
'1 Qn the values quoted of dpm/kg for those lymph nodes may be inaccurate.
From the data in Table 4 it can be seen that the ratio of thoracic
lymph node to lung tissue concentration varies widely and there is no obvious
^
increase in the ratio with the years o£''exposure. However, if the exposure
pattern is non-uniform, as it usually is with plutonium, the years of
exposure might not necessarily be a guide to the mean duration of the deposit
in the lungs. Furthermore, the animal experiments, as typified by data in
Table 3, indicate that plutonium nitrate is not concentrated in these lymph
nodes to the same extent as plutonium oxide. The compounds to which humans
are exposed during a working life cannot be specified with certainty.
I The mean of the ratio of concentrations in the lymph nodes and lung
weighted by the amount of plutonium in the nodes is 5.8 and the unweighted
value is 12.5. These values are much lower than those measured in beagles
exposed to plutonium dioxide. Park et al. (1972) found in 5 dogs, all
surviving more than 7 years, a lymph node concentration relative to the lung of
between 150 and 3000.
The ratios of the amounts in bone and liver given in Table 4 vary widely
and again this is due partly to the duration of the exposure |^nd partly to the
type of compound taken into the body. The mean value of the ratio is 1.9
and this is well within the range of values found in animal experiments.
5. BIOLOGICAL EFFECTS
In animal experiments it has been well established that late biological
effects occur in the bone, liver, lung, thoracic lymph nodes and blood.
After the intake of soluble compounds of plutonium sufficient may' be transferred
from the site of entry, that is the lung or a wound site, to the bone and liver
so that late effects may occur in these organs. There is little transfer from
the lung and thoracic lymph nodes and the late effects after inhalation of
insoluble plutonium dioxide mainly occur invthese organs. The significant
effect in blood observed in beagles following inhalation of relatively large
amounts of p'lutonium dioxide is a chronic lowering of white cell count, .
particularly of lymphocytes, for which the count may be lowered by a factor of
2 (Park et al., 1972). No neoplasia of the haematopoietic sysiem such as^,
leukaemia have been observed in these dogs. ,i
5.1 Bono
Plutonium is transported in the blood and deposited on the endosteal
surfaces of bone where it is well situated to irradiate osteogenic cells.
The deposited plutonium may later become buried in the bone by apposition of
bone mineral. It may enter ostooclasts, bone cells concerned with renorption,
during bone remodelling or it may be phagocytosed by macrophages and move
into the bone marrow (Joe, 1972). Osteogenic sarcomas have been produced
_ 8 -
-------
399
4n experiments with mice, rats and dogs after administration of plutonium
by various methods;, intravenous injection, intratracheal injection, inhalation
and subcutaneous injection. A summary of the osteogenic sarcomas found in
rats, as reported by several investigators, is plotted in Fig. 1. Data
from intravenous injection experiments have been excluded because this is not
a relevant method of intake for humans and it could lead to a micro-
distribution on the bone surfaces different from that occurring when plutonium
reaches the blood slowly after crossing membranes, as in inhalation
experiments. On the basis of a linear analysis, the risk coefficient in
the rats is 3.9% per 100 rads average dose to bone.
At the University of Utah,beagles were injecte'd intravenously with
plutonium citrate and 4 out of 12 developed osteosarcomas after about 9 years
and they had an average dose to bone at death of 86 rads. At higher average
bone doses, 190 rads and 310 rads, 8 out of 13 and 10 out of' 12 developed
osteosarcomas. Again on the basis of a linear analysis these data indicate a
risk coefficient of about 40% per 100 rads which is about 10 times higher than
the value for rats. This could be due to species differences, in which case
it clearly demonstrates the uncertainties of extrapolation from one species
to another. Alternatively, there may be a difference in osteogenic sarcoma
induction depending on whether the plutonium is deposited rapidly by intra-
venous injection or is deposited slowly by transfer via the blood from the
lung.
5.2 Liver
Liver tumours are rarely seen after administration of plutonium to rats
and this is probably due to the fairly rapid clearance of plutonium from the
rat liver"to bile and into faeces. In beagles at the University of Utah,
Taylor et al. (1972) reported 10 bile duct tumours in 96 experimental dogs
and only 4 in 98 control dogs. In 2 dogs these liver tumours were the cause
of death and,the average radiation dose to their livers was about 60 rads.
The tumours appeared at the end of the expected life span and they caused
little life shortening. There are not enough data from animal experiments
i
to calculate a risk coefficient for liver tumours. >ji
..>.
5.3 Lung
Acute effects have been observed in dogs after inhalation of large
amounts of plutonium, equivalent to more than 500 mlcrocurles in man.
7, ..s*. ro;..;.i.st oC severe inflammatory reactions, oeaema and haemorrhage and
c,tMth occurs witha.n a few days. At lower intakes fibrosis is the critical
ch-rv- in the lung,.which reduces its capacity for gas-rous exchange and
'•'thin FI i\:w months deeith occurs due to pulmonary insufficiency and
associated heart failure.
9 —
-------
40G
The Important late effect is lung cancer and data from three experiments
involving inhalation of insoluble plutonium by rats are plotted in Fig.2.
On a linear analysis the risk coefficient is 7.5% per 100 rads, which is
higher than the similar value for bone.1' In a long-term experiment started
in the early 1960s, Bair and his colleagues at the Battelle Northwest
Laboratory exposed nearly 100 beagles to aerosols of plutonium dioxide. In
those animals which survived more than 1600 days, 20 out of 21 developed lung
cancers and it is therefore not possible to evaluate a risk coefficient from
these data (Bair and Thompson, 1974). It should be noted that the cancers
observed by Bair and his colleagues were often multifcjcal and all in the
peripheral region of the lung. Naturally occurring cancers in man are more
frequently found in the primary and segmental bronchi than in the peripheral
region of the lung (UICC, 1973).
5.4 Lymph nodes '
Lymph nodes associated with the lymphatic drainage system of the lung
and local lymph nodes near the site of subcutaneously-injected plutonium
may have plutonium concentration levels higher than most other tissues. In
the beagles exposed to plutonium dioxide aerosols at Battellfe Northwest
Laboratories 3 dogs developed thoracic lymph node malignancies out of 21
animals surviving more than 1600 days (Park et al., 1972). These malignancies
were classified as haemangiosarcoma, lymphangiosarcoma and endothelioma but
all 3 dogs also had primary cancers in the lung. The results of this
large-scale dog experiment indicate that although these lymph nodes received a
higher radiation dose than the lung,,they were not the organ in which most
cancers were observed. This view may change when the results from the low
dose experiment now under way at the Battelle Laboratories become available in
the next 10 years.
Experiments involving the implantation of plutonium dioxide in the fore-
paws of dogs have shown that plutonium is transferred to the cervical and
axillary lymph nodes. No dogs have shown any detrimental effect which can
be unequivocally ascribed to this implant in the first three years of the
experiment (Lebel et al., 1972). One dog with about 6 uCi of'plutoniun^
dioxide implanted in the paw died of a lymphosarcoma after 4 months. The
estimated dose to the cervical lymph nodes was about 7000 rads but this
single cancer developed very soon after implant and may not be due to the
radiation. It is, therefore, not sufficient evidence for conclusions to be
drawn.
Up to tho present the experiments with beagles and with rodents indicate
that the irradiation df lymph nodes with doses ranging from a few rads to a
few thousand rads does not induce primary cancer of lymphoid tissues in.
significant numbers.
- 10 -
-------
401
54.5 Blood
Park et al. (1972) have reported a chronic reduction of the lymphocyte •
cell count in.the blood of dogs starting within a few months of exposure to
Plutonium dioxide aerosols. Similar observations have been made by other
workers (Buldakov et al., 1969; Ballou et al., 1972).
Leukaemia and other haematopoietic neoplasia have not been found in dog
studies at Battelle Northwest Laboratories during the last 20 years (Bair,
1974). The only leukaemias observed are in rodents. Benste^d et al. (1965)
found 3 myeloid leukaemias in 26 rats given multiple intravenous injections
of plutonium nitrate with a total equivalent amount for man of over 200 uCi;
the permissible amount in man is 0.04 |aCi. They found one leukaemia in 22
rats given a single intravenous injection of about the same amount of plutonium.
Brooks and Mewhinney (1973) found chromosome aberrations in blood
lymphocytes of1 Chinese hamsters after inhalation of plutoniunv-230 oxide
particles. Presumably this damage was produced in the lymphocytes by alpha
irradiation as they passed through the lung capillaries or through the thoracic
lymph nodes. . .
6. BIOLOGICAL EFFECTS PI HAH
6.1 Health of workers exposed to plutonium
Hempelmann et al. (1973) reported on the health of 25 males who were
exposed to a range of plutonium compounds 27 years previously under the crude
working conditions existing during the production of the original atomic bombs
at Los Alamos Scientific Laboratory, New Mexico, USA. The bpdy content
estimated from the urinary excretion rates of plutonium for these men ranged from
5 nCi to 420 nCi, that is up to 10 times permissible amounts. They were
recently subjected to a comprehensive medical examination and none of the
findings could be attributed to the presence of plutonium In the body. Only
the diseases and physical changes characteristic of a male population entering
the sixth decade were observed.
More recently, Schofield and Dolphin (1974) have reported health
statistics for workers at BNFL, Windscale. In a cottparison with another
>i iii
BNFL establishment the number of days lost through sickness per year per 100
male employees was about the same. Hence no relevant general health problems
appeared to exist at Windscale where large quantities of radioactivity,
including tonnes of plutonium, are procensed each ye;ir. Cancor dar.thu in tho
male population at Windscale Works were given for the cix years 1967-72. In
this period 23 cancers were observed in the working population and over 37
were expected as calculated from national statistics, which were adjusted for
age distribution of the workers. The data given by Schofield and Dolphin
cannot yet conclusively show that the working levels for plutonium presently
accepted are correctly chosen hut they do allow a certain cautious optimism.
- 1.1 -
-------
402
6.2 Pathological effects
No cancers or detrimental biological effects in man can bo unequivocally
attributed to plutonium. Lushbaugh and Langham (1962) reported some
histological changes they had found near a particle of plutonium embedded in
the palm of a man's hand for about four years as showing "a similarity to
known pro-cancerous epidermal cytologic changes". The meaning of pre-
cancerous changes is far from precise but this statement certainly cannot be
used to infer the presence of a cancer in the man's hand at the time of
excision.
, Dolphin (1971) reported an average finding of 5 Reentries per thousand
cells in blood lymphocytes from eight workers with an average time of exposure
to plutonium at work of seven years. They had also received on average 14
rads from external radiation. The observed aberration yield was -not
significantly different from that of workers who were only exposed to external
radiation of about the same amount.
The yields of chromosome aberrations in blood lymphocytes from workers
known to be contaminated with plutonium are shown in Table 5. These
aberrations are presumably produced as the lymphocytes move close to plutonium
deposits; the range of the alpha particles is only 40 pn in tissue, about
4 cell diameters. At present the interpretation of these aberrations in terms
of body content of plutonium or in terms of the possibility of a late effect is
not yet possible.
7. THERAPEUTIC PROCEDURES TOR TUty REMOVAL OF PLUTONIUM FROM THE BODY
It is now well established that intravenous injections or infusions of
the chelating -agent, diethylenetriaminepentaacetic acid (DTPA), will
effectively clear all plutonium from the plasma and some from recent deposits
in the bone or liver. However, little plutonium can be removed from these
organs when the deposit is of long standing. Experimental work with animals
has shown that DTPA must be given very quickly after intake, within minutes,
if it is to prevent significant deposition in the bones and liver. This is
in agreement with the human data summarised by Durbin (1972) on the rapid
removal of injected plutonium citrate from the blood to the bone and liver'
with 50% leaving the blood within 20 minutes.
Thorn arc two main disadvantages of DTPA as n therapeutic agent. FJrnt,
it is rapidly cleared from the body fluids by excretion through tlio kidney with
a half-life of about 90 minutes in humans, so that multiple injections are
needed to maintain effective blood levels for a few days; secondly, it does
not cross cell membranes and as mo.'it of the colloidal and particul.ate
plutonium is engulfed by cells within a few hours of intake, particularly in
the lungs, it is not effective in removing this material.
-------
403
Attention has been directed in the NRPB laboratories to both these
problems and some progress is being made towards solving them. One other
factor in the use of DTPA has been opposition to its use in humans on the
grounds of toxicity but Smith and Morgan (1974) failed to demonstrate any toxic
effects of the substance in animals under all likely conditions of use.
The other technique now being developed for the removal of plutonium after
inhalation is lung lavage. This has already been used once on a man who
inhaled plutonium following a glove box accident at Rocky Flats, Colorado
(McClellan et al., 1972). The technique was only partially successful in this
case for only 13% of the initial lung content was remc(ved, but there is no doubt
that it must be developed as it offers the best hope of reducing the radiation
dose to the lung should a massive inhalation occur. In work with dogs at
the Lovelace Foundation (HcClellan et al., 1972) about 50% of inhaled plutonium
oxide particles were removed by lavage, and Nolibe (1974) working in France
has removed up to 90% from baboons.
8. THE RADIOLOGICAL PROTECTION OF PEOPLE EXPOSED TO PLUTONIUM
8 .1 Basic standards J |
It is proposed to review only those dose standards applicable to plutonium.
For workers the maximum permissible dose to the whole body, gonads and red bone
marrow is 5 rem in a year, as shown in Table 6. This is subject to certain
limitations given in ICRP Publication 9 (1966) but of no real consequence for
control of plutonium exposures. The maximum permissible dose for individual
organs of the body is 15 rem in one year except for the bone, thyroid and skin
where the dose is 30 rem per year. A quality factor, Q = 10, to allow for
the greater effectiveness of alpha emitters in producing biological damage is
used in calculating the dose to individual organs and for bone a modifying
factor, N = 5, is also used. In effect,the factor N is used to take into
V
account the evidence from animal experiments that plutonium is between 5 and
10 times more radiotoxic in bone than radium. This point will be discussed
in greater detail in the next section. For members of the public the dose
limits are 10 times lower than the maximum permissible doses for workers.
For purposes of comparison with animal and other data the dose limits are'Salso
expressed in rads in Table 6.
8.2 Derivation and adequacy of tho basic standards
Radiological protection standards have evolved over the last 50 years
since the first recommendation of Mutscholler and Sievert in 1925. They
suggested an annual dose limit to the body from external radiation eqvwl to
10% of the dose requires) to produce erythema. Erythema, skin reddening, was
known to be produced by a single dose of about 500 fads from 200 kV X-rays
(the term rontgen was used at that time for units of dose). Hence,the first
- 13 -
-------
404
standard for external radiation was 50 rods per year; this was reduced in
1950 to 15 rads per year and again by ICRP in 1956 to 5 rads per year where
the standard currently remains.
This standard is based essentially on experience of human exposure in
medicine and in industry. Two other sources of information are available for
consideration in setting standards. One source is epidcmiological studies
of irradiated population groups, such as atomic bomb survivors and radio-
therapy patients. The other source is animal experiments. Although there
is great uncertainty in extrapolation of data from animal experiments to man,
these experiments do facilitate the study of the mechanisms of radiation
carcinogenesis, genetic effects, metabolism and the'relative toxicities of
internally deposited radionuclides.
The first basic exposure standard set as a result of an epidemiological
study was that for radium-226. By 1941 sufficient data had been accumulated
on the skeletal effects of radium in persons accidentally contaminated during
the period 1910-1930 to allow a choice of 0.1 pCi of radium-226 as the maximum
safe skeletal content. Although many more data have been accumulated on the
health of these radium patients since 1941 the value of 6J1 uCi still remains
a radiological protection standard and corresponds to an average dose
equivalent of 30 rem per year to the bone.
The toxicity of plutonium-239 relative to radium-226 has been studied
at. the University of Utah in long-term experiments with beagles. The results
of these experiments (May and Dougherty, 1972) show that for equal toxicities
in terms of the induction of osteogenic sarcomas, 5 to 10 times more energy
must be deposited in the bone from radium-226 compared with plutonium-239. It
is,generally accepted that plutonium-239 is more effective in producing bone
cancers because it is deposited and remains mainly on endosteal surfaces where
it is well placed to irradiate or,teogen|c cells from which the sarcomas originate,
whereas some radium becomes buried in bone mineral where there are only a few
cells, i In effect the modifying factor for calculation of dose equivalent in
bone, N = 5 for plutonium and N = 1 for radium, takes account of the higher
radiotoxicity of plutonium relative to radium and this leads to the equivalence
of the maximum permissible body contents of 0.1 pCi of radium-226 with? 0.04 uCi
of plutonium-239, given in ICRP IMblication 2. Hence tho standard for
plutonium-239 is linked with the human radium cases.
Lloyd and Marshall (1972) drew attention to differences between bones in
beagles and humans. They made measurements on lumbar vertebrae from man and
beagles and found that the surface to volume ratio was a factor of two higher
in beagles. They Suggested that bone turnover was higher in beagles and from
this evidence they claimed that the potential risk for pluton.ium-239 relative
to radium-226 would be expected to be a factor of two higher. In making this
- 14 -
-------
claim several assumptions have to be made rojarding, for instance, the
representativeness of vertebrae for all bones and the numbers and distribution
of cells on bone surfaces in man and in dogs. Hence the observations of
i
Lloyd and Marshall are of great interest but their significance to the
relative toxicity of radium and plutonium in man is difficult to assess.
The first quantitative study of the risk of cancer production in an
irradiated group was for a group of children and adults who had received
radiation to the thyroid, published by Beach and Dolphin (19G2). On the
assumption of a linear relation between the incidence of thyroid cancer and
radiation dose they calculated a risk coefficient for, the induction of
'thyroid cancer. Since this original work many quantitative risk evaluations
have been published both by individual scientists and'by committees such as
UNSCEAR (1972) and BEIR (1972).
A summary of some risk coefficients pertinent to the radiological protection
of persons exposed to plutonium is given in Table 7. Goss (1974) has analysed
the mortality statistics for the atomic bomb survivors in Japan published by
Jablon and Kato (1972) and he found risk coefficients of 100 cancers per million
man-rads for all cancers and 30 for leukaemias. In making |l)hese risk
estimates, allowance was made for 10% more leukaemias not already manifest by
1970. Similarly an allowance was made for all the other cancers but due to
their long latent period the number occurring before 1970 was doubled to
obtain the ultimate number expected to occur. Goss found that the RBE value
for cancer induction by neutrons at Hiroshima was about 5 and it should be
noted that the data given in the table are for gamma radiation only. For
patients with ankylosing cpondylitis treated with 250 kV X-rays data have
been published on excess cancers by Gourt Brown and Doll (1965) and these
have been analysed in terms of risk coefficients by Dolphin and Marley (1969)
who gave a value of 10 leukaemias per million mad-rads and 5 times this value
\
for all cancers.
In the next1, line of the table a risk coefficient has been calculated
from data on the mean dose to bone for 1417 cases of radium contamination
including 71 with bone sarcoma (Rowland, 1973). Most of thesp people were
contaminated during the period 1910-30, often when they were quite young^1
the studied population therefore involves a large number of'man-years at risk.
The value for the risk coeff5.cient, 00 cancers per million man-rads (menn doce
to bone), may be taken as the upper limit; this is not a truly random
survey because there is a greater likelihood of including cancer cases
that were less affected by the radium contamination.
Spiess and Mays (,1970) reported on the incidence of bone sarcoma in
700 adults injected, mainly during the years 1945-51,with radium-224 (half-
life, 3.64 days) for the treatment of tuberculosis, ankylosing spondylitis and
405
- 15 -
-------
406
other diseases. They calculated a risk coefficient for this group of 90
cancers per million rtvn-rads (mean dose to bone). An important point made by
them was that'radium-224 is initially deposited on bone surfaces where it
delivers most of the dose due to a short half-life. Hence the spatial
distribution of the radiation in the bone is like that from plutonium but the
dose from plutonium is spread out in time.
An increased incidence of lung cancer among miners exposed to radon in
uranium mines, fluorospar mines, haematite mines and hard-rock mines has been
observed for many years. A summary of these exposures of lung to radon ..
together with exposures of lung to thoron in patients injected with thorotrast
was given by Lundin et al. (1971). From their summary an average risk
coefficient has been obtained by we.ight3.ng the individual risks by the square
root of the number of lung cancers attributed to radiation in each group.
The value obtained in this way is 30 lung cancers per million' man-rads (mean
dose to lung) based on the assumption that the annual risk rates given by
Lundin et al. existed for a period of 20 years. If the experimental obser-
vation by Lafuma (1974) applies to man then this risk coefficient for lung
cancer where the dose would be diffusely distributed throughout the lung may
represent a greater risk than could be expected from the same radiation dose
from alpha-emitting particulate material. In summary this value of 30 lung
cancers per million man-rads may well over-estimate the risk estimate following
inhalation of radioactive particles.
If the risk coefficients for human cancers in Table 7 are taken to have
equal reliability so that meaningful comparisons can be made,1 then the important
question concerns the risk coefficients of alpha emitters relative to external
radiation." With external radiation the exposure is usually prolonged in time
and the risk coefficient given in the table must be reduced by a factor in
the range 3 to 10 to allow for the lower effectiveness of chronic irradiation.
This factor is derived from experimentally-induced cancers and genetic mutations
in animals such as thyroid cancer in rats (Doniach, 1964), leukaemia in male
mice (Upton et al., 1.970) and specific locus gene mutations in the offspring
of irradiated male and female mice (Russell, 1965). With this factqr, the
risk coefficient for leukaemia and all cancers is reducec} to the ranges 3 to
10 and 10 to 30' per million man-rads respectively and with tho associated
|-orini.r..':.H)l f .inriii.il elo.-.n (if !> nul.'i tin* IHMX linnrn nnnu.nl r I fikr. nl. cquj 1 |]>J..1 urn euro
15 to !>0 iiiKl :'>0 lu VM per million per you-.
For incorporated alpha emitters the biological effect is less dependent
on the dose rate ns indicated by the rick coefficients for radium-,0,'"! and
radium-??G in Table^ 7. Hor.ce for bone sarcomas induced by radium-22G tho
upper rick estimate remains unmodified at BO per million man-rads associated
with a permissible annual dose of 3 rads. The permissible annual ri.sk to bone
- 16 -
-------
. 407
from/radium-226 is 240 and is higher than that for external X- or J-radiation.
The greater effectiveness of plutonium in producing bone sarcomas is taken
into account by the lower permissible annual dose, 0.6 rads. The risk
coefficient for radium-224 is about the same as that for radium-226 but the
dose to bone is quite different in distribution and dose rate. No inference
can therefore be drawn from the radium-224 data until studies on its
effectiveness in producing bone sarcomas relative to plutonium-239 have been
completed in beagles at the University of Utah.
For the lung, the risk coefficient 30 per million man-rads is associated
with a permissible annual dose of 1.5 rads and the permissible annual risk at
equilibrium for alpha emitters, 45 per million per year, is within the range
given above for externalY-radiation. The effectiveness of radon and thoron
per unit of radiation dose in producing lung cancer relative to plutoniurn is
not known but can be assumed to be about the same.
In summary, the risk coefficients of the radium alpha emitters; in bones
of humans appear to be higher by a small factor than those for whole body
irradiation by external^-radiation. It is for general consideration whether
this should be taken into account in setting current maximum'permissible levels.
From Table 7 is can be seen that the risk coefficients for the rats
exposed to plutonium for both bone sarcoma and lung cancer ( Figs. \ and 2)
are considerably higher than those derived from observation of human popula-
tions. There appears to be no reason for these differences other than species
differences. The risk coefficient which may be derived from the beagles
injected with plutonium-239 citrate are about 10 times higher than the rat
data. At present there is no explanation for the differences between animal
and human dat£ but clearly great care must be exercised v/hen extrapolating
from one species to another.
8.3 Derived standards for air concentration and annual intake
The important parameters required in the derivation of exposure standards
i
from the basic radiation doses are given in Table 8. The presently used values
from ICRP Publication 2 (1959) are given in the first and second lines. Other
i
values which could be derived using the later data given in ICRP Publication 19
(1972) are given in the third and fourth lines. It should-be noted that data
from Publication 19 have not yet been incorporated in ICRP recommendations.
It can be seen in the table that some changes would be introduced if the later
data were used for lung clearance to blood and 45% each to liver and bone from
blood; these changes are not very significant. The two values from Publication
19 for soluble and insoluble compounds are closer than those in Publication 2.
i.
Dolphin (1972) has pointed out that from a practical stand-point the most
convenient change in derived standards would be to use a single value for
(MPC) applicable to all plutonium compounds. This single value could be
- 17 -
-------
^~ " somewhere between those for class W and class Y compounds given in the third
and fourth lines of the table.
The annual permitted intakes of activity by the oral route are relatively
high due to the low gut absorption as already noted in the section on
Metabolism.
8.4 Determination of body content from bioassay measurements
Two techniques are available for estimation of the amount of plutonium
in the body; the measurement of the daily rate of urinary excretion of
plutonium and the measurement of the counting rate over the chest of L X-rays
from plutonium-239 and plutonium-240 or 60 keV gamma rays from americium-241,
the decay product of plutonium-241.
The body content estimation from urinary excretion data is based on human
cases injected with known amounts of plutonium in 1944 and 1945 by Langham (1957)
and his associates. The data from these experiments were recently reviewed
in depth by Durbin (1971). There are many limitations to these data; first,
they were obtained after intravenous injection of plutonium citrate or nitrate
compounds into 16 patients and this is not a normal route of entry into the
body except in experimental conditions; second,the excreta were collected for
only a few days in many cases and for more than 138 days in only 4 cases;
third,the data were obtained from terminal patients whose metabolism was in
differing degrees abnormal. Nevertheless these are the only data available
for relating excretion rate to body content.
The use of these excretion data in estimating body content has been
described by Beach and Dolphin (,1964), Beach (1973) and Adams land Watts (1974).
The formula derived from Langham1s original equation by Beach and Dolphin is
as '-follows i-
f-
(b-1) 0.16 I -T tt>t) "'"" df
where Y is the urinary excretion rate expressed as a percentage of the plutonium
intake, tt~b is a function of time representing the transfer of plutonium from
the lung to the body, t is in days and b is a constant. To use this formula for
the function for transfer into the body a value of b must be assigned,, ^if
possible, froip knowledge of the intake conditions. (
The formulae based on Langham's equation are known to over-estimate the
body content in most cases where the exposure occurred some years previously.
Schofield and Dolphin (1974) found that the amount of plutonium at death
estimated from autopsy tissue samples obtained from persons exposed to plutonium
for a number of years was between 1.2 and 8.3 times lower than that calculated
from measurements tif the excretion rate in all 6 cases for which urine data
were available. Lagerquist et al. (1973) also reported the same over-estimation
from the urinary excretion data. In addition, Dolphin (1972) has shown that
- 18 -
-------
use of the Langham equation to estimate body content within a few weeks of 4 U 9
intake can lead to an over-estimation by a factor which could be as high as 10.
Recently, data on urinary excretion rates have been obtained from two of
the original cases injected with plutonium designated as HP-3 and HP-6 (Durbin,
1972). HP-3, a white female, was injected with 0.3 pCi of plutonium citrate
in November 1945. She is now 77 years old and her plutonium excretion rate
is 1.4 x 10~ % per day. The other case, HP-6, a white male, was also injected
with 0.3 uCi of plutonium citrate and i-s now 73 years old with a plutonium
' _3
excretion rate of 2.5 x 10 % per day (Rundo et al., 1974). The equation
—4
proposed by Langham (1957) predicts a value of 2.9 x 10 % per day. Hence '
the excretion rate is much higher than expected in these two cases and if these
data were included in the Langham equation the effect would be to lower the
estimates made from urinary measurements on those people who have a long standing
body content.
In summary, body content estimates based on Langham1s data are likely to
be an over-estimate of the true content but many more autopsy data correlated
with urinary excretion data are required before Langham1 s equation :"can be
confidently amended or replaced. , j
Techniques for the measurement of plutonium in the chest by external counting
have been developed over the last 15 years, first using large proportional
counters and more recently by a system of combined thin and thick crystals. For
either technique the limit of detection is between 5 and 10 nCi of plutonium~239
plus the other alpha-emitting isotopes depending on the amount of absorbing
tissue over the rib cage of the individual. This lower limit of detection
corresponds to a total radiation dose of about 15 rem to the lung during the
following few years. Hence the chest monitoring systems available at the moment
are just adequate; more development work is required to increase the sensitivity.
As the alpha-emitting isotopes of plutonium,which vary in relative amounts
depending on fuel irradiation,emit varying numbers of L X-rays per disintegration,
this adds another difficulty in the interpretation of chest monitoring results.
i
The presence of americium-241, the decay product from plutonium-241,
increases the efficiency of detection due to the emission of 60 keV gamma-rays
i
, which are less absorbed in the chest wall. If a sample of the inhaled Material
is available then the ratio of americium-241 to alpha-emitting plutonium
isotopes plus plutonium-241 may be determined outside the body and used to .
estimate the total plutonium plus americium content of the lung. However,
caution is necessary for it is known that americium-241 is more transportable
than plutonium in the lungn and therefore it cannot be considered as a true
tracer for plutonium, particularly over long periods.
Holliday et al. (1970) have described a comprehensive system for the
radiological protection of workers from airborne plutonium particles. This
- 19 -
-------
"1 f| involves routine chest measuring for insoluble plutonium in the lung at six-
monthly intervals and annual or six-monthly urine samples taken over five
consecutive days for estimation of systemic plutonium.
8.5 Dosimetric model for thoracic lymph nodes
One of the outstanding problems in radiological protection related to all
insoluble materials concerns the high accumulation in lymph nodes associated
with lung drainage, as indicated by animal experiments. The experiments with
beagles by Park et al. (1972) show that on average 40% of the alveolar deposit
passes into these lymph nodes and as there appears to be little clearance,
this leads to tissue concentrations between 150 ana 3000 times higher than
those in the lung. In man, the small amount of information available,
reviewed in Table 4, does not match such high relative concentrations and an
average value is about 10 for lymph nodes relative to lung. This lower value
may be due either to the human exposures being more predominantly to soluble
compounds of plutonium or to routes of clearance in man following chronic
inhalation which do not involve lymph drainage.
The lymph nodes are part of the lymphoid tissue in the body which are
estimated to have a total mass of over 2000 g. The kinetics of lymphoid
tissue are not well understood but they consist broadly of two fractions;
about 700 g of stationary reticulum cells and about 1500 g of mobile
lymphocytes (ICRP Reference Man, 1974). Due to the mobility of the
lymphocytes the amount of lymphoid tissue irradiated is considerably more
than the 16 g of lymph nodes associated with human lung, as reported by
Pochin (1966). Hence, the effective concentration in lymphdid tissue is
less than that calculated for the thoracic lymph nodes as individual tissues.
! The most appropriate dosimetric model to use for the thoracic lymph nodes
has not yet been resolved by ICRP but it certainly should not be based on
the very high concentrations found in tfie dogs exposed to large amounts of
plutonium dioxide at the Battelle Laboratories. The question of tissue mass
to be used in the model and the residence time of the material in the nodes
must be carefully chosen and above all the absence of large scale late effects
in these lymph nodes, as observed in animal experiments, mdst be given due
regard as no human data are available.
9. HOT PARTICLES
The radiological protection problems associated with insoluble particles
of alpha-emitting radionuclides have been known and considered for a number
of years (Dolphin, 1964) but recently public attention has been drawn to
these problems by *& petition submitted to the USAEC by Tamplln and Cochran
(1974) which caused comment in the national press. The problems concern
the biological effect of high but localised doses. Alpha radiation from
- 20 -
-------
411
plutonium-239 only penetrates about 40 microns in unit density tissue and
consequently only a small volume of cells around the plutonium particles is
—7 3
irradiated, about 2.7 x 10 cm . The average radiation dose to such a
volume around a one micron particle of plutonium-239 oxide is 300 rads per day
or about 90000 rads per year. However, radiological protection dose standards •
cannot be applied to small volumes as they have been derived from observation
of the biological effects in the whole body or in body organs.
The arguments used by Tamplin and Cochran were essentially based on the
data of Albert et al. (1967) who induced skin cancers in rats either by high
doses of beta particles or by electron irradiation. These skin cancers '
originated in hair follicles and Tamplin and Cochran argued that high doses
of the order of 1000 rads or more to the small number df cells in the >
follicles could induce these cancers. They then transferred this concept from
rat hair follicles to the irradiation of small numbers of cells ,in human lung
after the inhalation of plutonium particles. They concluded that lung cancer
in humans might be expected following the inhalation and deposition of 2000
particles but they were unable to present evidence of cancer of the' lung '
following such small intakes either in animals or in humans. ()
The amount of plutonium-239 in the lung which would deliver a mean dose at
the permissible rate of ISremsper year is 0.016 pCi. Some estimates of the
number of cells irradiated by this amount of activity are given in Table 9 for
three particle sizes. The table shows clearly that if 0.016 uCi is divided
into large particles then fewer cells would be irradiated, considerably less
than if• this amount of activity was/divided into very small particles. In
making this calculation the cell volume was taken to be 10~9 on3 and no
allowance was made for energy absorption by the air inside the lung. Hence,
if the radiotoxicity is related to the number of cells irradiated then particles
are less hazardous than diffuse deposits in the lung or elsewhere in the body.
Lafuma (1974) has studied life-shortening and lung cancer in rats following
inhalation of various actinides. He reported finding greater life-shortening
and more lung cancer (Lafuma, 1974) in animals with curium-242 compared with
those given an equal average lung dose from plutonium-239. Luqg autoradiographs
show that the curium-242 is diffusely distributed in the lung whereas the',f
plutonium-239 in his experiments was in particulate form. This experimental
finding supports the view that the risk of biological damage from a given mean
dose to lung increases as the number of cells irradiated increases and is at
variance with the "hot spot" hypothesis advocated by Tamplin and Cochran.
Other evidence which shows that particles of plutonium dioxide are less
effective at producing biological damage than equal amounts of diffusely
distributed plutonium comes from the work of Brooks.et al. (1973). They
studied the chromosome aberrations induced by plutonium in hamster liver cells,
- 21 -
-------
412
in vivo. Plutonium citrate produced a linear increase of aberrations with an
average radiation dose to the liver which was greater than the aberration
yield produced by plutonium dioxide..- particles at the same average dose levels.
There are more data from animal experiments available to support the
hypothesis that for a given average organ dose the particles are less effective
than uniform distributions. These have been reviewed by Bair et al. (1974).
In summary, there is no biological evidence available at present which
suggests that "hot spots" carry a higher risk of cancer induction. Hence
there is no necessity to change from the present system of using average dose
to organs or tissues. However, it would be prudent to continue research into
the biological effects of non-uniform dose distributions within organs.
10. PUJTOniuH-asB OXIDE
Plutonium-238 with a half-life of 06 years is an important heat source
used to drive long-lasting thermoelectric generators which have applications
as implanted batteries for human heart pacemakers, for the development of
artificial hearts and for space exploration. Worldwide public attention was
attracted to this material when 17,000 Ci were dispersed 'into the atmosphere
during an abortive rocket launch in 1964 by the USA.
The radiation dose rate in an 80 micron diameter sphere of unit density
tissue around a one micron diameter plutonium-238 oxide particle is about
93000 rads per day. The effect of this high emission of energy is not only
to raise the temperature of the particle but also to cause radiolytic action
in and around it which tends to'',break up the particle. Experimental work
with animals shows that inhaled material diffuses freely into body tissues,
for example, Willard and Park (1970) found only 4% of the terminal body content
in the lungs of dogs 23 months after Inhalation of plutonium-238 oxide; 63%
was in the skeleton and 23% in the liver, which is a translocation even greater
than that expected for plutonium-239 citrate.
Fotf radiological protection purposes all plutonium-238 compounds should
therefore be considered as soluble.
t
11. PLUTONIUM IN THE ENVIRONMENT >f
J.
11.1 Sources and chemical form
Some sources of plutonium either worldwide or local in the environment
are:-
(a) from nuclear weapons tests which have dispersed over 320 kCi
of plutonium-239 and plutonium-240 throughout the world;
(b) dispersal of 17 kCi of plutonium-238 from a nuclear-powered
battery in a space rocket which burnt up in the atmosphere in
1964;
-------
Cc) local dispersal of plutonium-239 at Palomares and Thule as a
result of nuclear weapons breaking up in crashes of US
bombers; *
(d) local dispersal at the nuclear weapons test site in Nevada;
this includes experimental release in operation "Rollercoaster"
(Wilson and Terry, 1968);
(e) liquid waste disposal into the Irish Sea from Windscale.
The predominant chemical form of the plutonium in the atmosphere and on
the ground from these sources is oxide and in the mariVie environment, from liquid
waste discharge, hydroxide. Sufficient data are available from these
dispersals to enable some predictions to be made of the effects of an
accidental release of plutonium oxide from a reactor, chemical plant or
in a transport accident. Some of these effects will be discussed in the
succeeding sections.
11.2 Routes to man ;•
There are tv;o principal routes for plutonium in the environment back to
man; by inhalation, either from a cloud of airborne particles during the
initial dispersal or from resuspension of plutonium already deposited on the
ground or vegetation; by oral ingestion of foodstuffs with surface contamina-
tion or possibly incorporated in vegetation.
The amount of plutonium inhaled directly from the cloud immediately after
the release will depend on factors ,such as air concentration, its variation
with time and breathing rate of the exposed persons. If the release is of
very short duration there is little that can be done to avoid or reduce
exposure. In a release of longer duration some exposure to the population
could be avoided in the immediate vicinity by evacuating the area.
In operation "Rollercoaster" (Wilson ind Terry, 1968} sheep, dogs and
burros, 300 animals in all, were exposed to airborne plutonium oxide generated
by a non-nuclear explosion. Measurements of initial lung deposition and
accumulation due to continued exposure to resuspended activity agreed well with
t
the amounts predicted from measurements of airborne plutonium concentrations
and particle size distributions. This was reassuring,for in previous
experimental work of thi.'; type, code named Test Group 57, the
-------
414
The amount of rcsuspension may be measured in terms of a rcsuspcnsion
factor which is defined as the ratio of the airborne concentration, ug/m to
2
the average ground contamination ug/m ". Measured values of this factor
' —2 —11 —1
on the Nevada test site ranged from 40 to 10 . m (Langham, 1971) and this
wide variability shows the difficulty of predicting airborne concentrations •
from resuspension factors and measurements of ground surface concentrations.
The route back to man via plants and vegetation is not favourable for
plutonium transfer. Fractional uptake -by plants from contaminated soil or
—3 —4
other growth media is of the order of 10 to 10 on a dry weight basis
(Langham, 1971). This discrjjnination coupled with gut uptake of only 10~; %
' in humans makes this food pathway highly selective against plutonium.
One potential pathway through the food chain to man is being investigated
by Wildung et al. (1974). Although previous studies indicate that plutonium
is insoluble and not accumulated by plants, there is a remote possibility
that naturally occurring chelating agents arising from organic decomposition
could complex plutonium in the soil into a soluble form. More research
is needed on this topic and it must be extended to include feeding the
contaminated plants to animals in order to ascertain if th)a high gut
discrimination applies to this plutonium complex.
11.3 Aquatic environment
Plutonium normally found in the aquatic environment is associated with
particles and sediments probably adsorbed in an insoluble form. Marine
invertebrates which form a food supply both to man and to fish may spend
much time close to or in these Sediments and could be exposed|to high
concentrations. At Bikini Atoll where many nuclear weapons were tested
invertebrates were sampled and the mean level was 2350 pCi/kg wet weight and
at Thule after the accident in which a large amount of plutonium was dispersed
in 1968, the levels ranged from 95 to 8QOO pCi/kg. In a more normal situation
around Cape Cod in 1970 the mean values were found to be between 0.1 and
3.5 pCi/kg. Concentration factors in these invertebrates can only be
satisfactorily estimated for an equilibrium situation which does not exist
after an accident but values have been estimated to lia between 300 and 3000.
Vji
In fish, concentration factors relative to sea water range between 20 and
500 for bone, 50 and 170 for liver and 1 to 13 an muse]c (Noshkin, 1972). It
is noted that the normally edible parts of the fish have Uie lowest concentration
but there are special situations where some bone may be eaten such as in tinned
salmon or sardines.
Thus in the marine environment concentration of plutonium can occur.
Further information' in needed however about the chemical form of the plutonium
in those species of fish eaten by man and about the degree of absorption of
these forms from the human gut.
-------
11.4 Experience at Palomarf'S / "I J~
Following the dispersal from nuclear weapons by a non-nuclear explosion
at Palomares, crops were removed from the area where plutonium contamination
2
was above 5 yjg/m" and the ground w&s ploughed to a depth of 25 cm to minimise
the possibility of resuspenr.ion. The area involved was 550 acres. At ground
2
contamination levels over 500 urj/m , the vegetation and top soil were stripped
off and put into drums for return to the USA. About 5.4 acres were involved
(Langham, 1968). •
In follow-up studies of 100 potentially contaminated residents no
detectable amounts of plutonium were found in the chest hut the lower limit
of detection v;as initially 40 nCi, and only later reduced to 16 nCi. Urine
samples collected over 24-hour periods were all found to be negative but this
is not surprising as the plutonium was insoluble. Thus residents may have
been contaminated but not at detectable levels.
Measured air concentrations in the village even under conditions of high
15 -i
wind velocities were low. In 1966 a value of 0.38 x 10 uCi/on was
15 ^
obtained and in 1967 the value was lower at 0.09 x 10 uCi/qn . For
continuous exposure to insoluble plutonium the air levels given for adult
workers in ICRP Publication 2 (1959) are 1 x 10"11 ^Ci/cm which is 104 to
10J times higher than the measured value at Palomares. If the air concentration
measurements are representative of continuous exposure then the hazard is very
low. By implication the consequences of dispersal of a few kilograms of
plutonium dioxide in a limited area of undeveloped or agricultural land are not
too serious but in a developed area the cost of decontamination could be very
high. '' I
1^.5 Plutonium in man
Worldwide contamination of the atmosphere from nuclear weapons tests has
produced measurable amounts of plutonium in the air at ground level. For
example, in 1965 and 1966 in mid-northern latitudes the measured air
-4 3
concentration was 10 pCi/m (Parker, 1973). Using the metabolic models in
ICRP Publication 19, it is possible to calculate tissue deposition from
continuous breathing of this concentration. The daily alveolar deposition
would be 3 x 10~ pCi and if the retention half-life is 500 days then)1 the
equilibrium amount in the lung is about 0.2 pCi. Transfer from lung through
the blood to the bone would amount to 0.5 x 10~ pCi per day and in 10 years
the accumulated amount in the skeleton would be about 0.2 pCi.
Hurley (1971) published data on tissue concentrations in humans. He
found an average concentration in the lung of 0.45 pCiAg, the range in tone
0.04 to 0.12 pC.lA$ and a daily dietary intake of 7 x 10~3 pCi. The values
for lung and bone are in reasonable agreement with those calculated from the
air concentration levels in the previous paragraph. This agreement gives
Some confidence Jn the ICRP models.
- 25 -
-------
The daily transfer from the diet.to th<; blood is the daily intake,
*-*• O 7 x ^o~ pCi, multiplied by the gut discrimi nation factor, 10~ , which equals
-9
7 x 10 pCi. This is an extremely low daily intake to the blood and even
after 50 years this would only lead to. a bone level of 8 x 10~ pCi/kg according
to the ICRP metabolic model. However j' dietary contamination from plutonium
in fallout under most circumstances has probably had a negligible effect on the
concentrations found in the bone of humans.
12. CHEMICAL TOXICTTY
Statements have recently been made in the popular scientific press that
plutonium is not only toxic due to its radioactivity but also due to its
Chemical nature. There are no experimental data available on the chemical
toxicity of plutonium-239, 240 and 242, the long-lived alpha-emitting isotopes,
but some inference can be drawn from experimental data on related elements.
The most stable oxidation state of plutonium is +4 in biological fluids
and it has an ionic radius of 0.90 A. Related elements are cerium and
neptunium which both have stable oxidation states at +4 and both have ionic
radii of 0.92 A which is close to that of plutonium. It is noted that •
neptunium has no stable isotopes but neptunium-237 has a half-life of 2.2 x 10
years and this is sufficiently long to allow the acute symptoms of chemical
toxicity to be separated from the late effects of irradiation.
The acute and sub-acute toxic effects of cerium in the liver of rats
are just detectable after the intravenous injection levels of 4 tag/kg of body
weight (Snydcr et al., 1959) and for neptunium at 3 mg/kg of body weight
(Markham, 1967). These levels correspond to an intravenous intake in a 70 kg
man of over 200 mg and may be compared with the maximum pennissilile body burden
(ICRP Publication 2, 1959) of 0.64 jig (0.04 nCi) of the alpha-emitting isotopes
plutonium-239,' 240 and 242. Hence, the acceptable plutonium mass in the body
from radiological protection considerations is 330,000 times less than that
which might be expected to produce detectal>1.e chemical effects in the liver.
The mass of inhaled plutonium, determined from dog experiments, which
might be expected to cause death within days due to severe oedema and
haemorrhage in the lung is over 8 mg (500 jjCi). This mass of plutonium
required to produce acute effects due to radioactivity is still less than ,
the estimated 200 mg which might be expected to just cause toxic effects when
injected into the blood. It should be noted that it would not be possible
to transfer from the lungs into the liver sufficient plutonium to cause
chemical toxicity.
It must be concluded that the mass of plutonium-239, plutonium-240 or
plutonium-242 required to produce either acute or late biological effects due
to alpha activity is considerably lower than that expected to cause toxic
effects in the liver due to its chemical nature.
- 26 -
-------
13. SUMMARY
/ ~
For the proper protection of persons exposed to plutonium isotopes and
higher actinides, there are five important requirements:-
(1) Evaluation and acceptance of basic dose standards for the
exposure of body organs, particularly bone, liver and lung
(2) Derivation of standards for maximum permissible air
concentrations and annual intakes
(3) Facilities for the assessment of the amount in the body by
measurements of urinary excretion rate, or by external counting
of X- or ])-rays emitted by incorporated plutonium
(4) Availability of methods for the treatment of over-exposed
cases
(5) Derivation of acceptable ground contamination levels in
areas where plutonium has been accidentally released.
All these topics have been discussed in this report. It is noted
that knowledge is better founded in some of these topical than Jn others.
More consideration of the basic dose standards is required, especially
in terms of the relative effectiveness of external radiation and incorporated
alpha emitters. It is unlikely that information on cancer incidence due
to exposure of groups of people to plutonium will become available in the
next few decades therefore the greatest effort must be made to study the
biological effect of plutonium, relative to radium in many animal species.
In this way the fullest use can be made of the human experience with radium-226
and radium-224.
The second topic involves knowledge of a metabolic model for the trans-
location to and retention in body organs of plutoniun entering the body after
deposition in the lung or at a wound site. The model proposed by the ICRP
Task Group and given in ICRP Publication 19 (1972) is adequate and has the
advantage of not over-emphasising a single organ for it implicates bone, liver
and lung, whereas in ICRP Publication 2, the liver was not, considered a very
vulnerable tissue. The major problem in the metabolic model concerns the
lymph nodes and lymphoid tissue associated with lung clearance where there
are uncertainties both about the retention and about the mass of these tissues
in the human.
Measurement of the amount present in the body, the third topic, gives
rise to difficulties, but improvements are continually being made in the
techniques. Reliability of the interpretation of urinary excretion rate in
terms of plutonium body content will improve ac more data become available on
body content at death, made from analyses of tissues obtained at post mortem,
- 27 -
-------
8
U
and its relation to the urinary excretion r;il:es measured before death. So
far all the indications are that the current methods overestimate body content.
The technique of measuring body content by external counting of X-rays from
plutonium or gamma-rays from amcricium-r241 are improving continually but still
more improvements are required to obtain a satisfactory sensitivity for
detecting the amounts of these materials in the lung.
The fourth topic is very important in cases of accidental over-exposure.
The new technique of lung lavage offers a good possibility of removing insoluble
compounds from the lung. Inside the tody, the problems of removal of plutonium
from intracellular sites has not been successfully solved and more research
iis required in this field.
The final topic listed above will lie important if large quantities of
plutonium are accidentally released to the environment. There is some
experience of ground contamination at the sites of weapons tests and from the
accidents at Palomaces and Thule, and this will be very useful in setting
acceptable ground contamination levels. Naturally, these levels would vary
from place to place and country to country depending upon factors such as climate,
ground usage, population, density, etc. \\
Finally, the best indicator of the adequacy of radiological protection
standards is the health of those people who are exposed to these materials.
It is therefore important that health statistics as well as information on
work histories and smoking habits be collected and analysed for these
individuals.
14. SUMMARY OF NKPB RESEARCH PROGRAMMES ,
The Board recognised the biological problems posed by the large—scale
use of plutonium and the associated higher actinides in the nuclear power
programme and consequently set up an extensive biological research programme.
The main areas of research are:- '
1. Study of the comparative metabolism of plutonium, amcricium
i
and curium in animals following entry by four main routes;
inhalation, ingestion, wounds and intravenous injection.
The amounts of activity used are comparable with a few body ); j1
burdens in humans. The effect of factors such ad particle
sixe, chemical form, solubility and binding in biological
fluids on the translocation process are being studied. In
addition, attempts are being rrtide to elucidate the fundamental
mechanisms of urinary and faecal excretion.
2. Study of tlio. biological consequences of deposited plutonium
in lung, bone, liver, lymph nodes, skin and gonads.
-------
3. Development of techniques and regimes for the removal of >T T Q
plutonium from the body. Tiv>ne include:
(i) removal of plutonium by injection or inhalation
(ii) development of techniques for.washing insoluble
particles from the lung
(iii) development of methods for increasing the release
of intraceljular plutonium.
4. Assessment of dose from internally-deposited actinides:
(i) improvement of methods for estimating body content
by external counting over the chest and by
measurement of urinary excretion rate
(ii) analysis of selected autopsy samples in order to
estimate body content at death.
15. ACKNOV/LEDGU-1EHTS
The authors wish to thank Mrs. Elaine Henry and Miss Anne Wotherspoon
for their help in the preparation of the manuscript.
- 29 ~
-------
420 16.
Adams, N. and Watts, L.M.
NRPB Report (in Preparation) i
Albert, R.E., Burns, F.J. and Heimback, R.D. The effect of penetration
depth of electron radiation on skin tumour formation in the rat.
Radiat. Res., jiO, 515 (196?).
Bair, W.J. Toxicology of Plutonium. Advan. Radiat. Biol., Ji, 255, (1974).
Bair, W.J. and Thompson, R.C. Plutonium: Biomedical Research.
Science, 183, 715 (l97'i). |
Bair, W.J., Richmond, C.R. and Wachholz, B.W. A radiobiological assessment
of the spatial distribution of radiation dose from inhaled plutonium.
Wash. 1320, DBER, USAEC, Washington. (l97'i) .
Bair, W.J., Ballou, J.E., Park, J.F. and Sanders, C.L. Plutonium in soft
tissues with emphasis in the respiratory tract. IN Uranium, Plutonium
and Trans])] utonic Elements. Edited by H.C. Hodge, J.N. Stannard and
J.B. Hursh, Berlin, Springer Verlag (1973).
Bair, W.J. and Willard, I). II. Plutonium inhalation studies. IV Mortality
in dogs after inhalation of PuP^O . Radiat. Res., l_g, 811 (1962).
Ballou, J.E., Park, J.F. and Morrow, W.G. On the metabolic equivalence
of ingested, injected and inhaled 239pu citrate. Health 'Phys ., 22,
857, (1972). —
Beach, S.A. SEREACH, a digital compxiter program for the estimation of body
content of plutonium from urine data. Health Phys., 2>i , 9 (1973).
Beach, S.A. and Dolphin, G.W. A ..study of the relationship between X-ray
dose delivered to the thyroids'1 of children and the subsequent development
of malignant tumours. Phys. Med. Biol., j>, 583 (1962).
Beach', S.A. and Dolphin, G.W. International Atomic Energy Agency, Assessment
of radioactivity in man. Proc. Symposium on the Assessment of Radio-
active Body Burdens in Man, Heidelberg, May 11-16, 1964, Vienna,
IAEA/JI,0/WI10 , p. 603 (196'j). V
BEIR Report. National Academy of Sciences/National Research Council. The
effects on populations of exposure to low levels of ionising radiation.
Report of the Advisory Committee on the Biological Effects of Ionising
Radiations, Washington, National Academy of Sciences (1972).
/• ' '.1'
Bc/nsted, J.P.M., Chi»^«=B- , Taylor, D.M. and Sowby, F.I). The carcinogenic
effects of amnricium-241 and plutonium-239 in the rat. •' Brit. J. Radiol.,
38, 920 (1965)'.
Boocock, G. and Popple-well, U.S. Distribution of plutonium in scrum proteins
following intravenous injection into rats. Nature 208, 282, (l
-------
Buldakov, L.A. and Lyubchansky, EiR. Report ANL-trans-864, Argonne National
Laboratory, Argonnc, Illinois, (translated from a Russian Report) (1970). 4 Li 1
(Buldakov, L.A., Lyubchansky, E.R. , Moskalov, Yu.I. and Nifatov, A.P.
IN Problomy Toksikologii Plutoniya Atomizdat, Moscow, 1969-
Translated (Problems of plutonium toxicology) by A.A. Ilorvath, Lovelace
Foundation, Albuquerque, New Mexico. USAEC LF-7R-41, p.149 (1970).
Buldakov, L.A., Nifatov, A.P., Erokhin, R.A. and Filippova, L.G.
IN Remote after effects of radiation damage. Ed, Yu.I. Moskalcv.
pp.350-355. Atomizdat, Moscow. (Translated in AEC-tr-7387, 381-38?)(1971)
*
Campbell, E.E., Milligan, M.F., Moss, W.D., Schulte, II.F. and Mclnroy, J.F.
Plutonium in autopsy tissue. Los Alamos Scientific Laboratory Document,
LA-4875- (1973).
Court Brown, W.M. and Doll, R. Mortality from Cancer and other causes after
radiotherapy for ankylosing spondylitis. Brit. Med. J., ii, 1327 (1965).
Cowan, M. Plutonium contamination from one-point detonation. Report WT-1510,
Sandia Corp. Albiiquerque, New Mexico, (i960).
Dolphin, G.W. International Atomic Energy Agency. Assessment of radioactivity
in man. Proc. Symposium on The Assessment of Radioactive Body Burdens
in Man, Heidelberg, May 11-16, 1964, Vienna, IAEA/ILO/WHO, p.589 (1964).
Dolphin, G.W. and Marley, W.G. Risk evaluation in relation to the protection
of the public in the event of accidents at nuclear installations. Harwell,
UKAEA Health and Safety Branch, AIISB(RP)R93 (1969). U
Dolphin, G.W. The biological problems in the radiological protection of workers
exposed to 239pu. Health Phys., 20, 549, (l97l).
Dolphin, G.W. Problems, associated with setting safe levels for working with
plutonium. Health Phys., 22, 937 (1972).
Doniach, I. Effects including carcinogcncsis of iodinc-131 and X-rays on the
thyroid of experimental arf-imals. Biology of Radioiodiiiej p.277 (Ed . L.K. Bustad)
Pergamon Press, Oxford. (1964).
Durbin, P,W. Plutonium in man: A twenty-five year review. California University,
Berkeley. Donner Laboratory, Report No. UCRL 20850, June (l97l).
Durbin, P.W. IN Radiobiology of Plutonium, p.469, Edited by B.J. Stover and
W.S.S. Lee. J.W. Press, University of Utah (1972).
Erokhin, R.A., Koshurnikova, N.A., Lemberg, V.K., Nifatov, A.P. and Puzyrev, A.A.
Gig. Tr. Prof. Zabol., 13. (5), 6l, (1969).
Goss, S.G. The risk of death from radiation-induced cancer as estimated
from the published data on the Japanese atomic bomb survivors.
Harwell, National Radiological Protection Board, NR!*B-R20 (1974).
Harley, J.II. Worldwide plutonium fallout from weapons tests. IN Environmental
Plutonium Symposivm. Los Alamos Scientific Laboratory, Report LA-4756
(1971).
Hempelmann, L.H., Richmond, C.R. and Voclz, G.L. Twenty-seven year study of
selected Los Alamos plutonium workers. Los Alamos Scientific Laboratory,
Report LA-51'iSr-MS (1973).
Holliday, B., Dolphin, G.W. and Dunster, H.J. Radiological protection of
workers exposed to airborne plutonium particulate. Health Phys., 18,
529 (1970).
International Commission on Radiological Protection. Permissible Doses for
Internal Radiation. 1CRP Publication 2, Pergainon Press (1959).
-------
422
International Commission on Radiological Protection. Recommendations of the
International Commission on Badiofogical Protection. ICIIP Publication 9,
Pergamon Press (1966).
International Commission on Radiological Protection. Metabolism of Compounds
of Plutonium and Other Actinides. ICRP Publication 19, Pergamon Press
(1972). ,
International Commission on Radiological Protection. Reference Man.
(To be published).
Jablon, S. and Kato, H. Mortality among A-bomb survivors 1950-70.
Hiroshima Atomic Bomb Casualty Commission, JNIH-ABCC Life Span Study,
Report No. 6 (1972).
Jee, W.S.S. Distribution and toxicity of "PU in'bone. Health Phys.. 22,
583 (1972). , —
Lafuma, J. La contamination radioactive interne. Paper presented at the
French Society for Radiation Protection Paris (1974) and Personal Communication.
Lagerquist, C.R., Hammond, S.E., Bokowski, D.L. and Hylton, D.B. Distribution
of plutonium and americium in occupationally exposed humans>as found from
autopsy samples. Health Phys., 25, 581 (1.973). ,
Langham, W.H. The application of excretion analyses to the determination of
body burden of radioactive isotopes. IN The Measurement of Body
Radioactivity, papers read at a conference held at Leeds April 16-17, 1956
p.95. Brit. J. Radiol., supplement no. 7 (1957). J,|
Langham, W.H. Plutonium distribution as a problem in environmental science
IN Proc. Symposium on Environmental Plutonium, Los Alamos Scientific
Laboratory, August 4-5, 1971. Los Alamos Scientific Laboratory Report LA-
4756, December (l97l).
Langham, W.H. The problem of large area plutonium contamination. Seminar
paper 002 Bureau of Radiological Health, Public Health Service US Department
of Health, Education and Welfare (1968).
Lebel, J.L. and Watters, R.L. Study of the translocation of plutonium and
americium from puncture wounds. Fourth International Progress Report,
June 16, 1-971 - June 15, 1972. Colorado State University, Fort Collins,
Dept. Radiology and Radiation Biology, COD-1787-16 (1972).
Lister, B.A.J., Morgan, A. and Sherwood, R.J. Excretion of plutonium following
accidental skin coratamination. Health Phys., £, 803 (1963)..
Lloyd, E. and Marshall, J.H. IN Radiobiology of Plutonium, p.377.
Edited by B.J. Stovet and W.S.S. Lee. J.W. Press, University of Utah (1972).
Loveless, B.W. Personal Communication (1974). '
Lundin, F.E., Wagoner, J.K. and Archer, V.E. Radon daughte* exposure and
respiratory cancer quantitative and temporal aspects. Virginia USA,
National Institute for Occupational Safety and Health and National Institute
of Environmental Health Sciences, Joint Monograph No. 1 (l97l).
Lushbaugh, C.C. and Langham, J. A dermal lesion from implanted plutonium.
Archs. Dcrmat. £6, 461, (1962).
McClcllon, R.O. and Ruuprecht, F.C. Fission product inhalation program.
Annual Report (19721, October 1, 1971 - September 30, 1972. Report No. LF-45,
Albuquerque, Lovelace Foundation (1972).
Mahlum, D.D. Neptunium-237 toxicity in rats II Intracellular distribution of
neptunium and cerium in rat liver. , Toxicology and Applied Pharra. 11.
264-271 (1967). —
Mays, C.W. and Dougherty, T.F. Progress in the beagle studies at the
University of Utah, Health Phys. 22, 793 (1972).
-------
Mays, u.W., Lloyd, II.1). and Athcrtcm, D.K. Personal Communication (I97'i).
Mercer, T.T. On the role of particle fi.ze in the dissolution of lung burdens.
•_ Healtli Phys., 13., 1211 (196?).
490
Morrow, P.E. and Casarett, L.J. An experimental study of the deposition and '-'
retention of plutonium-239 dioxide norosol. IN Inhaled Particles and
Vapours, p.l67- Kdited by C.N^' Davies, New York, Pergamon Press (l96l).
Mutscheller, W.II. Am. J. Roentgcnol. Radium Therapy 1/3, p.65 (1925).
Nolibe, I). CEA, Montrouge. Personal Communication (l97'i).
Norcross, J. A. and Newton, C.E. Jr. US transuranium registry: a progress
report. Health Phys., 22, 887 (1972).
Norwood, W.D., Norcross, J.A., Newton, C.E., Hyltipn, D.B. and Lagcrquist, C.
IN Radiomiclide Carcinogenesis. Proceedings of the 12th Annual Hanford
Biology Symposium at llicliland, Washington, May 10-12, 1972. Oak Ridge,
Tennessee, USAEC Technical Information Centre,' AEC Symposium Series 29,
p.'i65 (1973).
Noshkin, V.E. Ecological aspects of plutonium dissemination in aquatic
environments. Health Phys., 22, 537 (1972);
Park, J.F., Bair, W.J. and Howard, E.B. IN Pacific Northwest Laboratory,
Annual Report for 1967 to the USAEC Division of Biology and Medicine,
Vol. 1. Biological Sciences, p.322. BNWL-714 Vol. 1. Battelle Northwest
Laboratories, Richland, Washington (1968). U
Park, J.I1'., Bair, W.J. and Busch, 11.H. Progress in beagle dog studies with
transuranium elements at Battelle Northwest. Health Pliys., 22, 803 (1972).
Parker, II.M.. Plutonium, Industrial Hygiene, Health Physics and related aspects
in Uranium, Plutonium and Transplutonic Elements, Chapt. 14, p.6l3,
Ed. by H.C. Hodge, J.N. Stannard and J.B. Hursh, Berlin, Springer Verlag,
Pocliin, i;.K. The mass of the tracheobronchial lymph glands. Health Phys.,
12, 563 (1966).
Popplcwell, D.S., Stradling, G.N. and Ham, G. The determination of
plutonium in urine by ultrafiltration. Harwell, National Radiological
Protection Board, NRPB-R17 (1973).
Ilichmond, C.R. and Sullivan, E.M. Annual Report of Diomedical and Environ- •
mont-al Research Programme LA-5633-PR P-30, Los Alamos Scientific Laboratory,
New Mexico (l97'i) •
Rowland, II.E. Radiological and Environmental Research Division Annual
Report, Argonnc National Laboratory Report ANL-8060, Part II, Appendix A
Exposure data for radium patients, p.289, Argonnc, Illinois (l973J.
Rundo, J., Star/ylt, P.M. and Sedlot, J. The excretion rate of plutonium
10,000 days after ncqnisition. Fifth International Congress of Radiation
Research, Seattle, July (l97'i).
Russell, W.L. Studies in mammalian radiation genetics. Nucleonics, 23,
p.53, (1965). ~"
•t:
Sanders, C.L. Tho distribution of inhaled plutonium-239 dioxide particles
within pulmonary inacrophages. Archives of Environmental Health,
18, 905 (1969).
Snridrrs, C.L. find Adoe, R.R. Ultrnstructural localisation of inlialcd
*-5Jpu00 particles' in alveolar cpitlioliiim ond macrophages. Health Phys.,
18, 293, (1970).
-------
Sanders, C.L., Adeo, E.H. and Jackson, T.A. Fine structure of alveolar
areas in the lung following inhalation of 239fu09 particles. Arch. Environ.
Health, 22, 525 (197l).
Sanders, C.L. and Jackson. T.A. Induction of mesotholiornas and sarcomas
from "hot spots" of 239pu02 activity. Health Phys., 22, 755 (1972).
Sanders, C.L. Personal Communication (1972).
Schofield, G.B. Personal Coramunication (1974).
Schofield, G.B. and Dolphin, G.W. UK experience on the medical aspects of
radiological protection of workers handling plutonium. Annals. Occup. Hyg.,
(in Press).
,Schofield, G.B. , Howells, II., Vard, P., Lynn, J.C. and Dolphin, G.W.
Assessment and management of a plutonium contaminated wound case.
Health Phys. 26, 541 (1974).
Smith, H. and Morgan, R.M. The effect of acute and sub-acute treatment with
diethylcnotriaminepentaacetic acid on the hepatic function of mice.
Toxicology Vol. 2 p.43 and p.153 (1974).
Snyder, F., Cress, E.A. and Kyker, G.C. Liver lipid response to intravenous
injection of rare earths in rats. Journal of Lipid Research, 1, 125-131
'(1959). '-
Spicss, H. and Mays, C.W. Bone cancers induced by 22/1Ra (Tli X) in children
and adults. Health Phys., 1_9, 713 (1970).
Stannard, J.N. Plutonium in the environment. IN Uranium, Plutonium and
Transplutonic Elements, p.669. Edited by H.C. Hodge, J.N. Stannard
and J.B. Hursh, Berlin, Springer Verlag (1973).
Stather, J.W. and Howden, S. The effect of chemical form on the clearance of
plutonium-239 from the respiratory system of the rat. Health Phys.
(in Press). ',• I
Stather, J.W., Carter, R.F. and Ilowden, S. A method for investigating the
metabolism of the transportable fraction of plutonium aerosols.
Phys. Med. Biol. (in Press).
Stevens, W. , Bruengor, F.W. and Stover, B.J. In vivo studies on the inter-
actions of PuN with blood constituents. Rad. Res., 33, 490 (1968).
Stover, B.J1., Atherton, D.n., Bruenger, F.W. and Buster, D.S. Further studies
of the metabolism of Pu239 in adult beagles. Health Phys., 8, 589 (1962).
Tamplin, A.R. and Cochran, T.B. Radiation standards for hot particles.,, A
report on the inadequacy of existing radiation protection standards ''
related to internal exposure of man to insoluble particles of pluLonium
and other alpha-emitting hot particles. Washington, National Resources
Defense Council (1974).
Taylor, D.M. The metabolism of plutonium in adult rabbits. Brit. J.
Radiol., 42, 44 (1969).
Taylor, G.N., Jco, W.S.S., Williams, J.L. and Slmbestari, L. IN HadioMology
of Plutonium, p.1)05. Edited by B.J. Stover and W.S.S. Loo. J.W. Press,
University of Utah (1972).
UICC Committee on Professional Education (eds). p.l67 IN Clinical Oncology,
A Manual for Students and Doctors. Springcr-Verlag, Berlin (l973).
UNSCliAR Ionising Radiations: Levels and Effects. New York, United Nations,
(1972).
- 3'i -
-------
Upton, A.C., Randolph, M.L. and Conklin, J.W. Late effects of fast
- neutrons find gamma rays in mice as influenced by the dose rate of
irradiation; induction of ncoplasia. Had. Hes. 41, '16? (1970).
Vaughan, J. Distribution, excrcti'qn and effects of plutonium as a bone seeker
IN Uranixim, Plutonium and Tran'.iplutonic Elements. Edited hyll.C. Hodge,
J.N. Stannard and J.B. Hursh, Berlin, Springer Verlag (1973).
Watts, L.M. Determination of the rates of clearance of insoluble compounds
of plxitonium from the lung. Harwell, National Radiological Protection
Board, NRPB-R22 (l97't)-
Weeks, M.I1., Katz, J., Oakley, W.D., Ballou, J.E., George, L.A., Bustad, L.K.
Thompson, R.C. and Kornberg, H.A. Further studies on the gastrointestinal
absorption of plutonium. Rad. Res. ^, 339 (l9p6).
Wildung, R.E., Garland, T.R., Dracker, M. and Sclmeidcrman, G.S. IN Pacific
Northwest Laboratory Annual Report for 1973 to'the USAEC Division of
Biology and Medicine, Richland, Washington, Battelle Northwest, BNWL-1850
(Part 2) (I97'i).
Willard, D.II. and Park, J.F. IN Pacific Northwest Laboratory Annual Report
for 1969 to the USAEC Division of Biology and Medicine. Vol. 1, Life
Sciences. Part 1. Biomcdical sciences edited by R.C. Thompson, Richland,
Washington, Battelle Northwest, BNWL-1306 (Part l) (1970).:
Wilson, R.II. and Terry, J.L. Plutonium uptake by animal^,! exposed to non-
nuclear detonation of plutonium-bcaring weapon simulant. Report No. POR-2512.
Washington, Defense Atomic Support Agency (1968).
-------
to
05
TABLE 1. SOME IMPORTANT TRANSURANIC NUCLIDES PRODUCED IN NUCLEAR REACTORS
Isotope
2^Vu
25-V ™«,M«\^^
2*°P»(n,Y)2«Pu
~ Pu(n,v) ru
i*!! — ' ^ Ani
241 / \ 242 8 242 ~
Am(n,Y) Am i A hr^ ^m
24^Pu^ ^(n*)244*. rf^ ^Cm
244Cm(n,Y)245Cm(n,Y)246Cm
Principal
Mode of
Decay
a , Y -rays
a , X-rays
a
P
a
""a, Y -rays
a
a
a
Relative Activities at
fuel irradiations
1000 Mwd/t
-
1
0.35
23
-
-
-
-
-
24000 Mwd/t
3-8
1
1-9
560
0.01
1.3
190
7.8
•:
Spontaneous
fissions/min
per d/min
1.8 x 10"11
4.4 .x_10~12
4.9 x 10~8
1.3 xlO-29
5-3 x 10"6
-12
2.3 x 10
6.2 x 10"8
1.3 x 10'6
3.2 x 10~4
-------
TABLE 2. THE SPECIFIC ALPHA ACTIVITY OF PARTICLES OF Pu02 AND NITRATE FROM FUEL IRRADIATED
TO A LEVEL OF 2060 MWd/t AND UNIT DENSITY EQUIVALENT AERODYNAMIC DIAMETER OF I urn
Compound
Pu02
Pu(NO..)45H20
Density
g/cm5
11.5
2.9
Mass of Pu/oarticles
(e)
1.4 x 10~lj
1.3 x 10"1-5
dPm(239Fu+ 24°Pu)
0.03
0.03
No. of particles
equivalent to 40 nCi
2.9 x 106
3.1 x 10^
CO
-------
CO
CO
TABLE 3- PERCENTAGE DISTRIBUTION OF PLUTONIUM IN TISSUE OF BEAGLES AFTER INHALATION AND INTRAVENOUS INJECTION
AND IN RABBITS AFTER INTRAMUSCULAR INJECTION
Duration
Percentage distribution:
i
Lungs
Thoracic Lymph Nodes
Skeleton
Liver
Reference
Inhalation
(beagle)
Pu02
11 yr
9
40
5
1 5^-
Park et al.
1972
Pu nitrate
,^250 days
33
1.5
26
14
Park et al.
1968
Intravenous Injection
(beagle)
Pu citrate Pu citrate
1
I'O'O days | 4 yr
i
i
1
•
29
0.4
38
16
Bailou et al .
1972
-
-
44
••- !3
Stover et al.
1962
Intramuscular Injection
(rabbit)
Pu nitrate
-
1 yr
-
~ 31
1
Taylor et al .
1969
-------
429
TABLE >t. DISTRIBUTION OF PLUTONIUM IN IIUMANS AS MEASURED IN TISSUES
OBTAINED AT AUTOPSY
Years
of
Exposure
5
-
21
13
-
11
6
12
9
7
11
k
Lung
dpm/kg
97600
34100
14700
8540
8460
6330
5930
4050
3960
2690
2520
2510
Liver
clpm
527
505
5460
4880
-
16700
102
15900
1470
425
-
132
Concentration
Ratio
TLN*/Lung
0.009
0.3
13-3
17-7
66.7
13-4
0.4
0.8
1.7
6.0
25-5
' 4.4
Bone/Liver
i
t
2.3
0.8
0.4
0.88
-
1.0
2.3."
3.2 ,
1.3
0.6
-
6.7 !
Reference
B
B
D
A
A
A
B
C
D
B
A
D
*TLN = Thoracic Lymph Nodes
References: A = Campbell et al. (l97j>)
B = Lagerquist et al. (1973)
C = Norwood ct al. (1973)
D = Schofield and,, Dolphin (1974)
-------
430
TABLE 5. CHROMOSOME ADERMTIONS VoUND IN BLOOD LYMPHOCYTES OF INDIVIDUALS
KNOWN TO HAVE BEEN ACCIDENTALLY CONTAMINATED WITH Pu
Cells
Scored
1000
500
1000
500
Dicentrics
, 2
14
12
2
Accntrics
12
22
34
'- 8
Exposure
Six years after inhalation
of about 0.3 ^Ci
Wound puncture contaminated
with 14 nCi. Schofield et al..
1974 .If
15 years exposure to Pu with
an estimate of about 0.04 |j,Ci.
External radiation 10 rads
Second sampl'e 7 years later
with no further exposure
-------
TABLE 6. BASIC DOSE STANDARDS EXPRESSED BOTH AS REM IN A YKAK AND AS RAD IN
A YEAR FOR ORGANS OF IMPORTANCE IN HIE PROTECTION OF PERSONS
EXPOSED TO PLUTONIUM, FROM ICRP PUB. 9 (1966)
431
Organ
Gonads , red
bone marrow
(whole body
irradiation)
Liver)
Lung
Bone
MPD for adults
at work
Rein in a
year
5
15
30
i
Rad in a
year*
—
1.5
0.6
Dose Limits
for Members
of the Public
Rem in a
year
0.5
U5
3
Rad in a
year*
—
0.15
0.06
* The radiological protection units are derived from the energy
deposition units by tire use of a quality factori Q = 10 for
liver and a modifying factor N = 5 and Q = 10 for bone.
-------
TABLE 7- ESTIMATED VALUES OF RISK COEFFICIENT FOR VARIOUS TYPES OF
CANCER IN EXPOSED POPULATION GROUPS FOR EXTERNAL y AND a RADIATION
CO
to
Biological Effect
Leukaemia
All cancers
Leukaemia
All cancers in
X-ray field
Bone sarcomas
Bone sarcomas
Lung cancer
Bone sarcoma
Lung cancer
Population
Group
A-bomb survivors
A-bomb survivors
Ankylcsing
spondylitics
Ankylosing
spondylitics
Radium-226 cases
Radium-224 cases
Miners exposed to
radon
Thorotrast patients
Rats exposed to Pu
Rats exposed to Pu
Type of
Radiation
Y
Y
X-rays
X-rays
- ---a
a
a
a
a
Risk Coefficient
Cancers/10" man-rad
30
100
10
50
801
90
302
400
650
Reference
Goss (1974)
Goss (1974)
Dolphin and Marlev
(1969)
Dolphin and Mar ley
(1969)
This paper
Spiess and Mays
(1970)
Lundin et al. (l97l)
Thijs paper
This paper
Calculated from data given by Rowland (1973) assuming a linear .relationship for cases with
average accumulated dose to bone of less than 10.000 rad.
Calculated from data on risk coefficients taken from Lundin et'al. (l97l), for US uranium
miners, Newfoundland, fluorospar miners, British haematite miners, US hard-rock miners,
Portuguese thorotrast patients and Danish thorotrast patients weighted by the square root
of the number of lung cancers attributed to radiation in the survey.
-------
TABLE 8. PERCENTAGE OF INHALED PLUTONIUM-239 ACTIVITY TRANSFERRED TO BLOOD FROM LUNG AND INTO
.BONE AND LIVER, HALF-LIVES OF RETENTION AS USED TO CALCULATE (MPC)a AND MPAI FOR SOLUBLE,
INSOLUBLE, CLASS ¥ AND CLASS Y COMPOUNDS
Compound
Inhaled
Soluble
Insoluble
Class W?
Class Y2
Percentage
Transfer
to Blood
.^-
25
_
124
54
Percentage ot Inhaled Activity in Organ and Half-Life
Bone (7000 g)-
Amount
%
20
-
5.4
2.25
Half-life
(days)
7-5 x 104
-
3.6 x 104
3.6 x 104
Liver (1700 g)
Amount
"jo
3-8
-
5-4
.- 2.25
Half-life
(days)
3 x 104
•
1.5 x 104
1.5 x 104
Lung (1000 g)
Amount
%
-
12.5
15
15
Half-life
(days)
•
365
50
500
Maximum
Permissible
Concentration
(MPCa)
-12 , T
x 10 |iCi/cnT
2
40
8
18 •
Maximum
Permissible
Annual Intake3
Inhalation
,iCi
5 x 103
0.1
O....D2
0.04
Oral
iiCi
27-5
220
"..—
-
1. As defined in ICRP Publication 2 (1959)
2. Solubility classes and lung model defined in ICRP publication 19 (1972)
3. Only half this amount is permitted in a single intake (vide ICRP--i£ublication 9)
4. Deposition fractions in the lung compartments for'l ^m AMAD particles given in ICRP Publication 19 (1972)
CO
CO
-------
434
TABLE 9- THE VARIATION WITH PARTICLE SIZE OF THE NUMBER OF
PARTICLES AND THE NUMBER OF CELLS IRRADIATED FOR A CONSTANT
ACTIVITY OF 0.016 (iCi OF PLUTONIUM-239 OXIDE
Particle
Diameter
(micron)
0.1
1
10
Particles
per
0.016 nCi
4.9 x ]07
4.9 x 10 l
4.9 x 10
Irradiated
Cells
Per Particle1
270
280
380
Total Cells
Irradiated
1.3 x io10
1,.4 x IO7
1-9 x 10*
Cell volume assumed to be 10 cm
-------
Figure!. Plutonium induced osteogenic sarcomas in rat
Incidence
50
4O
.30
2O
IO
X
o
X
Inhaled Pu Citrate (Buldakov & Lyubchansky, I97O)
Inhaled ammonium plutonium pentacarbonate (Buldakov s Lyubchansky, I97O)
Intratrachea! Pu nitrate and sodium plutonyl triacetate (Erokhin etal., 1969)
Intra t subcutaneous injection plutonium citrate ( Buldakov et al., 1971)
I ntrcperitoneal injection PuO2 (Sanders & Jackson, 1972}
Inhaled PuO2 (Sanders, 1972)
Risk coefficient - 3-9% per lOOrads
Q"
DO
Average dose to skeleton in rods
2OO
3OO
4OO
500
CO
en
-------
Figure 2. Plutonium induced lung cancer in experimental animals
CO
Incidence
50 r
40
3O
20
X Inhaled Pu citrate, rat, ( Buldakov & Lyubchansky, I97O)
JD Inhaled ammonium plutonium pentacarbonate, rat,(Buldakov & Lyubchansky. I97O)
A Inhaled PuO2, rat, (Sanders, 1972)
Risk coefficient = 6-5 °/o per IOO rods
IOO
Average dose to lung'in rods
2OO
3OO
4OO
X
500
-------
I
National Radiological Protection Board A o 'n
^ .f
R15 The NRPB Interim Radiation Dose Record Service. E. Green'slade.
ISBN 085951 015 8.
R16 A Thermoluminescent Personal Doseineter Compatible with Automatic Processing and the
Central Recording of Dose Histories. P. N, Casbolt, T. O. Marshall and K. B Shaw
ISBN 085951 013 1,
R17 The Determination of Plutonium in Urine by Uitrafiitra'don. G. N. 3 .,« ^
D. S. Popplewell and G. J. Ham.
ISBN 085951 014 X.
Continued on inside
-------
4 IP '
R18 Measurement of Activity of Surfaces ContaminaL-d by Electron-capture Nuclidqs W J lies
and D. F. White.
ISBN 085951 0166.
R19 The Identification of an Homogeneous Critical Group using Statistical Extreme-Value
Theory: Application to Laverbread Consumers and the Windscale Effluent Discharges S
Beach.
ISBN 085951 0174.
R20 The Risk of Death from Radiation-Induced Cancer as Estimated from the Published Data on
the Japanese Atomic Bomb Survivors. S. G Goss
ISBN 085951 018 2.
R21 Assessment of Contamination from the Release of Activate^ Sulphur Hexafluoride from a
iQ-lube Neutron Generator Used for Radiotherapy. R. P. Rowlands and D. L O
Humphreys.
ISBN 085951 0190.
R23 The Study of Chromosome Aberration Yield in Human Lymphocytes ,as an Indicator of
Radiation Dose, IV A Review of Cases Investigated, 1973, R. J. Purrott.'D C Lloyd J S
Prosser, G. W. Dolphin, Elaine J. Eltham, Patricia A. Tipper, Carolyn M. White and Susan J
Cooper.
ISBN 085951 021 2.
R24 Radiation Exposure of the Public - The Current Levels in the Unitbb Kingdom. G. A. M.
Webb.
ISBN 085951 0220.
R25 Radioactive Fluorescers in Dental Porcelains. M. C. O'Riordan and G J Hunt
ISBN 085951 023 9. '
R26 Report on the First International Symposium on CAMAC in Real Time Computer
Applications. R. T. Hankins. ,' '
ISBN 085951 0247. "<- !
R27 Factors for Deriving Absorbed Dose-rates in Air due to Beta Particles from Measurements of
Absorbed Dose-rates in Tissue-equivalent Material. T. M. Francis and E A Pook
ISBN 085951 0263. '
-------
-------
443
Hot particles
DrGW Dolphin
NATIONAL RADIOLOGICAL PROTECTION BOARD, HARWELL
This is a brief critical review of "A report on the inadequacy of existing
radiation protection standards related to internal exposure of man to
insoluble particles of plutonium and other alpha-emitting hot particles" by
A R Tamplin and T B Cochran, 14 February 1974.
It should be noted that no human cancers have been positively associated
with exposure to insoluble particles or soluble compounds of plutonium.
Hence the conclusions in the Report are based on implication or extrapolation
from animal experiments.
The authors have no new biological evidence. The Report is based on data
published during the last 15 years by other scientists.
Tamplin and Cochran refer to the only well-documented human case of
biological changes in cells surrounding a particle of plutonium embedded in
the palm of a man's hand. This was reported by Lushbaucjh and Langham in
1962. A 5 nCi particle of plutonium was excised from the palm 4 years after
it had become embedded as a result of an accident. Lushbaugh, a pathologist,
carefully described the cell changes as having "a similarity to known pre-
cancerous epidermal cytologic changes". Tamplin and Cochran acknowledge
this wording in the first reference to it in their Report. However, in the
second reference the wording is altered slightly to "pre-cancerous changes in
human tissue" and on the third reference another alteration is made and it
becomes "particle induced cancer". In summary, the authors use the old
trick of progressively changing words to arrive at a dramatic conclusion.
From this alleged "cancer" in the palm of the hand, they go to tha conclusion
that the risk of cancer from a hot particle is 1 in 1,000 for they assume that
there are 1,000 men with plutonium embedded in tissues as a result of wound
accidents who have not developed cancers at the wound site. Clearly this is an
absurd conclusion from the available human data.
Albert era/. (1967) reported the incidence of skin cancer in rats exposed to
doses of between 500 and 7,000 rads of beta particle radiation. The cancers
observed were in hair follicles and they showed a sharp increase at doses above
1,000 rads. From these data Tamplin and Cochran conclude that doses of over
1,000 rads to small volumes of cells, as in hair follicles, can produce cancers
and it therefore follows that hot particles can produce cancers if the dose to a
small number of surrounding cells exceeds ubout 1,000 rads.
From a paper by Geesaman (1968), the authors extracted a value for the risk
of cancer in a hair follicle of a rat in the range 1 in 1,000 to 1 in 10,000 at
doses over 1,000 rads to follicles. From these data and the human data
quoted above, Tamplin and Cochran conclude that the risk of cancer
developing in cells surrounding a hot particle is 1 in 2,000. It should be noted
-------
444
here that the follicles were irradiated together with thiR rest of the epidermis
and some of the clermis and the effects of these irrad'uited tissues on the
development of the follicular cancer cannot be assessed in these experiments.
The hair follicle cancers found by Albert ct al. in rats were not found in
similar experiments carried out by by Hulse (1969) using mice. He found only
epidermal and dermal cancers. Hence the hair follicle cancers described by
Albert et al. may be peculiar to the rat species. If extrapolation from rat skin
to mice skin is not possible in this work, then little confidence can exist in the
extrapolation from rat skin to human lung tissue.
Some human experience on the incidence of skin cancer comes from 11,000
children treated by 100kV X-rays for ringworm of the scalp with doses of
about 400 rads. One skin cancer has developed in these children in a period
up to 21 years after irradiation (Modan et al., 1974). Furthermore, no deaths
from skin cancer have been reported by Court Brown and Doll (1965) among
patients treated with doses of about 1,500 rads for ankylosing spondylitis.
The field size on the skin of these patients was about 450 cm2.
This human experience of skin irradiation indicates that large doses to a few
hundred square centimetres of skin do not produce significant numbers of
skin cancers and therefore it is unlikely that a comparable dose of alpha-
radiation to a small number of cells in the skin would produce cancer as
suggested by the hot particle concept of Tamplin and Cochran.
Bair (1974) reports the finding in dogs studied for periods up to 4068 days
after deposition in lungs of 10 million to 100 million plutonium oxide
particles (0.2/vCi to 3.3/jCi). One dog out of 21 living for more than 1,600
days has not developed a lung cancer. Tamplin and Cochran note this finding
but dismiss it and make no estimate of the risk of cancer per particle in the
lung. If they had made an estimate, it would be that the cancer risk in this
dog that survived was in the range 1 in 500,000 to 1 in 5 million per particle.
Lafuma (1974) has reported greater toxic effects including cancer in rats
following deposition of curium-242 in lungs compared with equal amounts of
plutonium-239 activity. This he attributes to the diffuse nature of the curium
deposit arid the particulate nature of the plutonium, as shown by
autoradiographs. This is in direct contradiction to the Tamplin and Cochran
hot particle hypothesis.
It is noted that the basis of ICRP recommendations is the average radiation
dose to an organ and not the number of radioactive particles in the organ.
This dosimetric basis of radiological protection has been established for many
years by observation of humans and experimental work with animals. A
better evaluation than that offered by Tamplin and Cochran would be needed
for this system to be set aside in favour of the hot particle concept. Their
estimate that there is a risk of cancer being generated in cells surrounding a
hot particle of 1 in 2,000 cannot be substantiated by our present knowledge.
References
Albert, R E, Burns, F J and Heimbach, R D Radiation Res., 30, 590, 1967.
Bair, W J Advances in Radiation Bio/., 4, 255, 1974.
Court Brown, W M and Doll, R Brit. mad. J., Dec. 4,1327, 1965.
Geesaman, D P UCRL-50387, Op. cit., p.11, 1968.
Hulse, E V Brit. J. Cancer, 21,531, 1967.
Lafuma, J Paper presented at the French Society for Radiation Protection,
Paris, March 1974 on "La Contamination Radioactive Interne".
Lushbaugh, C C and Langham, J Archs. Derma;., 86, 461, 1962.
Mocbn, R, Haiclntz, D, Mart, H, Steint/, R pnd Levin, S G Lancet, Feb. 23,
7852, 1974.
-------
445
Hillsboro, N.H 03244
7 »
November 3.9, 1974
Office of Radiation Programs
AW-560
EPA
Washington, D.C. 20460
Dear Sirs,
In reply to a recent EPA Citizen's Bulletin,
inviting comments "from all interested parties" on setting
Plutonium standards", I enclose a recent clip (Octoberll,
1974) from the New York Times on Plutonium Found in Plants'.
Roots. The Battelle Laboratories research would tend to
prove that no amount of plutonium should be introduced into
our biosphere. In which case, as well as for many other
reasons, a moratorium on future development of nuclear
fission products should be declared.
I call to your attention a book published in 3973: Unclear
Energy - Its Physics and Its Social Challenge, by David R.
Inglis of the University of Mass ihcusetts (Addision-Wesley
Publishing Co., Heading, Mass.). He devoted pages to the
question of plutonium.
Having attended AEC Liscencing Board hearings on the Vermont
Yankee plant in Vermont and the Seabrook Plant proposed in
our state, I would urge your more active participation and
involvement - not to say control - of nuclear plaftfa develop-
ment.
With all good wishes, I a^yt,
^ Sincerely,
Annette B. Cottrell, Honorary Trusfeee
New England Coalition on Nuclear Pollution
P.S.
I assume you are in touch with The Union of Concerned Scientists
at I-1IT as well as Ralph Nader
enc:'
N.Y. Times clip (Note: not printed because copyright release
not obtained.)
-------
446
BIOMEDICAL DIVISION
L-523
November 20, 1974
Director
Criteria and Standards Division (AW-560)
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D. C. 20460
Dear Sir:
This letter is in response to EPA's request for interested parties
to submit testimony or materials relevant to a review of the need for
establishing new rules for contamination limits for plutonium and the
transuranium elements.
Although the data are equivocal, it is frequently assumed that
the food-chain transport of Pu to man is so low that the most significant
pathway to man is via inhalation. We have recently presented a paper
entitled "Evaluation of the Resuspension Pathway Toward Protective
Guidelines for Soil Contamination with Radioactivity" at an International
Atomic Energy Agency Seminar held in Portoroz, Yugoslavia, May 20-24,
1974. This paper summarizes experimental studies concerning the
resuspension of ground-deposited radioactivity, presents models useful for
predictive purposes, applies these models to rules development for
plutonium in soil, and discusses cost-benefit aspects of clean-up procedures
We believe the topics considered in this paper are highly pertinent
to your review of the need for establishing new rules for plutonium and
transuranic elements. This paper is currently in press, but we are
enclosing 20 copies of the Preprint for your consideration.
Sincerely yours,
L. R. Ansj
Group Leader
Applied Environmental Science Group
Bio-Medical Division
LRA:sc
Enc: (20)
-------
-------
449
IAEA-SM-18U/13
EVALUATION OF THE EESUSPENSION PATHWAY TOWARD
PROTECTIVE GUIDELINES FOR SOIL CONTAMINATION WITH RADIOACTIVITY*
L. R. Anspaugh, J. H. Shinn, and D. W. Wilson
Bio-Medical Division
Lawrence Livermore Laboratory, University of California
Livermore, California 9^550 U.S.A.
ABSTRACT
The resuspension and subsequent inhalation of surface-deposited
radioactivity released to the environment can be a significant mode of
exposure for a few radionuclides such as 239pu. Two simple, interim models
which may be used to predict the average concentration of resuspended
aerosols are developed on an empirical basis. One method uses the time-
dependent resuspension factor approach, and differs from previous work in
placing more emphasis on resuspension at late times. The second method is
appropriate only for aged sources, and uses a straight-forward mass-loading
approach. The relative significance of the resuspension pathway is also
modeled in comparison to the initial exposure resulting from a nonnuclear
explosion which disperses radioactivity. Two hypothetical 239pu contamination
situations are modeled. In the first case the 50 yr dose commitment resulting
from an initial deposition of 1 p,Ci/m2 is calculated as a function of time
post deposition. Half of the total dose commitment is accumulated in the
first 100 d. In the second situation, the reoccupation of an area contaminated
many years previously is considered. Protective guidelines for 239pu soil
contamination are derived from these studies — 1 p,Ci/m2 for a freshly
deposited source and 7 nCi/g in the top 10 mm of soil for a source which
has aged several years. An estimate of the biological cost of not cleaning
up contaminated areas is compared with the engineering and agricultural costs
of soil removal.
This work was performed under the auspices of the U.S. Atomic Energy
Commission.
-------
452
A convenient way to model the airborne concentration of resuspended
contaminant over long periods of time is to make the resuspension factor
a function of time to account for the observed decrease in air concentration
which has been noted to occur in the abscence of a significant net loss of
the deposited contaminant. Conceptionally, it would be more appropriate to
define a time-dependent fraction of the total deposition which is available
for resuspension. However, there is no realistic way in which such a
fraction can be experimentally determined, so this approach will be avoided
for the present purpose. With the time dependency inherent in the resuspension
factor, it follows that the average airborne concentration, "x, of resuspended
contaminant will be given by
X (t) = K (t) SA
where S^ is the total amount of contaminant deposited per unit area. Sj^ is
therefore considered a constant although the actual distribution of the
contaminant with soil depth will change with time.
Kathren [15] and Langham [16] have each formulated predictive resuspension
models which, when expressed in the above format, give the following time
dependency
K (t) = KQ exp (-Xt)
with values of X corresponding to half-times of ^5 d and 35 d. Such a
formulation appears to simulate reasonably well the available observations
up to several weeks post deposition [U, 8]. After a few years, however,
such a formulation underestimates by many orders of magnitude the airborne
concentration of resuspended contaminants which have been measured over
aged sources [5, 7, 9]. For example, the Kathren and Langham models would
predict values for K (t) of 10-29 and 10-38 m-l respectively 10 yr after a
contaminating event whereas an average value determined from 236 individual
air concentration measurements at a location contaminated with plutonium
17 yr previously was found to be 10~9 nr1 [9].
We have derived a different formulation of the time dependency of the
resuspension factor which more accurately reflects the resuspension process
as it is observed in the proximity of aged sources. This model was empirically
derived to conform to the following constraints: l) The apparent half-time
of decrease during the first 10 weeks should approximate a value of 5 weeks
and should approximately double over the next 30 weeks; 2) The initial
resuspension factor should be 10-^ m-l; and 3) The resuspension factor
17 yr after the contaminating event should approximate 10-9 nr1.
A simple model which closely approximates these constraints is
K (t) » 10"^ exp (-0.15 d~^/t) m"1 + 10"9 m"1
-------
453
-5-
The second term was added based upon the assumption that there may be no
further measurable decrease in the resuspension process after 17 yr which
is the longest period post deposition for which measurements have been
reported. This was deemed appropriate because such a "model" was derived
empirically to simulate experimental measurements, and contains no
fundamental understanding of the resuspension process. A graphical
representation of this model, both with and without the second term is
given in Fig. 1; the model equations used by Kathren and Langham are also
shown for comparison.
This model is an attempt to provide protective guidance for the evaluation
of the resuspension pathway over long time periods beginning with the initial
contaminating event. It assumes that resuspension is a local phenomenon
and that the concentration in air drops off rapidly downwind of the deposited
source; this is consistent with experimental observations [3, 93• The model
is suitable only for the prediction of long-term averages of airborne
concentrations; extreme short-term fluctuations are to be expected and
suitable long-term averages of experimental data were used to define the
model contrainsts. The initial value for the resuspension factor, however, -
was deliberately chosen to be sufficiently high to include the effects of
artificial disturbance.
2.2 Mass-loading approach
Nearly all of the experimental measurements of the concentration of
resuspended contaminants have been conducted in the vicinity of freshly
deposited sources. This is appropriate for most situations of practical
concern such as accidental events. However, there are some situations
such as the contemplated reoccupation of test areas contaminated many years
previously where an alternate method of predicting the concentration of
resuspended contaminant may be used to supplement the results derived from
the resuspension factor model.
It has been observed by many authors [17-20] that radionuclides deposited
on the earth's surface in either solution or particulate form penetrate within
a few months to depths of more than 10 mm. Eventually their distribution
with depth is well approximated by an exponential function characterized by
a relaxation depth of 10 to 100 mm. Such a distribution with depth implies
an intimate mixing of the contaminate with the host soil. Therefore, a
method of predicting the average airborne concentration of the contaminant
several years after the contaminating event is to simply multiply the measured
activity of the contaminant per unit weight of soil taken from the top 10 mm
by the concentration of particulate matter in the atmosphere.
For predictive purposes, an average atmospheric concentration of
100 ng/rn^ appears to be reasonable [9]. The choice of this value is partly
based upon measurements of particulate concentration reported for 30 nonurban
-------
454
-6-
locations in the United States [21]. Annual arithmetic averages varied
from 9 to 79 V-S/JD? with a mean for all 30 stations of 38
Several experimental results are available to check the accuracy of this
simple prediction method [9, 22-26]. These values are tabulated in Table I;
the agreement between the predicted and measured values is generally
excellent .
2.3 Relative importance of resuspension in the inhalation pathway
Some accident situations may produce an initial contaminant aerosol
cloud with a resulting dose commitment to an exposed population. In such
cases, it is of practical interest to compare such an unavoidable dose
commitment to that predicted via the resuspension pathway.
If the initial integrated air activity is AQ (activity-time/volume),
the ground deposition may be calculated by multiplying by a deposition
velocity, V, (length/time). The integrated air activity, A, due to
resuspension is then given by
A = VAo J K (t) dt
which may then be compared conveniently with the initial integrated air
activity, Ao. One problem in such a comparison, however, is the choice of
an appropriate value for the deposition velocity. This varies as a function
of particle size and wind speed, and in close proximity to an explosion the
actual deposition would be strongly influenced by the ballistic effects of
the explosion itself. At such close-in distances, however, the initial
resuspension factor is also lower [2, k, 10]. Because the initial resuspension
factor chosen for use in the model is relatively high and is presumed to be
appropriate for smaller particle size distributions of the contaminant aerosol,
it is assumed that an appropriate value for V is ^0 m/h. This is an average
value which can be derived from several years of fallout data [27].
2.4 Dose commitment due to the resuspension of "Tu
In order to derive a protective guideline for soil contamination, some
reference must be made to a primary standard. For 239pu, which will be used
as an example, it will be assumed that the desired primary reference standard
is. the accumulated 50 yr dose commitment. The dose commitment calculations
were made with the additional assumptions that the plutonium is non-transportable,
the lung is the critical organ [28], 25% of the inhaled plutonium is deposited
in the pulmonary region, and that the metabolic parameters listed by Morgan [29]
for Class Y compounds were appropriate.
Representative calculations are presented in Tables II and III for two
hypothetical situations. The first assumes a nonnuclear explosion which
produces a 239pu deposition of 1 iiCi/m2. The 50 yr dose commitment due to
-------
455
-7-
the initial cloud passage and resuspension of deposited material as a
function of time post deposition were calculated using the models given in
sub-sections 2.1 and 2.3. The results in Table II indicate that any
protective action must be undertaken fairly rapidly if a significant reduction
in the 50 yr dose commitment is to be achieved.
The second situation assumes the reoccupation of landscape contaminated
many years previously and where the 23?pu concentration in the top 10 mm of
soil is 1 |j,Ci/g. Calculations of the 50 yr dose commitment as a function
of time post reentry were made using the model given in sub-section 2.2, and
are presented in Table III.
If we assume that an acceptable 50 yr dose commitment in such situations
is 50 x 1.5 rem, or 75 rem, then protective guidelines of 1 nCi/m2 and
7 nCi/g are derived for the two hypothetical situations. It is emphasized,
however, that this analysis has considered only the inhalation of ambient
air. Other pathways such as personal contamination and ingestion may be
more restrictive in some situations.
3* Cost-benefit aspects of protective guideline application
Models developed in this study can be applied to a general analysis of
costs and benefits associated with the clean-up of environmental plutonium.
In this instance, costs are defined as all expenditures and monetary losses
derived from clean-up action. Benefits are the reductions in potential
health costs which may be derived from any proposed clean-up action.
Comparative costs have been derived for clean-up of a hypothetical km2
of agricultural land containing one Ci of 23$>u in the soil surface (Table IV).
The objective of this exercise is to provide a semi-quantitative analysis
of the economic trade-offs between clean-up and no clean-up.
Costs of removal of soil depend upon availability of equipment, costs
of transportation, and the complexity of terrain. In 197^, U.S. public
works projects involving soil surface pick-up cost U.S. $0.15/m3 of soil-
associated transportation costs for long hauls were U.S. $ 0.06/m3 _ km hoi
Clean-up costs for removing the top 30 mm of soil from a km2 of land would-be
approximately U.S. $1^00. Transportation of contaminated soil to a storage
site 500 km away would be approximately U.S. $ 1 X lo6/km2 of surface removed.
Thus, clean-up costs are likely to be small compared to transportation
costs for clean-up in impacted areas which are remote from a radioactive
waste management area. Costs associated with long-term waste management
will be ignored here.
Land values are highly variable and depend upon the specific land use.
Currently, U.S. agricultural land is valued at approximately U.S.
$50,000/knr [31]. Restriction against crop production would result in
-------
456
this economic loes as well as losses of annual crop production, valued at
U.S. $ 2 X loVkm2 [31]. Clean-up could result in costs from temporary
decreased agricultural production due to interruptions in the crop cycle
or decreased soil fertility. For locations with marginal food supply,
restrictions in agricultural production could lead to more serious
biological costs than costs from radiation exposure.
Potential health costs arising from radiation exposure in populations
have been evaluated in monetary terms by others [32]. Such figures are
useful for comparison with the monetary costs of remedial action against
radiation exposure. Health cost estimates are developed in this study
using a value of U.S. $250/man-rad. At a dose commitment level of
75 rem, the calculated cost per person exposed is U.S. $ 2 x 10 . On
typical agricultural land, one could reasonably expect a population density
of one to ten persons per km2. Potential biological costs could be approximately
U.S. $ 2 x KK. The benefit-cost ratio for clean-up is therefore approximately
0.2. This ratio is very sensitive to the costs of transportation and the
number of human receptors which are involved. Alternatives, such as
restriction against crop production incur costs which are comparable to the
benefits of reduced radiation exposure; for example, the economic crop loss
of creating an exclusion area for ten years is approximately U.S. $ 2 x
In summary, the deposition of a Ci per km2 of 239pu on agricultural
land can be evaluated as leading to potential health costs which are comparable
in economic value to the costs of remedial actions which remove the potential
exposure. The judgement regarding proper action involves consideration of
qualitative features, such as economic policies and societial priorities
for utilizing finite monetary resources to promote human welfare. Some
consideration should also be given to an implied long-term commitment should
a decision be made not to clean-up a contaminated area. If such an- area
is used for agricultural production, some monitoring program will be necessary
to assess the level of 23xFu in food crops. While the food-chain transport
of 239pu is generally believed to be negligible based upon short-term studies,
it cannot be stated with certainty that this will remain true over long
periods of time [19].
The short time period available for making an effective decision is
also apparent from the results in Table II. By 100 d after the contaminating
event, one-half of the total 50 yr dose commitment has already been
accumulated. An alternate couse of action would be to evacuate the area
and/or plow the affected ground surfaces. This should be effective in
greatly reducing the biological costs, but also substantially increases
the ultimate cost of clean-up should it eventually be deemed necessary.
Finally, some mention should be made of urban environments. Here, the
potential for rapid spread of the material and the large population density
appear to offer no choice but to contain and remove the contamination as
rapidly as possible.
-------
457
-9-
REFERENCES
[l] LANGHAM, W.H., Plutonium distribution as a problem in environmental
science, Environmental Plutonium Symposium (Proc. Symp. Los Alamos,
New Mexico, 1971) USAEC Rep. IA-kj^6 (1971) 3.
[2] LARSON, K.H., NEEL, J.W., HAWTHRONE, H.A., MORK, H.M., ROWLAND, R.H.,
BAURMASH, L., LINDBERG, R.G., OLAFSON, J.H., KOWALEWSKY, B.W.,
Distribution, Characteristics, and Biotic Availability of Fallout,
Operation Plumbbob, USAEC Rep. WT-lWS (1966).
[3] SHREVE, J.D., JR., Summary Report, Test Group 57, USAEC Rep.
ITR-1515 (DEL) (1958).
[>] WILSON, R.H., THOMAS, R.G., STANNARD, J.N., Biomedical and Aerosol
Studies Associated with a Field Release of Plutonium, USAEC
Rep. WT-1511 (I960).
[5] OLAFSON, J.H., LARSON, K.H., Plutonium, Its Biology and Environmental
Persistence, USAEC Rep. UCLA-501 (1961).
[6] STEWART, K., The resuspension of participate material from surfaces,
Surface Contamination (Proc. Symp. Gatlinburg, Tenn., 196^)
Pergamon, London (196^) 63.
[7] VOLCHOK, H.L., Resuspension of plutonium-239 in the vicinity of Rocky
Flats, Environmental Plutonium Symposium (Proc. Symp. Los Alamos,
New Mexico, 1971) USAEC Rep. LA-^756 (1971) 99.
[8] ANSPAUGH, L.R., PHELPS, P.L., KENNEDY, N.C., BOOTH, H.G., Wind-driven
redistribution of surface-deposited radioactivity, Environmental
Behaviour of Radionuclides Released in the Nuclear Industry (Proc.
Symp. Aix-en-Provence, France, 1973) IAEA, Vienna (1973) 167. '
[9] ANSPAUGH, L.R., PHELPS, P.L., KENNEDY, N.C., BOOTH, H.G., GOLUBA, R.W.,
REICHMAN, J.M., KOVAL, J.S., Resuspension element status report, The
Dynamics of Plutonium in Desert Environments, USAEC Rep. NVO-1^2
(in press).
[10] ANSPAUGH, L.R., PHELPS, P.L., HOLLADAY, G., HAMBY, K.O., Distribution
and redistribution of airborne particulates from the Schooner cratering
event, Health Physics Aspects of Nuclear Facility Siting (Proc. Symp.
Idaho Falls, Idaho, 1970) 2, Eastern Idaho Chapter, Health Physics
Society, Idaho Fans (1971) ^28.
[11] MORK, EM., Redistribution of Plutonium in the Environs of the Nevada
Test Site, USAEC Rep. UCLA-12-590 (1970).
-------
458
-10-
[12] SEHMEL, G.A., Particle resuspension from an asphalt road caused by
car and truck traffic, Atmos. Environ. J^ (1973) 291.
[13] VOLCHOK, H.L., KNUTH, R.H., The respirable fraction of plutonium
at Rocky Flats, Health Phys . _23 (1972) 395-
[I1*-] MISHIMA, J., A Review of Research on Plutonium Releases during
Overheating and Fires, USAEC Rep. HW-83668 (196U).
[15] KATHREN, R.L., Towards interim acceptable surface contamination
levels for environmental Pu02, Radiological Protection of the
Public in a Nuclear Mass Disaster (Proc. Symp. Interlaken, Swit.,
1968) EDMZ, Bern (1968) k60.
[l6] LANGHAM, W.H., Biological Considerations of Nonnuclear Incidents
Involving Nuclear Warheads, USAEC Rep. UCRL- 50639 (1969).
[17] BECK, H.L., Environmental gamma radiation from deposited fission
products, 1960-1961+, Health Phys. 12 (1966) 313.
[18] ROGOWSKI, A.S., TAMURA, T., Erosional behavior of cesium-137, Health
Phys. 18 (1970) U6?.
[19] ROMNEY, E.M., MORK, H.M., LARSON, K.H., Persistence of plutonium in
soil, plants and small mammals, Health Phys. !£ (1970)
[20] KREY, P.W., HARDY, E.P., Plutonium in Soil Around the Rocky Flats
Plant, USAEC Rep. HASL-235 (1970).
[21] NATIONAL AIR POLLUTION CONTROL ADMINISTRATION, Air Quality Data
from the National Air Sampling Networks and Contributing State and
Local Networks, 1966 Edition, USHEW Rep. APTD 68-9 (1968).
[22] " GUDIKSEN, P.H., LINDEKEN, C.L., GATROUSIS, C., ANSPAUGH, L.R.,
Environmental Levels of Radioactivity in the Vicinity of the Lawrence
Livermore Laboratory, January through December 1971, USAEC Rep.
UCRL- 512^2 (1972).
[23] GUDIKSEN, P.H., LINDEKEN, C.L., MEADOWS, J.W., HAMBY, K.O., Environmental
Levels of Radioactivity in the Vicinity of the Lawrence Livermore
Laboratory, 1972 Annual Report/ USAEC Rep. UCRL-51333 (1973).
[2^.] SILVER, W.J., LINDEKEN, C.L., MEADOWS, J.W., HUTCHIN, W.H., MCINTYRE,
D.R., Environmental Levels of Radioactivity in the Vicinity of the
Lawrence Livermore Laboratory, 1973 Annual Report, USAEC Rep.
UCRL- 51 5^7 (197*0.
[25] SEDLET, J., GOLCHERT, N.W., DUFFY, T.L., Environmental Monitoring at
Argonne National Laboratory, Annual Report for 1972, USAEC Rep.
ANL-8007 (1973).
-------
459
-ii-
[26] HAMILTON, E.I., The concentration of uranium in air from contrasted
natural environments, Health Phys. _1£ (1970) 511.
[27] KLEINMAN, M.T., VOLCHOK. H.L., Radionuclide concentrations in surface
air: Direct relationship to global fallout, Science 166 (1969) 376.
[28] ICRP COMMITTEE k, The Assessment of Internal Contamination Resulting
from Recurrent or Prolonged Uptakes, ICRP Publication 10A, Pergamon,
Oxford (1971).
[29] MORGAN, K.Z., Proper use of information on organ and body burdens
of radioactive material, Assessment of Radioactive Contamination
in Man (Proc. Symp. Stockholm, 1971) IAEA, Vienna (1972) 3.
[30] MCMAHON, L.A., Dodge Estimating Guide for Public Works Construction,
197^ Annual Ed., No. 6, McGraw-Hill, New York (197*0.
[31] US DEPT. OF AGRICUHTUKE, Agricultural Statistics, 1973, USGPO,
Washington (1973).
[32] COHEN, J.J., EEGGINS, G.H., The socioeconomic impact of low-level
tritium releases to the environment, Tritium (Proc. Symp. Las Vegas,
1971) Messenger Graphics, Las Vegas (1973) 1^.
-------
460
-12-
Table I. A comparison of observed and predicted air concentrations based
upon a simple mass loading model.
Air Concentration
Location, etc. Radionuclide
OCC site, USAEC Nevada
Test Site [
-------
461
-13-
Table II. Calculated dose commitment to the lung from a hypothetical
accident dispersing 239pu in the environment which produces
a ground deposition of 1
Accumulated 50 y dose commitment, rem
Time Resuspension Total
Intial cloud passage
1 d
5 d
10 d
50 d
100 d
i y
10 y
50 y
0.53
2.U
*.3
15.
23.
in.
52.
52.
6.1
6.6
8.5
10.
21.
29.
*7.
58.
58.
-------
462
Table III. Calculated dose commitment to the lung for population reentry
into an area of aged 239pu contamination with 1 iiCi/g in the
top 10 mm of soil
Accumulated 50 yr
Time dose commitment, rem
1 y 210
10 y 2,100
30 y 6,UOO
50 y 10,000
-------
463
-15-
Table IV. Estimates of the costs and benefits result|ng from the clean-
up of agricultural land contaminated with 39Pu. All values
are in US $.
Factor System value Cost Benefit
Biological effect* 3.0 x 105
Soil pick-up V.5 x 103
Waste transportation 1.0 x 10
Agricultural land0 5.0 x 10
Annual crop yield0 1.6 x 10
Population density of 10/km and a 50 yr dose commitment-of 75 re}n.
Transportation of the top 30 mm a distance of 500 km.
US average.
-------
464
-16-
FIGURE CAPTION
Figure 1. A graphical representation of several time-dependent resuspension
factor models. The two curves on the far left represent the
models of Langham [16] and Kathren [15]. The remaining two
curves represent models developed in this paper, both with and
without a constant term of 10'9 m'1. The hatched area represents
measurements recently reported at an aged source [9].
-------
10
CO
TIME POST DEPOSITION, YR
Fig. 1. A graphical representation of several time-dependent resuspension factor models. The two
curves on the far left represent the models of Langham [16] and Kathren [15]. The upper two curves
represent models developed in this paper, both with and without a constant term of 10-9 m"-1-.
The hatched area indicates values recently measured at an aged source [9].
-------
0}
DISTRIBUTION
LLL Internal Distribution No. of Copies
L. Anspaugh 10
J. Shinn 10
D. Wilson 10
P. Machado 100
D. Schilf i
T.I.D. File 15
NOT 1C K
"This report was prepared as an account of work sponsored by
the United States Government. Neither the United States nor
the United States Atomic Energy Commission, nor any of their
employees, nor any of their contractors, subcontractors, or their
employees, makes any warranty, express or implied, or assumes
any leg;il liability or responsibility for the accuracy, completeness
or usefulness of any information, apparatus, product or process
disclosed, or represents that its use would not infringe privately-
owned rights."
dks
-------
FREDERICK FDRSCHER
£nf.iqu f^v\anaqe.mc.nt doniuLtant ty f\ ^7
6SBO BEACDN STREET PITTSBURGH, PA. 15217
•412/5Z1-O61S
20 November 19?4
W. Hills
EPA, Criteria and Standards Div.
401- M Str. SV.;.
Washington, D.G. 20460
Dear Dr. hills:
This is to offer my testimony as chairman of ANSI's N 46-4 at the forthcoming
hearings on Plutonium, starting December 10, 19?4. The subject matter of.
sub-committee N46-4 concerns fuel fabrication plants. Since early in 1972
this committee has worked on the development of an A+ priority standard
N 28? "Criteria for Siting, Design, and Operation of Plants for the the
Manufacture of Nixed Oxide (U-Pu) Fuels."
The Purpose of the standard is defined by Sectionl.O. "These criteria establish
the necessary siting, design, fabrication, testing, and performance requirements
for structures, systems and components important to safety, to the physical
security and accountability of special nuclear materials, and to the protection
of the environment; thus to provide reasonable assurance that a facility,
meeting these criteria, can be operated without undue risk to the health and
safety of employees and the public, to the national security, and the natural
environment."
The standard has gone through five drafts. Recently , the standard was balloted
by the full N46 committee (Fuel Cycle Facilities) and the subcommittee has
just finished the resolution of all the comments received.
The finished, standard ' contains many (.quantitative design bases, some of which
have not yet been adopted by any regulatory agency. A series of design basis
accidents and events constitute a novel aspect of this standard.
My testimony ( 20 minutes) will discuss the reasons behind the development
of this specific standard, and give some explanation for the numerical limits
as recommended by the consensus of the committee.
MEMBER: ABME AIME ANS ABM AIF INMM AAAS ANSI ASTM
-------
Department of Environmental Health Sciences
Harvard School of Public Health
665 Huntington Ave., Boston, MA 02115
21 November 1974
Director, Criteria and Standards Division (A$-560)
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D.C. 20460
Dear Sir:
Attached is a written statement which I wish to submit
for your hearings on "Plutonium and the Transuranium Elements".
I do not intend to make an oral presentation.
Sincerely,
William V. Lipton
-------
William V.Lij n, Doctoral Candidate 21 November 1974
Department of Environmental Health Sciences, Harvard School of
Public Health, 665 Huntington Ave., Boston, MA 02115
Comments for EPA hearings on "Plutonium and the Transuranium
Elements"
Category 3: "Environmental Levels and Pathways"
In the event of widespread Pu-239 contamination of an
agricultural area, population exposure through the food chain
must be considered. Presently, plant uptake is not considered
a significant pathway because of observed soil to plant
concentration factors of around 10 . However, there are
indications of an increasing plant uptake over time, as shown
in a recent plutonium plant uptake experiment by Romney, Mork,
and Larson. 2 Because of the 24,400 year half-life of Pu-239,
even a slight increase from year to year could indicate a
significant long-term problem.
Among the hypotheses advanced to account for this increase
in Pu-239 uptake over time are: chelation of the plutonium- in
the soil, an increase ifl plutonium colloid size over time, and
a more intimate contact of the plant roots with Pu-239 over
4
time, as the Pu-239 moves down into the soil. In order to
test these hypotheses, we are conducting Pu-239 plant uptake
experiments where the following variables are controlled:
a. Chelation: Some of the plants are grown with DTPA,
a chelating agent, added, and some are grown without
added DTPA.
b. Colloid size: A hydrated PuOo colloid is created
through the titration of plutonium nitrate. This colloid
is then separated into 3 size groupsJ using Nuclepore
filters, with different groups being applied to
different plants.
c. Depth in soil: The plutonium is applied as a
layer of contaminated sand buried at various depths
below the surface.
The plants are grown indoors, under artificial lighting.
The growing medium is washed, sterilized sand, since this would
have a minimum of possibly confounding factors. The containers
used are cylindrical jars, 3i" in diameter and 6" tall.
-------
William V.Lipton EPA statement, 21 November 1974 page ?
470 Colloidal plutc urn, as described above, i~ used, since this is
the form most likely to result under accident conditions.
The principal result, so far, is that chelation has a
significant effect on uptake. Comparisons of samples which
were similar, except for DTPA application, indicate that,on the
average, DTPA applied at a level of 100 ppm (based on dry soil
weight) increased uptake by a factor of about 50. Some of the
chelated samples showed soil to plant concentration factors
greater than 1.
The results for colloid size are inconclusive,so far.
Additional experiments are being undertaken, in order to increase
the precision of the results and, hopefully, show any effect
of this variable.
The results show a decreasing uptake with increasing
depth of burial. This is the reverse of what was expected
and could be an artifact of the experimental conditions, since
the plants in this investigation are grown in a confined
space, and the shallower plutonium is in-contact with the roots
for a longer period of time.
Although the relevance of these results to an environmental
situation is open to question, they certainly indicate that
at least one factor can significantly increase plant uptake,
and that all possibly significant factors should be thoroughly
studied. Environmental plutonium can no longer be dismissed,
out of hand, as a food chain hazard.
Notes
1. Langham, WH, "Biological considerations of nonnuclear
incidents involving nuclear warheads," UCRL-50639 (1969).
2. Romney, EM, Work, HM, and Larson, KH, "Persistence of
plutonium in soil, plants, and small mammals," Health
Physics 19:487-491 (1970).
3. Price, KR, "A review of transuranic elements in soils,
plants, and animals," Journal of Environmental Quality 2:62-66(1973).
4. Romney et. al., Health Physics 19:487-491(1970).
5. Langham, WH, UCRL-50639 (1969). \
-------
471
Nov. 21 1974
MRS. D. GORDON SHARP
307 GRANVILLE ROAD
CHAPEL HILL, N. C. 27514
EPA
Washington DC 20460
Gentlemen:
Having read thousands of pages on nuclear and breeder
reactors and having hoped against hop that clean, safe
energy was at hand, I believe coal is cheaper; and - with
scrubbers, gassification § liquification, will be safer
than nuclear. Surely the breeder i£ a "Faustian bargain" -
"No," I say. Men are yet too undependable to use such
dangerous sources. Proponents are whistling in the dark.
If solar § fusion are better in the long run, they're
better now. Let us not waste more manpower and resources
on nuclear.
We'd rather conserve and live for solar and fusion.
MORATORIUM
ON NUCLEAR
NOW
I CANNOT MAKE THE HEARINGS BUT WISH TO BE COUNTED ON
RECORD.
-------
GEORGIA INSTITUTE OF TECHNOLOGY
ATLANTA. GEORGIA 3O332
SCHOOL OF
NUCLEAR ENGINEERING November 22, 1974
Criteria and Standards Division,
Director (AW-560)
Office of Radiation Programs
United States Environmental Protection Agency
Washington, D. C. 20460
Dear Sir:
Please find enclosed a copy of the testimony I wish to present before
the hearings on Environmental Impact of Releases of Pu and Other Trans-
uranium Elements. I do not wish to give oral testimony since I have
accepted membership on the panel. I have sent twenty (20) copies of
this paper to you under separate cover.
Thank you for your assistance in this matter.
Sincerely,
Kai/1 Z. Morgan
Neeley Professor
KZM:f
Enclosure
cc: Mr. Claire C. Palmiter
-------
473
SUGGESTED REDUCTION OF PERMISSIBLE EXPOSURE
TO PLUTONIUM AND OTHER TRANSURANIUM ELEMENTS
by
Karl Z. Morgan
School of Nuclear Engineering
Georgia Institute of Technology
Atlanta, Georgia 30332
INTRODUCTION
Perhaps there has never before been an enterprise that was planned
so carefully for its safety and never before a risk that has been so
thoroughly studied and guarded against as has been the case with the
nuclear energy industry and its concern to avoid unnecessary exposure to
ionizing radiation. It is ironical that in part because of this concern
and in spite of the fact that we now probably know far more about the ef-
fects of this radiation on man than about any of the other common hazards,
exposure to the radiations associated with nuclear energy seem to frighten
and engender fear that is all out of proportion in comparison with the
everyday risks from such things as medical x-ray, food additives, and
environmental pollutants from the burning of fossil fuels. However, on
second thought this public concern for radiation exposure probably should
not be surprising because, except for unusual precautionary measures and
constant vigilance, there likely some day will be a major accident with very
serious consequences. Even though most of the public may be convinced of
a very low probability of such a serious accident, we are reminded fre-
quently in our newspapers of what could happen from accidental release into
-------
474
the public domain of large quantities of radioactive material from nuclear
power plants, from spent fuel operations, or from shipping accidents.
A considerable portion of the credit for the remarkable safety record of
the nuclear energy industry as one of the safest of all modern industries
must be given to the untiring efforts of members of the health physics pro-
fession with whom I have been associated for over 30 years, and which pro-
fession I have seen grow from a group of 5 health physicists at the University
of Chicago in 1943 to a worldwide organization today of over 10,000 profes-
sionals. Our lot as a growing profession of health physicists has been a
most interesting and challenging one but it has not always been easy, because
there were times when some of my associates were demoted or lost their jobs
bcc.T.ir.e they refused to yield to pressures tc lower our standards or compro-
mise for unsafe conditions.
We were constantly resisting pressures of engineers and production
supervisors to relax what they called our ridiculous conservatism. Sometimes
we were forced to set exposure limits that were lower than our management
wanted and perforce they were often little better than guesses because in
some areas we had almost no experience or supporting pxperimental data. For
example, one of the earliest papers *• ' showing how to calculate dose from
internally deposited radionuclides and giving values of permissible body
burden and permissible concentration of some 20 radionuclides was delayed
for almost a year when I presented it for publication in 1945 because some
of the permissible occupational exposure values I calculated were much lower
than those in use in weapons production operations. I had at that time al-
most no metabolic data for some of these radionuclides. For the most part
-------
475
I had to rely on a series of publication by J. G. Hamilton et al.(2) on the
metabolism of fission products, plutonium, and the other actinide elements
in mice and rats and in a few cases data on only 3 or 4 rats were available.
The maximum permissible internal dose rates for occupational exposure that
I used in making these early calculations were 36 R/y for p and y radiation
and 3.6 rep/y (~ 3 rad/y) for a radiation. On this basis and using avail-
able metabolic data the value I obtained for 239Pu for maximum permissible
lung burden of the occupational worker was 0.035 ^Ci and for bone burden was
0.42 uCi. The standard man data I used were based on typical human values
collected and summarized for me by M. J. Cook. ^
The first semiofficial values for body burden of the radionuclides were
developed at the Chalk River Canada Conference(4) in 1949. These vatt.os
were later reviewed at the Harwell, England Conference in 1930. From about
1940 to 1973 I was chairman of the Internal Dose Committees of both the
International Commission on Radiological Protection (ICRP) and of the
National Council on Radiation Protection (KCRP) and so must assume some of
the blame for shortcomings of our Handbooks on Internal Dose. During this
period there were four principal publications of our Internal Dose Handbooks
giving values of organ burden (qf^ and body burden (q) and maximum permis-
sible concentrations in air (MPC)a and water (MPC)w for a large number of
radionuclides including values for 239Pu and some of the other actinide ele-
ments. Table I summarizes these values of q and qf for 239Pu. Similar
values to those in Table I have been given in these same publications for
the other actinide radionuclides and for the most part there have been few
changes since 1953. In most cases the ICRP and NCRP recommended dose limits
are identical. In 1964, ICRP(9) made a few revisions for the actinide ele-
-------
476
239,
merits but the values for Pu remained unchanged.
TABLE I
239T
MAXIMUM PERMISSIBLE BODY BURDENS FOR Pu
Source of Value
Occupational
,(p,c) q(|ic)
For Population at Large
Chalk River Conference
1949<4)
0.006
B
Early Oak Ridge Nat. Lab.
(K.M-1947) ^
0.42 B
0.035L
0.70 B
0.12 L
I
0.00006
B
Early Los Alamos Nat. Lab.
C4V
(WHL-1938)^ '
NCRP--Handbook 52
(1953 )(5)
0.03 a
0.0081
0.063
0.04 E
0.0081
:0.003)
(0.0008)
*B
(0.004)
(0.0008)
*B
*L
ICRP--Br. J. Radiol.
Supp. 6 (1954)<6)
0.03
0.02
L ,
0.04
0.02
NCRP--Handbook 69
(1959) (?>
ICRP--Handbook 2
(1959)(8)
0.036
B
0.04
0.04
(0.004)
B - value based on dose to bone; L - value based on dose to lung; * - values
in parentheses are based on suggested safety factor of 10; q - ^c in total
body based on indicated organ; qf2 - ^c in indicated organ (bone or lung);
** - W H. Langham gave 0.032 nCi as a proposed LNL value in 1950.
-------
477
Changes Being Considered for Revised ICRP Internal Dose Handbook
There are many changes being considered for the ICRP Internal Dose
Handbook which has been under revision for over 12 years. Only a few of
these changes which relate to the permissible exposure levels for the trans-
uranium radionuclides will be mentioned here. Two rather obvious improve-
ments are: 1) Where possible doses to the bone will be calculated for spe-
cific critical tissue of this organ rather than average the dose over the
entire bone and 2) The dose to a critical organ (or tissue) will be the sum
of the doses to that organ originating from deposits of the radionuclide in
all body organs including that from deposits in the critical organ.
The present ICRP and NCRP values^7'8>9^ of qj qf (fopC) > and (ppC)
i a w
ware calculated on the basis of uniform distribution of the radionuclides in
the critical body organ (e.g. uniform deposition in the skeleton) and irra-
diation only from the deposits of the radionuclide within this organ. These
assumptions were made because of a lack of biological information. The as-
sumption of uniform distribution of a radionuclide may have given rather re-
liable results in some cases for gamma and high energy p-emitting radionu-
clides that are fairly uniformly deposited in an organ but the risk (of bone
239
cancer) from Pu could have been seriously underestimated because most of
239
the a-emitting Pu is deposited on bone surfaces of the trabecular matrices
adjacent to the thin layer of endosteal tissue which happens to be the most
critical tissue in this case. Obviously, the inclusion in the calculation
of dose only from the radionuclide deposited within the critical tissue it-
self could lead to underestimates of the risk except for a and low energy p-
emitting radionuclides that are highly localized in the critical organ so
that cross irradiation from other organs is insignificant. The decision of
-------
the ICRP has been to consider the critical tissues of the skeleton the
endostial tissue (as it relates to bone cancer) with an average thickness of
10 pjn and the active (red) bone marrow (as it relates to leukemia), and to
limit the maximum permissible annual dose (MPAD) to these tissues to no more
than 15 rem/y (a limit of 1.5 rem/y for members of the general public). Un-
239
fortunately our knowledge of the microdeposition of Pu in the bone prob-
ably is too limited at the present time to apply these refinements and so it
Is likely the present practice will be continued; namely, calculate the dose
from 239Pu to the entire skeleton, as is done with some justification for
226Ra, «ad *ppiy an N-factor (= 5) to the absorbed dose (rad) as well as
the usual Q factor (= 10) for a-radiation in obtaining the dose equivalent
(rem) dose.
The new ICRP Internal Dose Handbook probably will not give values of q,
qf , or (MPC) but these quantities can be calculated from values of A (|j,Ci
days of residence time in the critical tissue of reference or standard man),
B (dose commitment in rem to this critical tissue for the next 50 years per
tiCi intake)^ and MPAD (maximum permissible annual dose, e.g. occupational
limits of 5 rem/y to gonads, total body, and gonads; 30 rem/y to total bone,
thyroid, and skin; 75 rem/y to hands, feet, arms, and ankles; and 15 rem/y
to all other body organs or tissues). Two equations as follows can be
used in making these calculations:
5.4 X 10"5 m (MPAD) ri\
=
_ (MPAD)A
q ~ 365 f2B
in which A,B and (MPAD) are defined above, f2 is the fraction of the radio-
-------
479
nuclide in the critical tissue of that in the total body, £(MeV) is the
total energy deposited in the critical tissue of mass m(g) per disintegration
of the radionuclide in the entire body.
The Linear Hypothesis May Not Be Sufficiently Conservative
Frequently in the literature it is stated that the linear hypothesis is
j-
a very conservative assumption. During the past few years, however, many
studies have indicated that this probably is not true in general and that at
low doses and dose rates somatic damage per rad (and especially that from a-
irradiation) probably is usually greater than would be assumed on the linear
hypothesis. There are many reasons for this, some of which are:
1. The linear hypothesis is based on extrapolations to zero dose of
effects of radiation on animals or humans at intermediate to high doses.
The points used on the curves at high doses may be on the descending part of
the curve, i.e. from portions of the curve where there was overkill or where
a large fraction of the highly exposed died of other types of radiation dam-
age and did not survive to die of the radiation effect under study.
2. Extrapolations are made on human data which in general relate human
239
damage such as bone cancer from Pu for observation periods of no more
than about 20 years. Many of the conclusions are based on studies of ani-
mals of life spans less than 10 years. Since man lives for more than 70
years, the slopes of these curves can only increase as more human data are
accumulated over his entire life span.
3. The linear hypothesis assumes that man is a uniform and more or less
homogeneous population. It applies to the average man and may not be suffi-
ciently conservative for the fetus and for old people. It never takes into
consideration special groups such as those studied by Bross^11) where he found
-------
480
that children of age 1-4 had 3.7 times the risk of developing leukemia if
they have allergic disease such as asthma and 24.6 times the risk of the
children of this age group if they had both allergic disease and had received
intrauterine x-ray exposure.
4. There may be cell sterilization at intermediate and high doses. By
this we mean there may be many cells in the body which are likely targets
to become precursors of a clone of cells which are malignant but they are
killed by the higher doses. In other words, these cells may already have
two of the "series cancer switches" closed and a low dose of radiation would
likely close the final switch in the step toward cancer production. A high
dose such as that from which extrapolations usually are made, however, might
kill most such cells as it does in radiation therapy which is used to destroy
a cancer.
5. For many types of radiation damage the best fit curve is a plot of
equation E = CDn in which E = effect, C = constant, D = radiation dose, and
n = constant. For the linear hypothesis n = 1. In some cases n > 1 indi-
cating lesser damage per rad at low doses but in many cases the best fit to
(12)
experimental data is obtained when n < 1. Baum recently showed a best
fit for cancer induction when n = 1/2. In such case the linear hypothesis
would be non-conservative.
239
6. As pointed out above Pu is an a-emitting, bone seeking, radio-
f) f) fl O O (i
nuclide like Ra, but unlike Ra, it is deposited on the bone surfaces
adjacent to the radiosensitive endosteal and periosteal tissues. The use of
996
the N-factor equal to 5 for all a-emitting radionuclides in bone except Ra
somewhat compensated for this increased risk from surface deposition but has
always left some questions to be answered when we determined all q and qf^
-------
481
values for bone as given in Table I by comparison with Ra burdens in man.
o o c
Our 50 year human experience with Ra has been of extreme importance in
setting these values for bone but one was not completely satisfied in using
(13) 239 226
the University of Utah data on Pu and Ra in dogs to provide guid-
ance in making these extrapolations in humans where there are very little
239
Pu data. Fortunately, a recent finding may be of great assistance in
r\ o Q O O f"
relating Pu exposure to Ra which has been studied intensively for many
years in some humans who have varying quantitatively determined body burdens
of Ra in their skeletons. Here I refer to the important studies of Mays
(14)
et al. of over 1000 patients in Germany who were injected with known
224
amounts of the short lived (3.64 day), a-emitting radionuclide, Ra as a
treatment for extra -pulmonary tuberculosis. Because of its short radio-
p O/i O O (C
active half life Ra, unlike Ra, does not have time to be deeply im-
bedded in bone and thus may simulate to a considerable degree the deposition
239 (14)
of Pu in man. Mays et al . have made an interesting observation regard
224
ing human exposure to Ra which may have important bearing on chronic expo-
sure of large populations to a-emitting, bone surface seeking radionuclides ;
namely, there is a greater incidence of bone sarcoma from a given total dose
224
of radiation when the span of Ra injections was increased. This increased
risk with increased protraction of a-radiation exposure is opposite from
what has been observed generally with exposure to x-rays where protracted
dose allows time for more repair of radiation damage. Mays has suggested
that maybe this may be attributable to a) increased number of cells irradi-
ated, b) less kill of pre-malignant cells (i.e. cell sterilization), c) pro-
longed stimulus of cell division, and d) greater difficulty for cell repair
of local a-damage.
-------
482
Since 239Pu when dispersed into the environment in very low concentra-
tion (except in the unlikely accident) delivers a protracted rather than an
acute exposure to man, the risks may be greater than those suggested by
239
animal studies at high acute levels of exposure to Pu.
239
Changes in the Permissible Exposure Level for Pu as Suggested
by the Author
As noted in Table I, no values of q and qf2 for occupational exposure
are given at the present time in NCRP and ICRP Handbooks on Internal Dose
for lung. However, using the data provided in ICRP Handbook 2, the value of
0.015 p,Ci 239Pu for uniform distribution can be obtained. This of course
raises the question of the so-called hot particle problem and adequacy of
a value of q or qf2 based on the assumption that the risk of lung damage
(i.e. lung carcinoma) is proportional to the average dose delivered to the
3
entire lung (m =10 g).
No one knows the answer to this question at the present time. Certainly
we would like to have more information. Tamplin and Cochran suggest that
because of the very large dose (thousands of rem/y) in the vicinity of a mi-
cron size particle of 239Pu lodged in lung tissue, the present q for lung
(~ 0.015 liCi) and the corresponding values of (MPC)a for occupational expo-
sure as well as those for members of the public should be lowered by a factor
of 105. Perhaps they are right, but I believe they have not made a strong
case for this factor simply because adequate biological data are not avail-
able and much of that which we have seems to give contradictory information.
Early experiments of Lisco, Finkel, and Brues(16) have indicated there is a
high probability (about 50%) of a malignancy at the site of injections of as
little as one ^g (~ 0.06 p,Ci) of 239Pu in the skin of anfcnals and data of
10
-------
483
Cember perhaps suggest a higher risk due to localized doses in the lungs.
f-t o \
On the other hand, later experiments of Bruesv ' have shown when plaques
of radioactive materials are placed on the skin of an animal, the risk of
skin carcinoma is greater for a uniform distribution of a |j,Ci than for a
(j,Ci localized in .hot spots. The outstanding research of Bair and Thompson^19^
shed much light on the hot particle problem but unfortunately they do not
provide us with unequivocal proof that there is or isn't a hot particle
0.9)
problem. They leave the question as one still to be resolved when they
state "The mean dose to a tissue may be less important, however, than the
dose to localized regions within the tissue." There is no question that
epithelial cells of the skin are very radiosensitive and local doses such
239
as are produced by (j,g quantities of Pu in wounds are very carcinogenic.
The tissues at risk in the lungs also are epithelial and the most important
question remaining is whether or not this large localized dose to the epi-
thelial cells of the lung can likewise result in a high incidence of lung
O"3 Q
tumors when small dust particles of the highly insoluble PuO are inhaled
and find their way to the terminal bronchioles, alveolar epithelial cells, or
are translocated to thoracic and abdominal lymph nodes. It certainly is en-
couraging that there is no clear evidence at the present time that human
occupational exposure to plutonium and other transuranium elements has re-
sulted in any form of cancer. We should realize, however, that no extensive
epidemiological and autopsy study of the exposed human populations has been
completed and with man the average incubation period for tumors of the lung,
bone, liver, or lymph nodes may be 40 to 50 years.
In theory at least the occupational exposure values of q and qf~ for a-
emitting radionuclides that are bone seekers have not been set by the use of
11
-------
484
equations 1 and 2 in the past but by direct comparison with the value of
q = 0.1 |j,Ci of Ra in the human body. It develops, however, that the same
values of q and qf~ as are given by NCRP^ ' and ICRP ^ ' can be obtained by
setting (MPAD) in equation 1 equal to 30 rem/y for bone seeking radionuclides.
This standard of 0.1 (j,Ci of 226Ra was set by the U. S. Advisory Committee on
Safe Handling of Radioactive Luminous Compounds^ ' in 1941. The ICRP
stated, "At the present time, it would be difficult to say which is more
harmful to man a) the dose rate to the total body of 0.1 rem/wk or b) the
O *? A
dose rate to the bone resulting from a body burden of 0.1 |j,Ci of Ra . . ..
Although tumors have not been observed in persons with body burdens of radium
as low as 0.1 u£i, the factor of safety may not be as large as 10 because
turaors have been observed in persons having a body burden less than 1 ^Ci
of radium at the time the tumor was first detected. . . . Several workers
have described changes in skeletal density and/or histopathological changes
in the bone of patients who had 0.1 ^d or less of radium, and more patho-
logical changes may be expected as these individuals become older." In
o o/:
spite of uncertainties regarding the 0.1 |j,Ci standard for Ra, it is
based on over 50 years of human (not other animal) ex erience. With proper
adjustments to determine the equivalent dose (rem) to the critical body tissue
0 0 f\
from a-emitting actinide radionuclides, I believe comparison with Ra and
Ra provides the best method now available for setting suitable radiation
protection standards for these radioactive materials.
I believe the most reliable values of q based on bone as the critical
O*5Q
tissue can be obtained for Pu and some other transuranium radionuclides
by making use of the comparative data on bone carcinoma and sarcome incidence
12
-------
£85
226 239
in dogs that have been injected with known amounts of Ra and Pu as
well as a number. of other a-emitting radionuclides . This outstanding work
has been carried out over a period of many years by a team at the University
of Utah and as pointed out by Bair and Thompson these data can be
239
used in making comparison of the values of q for Pu and the other trans -
uranium a-emitting radionuclides with Ra. If one makes these compari-
sons, the corrections listed below should be made to the value of q = 0.04
239
|j,Ci of Pu which as -indicated above is based on the 0.1 p,Ci Ra standard
when setting N = 5 or on the average dose rate of 30 rem/y to the adult
skeleton :
a) The value of q = 0.04 |j,Ci makes use of an N-f actor of 5 for the
239
a-radiation of Pu and other a-auitting radionuclides in the
skeleton. As pointed out above, this N is intended to be the
relative risk from bone seeking, a-emitting radionuclides (e.g.
239
Pu) in comparison with Ra on the basis of absorbed dose
/ 91 \
(i.e. on a per rad basis). Data of Daugherty and Mays v ' have
shown that this value of N for dogs is somewhere between 5 and 15.
If we accept the value of 15, the appropriate value of q, =0.04
X 5/15 = 0.01
b) The surface to volume ratio for the trabecular bone of the dog
(the tissue in which it is believed most of the bone cancers
originate) is about twice that for man. Thus the same amount of
239 239
Pu in man would have twice the concentration of Pu near
the trabecular surfaces as that in the dog. Making this correc-
tion we have q2 = 0.01 X 1/2 = 0.005
13
-------
C86
c) The rate of turnover (burial) by apposition of new bone of the
deposits of a-emitting radionuclides on the trabecular surfaces
is probably about ten times that in the dog of that in man. Mak-
ing this correction we have q_ = 0.005 X 1/10 = 0.0005 )j,Ci.
(22)
d) Studies of Metivier et al. on the survival time of baboons
X
239
relative to the dog for various concentrations of PuO_ in the
lungs suggest that the baboon is about 4 times as radiosensitive
as the dog. Assuming this same ratio would apply for bone burden
239
of Pu (perhaps a poor assumption) and that the radiosensitiv-
ities of the baboon and man are the same we have then applying
this correction factor q, = 0.0005 X 1/4 =- 10 p,Ci Pu.
The above would correspond to an overall reduction in q of 0.04/10"
• 400 when endosteal tissue of the bone is the critical tissue. Insuffi-
cient data are available to attempt any such correction to the value of q for
the lungs other than apply correction (d) above. Thus we would have q =
0.015/4 =• 0.004 n,Ci when total lung is the critical tissue. This of course
does not address the hot particle problem but rather shelves it until we
have more data.
A somewhat similar problem, namely the possible use of pulmonary lymph
239
nodes as the critical body organ for PuOj, has been under discussion for
many years by Committee 2 of ICRP. There is no question but that when dogs
239
inhale Pu02 in finely divided particles a major fraction ends up in the
(23)
thoracic lymph nodes. Park et al. for example give the percents of
239
alveolar-deposited PuOj 11 years after exposure of about 40% for thoracic
lymph nodes, 13% for liver, and 5% for bone. After many years of consider-
ation of this question the ICRP finally decided not to use the lymph nodes
14
-------
487
as critical body tissue because no animal studies had indicated this to be
the critical tissue in terms of carcinogenesis. Perhaps in this case of
large doses to the lymph nodes we have a good example of cell sterilization.
or complete kill of all the radiosensitive cells in the nodes that are
within the range of the a-radiation. The picture might be quite different
239
for lesser Pu02 concentrations in these nodes which might be experienced
by members of the public from chronic exposure to low dust levels of 239PuO .
Perhaps only time can tell whether or not the present practice of ICRP of
239
averaging the Pu dose in the pulmonary lymph nodes and in alveoli and
terminal bronchioles with the dose to the total lung mass (1000 g) is non-
conservative. Likewise, as many researchers have pointed out, plutonium
and the other transuranium elements tend to localize in the liver during
chronic environmental exposure or from chronic leakage of Pu from the lymph
nodes to the body fluids. Thus in the years ahead we could have some sur-
prises and find that not the bone but the liver or even the lymph nodes
after all are the critical tissues for human damage from chronic exposure
to low levels of the transuranium elements. Hopefully, in the meantime we
will learn more also about other environmental insults because when we do,
I believe we will recognize an even greater urgency to keep their exposure
'i man as low as practicable.
15
-------
REFERENCES
1. K. Z. Morgan, "Tolerance Concentrations of Radioactive Substances,"
J. of Physical and Colloid Chem. 51. 984-1003 (1947).
2. J. G. Hamilton et al. A series of 80 papers published by Hamilton
and his group at the University of California from 1937 to 1947.
Summarized in the Bibliography for Biological Data by M. J. Cook,
x Health Physics 3_, 235-380 (1960).
3. M. J. Cook. These data on the standard man collected by Ms. Cook of
Oak Ridge National Laboratory in 1946 were never published but these
data together with data collected by H. Lisco of the Argonne National
Laboratory were the basis of the standard man data in the 1949 Chalk
River Reports.
4. Chalk River, Canada Conference of members of radiation protection
committees from the United States, United Kingdom, and Canada,
September 29 and 30, 1949. Minutes of this meeting were never pub-
lished but separate sets of minutes by K. Z. Morgan, W. H. Langham,
G. J. Neary, and G. E. McMurtrie were rather widely circulated in
1950.
5. Maximum Permissible Amounts of Radioisotopes in the Human Body and
Maximum Permissible Concentrations in Air and Water, NCRP - Handbook
52 - NBS - March 20, 1953.
6. "Recommendations of the International Commission on Radiological
Protection," British J. of Radiology, Sup. No. 6. 1-92 (1955)
7. Maximum Permissible Body Burdens and Maximum Permissible Concentrations
of Radionuclides in Air and Water for Occupational Exposure, NCRP -
Handbook 69 - NBS - June 5, 1959.
8. Permissible Dose for Internal Radiation, ICRP - Pub. 2, Pergamon
Press (1959).
9. Recommendations of the International Commission on Radiological
Protection, ICRP Pub. 6, Pergamon Press (1964).
10. K. Z. Morgan, "Proper Use of Information on Organ and Body Burdens of
Radioactive Materials," IAEA/WHO Symposium on the Assessment of Radio-
active Organ and Body Burdens, Stockholm, Sweden, Nov. 22-24, 1971,
IAEA/SM/150-50.
11. I. D. J. Bross, "Leukemia from Low-Level Radiation," New Eng. J. of
Med. 287. 107-110 (July 20, 1972).
16
-------
12. J. Baum, "Population Heterogeneity Hypothesis on Radiation Induced
Cancer," given orally at Houston, Tex. meeting of the Health Physics
Society, July 10, 1974.
13. C. W. Mays and T. F. Daugherty, "Progress in the Beagle Studies at the
University of Utah," Health Physics 22., 793-801 (June 1972).
14< 224W* MaYs» H< sPifiss, and A. Gerspach, "Skeletal Effects Following
^Ra Injections into Humans," Reported at the Symposium on Biological
Effects of Injected z^4Ra and Thorotrast, Alta, Utah, July 21-23, 1974.
To be published in Health Physics early in 1975.
15. A. R. Tamplin and T. B. Cochran, "Radiation Standards for Hot Particles,"
publication of Natural Resources Defense Council, 1710 N. Street, N.W.,
Washington, D. C. 20036, February 14, 1974.
16. H. Lisco, M. P. Finkel, and A. M. Brues, "Carcinogenic Properties of
Radioactive Fission Products and of Plutonium," Radiology 49, 361 (1947).
17. H. Cember, "Radiogenic Lung Cancer," Progress in Experimental Tumor
Research, Vol. 4, p. 251 (1964); H. Cember, J. A. Watson, and T. B.
Brucci, "Pulmonary Effects from External Radiation," presented at AIHA
meeting in Philadelphia, Pa., April 26, 1956.
18. A. M. Brues, unpublished experiments, Argonne National Laboratory (1953).
19. W. J. Bair and R. C. Thompson, "Plutonium: Biomedical Research,"
Science 183. 715-722 (Feb. 22, 1974).
20. National Bureau of Standards Handbook 27, "Safe Handling of Radioactive
Luminous Compounds" (1941).
21. T. F. Daugherty and C. W. Mays, ""Bone Cancer Induced by Internally-
deposited Emitters in Beagles," in Radiation Induced Cancer. International
Atomic Energy Agency, Vienna, 361-367 (1969).
22. H. Metivier, D Nolibe, R. Masse, and J. Lafuma, "Excretion and Acute
Toxicity of yPu02 in Baboons," Health Physics 27., 512-514 (Nov. 1974).
23. J. F. Park, W. J. Bair, and R. H. Busch, "Progress in Beagle Dog
Studies with Transuranium Elements at Battelle-Northwest," Health Physics
22, 803-810 (June 1972).
17
-------
490 GENERAL £$ ELECTRIC
NUCLEAR ENERGY
DIVISION
GENERAL ELECTRIC COMPANY, 175 CURTNER AVENUE, SAN JOSE, CALIFORNIA 95114
BWR PROJECTS DEPARTMENT
Phone (408) 297-3000, TWX NO. 910-338-0116
November 22, 1974
Director, Criteria and Standards Division (AW-560)
Office of Radiation Programs
U. S. Environmental Protection Agency
Washington, D. C. 20460
SUBJECT: PUBLIC HEARING - PLUTONIUM AND THE TRANSURANIUM ELEMENTS
Dear Sir:
In accordance with the Federal Register notice of October 24, 1974 and
Dr. W. D. Rowe's letter of October 25, 1974, the General Electric Company
requests the opportunity to present testimony at the subject hearing scheduled
for December 10, 1974. We plan to submit a written statement at that time,
and we also request the 20-minute period suggested in the hearing notice for
the presentation of an oral summary of our statement.
The General Electric statement will address the subjects of:
1. The views of the General Electric Company for the utilization of
Plutonium for power production from domestic fuel sources both
for recycling in light water reactors and in fast breeder reactors;
2. The need for environmental standards which are based on reasonable
and proper evaluation of risk, with due regard for costs and benefits,
so that the beneficial use of plutonium for power production may
be realized;
3. The experience of the General Electric Company on the environmental
aspects of plutonium, both in the operation of the SEFOR experimental
facility and in the handling of plutonium over the past fifteen years
at our Vallecitos Nuclear Center.
Our statement will be sponsored by Mr. George J. Stathakis, Vice President
and General Manager, Nuclear Energy Products Division, General Electric
Company, San Jose, California.
Sincerely,
Ivan F. Stuart, Manager
Safety and Licensing
Mail Code 683 Ext. 2791
/1ml
BE SURE TO INCLUDE MAIL CODE ON RETURN CORRESPONDENCE
-------
497
Atomic Industrial Forum, Inc.
475 Park Avenue South
New York, New York 10016
Telephone: (212)725-8300
Cable: Atomforum Newyork
Carl Walske
President
November 22, 1974
The Director
Criterion Standards Division (AW-560)
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D.C. 20460
Dear Sir:
In accordance with the notice published in the Federal Register,
October 24, 1974, time is hereby requested to make an oral presenta-
tion at the public hearing on plutonium and the transuranium elements
scheduled for December 10. Our presentation will be in the form of
a panel discussion which will include several experts in the pluto-
nium field. The names of the panelists will be forwarded to you as
soon as final arrangements are concluded and in any event, prior to
commencement of the proceedings. The panelists will discuss in depth
the items designated in paragraphs 1 through 5 of the October 24
Federal Register notice, with particular emphasis on adequacy of
standards, the health effects of plutonium and experience with pluto-
nium to date. It is anticipated that 60 minutes will be required for
this presentation.
Communications with respect to this matter should be directed to me
at the above address.
Sincerely,
CW:gjh
-------
Westinghouse Electric Corporation Power Systems PWR systems Division
Box 355
Pittsburgh Pennsylvania 1 5230
November 22, 1974
NS-RS-447
Director
Criteria and Standards Division (AW-560)
Office of Radiation Programs
U. S. Environmental Protection Agency
Washington, D. C. 20460
Dear Sir:
In response to the invitation of the Environmental Protection Agency
("EPA") appearing in 39 F.R. 37810 on October 24, 1974, the Westinghouse
Electric Corporation ("Westinghouse"), P. 0. Box 355, Pittsburgh,
Pennsylvania 15230, wishes to notify the EPA of its desire to present
an oral statement (and to submit a written statement for the record)
at the public hearing being conducted by EPA to ascertain whether any
new standards are needed to assure protection of the environment and
of the public health from potential contamination by radionuclides of
the transuranium elements. Mr. Frederick W. Kramer, Engineering Manager,
Nuclear Fuel Division, and Dr. J. H. Wright, Director, Environmental
Systems Department, will make the presentation on behalf of Westinghouse.
We estimate that about twenty (20) minutes will be needed to complete
our presentation. A-summary of the areas to be covered in our presenta-
tion follows:
1. General
Westinghouse is pleased to have this opportunity to participate
in EPA's effort to obtain further information on projected releases to
the environment of transuranic elements, the costs associated with these
projected releases, suggestions on possible alternative actions, and the
resulting potential environmental and public health impacts for the pur-
pose of evaluating the need to establish, at this time, new environmental
standards. Westinghouse suggests that generally applicable standards
for environmental levels of plutonium and the other transuranium elements
must be based on health effects data and, insofar as possible, on cost-
benefit analyses which compare alternative control options in activities
comprising the plutonium fuel cycle in the context of present fallout
-------
493
MS-RS-447 -2- November 22, 1974
levels, as well as with alternative energy options. With respect to data
on health effects, we urge that only authoritative, documented, and well
reviewed sources be used by the EPA in developing its standards. We
recommend that whatever risk estimates or radiation effects data are
utilized by EPA to develop new standards, that such factors be balanced
by careful consideration of the total environmental risks associated with
nuclear and non-nuclear options relative to the magnitude of radiation
from natural background, ambient levels of plutonium from fallout, and
medical applications in determining the total dose commitment to the pop-
ulation.
Westinghouse believes that the current regulations and pro-
cedures for controlling releases of plutonium and the other transuranium
elements are adequate and that there is merit in obtaining further
operational experience and R&D before developing revised or additional
standards. We fully endorse EPA's policy of issuing environmental impact
statements in connection with formulating generally applicable radiation
standards under the Atomic Energy Act of 1954, as amended.
2 & 3. Dosimetry, Health and Environmental Effects; Environmental
Levels and Pathways
With respect to the construction and operation of facilities
handling plutonium, Westinghouse identifies important pathways for any
possible releases of transuranics through the ecosystem. Westinghouse
also demonstrates how limits are placed on permitted plant effluents, and
how monitoring of plant effluents in the environment is performed to
assure that these limits are not exceeded.
In this connection, it is suggested that considerable information
exists to permit projections of health effects from measured concentrations
of plutonium, and of the pathways for transport of plutonium through the
ecosystem.
Admittedly, such projections are necessarily approximate, and
continuance of the already extensive research programs is encouraged.
However, it is suggested that use of this information in conjunction with
careful monitoring of the effluents from existing and near-term projected
plutonium handling facilities will verify that the impact of such oper-
ations is kept acceptably small.
-------
US-RS-447 -3- November 22, 1974
4 & 5. Applications Using Plutonium; Control and Cleanup Technology
The statement by Westinghouse presents current and projected
uses of plutonium as fuel in the light-water and breeder reactors for
commercial power generation. We present the Westinghouse estimate of the
projected quantities of plutonium available from the overall light-water
reactor industry during a period through approximately 1990. The West-
inghouse projections of the plutonium available from the light-water
reactors are consistent with the data on plutonium availability set forth
in GESMO (WASH-1327, August 1974). On the assumption that plutonium
recycle will constitute the most prominent use of plutonium until the
Liquid Metal Fast Breeder Reactor makes its substantial contribution to
the quantities available and used, we believe that the magnitude of the
release of transuranium elements can be quantified by consideration of
the actual operating experience of the Westinghouse Plutonium Fuels
Development Laboratory (PFDL) and on the basis of the projected effects
of the proposed Westinghouse Recycle Fuels Plant (RFP). Our presentation
includes data on the magnitude of possible releases to the environment
from the Westinghouse PFDL and the projected possible releases from the
proposed Westinghouse RFP.
The Westinghouse statement also identifies the plant protection
devices and installations utilized in fuel fabrication facilities for
minimizing and restricting possible releases of transuranium elements to
the environment. Methods for decommissioning fuel fabrication facilities
are described. Release data, demonstrating the effectiveness of currently
available technology, for the Westinghouse PFDL are also presented.
Very truly yours ,
Romano Salvatori, Manager
Nuclear Safety Department
/snih
-------
495
2677 Ellendale Place
Los Angeles, Calif. 90007
November 21;, 197U
Director
Criteria and Standards Division (AW-5>60)
Office of Radiation Programs
II. S. Environmental Protection Agency
Washington, D. C. 20U60
Dear Sir:
Pursuant to the hearings beginning December 10, 197U on plutonium
and the transuranium elements, I most strongly urge the Environmental Protec-
tion Agency to set forth definitive and detailed maximum permissible levels
of ground contamination for these elements (1) within occupied structures,
(2) outdoors in inhabited areas, (3) on cropland, (U) on grazing areas for
livestock. In those cases where significant solubility is involved, MFC's
for public water supplies are also requisite.
The importance of setting definite standards before the first major
releases of these substances cannot be overstressed. Following a large acci-
dental or malevolent dispersion in an urban area, there would be. tremendous
political pressure not to evacuate, or to engage in less than adequate decon-
tamination efforts, lest citizens be alarmed or discommoded by such measures.
This cannot be permitted to occur. The first urban incident, in the absence
of clear EPA guidelines, will no doubt set a norm of negligence with perhaps
cumulatively devastating effects.
As an indicator of the importance of the subject, I enclose some
recent correspondence, in which the Atomic Energy Commission did not dispute
my estimate that one pound of power-reactor-grade plutonium, if dispersed as
oxide particles, could bring £7 square miles of downtown Washington to levels
requiring some evacuation and cleanup, EPA is deserving of the highest com-
mendation for addressing this most vital topic.
Very truly yours,
/
Letter to President 8-2lt-7U
Reply from AEC 10-3-71;
Letter to President 10-7-7U
L. Douglas DeNike, Ph.D.
-------
496
26?? Ellendale Place
Los Angeles, Calif. 9000?
August 2h, 197U
President Gerald R. Ford
The White House
Washington, D. C. 20^00
Dear President Ford:
So-called "reactor grade" plutonium, as recovered from
nuclear power plant spent fuel, is 6.6 times as radiocontaminative as fairly
pure plutonium-239. The numerical proof of this is appended to this letter.1
Tvro eminent nuclear scholars, Mason Willrich and Theodore
B. Taylor, state that dispersion of 100 grams (less than f pound) of plutonium-
239 could produce "significant contamination requiring some evacuation and
cleanup11 over 5,000,000 square meters (1.93 square miles}.2 This works out to
8.7U -square miles per evenly distributed pound of Pu-239. But since reactor-
grade plutonium is 6.6 times as hazardous, one pound of the latter could bring
57 square miles to levels requiring some evacuation and cleanup.
This area is equivalent to a circle with its center at
the White House and its perimeter, U.3 miles distant enclosing virtually all
the essential government facilities of Washington, D. C. and adjoining Virginia.
Does it require an atomic explosion to destroy the nation's
capital as a center of government? It appears that the answer is in the negative.
It appears that the only requirement is possession of one pound of the material
(recycled plutonium) which the Atomic Energy Commission hopes to make the primary
energy source of the nation. • *•
Questions will occur to the reader with regard to this
conclusion. Would not plutonium be difficult to obtain by theft? Noj as recently
as last April the AEC's own consultants called for immediate and drastic upgrading
in the safeguarding of special (fissionable) nuclear materials.3
Would not the handling and dispersion of plutonium be
difficult and dangerous for unauthorized persons? No; the alpha-particle radio-
activity characteristic of plutonium is non-penetrating. Thus it would not
threaten criminals or terrorists who handled it in improvised gloveboxes.
Its dispersion could be simply effected in three ways: (1) By burning in an
ordinary fire. Plutonium metal is pyrophoric; i.e., it tends to ignite spon-
taneously, forming fine oxide particles which present an unparalleled lung-cancer
hazard if inhaled. (2) By attaching the packaged metal or oxide to an ordinary
chemical explosive charge. (3) By attaching a leaky container of an insoluble
plutonium compound to the underside of a public transit vehicle having s known
route.
-------
497
But granting the foregoing, could not dispersions.of radio-
nuclides be readily removed by hosing, or rainfall? Hosing woul3 be expensive,
and would presuppose evacuation until suited and masked decrv'. ^nation teams
could complete it. Whether plutonium particles could be sufficiently removed
by hosing, rainfall, or any other means within acceptable dollar and time limits
is very uncertain. A large number of surfaces, ranging from lawns to rooftops,
would tend to trap and hold radioactive particles for later resuspension (and
thus possible inhalation) by wind, earth-moving operations, etcetera. Maleficent
persons could compensate in advance for the estimated efficacy of decontamination
procedures by releasing a proportionately greater amount of radioactivity per
unit of area. In that regard, it should not prove significantly more difficult
for evil-doers to divert or smuggle from abroad ten or more pounds of plutonium
than a single pound of the material. Roughly eighteen pounds of reactor-grade .
plutonium would suffice for the construction of a "crude" atomic bomb, of course.'1
My contention here is that the radiocontamination of Washing-
ton, D. C. with long-lived extremely carcinogenic mixed isotopes of plutonium
in particulate form might be nearly as disruptive to the nation as its destruction
by a nuclear explosion. A "crude" low-yield implosion bomb might be expected to
scatter particles of unfissioned plutonium downwind, producing much the same
effect as a dispersal device.
Mr. President, let me be quite candid. If the nuclear power
reactor enterprise, involving the uranium-plutonium fuel cycle, is permitted to
expand as projected, the fulfillment of the above scenario is only a matter of
time. It is beyond the puissance of the government of the United States to
establish adequate safeguards for the handling of these materials when fifteen,
soon to be thirty, sovereign nations are involved. However, the government does
have the power to seek a bilateral declaration with the Soviet Union, stating
that the two superpowers will take any steps necessary to prevent additional
nations from acquiring nuclear-power capacity.
I am writing a popular-level book on radiological terrorism,
crime, and warfare. Nothing would give me greater pleasure than to be dissuaded
from publishing it by prompt government action toward the dismantling of the
fission-power aberration here and abroad. However, nothing short of that will
dissuade me from what I feel is necessary to prevent otherwise certain national
suicide. Needless to say, if I do not write the book, another will do so.
I do not enjoy the acute moral dilemma involved in presenting such information
as this to a general readership. Yet, circumstances have brought us to the point
at which patriotism must take unusual forms.
Very truly yours,
Enclosures
References L. Douglas Dellike, Ph.D.
Radioactive Malevolence
-------
- 3 -
Footnotes
1, Each metric ton of spent power-reactor fuel contains about 13.OU kilo-
grams of plutonium isotopes, with activity as follows:
Air concentration to lung
Isotope . Activity (curies) dose conversion factor
Pu-238 U 000 1
Pu-239 500 1
Pu-2UO 650 1
Pu-2la 150,000 (times .001=150) .001
Total activity 5,300 curies of Pu-239 equivalent lung-dose activity.
Each 16.2 grams of Pu-239 contain one curie of alpha activity; thus 5,300
curies of Pu-239 would weigh 85.86 kilograms, or 6.6 times the weight of the
equivalent in power reactor grade plutonium, 13.OU kilograms.
Reference: Environmental Protection Agency report EPA-520/U-73-002,
Environmental Radiation Dose Commitment; An Application to the Nuclear Power
Industry. February 197Uf Tables B.U and D.2.
2. Willrich M. and Taylor T. B. Nuclear Theft; Risks and Safeguards,
Ballinger, 19?U, p. 25, Table 2-2. "~
3, "The Threat of Nuclear Theft and Sabotage," Congressional Record.
April 30, 197U, pp. S 6621-6630.
Ij. Willrich & Taylor, op. cit., p. 13.
-------
UNITED STATES
ATOMIC ENERGY COMMISSION
WASHINGTON, D.C. 20545
C?T T '974
Dr. L. Douglas -J5*Nike
T6?7 Ellendale Place
Los Angeles, California 90007
Dear Dr. DeNike:
Thank you for your letter to President Ford dated August 2U, 197U, which
has been referred to me for response. Your letter, as well as articles
ar.d other correspondence you have had with the AEC, evidences a good know-
ledge of and concern for the possibilities of nuclear related terrorism.
Sone of the various problems to which your letter refers certainly require
vigorous and effective action in order to assure that the benefits of
nuclear energy may be obtained with minimum risk. Your view that the
spread of nuclear-power capacity in the U.S. and abroad presents so great
a hazard that this industry should be dismantled, is not universally
shared. There is broad concensus here and abroad that nuclear energy is
an essential element of the power industry of the future. Recognizing,
however, that the future development of this nuclear capacity may increase
the possibilities of nuclear terrorism, the AEC, (as well as other govern-
ment agencies), is expanding its safeguards efforts. Your letter men-
tioned the expansion of nuclear power operating capacity in sovereign
nations. The U.S. will participate in such expansion only when we are
confident that proper safeguards are to be adopted. However, there are
options open to foreign nations to develop their nuclear power capacity
vithout using U.S. (or Soviet) nuclear technology. We are not unmindful
cf the problems arising from this situation, and we are -trying to increase
the effectiveness of safeguards in pertinent areas so far as we are able.
The book you propose to write may serve a useful purpose. You are
evidently aware of some of the problems of dealing effectively with these
sheets without contributing to an increase in the hazards. If it would
** helpful to you, we would be happy to communicate further with you about
questions you may have as to the direction and effectiveness of our safe-
fjuards program.
Sincerely
499
Edward B. Ciller
Assistant General Manager
for National Security
-------
503
2677 Ellendale Place
Los Angeles, Calif. 90007
October 7, 197U
President Gerald R. Ford
The White House
Washington, D. C. 20^00
Dear Mr. President:
On August 2U, I wrote to you providing my calculation
that a single pound of plutcnium recovered from nuclear power plant spent
fuel would suffice to contaminate, to levels requiring evacuation and cleanup,
virtually all the essential government facilities of Washington, D. C. and
adjoining Virginia. I am now in receipt of the Atomic Energy Commission's
reply to this letter, dated October 3, over the name of Edward B. Giller.
Copies of both pieces of correspondence are enclosed herewith.
General Giller, the AEC's security chief, did not even
attempt to refute my claim. He could not have cone so successfully, for the
contamination of Denver from the plutonium fire at Rocky Flats (September 11,
1957) testifies adequately to the environmental mobility of wind-borne pluton-
ium particles. Indeed, the AEC has conducted extensive studies on the trans-
port of plutonium in the enviroa-nentj see, for example, pages U.G-23 through
U.G-26 of the draft AEC document, WASH-1535, in which plutonium releases at
smokestack level in Illinois are predicted to deposit throughout the eastern
United States.
One could not guess the subject matter of my letter from
General Giller1s reply, and his failure to address it can be construed as a
tacit admission of its accuracy. He goes on to credit me with "good knowledge
of and concern for the possibilities of nuclear related terrorism." The basic
truth of my assertion appears in itself to be adequate cause for the White House
to hold in abeyance the AEC's proposal for the large-scale use of recycled
plutonium reactor fuel, which is presently in the stage of draft environmental-
statement review.
General Giller states that there is "broad concensus (sic)
here and abroad that nuclear energy is an essential element of the power indus-
try of the future." Herein I will indicate why any existent consensus is spur-
ious, inasmuch as it is based upon unexamined hopes regarding the possible effi-
cacy of safeguards in the atomic power field. This topic is further explored in
my enclosed review from the October issue of the Bulletin of_ the Atomic Scientists.
There exists only one possible precedent for the level of
security presumed to be maintainable for fuels in a fully developed fission-
power economy. This is the relatively good record held thus far by the nuclear
weapons industry in preventing the theft and deliberate dispersion of radioactive
materials. For several reasons, the past record provides insufficient assurance
-------
President Gerald R. Ford - October 7, 197U - page 2
501
for th3 future. (A) Initially, the safeguarding of American nuclear weapons
abroad has recently been criticised as "deplorable" by Senator John 0. Pastore,
Vice-Chairman of the Joint Comnittee on Atomic Energy. This suggests that the
security of such weapons inheres to a significant degree in the fortuitous
ignorance of would-be thieves and terrorists regarding their vulnerability.
(B) In contrast to the six sovereign nations now known to be involved in the
manufacture of nuclear explosives, by 1980 there will be thirty nations expected
to have nuclear power stations (M. Willrich and T. B. Taylor, Nuclear Theft:
Risks and Safeguards, page 197). (C) As demonstrated in my letter of August 2U,
the plutonium utilized in this burgeoning industry will be 6.6 times as radio-
contaminative, weight for weight, as pure plutonium-239—capable of bringing
5>7 square miles per pound to evacuation levels.
(D) Roughly 200 tons of plutonium-239 have thus far been
produced for U.S. nuclear weapons. The quantity of plutonium anticipated to
be generated in U.S. civilian power reactors will exceed this within ten years.
(E) Information concerning safeguards and security measures in the plutonium-
fuels industry will over tine leak irreversibly to the public, and to public
enemies. Coordinately, the information-gathering abilities and weapons-con-
struction talents of public enemies can be expected to improve.
In clear recognition of the inadequacy of present safeguards-
security standards for the future, the AEG has proposed creation of a federal
guard force, and the requirement of AEG security clearances for plutonium workers,
in its generic environmental statement on plutonium recycle (August, 197U). Such
tightened precautions will not directly affect the practices of other nuclear
nations, whose diverted materials may promptly reappear in criminal or subversive
possession within the United States. The clear international ramifications of
the fissile-materials problem are for some a signal for despair. For the govern-
ment of this country, they should be a signal for top-priority efforts to remove
the peril.
Exhaustive study reveals only one way by which this peril
can be removed. Even if a paper-perfect safeguards system is implemented on
a planetary basis, actual practice will fall short of the regulations—and
shortfalls are unacceptable. We note that in the American nuclear power industry
during fiscal 197U, the AEC logged a total of 3,333 safety violations. We may
look forward to violations of safeguards regulations. Perfection is necessary
and perfection is unattainable.
Another approach will demonstrate that the manageability of
the nuclear safeguards problem is an article of faith, not a scientifically
grounded judgment. It suffices to note the absence of any formal or informal,
public or secret "stop criterion" for nuclear-power development. Every nuclear
plant has an elaborate set of pre-specified quantitative limits, whose breach
results in automatic shutdown, lest continued operation result in an unmanageable
situation. Yet no such advance set of shutdown criteria exists for the nuclesr
industry a_s a whole. There may be good reasons wny such criteria^""if they exist,
should not be made public. Yet it is my confident assertion that they do not
exist, even as top government secrets.
-------
President Gerald R. FoTd - October 7, 197U - page 3
There is, furthermore, no assurance that sh-- ^ d shutdown
of the fission power industry be undertaken (at svch future r ,• as criminal
acts involving it have become clesrly unacceptable), that this can be accom-
plished with reasonable safety from further depredations. In brief there
appears to be no contingency planning whatever for the orderly phaseout of
nuclear power, should untoward events show this to be necessary. Perhaps the
government fears that such contingency planning, if undertaken, would leak out
to the public, further demoralizing the atomic energy industry. If so the
government might do well to apply the same concern about information leakage
to the utilities' proprietary facts relevant to nuclear sabotage and theft
which are bound to seep out via loose-lipped and disgruntled employees.
Considerably more could be written to the effect that the
fission-energy enterprise is an outgrowth of faith, and not p, technology tied
to defensible suppositions about the nature of human beings and their social
arrangements. But for now, I submit the necessity of the Executive Branch's
developing the contingency planning delineated above. This should include:
(1) Unambiguous quantitative criteria for reaching the conclusion that nuclear
safeguards and security measures are unmanageable in principle, based upon
analysis of possible future events. (2) Plans for the orderly and reasonably
secure phaseout of fission-based energy systems, on a transnational scale,
should the first condition materialize. Even with its broadened mandate as
ERDA. I doubt that the Atomic Energy Commission can be entrusted with the
development of these necessary contingency plans. Its unwillingness to
address such issues objectively is legendary. Rather, the White House must
seek a source of expertise which is independent of the AEC or its successor.
Sincerely yours,
Enclosures L. Douglas IMike, Ph.D.
-------
LEON LEVENTHAL
503
LFE ENVIRONMENTAL
CORPORATION
ANALYSIS LABORATORIES DIVISION
2030 WRIGHT AVE. • RICHMOND, CALIFORNIA 94804
GENERAL MANAGER
18 November 1974
Office of Radiation Programs
East Tower
Environmental Protection Agency
401 M Street, S.W.
Washington, D. C. 20460
Gentlmen:
I recently noted there will be public hearings starting December 10th,
1974 to examine the need for establishing radiation protection standards for
plutonium and other transuranium elements in the environment. I would
appreciate a copy of the detailed agenda and schedule. I would also like to
get a copy of the hearing transcript when it is available.
Our organization has been involved in the analysis of the transuranium
elements for a number of years. For the record, I gave a paper on "Analytical
Considerations Connected with the Transuranium Elements", at the American
Nuclear Society Meeting in Washington, D, C. on October 31st. This was part
of an invited session on Environmental Levels of the Transuranium Elements,
which I chaired. I also gave a paper the previous week at the Analytical
Conference at Gatlinburg entitled, "A Survey of Radiochemical Techniques
for the Assessment of Plutonium and Americium in Environmental Samples".
So you see, we are very much interested in this subject.
Very truly yours,
•
Leon Leventhal
LL/kc
-------
11 Brown Road
Great Neck, N. Y. 11024
November 19, 1974
Environmental Protection Agency
Office of Radiation Programs
AW - 560
Washington, D.C. 20460
Gentlemeni
This is with reference to the item entitled "EPA to
Weigh Setting Plutonium Standards", Citizens Bulletin,
October 1974.
An attempt to set standards for release of plutonium
into the environment would be tantamount to legitimizing
the spread of a very toxic and longlasting pollutant as a
legacy for our children and their children.
The public should not be exposed to even minute
quantities of plutonium. It is inconceivable that so
poisonous, pernicious and irreversible a poison as plutonium
should be accepted, even in micrograra quantities, as "limits",
by EPA.
Mankind can no more coexist with plutonium than it can
with botulin toxin. Setting standards for either poison
would make no sense and would be equally irrelevant.
Please do not help legitimize the ultimate pollutant.
Sincerely yours,
Nat. H. Sauberman,P.E.
-------
505
UNITED STATES
ATOMIC ENERGY COMMISSION
WASHINGTON, D.C. 20545
November 29, 1974
Director
Criteria and Standards Division
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D. C. 20460
Dear Sir:
Pursuant to the Federal Register Notice of Thursday, October 24, 1974
(39 FR 37810), this is to give notice of the Atomic Energy Commission's
(AEC) intent to participate in the public hearing to be held by the
Environmental Protection Agency beginning December 10, 1974, on
plutonium and transuranium elements.
In order to cover adequately the overall activities of the AEC and
to reflect the division of responsibilities and programs within the
AEC, separate testimony will be presented by the General Manager's
operating side and the Regulatory side. Testimony from the General
Manager's side will be presented first since, it does reflect the
scope of the entire subject of plutonium and as such better sets
the stage for the Regulatory input. For your information, please
find enclosed two summary outlines which identify the major topics
to be addressed in the AEC testimony.
As indicated in the outline, there are a number of individuals under
the leadership of Dr. James L. Liverman, Assistant General Manager
for Biomedical and Environmental Research and Safety Programs,
scheduled to address the General Manager's program. In addition,
supplementary information will also be submitted for the hearing record.
The General Manager testimony will include an introductory statement
which provides an overview and scoping of the subject. This will
be followed by a series of presentations by AEC Headquarters and
laboratory representatives which address: (1) potential source terms
and control measures; (2) environmental levels and pathways; and (3)
biomedical effects.
-------
506
Director -2-
Lester Rogers, Director of Regulatory Standards, will make a brief
statement, approximately 30 minutes long, on the regulatory program.
This statement will summarize the detailed written information being
submitted by Regulatory for the record. Mr. Rogers will describe
the manner in which the AEC develops its regulations and exercises
its regulatory responsibilities for commercial activities involving
plutonium and transuranium elements. The testimony will summarize
AEC regulations already issued or under development which concern
the releases of plutonium and transuranium elements to the environment.
In addition, it will summarize licensing experience and future pro-
jections concerning the magnitude of the quantities of plutonium and
transuranium elements in commercial fuel cycle facilities and products.
As the General Manager testimony is still in preparation, specific
times for each presentation have not been assigned as yet. However,
it is anticipated that the total time necessary for both General
Manager and Regulatory presentations will approximate four hours.
Your office will be advised as soon as possible of more definitive
time requirements.
Sincerely,
Paul C. Bender
Secretary of the Commission
Enclosures:
1. Outline of General Manager Testimony
2. Outline of Regulatory Testimony
-------
L:\CLUS URK 1
507
OUTLINE OF GM TESTIMONY FOR EPA HEARING
December 10, 1974
A. Headquarters Introduction - James L. Liverman
1. General scoping of the subject
2. Existing information, location, how to find it
3. How this information has been used
4. What additional information is needed
5. Current and projected research to address those needs
B. Potential Source Terms and Control Measures - Robert E, Yoder
1. Transuranium fuels and recycle
2. Weapons and production
3. SNS operations
4. Waste handling
5. Medical uses
C. Environmental Levels - Burton Bennett/McDonald E. Wrenn
1. Location, composition, and origin
a. worldwide
b. local
c. med ia
2. Disposition with time
3. Environmental pathways
D. Biomedical Effects - William J. Bair, Chet Richmond, William Burr,
Roy Thompson
1. Health effects - experimental
2. Health effects - human experiences
3. Implications with respect to protection criteria
-------
ENCLOSURE 2
508
OUTLINE OF REGULATORY TESTIMONY FOR EPA HEARING
December 10, 1974
A. Regulations Controlling Population Exposures to Radiation
B. Relative Regulatory Roles of AEC and EPA
C. Examples of the Exercise of Regulatory Responsibility by
AEC
D. Characterization of Commercial Facilities Processing Large
Quantities of Plutonium and Transuranium Nuclides
E. Releases of Plutonium and Transuranium Nuclides to the
Environment from Commercial Facilities
F. Use of Technical Specifications and Monitoring to Assure Safe
Operation of Facilities Processing Large Quantities of Plutonium
and Transuranium Nuclides
G. Standards for Controlling Levels of Plutonium and Transuranium
Nuclides in the General Ambient Environment
-------
CENTRAL
MIDWEST
REPRESENT/HI^ g
NATIONAL AUDUBON SOCIETY
CENTRAL MIDWEST REGIONAL OFFICE
ROUTE 1, BOX 19 • MAUCKPORT, IN. 47142 • (812) 732-4349
November 2lr I974
Director, Criteria and Standards Division (AW-560)
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D. C. 20460
Dear Sir:
As per your request for comments, either written or oral, re: the
potential adverse environmental impact of releases of plutonium and
other transuranium elements, would you please enter the enclosed
written comments into the record on behalf of the:
Central Midwest Regional Office of the National Audubon Society
Ohio Audubon Council
Indiana Advisory Committee to the National Audubon Society
Kentucky Audubon Council
Audubon Council of Illinois
Special credit should be given to our specialist, Dr. Owen Davles of
the Black River Audubon Society, Elyria, Ohio.
Sincerely,
Ayron J. Swenson
Central Midwest Representative
MJS/tma
Central Midwest Region
Illinois • Indiana • Kentucky • Ohio • Tennessee
-------
510
The U.S. Environmental Protection Agency would not be conducting
a public hearing on plutonium and the transuranium elements if major uses
of these elements were not planned. Certainly among the applications
being considered is the fast-breeder nuclear reactor and the use of
plutonium produced therein as a fuel for the light water reactors. The
major question really should be : "Can our society in any way accept
the wide spread use of plutonium?" For plutonium is not just another
run-of-the-mill potential environmental pollutant.
The Atomic Energy Commission states that:
(I) The alpha radiation given off by plutonium is especially damaging
to the blood-forming organs of the bones and can produce bone diseases
many years later.
(2) Plutonium may enter the body through cuts or abrasions of the skin,
by being swallowed, or most importantly by inhalation. (Small amounts
of inhaled plutonium can cause lung cancer.)
(3) Once in the body, plutonium is eliminated so slowly that as much
as 80% of any amount taken in will still be there 50 years later.
(4) The maximum permissible body burden, or the total amount of
plutonium that can be accumulated in an adult without producing undue
risk to health, has been set at 0.6 microgram.
(The reference for items I through 4 is "Plutonium", a booklet of the
Understanding the Atom Series of the Division of Technical Information
of the Atomic Energy Commission.)
(5) Plutonium-239 has a half-life of approximately 24,000 years and thus
will take hundreds of thousands of years to decay to an innocuous level
of radiation.
-------
511
(6) There will be an unavoidable loss rate of I to 2% in handling
plutonium. (Science/ April 9, 1971, pp. 143-146) This is most
serious, since the plutonium inventory has been projected to be
720,000 kilograms by the year 2000. (Science, April 9, 1971,
pp. 143-146)
The tons of plutonium that would be produced by the fast-
breeder reactors would be transported across the nation. Such
shipments will inevitably be involved in highway accidents and will
be subject to hijackings and diversion for the production of
nuclear bombs.
It would seem inevitable that large groups of citizens would
be subjected to security clearance and security procedures. The
present situation, where Texas state police maintain files on nuclear
power plant opponents, would be minor by comparison.
The Environmental Protection Agency is attempting to
perform a cost-benefit analysis on plutonium. Yet how can such an
analysis take into account the certain loss of individual freedom and
rights to individual privacy? How can the value of human life be
evaluated in a cost-benefit analysis?
The recent disclosure of the leakage of plutonium at the Mound
Laboratory at Miamisburg, Ohio does not inspire confidence that humans
can maintain the necessary vigilance to operate a plutonium industry
successfully. In 1974, unexpectedly high plutonium levels were found
in nearby water areas and on portions of the land at the laboratory. The
-------
512
source of the plutonium has subsequently been indicated to be a pipe which
reportedly had been leaking since 1969. One wonders how many incidents
of a like nature have occurred and have either remained undetected or
have been "covered-up". There apparently is no possible way to evaluate
the consequences of the Miamisburg leak, since there is no reliable means
to establish that the plutonium that leaked has been completely contained.
The monitoring program at the Mound Laboratory obviously was not proper
or the leak would not have gone undetected for such a length of time.
With a widespread plutonium industry, such lax monitoring techniques
would eventually lead to a major contamination problem which just would
not go away within the lifetimes of humans. How could this be evaluated
in a cost-benefit analysis?
The question that we should be asking would seem to be "Should
we proceed at all with the development of applications using plutonium
when problems raised by the toxicity of plutonium and problems of nuclear
theft are apparently far from being solved and may remain so for a great
number of years? "
-------
-------
515
BASIC REQUIREMENTS FOR STANDARD SETTING ON THE CONTROL
OF TRANSURANIUM ELEMENTS IN THE ENVIRONMENT
by
R. A. Karam
School of Nuclear Engineering
Georgia Institute of Technology
Atlanta, Georgia 30332
Like all standards, environmental standards for the protection of the
general environment from transuranium elements require: (1) that society
define the cost (risk) it is willing to pay for the benefits it derives
from the use of plutonium, and (2) that the technical know-how is at hand
to assure that that cost is not exceeded.
Cost (Risk) - Benefit
The cost (risk) society is willing to pay for a given benefit is by
no means easy to establish. It involves, among other things, putting a mone-
tary value on human lives and on ecological changes which may not be revers-
ible. In many cases the detriments to people and to the environment result-
ing from all the activities involved in producing the benefit are not known.
This is especially true of effects on future generations. The identification
and quantification of costs (risks) in the broad societal sense and the syn-
thesis of these costs into decision making machinery should be a continuing
goal of responsible society.
The term cost-benefit analysis correctly implies that there is a price
that society pays for every benefit it derives from its industrial activities.
The price may not be readily equated to a lump sum when one considers the
price associated with the death of Lake Erie, the hazards of vinyl chloride,
-------
517
such benefits as the automobile and the risk associated with events such
as lightning, falls, drowning, firearms, and natural diseases. The price
— 2 — ft
varies between 10 and 10 . It should be noted that although the probabil-
_2
ity of death per person due to natural causes is 10 , this value may be
largely due to people in the old age category where death is a natural end.
Death at birth when susceptibility to disease is high may also be a con-
tributing factor.
Table I
U. S. Accident Death Statistics - 1967, 1968
Accident
Motor Vehicle
Falls
Fires, burns
Drowning
Firearms
Poisoning
Cataclysm
Lightning
Natural diseases
Total
1967
53,100
19,800
7,700
6,800
2,800
2,400
155
110
Deaths
1968
55,200
19,900
7,500
7,400
2,600
2,400
129
162
Probability of
Death per Person per Year
1967 1968
-4 -4
2.7 x 10 2.8 x 10
1.0 x 10"4 1.0 x 10"4
3.9 x 10"5 3.8 x 10"5
3.4 x 10"5 3.7 x 10"5
-5 -5
1.4 x 10 1.3 x 10
-5 -5
1.2 x 10 1.2 x 10
-7 -7
8 x 10 6 x 10
-7 -7
6 x 10 8 x 10
1 x 10"2
The probability of death due to motor vehicle accidents is not the total
price that society pays for the benefit of the automobile. Motor vehicle air
pollution contributes directly to an increase in the probability of death and
this increase may be currently attributed unjustly to natural causes.
Regardless of the precise cost (risk) society pays for the benefit of
the automobile, its magnitude is at least a probability of 10" death per
person per year. Should this value of cost (risk) be adopted as a standard
-------
518
for the control of transuranium elements? Would society accept a death
-4
probability of at least 10 per person per year for the benefit of using
plutonium as a major source of energy for the generation of electricity?
According to reference (1), Otway and Erdmann (ref. (2)) point out
_ o
that when the probability of death risk approaches 10 per person per year
society takes immediate action to reduce the hazard. This level of fatality
risk is not acceptable to anyone. At a risk of 10" per person per year,
people are less inclined to concerted action but are willing to spend money
to control the hazard. At a level of 10 per person per year society is
still concerned and may accept a certain amount of inconvenience to avoid
such risks. For example, rules are adopted by community swimming pools
against anyone swimming alone and by himself. At a level of 10" per person
per year, the risk is not of great concern to the average person.
Suggested Standard for Cost (Risk)
If the assessment of Otway and Erdmann of what society accepts in terms
of risk is correct, then it is reasonable to propose a draft of a standard
on the control of transuranium elements defining the cost (risk) society is
willing to pay for the benefit it derives from the use of plutonium, such as :
1. For occupational exposure, the cost (risk) society pays for the use
of transuranium elements shall be a probability of death not to
-4
exceed 10 per person per year.
2. For the general public, the cost (risk) society pays for the use
of transuranium elements shall be a probability of death not to
-6
exceed 10 per person per year.
The occupational cost (risk) recommended here is comparable to occupa-
tional risks from other industrial activities (see reference (1), pp. 6-18).
-------
5
519
The general public cost (risk) is somewhat arbitrary and requires full public
scrutiny.
Technical Know-how Needed
Once the cost (risk) is defined, the technical know-how needed to assure
that the cost (risk) is not exceeded, must be supplied through research and
development. The goals of the research should be providing answers to the
following problems :
1. Identification in man of the critical organ which is most sensitive
to transuranium radiations (lungs, lymph nodes, bones, liver, etc.)
2. Determination as closely as possible of the relationship between
dose and the probability of death per person per year. Here the
"hot particle" theory must be scrutinized by experiments. Until
and unless experiments discount the 'hot particle" theory, it
would be foolhardy to ignore it!
3. Identification of the environmental pathways of the transuranium
elements released during normal and/or during off-normal operations
of nuclear power plants and the relationship of the release to man.
4. Realistic projection of the accumulation of the released trans-
uranium elements and an assessment of their impact on the environ-
ment as a function of time.
Agencies charged with the development of nuclear power could also be
charged with supplying the technical know-how needed to assure that the
cost (risk) of such technology does not exceed adopted standards.
\
-------
520
References
1. "The Safety of Nuclear Power Reactors (Light Water-Cooled) and Related
Facilities," U. S. Atomic Energy Report WASH-1250 (1973).
2. H. J. Otway and R. C. Erdmann, "Reactor Siting from the Risk Viewpoint,"
Nuclear Engineering and Design, 13_, 365-376 (1970).
-------
521
Karl H. Puechl
Nuclear Consultant
34 River Park Drive
Atlanta, Georgia 30328
Telephone 404/252-8821
**
December 10, 1974
Director
Criteria and Standards Division (AW-560)
Office of Radiation Programs
U. S. Environmental Protection Agency
Washington, D.C. 20460
Subject: Plutonium and the Transuranium Elements
Gentlemen:
In your review of the subject environmental standards, I
wish to alert you to the fact that for reactor use, the
Plutonium is significantly diluted with .uranium in almost
all processing operations. For example, mixed oxide fuel
for light water reactors is expected to contain less than
5% plutonium. As a consequence of this dilution and the
chemical stability of the oxide, generalized models of
long-term exposure pathways relative to pure plutonium
and/or soluble compounds can be misleading. I urge that
particular attention be paid to the specific material in-
volved and its associated chemistry and radiological be-
havior.
I suspect that technical information relative to this sub-
ject (including material compositions, particle sizes, etc.)
will be further developed during the anticipated AEC hear-
ings on the Generic Environmental Statement on Mixed Oxide
Fuel, consequently, this comment is not elaborated upon
herein.
Very truly yours,
Karl H. Puechl
-------
522
To
UNITED STATES ENVIRONMENTAL PROTECTION AGENCY
WASHINGTON, D.C. 20460
DEC 19 1974
Dr. Richard Perkins
iiattelle Northwest Laboratories
Richland, Washington 99352
Dear Dr. Perkins:
At the £I»A hearings on plutoniua on December 10 and 11 in
Washington, a graph (enclosed) attributed to you vas introduced by
Dr. wreon. The lack of unit, on the ordinate axis was questioned
by one «f tiw panel ranbers and, in my capacity as chairaan of the
technical hearing panel, I a* writing to you to attest to resolve this
difficulty. If you can supply any additional Information on this graph,
or wish to supplenont the information presented, your contribution would
be nost welcome. You aiBht wish to reply through Dr. Liveman, Director
of the Division of Biomcdical and Environmental Research, who coordinated
the AEC presentations.
Sincerely yours,
. /V-
William A. Kills, Ph.D.
Director
Criteria & Standards Division (AW-5bQ)
cc: Dr. J. L. IJ.vcrnian, AEC
Dr. ,'lcD. Z. Urann, D3E2
-------
523
€«Baiteiie
I'.n ili< Northwest I .
ilK'llr llrinlcv.iti!
i hl.mil. V\,i-.!'i»!;tini '
December 18, 1974
Dr. William Mills
Criteria and Standards Division
AW_560
Environmental Protection Agency
401 M Street, S.W.
Washington, D.C. 20460
Dear Dr. Mills:
Enclosed is a copy of a section of our Annual Report for
1972, BNWL-1751 PT2 UC-48, which includes the information
used in a viewgraph by Dr. M. E. Wrenn in the hearing last
week. It was called to my attention by both Herb Parker
and Ed Wrenn that the absolute plutonium-238 and plutonium-
239 concentrations which are included in this report, but
were not on the viewgraph, would be important for inclusion
in the proceedings of the hearing.
I am also sending a copy of this material to Dr. Edward
P. Radford who I am told showed particular interest in this
data.
Sincerely,
Richard W. Perkins, Manager
Radiological Chemistry Section
RADIOLOGICAL SCIENCES DEPARTMENT
RWP/liz
Enclosure
cc: Dr. Edward P. Radford
Dr. M. E. Wrenn
Dr. H. M. Parker
-------
524
40
BNWL-1751 PT2
C. W. Thomas
The plutonium isotopes released
by atmospheric nuclear testing are. a
combination of unreacted plutonium
in the device and isotopes of plu-
tonium formed by neutron capture in
plutonium and any 238U in the device.
The most abundant isotope of plu-
239
tonium is Pu, with lesser amounts
of 238Pu, 24%, 241Pu and 242Pu.
238
The Pu is produced by either the
reaction of fast neutrons with Pu
or by the decay of 238Np or 242Cm.
Plutonium-238 to Pu ratios vary
from detonation to detonation depend-
ing upon the burst conditions and the
material used.
In April 1964, a transit naviga-
tional satellite was launched from
Vandenberg containing a System for
Nuclear Auxiliary Power (SNAP-9A)
generator. The satellite failed to
achieve a stable orbit and subse-
quently burned upon re-entry, releas-
2*Q
ing approximately 17 kCi of Pu
(^1 kg) at 46 km over the Indian
Ocean. This Pu almost tripled
238
the global atmospheric Pu inven-
tory. Plutonium from this device was
first detected in a sample collected
by balloon at 33 km over Australia
in August 1964. Since that time, it
has been detected in stratospheric
and tropospheric air from both
hemispheres.
The atmospheric concentrations of
238 239
Pu and Pu were measured in sur-
face air samples collected at Rich-
land, Washington from 1963 to 1972
as a part of a program to define the
rates of long term stratospheric pro-
cesses in the northern hemisphere as
well as the rates of interhemispheric
mixing. The seasonal variations in
the concentrations of 238Pu and 239Pu
in surface air at Richland were simi-
lar to those of other nuclear-weapons-
produced radionuclides of strato-
spheric origin; maximum concentra-
tions occurred in the late spring and
minimums occurred in the winter. The
T 7 q
rate of decrease in the Pu con-
centration from 1963 through 1967
corresponded to a stratospheric half-
residence time of 10 to 11 months,
which is the same as the half-
residence times calculated from
measurements of other radionuclides
of stratospheric origin. The Pu
concentrations remained fairly con-
stant from 1967 to 1972, primarily
because of yearly injections of plu-
tonium by thermonuclear tests con-
ducted by the Chinese at Lop Nor
(35° N); the contribution from the
French tests in the South Pacific
(23° S) may also have been signifi-
cant. Fission product yields indi-
cate that the Chinese used 235U as
the fissile material in their high-
yield tests of 1967 through 1970.
237
However, large amounts of U,
Np, and Pu were produced, in-
238
dicating that U was used as a
component part of the devices.
From 1962 through 1965 both the
238Pu and the 239Pu in surface air
at Richland came primarily from the
1961-62 U.S.-Russian test series.
The 238Pu/239Pu ratio averaged 0.015
in 1964. The ratio increased
slightly in 1965, and by the spring
of 1966 it had increased to 0.042,
-------
525
41
BNWL-17S1 PT2
J T.Q
indicating that Pu from the SNAP-
9A buriiup was present. The amount'
T -1 O
of SNAP-9A " Pu present was calcu-
? 3 8
l;ited from the ' Pu concentrations
and the Pu/ ' Pu ratios, assuming
that the ratio in debris from nu-
clear weapons tests was 0.015. These
J -i o
calculations indicate that the " Pu
in Richland air from 1967 to 1971
came primarily from SNAP-9A. From
1967 to 1969 the concentrations of
SNAP-9A plutonium at Richland re-
mained fairly constant, indicating
238
that the Pu was being transferred
across the equator into the northern
hemisphere at a rate comparable to
238
the rate at which Pu was being
deposited on the earth's surface.
238
The Pu concentration:; showed
seasonal variations typical of radio-
nuclides of stratospheric origin, so
the transfer was probably taking
place primarily in the stratosphere.
Concentrations of SNAP-9A plutonium
at Richland have decreased rapidly
since that time. These results in-
dicate that the stratospheric debris
injected into the high stratosphere
of one hemisphere will produce high
concentrations of the debris in
ground level air in the other hemi-
sphere in the spring 1 to 2 years
later. These concentrations will
then remain constant for about three
years before beginning to decrease.
The Average Yearly Ratios of 239Pu, 138Pu, and 90Sr
in Surface Air at Richland, Washington
dpm/KSCM
1962
1963
1964
1965
1966
1967
1968
1969
1970
1971
90Sr
90.6
119
80.5
40.0
22.9
7.08
10.3
11.4
239j
1.15 ±
1.20 ±
1.02 ±
0.704 i
0.325 i
0. 125 i
0.230 i
0.310 i
0.284 i
0.275 t
>u
0.169
0.02
0.015
0.012
0. 007
0.002
0.003
0.004
0.004
0.003
—
'•• 'i ;••.
.o;»:-,4
.o:<:>.o
. (•' -;;i
.(MO;;
.0"0)
.O'iGV
.O.SV,
. .1. jl i
.
.04.'0
.0.1 (-2
239pu/!
0.0127
0.010 ±
0.0127 t
0.0176 t
0.0142 ±
0.018 i
0.022 ±
0.027 t
>°Sr
0.0043
0.012
0.0072
0.0055
0.0049
0,0068
0.0076
? ; '• i 7 a
.o:n
.019
.fil.'i i 0.00] 5
.015
.062
.374
.:>fir>
. 338
.344
.o;>9
-------
526
BNWL-17S1 1>T2
0,1
0»10MT
MO Ml
ai -1 MI
att-ai MI
V\ .A A
_i 1_
i I i OHONAflONS
U.S.
U.S.S.R.
CHINtSt
1MI
Ncg 726084-2
S*Pu (ROM SNAP-9A WRNUP ' ! I
t j I j j !
1 IW ' MM I 1M5 ' i«M ' IW ' 1MI
J L
' no '
ino ' mi i iwi ' iwj
Pu and 239Pu Concentration in Surface Air
at Richland, Washington
.' 9 n 1
a *
tions at Ri clijj-ind^ Wo_sh i nj^t on aiuj_ at
Point Bar row ? Aln_sjca
C. W. Thomas and J. A. Young
The rad ionucl ide concontrat ions in
surface air arc being measured con-
tinuously at Richland, Washington
(45° N) and at Point Barrow, Alaska
(71° N) by filtering large volumes
of air through membrane filters and
then analyzing the filters by gamma-
ray spcctrometry. A few of the radio-
nuclides must be separated chemically
-------
527
UNITED STATES
ATOMIC ENERGY COMMISSION
WASHINGTON, D.C. 20545
January 15, 1975
Dr. William A. Mills, Director
Criteria and Standards Division
(AW-560)
Environmental Protection Agency
401 M. St., S.W.
Washington, D.C. 20460
AEC SUBMISSIONS FOR THE HEARING RECORD
Dear Dr. Mills:
The following documents are transmitted hereby for inclusion in the record
of the EPA public hearing concerning plutonium standards. These materials
will supplement the AEC-Operations presentations in Washington, D.C. on
December 10-11, 1974.
(1) A figure concerning Plutonium Concentration in Surface
Air at Rich!and, Washington and a table concerning
Preliminary Estimates of Local Sources of Plutonium
in the Environment. These materials supplement the
testimony of Dr. McDonald E. Wrenn on December 10, 1974.
The hearing board at that time expressed interest in the
numerical values of the figure, which was presented as
Figure 3 of Dr. Wrenn's testimony. These values have been
added and are expressed in disintegrations per minute
per thousand standard cubic meters of air (dpm/KSCM).
This work is referenced in BNWL-1751, PT2- UC48, page 2,
1974. The enclosed figure is a copy of the referenced page.
The table is a correction of Table 4 of Dr. Wrenn's testi-
mony. The major change is the deletion of the first three
entries under Rocky Flats, which were typographical errors.
(2) A response to panel member, Dr. Me'lvin First's question
at the hearing in Washington, D.C. concerning the effec-
tiveness of cleanup activities. This document is in the
form of a memorandum from Robert E. Yoder, Assistant
Director for Facilities Safety, Division of Operational
Safety to Gregory A. Thomas, Office of the General Counsel,
both of the AEC.
(3) A response to a question of panel member Dr. Radford to
Mr. Edward Hardy, who testified on behalf of the AEC, con-
cerning tiie relationship of plutonium in soils in the
vicinity of AEC's Rocky Flats plant to existing radiation
standards. Additionally, this material presents a response
-------
528
Dr. William A. Mills
- 2 -
to Dr. Radford's comment, addressed to AEC spokesmen
Drs. W. J. Bair and C. Richmond, concerning AEC's perform-
ance in monitoring the environment.
Additional materials to supplement the record of the second hearing in
Denver, Colorado will be forthcoming under separate cover.
Sincerely,
Gregory A. Thomas, Attorney
Office of the General Counsel
Enclosures:
As stated
-------
529
UNITED STATES
ATOMIC ENERGY COMMISSION
WASHINGTON. D.C. 20545
DEC 2 3 1974
Gregory A. Thomas
Office of the General Counsel
SUPPLEMENTARY INFORMATION FOR THE RECORD OF THE EPA HEARINGS CONCERNING
PLUTONIUM ENVIRONMENTAL STANDARDS, DECEMBER 10-11, 197^
In response to Dr. Melvin First's question in which he asked for an
indication of the improvement of the effectiveness in cleanup activi-
ties as a result of experiences at Palomares and Thule, the following
information is presented.
Because the United States has not had another incident such as those
which occurred at Palomares, Spain, and Thule, Greenland, the answer
can only reflect anticipated results. The following improvements
have been incorporated into our accident response posture.
1. Instrumentation to evaluate the extent and degree of contamination
was developed following the Palomares incident and prototypes were
used at Thule. The difficulties experienced in the arctic have
led to further refinements so that now portable instrumentation is
available to monitor specifically for plutonium at the 0.1 uCi/m^
level. This instrumentation is capable of operating under any
climatic condition and in any terrain. These devices are availa-
ble in sufficient numbers and locations to allow good initial
surveys basic to establishing control lines to prevent the spread
of contamination. This equipment also is sufficiently sensitive to
permit a field analysis of bioassay specimens which can indicate a
significant internal exposure to plutonium contamination (l/2 to 1
lung burden) so that cleanup personnel or the affected population
can receive prompt medical attention.
2. Techniques to fix contamination, prior to removal, to prevent its
translocation by wind and water are under development. These
techniques have been used in a few instances in protected environ-
ments (indoors) and are being evaluated, for other environments.
3- Aerial snapping, including a capability to remotely determine radio-
activity surface contamination levels at the 0.3 iiCi/m^ level, and
downwind air sampling to allow an assessment of windborne debris
movement are now available. This capability complements the improve-
ments noted in 1., above, so that the entire accident area can be
more accurately defined.
-------
Gregory A. Thomas -2-
OtC 8 3 1974
The methods for removal or fixation (i.e., rendering gontamination
unavailable to man) of radioactivity still require excavation,
watering, and plowing. The improvements in executing these functions
are derived from our improved ability to delineate the degree of
dispersed radioactive materials and our preventive techniques to
temporarily fix, "tie down," contamination. Where previous remedial
operations have removed between 50 and 90 percent of the radioactivity,
future operations may allow removal of 70-95 percent of the dispersed
material.
^Robert E. Yode:
Assistant Director for
Facilities Safety
Division of Operational Safety
-------
531
Question by Dr. Radford to Mr. Edward Hardy, AEC-HASL, concerning the re-
lationship of plutonium in soils in the vicinity of the AEG's Rocky
Flats plant to existing radiation standards. Mr. Hardy disqualified
himself from responding to the question and it was not answered.
Answer: Extensive soil sampling conducted by the RF plant and the AEC's
Health and Safety Laboratory has permitted the definition of the distri-
bution and levels of plutonium in soils in the vicinity of the plant.
The concentrations of Pu observed in soil, which vary with location and
depth, cannot be reliability translated by a calculation into an expected
dose to man. The difficulty of translating observed soil concentrations
into expected dose is probably the major reason why no national or inter-
national concensus standards exist relative to Pu levels in soil. Accord-
ingly, the usual method of evaluating the significance of such contam-
ination is to conduct site specific air sampling programs over periods
of time sufficiently long for comparing concentrations of Pu in air with
established consensus standards for airborne activity. Concentrations
of Pu observed in air can then be compared with established concensus
standards for airborne activity. The radioactivity concentration guides
(RCG's) legally established for annual average levels of plutonium in
air by AEC are based on recommendations of the National Council on Radia-
tion Protection and Measurement and the International Commission on Radio-
logical Protection. The RCG of 3 X 10"13 nCi/ml for plutonium oxide, the
chemical form of plutonium encountered at the plant, is the standard that
would normally be used in assessing the significance of plutonium air
concentrations around the plant. However, the more restrictive RCG of
-------
532
- 2 -
2 X lO"1^ [id/ml for soluble forms of plutonium was used by the Rocky
Flats plant as the reference standard since it results -in the most con-
servative assessment of potential public exposure.
In the vicinity of the Rocky Flats plant, the public health significance
of the soil contamination (estimated to be about 14 curies of Pu distributed
in surface soils, mostly onsite) has been evaluated by operating air
sampling stations located around the plant and analyzing the samples for
radioactivity. The 1973 annual average concentration of plutonium in
air among the 12 stations located between 2 and 4 miles distant averaged
less than 0.3 percent of the reference RCG. The maximum annual average
concentration observed at a single station in 1973 was about 0.7 percent
of the reference RCG.
It should be noted that air concentrations of plutonium as indicated
from sampling in the near vicinity of the plant would reflect contribu-
tions of plutonium from worldwide fallout, plant stack emissions and
any resuspension of plutonium present in surface soils. Direct contri-
bution of plutonium in air in the RF plant area from worldwide fallout
is estimated to be 1-2 X 10'17 uCi/ml of air, about 0.1 percent of the
reference RCG.
-------
533
Comment: Dr. Radford commented to Drs. W. J. Bair and C. Richmond that
whereas the AEC's performance has been commendable in regard
to studies and research conducted towards protecting employees
at AEC facilities, the AEC's performance in monitoring the
environment has not been good. AEC was not given an opportunity
during the hearing to respond to Dr. Radford's comment.
Response: Environmental radioactivity monitoring programs have been
conducted at each AEC site since at least one year prior to
the initiation of nuclear operations at the site. Beginning
in 1959, each AEC site has been required to issue a public
report, at least annually, summarizing the results of the
site environmental monitoring program. The monitoring
programs and reports have always placed emphasis on radio-
activity levels in air, water and foods to which members of
the public might have been exposed. The data have indicated
that members of the public have not been exposed to radio-
activity in excess of a small fraction of the applicable NCRP
radiation standards. In recent years, exposures to the public
near AEC facilities have generally been well below one percent
of the applicable radiation standards. The 1973 site environ-
mental monitoring reports not only include summarizations of
monitoring results, but also the total annual curie releases
of specific radionuclides and estimates of individual and
population doses due to site operations.
-------
42
BNWL-17S1 PT2
534
1.01
,001
aoi
i
ai
an
>UMT
I-10KT
(11 - HI
aoz-ai MI
'"PU
-I 1 1 L.
W\ A A
' ^VUAAAA
OETQfiAtlGNS
CHINESE
D1Pu FROM SNAP-W !USNUP ! ! !
°'PU
Jl ^J I 1_
1M
1W
19M > !W
1M ' 1*7
Neg 726084-2
2 TO 239
Pu and Pu Concentration in Surface Air
at Richland, Washington
Atmospheric Radionuclidc Concentra-
tions at RichlanJ, V/ashington and at
Point Barrow, Alaska
C. W. Thomas and j. A. Young
The radionuclide concentrations in
surface air are being measured con-
tinuously at Richland, Washington
(45° N) and at Point Barrow, Alaska
(71° N) by filtering large volumes
of air through membrane filters and
then analyzing the filters by gamma-
ray spectrometry. A few of the radio-
nuclidcs must be separated chemically
-------
Table 4
Preliminary Estimates of Local Sources of Plutonium in the Environment (Quantities > 0.1 Ci)
Facility
NV NTS + Pacific
Thule «
Rocky Flats
Mound Laboratory
Quantity
— 1,000 Ci
— 25 Ci
0.04 Ci
0.1 Ci
4.0 Ci
10.0 Ci
0.4
0.5
5.0
0.5
Ci
Ci
Ci
Ci
Location
Pu-239 to Onsite Soil
Pu-239 in Marine Sediments and Surface Soils
Pu-239 to Atmosphere
U + Pu-239 to Offsite Streams
Pu-239 to Offsite Soil
Pu-239 to Onsite Soil
Pu-238 to Atmosphere
Pu-238 to River - Routine Releases •
Pu-238 to Canals and Ditches
Pu-238 to Soil
Savannah River
*2.9 Ci
0.6 Ci
1.5 Ci
0.1 Ci
Pu-239 to Atmosphere
Pu-239 to Atmosphere
Pu-239 to Onsite Soil
Pu-239 to Onsite Soil
LASL
1.3
0.3
Ci
Ci
Pu-239 to Atmosphere
Pu-239 to Soil
CJI
CO
01
-------
536
UNITED STATES
ATOMIC ENERGY COMMISSION
WASHINGTON, D.C. 20545
v'AN 1 0 5J75
William A. Mills, Ph.D., Director
Criteria and Standards Division (AW-560)
U. S. Environmental Protection Agency
Washington, D. C. 20460
Dear Dr. Mills:
In addition to the formal statement which the AEC presented at the
EPA Hearing on Transuranium Elements on December 10, 1974, we would
like to submit the following for the record.
The National Conference of Radiation Control Program Directors is an
organization of the Program Directors of the 50 States. This organi-
zation includes the representatives of the 25 Agreement States (those
States which have entered into agreements with the AEC pursuant to
Section 274 of the Atomic Energy Act of 1954, As Amended). These
agreements provide for the transfer of certain regulatory authority
over byproduct material, source material and small quantities of
special nuclear material to States. Both of these groups have re-
quested that we indicate their interest in the establishment of
uniform soil contamination limits for transuranium elements.
Sincerely,
G. WavmTKerr, Chief
Agreements and Exports Branch
Directorate of Licensing
-------
537
COLORADO DEPARTMENT OF HEALTH
4210 EAST 11TH AVENUE • DENVER, COLORADO 80220 • PHONE 388-6111
Edward G. Dreyfus, M.D., M.P.M..Executive Director
December 13, 1971*
William A. Mills, Ph. D., Director
Criteria and Standards Division (AW-56)
Office of Radiation Programs
U. S. Environmental Protection Agency
Washington, D.C. 20460
Dear Dr. Mi 11s:
In reference to the announcement of the public hearing on the
information required for standards development for Plutonium and the
other transuranic elements, your letter of November 26 and a phone
call from Carl Miller, (EPA), on December 12, the Department wishes
to make a presentation at the hearing continuance in Denver,
We understand that the Denver session is scheduled for January
10, 1975 beginning at 9 a.m. at the Post Office Building Auditorium.
Our presentation will last approximately 30 minutes.
Your agency's attention to our request is appreciated.
Robert D. "Siek
Assistant Director of Public Health
Environmental Programs
RDS/ljw
cc: A. J. Hazle, Occupational and Radiological Health, CDH
Paul Smith, Environmental Protection Agency, Region VIII
-------
538 NATIONAL CENTER FOR ATMOSPHERIC RESEARCH
P. 0. Box 1470 • Boulder, Colorado 80302
Telephone: (303) 494-5151 • TWX: 910-940-3245 • Telex: 45 694
16 December 1974
Dr. William Mills, Director
Criteria and Standards Division (AW-560)
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D. C. 20460
Dear Dr. Mills:
I was unable to participate at the recent EPA public hearings on
Plutonium standards in Washington, D. C., on December 10 and 11, 1974.
However I am advised by Dr. Gordon Burley of your staff that another
public hearing will take place in Denver, Colorado, on January 10, 1975.
I wish to present written and oral testimony at these Denver hearings
on the subject of plutonium standards applicable to the long term
inhalation exposure of the general public.
My oral and written testimony will include a brief critique of the
basis of current plutonium standards, followed by a discussion of the
published evidence on the nature and effects of alpha interactions with
cells and the trends in the relative distribution of such effects at
low dose rates. My presentation also will include a brief discussion
of the possible mechanisms of tumor induction for "hot" plutonium oxide
particles. It will be shown that even the incidence of tumors associated
with "hot" particles may be explained by the irradiation of large numbers
of cells which have been subjected to only a limited number of alpha
interactions. On this basis a significant tumor risk can be attributed
to very small burdens of alpha emitting particles of low activity per
particle. Similarly, unacceptable risks can be attributed to as little
as tens of picocuries of low activity particles. These conclusions
imply serious health risks for tobacco radioactivity, for fallout
plutonium and for other insoluble alpha emitter contaminants and, if
confirmed, will call for a drastic downward revision of plutonium standards
and other alpha emitter standards.
In addition I plan to discuss plutonium standards applicable to
surface soils and urban dusts, including discussion of a new approach
to the prediction of organ burdens that will result from long-term
inhalation exposure to such sources. Based on these and the above
considerations I shall propose interim standards applicable for public
exposure to insoluble alpha emitting particles in surface soils and urban
dusts.
The National Center for Atmospheric Research is Operated by the University Corporation
for Atmospheric Research under sponsorship of the National Science Foundation.
-------
539
Dr. William Mills, Director
16 December 1974
Page 2
For my oral presentation I would appreciate it if you could allocate
at least 30 minutes, and preferably 45 minutes. Thank you.
Sincerely yours,
Edward A. Kartell
-------
540
UNIVERSITY OF MINNESOTA ; school of Public Affairs
TWIN CITIES Social Sciences Building
Minneapolis, Minnesota 55455
18 December 1974
Dr. William Mills
Director, Criteria and Standards
Division
Office of Radiation Protection
Environmental Protection Agency
Washington, D.C. 20460
RE: Public Hearing/Plutonium Contamination Limits
Dear Dr. Mills:
I ask that I be given the opportunity to testify at your Public
Hearing on Plutonium Contamination Limits (scheduled for Denver,
Colorado on January 10, 1974). My testimony would be approximately
30 to 40 minutes in duration. If it would not inconvenience you,
it might be advisable for my testimony to be scheduled no earlier
than 10 A.M., since I may have to take an early morning flight,
Minneapolis to Denver, on the 14th.
Thank you.
Youlvs truly,
Donald P. Geesaman
Associate Professor
DPG/lam
-------
UNIVERSITY OF COLORADO
MEDICAL CENTER
4200 EAST NINTH AVENUE
DENVER, COLORADO 80220
541
SCHOOL OF MEDICINE
DEPARTMENT OF PREVENTIVE MEDICINE
AND COMPREHENSIVE HEALTH CARE
DIVISION OF HEALTH ADMINISTRATION
JOHN EDWARD KRAIEWSKI. Ph.D.
DIRECTOR
December 20, 1974
Director, Criteria and Standards
Division (AW-560)
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D.C. 20460
Dear Sir:
I request about 15 minutes for a statement at the plutonium standards hearings
in Denver on January 10th, 1975. The information requested follows:
Name: John C. Cobb, M.D., M.P.H.
Professor of Preventive Medicine
University of Colorado Medical School
Denver, Colorado 80220
Affiliations: Member, Governor's Scientific Advisory Council
Member, Governor-elect's Task Force on Rocky Flats
Member, Denver Medical Society, Public Health
Commission
Chairman, Rocky Flats Action Committee of the
American Friends Service Comm.
Topic> "Value Decision in the Face of Scientific Uncertainty."
Summary, I would briefly summarize critical evaluations by various members
of the Medical School faculty of the report by Arthur R. Tamplin
and Thomas B. Cochran, entitled, "Radiation Standards for Hot
Particles" dated February 14, 1974, which was prepared for the
Natural Resources Defense Council in support of their petition to
the EPA and AEC. (I presume it is not necessary for me to sum-
marize the.content of that report, but would be glad to do so if
you desire, and want to give me more time to do it.)
I would then point out the implications of this report and other
related research findings to the control of hot insoluble plutonium
particles emanating from The Rocky Flats Plutonium Project.
-------
54-2
Director, Criteria and Standards
Division (AW_560)
Continued, Page 2
December 20, 1974
Finally, I would review the possible dangers to populations
living now and in the future in the area surrounding the
Rocky Flats Project, and make a recommendation of how the
scientific data, with its recognized degree of uncertainty,
should be utilized in making a decision regarding standards
for plutonium in the environment.
I would appreciate hearing from you regarding how much, if any, of the above
you would like me to present orally; and in particular whether you want me
to summarize the content of the report by Tamplin and Cochran, which I pre-
sume you already have in your files. I will, in any case, prepare a written
statement for the record.
Yours sincerely,
,• *<.. (. C- ti
John C. Cobb, M.D., M.P.H.
Professor
JCC/ma
cc: Paul Smith
-------
543
AMERICAN FRIENDS SERVICE COMMITTEE
Staff:
KAY JOHNSON. Ailmtnlamivr Secretary
JUDY DANIELSON. Feme Ktlmalimi
PAM SOLO. Peace Education
BEN REYES. Justice Program
Cultiratlo Area
Executive Committee:
ROBERT HUBBARD. Chairman
MIDORI ABE
DOROTHY ALDRICH
MURIEL ASHMORE
LEE SANNE BUCHANAN
GINNY COWLES
JIM GRAHAM
LEE HAMBY
JACK JOURGENSEN
CURTIS KING
JERRY KRENZ
HELEN LUCERO
MARIAGNES MEDRUD
KAREN MOORE
LARRY NAVES
ROSINA OLSON
ROY SMITH
TONY UMILE
MARC1A WARNER
PAULWEHR
GLENN WILLIAMS
COLORADO AREA OFFICE
2801 E. COLFAX AVE., #304
DENVER, COLORADO 80206
(303) 388-5896
December 22, 1974
Director, Criteria and Standards Division
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D.C. 20460
Dear Sir:
I am writing to request time to give testimony at the Plutonium
Standards Hearings to be held in Denver on January 10, 1975.
The testimony of the American Friends Service Committee will
require five to eight minutes only. Our testimony will be
concerned with the social and moral impact of plutonium.
We look forward to your response in this matter. Thank you.
Sincerely,
Pam Solo
C»-Director
Peace Education
-------
544
AMERICAN FRIENDS SERVICE COMMITTEE
KAY JOHNSON. Adminiurativ
JUDYDANIELSON. Peat? F-ih
PAM SOI.O. Feme Kduialior,
BEN REYES. Justice Program
Colorado Area
£.vc
-------
-2- 545
of human understanding, indicating an unfortunate limited point of
view. They evidently were most reluctant to hear discussion of
risk-cost-benefit value judgments which necessarily involve husan~
istic or moral considerations. An example is the question of whether,
for the benefit of a few people who are living today, we should run
even a slight risk of endangering the health and life of every liv-
ing thing for thousands of generations. They branded the considera-
tion of such questions as "emotionalism" and proceeded immediately
to readjust their blinders in order to focus only on the technical
questions. This, in spite of the specific request by Dr. W. D. Rowe,
in his opening remarks on behalf of EPA, requesting comment on this
type of value judgment. Since the hearings were to be "evidentiary"
in nature, persons giving testimony before the panel hardly expected
to be cross examined by panelists — and for them to be so treated
was unfortunate and unfair.
Perhaps the panelists guilty of such conduct forget that in the his-
tory of mankind, attempts to resolve moral problems of humanity
simply by technological means have generally resulted in the crea-
tion of worse moral problems. The testimony given before the panel
rightly addressed itself not only to protection of the immediate
environment of the Denver metropolitan area, but to the global en-
vironment as well. The risks of local radiation pollution inter-
sect with those represented by the nuclear weapons produced at Rocky
Flats.
All nations will have to realize soon that this multi-national atomic
arms race provides more danger to humans and their environment than
security. The Pentagon has a name for it, "Mutual Assured Destruc-
tion," which goes by the appropriate acronym "MAD."
Sincerely,
Paul Wehr
Co-chairman, Peace Education
Committee
PW:kj
-------
546
BOULDER
OFFICE OF THE CITY MANAGER
December 24, 1974
Dr. William A. Mills
Director for Criteria and Standards Division
AW 560
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D.C. 20460
Dear DrvrMills:
The City of Boulder would appreciate an opportunity to make a ten-minute
presentation at the public hearing regarding the environmental impact of
Plutonium and transuranium elements, being held in Denver on January 10, 1975.
Our presentation will present some of the concerns relevant to the City of
Boulder, particularly those resulting from a brief staff study of the potential
impact of the Atomic Energy Commission's Rocky Flats Plant.
Our City Council has not yet had the opportunity to establish its position
regarding the potential impact of plutonium but plans to address the questions
involved prior to the public hearing. Until that time, it will not be possible
to provide a complete outline of our concerns or an official statement of
our position. However, if any additional information is needed prior to
the public hearing I would be pleased to supply it.
Thank you for your consideration and for the opportunity to participate
in the public hearing.
cc: John Green
Regional Administrator
U.S.E.P.A.
Ruth Correll
Boulder City Council member
LFD:jw
POST OFFICE BOX 791
BOULDER, COLORADO 80302
TELEPHONE (303) 442-2020
-------
JOHN C. SELNER, M.D.
ALLERGY AND PEDIATRIC ALLERGY
saao e. EVANS — TEL. 756-3614
DENVER, COLORADO 8O222
7
ZO2O WADSWORTH — 234-1Q67
LAKEWaOO, COLORADO 8D215
December 30, 1974
Director, Criterion and Standards Division
(AW—560) Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, B.C. 20460
Dear Sir:
This note is to notify you of our desire to offer a statement at the hearings
to be held at the Post Office building on Stout Street in Denver January 10
regarding plutonium standards. I would identify myself as John C. Seiner, M.D.,
5800 East Evans representing the Colorado Medical Society. Our testimony
should take not more than ten minutes and be offered here in Denver. The topic
of the presentation is regarding plutonium standards and their specific appli-
cation to the Rocky Flats plant.
The Colorado Medical Society appreciates your allowing us this time. I am
uncertain as to how I will know that this time is being made available to us, as
I am not sure of your confirmation procedures. Perhaps we could attain this
by inquiring with the local EPA office. Thank you very much for your attention
to this matter.
/ J6HN C. SELNER, M.D.
JCS:ks
-------
548
6th
DES M01NES.IA. 50309
PH. (515)282-8191
December 31, 1971*
Dr. William Mills
Director of Criteria and Standards Division (AW 5fO)
Office of Radiation Program
_..*ironmental Protection Agency (EPA)
Washington, B.C. 20460
aar sirs:
Citizens United for Responsible Energy most strenuously objects to
the proposed policy of plutonium recycle. Our objections are well based
because of the present Insecure method of handling plutonium and uranium.
The recent New York Times story indicating that plutonium is missing
from i.5 commercial reactors only points up the validity of our contentions,
We must be a mad society to even contemplate adding to the plutonium risk
when we obviously have not assured control of it now.
The use of plutonium recycle in the present reactors will only esca-
late the risks of nuclear power, risks that we feel are unbearable even
now. The plutonium risk Is not necessary and puts a grave cloud over
the future of man's activity and genetic base. No way exists to allow
this technology to proliferate without Jeopardizing man's freedom,
and literally putting us under military control.
Instead we feel our energy should be moving toward decentralized,
less complex sources that do not require the extensive, expensive backup
and safeguard systems that essentially make us captives of our own
technology.
Enclosed is the essence of our thinking as expressed by three
experts, J. Oustave Speth, Arthur Tamplin and Thomas Cochran, in their
article, "Plutonium Recycle: The Fateful Step", printed In the
Bulletin of the Atomic Scientists November, 197*K We ask that the
entire article be entered as part of the record.
opjec to: Iowa Congressmen
Iowa Dept. Environ. Quality
2$ Iowa citizen groups
Sincerely,
ne Magers, chairperson, CURE
-------
bulletin
OF THE ATOMIC SCIENTISTS
549
(Reprinted by permission of the" Bulletin of the Atomic Scientists
and the authors. Copyright (c) by the Educational Foundation for
Nuclear Science.)"
Plutonium Recycle:
The Fateful,Step
• i
Impending move to reprocess fuel would escalate the risks of nuclear power '
I fear that when the history of this century is
written, that the greatest debacle of our nation
will be seen not to be our tragic involvement in
Southeast Asia but our creation of vast armadas
of plutonium, whose safe containment will rep-
resent a major precondition for human survival,
not for a few decades or hundreds of years, but
for thousands of years more than human civili-
zation has so far existed.
James D. Watson
Nobel Laureate, Medicine
J. GUSTAVE SPETH, ARTHUR R. TAMPLIN
and THOMAS B. COCHRAN
The Atomic Energy Commission, if unchecked, is
.about to sow the seeds of a national crisis. The Com-
mission now proposes to authorize the nuclear power
industry to proceed to use plutonium as fuel in com-
mercial nuclear reactors around the country. The re-
sult of a decision approving this commercial use of
plutonium will be the creation of a large civilian plu-
tonium industry and a dramatic escalation in the
risks posed by nuclear power.
This decision to launch what the AEC calls the
plutonium economy is the conclusion of the AEC's
recently released draft environmental impact state-
ment for plutonium recycle: the recycling of plutoni-
um as fuel in the present generation of light water
reactors [1,2]. The final version of the impact state-
ment, which is expected to confirm the decision to
authorize plutonium recycle, is due in a few months.
Plutonium is virtually unknown in nature; the en-
tire present-day inventory is man-made, produced in
nuclear reactors. Plutonium-239, the principal iso-
tope of this element, has a half-life of 24,000 years,
J. Gustaue Speth ('attorney), Arthur R. Tamplin
fbiophysicist) and Thomas B. Cochran (nuclear
physicist) are on the staff of the Natural Resources
Defense Council in Washington, D. C. Dr. Tamplin
is on leave of absence from the Lawrence Liuermore
Laboratory of the University of California.
hence its radioactivity is undiminished within human
time scales. It is perhaps the most toxic substance
known. One millionth of a gram has been shown ca-
pable of producing cancer in animals [3]. Plutonium
is also the mate'rial from which nuclear weapons are
made. An amount the size of a softball is enough
for a nuclear explosive capable of mass destruction.
Scientists now widely recognize that the design and
manufacture of a crude nuclear explosive is no longer
a difficult task technically, the only real obstacle
being the availability of the plutonium itself [4].
We believe that the commercialization of plutoni-
um will place an intolerable strain on our society
and its institutions.1 Our unrelenting nuclear tech-
nology has presented us with a possible new fuel
which we are asked to accept because of its potential
commercial value. But our technology has again out-
stripped our institutions, which are not prepared or
suited to deal with plutonium. Those who have asked
what changes in our institutions will be necessary to
accommodate plutonium have come away from* that
enquiry profoundly concerned. And the AEC's en-
vironmental impact statement does not allay these
concerns. It reinforces them.
The AEC concedes that the problems of plutonium
toxicity and nuclear theft are far from solved and in-
dicates that they may not be for some years. Yet it
concludes, inexplicably, that we should proceed.
Whether stemming from blind faith in the technol-
ogy it has fostered or from callous promotion of the
bureaucratic and industrial interests of the nuclear
power complex, the AEC's proposal cannot be justi-
fied in light of what we know and, just as important,
what we do not know.
The fuel now used in present-day reactors, the
light water reactors, is uranium which has been en-
riched; the uranium-235 content is increased from
0.7 percent present in natural uranium to, about 3
or 4 percent. Uranium-235 is a fissionable isotope of
uranium, the remainder being non-fissile uranium-
238. Unlike plutonium, uranium fuel is not extreme-
ly toxic, and it is not sufficiently rich in uranium-235
to be fashioned into nuclear weapons. The uranium
NOVEMBER 1974 VOLUME XXX
-------
550
The current AEC radiation protection standards governing the amount of plutonium to
which members of the public can be exposed are roughly 100,000 times too lax.
can be enriched to weapons grade material only with
extremely sophisticated technology which is not
available to the public, notably gaseous diffusion
plants.
While present-day reactors are operating, how-
ever, they are also producing as a by-product mod-
erate amounts of plutonium, principally plutonium-
239. A typical large reactor produces about 200 to
250 kilograms of plutonium each year. Since this
plutonium is easily fissioned, it can be used as reac-
tor fuel. Plutonium recycle is the nuclear industry-
AEC proposal to recover the plutonium produced in
light water reactors, process it and recycle it as fuel
back into these reactors.
Several critical steps are involved in recycling this
plutonium. First, the used or spent fuel from the re-
actor must be shipped to a fuel reprocessing plant
where the plutonium is recovered from the spent fuel,
converted to oxide form and shipped to the next fuel
cycle stages—the fuel fabricating and assembly
plants. At a fuel fabricating plant the plutonium ox-
ide will be mixed with uranium oxide into mixed
oxide fuel. This mixed oxide fuel will be fabricated
into fuel pellets, the pellets will be placed in fuel rods,
and these rods will be collected into fuel assemblies.
These assemblies will then be sent to the reactors for
use, thus completing the fuel cycle.
At this point plutonium recycle has not yet begun,
and there is no major industrial commitment of re-
sources to it [5]. No major commercial plutonium
fuel fabricating plants^are operating or under con-
struction.* No commercial reprocessing plants are
operating now.** Reprocessing plants, in addition to
recovering plutonium and other fission products from
the spent fuel, are supposed to solidify high-level
wastes and ship them to a permanent AEC reposi-
tory for perpetual management. As yet, however, the
AEC has no such repository. Nor does the AEC know
whether the technology and social institutions for
isolating these high-level wastes for geologic periods
can be made available.
If the plans of the AEC and the nuclear industry
are permitted, however, a major plutonium industry
will develop quickly. Some 1-10 Ions of plutonium
could be recovered from commercial reactors by 1985
*There are, however, several small commercial facilities
that process plutonium for research and development pur-
poses.
*'The first commercial reprocessing plnnt built in the
United States, Nuclear Furl Services in West Valley, New
York, was shut down in 1972 for repairs and enlargement.
The Midwest Fuel Recovery Plant under construction near
Morris, Illinois, has been declared an almost total loss due to
faulty design and construction [6]. The Darnwell Nuclear
Fuel Plant in South Carolina is 70 |>ercent complete. Thus,
since mid-1972, all spent fuel from light water reactors has
been simply stored and not reprocessed.
16
and some 1,700 tons by the year 2000 [7]. A pluto-
nium industry by the turn of the century could in-
volve hundreds of light water reactors fueled with
plutonium, perhaps a score of fuel reprocessing and
fabricating plants, and thousands of interstate arid
international shipments containing hundreds of tons
of plutonium.
Plutonium Toxicity
The most pernicious product of the nuclear indus-
try is plutonium. Microgram quantities in skin
wounds cause cancer, and in the body plutonium is
a bone seeker where, once deposited, it can cause
bone cancer. But plutonium is most dangerous when
inhaled. Donald Geesaman explains this hazard:
Under a number of probable conditions plutonium
forms aerosols of micron-sized particulates. When lost
into uncontrolled air these particulates can remain sus-
pended for a significant time, and if inhaled they are
preferentially deposited in the deep lung tissue, where
their long residence time and high alpha activity can
result in a locally intense tissue exposure. The lung
cancer risk associated with these radiologically unique
aerosols is unknown to orders of magnitude. Present
plutonium standards are certainly irrelevant and prob-
ably not conservative. Even so, the fact that under
present standards, the permissible air concentrations
are about one part per million billion is a commentary
on plutonium's potential as a pollutant [3].
To determine whether the AEC's radiation pro-
tection standards for plutonium are inadequate, as
Geesaman suggests, two of the authors of this article
undertook a review of the biological evidence for the
Natural Resources Defense Council (NRDC). Their
report, Radiation Standards for Hot Particles [9],
concludes that plutonium particulates or hot par-
ticles are uniquely virulent carcinogens and that'the
current AEC radiation protection standards govern-
ing the amount of plutonium to which members of
the public can be exposed are roughly 100,000 times
too lax. '
The lung cancer risk associated with hot particles
of plutonium, as estimated by Tamplin and Cochran,
is comparable to the lethal dose of botulin toxin, a
biological warfare agent. Certainly one would hope
that this nation would give careful consideration and
pursue all alternatives before implementing an ener-
gy policy based on such toxic materials.
As a result of this study, NRDC formally petitioned
the AEC and the Environmental Protection Agency
to reduce the present maximum permissible exposure
. levels by 100,000. Neither the AEC nor the EPA have
responded finally to NRDC'S petition, but the petition
is now being considered by National Council on
Radiation Protection and Measurements, National
Academy of Sciences, Biophysical Society and sev-
eral AEC national laboratories. Moreover, EPA will
-------
shortly commence a series of hearings and other in-i.
itiatives on plutonium-related issues, including the
hot particle controversy.
Although the adequacy of the AEC's plutonium
standards is thus a matter of considerable doubt and
great controversy, the AEC's draftcnvironmental im*,.
pact statement for plutonium recycle simply assumes
that the present standards are adequate. The entire
risk analysis of the statement, as well as the ultimate
decision to proceed with plutonium recycle, are based
upon a premature and unexplained rejection of the
hot particle hypothesis. Yet, the AEG is forced to
concede that this hypothesis "is being given careful
consideration in a separate proceeding" [2, chap 4,
pp. 5-7].
We submit that the AEC has no basis whatever to
conclude that plutonium recycle will not cause undue
risk to the public health and safety until it has either
satisfactorily resolved the hot particle issue or calcu-
lated the impacts of plutonium recycle using the as-
sumption that hot particles are uniquely carcino-
genic. The AEC's draft environmental impact state-
ment for plutonium recycle does neither. However,
the more basic issue is whether we want our energy
system based on a material of unprecedented
toxicity.
Some plutonium contamination of the environ-
ment has already occurred, due principally to the
atomic weapons program. The leakage of plutonium
from contaminated oil at the AEC's plutonium wea-
pons plant at Rocky Flats, 10 miles west of Denver,
Colorado, led to an uncontrolled source of plutonium
which was much larger than the integrated effluent
loss during the 17 years of plant operation. Tens to
hundreds of grams of plutonium went off-site* 10
miles upwind from Denver [3, p. 59],
The Nuclear Materials and Equipment Corpora-
tion (NUMEC) of Apollo, Pennsylvania, was recently
fined $13,720 for a 16 count violation of AEC regu-
lations ranging from failure to follow radiation moni-
toring procedures to failure to comply with certain
safeguards requirements [9]. Production workers
at Nuclear Fuel Services, Inc. in Erwin, Tenn., a fuel
processing and fabricating facility, met with AEC
inspectors on August 13, 1974 to complain about
the absence of even the rudiments of accepted health
physics practices at that plant. Occurrences such as
these can reasonably be expected to multiply greatly
if plutonium is made a major article of commerce.
Nurlcar Theft
On May 18 of this ycnr the world was made dra-
matically aware of the relationship between nuclear
'power and nuclear weapons when India exploded a
nuclear device made from plutom'um taken from a
peaceful reactor built with Canadian assistance. The
magnitude of the threat posed by the availability Q CJ "1
plutonium from power reactors is set out by Willricn
and Taylor in their book Nuclear Theft: Risks and
Safeguards:
As fuel for power reactors, nuclear weapon material
will range in commercial value from $3,000 to $15,000
per kilogram—roughly comparable to the value of black
market heroin. Tho same material might be. hundreds
of times more valuable to some group wanting a power-
ful means of destruction. Furthermore, the costs to so-
ciety per kilogram of nuclear material used for destruc-
tive purposes would be immense. The dispersal of very ,
small amounts of finely divided plutonium could neces-
sitate evacuation and decontamination operations cov-
ering several square kilometers for long periods of time
and costing tens or hundreds of millions pf dollars. The
damage could run to many millions of dollars per gram
of plutonium used. A nuclear explosion with a yield of
one kilotnn could destroy a major industrial installation
or several large office buildings costing hundreds of mil-
lions to billions of dollars. The hundreds or thousands of
people whose health might be severely damaged by dis-
persal of plutonium, or the tens of thousands of people
who might be killed by a, low-yield nuclear explosion in
a densely populated area represent incalculable but im-
mense costs to society [4, pp. 107-108].
In our troubled world, terrorist activity and other
forms of anti-social violence are an almost daily oc-
currence. A recent AEC study identified more than
400 incidents of international terrorism carried out
by small groups during the past six years [10]. In an
age of bombs and bomb threats, of aircraft hijacking,
of the ransom of diplomats and the murder of Olym-
pic athletes, the risks of nuclear theft, blackmail and
terrorism are not minimized even by some of the
most ardent supporters of nuclear energy. Thus
former Atomic Energy Commissioner Clarence Lar-
son has described the evplution of a plutonium black
market:
Once special nuclear material is successfully stolen in
small and possibly economically acceptable quantities,
a supply-stimulated market for such illicit material is
bound to develop. And such a market can surely be ex-
pected to grow once the source of supply has been iden-
tified. As the market grows, the number and size of
thefts can be expected to grow with it, and I fear such)
growth would be extremely rapid once it begins... .Such
theft would quickly lead to serious economic burdens to
the industry, and a threat to the national security [11].
The critical point here is that these tremendous
risks will become real with the ucivent of plutonium
recycle. Unless plutonium is reprocessed and recy-
cled, the possibility that it will be stolen is small. If
the plutonium has not been detoxified by separating
it from the high-level wastes in the spent fuel nt n re-
processing plant, it is very effectively protected from
theft, nt least for hundreds of years. Willrich and
Taylor explain these relationships:
In the light .water reactor (LWR) fuel cycle without
plutonium recycle, plutonium which is produced in a
power reactor, if reprocessed, might be stolen at the
Is the American public willing to accept the risks of plutonium in exchange for the
promised benefits?
November 1974 Bulletin of the Atomic Scientists 17
-------
552
output crnLof a reprocessing plant, during transit from
the reprocessing plant to any separate storage facility
ised, and from a long-term plutonitim storage facility.
(Inlil irrnrlinlcrl furl ii rcprw.rssc.rl, Ihc Ihrft /rnxsibil^
ilii'x in the LWIt fuel cycle arc. minimal. (Emphasis''
added.)
In the LWR fuel cycle with plulonium recycle, in
addition to possibilities without recycle, plutonium
might he stolen during transit, from any separate long-
term storage facility, and from a fuel fabrication plant.
Complete LWR fuel assemblies, each containing a sig-
nificant quantity of plutonium might also he stolen
during transit from a fuel fabrication plant to a power
reactor, and at a power plant prior to loading into the
reactor, although the weight of each assembly makes
this difficult [4, p. 168].
In sum, plulonium recycle will bring with it all the
risks associated with nuclear theft that numerous
authors have described [12]. Reasonable prudence
dictates, therefore, that we have adequate answers
to the problem of nuclear, theft well in hand before
we begin plutonium recycle.
Safeguards and the AEC
In the language of the nuclear industry, the vari-
ous programs and techniques to prevent nuclear theft
and recover stolen nuclear material are called 'safe-
guards.' There is now widespread agreement—at
least among those outside the nuclear industry—that
present safeguards against nuclear theft are woefully
inadequate [13]. The AEC's Rosenbaum Report
concluded:
In recent years the factors which make safeguards a
real, imminent and vital issue have changed rapidly for
the worse. Terrorists groups have increased their pro-
fessional skills, intelligence networks, finances and level
of armaments throughout the world. . . .Not only do
illicit nuclear weapons present a greater potential pub-
lic ha/ard than the radiological dangers associated with
power plant accidents, but. . .the relevant regulations
are much less stringent [13].
The problem is not simply that the AEC has not im-
plemented the necessary safeguards programs; rather
the agency has not even developed an adequate pro-
gram on paper.
On the subject of safeguards, the AEC's draft im-
pact statement on plutonium recycle is a marvel of
clouded reasoning and breezy optimism. The state-
ment concedes that the objective of keeping the risk
of nuclear theft small "will not be fully met for the
recycle of plutonium by current safeguards meas-
ures" [2, pp. 5-6]. Steps which might be taken to
correct current inadequacies are then summarized
in the statement as follows:
1. Minimization or elimination of the transportation
of plutonium from reprocessing plants to mixed oxide
fuel fabrication facilities which is the operation most
vulnerable to an attempted act of theft or sabotage. To
the extent that such shipments are minimized or elim-
inated, the safeguarding of plutonium would be en-
hanced. This objective can be accomplished by locating
mixed oxide fuel fabrication plants in close proximity
to or adjacent to reprocessing plants in Integrated Fuel
Cycle Facilities. .. .
2. Further protection of transportation functions by
use of massive shipping containers, special escort or
•onvoying measures, vehicle hardening against attack,
improved communications and response capabilities.
3. Additional hardening of facilities through new bar-
rier requirements, new surveillance instrumentation,
new delaying capabilities (e.g., incapacitating gases).
4. Upgrading of operating and guard functions
through the use of ]>ersonnel security clearance pro-
cedures, a federally operated nuclear security system,
more advanced systems for monitoring and searching
of personnel, and closer liaison with law enforcement
authorities.
5. Improving the timeliness and sensitivity of the sys-'
tern of internal control and accountability of plutonium.
6. Use of 'spiked' plutonium which would be less sus-
ceptible to theft and would be more difficult to manu-
facture into a nuclear explosive because of the required
elaborate handling procedures [2, pp. 5-7],
Despite the facts that: (1) these proposals are pre-
liminary and their content not well defined, (2) they
are still being studied, some apparently for the first
time, (3) some would require Congressional action,
(4) some would necessitate substantial changes in
the structure of the U.S. utility industry, and (5) a
sophisticated safeguards program would pose a major
threat to civil liberties and personal privacy—despite
all these facts the draft impact statement neverthe-
less recommends that we proceed now with plutoni-
um recycle because "the Commission has a high de-
gree of confidence that through implementation of
some combination of the above concepts the safe-
guards general objective set forth earlier can be met
for plutonium recycle" [2, pp. 5-7]. The Commis-
sion's faith, unfortunately, is hardly reassuring.
The AEC's lead safeguards suggestion—the Inte-
grated Fuel Cycle Facility concept—merits special
comment. It actually represents a major watering
down of a far more significant concept, that of nu-
clear power parks where reactors as well as fuel re-
processing and fabricating plants are all located at
one site [14]. In our judgment, a safeguards system
which does not require nuclear parks is not address-
ing the problem of theft during transportation in a
.serious and responsible way. Moreover, the nutflear
industry's current plans, already well advanced, do
not call for the implementation of even the Integrat-
ed Fuel Cycle Facilities concept.
Adequate Safeguards? .. t,
While it may ibe possible to devise an adequate
safeguard system in theory, there is little reason to
believe that such a system would be acceptable in
practice [15]. This is true for several reasons.
First, the problem is immense. The illegal diver-
sion of weapons material is only one type of anti-
social behavior a safeguards program must protect
against. Terrorist acts against the reactors, ship-
ments of radioactive wastes, fuel reprocessing facili-
ties and waste repositories can result in catastrophic
releases of radioactivity. Such threats against nu-
clear facilities have already occurred [16]. More-
over, a safeguards system would have to exist on a
vast, worldwide basis. Some 1,000 nuclear reactors
are projected for the United States in the year 2000,
with hundreds of shipments of radioactive materials
daily. Hundreds of tons of plutonium will be in the
commercial sector of our economy by that date.
-------
553
To accommodate plutonium we shall have to move toward a more intimidated society
with greatly reduced freedoms.
Abroad, American firms are constructing nuclear re-
actors in countries that have little political stability
and in countries, such as Japan, who have not sighed
the Non-Proliferation Treaty. Safeguarding nuclear
bomb material would ultimately require a restruc-
turing of the socio-political institutions on a world-
wide scale. The United Nations unfortunately gives
us little( reason to believe that this is a practical re-
ality.
Second, safeguards measures are strongly opposed
by the nuclear industry. The degree to which the in-
dustry is sensitive to the diversion hazards and is
likely to be an effective partner in the enforcement
and implementation of safeguards programs was ap-
parent in the vociferous industry opposition to the
modest strengthening of the AEG safeguards rules
which were first published in the February 1, 1973,
Federal Register [17].
Third, experience with present safeguards is hard-
ly reassuring. Nuclear Materials and Equipment
Corporation, over several years of operation, was un-
able to account for six percent (100 kilograms) of
the weapons grade material that it handled. As noted
previously, it was also fined by the AEG, in part,
because of safeguards violations. At a safeguards
symposium the director of the AEC's Office of Safe-
guards and Materials Management observed 'that
"we have a long way to go to get into that happy land
where one can measure scrap effluents, products, in-
puts and discards to a o'ne percent accuracy" [3, p.
59]. This statement takes on particular significance
when it is realized that only one-half of one percent
of the plutonium utilized by the commercial sector in
the year 2000 is enough to make hundreds of atomic
bombs. The editors of the Bulletin have noted that
the frequent 'misroutings' of shipments of weapons
grade materials highlights a key safeguards problem
—hijacking [18].
A spot-check by General Accounting Office inves-
tigators at three AEC-licensed contractors showed
that in some cnses access to easily portable quanti-
ties of special nuclear material could be gained in less
than a minute using the simplest of tools. At two of
the three plants checked, GAO found weak physical
barriers, ineffective guard patrols, ineffective alarm
'Systems, lack of automatic-detection devices, and the
absence of an action plan should material be stolen
or diverted. AEC's inspectors, however, were giving
the same facilities good marks on virtually every se-
curity category [GAO, 13].
Fourth, and perhaps most basically, there is little
reason to believe that safeguards will work when little
else does. For example, the AEG supports the crea-
tion of a federal police force to provide an immediate
federal presence whenever the use of force may be
needed to protect these incredibly dangerous mate-
rials from falling into the hands of would-be sabo-
teurs and blackmailers. But is there anyone who be;-
lieves that police are effective at a level commen-
surate with the potential nuclear hazard? The New
York City police department was proven incapable
of maintaining security over confiscated heroin. Are
similar losses of plutonium acceptable?
The general point here is that our safeguards sys-
tem must be essentially infallible. It must maintain
what Alvin Weinberg, former director of the Oak
Ridge National Laboratory, has called "unaccus-
tomed vigilance" and "a continuing tradition of
meticulous attention to detail" [19]. Yet our human
institutions are far from infallible. Our experience
indicates that rather than sustaining a high degree
of esprit, vigilance and meticulous attention to de-
tail, our governmental bureaucracies instead become
careless, rigid, defensive and, less frequently, cor-
rupt. A basic question, then, is whether we want to
entrust so demanding and unrelenting a technology
as plutonium recycle to institutions wliich are negli-
gent of their own responsibilities and insensitive to
the rights of others and to technical fixes which are
untried and unproven.
Threat to Civil Liberties
One principal reason for our believing that an ade-
quate safeguards system would not be acceptable in
practice is the tremendous social cost of such a sys-
tem in terms of human freedom and privacy. Safe-
guards necessarily involve a large expansion of police
powers. Some one million persons have been trained
in the handling, moving and operation of nuclear
weapons. The projected growth of the nuclear indus-
try will give rise to a parallel and, ultimately, a much
larger group of persons, in this case civilians, who will
be subjected to security clearance,and other security
procedures now commonplace iri' the military wea-
pons program. Indeed, the AEC makes the following
disturbing statement in its draft environmental im-
pact assessment of plutonium recycle:
Security problems arc much simplified when it can he
established with high probability that the persons who
are responsible for the handling of plutonium or imple-
menting of related safeguards programs are trust-
worthy. Various court rulings in recent years have been
favorable to the protection of individual privacy and of
individual right-to-work. These rulings have made it
difficult to make a personnel background check of an
individual in commercial activities to assure with high
probability that he is trustworthy and, hence, poten-
tially acceptable as a steward for the protection of plu-
tonium. The AEC has requested legislation which would
allow background checks of individuals with access to
plutonium and related material accountability records
[2, chap. 5, p. 42].
November 1974 Bulletin of the Atomic Scientists 19
-------
554
The keeping of police dossiers will not be limited
to nuclear industry personnel. The New York Times
reported August 11 that Texas state police maintain
files on nuclear power plant opponents. How much
more government investigation into the private lives
of individuals can be tolerated by a free society? Se-
curity and surveillance procedures at best infringe
upon the privacy of families and their friends. At
worst, they are the instruments of repression and
reprisal.
A second AEC safeguards proposal is the creation
of a federal police force for the protection of plutoni-
um plants and shipments. The draft impact state-
ment for plutonium recycle justifies such a federal
force in the following terms:
A federal security system would he less apt to hove the
variations in staff and capability that would he en-
countered in use of private security guards. In addition,
it should be noted that the consequences of a successful
theft or diversion of plutonium would undoubtedly
have nationwide impacts and could hest he handled by
Federal authorities; certainly, with Federal participa-
tion, there is the potential for a larger force, more ef-
fective weapons, and better communications [2 chap 5
P. 42].
How large would such a force be? What standards
should govern and restrain its operations? The Wash-
ington Post reported in October 1973 that the AEC
issued shoot-to-kill orders to personnel directing the
production, shipment and storage of atomic weapons
at the height of the Yom Kippur War.
Once a significant theft of plutonium or other wea-
pons material has occurred, how will it be recovered?
To prevent traffic in heroin, police have asked for no-
knock search laws. This infringes upon one of our
most cherished freedoms. To live with plutonium we
may have to abandon this freedom along with others.
In the presence of nuclear blackmail threats, the in-
stitution of martial law seems inevitable. It has been
said that the widespread availability of weapons ma-
terial and terrorists targets in the nuclear fuel cycle
will radically alter the power balance between large
and small social units (De Nike [16]). It should be
added that the threatened society will undoubtedly
attempt to redress that balance through sophisticat-
ed and drastic police action.
In sum, to accommodate plutonium we shall have
to move toward a more intimidated society with
greatly reduced freedoms. In this respect the follow-
ing passage from the report, of the distinguished in-
ternational group of scientists attending the 23rd
Pugwash Conference on Science and World Affairs
is instructive:
The problem of theft of nuclear material by internal
groups of individuals intent on sabotage, terrorism or
blackmail was agreed to lie a very serious one, although
there was some sentiment expressed that the possibility
of such activity was much smaller in socialist states.
We believe that sentiment to be true. It is also ap-
parent that that is the direction in which we must
move to accommodate the nuclear industry. After
having spent billions of dollars for our nuclear de-
terrent, our civilian nuclear industry might well ac-
complish that which our defense system is trying to
prevent.
Alvin Weinberg is one of the few persons closely
associated with the nuclear power complex who has
looked carefully at the political and regulatory insti-
tutions that will be necessary to support a plutonium-
based nuclear power economy, and his views on this
subject merit close attention [19]. Weinberg's basic
premise is that nuclear power will place unprecedent-
ed strains on our society. In an unpublished paper
circulated prior to a conference in June 1973 at the
Woodrow Wilson International Center for Scholars
in Washihgton, D.C., Weinberg set out his views on
the type of new institutions required to cope with
the plutonium economy:
One suggestion (proposed by Sidney Siegel) that is
relevant to the situation in the United States would be
to establish a national corporation patterned after
COMSAT to take charge of the generation of nuclear
electricity. Such an organization would have technical
resources that must exceed those available to even a
large utility: and a high order of technical expertise in
operating reactors and their sub-systems is essential to
ensuring the continued integrity of these devices. [Here
Dr. Weinberg suggests nationalization of the industry.]
Each country now has its own AEC that sets stand-
ards or, in some cases, actually monitors or operates re-
actors. Perhaps this will be sufficient forever. Yet no
government has lasted continuously for 1,000 years:
only the Catholic Church has survived more or less con-
tinuously for 2,000 years or so. Our commitment to nu-
clear energy is assumed to last in perpetuity—can we
think of a national entity that possesses the resiliency
to remain alive for even a single half-life of plutonium-
239? A permanent cadre of experts that will retain its
continuity over immensely long times hardly seems
feasible if the cadre is a national body.
It may be that an International Authority, operating
as an agent of the United Nations, could become the
focus for this cadre of expertise. The experts themselves
would remain under national auspices, but they would
be part of a worldwide community of experts who are
held together, are monitored, and are given long-term
stability by the International Authority. The Catholic
Church is the best example of what I have in mind:
a central authority that proclaims and to a degree en-
forces doctrine, maintains its own long-term social sta-
bility, and has connections to every country's own Cath-
olic Church. (Emphasis added.)
These are far-reaching concepts presented by
Weinberg. The basic question they pose is: Will the
plutonium economy raise socio-political problems of
such magnitude that their resolution will be unac-
ceptable to society? In attempting to do the impos-
sible—live with plutonium—we may create the in-
tolerable.
Super-Human Requirements
The commercialization of plutonium will bring
with it a major escalation of the risks and problems
already associated with nuclear power. Plutonium
will further strain the already weakened regulatory
fabric of the nuclear industry.
Hannes Alfven, Nobel laureate in physics, has de-
scribed'the regulatory imperatives applicable to the
nuclear industry:
Fission energy is sale only if a number of critical de-
vices work as they should, if a number of people iA key
-------
positions follow nil their instructioas, if there is no (
salxitagc, no hijacking of the transports, if no reactor
fuel processing plant or reprocessing plant or reposi-
tory anywhete in the world is situated in a region of
riots or guerrilla activity, and no revolution or war—
even a "conventional one"—tikes place in these re-
gions. The enormous quantities of extremely dangerous •.
material must not get into the hands of ignorant people •'•'
or desperados. No acts of God can be permitted [20].
Weinberg similarly stresses the need ". . . of creat-
ing a continuing tradition of meticulous attention to
detail" and suggests that "what is required is a cadre
that, from now on, can be counted upon to under-
stand nuclear technology, to control it, to prevent
accidents, to prevent diversion" [19].
The public and its decisionmakers must seriously
question whether it will be possible to attract, train
and motivate the personnel required for these func-
tions. These must be highly qualified persons who
will maintain a tradition of "meticulous attention to
detail" even when the glamorous aspects of a new
technology become the commonplace operations of
an established industry. We suggest that it is beyond
human capabilities to develop a cadre of sufficient
size and expertise that can be counted upon to under-
stand nuclear technology, to control it, and to pre-
vent accidents and diversion over many generations.
There is considerable evidence at the present time
to suggest that the fledgling nuclear industry is al-
ready unmanageable. Consider, for example, that a
previously secret AEC study released by Ralph
Nader concluded that:
The large numher of reactor incidents [850 abnormal
occurrences], coupled with the fact that many of them
had real safety significance, were generic in nature,
and were not identified during the normal design, f,'ib-
rication, erection, and proopcrational testing phases,
raises a serious question regarding the current review
and inspection practices both on the part of the nuclear
industry and the AEC [21].
In addition, consider the tritium that recently ap-
peared in the drinking water of Broomfield, Colorado.
Consider the 115,000 gallons of high-level radioac-
tive wastes that leaked from the tank at Hanford,
Washington, over a period of 51 days while no one
monitored the tank. Consider that the radioactive
releases from the famed Shippingport reactor in
Pennsylvania were higher than recorded. Consider
that the executives of Consumers Power Corporation
in Michigan failed to notify the AEC that their
radioactive gas holdup system was not functioning.
Consider that two reactors in Virginia were half com-
pleted before the AEC was informed that they were
being constructed over an earthquake fault. Con-
sider that the GAO found security at plutonium
storage areas totally inadequate after the AEC in-
spectors had certified the facilities.
Considering all this, there is go'od reason to sug-
gest, because of the meticulous attention to detail
that will be required at every stage of plutonium re-
cycle, that a decision to proceed with plutonium
recycle will precipitate an already unmanageable sit-
uation into a national crisis.
Given that the risks of plutonium recycle are un-
acceptably high, particularly in light of the present
Plutonium in cake form. This batch was produced
at the AEC's Savannah River Plant near Aiken.
S.C.
uncertainties, a key question is what are our options?
What are the alternatives to the AEC's proposal to
proceed now with plutonium recycle? We believe that
there are essentially three options, each of which is
preferable to the AEC's announced plan.
Alternatives to Plutonium Recycle
• We could phase out nuclear power reactors.
There is mounting apprehension among knowledge-
able persons concerning the human and societal haz-
ards of fission reactors, which would only be com-
pounded by plutonium recycle. The 23rd Pugwash
Conference on Science and World Affairs in Septem-
ber, 1963, concluded:
1. Owing to potentially grave and as yet unresolved
problems related to waste management, diversion of
fissionable material, and major radioactivity releases
arising from accidents, natural disasters, sabotage, or(
acts of war, the wisdom of a commitment to nuclear
fission as a principal energy source for mankind must
he seriously questioned at the present time.
2. Accordingly, research and development on alter-
native energy sources—particularly solar, geothermal
and fusion energy, and cleaner technologies for fossil
fuels—should be greatly accelerated.
3. Broadly based.'.studies aimed at the assessment of
(he relnfion between genuine and sust-ainable energy
needs, a.s opposed lo projected demands, are required.
This third recommendation implies the implementa-
tion of energy conservation measures. It is important
to recognize that energy conservation can be our ma-
jor energy source between now and the year 2000.
Conservation means using our present energy more
efficiently; it need not mean a change in life styles.
Coupled with the use of solar and geothermal energy,
energy conservation could eliminate the need for new
nuclear power stations.
• We could continue with the present generation
of light water reactors but strictly prohibit plutonium
recycle for the foreseeable future. Such a decision
would be premised upon a judgment that plutonium
November 1974 Bulletin o\ the Atomic Scientists 21
-------
is too dangerous because of its toxicity and explosive
potential to be allowed to become an article of com-
merce. Of course, we would still have plutonium to
cope with because it is produced in present-day reac-
tors. But without plutonium recycle there should be
little incentive to reprocess the plutonium out of the
spent fuel, so the plutonium could remain in the
spent fuel where it is effectively protected from theft
and, hopefully, confined and contained.
The benefits of plutonium recycle are small. Pluto-
nium recycle would reduce the annual uranium re-
quirements by about 10 to 15 percent and reduce the
light water reactor fuel cycle cost by about the same
amount. But the nuclear fuel cycle cost represents
less than 20 percent of the total cost of power from
nuclear plants, and nuclear plants by 1985 will rep-
resent less than 40 percent of the electric, or about
15 percent of the total, domestic energy supplied. In
other words, plutonium recycle involves an economic
savings of less than one-half of one percent.
Plutonium differs from the high-level wastes in the
spent fuel in one critical respect: whereas the radio-
activity of high-level wastes will continue for thou-
sands of years, that of plutonium will continue for
hundreds of thousands. Thus, while the problem of
effectively storing both those materials and prevent-
ing their entering the environment are unprecedent-
ed in human history, plutonium must be contained
for eons longer. For this reason, an argument can be
made that, ultimately, the safest thing that can be
done with plutonium is to burn or fission it in reac-
tors, thus making it into high-level wastes rather
than plutonium. But that is an activity that is best
left for decades or even centuries hence—for a society
more capable and less violent than today's.
• We could defer for several years the decision re-
garding plutonium recycle until present uncertainties
regarding safeguards and plutonium toxicity are sat-
isfactorily resolved and a basis has been laid for a
more intelligent judgment regarding the risks and
benefits of the commercialization of plutonium. We
believe that this option must command general sup-
port. Too many questions, both technical and social,
are unanswered today. And until these questions are
answered it would be a grave error, we believe, to rush
into the AEC's plutonium economy.
Is the American public willing to accept the risks
of plutonium in exchange for the promised benefits?
The national debate which must occur on this basic
question has hardly begun.
NOTES
1. Glenn T. Seaborg, "The Plutonium Economy of the
Future," Release No. S-33-70 (Washington, D.C.: Atomic
Energy Commission, October 5, 1970).
2. Atomic Energy Commission, "Draft Generic Environ-
mental Statement on the Use of Mixed Oxide Fuel," WASH-
1327 (Washington, D.C.: The Commission, July 1974).
3. Donald P. Geesaman, "Plutonium and the Energy De-
rision," in The Energy Crisis, ed. R.S. Lewis and B.I. Spinrad
(Chicago, 111.: Bulletin of the Atomic Scientists, 1972), pp.
58-59.
4. Mason Willrich and Theodore B. Taylor, Nuclear
The/1: Risks and Safeguards (Cambridge, Mass.: Ballinger,
1974).
5. The AEC's attempt to recycle plutonium into the Big
Rock Point (Mich.) reactor was stopped by a lawsuit. West
Michigan Environmental Action Council v. AEC (W. D.
Mirh. Dkt. No. G-!")8-73).
6. Weekly Energy Report, "GE Fuel Recovery Plant 'In-
operable,'" II (July 15, 1974), 1.
7. Atomic Energy Commission, "Nuclear Power Growth:
1974-2000," WASH-1139 (Washington, D.C.: The Commis-
sion, 1974), p. 34 (Case D projection). The year 2000 figure
includes plutonium produced in liquid metal fast breeder
reactors.
8. Arthur Tamplin nnd Thoma.s Corhrnn, Radiation Stand-
ards of lint I'drlU'lrN (WjiMhin(;lon. !).('.: Nat.ural Re-
sources Defense Council, Feb. 14, 1974). Copies of this rc|M)rt
arc- available from NRDC (1710 N St., N.W., Washington,
D.C. 20030) for $3 per copy.
9. Atomic Energy Commission, press release, August 14,
1974.
10. W. C. Bartels and S. C. T. McDowell, quoted in Nu-
r/rar A'eu.n, 17 (Aug. 1974), 4G. «
11. Clarence E. Larson, "Nuclear Materials Safeguards:
A Joint Industry-Government Mission," in Proceedings of
AEC Symposium on Safeguards Research and Development,
Oct. 27-29, 1969, WASH 1147 (Washington, D.C.: The
Commission, 1969); and Deborah Shapley, "Plutonium: Re-
actor Proliferation Threatens a Nuclear Black Market,"
Science, 172:3979 (April 9, 1971), 143.
12. See, for example, Bernard T. Feld, "The Menace of
a Fission Power Economy," Bulletin, 30 (April 1974), 32-34;
22
Lawrence Scheinman, "Safeguarding Nuclear Materials,"
Bulletin, 30 (April 1974), 34-36; David T. Rose, "Nuclear
Electric Power," Science, 184:4134 (April 19, 1974), 351-359.
See also Robert L. Heilbroner, An Inquiry into the Human
Prospect (New York: W. W. Norton, 1974), pp. 40-43.
13. See, for example, Atomic Energy Commission, "The
Threat of Nuclear Theft and Sabotage" (Rosenbaum Re-
port), Congressional Record, April 30, 1974, p. S 6621; Gen-
eral Accounting Office, "Prelecting Special Nuclear Mate-
rial in Transit: Improvements Made and Existing Problems,"
B-164105 (Washington, D.C.: U. S. Government Printing
Office, 1973).
14. Dean E. Abrahamson, "Energy: Nuclear Theft and
Nuclear Parks," Environment (July/August, 1974), 5.
15. Taylor and Willrich believe that "a system of safe-
guards can be developed that will keep the risks of theft of
nuclear weapon materials from the nuclear power industry at
very low levels" [4, p. 171]. Yet they also emphasize'that
"regardless of its effectiveness, a nuclear safeguards system
applicable to the nuclear power industry in this country can-
not provide complete assurance that unannounced fission ex-
plosions will not occur in the United States in the future."
They point out that "nd future safeguards system that will be
practical can offer 100 percent assutance against theft" [4,
p. 123]. They never,say what level of nuclear theft, or what
size plutonium black market or bow many unauthorized nu-
clenr explosions are in fact acceptable to them.
16. L. Douglas DeNike, "Radioactive Malevolence," Hitl-
Iclin, 30 (February 1974), 10. Son also the story on the bomb
threats that have occurred at the Zion nuclear power plant in
northern Illinois reported in Environment, "Spectrum" (Oc-
tober 1974).
17. Nuclear Industry, "Industry Inundated by Proposed
New Safeguards Rules" (February 1973), pp. 45-47.
18. R. S. Lewis and B. I. Spinrad, eds., The Energy Crisis,
(Chicago, 111.: Bulletin of the Atomic Scientists, 1972), p. 59.
19. Alvin Weinherg, "Social Institutions and Nuclear
Energy," Science, 177:4043 (July 7, 1972), 32-34.
20. Hannes Alfven, "Energy and Environment," Bulletin,
29 (May 1972), 5.
21. AEC Task Force Report, dated October, 1973, page 16,
released in testimony presented to the Joint Committee on
Atomic Energy by Ralph Nader and the Union of Concerned
Scientists, January 29, 1974.
-------
557
ENVIRONMENTAL ACTION
OF COLORADO
January 1, 1975
Dr. William Mills, Director
Criteria and Standards Division
Office of Radiation Programs
Environmental Protection Agency
401 M Street, S.W.
Washington, D.C. 20460
Dear Dr. Mills:
I am writing to request an opportunity to provide testimony at the upcoming
Plutonium standards hearing to be held in Denver on the 10th of this month. It
is my understanding from a conversation with Paul Smith of E.P..A., Denver regional
office, that it is necessary for those who wish to testify to submit a written
request prior to the 3rd of January outlining the gist of one's testimony.
It is also my understanding that the Denver hearing is a continuation of a
one-day hearing held in Washington, D.C. on the 10th of December. Paul didn't
have any reports that had resulted from that first section of this hearing, but
he said that he believed the testimonies from both were going to be compiled and
distributed sometime after January 10th and that to the best of his awareness
there was not going to be any other opportunity for public participation or input
(i.e. no other hearings or public forums). Is this true? Are there any other
hearings or programs planned that involve the public at large? I would also
greatly appreciate any documentation of the Washington hearing that may be acces-
sible, including a list of who testified about what, who makes up the E.P.A.
panel, etc.
I plan on giving a curt statement, not longer than 10 minutes, regarding
the overall health hazards to the public, particularly from plutonium releases
in the past and potentially in the future in this area, and how they relate to
Denver regional planning. I will also touch upon the federal government's and
industry's approach to public awareness and educational efforts that have been
made in the past and how these efforts have fallen short of what is needed. I
would like, if possible, to utilize a slide presentation and would also like to
submit reprinted material to be included in the record.
If you have any questions or comments, please don't hesitate to contact me.
We are very happy to see that this important subject is being dealt with and that
the public is allowed to participate. I look forward to your response.
Sincerely,
Albert Nunez, Jr. 11OO
AN:jmj DENVER, COLORADO BO2O2
PHONE C 303) 534-16O2
-------
!?*
Coalition
oflfexas
, . § . E • C • T • • • P.O. Box 281 83, Sr.n Antonio, Texas 78228 •
(512)732-4181 •(512)733-0557
MATERIAL SUBMITTED REr HEARING ON PLUTONIUM
January 1, 1975
Dr. William Mills
Director of Criteria and
Standards Division
Office of Radiation Program
Environmental Protection Agency
Washington, D.C. 20460
Dear Sir:
We submit the enclosed items for your record and also
wish to express our opposition to the building and operation
of nuclear fission reactors, since they produce radioactive
wastes including plutonium 239 and since they are bsing
designed to use plutonium as fuel.
Sincerely yours,
—•
Enclosures: Physicians letter, Plutonium items.
»*
"Nuclear fission is one of the main obstacles to other new energy systems. If we were
not in the middle of a sales campaign for nuclear fission, we would be in the middle
of a sales campaign for the alternatives - and solar energy is the outstanding
alternative. The moment a moratorium on the operation of nuclear power plants seems
certain, we will see solar energy systems blossom into commercial readiness with
breath-taking speed." Egan O'Connor, energy consultant, Committee for Nuclear
Responsibility, Washington, D.C. 20003.
-------
559
HERMAN R. L.EVINE, M. D.
1OI7 DONALDSON AVENUE
SAN ANTONIO, TEXAS 78328
732-4181
January 1, 1975
Dr. William A. Mills, Director of
Criteria and Standards Division
Office of Radiation Program
Environmental Protection Agency
Washington, D.C. 20460
Dear Dr. Mills:
As a physician, I wish to take this opportunity to
express my deep concern regarding the proposed move to
use plutonium 239 as a power source.
With just a comparatively few fission reactors operating,
there are already numerous accidental plutonium contaminations
and spills. With increased use of this chemical as fuel,
accidents will multiply and plutonium pollutants will eventually
reach out and cause widespread tragic disease and deformities.
It is therefore essential that plutonium be banned from
use as nuclear fuel and that the operation of nuclear reactors,
since they produce plutonium, be halted.
Sincerely yours,
evine, M.D.
-------
ISO
No. T U1.T
Contact: Carl C-usiin
Tel. 3U1/H7.1-7771
IMMI UIA'II. Ill I I ASI-
, l)e> embi-r 1 i , I'.I'M )
AEC i'KOPOSl;S I'ININC CUMMONNIIALTII IHHSON iJS.SU
I;UK AI'I'AKLNI VIOLATIONS 01' AI;C Itl.DUI.A I IONS
The Atomic linergy Commission's Director of Regulatory
Operations has proposed lining Commonwealth Ldison Company
ol Chicago JiS.SOU for 18 apparent viuUtiuna ol AI:C RL-K-
uiations which occurreJ at the thi-fc-uni t DrcsJucc NucU-ur
I'owcr I'Jacit in Monis, iilicioi^, between June and Scp I umber.
The apparent vcola'ions involved manuumiuut ot tin;
plant's radioactive wa: te (.r.ldwabtej system, an unplanned
and uncontrolled relea c of radioactivity i'roin Ijce^den Unit 1
and implementation of ihe facility's betuccty plan. None of
the violations involved an immediate thle.u to public health
and safety.
ccurred on August 2S wlien
Director of Regulatory cj]>erat ions, In. UonalJ i . Kmuh,
in a letter to the Company, said the incident hus the lau-bt
example of failure to properly manage radioactive waste
operations.
Other apparent violations involving the i-adwa^tc system
include the Company's failure to exercise control over the
use of valves through which radioactive liquids can be
discharged, to conduct required analyses lor ladioactivi
isotopes and to calibrate monitoring instrumentation. i In-
systems are desi^nud to keep the routine release oi radio
activity from nuclear plants is low a:, practicable.
Violations ol the securit/ plan involved control of
limited access areas, traininj of guards and the adt>iua,_y
of communications between secjrity lorce personnel. II,e
Company's security plan is intended, to meet sub •, l ant la 1 1 v
strengthened Al:C security requirements which went into eiiei
on March 6, 1"74.
In his letter to the Company, Dr. Kiiuth said the AI.C
plans to continue to conduct unannounced inspections to
assure full compliance in the luture with Ai:c requirements.
-------
561
\
Page 4
(Reprinted by permission of Not Man Apart.)
Radiation Leaks
In Ohio, South
Carolina, and Illinois
lievcd to be biologically very nearly harmless
he discovery thatx
out of the ALiC's j
y in Miamisburg, '
JEFF KNIGHT'
The pa»t month has seen three accidental re-
Icasesof vauous kinds of ludiation into the envi-
ronment. ' v
' Th,: mcr.i serious was the discovery that\
I'iuioniumO3ti had le
Mound Weapons Laboratory
Ohio (p.t'-KiUion 1-4,000) into .1 portion of the r
Uric Canal near the factory. 'I'l.c plutouium was
discovered by city officials taking samples of
the -A-jin:..!!! i-i Ihir canal. \
^ "We liavr no idea how the plutonium leaked 1
out of the liictory into the mud," an AliC j
spokesman toU the Washintf-in 1'o.tl. "This \
comi!sji.s_a corajiHc surprise." The A EC said it '
is""hivest>>>a!ii'.g liie" ie.il\~l'uf did not know how
long it had i--i:n I'oing on or how extensive it
was. 'Hie AI-C said (here is.no danger as long as
the l'u-238 remains in the mud. (Tlie Cincinnati
/VIA/ reported tiiut the plulonium may have been
leaking for 16 years.)
l'lutonium-2.)8 i' about 250 tim»s more
l!.«;irdous than Pu-2W. It h.is a half-life of 90
yeaiS and is less hazardous if it is in water than
in tfc atmosphere, l-ike lJu-239, it is most
dangerous if taken into the lungs. Nevertheless,
some scientists L-el thai the AhC's standards for
pKitoaiuin in ualcr aic much UK1- hi;;.!). N
The second "incident" occurred at O'Hare \
Airport in Chicago, where a container with one j
mtllicuric of Iodine-131, a medical isotope, fell I
10 the runway und was tun over by a fork-lift. It '
contaminated 1,000 square feet of runwrv. \ofradiation is needed to damage the membranes
which was hosed down.'While the danger (isis /of living cells. Dr. Scott's experiments "iver?
accident created may have been negligible ' able to detect an increase in the leakage ute ol
(Iodine-131 is normally disposed of by din,- blood-cell membranes at only 0.008 raos nor
charge into the sewer system), the accids-r,! month, comparable to the dose received ln.-m
highlights the problems in safely transponin.^ natural background radiation previously
radioactive materials.
The third release was on May 8, at the A£C
special nuclear weapons production facility on
llie Savannah River in South Carolina. Fifty
grams of radioactive tritium gas were released
from a 7.00-foot stack on the 200,000-acre site.
The "cloud" of gas moved northward into a
rainstorm as it dispersed. Extensive testing by
state and federal officials revealed virtual!}, no
radiation on the ground the next day, according
lo the AEC. Apparently, the gas had dispersed
and diffused into the upper atmosphere, out of
harm's way. The rmo'int of radiation re!e;«*.!
was about half a pii'lion curies. Tritium tms a
half life of 12.2 years.
While the ABC reported that the local release
caused no harm, it did add radiation to tile envi-
ronment. The dangers of this were highlighted
in a letter by Dr. l-rnest Stemslass of the Uni-
versity of 1'itlsburgh School of Medicine to The
New Yurk Times on May 23,
'' Recent experimental studies of the elfecis of
very low doses of radiation on human cell nu'tit-
branes now indicate that the small releases of
radioactive gases and liquids in the course of
normal operations appear to produce biolo^ic.il
damage at a rate thousands ol times greater »hai
had been expected on the basis of our experi-
ence with medical X-Rays."
Dr. Stemglass cited experiments by Dr. A.
Petk.'U at the Canadian Atomic Energy
Laboratories in Manitoba and by Dr. E.G. Si'olt
at the University of California Medical Center in
San Francisco. Dr. Pctkau confirmed that the
more ptotracted the exposure, the smaller do:>e
-------
(Reprinted by permission of the Associated Press.)
Workers'bodies
DKNVER, Colo. (AF) -
Radioactive plutoniuni, a dan-
gerous substance linked to
canrer. has been detected in
the bodies of 171 present and
former employes at the Rocky
Flats nuclear weapon; plant.
The figure, compiled by the
Dow Chemical Co., represents
an increase from 105 in March
1972.
The figures indicate that
eight present employes and
six former workers show more
plutonium in their lungs than
is considered permissible, and
12 others have more than the
permissible body burden,
based on urine analysis.
Dow, which operates the'
plant for the Atomic Energy
Commission, said the overall
figure of 171 is for employes
showing a measurable amount
of plutoniuni in tlidr lungs.
The plant employs 2,9-10per-
sons altogether.
Plutonium, used at Rocky
Flats in the manufacture of
components for nuclear weap-
ons, is known to cause cancer
in persons who inhale large
amounts, and a study is being
conducUd of the effect on
plant wo-kers.
Some 178 Rocky Flats em-
ployes have already signed
c o n t r acts permitting
autopsies to aid the study.
The pi int's medical director
says tl ere have been no
deaths tiaced to the exposures
so far.
(Two articles were also submitted from the New York Times
but are not printed here because copyright releases were
• ' t obi", lined. They are:
1. ' L Senators Warn on Plutonium as Fuel" by Anthony
Ripley, 9-28-74, and
£. 'Plutonium Found in Plants' Roots" by Walter Sullivan
>11-74.)
-------
563
"Transient" Nuclear Workers:
A Special Case for Standards
(BY R. Gillette)
DutJalo, New York. For Ihe Buffalo
area's unemployed laborers, for the
moonlighters, college students, and the
young men recruited from small farm-
ing towns south of the city, the guar-
antee of half a day's pay for a few
minutes' work was an oll'cr they couMn't
refuse. Attracted by tho prospect of
easy money, they flocked by the lun-
dreds to the.Nuclear Fuel Services com-
pany between 1966 and he middle of
1972 to perform some of the dirtiest
jobs in what one official of the Atomic
Energy Commission (AUC) calls "the
dirty end of the nuclear business."
The business of Nuclear Fuel Ser-
vices (NFS) is the chemical extraction
of uranium and plutonium from the
highly radioactive spent fuel rods of
nuclear power reactors. Situated in pas-
toral, wooded hills 40 miles south ol
Buffalo, the chemical plait was the
nation's first commercial f ic! process-
ing facility. Although the technology it
used was far from experimental, the
NFS plant proved less than a smashing
technical success. Almost frjm the time
it opened in 1966 until it ceased operat-
ing in June of 1972 (for a major repair
and enlargement program ti> be finished
in 1977) the plant sutler :d lepeatcd
breakdowns and leaks of i idioactivity.
To clean things up and mike repairs,
the company relied heavily on the Buf-
falo area's abundant labor pool,
11 OCTOBER 1974
During 5l/i year-, of operation, ac-
cording to correspondence between NFS
and the AEC, Ihe company each year
hired an aveiage of 1400 "supplemental"
workers from surrounding communi-
ties, making up a temporary, -contin-
ually changing work force that out-
numrtcu'd the plant's permanent, trained
operating stuff by more than 10 to I.
With an apparent minimum of instruc-
tion in safety procedures and the poten-
tial hazards of their jobs, the supple-
mental men were put to work
decontaminating equipment and work-
ing areas, burying low-level nuclear
waste, and repairing radioactive equip-
ment.
Some of these workers were as young
as 18 and others are alleged to have
been recruited from bars for an after-
noon's work. Some would last a week
or more on the job. Others reached
legal exposure limits within minutes
and were promptly paid off—half a
day's pay (at around $.1 an hour) —
and replaced, in the derisive phrase of
a former full-time employe;, by "fresh
bodies."
On the average, according to AEC
inspection reports, the plant's tempo-
rary workers received a whole-body
radiation dose of 1.73 to 2 rems, an
amount not considered harmful, but
the equivalent nevertheless of five chest
x-rays. This is less than the maximum
Ihe AI:C allows for full-time radiation
workeis but much more than the in-
dustrywide average of 0.2 rem per year
and more than the 0.5 reni allowed lor
piiicmbcrs of the general public.*
The lempv rary workeis, like the
plum's permanent stall, also were ex-
posed (o small airborne conccntiations
°' P1"'"""_"_" -"id other radioactive fis-
sion products ivhose ha/ards are under
t debate (Scirmv, 20 and 27 September).
At one time the plant and its radio- ,
active diluents were the focus of en-
vironmental protests, but these objec-
tions largely subsided, first as waste
treatment imp:ovcd and later when the
plant closed. The company's public re-
lations efforts' have generally been ef-
fective, and a predominantly blue-collar
region now sejms to regard NFS as u
welcome source of jobs. Local opposi-
tion to a planned tripling of the plant's
capacity thus have been limited to a
handful of conservationists and a few
families whose sons worked at the plant.
It is expected to reopen in ahoi.t 3
years, at which time, AUC officials say,
the plant will be much cleaner. If it
isn't, one official adds, "we're in
trouble."
Dormant as it is light now, the NFS
plant provides a particularly vivid ex-
ample of a common a:id longstanding
practice in the nuclear industry. The
AF.C has long condoned thj use of
• federal rudialion pnHecliun vuideliiK-s in forte
MIICC IVOO Kininmc-nU thai individual-, in lite
lleneral population icccivc no nuue tli.in o ? iem
per year ol miiiuicJi.-ji laUuiinn to the whole
body. Ntulear winkers arc limited u> 5 rems per
year, but the t:uiik-lines allow a wuiki-r to iii>
lumulalc unused exposure aceoidii'.B u> the foi-
mula 5(«—18) wlieie « i» hi-i ate. I he worker
may draw on hi* "body bank" at a ule up to .1
rems per quarter or t2 letn-* pet jear.
us
(Reprinted by permission of Science. Vol. 186, pp. 125-129, 11 October 1974.
Copyright 1974 by the American Association for the Advancement of Science.)
-------
564
THE CITIZEN REGISTER
Ossining, N.Y., Fri., July 12, 1974
Jack
Anderson
WASHINGTON -
CONTAMINATED YOUTHS
A nuclear plant run by billio-
naire J. Paul Getty has h red
youths of 18 and older, worked
them in radiation areas, and
then allegedly cut them loose
in two days after they got ra-
diated.
In some cases, environmen-
talists charge, the young peo-
ple were never given forms
telling them how much radia-
tion they got, as required by
the Atomic Energy Commis-
sion.
The A EC is now holding
hearings on a request by Get-
ty's Nuclear Fuel Services to
expand the plant, which has
been out of major operation
since 1972. At present, the
sprawling facility at West Val-
ley, N.Y., is doing mainly
waste burial, decontamination
and storage work.
Already, 1,300 residents of
the West Valley area have pe-
titioned against the expansion,
according to the antinuclear
National Interveiiers. The
local Sierra Club's energy
chief, physicist Dr. Marvin
Resnikov, is collecting affida-
vits from some of the young
people who worked in the Get-
ty plant.
RESNIKOV HAS already
produced a horror gallery of
the plant inspection reports
riiowing workers skin acciden-
tally punctured by discarded
Plutonium needles, a w>rker
whose head was so contami-
•ated it left radiation on his
pillow, and other incidents.
Spokesmen for the coinpany
insist that the plant is well run
and safe, that the doses re-
ceived by workers were well
within the allowable lifetime
range for radiation set by the
AEC.
Since its reprocessing shut-
down fur expansion in 1972, the
spokesman said, the plant has
had virtually no exposure
problems, which previously
were minimal, they insisted.
The hiring of young people is
done through a contractor,
they explained, and all get
close radiation monitoring.
"Reprinted by permission of
United Feature Syndicate"
-------
us al
'
by Lloyd Nelson
"There is more than
enough nuclear waste stored
now to kill every individual In
the world/' said Charles W.
Huver, associate professor of
the University of Minnesota.
Ha lectured on the ecological
•environmental effects of
power plants on Wednesday,
Jan. 23, at the Collins
Classroom Center.
Huver has done special
research on radiation physics
and presented testimony at
congressional and state
hearings on environmental
effects of power plants.
Nuclear wastes are from
one million to one billion
timet, more toxic than poisons
such as cyanide on a per
weight basis, he said. At
present there are 90 million
gallons of waste on hand.
HUVCT countered Atomic
Energy Commission (AEC)
claims that those wastes are
being convert,id to sdts by
saying that only l per cent of
these nuclear wastes have
been successfully treated.
Wastes have even been
released into open waters, he
said.
According to Huver, the
\ most important question in
\ what should be done with
I radioactive waste materials.
/ The costs alone arc very high.
At present it is costing be-
tween two to three million
dollars for waste storage
After World War II we felt a
moral need to develop a
'good' use for atomic power,
according to Huver. This
need was felt as a result of
guilt feelings after dropping
nuclear bombs on Japan. It
was a means of atonement,
Huver said.
Because of these feelings
we rushed into nuclear power
production without proper
regard to the safety aspects.
Nuclear power was at first
viewed as a savior, he said.
Of the first generation of
nuclear power plants, seven
or eight have been declared
failures and have either been
- THE POINTER
termed inoperative or have
been closed for safety
reasons, said Huver.
Huver went on to say II
there are still many unan{|
swered safety problems ar,ci>
what we are left with is a
number of "dead white
elephants,"
. If a major accident occured
at a plant such as the one
proposed at Rudolph, Wis.,
immediate damage would
amount to $7 million property
damage and e human life loss
of about 3,400. These are old
figures and have been up-
dated to even higher num-
bers, he said.
Huver said that even at
present, nuclear con-
taminants have been linked
with genetic mutations and
occurances of stillborn
babies.
Although nuclear power
appears to be the answer to
our present energy crisis, it is
not the savior that it seems to
be, commented Huver.
Energy consumption in the
building and operating of
these plants should be con-
sidered, Huver said. As of
1970, 10 times the energy was
consumed in the building and j
operation of nuclear power
plants than all that had been
produced, he add*
^J^'IV,*. t?°~*\.*">-^nH*»Mqrf
-------
TH Cl«»elajif! Ifess, Tkunday. Kay Z3. 1974 (Reprinted by permission of the Cleveland Press)
CJ1
cn
CD
AEC probing radioactive water in Erie Canal
near Dayton
By RICHARD GIBEAU
Press Ohio Bureau
DAYTOX — Bob Wain-
wright, the Atomic Energy
Commission's manager for
Monsanto's Mound Labora-
tory in Miamisburg. has a
problem, and it's highly ra-
dioactive.
It's called plu.tonium-238,
a deadly man-made radioac-
tive element.
A concentration of t h e
hot plutonium particles,
which emit Alpha rays, has
beer found in the deceptive-
ly ~?cefu!-looking Old Erie
Canal and three small ponds
below the hilltop atomic
production plant operated
by the Monsanto Research
Corp. It is about 10 miles
from Dayton.
The problem is com-
pounded by the possibility
that the plutonium may
have been flowing Into the
canal and ponds for 16
years through a pipe that
was discovered only recent-
ly-
Wainwright's job is to
find out how much of the
plutonium has accumulated
in the silt and mud at the
bottoms of the canal and
ponds, and then to deter-
mine what must be done
with the material.
The plutonium-238, which
has been used in M o u n d
Laboratory's production
since 1958, is not supposed
the water and vegetation," will not cause instanteous
he said. desth.
to be in the canal and pond
beds.
It was only in recent
weeks that Monsanto's envi-
ronmental monitoring per-
sonnel discovered that what
they describe ~- z* the plant's
"effluent stream" was being
diverted by the pipe from
its intended patthway to the
Great Miami River.
Samples were t a fc e n of
the silt content, including
some obtained by driving a
pipe four feet deep into the
sediment.
"We got something of i
surprise, something we
d i d n 't anticipate," ".Vali.-
wright said.
Waimvright refuses, how-
ever, as do others at the
Mound Laboratory, to be
specific about the plutonium
concentrations found, em-
phasizing that a "very limit-
ed number" of random sam-
ples was taken.
"In the bottom, the levels
appear to be higher than in
Because the follow-up in-
vestigation will be an inten-
sive effort in the canal and
pond area, owned by the
city of Miamisburg, Wain-
wright said Mound Labora-
tory announced the findings
to allay public suspicion
about the activities to come.
The announcement, made
last Tuesday, was couched
in cautious language, de-
scribing the "small amount
of pIulonium-238" found as
presenting "no health prob-
lem."
Even that admission was
an unusual break in the
tone of serene perfection in
safety and engineering that
characterizes Mound Labora-
tory's annual environmental
reports.
A radiological chemist in
Cincinnati, a recognized au-
thority in the nuclear field,
said, "It must be pretty big
if they are making a special
announcement."
Monsanto's announcement
triggered a flurry of news
reports across the country,
including some containing
the statement that plutoni-
um 238 "can cause instan-
taneous death if inhaled."
Plutonium-238 i s among
the deadliest elements, but
the degree of its effect is
proportionate to the expo-
sure. Microscopic quantities
Just three weeks ago,
Mound Laboratory's 1973
monitoring report was dis-
tributed. It cited Mound's
"effective systems for the
containment of radioactive
materials." and "on-site and
off-site monitoring programs
which verify the integrity of
the control systems."
The case of the effluent
stream gone astray deflates
those claims.
Mound's monitoring pro-
gram was fairly Intensive,
Wainwright said, but added,
"We did not, however, sam-
ple the bottoms of these wa-
terways."
Now, M o u n d and AEC
face the task of determining
how much of the pluton-
ium-238 has settled below
those waters in the last 16
years.
"We got something
of a surprise, some-
thing we didn't an-
ticipate."
An AEC operation safety
officer in Washington specu-
lated earlier in the week
that tons of radioactive silt
and mud may have to be ex-
cavated, sealed in containers
and buried in a disposal site.
Plutonium 238 has a half
life of about 86 years, which
means half of it decays in
that time. It is highly radio-
active, the reason it has
been used as a heat-produ-
cer in the auxiliary power
systems for the Apollo space
vehicles and for satellites.
But Wainwright refuses to
speculate about what will
have to be done to eliminate
whatever radioactive mate-
rial may lie in Miamisburg's
ponds. They are planned as
part of a future city park.
He also reserves for later
consideration the question
of w h e t h e r the effluent
stream might also be depos-
iting hot plutonium in silt
in a drainage ditch leading
to the river, and in the bot-
tom of the Great Miami it-
self.
His immediate task is to
develop "a basic outline of
how to comprehensively
sample the whole area so we
can have a statistical base . .
. to define the problem, if
there is a problem, and then
decide what we're going to
do," he said.
Wainwright took that plan
this week to AEC's oper-
ations office in Albuquer-
que, headquarters for its at-
omic weapons complex for
approval.
He estimates the invest!-
g a 11 o n of the canal and
pond sediment will get un-
derway next Friday, *• !'h
sampling being don /
Mound personnel.
Other agencies will be in-
volved in addition to AEC,
including the U.S. Environ-
mental Protection Agency.
Gary Bramble, environ-
m e — t 2 1 *vslustior_ group
chief in the Dayton office of
the Ohio EPA, said the state
agency also intends to be in-
volve i,
"We wsnt to be on hand
when they sample and vre
want to take our own sam-
ples and o b t a i n an inde-
pendent analysis," he s'
Amid all the furor about
the plutonium threat in the
midst of his future park for
peaceful Miamisburg, that
city's manager, John Laney,
refused to be dismayed.
"We don't feel the least
bit concerned about our
park development. We ex-
pect it to proceed," he said.
-------
567
HC It'Q
•• \» ,,tlme to hsten to your own c°mrnon sense when you hear the claim that nuclear electric power will be
clean and safe , or the odds on a catastrophic nuclear power accident are "one-in-a-billion".
*l M
I • •
III order to keep those important promises - when nuclear plants will produce as much radioactivity as a
fa! T,f M ^L^0^ eXp*°Si°nS every year - the nuclear industrV ""1 have to contain its radioactive poisons with
better than 99.99% success. Total poisonmg of the planet is a certainty if just 1% of the long-term radioactivity escapes
into the environment. There is no disagreement over"that "" " - -~~
5k No—~~.
u ,-, 7u j0"6 " the re1uirement for perfect performance in the nuclear power industry. The argument is
over the likelihood of meeting the requirement and keeping the promises.
1. How many industries come close to 99.99% perfection in performance; Or even 997o?
2. What about mistakes and carelessness already appearing in the civilian nuclear program?
3. What about the performance record with nuclear submarines? (Please see inside page.)
Some Mistakes Already
"Review of the operating history associated with
30 operating nuclear reactors indicated that during
the period 1/1/72 to 5/30/73 approximately 850 ab-
normal occurrences were reported to the Atomic Energy
Commission (AEC). Many of the occurrences were
significant and of a generic nature requiring follow-up
investigations at other plants. Forty percent of the
occurrences were traceable to some extent to design
and/or fabrication-related deficiencies. The remaining
incidents were caused by operator error, improper
maintenance, inadequate erection control, administra-
tive deficiencies, random failure and combination
thereof. . .
"The large number of reactor incidents, coupled
with the fact that many of them had real safety sig-
nificance, were generic in nature, and were not
identified during the normal design, fabrication, erec-
tion, and pre-operational testing phases, raises a serious
question regarding the current review and inspection
practices bolh on the part of the nuclear industry
and the AEC." (Source: AEC Task Force Report:
Study of Reactor Licensing Process, by AEC Asst.
Director of Regulation, I.. V. Gossick and 7 additional
AEC experts, the Octuber 1973 version; see also Study
of Quality Verification, AEC, Jan. 1974, p!5-17)
From years of living, YOU know that the very
things which fine, intelligent people work hard to
prevent often happen ANYWAY. Even statistically
"impossible" events have occurred in YOUR lifetime.
WOULD YOU BELIEVE ...
-------
'"'CO '^ne Guinness Book of World Records lists park explained to the Associated Press in Wayncsboro,
i3 b 0 ranger Roy Sullivan as the "only living man to be Virginia.
,•':'• struck by lightning four times". On August 7, 1973, he . Sullivan was first hit in 1942, when a .bolt
stepped out of his truck and was zapped for the clipped off a toenail. In 1969, lightning burned off
fifth time; he suffered second-degree bums. his eyebrows and knocked him unconscious. In 1970,
"The bolt struck me right on the head, set my lightning struck and burned his shoulders. In 1972,
hair on fire, traveled down my left arm and leg, another bolt burned off his hair.
knocking off my shoe but not untying the lace," he (Washington Post, August 27, 1973'
Short Amazing Stories
,* NOT VERY LIKELY: What are the odds that, in an 8-vehicle collision on Los Angeles' Golden State Freeway, -
1 four of the vehicles will be fuel trucks? It happened, on January 8, 1974 ... and in the middle of a fuel-shortage.
2 THEN THERE WERE TWO: "With what one observer called a 'tremendous cracking sound', a 9-month-old, $12-
- * million tanker operated by the Ingram Corp. split down the middle and sank in Port Jefferson Harbor on New .^
•'"""' York's Long Island. The 620-foot ship, which had cruised unscathed through two hurricanes, had already un-£*
loaded its cargo of 6 million gallons of gasoline and fuel oil, and authorities suggested that the tanker might have|*
been under unusual stress amidships from improper ballasting." (Newsweek, 1/24/72) The odds? Human error ;
somewhere? ;•.•*»•>;
3 DESIGNED TO PRODUCE A BETTER PRODUCT: After several months of investigation and 300 controlled
tests, the Campbell Soup Co. discovered how lethal bacteria got into some chicken vegetable soup in the summer
of 1971. On Nov. 20, 1971, Campbell's president, W. B. Murphy, announced that the botulism occurred by
"several unusual conditions happening simultaneously — above average viscosity of the can contents, over-fill
of the can, and incomplete hydration of the dry ingredients, coupled with a new process designed to produce a
.;, better product." , • .
Said Dr. Willis Irvin/USDA inspector at the Campbell plant, "We have our men spread pretty thin... . It's a very
large and complex plant, but I doubt if having another inspector would have prevented this. ... It was a com-
bination of very obscure things that no human being would have picked up." (Washington Evening Star,
11/20/71)
.• COULD NEVER HAPPEN TO US: Remember the hapless bank clerk in Idaho who inadvertently shredded 8,000
4 unprocessed checks worth an estimated $850,OQO? The bank president appeared on national news saying, "We
never dreamed it could happen to us," while a team of clerks were seen in the background trying to fit the
right pieces back together with scotch tape. (From the CBS evening news, 7/21/71)
H THIS IS AN EMERGENCY ACTION: If there is one system whose credibility must be protected at all cost,,
9 it is the Army's system to warn the nation of a military emergency. Nevertheless, in February 1971, the Army's
National Warning Center sent out this fully authenticated national emergency alert instead of the routine test-
message: MESSAGE AUTHENTICATOR, HATEFULNESS - HATEFULNESS. THIS IS AN EMERGENCY
,,,^ACTION NOTIFICATION DIRECTED BY THE PRESIDENT. NORMAL BROADCASTING WILL CEASE
IMMEDIATELY. Scores of radio and TV stations broadcast the emergency. • >':!''T. ,• .y't •. ,.
It took the Associated Press and United Press International only 10 minutes to find out the alert was a dud, but
it took the Army 37 minutes to cancel it. The first cancellation message had no authenticator - the necessary
code-word. The second cancellation message had the wrong authenticator. On the third try, the Army got the
right code-word: IMPISH - IMPISH, and officially called off the national "emergency", which was nothing more
than one human who had selected the wrong pre-punched teletype tape.' .• ' , i .
g+ TENDER LOVING CARE: Although thousands of Americans, from people soldering circuits to computer pro-
O ':••"• grammers, felt personally responsible for the safety and success of the Apollo astronauts, two out of seventeenv
'.:' Apollo missions failed not from outer-space surprises, but from simple human errors (1967, 1970). ,;Y :
— WIDE OPEN SPACES: Although pilots try harder than anything not to run into other airplanes, two airliners
i traveling in the same direction collided in the mid-morning skies over the Grand Canyon in July 1956. The odds?
Pilots also try to avoid well-known buildings. On an August morning in 1945, a bomber flying under a 900-ft.
ceiling, flew smack into the Empire State Building. .-'
A A PERFECT RECORD . . . UNTIL: Leon Moisseiff, the famous engineer who designed and built the Manhattan,
O Triborough, and George Washington bridges, also built a giant suspension bridge across the Tacoma Narrows. The
'\ i bridge collapsed 4 months after completion. "Moisseiff said only that the bridge failed because engineers do not
. .';yetknow enough about aerodynamics." (Time magazine, 11/18/40) ^ ^ ^ ^>
-------
Till', MOLASSES TIDAL WAVE: In all of luim;m liisloiy, there may have been only one killer tidal-wave made
of molasses. On Jan. 15, 1919, an "incredible" 15-loot wave of molasses killed 21 people and demolished a
block area of Boston immediately after the rivets 1>; gan popping from a tank holding 2.2 million gallons of the
sticky goo. Damage was $2 million. (Boston Evening Globe, 8/12/71) Even the AEC might have said, when the
21 victims were born, that the odds were EXCEEDINGLY REMOTE that they would die in a molasses tidal-
wave. But that is how they died. Many more died in 1912 when, in defiance of all mathematical probabilities,
the "unsinkable" Titanic sank on her maiden voyage.
Nuclear Submarines
The captains of our nuclear submarines are key-pins in our policy of deterring nuclear war, and surely
they are more alert than the average man-in-the-street. You would expect them to know when a freighter is right on top
of them. Nevertheless, on Oct. 6, 1972, one of our nuclear submarines - the USS TULLIBEE - collided with the West
German merchant ship HAGEN 150 miles off the coast of North Carolina. "First reports indicate the collision involved
a glancing blow on the upper part of the submarine bow with no internal damage. At that trine, the TULLIBEE apparently
was operating just below the surface. . . ." (Release issued in Norfolk, Virginia, by the Commander in Chief, Atlantic.)
Nuclear submarines, which are supposed to survive the problems of wartime attack, are not supposed to
sink under peacetime conditions. However, in 1963, the USS THRESHER vanished and was found at the bottom of the
sea. The causes: faulty pipe joints and an inadequate deballasting system, according to the Navy. In 1968, the USS
SCORPION also went down forever. And imagine the Navy's dismay when a nuclear submarine sank at dockside in May
1969. Fortunately, the nuclear power plant had not yet been installed in the USS GUITTARO when it suddenly flooded
and sank at the Mare Island Shipyard in California. The odds?
As for the submarine missiles, in August 1973, Rear Admiral Levering Smith acknowledged that 58% of the
Poseidon missiles on nuclear submarines had failed their operational tests, and that "essentially all of the missiles" would
have to be recalled.
Nuclear submarines have even sent false alarms about attack. On Jan. 16, 1974, the United Press carried
this story: "Emergency transmitters on Polaris submarines mistakenly signaled they had been 'sunk by enemy action' on
two occasions in 1971, and raised the threat of accidental nuclear war, Rep. Les Aspin (D-Wis) said yesterday. The signals
set off general military alerts until the subs themselves surfaced and advised by regular radio signals that the buoy-borne
emergency transmitters had malfunctioned, Aspin said. . . . The Navy confirmed that the two incidents took place. . . .
Spokesmen declined direct comment, however, on whether alerts resulted."
THE ACCIDENT RECORD IN THE NUCLEAR SUBMARINE PROGRAM IS A REAL-LIFE WARNING
ABOUT WHAT WE MUST EXPECT IN THE CIVILIAN NUCLEAR POWER PROGRAM. When 2 out of 125 operating
nuclear submarines have completely failed to perform (just stay afloat) during peacetime, what are the odds that no
civilian nuclear power plant will ever experience a disastrous failure to contain its radioactivity?
THE ANSWER: As of January 1, 1974, there were 42 nuclear reactor plants licensed to operate, 56 under
construction, and 101 on order (planned). The AEC plans to license 280 for operation by 1985, and 1000 by the year
2000 (average: 20 in every state). // we permit a thousand plants to operate, and if the probability of a major accident
were really as low as one-in-a-million per reactor per year, then the probability of a major accident during the 40-year
lifespan of the plants would be about one-chance-in-25.
Committee for Nuclear Responsibility, Inc. P.O. BOX 2329, Dublin, California 94566
Lenore Marshall
Founder (1899-1971)
Richard E. Bellman RamMy Clark John T. Ediall Paul R. Ehrlich John W. Gofman Charles E. Goodoll David R. Inglii
Richard Max McCarthy Ian McHarj Lcwii Mumford Linui Pauling Harold Urey George Wald Jamei D. Wawon
Reprinted by EARS
Environmental Action Reprint Service
University of Colorado at Denver
1100 14th Street
Denver, Colorado 80202
Phone (303) 534-1602
Distributed by:
NO PERMISSION IS REQUIRED TO REPRINT THIS FLYER, IN WHOLE OR IN PART.
EARS
-------
••*
One-Chance- in-a-Billion JM*~
Several stories inside this flyer show that statistically "impossible" events happen frequently, and that
extremely complex systems like moon-rockets (or nuclear power plants) can be destroyed by something as common as
faulty wiring or valves, a bad welding job, or a person simply doing the wrong thing. Recently, the AEG paid professors
at M.I.T. two million tax-dollars to estimate the probability of a nuclear power catastrophe. The report, which is known
as "the Rasmussen study," provides the AEC with figures like one-chance-in-a-billion per plant per year, according to
the AEC.
Such Figures Have No Meaning}
FIRST REASON is the difficulty of predicting either the frequency or the consequences of human error
(and malice). Error or malice could instantly reduce the catastrophe-odds from one-per-billion to near certainty. Estimates
about the small chance of a nuclear disaster depend on the reckless assumption that operators of nuclear plants will make
no serious errors during emergencies; also, that no demented or hostile people will try to destroy the plants.
SECOND REASON is the lack of experience with operating nuclear hardware. Since the very first 1,000-
megawatt nuclear plant went into operation in June, 1973, experts have hardly one reactor-year of experience to examine.
They can do little better than guess when they assign reliability estimates to nuclear hardware of this type. Furthermore,
for 4 years in a row, the AEC has had to scold and to fine nuclear equipment firms, engineering firms, and utilities for
unacceptably sloppy quality-control, but according to a report in the Los Angeles Times, Dec. 26, 1973, the industry
is still unresponsive.
THIRD REASON is the unjustifiable assumption that nuclear safety-systems (some of them never tested)
have been properly designed. This assumption denies all the recent nuclear "surprises" which show that nuclear engineers
are failing to foresee all the design problems. If the design of a safety-system is defective, even perfectly working hardware
will not make it effectivet
FOURTH REASON is the flaw of assuming that all possible paths leading to a catastrophe have been
recognized and considered. As recently as October 1973, the AEC's Director of Regulation, L. Manning Muntzing,
.admitted to a Congressional Committee (JCAE): "I'm really concerned about some of the surprises we see." How many
unsuspected paths to catastrophe are still waiting to be discovered?
HUMAN ERROR
Reactor Operating Experiences in the
journal "Nuclear Safety" show over and
over that a human decision is required on a
number of occasions.
When there are enough reactors opera-
ting, the total number of occasions requir-
ing a human judgment will increase ap-
preciably.
Let's play with some numbers which I
think grossly minimize the danger to be
faced.
Suppose you have 500 nuclear power
reactors in operation. Let's further sup-
pose that a serious human decision is requir-
ed once in ten years for each reactor; a
study of the literature might show that
the frequency is far greater. This means
SO serious decisions requiring human judg-
ment per year.
Suppose further that the judgments arc
98 percent right and 2 percent wrong,
which is a very optimistic estimate.
This finally gives us one reactor per
year suffering the consequences of wrong
judgment on a serious matter. Clearly if
the judgmental error results in a nuclear
melt-down, that's a disastrous event Even
less than melt-down accidents could be
very, very serious.
The requirement for a human judgment
is a source of immense weakness in nuclear
safety. Even if all other safety problems
could be solved, the human factor all by
itself means that nuclear power makes
no sense.
John W. Gofman, Ph.D., M.D.
SOME NUCLEAR 'SURPRISES'
Discovery in 1972 that nuclear en-
gineering firms have built the Prairie Island
and Kewaunee plants with steam lines
running underneath the control rooms,
where a rupture of a line could destroy
the controls and kill the nuclear plant
operators; extensive modifications will be
required in about six plants.
Unexpected densification of nuclear fuel,
one of the most tested elements of the
whole nuclear power system; this discovery
forced the AEC to cut back permissible
power levels by 5 to 25 percent at 10
nuclear power plants on August 24, 1973.
Failure of the vital emergency core
cooling system to provide AEC experts
with assurance of effective performance;
the system, which has never had a large-
scale test, failed six out of six miniscale
tests in late 1970.
As of Spring 1974, the emergency cool-
ing system has never had a successful
large-scale test.
SURPRISE! SURPRISE!
Discovery in 1971 that the allegedly
watertight salt mine chosen for radioactive
waste storage in Kansas was full of holes;
the AEC has been forced to improvise
"surface storage" plans.
Confirmation by the National Academy
of Sciences in November 1972 that low-
level radiation exposure is at least 500 per-
cent more harmful than the experts had
previously admitted; this surprise had al-
ready forced the AEC to suggest drastically
reduced "permissible emissions" from nu-
clear power plants.
Discovery by the North Anna Environ-
mental Coalition in August 1973 that two
nuclear power plants in Virginia have been
built on an earthquake fault in undeniable
violation of AEC policy.
Apparently nuclear experts did not
foresee, either, that on November 11, 1972,
three skyjackers would threaten to bomb
the nuclear reactor at Oak Ridge, Tenn.;
helpless, the AEC shut down its reactor
and evacuated. The skyjackers did not
carry out their threat
DO YOU WANT NUCLEAR POWER? C 0 H S U I t
Your Common Sense.
-------
Jan. 2 1975 571
15 Westminister Rd.
Summit, N.J. 07901
Dr. William A. Mills
Director of Criteria and Standards Division (AW 560)
Office of Radiation Program
Environmental ^ritection Agency
Washington, D.C. 20460
Dear Dr. Mills:
I ask that the attached article the Hazards of
Plutonium by .T.G> Speth be read and made part of the
Hearings on environmental plutonium standarj^ whdch are
being held by the EPA in Denver, on Jan. 10, 1975.
In place of an insane plutonium power source our
government should crash program wind generator development,
using the best ingineering minds and all needed investment
capital. 150 miles of wind generators could produce 60%
of New Jersey's electric needs estimates Heronemus of
U. of Mass., Amherst Mass. Let us stop paying tribute to
OPEC. Once wind generator prototypes are built, the price
of OPEC oil will frii. The development >f the fly wheel
for power storage and automotive power would als© free us
from dependence on dwindling natural resources.
Money for such deve lopment can ^come avai lable if we
stop the production of useless atomic weapons, and inefficient
atomic power plants.
Sincerely -
Frances Tysen
100% recycled paper earth color
-------
("Reprinted, with permission, from Natural, History; Magazine, January,
572 Convright (c) The American Museum of Natural History, 1975.")
The Hazards of Plutonium
by J. Gustave Speth
1975.
The recycling of this element—the stuff of
nuclear bombs and one of the most toxic
substances known— is highly controversial
The Atomic Energy Commission, if unchecked, is
about to sow the seeds of a national crisis. The
commission proposes to launch what it calls the
"plutonium economy," which would authorize the
nuclear power industry to use recycled plutonium as
fuel in commercial nuclear reactors around the
country. The result of such a decision would be the
creation of a large civilian plutonium industry and a
dramatic escalation in the risks posed by nuclear
power.
Plutonium barely exists in nature: the entire
present-day inventory is man-made, produced in
nuclear reactors. Plutonium-239, the principal isotope
of this element, has a half-life of 24,000 years; hence
its radioactivity is undiminished within human time
scales. That isotope is one of the most toxic substances
known. One millionth of a gram has been shown
capable of producing cancer in animals. Plutonium-
239 is also the material from which nuclear weapons
are made. An amount the size of a Softball is enough
for the production of a nuclear explosive capable of
mass destruction. Scientists now widely recognize that
the design and manufacture of a crude nuclear
explosive is no longer a technically difficult task; the
only real obstacle is the availability of plutonium
itself.
We believe that the commercialization of plutonium
will place an intolerable strain on our society and its
institutions. Our nuclear technology has presented us
with a possible new fuel that we are asked to accept
because of its potential commercial value. But in our
opinion, technology has outstripped our institutions.
which are not prepared or suited to deal with
plutonium. And those of us who have asked what
changes in our institutions will be necessary to
accommodate plutonium have conic away from the
inquiry profoundly concerned.
The AFC's recently released draft environmental
impact statement assessing the effects of recycling
plutonium reinforces these concerns. It concedes that
the problems of plutonium toxicity and nuclear theft
are far from solved and indicates that they may not be
for some years. Nevertheless, the statement conclude-
that we should proceed. The AEC decision, whether a
stems from blind faith in the beneficence of the
technology the commission has fostered or from a
callous promotion of the bureaucratic and industrial
interests of the nuclear power complex, cannot be
justified in light of what we know and, just as
important, what we do not know about the
implications of a plutonium industry.
The fuel used in today's nuclear reactors-light-
water reactors, or LWRs-is uranium that has been
enriched so that its uranium-235 content is increased
from 0.7 percent, the amount present in natural
uranium, to about 2 to 4 percent. Uranium-235 is a
fissionable isotope of uranium. The remainder of the
fuel is nonlissile uranium-238. Unlike plutonium, this
uranium fuel is not extremely toxic and not
sufficiently rich in uranium-235 to be fashioned into
nuclear weapons. When the LWRs are in operation,
however, they also produce as a by-product moderate
amounts of plutonium, principally plutonium-239. A
typical large reactor produces about 200 to 250
kilograms of plutonium isotopes each year. Since
much of this plutonium is easily fissioned, it can be
used as reactor fuel. Plutonium recycle is the nuclear
industry-AEC proposal to recover the fissionable
plutonium produced in LWRs, process it, and recycle
it as fuel back into LWRs.
Several critical steps would be involved in recycling
this plutonium. First, the used, or spent, fuel from the
reactor must be shipped to a fuel-reprocessing plant
where the plutonium would be removed.
It would then be shipped to fuel-fabricating and
assembly plants for the next fuel-cscle stages. At the
fabricating plants the plutonium oxide would be
mixed with uranium to form fuel pellets; the pellets
would be placed in fuel rods and the rods would be
collected into fuel assemblies. These assemblies would
then be sent to the reactors for use. thus completing
the fuel cycle.
Plutonium recycle has not yet begun, and so far
there is no major industrial commitment of resources
Snclli iinil nln wr/.vA Arthur K. Tiimplin tint! Tlxinhis h
74
-------
plants are in operation or under construction, and the"
three nuclear-fuel-reprocessing plants that have
already been built do not represent a substantial
investment in national terms. They may be needed, in
any case, to prepare spent fuel for long-term storage.
But if the plans of the AEC and the nuclear industry
are carried out, a major plutonium industry will
quickly develop. Such an industry could recover some
140 tons of plutonium from commercial reactors by
1985 and 1,700 tons by the year 2000. By the turn of
the century the industry could involve hundreds of
LWRs fueled with plutonium, perhaps a score of fuel-
reprocessing and -fabricating plants, and thousands of
interstate and international shipments containing
hundreds of tons of plutonium.
The most pernicious product of the nuclear industry
is plutonium. Microgram quantities in skin wounds
cause cancer in experimental animals. Inside the body,
plutonium is a bone seeker; once deposited there it
can cause bone cancer. But plutonium is most
dangerous when inhaled. In a recent article in the
Bulletin of the Atomic Scientists, Donald Geesaman, a
biophysicist formerly with the AEC and currently at
the School of Public Affairs of the University of
Minnesota, explains this hazard:
Under a number of probable conditions plutonium
forms aerosols of micron-sized particulates ... if
inhaled they are preferentially deposited in the deep
lung tissue, where their long residence time and
high alpha activity can result in a locally intense
tissue exposure. The lung cancer risk associated with
these radiologically unique aerosols is unknown to
orders of magnitude . . . [but] under present
standards, the permissible air concentrations are
about one part per million billion ... a
commentary on plutonium's potential as a
pollutant.
To determine the adequacy of the radiation
protection standards for plutonium enforced by the
AEC, two of the authors of the report from which this
article was adapted, physicists Arthur R. Tamplin and
Thomas B. Cochran, undertook a review of the
biological evidence for the Natural Resources Defense
Council. The conclusions of Tamplin and Cochran,
found in their study "Radiation Standards for Hot
Particles," are that insoluble plutonium particulates,
or hot particles, are uniquely virulent carcinogens and
that the current AEC radiation protection standards
governing the amount of plutonium to which members
of the public can be exposed are roughly 100,000 times
too lax. The lung cancer risk associated with hot
particles of plutonium, as estimated by Tamplin and
Cochran, is comparable to the lethal dose of botulin
toxin, a biological warfa.e agent. One would hope that
this nation would give careful consideration to the risk
involved and pursue all alternatives before
implementing an energy policy based on such toxic
materials.
Although the adequacy of present plutonium
standards is a matter of considerable doubt and great
controversy, the AEC's draft impact statement for
plutonium recycle simply assumes that those
standards are adequate. The entire risk analysis of the
with plutonium recycle, is based on a premature and j- n O
unexplained rejection of the hot particle hypothesis, 0 / «J
which asserts that the intense local radiation
emanating from minute hot particles is more
carcinogenic than the same amount of radiation
distributed over a larger tissue area. Yet despite the
AEC's dismissal of this hypothesis in its impact
statement, the commission concedes, in answer to a
petition brought by the Natural Resources Defense
Council in a separate proceeding, that the hypothesis
"is being given careful consideration."
We submit that the AEC has no basis for concluding
that plutonium recycle will not cause undue risk to the
public health and safety until it has either
satisfactorily resolved the doubts over current
plutonium radiation protection standards or
calculated the impacts of plutonium recycle on the
assumption that hot particles are uniquely
carcinogenic. The draft environmental impact
statement for plutonium recycle does neither.
Some plutonium contamination of the environment
has already occurred, principally as a result of the
atomic weapons program. The leakage of plutonium
from contaminated oil at the AEC's plutonium
weapons plant at Rocky Flats, ten miles west of
Denver, Colorado, in the late 1960s led to an
uncontrolled source of plutonium that was much
larger than the reported discharge from seventeen
years of plant operation. Tens to hundreds of grams of
plutonium went off site ten miles upwind from
Denver.
The Nuclear Materials and Equipment
Corporation, a facility in Apollo, Pennsylvania, that
processes plutonium for energy research and
development, was recently fined $13,720 for a sixteen-
count violation of AEC regulations, ranging from
failure to follow radiation monitoring procedures to
failure to comply with certain safeguards
requirements.
Production workers from the Nuclear Fuel Services
facility in Erwin, Tennessee, which processes
plutonium, met with AEC inspectors on August 13,
1974, to complain about the absence there of even the
rudiments of accepted health physics practices.
Occurrences such as these could multiply greatly if
plutonium is made a major article of commerce.
As a fuel for power reactors, plutonium is expected
to range in price from $3,000 to $ 15,000 per kilogram,
roughly the equivalent of the street price of heroin.
This same material might be hundreds of times more
valuable to fanatics and desperadoes bent on
obtaining power or wealth through the use of nuclear
devices. A recent AEC study identified more than 400
incidents of international terrorism carried out by
small groups during the past six years. In an age of
bomb threats, aircraft hijackings, the kidnapping of
diplomats, and the murder of Olympic athletes, the
risks of nuclear theft, blackmail, and terrorism are not
minimized even by sonic of the most ardent
supporters of nuclear energy. Thus. Clarence Larson,
former Atomic Energy Commissioner, has described
the evolution of a plutonium black market:
Once special nuclear material [plutonium| is
successfully stolen in small and possibly
-------
C ij r economically acceptable quantities, a supply-
' * stimulated market for such illicit material is bound
to develop. And such a market can surely be
expected to grow once the source of supply has been
identified. As the market grows, the number and
size of thefts can be expected to grow with it.
The critical point here is that these tremendous risks
will become real with the advent of plutonium recycle.
Black marketeers or terrorists would find it too risky to
steal plutonium that has not been made easier to
handle by being separated from the highly penetrating
radiation in the spent fuel of present-day reactors.
Until irradiated fuel is reprocessed and the plutonium
separated out, the possibilities of theft in the light-
water reactor fuel cycle arc accordingly minimal. But
once the plutonium is reprocessed and recycled, the
picture changes dramatically. Reasonable prudence,
therefore, dictates that we have adequate answers to
the problem of nuclear theft well in hand before
plutonium recycling begins.
There is now widespread agreement, at least among
those outside the nuclear industry, that present
safeguards against plutonium theft are woefully
inadequate. The AEC's own "Rosenbaum Report," an
assessment of the adequacy of the agency's safeguards
of special nuclear material made in 1974 by outside
consultants, concluded:
In recent years the factors which make safeguards
[against plutonium theft] a real, imminent and vital
issue have changed rapidly for the worse. Terrorist
groups have increased their professional skills,
intelligence networks, finances, and level of
armaments throughout the world.. . . Not only do
illicit nuclear weapons present a greater potential
public hazard than the radiological dangers
associated with power plant accidents, but. . . the
relevant regulations are much less stringent.
The problem is not simply that the AEC has not
implemented the necessary safeguards programs;
rather the agency has not even developed an adequate
program on paper.
On the subject of safeguards, the AEC's draft
impact statement for plutonium recycle breezily
concedes that the objective of keeping the risk of
nuclear theft small "will not be fully met . . . by
current safeguards measures." Among the several
steps suggested by the AI:C to correct inadequacies
are the following: (1) Location of reprocessing and
fabricating plants next to each other in order to
minimize or eliminate the shipment of plutonium
between them; (2) establishment of a new federal
plutonium security police force to protect facilities and
shipments; (3) creation of a sophisticated security
clearance system for nuclear industry personnel.
These and other proposals are still under study;
their content is not yet well defined. Some would
necessitate substantial changes in the structure of the
United States utility industry; others might require
congressional action. And the initiation of a
sophisticated safeguards program would pose a threat
to civil liberties and personal privacy. Nevertheless the
draft impact statement recommends that we proceed
now with plutonium recycle because "the Commission
has a high degree of confidence that through
implementation of some combination of [its
recommended steps] the safeguards general objective
. . . can be met for plutonium recycle."
The commission's faith, unfortunately, is hardly
reassuring. While it may be possible to devise an
adequate safeguard system in theory, there is little
reason to believe that such a system would be
acceptable in practice. This is true for several reasons.
First, the problem is immense. The theft of
plutonium is only one type of antisocial behavior a
safeguards program must protect against. Terrorist
acts against the reactors, fuel-reprocessing facilities,
waste repositories, and shipments of radioactive
wastes could result in serious releases of radioactivity.
Moreover, a safeguards system would have to exist on
a vast, worldwide basis. Some 1,000 nuclear reactors
are projected for the United States by the year 2000,
with hundreds of shipments of radioactive materials
daily. Hundreds of tons of plutonium will be in the
commercial sector of our economy by that date.
Abroad, American firms are constructing nuclear
reactors in countries that have little political stability
and in others, such as Japan, that have not signed the
nonproliferation treaty. Safeguarding nuclear bomb
material would ultimately require a restructuring of
sociopolitical institutions on a worldwide scale. The
record of the United Nations unfortunately gives us
little reason to believe that this is a practical reality.
Second, safeguards are strongly opposed by the
nuclear industry. The degree to which the industry is
sensitive to the hazards of theft, and likely to be an
effective partner in the enforcement and
implementation of safeguards programs; was apparent
in its vociferous opposition to the modest
strengthening of AEC safeguards, which was recently
adopted.
Third, experience with present safeguards does not
inspire confidence. Over several years of operation, the
Nuclear Materials and Equipment Corporation was
unable to account for 6 percent (100 kilograms) of the
weapons-grade material it handled and, as already
noted, was recently fined by the AEC, partly because
of safeguards violations. At a recent safeguards
symposium the director of the AEC's Office of
Safeguards and Materials Management observed that
"we have a long way to go to get into that happy land
where one can measure scrap effluents, products,
inputs, and discards to a I percent accuracy." This
statement takes on particular significance when we
realize that only 0.5 percent of the plutonium utilized
by the commercial sector in the year 2000 would be
enough to make hundreds of atomic bombs. The
editors of the Bulletin of the Atomic Scientists have
noted that the frequent misrouting of shipments of
weapons-grade material highlights a key safeguards
problem:""hijacking. A spot check by investigators
from the General Accounting Office at three AEC-
licensed contractors showed that in some cases access
to easily portable quantities of special nuclear material
could be gained in less lhan a minute using the
simplest of tools. At two of the three plants checked.
the General Accounting Oflice found weak physical
barriers, inelfective guard patrols, ineffective alarm
systems. Lick of automatic detection devices, and the
absence of an "action plan" should material be stolen
-------
or diverted. In contrast, the AEC's inspectors gave the
same facilities good marks in virtually every security
category.
Fourth, even if an effort is made to improve current
safeguards, there is little reason to believe that the new
system will operate with the virtual perfection that is
essential. For example, the AEC supports the creation
of a special federal police force to provide an
immediate federal presence whenever the use offeree
may be needed to protect these incredibly dangerous
materials from falling into the hands of would-be
saboteurs and blackmailers. But is it plausible to
believe that police would be effective at a level
commensurate with the potential nuclear hazard? The
New York City police department has shown itself
incapable of maintaining security over confiscated
heroin. Are similar losses of plutonium acceptable?
The point is that our safeguards system must be
essentially infallible; it must maintain what Alvin
Weinberg, former director of the Oak Ridge National
Laboratory, has called "unaccustomed vigilance" and
"a continuing tradition of meticulous attention to
detail." Yet our human institutions are far from
infallible. Our experience indicates that rather than
sustaining a high degree of esprit, vigilance, and
meticulous attention to detail, our governmental
bureaucracies instead become careless, rigid,
defensive, and sometimes, corrupt. A basic question
then is whether we want to entrust so demanding and
unrelenting a technology as plutonium recycle to
institutions that are often negligent of their own
responsibilities and insensitive to the rights of others.
A final reason for believing that an adequate
safeguards system would not be acceptable in practice
is the tremendous social cost of such a system in terms
of human freedom and privacy. Safeguards
necessarily involve a large expansion of police powers.
To deal with the terrorist threat, the AEC is
considering surrounding us with what it calls a new
"federal security system." In its draft environmental
impact statement, the AEC decries court rulings
"favorable to the protection of individual privacy" and
calls for legislation to authorize expanded
"background checks" and to create a federal
plutonium police force. The plutonium police would
meddle with our civil liberties on a vast scale.
Surveillance would inevitably cover not only the
millions seeking jobs in the plutonium economy but
also those close to the job seekers and those in allied
occupations.
The commercialization of plutonium will bring with
it a major escalation of the risks now associated with
nuclear power-risks that many already believe to be
too great. And plutonium will further strain the
weakened regulatory fabric of the nuclear industry.
Hannes Alfven, Nobel Laureate in Physics, has
described the regulatory imperatives applicable to the
nuclear industry in an article in the Bulletin of the
Atomic Scientists:
Fission energy is safe only if a number of critical
devices work as they should, if a number of people
in key positions follow all their instructions, if there
is no sabotage, no hijacking of the transports, if no
reactor fuel processing plant or reprocessing plant
or repository anywhere in the world is situated in a
82
region of riots or guerilla activity, and no revolution
or war-even a "conventional one"-takes place in 5 7 5
these regions. The enormous quantities of extremely '
dangerous material must not get into the hands of
ignorant people or desperadoes. No acts of God can
be permitted.
Writing in Science magazine, Alvin Weinberg
suggests that "what is required is a cadre that, from
now on, can be counted upon to understand nuclear
technology, to control it, to prevent accidents, to
prevent diversion" of plutonium to nonpeaceful
purposes. The public and its decision makers must
seriously question whether it will be possible to attract,
train, and motivate the personnel required for these
functions. These would have to be highly qualified
persons able to maintain a tradition of "meticulous
attention to detail" even when the glamorous aspects
of a new technology become the commonplace
operations of an established industry. We suggest that
it is beyond human capability to develop such highly
qualified groups generation after generation:
There is a sizable body of evidence at th'e present
time to suggest that the fledgling nuclear industry is
already unmanageable. Consider, for example, that
115,000 gallons of high-level radioactive wastes
recently leaked from the tank at the AEC's reservation
at Hanford, Washington, over a period of fifty-one
days while no one monitored the tank. Radioactive
releases from the Shippingport, Pennsylvania, reactor
were higher than recorded. Executives of Consumers
Power Corporation, a utility company in the Lake
Michigan area, failed to notify the AEC that their
radioactive gas holdup system was not functioning.
Two reactors were half-completed before the AEC was
informed that they were being constructed over an
earthquake fault. The General Accounting Office
found the security at plutonium storage areas totally
inadequate after AEC inspectors had certified the
facilities. Finally, one of the AEC's leading reactor
safety experts recently quit in protest, stating that he
was going to work with Ralph Nader and the Union of '
Concerned Scientists because the AEC has misled the
public about the safety of nuclear reactors.
In view of this spotty record and considering the
extreme toxicity of plutonium and the major
difficulties of safeguarding it from theft, we believe
that a decision at this time to proceed with plutonium
recycle will escalate an already unmanageable
situation to the crisis level.
An opportunity for a review of the decision has
fortuitously appeared. In October of last year,
President Ford signed a bill that splits the Atomic ':
Energy Commission into two new agencies-one to j
regulate the nuclear industry, the other to develop |
energy technologies-both nuclear and nonnuclear. !
Critics of the AEC, which combined both functions '
under one roof, had long requested the government to
take that action. The new regulatory agency is the '>
Nuclear Regulatory Commission; the new promo-
tional authority is the Energy Research and
Development Administration. We cannot urge too
strongly that upon assumption of office, the heads of
both agencies take an independent and searching new
look at the plutonium question before we start on such
a risky and irrevocable course as plutonium recycle, fj
-------
576
R.R. 1
Carlock, II. 61725
6 January 1975
Roger Strelow, Asst. Adm. for Air and Waste Mngt.
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, D.C. 20460
Dear Mr. Strelow:
I would like a transcript of the hearing and documents con-
cerning Plutonium and Transuranium Elements.
In addition, I would like to comment that any plutonium
produced is too much. Our radiation storage facilities have
already proven to be inadequate (refer to Hanford, Wash.)
plus incidents at on sight escapes to the environment have
been recorded (refer to Miami R. in Ohio). Now I read that •
Plutomium is missing at a production unit of the Kerr-KcGee
Corporation in Crescent?, Ok.. (Wall Street Journal, 30 Dec.
197^).
Plutonium is among the most hazardous materials (potentially)
known to man. Uhcompoaraiizing and only nothing short of per-
fect storage procedures must be devised which must last more
than 500,000 years (approximately 20 half-lives). Human erroe,
intentional sabotage plus unpredictable climatic and seismotic
changes are too prevalent to take the risk of massive Pluto-
nium production for this great period of time. I believe the
breeder reactor and plutonium production programs should cease
immediately/ and direct our energjr efforts toward perfecting
solar power and deuterium fusion techniques.
David N. Paddock
-------
Si.
-------
578
-------
579
JUDITH C. FRIEI MAN
— Lawton Road ~
Canton, Connecticut 06019
(X0») 693-4377
"(*" * f * r *
• .
~ ;/ *
CLSTHs
,
-------
580
» ,8
, G^M^^A^^^^
' .. :•.;. -'\ V •:'«#'#
• '--'. 'ty**ffis$.
iiri sist^illis^i^ffi
-------
581
ELOISE W. KAILIN, M. D.
RTE. 1 BOX 253
SEQUIM, WASHINGTON 98382
AREA CODE 2O6
TELEPHONE 683-6644
DIPLOMATS. AM. BD. OP
ALLERGY AND IMMUNOLOGY
UJ*~r Mr: killtfi
V^J-
TXor
I*.
-------
Dr. William A. Mills
Director of Criteria and Standards Division (AW-560)
Office of Radiation Program
EPA
Washington, D.C. 20460
January 10, 1975
Dear Dr. Mills:
I am writing to express my protest to the use of
atomic reactors as a source of energy—plutonium being
the deadly by-product of these reactors.
I have read a great deal of material on the subject,
and feel the warnings made by authorities and scientists
alike, warrant the immediate halting of further work and/
or development on these reactors.
I am thoroughly disgusted with the people at the AEG,
who know of these reactors' potential danger, and yet,
refuse to believe the warnings of experts, preferring to
sit on their hands instead.
These people are supposed to be working for us, and
not against us. I believe the people at AEG are not
earning their keep. They should ;\>e thrown out of their
positions on their ears...unless they begin to take into
account the safety of people and the future of the world,
which is what they were hired to do.
It appears these people at AEG have run amuck and
are under the illusion they are all-knowing and all-powerful,
Need they be reminded they are working for the people of
this country and that we1 are to be given the last wort on
what type of energy we will have? This one government agency
is not to have the power of decision when there are so many
risks involved.
Perhaps the AEG has not heard, that there are several
safe sources of energy available to us-—solar, wind, ocean,
and geothermal to name a few. '
If the AEG does not mind, I have made plans and am
striving for a career. I would greatly appreciate having
the opportunity to fulfill my hopes and live to a ripe old
age—without the deadly danger of atomic reactors jeopor-.
dizing or thwarting my efforts.
-------
Dr\ JWilliam_A^ Mills
583 "Page" 2 "
January 10, 1975
Based on authoratative advice, stating that the use of
atomic reactors could only mean further destruction of life
in our already problem-riddled world, I demand that another
source of energy be researched and used, so I and everyone
else can live full lives.
./
For a change of pace, why don't the people serving us
use a bit of foresight instead of the hindsight they are so
very famous for?
Sincerely,
JAJ^7
Theresa Ursulskis
-------
UNIVERSITY OF COLORADO 584
BOULDER. COLORADO SO3O2
AREA CODE 3O3
443-2211. EXT. 8427
January 13, 1975
W. D. Rowe
Criteria and Standards Division
Office of Radiation Programs (AW-560)
U.S. Environmental Protection Agency
401 M Street, S.W.
Washington, B.C. 20460
Dear Sirs,
I am submitting the enclosed report as part of written test-
imony for the EPA hearings on radiation standards held recently in
Denver. It is an example of citizen research, one might say, since
it was done by students at the University of Colorado. It reflects a
growing concern on the part of Denver area citizens that the region
be adequately protected from radiation risks from the Rocky Flats plant.
It may be that current standards are strict enough. I believe,
however, that the EPA should be supportive of efforts of citizens to
protect themselves through citizen inquiry, research and action. Any
governmental organization such as the Atomic Energy Commission (AEG)
should have counter-control organizations in the "citizen sector."
Wise decisions are assured through such a checks-and-balance system.
I would hope that the EPA would concern itself with more than
just radiation standards—and would encourage wherever possible citizen
participation in projects that further their knowledge of the risks
involved in nuclear energy development, and alternatives for protecting
the health and welfare of their communities.
Sincerely,
Paul Wehr
Associate Professor
of Sociology
PW/gl
Enclosure
-------
-------
587
i.
This report is the product of the Action Research Group,
one of the several student working parties in the Sociology of Peace-
making course at the University of Colorado. Its research grew out of
two convictions: 1.) that students are capable of and prefer to do social
research on problems that seriously effect them, their society and their
world; and 2.) that students can simultaneously learn the skills of
research and contribute to the amelioration of a significant regional
and global problem.
This research group passed through each phase of the research
design: problem selection, data collection, analysis and interpretation
of results. The group then concerned itself with a fourth phase which
is an essentially equal component of reseuch methodology; the uses to
which its findings are put. Research utilization was a major concern
of the research project and use of this document continues far beyond
the dissolution of the research team.
The group defined the reseach problem as the existence and
potential environmental impact of two war-related government installations
in the Denver-Boulder area. Both the Rocky Mountain Arsenal- a repository
for deadly nerve gas- and the Rocky Flats Plant of the Atomic Energy
Commission have been in recent years charged with contaminating air,
water, and anil, resources in their environs. The Rocky Flats Plant
lias also been' accused ol" possible radiation contamination of its
employees and regional population.
The research team was concerned with what factual data could
be gathered, how it could be used to shed new light on the problem
and with suggesting citizen and decision-maker responsibility for
-------
588
2.
alternatives if the risks to local populations of operating these
installations were as considerable as was charged."
The team was confronted by several inhibiting factors. Since
both chemical and biological warfare (CBW) development and nuclear
weapons are highly secretive operations, factual data on risk factors
from the installations themselves are not readily accessible. Since
those in charge of the installations feel threatened by increased public
concern over their presence, the information provided voluntarily tends
to be highly selective and plays down the potential risk. The public
relations office of any bureaucratic organization, particularly those
with "classified" status, tends not to be the most accurate source of
complete and reliable data.
The limited research period (one academic semester) and the
lack of financial support also inhibited the research. This report,then, is
presented neither as exemplary of objective social scientific research
nor as propaganda. It is, however, a piece of serious research which
should raise the level of public awareness and lead to public debate
and action based on the amount of accurate knowledge available.
HISTORICAL PERSPECTIVE
It might be of some value to briefly describe the historical
and technological contexts which produced both the Rocky Mountain
Arsenal CBW installation and the Rocky Flats nuclear weapons plant.
Rocky Mountain Arsenal (RMA)
RMA is located northeast of Denver in Adams County. Its
southern perimeter is adjacent to 56th Avenue and Stapleton International
Airport, and is 2 miles due north of Fitzsimons Army Hospital.
-------
589
3.
RMA was created at the onset of World War II, its primary
function being the manufacture and storage of chemical munitions. Between
1951 and 1957, RMA manufactured the most lethal component of its
current stockpile, the nerve gas "GB1'.
US Army Field Manual 3-10 describes the effect of this gas:
"Nerve Gas 'GB' Type- Causes muscles to contract.
Breathing stops and death occurs. Paralysis of the
nervous system."
"GB can be employed for immediate casualties in
surprise dosage attack against targets containing
unmasked dug-in troops..."2 (emphasis added)
In addition to inhalation, a lethal dosage of nerve gas can be
inflicted by absorption through the skin, eyes, and intestinal tract.
Failure to suffer immediate death or incapacitation after exposure to
nerve gas does not necessarily suggest immunity. There may be gas-related
and delayed complications. A study by the University of Colorado School
of Medicine conducted under contract to the US Army describes the case of an
RMA employee "who had a very mild exposure to nerve gas" and was
treated at the RMA hospital and released:
"while driving home from work (he) suddenly pulled into a
filling station and called for help. The attendant found him
in a state of shock and called for an ambulance, and was
admitted to the hospital where he died two days later of
coronary thrombosis."-'
Nerve gas disrupts the action of the cholinesterase enzyme, which is
essential to the functioning of the nervous system; the immediate cause
of deatli is usually respiratory or coronary failure.
Although the exact quantity of nerve gas stored at RMA has never
been disclosed, in 1960, Representative Byron Johnson of Colorado told
Congress that there was enough nerve gas stockpiled outside Denver
"to kill every man, woman and child in the world."
-------
590
4.
Some of the nerve gas is in a variety of bombs, rockets and
underground storage tanks; but most of it is in one ton metal cylinders,
clustered in neat rows throughout the Arsenal, above ground, exposed
and unprotected, except against lightning, for which they are electrically
grounded.
Aside from GB gas, RMA also stores over 1,000 tons of obsolete
Q
phosgene gas; and beginning in 1955, Shell Chemical Company contracted
to manufacture commercial toxins at RMA, some with a similar chemical
9
structure to nerve gas. The Shell Pe-st Strip which hangs in many
American homes is one commercial product from this plant.
Groundwater Contamination. Liquid wastes and contaminated water from
the manufacturing process were disposed of in artificial lakes on
RMA grounds. Toxins filtered downward, polluting underground water
supplies which eventually spread beyond the perimeter of the RMA, a
fact which did not become public until 1959.
From 1951, the first year of GB production, farmers in the RMA
area complained of contaminated underground water supplies which caused
crop failures and livestock deaths. Although suspicion was directed
toward RMA, the nearest and most obvious source of contamination, RMA
officials maintained tliat the source of the problem lay somewhere else.
In 1955, howc'vur, ihu HMA Installed an asphalt-lined waste disposal pit,
which prevented further contamination but could not correct that which
had occured previously, and which became a serious problem calling
forth.public outcry in 1959.
In June of 1959, the Denver Post reported: "...livestock has
died and thousands of acres of crops have been destroyed."
-------
591
5.
Representative Byron Johnson wrote to the Secretary of Defense:
"Already farms have been destroyed and the water supply serving more
12
than 15,000 citizens is presently endangered." The Post noted that
the natural course of the groundwater flow from the RMA was toward
the contaminated area, but RMA officials made no comment.
In November of 1959, it was discovered that as early as 1954
the Army Chemical Corps began secret investigations in Adams County
on the possibility that RMA wastes were contaminating underground water.
At no time were the residents or the county health officials told that
waste's from GB-type nerve gas might be threatening their water supply.
When Army investigators who tested wells were asked the reason for
testing they answered, " It's just routine" or "You'll be told later"
14
or they refused comment. Earlier, in 1957, the commanding officer
of the RMA, Col. Ronald Martin, answered an inquiry from the Adams
County supervisor of the Tri-County Health Department by saying the
tests were secret but "there is nothing to worry about."
In November of 1959, the United State Public Health Service,
after conducting its own tests, concluded that RMA was directly
responsible for the contamination. The Chemical Corps commented that
their own years of testing were "inconclusive" Yet the following day
The Denver Post revealed that in 1956, the United States Geological
Survey had submitted a report to the Chemical Corps which concluded
that groundwater in the RMA area was "unsuitable for irrigation of
crops" and warned that " the effects may become serious." In addition,
The Post revealed the exsistence of a report by the University of
Colorado, rude on coniract with the Army between 1956 and 1959 which
concluded that herbicides manufactured at RMA were present in shallow
-------
592
wells near the RMA and that: 6-
"it is quite likely that moving water from the original
source of contamination will continue to carry toxic
materials ... for years to come and that soil to which
contaminated irrigation water has been applied will
produce poor crops for a number of years.
Furthermore, it may be expected that the
front of toxic materials in the groundwater will continue
to move toward the Northwest until the Platte River
is reached; at which point groundwater migration will
then carry the materials Northeastward down the valley."^
Both reports were classified and withheld from the public by the Army
until public pressure forced their disclosure; thereafter, a third
report, issued by the Army, suggested that a "Phyotoxicant has been
introduced into the groundwater from GB (nerve gas) plant wastes commencing
in 1953.
,,19
After all the disclosures of 1959, the chief of the Army Chemical
Corps, Major General Marshall Stubbs, was asked why residents had not
been warned of the possibility of contamination of their underground
water supplies. The Denver Post reported his answer:
"The residents were not informed because the
Chemical Corps was not aware of the probability that
their domestic water supply was seriously contaminated."20
Waterfowl Deaths_: In June of 1959, The Post commented;
"The_ Denver Post has carried stories about the mysterious
death of wild ducks that land on the 40 acre lake used
by the arsenal as a filtration pond."2l
And in November of 1959, in ;in aside Lo a story on water
pollution from KMA wastes,The Denver Post noted that the United States
Fish, and Wildlife Service had been conducting studies in the RMA vicinity
and had concluded that RMA liquid wastes were responsible for the
22
death of waterfowl in the area. This revelation failed to elicit
much public concern and was followed by intermittent news stories
-------
593
7.
over the years. In January 1963, the RMA commander, Col. Charles
McNary voiced objection to the publicity over the deaths of about 2,000
wildfowl per year due to dieldrin, a Shell Chemical Company toxin:
"I wouldn't say there isn't something in the
lakes that's harmful to ducks. But ducks can pick
up the insecticide on a farm where crops have been
sprayed, for example.
Shell and other companies are making chemicals __
that go all over the world. Someone has to make them."
Earthquakes. Beginning in 1962, a series of earthquakes occurred in
Northeast Denver, in the vicinity of the RMA. Some geologists suggested
that their cause was the operation of the RMA's newly^installed 12,000-
foot waste disposal well, into which liquid wastes were pressure-injected.
In November of 1965, the RMA commander said the well could not be
r\ I
blamed, but in December of 1966, after a panel of geologists concluded
that the pumping of wastes into the well lubricated the Derby Fault under
25
the RMA, causing earthquakes, its use was suspended.
At present, wastes produced at the RMA are transported to
9 f\
Nevada for disposal. More recently efforts to gain permission to
dump wastes in deep wells south of Denver were rejected by public
agencies.
Detoxification. At present, detoxification of all nerve gas and detox-
ification or removal of all phosgene gas at RMA is underway. The
projected completion date by the Army is late 1976 or 1977. Disposal
oi" some 21, 224 M-34 cluster bombs began October 26, 1973, after
Congress approved LIU environmental impact statement.
On November 9,1973, during detoxification, a borablet containing
GB, in an M-34 bomb exploded at 10:30 am. Public announcement of the
accident was made at 2:30 pm. The bomb was the 60th to undergo
27
detoxification.
-------
594
The actual impact on humans and other populations of RMA and
its nerve gas production and storage was a constant focus of debate
and study through the 1960's. Following are several accounts of the
environmental dangers which have already occurred. Additional accounts
are included in the appendix of this report. All quotes are from
the Denver Post, except where indicated.
June 14, 1959:
"Cattle Deaths, Ruined Crops Linked to Arsenal Chemicals"
"...some livestock has died and thousands of acres of crops
have been destroyed."
Representative Byron Johnson wrote to the Secretary of Defense:
"Already farms have been destroyed and the water supply serving more
than 15,000 citizens is presently endangered." Johnson said the contam-
ination north of the Arsenal was noted more than six years ago as covering
a strip of land about five miles long and almost two miles wide.
"There have been repeated attempts," he said,"to get a satisfactory
answer from the government."
April 26, 1964:
"Poison-Loaded Arsenal Lakes Kill Hundreds of Waterfowl."
"In 1959, the Bureau of Sport, Fisheries and Wildlife reported
that a Shell employee had been assigned the task of periodically
gathering dead ducks and burying them."
"Heavy waterfowl losses have been occurring on the lakes since
1951, and reports have listed bird deaths as 2,000 a year."
December 13, 1966:
Use of the deep disposal well was suspended after a connection
was established by geologists between pumping of wastes and Denver
area earthquakes.
Rocky Flats Atomic Energy Plant (RF)
Rocky Flats is located about 16 miles northwest of Denver and
six miles sotheaat of Boulder in Jefferson County. The facility,
completed in 1953, and employing 3,200 persons, is operated by the Dow
Chemical Company under contract with the Atomic Energy Commission.28
Plans to construct the Rocky Flats plant were announced by the United
States Atomic Energy Commission on March 23, 1951. There was no
citizen involvement in the decision to locate the plant. In 1953, the
initial construction of Rocky Flats was completed at a cost of
-------
595
9.
approximately $44 million. Geographically, the rocky cow pasture 16
miles northwest of Denver was chosen as the site because it was close
by Colorado University, skilled manpower in Denver and attractive
recreational opportunities in the mountains. The selected area was
also noted to be very adaptable for the stringent security procedures
that the plant demanded.
The primary function of Rocky Flats is the production and
manufacture of trigger mechanisms, which utilize radioactive plutonium,
for thermonuclear weapons.
Plutonium is one of the most highly toxic substances known, and
minute quantities of it inhaled or imbedded within the body can be
lethal. Its radiation can cause permanent celluar damage leading to
cancer, and the fact that plutonium oxidizes quickly makes it a serious
29
fire threat.
The refining process of plutonium and the resultant waste
material has resulted in the contamination of RF and the surrounding
area, despite elaborate safety precautions. Over 200 small fires
have occurred at Rocky Flats, and in May 1969, a $50 million fire in
two assembly buildings destroyed enough plutonium to build 77 Nagasaki-
type bombs, although radioactive particles in the smoke were supposedly
Crapped by a special tilt ration system.
Consequences for the external environment, should a fire
fail to be contained, would be tragic. A study in inhalation exposure
to plutonium at RF published in Health Physics describes the effects
of a small fire confined to a plutonium production area:
"Even though the fire was extinguished within a few
minutes, airborne contamination spread quickly
throughout the area. Air sampler filters indicated an
activity...at the remote areas."31
-------
596
10.
At this time it is uncertain what level of contamination of the
region, if any, has developed over the past years .from accidents and
strong winds. The environment, with certainty, has been contaminated
through accidental wastage spills. In one case, a tank of contaminated
oil being moved for disposal developed a leak, spilling oil over a
mile length of the road. The decision was made to pave over the
contaminated area with asphalt, which has a half-life far less than the
24,000 years of plutonium. When the paving wears away, then the
radioactive material will again be exposed.
Normal procedure at RF had been to seal radioactive wastes
in metal containers and bury them. Container leaks developed,
contaminating surrounding water and soil. If disturbed, radioactive
particles in the soil could become airborne, posing a threat to
nearby populations. Today, no radioactive wastes are buried on the
site; the plutonium and other radioactive waste that cannot be recovered
32
in the plant's recovery facility is shipped to Idaho Falls, Idaho.
Several things come through in an analysis of the development
of both RMA and RF:
1) There has been no citizen participation in any of
the decisions locating these installations or concerning
any policies affecting their impact on the regional community.
2) Some si'.rlous doubts luwe been raised in the public
mind about the existence or effectiveness of safeguards
which would prevent the contamination of populations
and environment.
3) Evidence of injurious effects upon local populations
and/or their natural resources does now exist and the
RMA and RF authorities with direct responsibility have
-------
597
ii.
concealed or attempted to minimize the importance of
that evidence. Bill Colston, the ^Atomic Energy Commission's
plant manager, in an interview concerning the federal
agency's championing of the pvblic's right to know
attitude stated:"They didn't care about the public.
They didn't believe the public had any right to know."
POTENTIAL CURRENT and FUTURE RISKS to LOCAL POPULATIONS
While history helps us understand how these installations developed,
their past effect on local population and environment, and how their
latent conflict of interests with local populations became manifest,
it tells us little about the level of current and future risk, if any,
these installations pose for the people of the area. As was mentioned
earlier in this report, the Rocky Mountain Arsenal is located adjacent
to Stapleton International Airport. A heavy fog, a light snow, or
perhaps a pilot's misjudgement could each set the stage for disaster.
Scenario:
It is 5:30 pm, a weekday. A fully loaded DC-10, one of 300
flights daily at Stapleton International Airport, attempts to land;
it crashes into a neat row of exposed, unprotected one ton nerve gas
containers two miles west of the perimeter adjacent to RMA.
Several tons of the nerve gas"GB" are released from the ruptured
containers. A subsequent explosion in the nearly empty fuel tanks of
the DC-10 has the same effect as a bomb of the type used to deliver
the nerve gas: detonation causes the gas to form a toxic cloud; there
is little fire to incinerate the gas.
A moderate 20 mph northerly wind causes the cloud of gas to
drift across the RMA south perimeter within 6 minutes. All the
passengers who survived the initial crash are now dead. RMA personnel
begin to die, some don protective clothing and masks, and medical
treatment is fairly efficient.
The cloud crosses Interstate-70 within 12 minutes, and motorists
begin to die; traffic comes to a halt and will hinder emergency
personnel when they are able to respond.
Ironically, the two hospitals best equipped to treat nerve gas
victims—RMA hospital and Fitzsincns Army Hospital— are closest to
spreading contamination. Hospital personnel and patients begin to die
within 18 minutes, but the gas cannot penetrate every corridor and room,
and many are spared. Panic breaks out; some personnel are aware that
supplies of the antidote atropine, and gas masks, are stored somewhere,
but few know where. Some personnel who don masks and administer aid
in the contaminated wards begin to absorb the gas through the skin.
-------
598
12.
Not all will die. Of those who receive a less-than-lethal dosage,
some will recover entirely, others will suffer brain damage, paralysis.
People begin to die at Stapleton Airport; •maintenance crews
on the tarmac die first, then passengers in the terminal complex. In
the surrounding residential area people also die, but they are less
vulnerable, small houses have even smaller openings for gas penetration,
and the gas is beginning to dissipate.
There are the usual accidents attendant to any disaster: fires,
explosions, and motor vehicle collisions.
After no more than half an hour, the toxic cloud dissipates
entirely. No one south of Coifax Avenue dies—6 miles from the point
of origin. Most of Denver still does not realize what has happened.
Even though, the densely populated areas of the city have been
spared, perhaps 50,000 are reported to have died. Emergency personnel
have been slow to react, there are only 5,000 doses of atropine at
Fitzsimons Hospital, and this is insufficient. Most of the affected
people are by this time dead. The majority of casualties are those
in the open; the highest proportion of death is, characteristically,
among the very young, the very old and the physically weak.
With three hundred take-offs over the arsenal daily, an event
such as the scenario describes is not impossible. Should such an
accident actually happen, what might be the consequences for Metro-
Denver residents? Since use of the nerve gas against humans has yet
to be verified beyond doubt, it is difficult to describe the exact
effects on humans. Extensive testing has been done however with
lower animals and we have a quite sufficient estimate of its potential
consequences for the human biosystem.
The Rocky Mountain Arsenal stores three types of gases: two
types of nerve gas, "VX" and "GB" and one other type of lethal agent,
mustard gas. Both of the nerve gases in their normal physical state
are a colorless liquid. In their disseminated form the "GB" type is
a vapor liquid and the 'VX" type is a liquid aerusol. Although the
nerve gases are usually used as harassing(small dose) or lethal(Iarge
dose) agents, they are also quick-kill agents of tremendous potency.
-------
599
13.
The onset of symptoms occurs up to ten minutes following inhalation,
or up to a half hour following percutaneous absorption. The overall results
of the two nerve gases are as follows:
NERVE GAS TYPE "GB"
Causes muscles to contract, breathing stops and death occurs.
Paralysis of the nervous system.
NERVE GAS TYPE "VX"
Causes muscles to contract, breathing stops and death occurs.
Much greater absorption through the eyes than the skin.
Paralysis of the nervous system.
Stephen Rose's book, Chemical-Biological Warfare relates how
nerve gas operations incapacitate an individual.
Nerve gases are anti-cholinesterase agents, working by
blocking the enzyme which the body uses to destroy one of its chemical
nerve signals transmitters after it has done the job. This has
two effects. One is that control is lost over the affected part
of the nervous system. The other is that a large concentration
of the chemical transmitter builds up in the body and that the
chemical itself is a powerful poison. The body is at first
incapacitated, and then forced to poison itself.
The symptoms of nerve gas poison are diverse and spectacular.
In a comparitively inactive man an exposure to "GB" of 15 mg-min/m3
dims the vision, the eyes hurt and become hard to focus. This
may last for a week or so. At 40 mg-min/m3, the chest feels tight,
breathing is difficult, and there is coughing, nausea, drooling,
heartburn and a twitching of the muscles. At 55 mg-min/m3, there
is a strangling tightness and aching of the chest, vomiting,
cramps, tremors and involuntary defecation or urination. At 70
mg-min/m , severe convulsions will set in followed closely by
collapse, paraysis, and death.
Mustard gas is also stored at the Rocky Mountain Arsenal. In its
normal physical state, mustard gas is a colorless-to-amber oily liquid, and
in its disseminated form it can be either a vapor liquid or an aerosol.
The symptoms of intoxication are:
HARASSING
Eyes: inflamation, photophobis, ulceration and blindness.
LETHAL
Coughing, retching, frothing at the mouth, asphyxia and
pneumonia.
-------
600
14.
This agent injures every type of body tissue with which it comes
into contact. The principal targets are the skin and the eyes which it
burns and blisters. Because mustard gas is not a very volatile substance,
it persists in the field for long periods and can be effective for days or
even weeks after dissemination. It was used briefly in World War I and killed
and blinded a number of combatants and perhaps civilians.
Preparedness. Should an air crash, a fire, an explosion, or some
other unforeseen incident cause the release of nerve gas in Metro-Denver,
how prepared would authorities and citizens be to respond effectively
to the disaster?
The State Health Department informed us that Jefferson, Boulder and
Denver counties have no immediate nerve gas contamination contingency plans
the only ones being state-developed.» In interviews with staff personnel at
specific health facilities the following questions were asked;
1. What are your contingency plans for a possible nerve gas leak?
2. How many people are trained to attend such an accident and
how many can be treated?
3. Are there any decontaminants or antidotes available?
4. Will future generations be affected by any leaks?
A registered nurse who heads the emergency room at Boulder Memorial
Hospital responded to the- questions by sayinj' that: i I: such an accident
occurred, the hospital would be able to handle it. Treatment for the
nerve gas poisoning, according to her, would involve washing the affected
area with soap and water and hoping Cor the best. Dr. Johnson of the Jefferson
County Health Department replied to the- questions by saying that plans for
* Interview with Mr. Montgomery, State Health Department.
-------
601
15.
treatment aren't practical since a person exposed to nerve gas would
die anywhere from a few seconds to a minute after exposure.
Still more variety in official opinion among those responsible was
reflected in interviews with Dr. Morris Gaon, a physician at the Rocky
Mountain Arsenal, and Mr. Arthur Whitney, the public information officer
at the Arsenal, who were questioned concerning the medical treatment of nerve
gas exposure. Dr. Gaon stated that nerve gas exposure is treated with
artificial respiration and atropine. Although he has treated more than 200
cases of nerve gas exposure, he declined to give the exact number for"reasons
of security.
At the Army's Fitzsimons Hospital, Lt. Chafy, the public information
officer, is the only person authorized to provide information on Fitzsimon's
role in emergency contingency plans. The hospital has facilities to treat
1,600 people in an emergency and will treat civilian casualties. They have
5,000 doses of atropine in stock to treat nerve gas victims and there are
200 doctors, 300 nurses and 500 enlisted men trained in atropine injection.
Col. William Allen of Denver's Emergency Preparedness Office was
interviewed about emergency plans for the city and the county of Denver.
Allen remarked that any nerve gas from the Rocky Mountain Arsenal would
have to be atomized by an explosion to be carried by winds and thus pose
a serious threat to Denver. Since nerve gas is extremely heavy, according
to Allen, if there were no explosion, the gas would remain concentrated
on the ground. Furthermore, Allen noted that in order for the gas to roach
Denver there would have to be northerly winds instead of the usual
southwesterlies. Allen stated that the gas would have to travel two miles
-------
602
16.
to reach Denver and would most likely be too diluted by then to cause
«
any harm.
According to Allen, gas masks are the only reliable protection
against nerve gas exposure. He felt it improbable that the entire
population of Denver would purchase or possess such masks. Since they
are made to fit adult males, they would be useless for women or children.
Inspite of his belief that Denver would probably never face a
nerve gas contamination problem. Allen did explain what emergency procedures
would be initiated in case of a nerve gas emergency.
a. The arsenal commander would contact the Denver Emergency
Preparedness Office and then the local media concerning the
impending disaster.
b. Citizens would be instructed to: l)find a place of safety
inside their homes or other buildings;2) close all windows and
doors and shut off all air-circulation and air-conditioning
equipment.
c. The fire department will move casualties to either Fitzsimions
or the Arsenal Hospital.
After interviewing the various departments and organizations directly
responsible for executing contingency plans in the case of a nerve gas
emergency in the Denver area, one could hardly feel reassured that everything
possible would be done expediently and efficiently. On the contrary, most
offices which would handle such a crisis,( The Denver Emergency Preparedness
office being an exception), were. Lotally unprepared for any nerve gas
disaster. The Adams County Civil Defense office Denver General Hospital,
and Jefferson, Boulder and Denver County authorities have no immediate
contingency plans for nerve gas contamination. Many of the offices contacted
refused to release the requested information stating that it was ''classified."
-------
803
17.
The Colorado Civil Defense Office was unable to present a contingency
plan because they didn't know whether the Rocky Mountain Arsenal was
in Denver or Adams County. (The arsenal is located in Adams County.)
What is perhaps even more disturbing is the lack of consistency of professional
opinions concerning the medical treatment of the nerve gas victims. Prescribed
treatment ranged from the simple washing of the affected parts of the body
with soap and water, to a resignation that death is inevitable and
treatment useless. Information on antidotes to treat nerve gas exposure
also differed from source to source. Dr. Gaon of RMA stated that the drug
pentamethonium and oximes were not used in nerve gas treatment while Lt.
Chafy at the Fitzsimmons Army Hospital said pantamethonium was indeed used,
although oximes were not. In contradiction to both their views is a United
f)i
Nations report which recommends the use of oximes for nerve gas exposure.
The United Nations Report also contradicts Dr. Gaon, Lt. Chafy, and Col.
Allen on the effectiveness of gas masks. According to the report, nerve
gas can be absorbed by the skin, the eyes and intestinal tract. Gas masks
then would provide insufficient protection.
Radioactive Contamination. Acute and rapid contamination of populations
and environment by radioactive material is a constant possibility at the
Rocky Flats plant. No scenario here is necessary to suggest the risk. A
serious accident has already occurred at Rocky Flats in 1969, the immediate
and long-term effects of which are still not publicly known. Should a
similar or more serious fire or explosion occur in the future, the resulting
oxidized plutonium could be spread over wide areas, depending on wind
conditions and other meteorological factors.
Since the city of Denver is sixteen miles downwind from Rocky Flats,
-------
604
18.
if a prevailing south-west wind was blowing and oxidizing plutonium
happened to leak from the plant, radioactive material would be blown
across highly populated areas such as Westminster, Arvada, Broomfield
and Central Denver. A worker who has been at Rocky Flats since the
plant first opened created his own scenario about what would occur
if the right wind conditions coupled with a plutonium leak should ever
materialize.
"... if some plutonium smoke leaked out we'd call all of the
police agencies, tell them which way the smoke was going and tell
them to move everybody out of its path. Afterwards, decontamination
teams would have to scrape all the plutonium off everyones'
roofs. It would take months! Then we'd have to bring all
the people and put them through our one body counter (designed
to measure radiation). It would be a hell of a mess."
Most of the immediate effects of a plutonium leak would be
experienced by the employees at Rocky Flats. In addition to serious
radiation burns, if particles of plutonium happened to enter a wound,
amputation of the limb would probably be necessary. Particles of
plutonium, breathed into the lungs, can result in death from radiation
contamination. So far there has been one known contamination death
at Rocky Flats.
In comparison with the inadequate plans that most Civil Defense
offices would employ if faced with a nerve gas crisis many of these
same ol'ficus have- relatively well-organized contingency plans for
an emergency involving Rocky Flats. According to a spokesman from
the Colorado Civil Defense Office, each city and county is responsible
for their own contingency plans in an emergency. The Jefferson County
law enforcement agencies have many responsibilities in the Civil Defense
-------
605
19.
plan. The officers have received training and carry instructions
on the procedures they are to follow if a crisis should occur. The
agencies will also help monitor contaminated and suspected contaminated
areas. The police departments will be responsible for evacuating
rural areas.
According to the Jeffco Civil Defense, if the plutonium radiation
were blown into a populated area, the people in the affected area
would be told to stay in their homes, wait for the wind to die down, and
then wash the radioactive dust off their home.
Dr. Johnston of the Jefferson County Health Department stated
that in the case of such an emergency the department would close
off the contaminated areas, organize decontamination centers staffed by
local physicians, and would monitor the affected population for the long
range effects of plutonium exposure. It would also impound all water
downstream from the contaminated area. Dr. Johnston felt that the
health department's most positive action would be in organizing local
physicians in the decontamination centers and in providing emergency
transportation for casualties.
Dave Berford of the Boulder County Civil Defense, Emergency,
Preparedness Office explained Boulder's well-organized contingency
plans. Berford pointed out that if an accident involving plutonium
occurs at Rocky Flats, only alpha particles will be released. Since
alpha rays cannot penetrate skin, the major danger of exposure to the
Plutonium will come from inhalation, exposure through an open wound,
or eating contaminated food.
Unlike the Arsenal, the Rocky Flats plant is a crucial link
-------
606
20.
in a chain of emergency communications. If there is a major accident
at RF, that would jeopardize the population of Jefiferson County, the
plant is supposed to immediately contact Jeffco Civil Defense which
in turn will contact the Atomic Energy Commission. Rocky Flats is
also responsible for notifying the State Department of Health, the
State Office of Military Affairs, the Boulder Police, the Boulder
Emergency Breparedness Office, the Jefferson County Sheriff's Department,
the Atomic Energy Commission's radiological assistance team, and any
other affected county. After a major accident, Rocky Flats will make
the first press release. Subsequently, the Boulder County Health Officer
will handle all press releases involving Boulder, which will be forwarded
to the State Emergency Operations Center at Camp George West. Here the
press releases will be coordinated with those from other agencies and
counties in order to minimize confusion.
After word is received of a major accident at Rocky Flats, it
is the respbnsibility of the State Health Department(SHD) to evaluate
the situation and recommend the action to be taken. The SHD will also
determine what areas are to be restricted. These secured areas will
be monitored and the data obtained will be reported to the Boulder County
Health Officer.
Both Lutheran and St. Anthony's Hospitals, in addition to other
local hospitals, stated they are prepared to handle a radiation emergency.
Although contingency plans for handling an emergency occurring
at Rocky Flats are better organized than those for handling an RMA
accident, much improvement is still necessary to guarantee the safety
-------
607
21.
of all the people within the affected area.
The organization that seems the least prepared to handle an KF
crisis is the Jefferson County Civil Defense. When interviewed about their
contingency plans, its officials stated that warnings to the population
would "probably" be by radio; sirens would not be used becaiise they feel
that the people would not know how to properly react to them. The endangered
population "might be told to go out of the area". The Jeffco CD advises
people caught in a plutonium contaminated area to wash any radioactive dust
off their homes. Although the alpha particles released by the plutonium
cannot penetrate skin, there is danger in the inhalation of the material.
For this reason, nearly all other emergency organizations recommend that
individuals keep as far away as possible from the contaminated area.
Possible Long Term Effects. Long term results of radiation contamination
(i.e. leukemia, other cancer forms, and heredity alterations,)however,
are more debatable and may be ultimately more dangerous than the risk of
accident. The Ford report gives us the latest research findings on this.35
Plutonium, when it burns, becomes an oxide. This oxide is a
source of alpha particles which in turn cause ionizing radiation. When
high speed electrons take negatively-charged electrons from atoms and
leave positively-charged ions, a chain reaction begins, setting electrons in
motion causing still more ionization. Radiation also destroys chemical bonds
between atoms. These processes cause various types of damage to body cells
HI random. Some rt'lln IUTOIIU- uiiahlr to reproduce while other cells are
killed instantaneously. Certain cells are Injured, not destroyed by the
radiation, but when they reproduce, the injury is passed on to the new cells.
-------
608
22.
Although there are over one billion cells in every gram of cells in the
human body, just one cell,injured in the proper way, -can cause cancer or
leukemia. Although the type of injury to a cell which could result in
cancerous growth occurs rarely, the amount of cells that a dose of
radiation affects greatly increases the chance of cancer incidence.-*"
It takes a while for leukemia and other forms of cancer to manifest
themselves. From the time of radiation exposure to the appearance of the
disease, there is an intervening latency period when the victim is unaware
of his or her illness. Although the latency period for leukemia lasts about
five years, other forms of cancer can remain latent for periods of up to
twenty years. Because of this, people may be unaware of the dangerous
effects Rocky Flats operations may be having on them and their families.
Plutonium radiation can also cause an affected individual to pass
damaged chromosomes to his or her unborn offspring. Since it is the
chromosomal structures within the nucleus of the cell that are primarily
affected by ionizing radiation, if persons receive radiation in their
reproductive organs and it resulted in mutated cells, their offspring-
will have every body cell mutated. The possible consequences of this are
not unimaginable; children could be born with many physiological and
genetic disabilities. We may soon have more definitive information on
long lerm effects of exposure to plulonium. The AEC has been ordered to do
a comprehensive health and death study of its plutonium workers before it
moves ahead with plans for breeder reactor development. Rocky Flats
-------
#09
23.
personnel will be the subjects for that study.
****
DECISION-MAKING STRUCTURES
That RMA and RF were located in the Denver- Boulder area and currently
pose a potential risk to regional populations are consequences of decisions
within organizations. The risks created by these decisions can also be
lessened or eliminated by decisions with citizen participation. Such
participation requires citizen knowledge of the decision-making roles
resposible for the current politicies.lt also requires the knowledge
of how they, as citizens might influence decision-making structures to
bring about policy change.
Rocky Mountain Arsenal. The Rocky Mountain Arsenal is controlled
by the United States Army and the Department of Defense. Presently, the
commander of the arsenal is Col. Watson. Orders relayed from top officials
in the Defense Department to Howard H. Callaway, Secretary of the Army,
then^passed down through the Chief of Staff to the United States Materiel
Command. Functions of this command are research, development, product
production, testing, evaluation, storage, maintenance and disposal of
material. The Sixth U.S. Army under the command of Lt. Gen. Richard G.
Stilwell is in charge of the Rocky Mountain and Western forces. The
Rocky Mountain Arsenal is under the jurisdiction of the Sixth U.S. Army .(Appendix
Rocky Flats AEG Plant. As a result of the Atomic Energy Act of
1946, the newly formed United States Atomic Energy Commission took over
the nation's energy program from the Army's Manhattan Engineer District
on January 1, 1947. The Act established the primary mission of the
Commission to be nuclear weapon research, development, testing, production
and stockpile surveillance.
-------
24.
Albuquerque Operations is the name given to one of the eight
operations in the United States organized by the Atomic Energy Commission.
Other operations are located in Chicago, Idaho, Nevada, Oak Ridge, Richland,
San Francisco, and Savannah River.(Appendix B) The Albuquerque
Operations of the AEC employs about 1,280 people, and its annual payroll
is approximately 18 million dollars. Integrated operating contractors
employ approximately 28,660 additional people. Some of these integrated
and support contractors include: The University of California, Western
Electric Company, Dow Chemical U.S.A., Monsanto Research Corporation,
General Electric, Mason and Hanger Silas Mason Co. Inc., The Bendix Corp.,
and the Zia Company. Rocky Flats is an area office of Albuquerque Operations.
We might note here the extensive network of sub-contracting which
spreads the economic impact of AEC operations into local communities. As
with other sectors of the war industry, this wide distribution of contractors
makes it difficult to build public opposition to the Rocky Flats operation
or any other installation. There are always local vested economic interests.
The Rocky Flats Area Office, established July 1, 1952, administers
the contract under which Dow Chemical, U.S.A. operates the Rocky Flats plant.
Although the Rocky Flats Area Office employs only 51 people, Dow Chemical
U.S.A. employs 3,480 people at the plant. The Rocky Flats Plant is a
production facility, handling nuclear materials. Fabrication, manufacturing
design and development, production engineering, and related activities are
performed at the plant.
The Dow Chemical Corporation, which operates RF has six world operations:
the U.S. area, Canada, Europe, Latin America and the Pacific area. (Appendix C)
Another operation called Life Science is primarily responsibile for medical
and technological research. Dow Chemical U.S.A. has several suboperations;
-------
611
25.
there are two in Texas, one each in Michigan, California, Louisiana and
an Eastern division. Rocky Flats is one of these divisions. In addition
to operating its nuclear weapon research and development laboratories,
Dow is a leading manufacturer of such household products as HandiWrap,
DowOven Cleaner, and Saran Wrap.
The decision-making process governing Rocky Flats is as follows;
the manager of Albuquerque Operations, General Donnelly, is administratively
resposible to the General Manager of the Atomic Energy Commission, Robert
E. Hollingsworth. In accomplishing its assigned mission, Albuquerque
Operations receives programmatic directions from various AEG headquarter
divisions. General Donnelly, as manager of the Albuquerque division
relays orders from the AEG to James Hanes, general manager of the Dow
Chemical Corp. at Rocky Flats. Above Hanes is B.W. Colston, manager of
the Rocky Flats area. Colston can appeal orders given to him to General
Donnelly, who can contact the AEG. Hanes, as manager of Dow at Rocky Fiats
can appeal decisions to J.M. Leathers, executive Vice President of all
U.S. Dow divisions. Above Leathers is Earl Barnes, President of the U.S.A.
area operation of Dow Chemical. (Appendix C)
The relationship between government and private industry is part
of the AEC's philosophy to utilize the resources and technical research of
private and industrial firms.
Because of the complex organizational structure of Rocky Flats
and the governmental and military restrictions at the RMA, it is very
difficult for citizens to press those bureaucratic structures for
complete and accurate information. Personnel at these two high-security
-------
612
26.
installations are extremely reluctant to answer any inquiries concerning
long or short term risks that could result from their presence. Most
public inquiries are handled by public relations officials who release
only that information which has already been carefully examined and
screened. For this reason, citizens must look more to sources of
information outside ,the jurisdiction of RF and KMA.
****
CONCLUSIONS
From the evidence it has gathered, the Action Research Group
reached certain conclusions concerning potential hazards posed by RF and RMA
and preparedness to respond adequately tp such hazards.
1. A negative impact from both installations on both the human
population of the area and its natural environment is suggested
by the data. Even if the degree of impact is not measurable(or
has not been revealed) to date, the potential risk is serious
enough to warrant thorough investigation by local and state
authorities and citizen's groups.
There is an interesting linkage between the potential for
disaster at the local and global levels. Denver's predicament
is shared by the world. The two installations posing a clear
and present danger to its limited ecosphere, manufacture and
store the two most awesome weapons in the superpower arsenal,
weapons that pose the same risk for the world1s population as
they do far Coloradans.
2. The disaster reponse and the contingency plans in Metro Denver
and surrounding counties arc totally inadequate given the dimensions
of the potential risk. The capacity of emergency agencies to
protect and care for the largo numbers likely to be affected
is minimal. The public in j',ene rally uninformed about facilities
that do exist and what means of self-protection there are.
Where contingency plans exist within counties and municipalities,
they are poorly coordinated with other plans.
3. The people in-decision-making roles who are responsible
for the cxsistcnce and operation of RMA and RF are not evil
persons, but they do need to respond with candor and action
to public concern and to discard the evasiveness and subterfuge
of the past. They need to be persuaded that the health and
safety of the local populations must come above all else.
-------
613
27.
4. Citizens must learn how to conflict creatively with forces
that may or seem to threaten their present^and future interests.
The commonweal is protected only through various interest groups
(in this case, citizen groups local, and state agencies, and these
installations and the federal and industrial bureaucracies that
operate them) engaging in creative conflict. Citizens must
organize as conflict parties to investigate and challenge and to
protect their health and that of their future generations. The
RMA and RF impact problem is not unlike chat raised by oil
shale development and strip mining. The federal government is
making decisions affecting the lives of Coloradans- who have
minimal participation in those decisions, and who increasingly
question that their best interests are served by the consequences
of those decisions.
Our research has led us to questions as well as conclusions.
1. While a decision has been made to detoxify existing nerve
gas supplies at RMA, the process is not scheduled for completion until
some time in 1976. What is to be done in the interim to minimize the
dangers of air disaster, toxic wastes and the like? By what means can
citizens monitor the disposal process to insure faithful adherence to the
schedule by RMA authorities and those higher in the Defense Department
structure? The public has developed a healthy mistrust, during the past
decade, of governments that misrepresent and manipulate in the "interest
of national security" or some other ambiguously-defined objective.
2.What are the incontrovertible facts regarding the less visible
long-term possibilites of radiation poisoning for populations surrounding
nuclear installations, including nuclear power plants? This question becomes
even more critical as concern over future energy supply pushes the nation
forward toward crash programs in nuclear power plant and breeder reactor
development.
-------
614
28.
POSSIBLE INTERVENTION STRATEGIES
The Action Research Group after completing ..its data-gathering turned
its attention to the question of citizen intervention. If citizens
are concerned about potential health and environmental hazards posed by
the Arsenal and Rocky Flats, how might they intervene creatively? An
analysis of the problem is certainly the place to begin, a process to
which we hope this document contributes. We plan to disseminate it
through several accessible communications networks including the mass
media, public and private educational systems, environmental and other
citizen groups. We would encourage other action groups to do more
thorough research on different dimensions of the problem. Citizen
action might lead in several directions.
1. Pressure for policy change through current state and federal
political representatives, who could intervene at various levels
in the two organizations. Don't expect overnight miraclesl
Very few congressmen are ready to take action on the subject
of nuclear products. It takes time and an understanding of the
problem to change opinions from:
a.) Not interested; "Nuclear plants are safe and clean."
to b.) Concerned; "Maybe there is a danger."
to c.) Determined; "I'll research and gather information."
to d.) Convinced; "Yes there is a danger."(or there is not.)
to e.) Ready for Action; "Its time to convince others."
Most members of Congress are somewhat between stage a. and
b. It is expected that a member of Congress will move from
stage b. to stage c. and d. whenever a significant number of
homo-state voters, groups, experts and newspapers voice their
opinions loudly enough.
2. Influence upon candidates for national, state and local
office. Make it an issue.
-------
615
29.
3. Pressure on local and state officials to investigate contamination
possibilities more thoroughly.
4. Pressure on industrial forms involved. Dow Chemical(Rocky
Flats), Campbell'Soup (Nerve Gas), and Shell Oil (Insecticide
Production at RMA) all have large individual consumer markets
and are sensitive to public atitudes.
5. Develop educational programs in schools and civic associations.
6. Symbolic acts and actual disruption of the contamination
process (eg. civil disobedience, vigils).
It is essential in intervening to bring about change, to have
a reasonably clear set of alternative policy goals to present. In the
intervention in question, the following might be among the conceivable
alternatives.
Rocky Flats.
1. Shifting nuclear operations at Rocky Flats to an unpopulated
area, or conversion of the plant to nonhazardous production. A
shift would have serious shortterm economic consequences for
the immediate area that would have to be dealt with.
2. ^Elimination of nuclear weapons production altogether.
Our overkill" capacity already assures us of nuclear "security".
Rocky Mountain Arsenal.
1. Increase the capacity of detoxification facilities to speed
up the schedule.
2. Create underground storage space for nerve 'gas now in
surface storage.
3. Prohibit any new (binary or other) toxic agents from being
stored there.
4. Phase out the Arsenal and create a wildlife
sanctuary on the site.
5. Press health and disaster agencies to develop and coordinate
adequate protection programs.
Although, letter writing is often not as effective a means of
-------
616
30.
protest as are other forms of intervention it can often call attention
to matters of citizen importance. The following agencies have shown
a real concern over the presence of RF and RMA in the Denver Metro area,
and could be of great help in planning strategies or simply for research
information.
Environmental Protection Agency Environmental Action Commit
1129 Twentieth St. N.W. 1100 Uth
Washington.D.C. 20460 Denver, Colorado
The American Friends Service Committee
Colorado Area Office
2801 E. Colfax Ave.,#304
Denver, Co. 80203
David Massebaum
Clean Water Action Project
1325 Delaware St.
Denver, Co.
For those individuals who wish direct contact with persons involved
in the decision-making process at Rocky Flats, the following addresses
will be of help.
Atomic Energy Commission
Washington, D.C. 20545
Albuquerque Operations Office
Harold C. Donnelly
P.O. Box 5400
Albuquerque, New Mexico 87115
Regulatory Regional Office of the AEC-Denver
John W, FJ,ora
10395 W. Colfax Ave.
Denver, Co 80215
Other individuals and groups that could provide information
or assistance in dealing with the Rocky Mountain Arsenal and Rocky Flats
are listed below.
-------
617
31.
Colorado Open Space Council
Sierra Club
Environmental Action Gr6up
Colorado Committee for Environmental Information
Floyd Haskell, Colorado Senator
Ralph Nader
Ruth Correll, Member of Boulder City Council
Ed Mendillo, Denver Representative
Peter Metzger, Columnist for "Rocky Mountain News"
Dr. Arthur Tamplin and Dr. John Gofman, authors of the book
Poisoned Power.*
THE PROJECT AS A LEARNING EXPERIENCE
Reflecting upon the value of this group research project, participants
mentioned a number of definite advantages they saw in the experience.
The value of cooperative research was emphasized time and again.
The sense of interdependence that develpped among us during the semester
was quite visible. This was a rather unique experience for most of us,
having been socialized in a highly individualized and competitive system.
In this project, shared learning was the major resource. The research
tasks were divided and reports scheduled so that each was responsible for
the others' learning and progress. If one of us failed to produce on
time the others suffered. The importance of cooperation and humor in
group research came through very clearly and participants expressed
substantial satisfaction with the shared learning experience.
Participants spoke often of the interest and excitement generated
*Both Gofman and Tamplin have testified before governmental , public and
professional groups to make Americans aware of the dangers of nuclear pollutioi
-------
618
32.
by doing research that would be utilized for and might make some difference
in solving a critical real-world problem. We cannot overemphasize the
value group members saw in the opportunity to benefit society as well as
themselves in the process of creating knowledge.
Others felt that the project had helped to sharpen their knowledge
of research methodology including library and action research skills.
Having to pass through the problem selection, data-gathering, and analysis
utilization phases and be forced to consider the third phase as you were
moving through the others was helpful to a number of us. The distinction
between committed research became quite clear and there was some discussion
within the project as to whether or not "committed" research was scientific.
The point is that values inevitably enter into research at both the
problem selection and analysis utilization stages while data-gathering
should remain as value free as possible.
The importance of data-gathering was another major realization
emerging from the project. The essential nature of factual material
on which to base conclusions and policy decisions is indisputable.
While much of the learning produced in the group concerned process (i.e.
how to get the factual material), group members did a good deal of content
learning as well. They learned a great deal about weapons production
and storage system, chemical/biological warfare, the military-industrial-
acadcmic complex and how it operates, and public attitudes and community
leadership in surrounding areas. They also demystified the bureaucratic
process as they learned how to "penetrate" bureaucratic organizations,
how to persevere in the face of bureaucratic inertia, evasive reponses
-------
619
33.
and misrepresentation. They also learned how accepting and passive people
generally are with respect to bureaucratic unresponsiveness to their
problems. The "success feedback" most of the project members received
from their persistence in gathering data proved to them that large
bureaucratic organizations are vulnerable to good strategy and are not
impenetrable. We should also note however, that some officials were
both open and helpful and this should be encouraged through citizen dialogue
with them.
The project group concluded that formal study in universities
should and can be related to real-world problem solving. The group felt
that there should be increasing concern for using the university
curriculum, both graduate and undergraduate, to gather factual material
on significant problems and make it available to citizen organizations.
This facilitates the informed involvement of citizens in decision-making
and action that affects their present and future.
Perhaps the most dramatic payoff the project had was the insight
it afforded students into the sharp internal contradictions current weapons
policies produce. One student remarked that one of the by-products of the
production process at the Rocky Flats installation could well be a long-
term serious increase in radioactivity-related morbidity in the surrounding
area's population. The question must be asked, then, how can we protect
ourselves from our own "defense" industries?
In the last group meeting, however, one student spoke of what
must be the ultimate contradiction-a mix of the tragic and the absurd.
-------
620
34.
She spoke of signs posted inside the Rocky Flats plant that she had
«,
visited, a facility which produces plutonium trigger-devices for the
nuclear weapons capable of destroying millions of people in seconds.
The sign read:
LIFE IS FRAGILE
HANDLE WITH CARE
ACTION RESEARCH GROUP
Joyce Durol - Report Editor
Tom Esposito - Report Editor
Jeff Calvin
John Marvuglio
Marcee Orlin
Harvey Tevah
Dan Morimoto
Jeff Jones
Sociology 482, Fall 1973
University of Colorado
Professor Paul Wehr
-------
APPENDIX A - 1
621
DEPARTMENT OF DEFENSE
uni rittis !
HUT CNICI :
SECRETARY OF DEFENSE
DEPUTY SECRETARY OF DEFENSE
i ruv)
MtllM K
iiinu KIUKI
in IMUUI
* HIIISI
ICMNnmi)
ISSISIIII
SltllltlT
II IIHISl
IIIUII III
iiriiiHiit)
ISSISI1II
SltlllUT
ii mint
ISSISlin
IICIHIII
ii iiinsi
IUHUIUUII
usismi
inn HIT
ti MIIIII
sumut uuisi
IISISIIII
sicuiut
K KIIISI
aiduuni
IIIMB
IIIU1UI
SltllHII
ii mini
nunrini in
mini iniiii
lillSIUl
SICUIUT
II KIIISI
mini
ISiHUlI
Sltllllll
II IIIUII
antu Hum
KIM
KPIIIWII
K HIIISI
num
mini
NHUI
UIITSH
HI IIIIMM
issnun i
m HCHM
IIMC (III
l»l till! V mil
CUimi. IWI CHI! K ITIII
cm m 11111. im
cm H MIU jpiiium
cm K sun m IHCI
cnmiuNi HUM civs
IIIIISI
CH1UICIIU1
ItllCI
cnnum
M
KllHil
KIIISI
Illlltll
IISIIICI
riiucii
mid
KIIISI
iiisiKin
IIIIKI
IIIIISI
cm
piirwiiisi
IUII1
KIIISI
IICIIIII
ISSISIIICI
IUK1
KIIISI
CIIIIKI
inn
KIKI
IIKISI
ami
ItllCI
KMIIIIII H m un
siuiim K m IUT
iwii sianin
in ISSEIIII
titimus K m im
KPUIIIH K III Ull
S1CBIII1 K II Ult
an
it
UNI
VtU
IKS
tlMI ,
SKHUII
IM
ISSBIUI
iiamits
• mun
un*
MM
am
MruiMii M w ii ina
sianui * m 11 iwt
MU Sltllllll
im ituiut
Honuis« m M iita
KIIISI
mmcnu
IUICI
must
limit
IIIICI
KIIISI
IKU1I
KUCT
nut
Im
Cllllll
muss smun
nuntc
-------
622
APPENDIX A - 2
Organizational Structure of the
ROCKY MOUNTAIN ARSENAL
Secretary of Defense
Deputy Sec. of Defense
- James Schlesinger
- William P. Clements, Jr.
Secretary of Army
- Howard H. Callaway
Chief of Staff
- Gen. Creighton W. Abrama
U.S. Army Forces
Command
U.S. Army Material
Command
- Gen. William
6th U.S. Army - Lt.Gen.Richard/ Rocky Mt. Arsenal - Col. Watson
G. Stillwell
-------
APPENDIX B - 1
623
ALBUQUERQUE OPERATIONS
GEQGRAPHICAL
x SANDIA-LIVERMORE * BURLINGTON
« ROCKY FLATS . * OAYTON
» TONOPAH TEST RANGE » KANSAS Cl T Y
« LOS ALAMOS
•Jyf- ALBUQUERQUE
*SAND1A»
®A.'URILLO
HO OPERATIONS
ARc A OFFICE
A!<<•<:!u<(l to Aien Office
M, i \ AS
U.S. ATOMIC ENERGY COMMISSION
1 0 F'MI in P'AIT E N E R G Y 4
i MATCKULS DE''fcLOP.
^ a
.. _1.~ " T
?EACTi°RTTAY (I ""*"",
3
| SAM FRANCISCO
OPERATIONS
j OFFICE
\ *
$ *
3 *
) <•
j ULl. •»**
-J
*******
<*
*
i ""•
LA SI..
•rue
COMMISSION j
1 '
GENERAL MANAGER
I
"I
Ik i !
? > APMiMISTOATIOM 1
I
' — -1" — $— " *"-^---v^~
ALBUOUCfJWE j »»*
OPERATIONS !««,»*
OFFICE j
^
s ,<
i
M)!.. I'J'AnV ;
COMMIT TEC; i
k " u •*'"""" ,
t ,. , *
J Of! A j
S
J f:IFLO COWM/.NJ'! J
! Mi-VAOA i
OPtRATICNS i
OFFICE
i(
1 tCST i
1 ' • '-•• i
t
•;A'(.>IA (. «
-------
CO
U.S. Atomic Energy Commission
ALBUQUERQUE OPERATIONS
ORGANIZATION CHART
OFFICES REPORTING fO THE MANAGER
I
OFFICE OF THE
CHIEF COUNSEL
WU&XATION
— ' Ot^SiO-
PATENT
WviHOf
—.».!..
lAHACEB
DEPUTY UAIIAOEB
1
OFFICE OF THE
ASST UA.AGER
FOIt
ADMINISTRATION
]
rjn
•>;«!.(«< TO* I
O>u»l.l ANCE OM CC
'••• 1 1
OFFICE OF THE OFFICE OF THE OFFICE OF THE
ASST. MANACEB »SST. OANACEH HST. UA«ACE«
fo" FOB FOB
PLANS S1UOCETS OPEBAT10HS LOGISTICS
L_^ 1 1
D«>10»
-------
APPENDIX C - 1
625
DOW CHEMICAL CORPORATION
U.S. Area Canada Europe Latin
America
Pacific Life Sciences
Barnes
G.J. William
J.M. Leathers
Executive Vice-President
Operations
Rocky Flats Texas Michigan California Latin Eastern
America
-------
626
APPENDIX C - 2
ATOMIC ENERGY COMMISSION
The Commission - Dixy "Lee Ray, Chairperson
General Manager - Robert Hollingsworth
Mfg.
Contractors
Dow Chemical - J. Hanes
N/
Albuquerque
Operations
- General Donnelly
T
Rocky Flats - B. W. Colston
U.S. Area - Earl Barnes
A
Area Operations - J.M. Leathers
ATOMIC ENERGY COMMISSION
Headquarters: Germantown, Md.
Mailing address: Washington, D.C. 20545
Phone. 301-973-1000
Chairman
Special Assistant to ihc Chairman
Commissioner
Special Assistant
Commissioner
Special Assisunt
Commissioner
Special Assistant
Commissioner
Special Assistant
Secretary of the Commission
Adminittrativc Law J.itlKc .
Cliairm.in, AF,C Iloaiil of Cnntriict Appeals
Oh.iirmaM, Atomic S..frly nml I.icriiiini/ Appeal PnncL
<"linilin.it>, Atomic. Sulrly »od l.irniiinx llo.uij I'.incl.
DIXY LEE RAY.
HARRY D. BRUNER,
JAMES T. RAMEY.
MARY IiAi.ow.
CLARENCE E. LARSON.
JOHN A. GRIFFIN.
WlLLrAM O. DOUD.
THOMAS E. MURLEY.
WILLIAM E. KHIEOSMAN.
(VACANCY).
PAUL C. HENDER.
SAMUEL W. JKNSCII.
PAUL II. GANTT.
ALAN S. RO.IKNTIIAL.
NATIIANIP.I. II. Gooouicn.
-------
627
FOOTNOTES
"Employment of Chemical and Biological Agents," U.S. Army Field
Manual, 3-10, Department of Army, Navy and the Air Force (March, 1966).
2Ibid.
"Chemical and Bacteriological Weapons and the Effects of Their
Possible Use," (NY: Ballantine, 1970; United Nations Report //E691.24).
4
Kurt von Kaulla and Joseph H. Holmes, "Changes Following Anti-
cholinesterase Exposure," Archives of Environmental Health. (Feb. 1961),
pp. 168-177. ~~~
5Ibid.
The Denver Post. Feb. 5, 1960, p. 3.
The Denver Post. Nov. 3, 1965, p. 38.
Q
The Denver Post. Nov. 9, 1973, p. 27.
9
The Denver Post. Dec. 6, 1973, p. 21; Shell Chemical Company now
produces at Rocky Mountain Arsenal: Aldrin (pesticide), Azodrin (insecticide),
Bidrin (insecticide), Ciodrin (insecticide), Nudrin (insecticide), Phosdrin
(insecticide), Vapona (insecticide), Nenagon (soil fumigant), Planavin (herbicide
The Denver Post. Nov. 12, 1959, p. 26.
The Denver Post, June 14, 1959, p. 1A.
12Ibid.
13Ibid, p. 3A.
14
The Denver Post. Nov. 13, 1959, p. 1.
15Ibid.
16Ibid.
The Denver Post. Nov. 18, 1959, p. 3.
TO
The Denver Post, Nov. 25, 1959, p. 24.
-------
. 2 -
628
19Ibid, p. 3
20
Ibid, p. 24
21The Denver Post, June 14, 1959, p. 3A.
22The Denver Post. Nov. 17, 1959, p. 1.
23The Denver Post, Jan. 3, 1963, p. 2.
o /
The Denver Post, Nov. 3, 1965, p. 38.
1 C
The Denver Post, Dec. 13, 1966, p. 3.
26The Denver Post, Dec. 6, 1973, p. 21.
27
Denver Clarion, Nov. 16, 1973, p. 1.
28
Roger Rapaport, "Secrecy and Safety at Rocky Flats, "The Los
Angeles Times, 1969.
29Ibid.
3°Ibid.
J.R. Mann and R.A. Kirchner, "Evaluation of Lung Burden Following
Acute Inhalation Exposure to Highly Insoluble PaC>2," Health Physics,
Vol. 13, #8, (Aug., 1967), p. 877.
32The Colorado Daily, April 4, 1974.
33Ibid.
op. cit.
3 S
Report by the Energy Policy Project of the Ford Foundation,
A Time to Choose: America's Energy Future, (Cambridge, Mass.: Ballinger, 1974).
"\f\
Edward A. Kartell, "Radioactivity of Tobacco Trichomes and Insoluble
Cigarette Smoke Particles," Nature, Vol 249, #5454, (May 17, 1974). A recent
article by atmospheric chemist Edward Kartell describes how this process
occurs in tobacco smoking. It is similar to the bombardment of healthy cells
by radioactive material such as plutonium oxide alpha particles.
-------
629
BIBLIOGRAPHY
The Boulder Daily Camera. Nov. 29, 1952; Feb. 14, 1953; Sept. 16, 1961-
Jan. 31, 1963; Aug. 15, 1968; Nov. 11, 13, 1969.
Boulder Eco-Center. "A Discussion of Objections to Nuclear Gas
Stimulation." Boulder, Colo., Sept. 15, 1973. (Mimeo).
"Chemical and Bacteriological Weapons and the Effects of Their Possible
Use." NY: Ballantine, 1970; United Nations Report //E69I.24.
The Colorado Daily. Apr. 4, 1974.
Colorado Department of Health, Division of Occupational and Radiological
Health. "Emergency Handling of Radiation Incidents: A Handbook for
Police Officers." n.d.
Colorado Department of Health, Division of Occupational and Radiological
Health. "Emergency Handling of Radioactive and Metallic Fires:
A Handbook for Fire Departments." n.d.
Colorado Department of Health, Division of Occupational and Radiological
Health. "Handling the Radiation Accident Victim: A Guide for
Hospital Personnel." n.d.
Colorado Department of Health, Division of Occupational and Radiological
Health. Radiological Response Plan." n.d.
Colorado Department of Health. "Radiation in the State of Colorado." 1972.
Denver Clarion. Nov. 16, 1973.
The Denver Post. June 14, Sept. 23, Oct. 17, Nov. 12, 13, 17, 18 25
29, 1959; Feb. 5, 1960; Jan. 3, 1963; Apr. 26, 1964; Nov. 3,
1965; Dec. 13, 14, 1966; Apr. 29, 1967; Nov. 1, 1971; Oct. 15
Nov. 9, Dec. 6, 1973.
Dow Chemical Company. "Dow Annual Report to Shareholders." Midland, Mich.,
"Employment of Chemical and Biological Agents." U.S. Army Field Manual
Department of the Army, Navy and the Air Force, March 1966. '
Gofman John and Templin, Arthur. Poisoned Power. Eammaus, Pa.: Rodale
Press, 1971.
Hersh, Seymour M. Chemical and Biological Warfare. NY: Doubleday, 1969.
Kaulla.Kurt von and Holmes, Joseph H. "Changes Following Anticholinesterase
Exposure. Archives of Environmental Health. Feb. 1961.
-------
.. 2 -
Mann, J.R. and Kirchner, R.A. "Evaluation of Lung Burden Following Acute
Inhalation Exposure to Highly Insoluble Pa02." Health Physics,
Vol. 13, #8, Aug. 1967.
Martell, Edward A. "Radioactivity of Tobacco Trichomes and Insoluble
Cigarette Smoke Particles." Nature, Vol. 249,"#5454, May 17, 1974.
McClintock, Michael, et.al. "Memorandum on the Possible Hazard to Denver
of the Rocky Mountain Arsenal's Storage of Nerve Gases."
Boulder, Colo., Aug. 15, 1968. (Typewritten).
Rapaport, Roger. "Secrecy and Safety at Rocky Flats." The Los Angeles
Times, 1969.
Rapaport, Roger. The Great American Bomb Machine. NY: E.P. Dutton, 1971.
Report by the Energy Policy Project of the Ford Foundation. A Time to Choose:
America's Energy Future. Cambridge, Mass.: Ballinger, 1974.
Rose, Stephen. CBW-Chemical and Biological Warfare. Boston: Beacon Press,
1968.
U.S. Atomic Energy Commission, Information Division. "The Story of
Albuquerque Operations." Albuquerque, N.M., Revised March 1973.
-------
, :-^ .'.-(My r moratorium
ii " iJ vi' Ci
'Otuiru)/ conservation
27 Hastings A v o. Croton-on-HucUon, Nov. York 10520 (9t4) ?-71-3 629
January U, 1974
Dr. V/.D. Rov;e
Radiation rrograms, Environmental Protection Agency
Washington, D.C. 20460
Dear Dr. Rowe,
We are pleased to respond to ycur call for "viewpoints of con-
cerned citizens as to the problems of plutoniurn in the environment« "
The prbbleras of plutoniun in the environment can be quickly and
easily reduced by STOPPING construction of all nuclear power plants
and phasing cut of operation those now in operation as quickly as
possible.
To some such a course of action may seem unreasonable, but to
informed citizens it is the cmlv_ reasonable solution. Plutonium,
with a radioactive half-life o~f 24,000 years, must be isolated for
the next 500,000 years - more than 250 times the period between the
birth of Christ arid the present. Because eac_h lar^e nuclear power
plant produces about 400 pounds of this poison eaoh yej^r, more than
99.999$ of it must be contained if serious healTn "efirccts (death)
on the citizenry are to be avoided. For example, just three pounds
of plutonium- is enough, evenly distributed, to produce nine billion
lung cancer cases (about three times the world's population).
•The chances of successfully containing such large quantities of
plutoniun to 99.999?' perfection are, to put it mildly, exceedingly
remote. What o.the_r industry approaches that kind of accountability?
Or even 99$? Hone that wo know of.
V/e are pleased to report to you that over 147,000 American voters
have consulted their common sense about nuclear power and petitioned
their representatives in Government to keep nuclear fission o_ut of thuir
lives. More than 30,000 from New York alone have. uigned Clean Snerci'
Petitions. If you doubt their authenticity, you are invited to inspect
them in Washington, where they are kept filed according to Congressional
District.
The only respjjnsiblo action EPA can take is to oppose all
development of Huclear pcv7er plants in favor of enorj-y from the sun
which can be clean, safe, reliable, cheap and plutonium-free.
Sincerely,
lln I,.
eo :The Pree.'.i Coordinator
-------
632
Jody Dittrich
301 East Virginia
Jamestown, New York
14701
Mr. Miller,
I am writing in response to your article in the December 28
issue of Rodales Environment Action Bulletin concerning the pluto-
nium emission standards being set up by the Environmental Protection
Agency.
I understand that plutonium is a very poisonous substance and
feel that the job you are doing to rid this from our air is indeed
commendable. With all that is wrong in the world today its good to
know that there are people who have not given up. I think you would
be wise in. making your fight more public. I'm certain there are
people who have never even heard of plutonium.
I am aware of the idea that plutoniuim can "live" for twenty
four thousand years or longer. At this rate with more plutonium
being put in the air every day one could begin forming concepts
that we will be doomed by the effects of plutonium on the human
body.
Once again I would like to comment on your efforts. Keep up
the good work.
Sincerely,
Jody Lea Dittrich
-------
633
UNITED STATES AIR FORCE
-------
V
S3-LV-LS a3-l-IMO
-------
/7, /?
•/
./?
, /
t
,
,,
-------
vUiicon&in C*coloyicai Society.
P.O. Box 514
Green Bay, Wis. 54305
January 20, 1975
Dr. William A. Mills,
Director of Criteria & Standards Div. (AW-560)
Office of Radiation Program
U. S. Environmental Protection Agency
Washington, B.C. 20460
Dear Dr. Mills:
Our comments on environmental plutonium standards are brief:
1. There can be no minimum limits.
2. The world cannot sustain a plutonium economy with
safety.
3. The breeder reactor is a disaster.
Cordially.
R. J. Bar lament
Secretary
-------
637
Colorado Open Space Council, Inc.
1325 Delaware Street, Denver, CO 80204
January 21, 1975
Director
Criteria and Standards Division (AW-560)
Office of Radiation Programs
U. S. Environmental Protection Agency
Washington, D. C. 20^60
Dear Sir:
We originally applied to offer oral testimony at the
Plutonium and transuranium elements public hearing held
in Denver on January 10, 1975. The representative for
our group, Dwight Filley, was called away suddenly and
was unable to appear before your panel. Unfortunately,
he neglected to inform the panel or me until last week.
We would greatly appreciate it if you could enter the
testimony as part of the written record at this time as
a demonstration of our concern with the possible dangers
of plutonium on the environment. I enclose two copies of
the testimony for this purpose.
I wish to apologize for the Colorado Open Space Council
for any inconvenience we may have caused. We shall make
every effort that this does not happen again.
Yours very truly,
Jnnie F. McCune
Administrator
Encs.
-------
Colorado Open Space Council, Inc.
1325 Delaware Stt. Denver,, CO 80204
January 10, 1975
STATEMENT' OF DWIGHT F1LLEY,
VICE PRESIDENT OF THE COLORADO OPEN SPACE COUNCIL,
FOR THE COUNCIL
*
-------
turn out to be other than expected* 639
We feel that the population is already sujected to multitudes
of strange chemicals,*ranging from food additives to atmospheric
pollutants. Time after time we learn that some new technological
inovation has an unexpected and harmful side effect* Examples
are phosphates in the water and aerosol propellants in the ozone
layers of the atmosphere.. We therefore favor strong limits to
further pollution.
We are proud that our state of Colorado h?s t?ken the lead
on many environmental issues. The Colorado Open Space Council
supports our state''s standards for Plutonium- contamination of the
soil as a Tnimimunr, and urge that the Federal Government protect
all U. S. citizens as Colorado citizens are now protected*
Plutonium-,, because of it's intense pathogenic characteristics,
as well as its fJamability,, require totally unprecidented control
to prevent harmful releases. Such control may in fact be impos-
sible to achieve.. The record so far is not encouraging. There
have been many accidental: releases, either admitted by the A.E.C.
or discovered by someone else* rtrhasubeen estimated that with
a fully developed -nuclear industry,, 99.999* containment is
necessary to protect the public* It is doubtful that any sub-
stance has ever freerr accounted for so carefully;, certainly
Plutonium has not been thus far*
If we are ever to determine if such control car. be achieved,,
standards must be set and compliance attempted* We urge that
Colorado standards become minimum national standards* Thank you.,
-------
640
^,rv>v$rv> cxW> t^j^^^X*^-*-*
^Wvi \>UiO >
-------
641
ex>
<4AJCS^yv^-«s,
SL^~ - - A Cf
HO
:=*&V<5U cL^-u^m
-------
-------
643
14-300 Lakehaven Drive, N.3.
Atlanta, Georgia 30319
January 21, 1975
Mr. Russell E. Train
Administrator, Environmental Protection Agency
Rm. 1200 Waterside Mall Bldg.
Uth & M Streets, S.W.
Washington, D. C. 201+60
Dear Sir:
It is my understanding that the EPA recently held public
hearings pertaining to establishment of emission standards for
Plutonium 239 by nuclear power plants. I would like to protest
the lack of publicity given these hearings.
n™«r,ASTa citi?en who is unalterably opposed to nuclear fission
follow th«ChS 1?cal.newapape™» national news magazines and closely
follow the broadcast media for news pertaining to nuclear energy
It seems incredible that permissible emission! for Pu239 woSld
even be considered. I would appreciate any available information,
regarding positions stated at the hearings and any decisions reached,
th + * a.PP.£arS J?8* nuclear fission is being rammed down the
throat of the public. The licensing process for construction and
£E8?h«ion of nuclear power plants is a tragic farce perpetrated
by the utility industry and its Washington hearquarters, the AEG.
With our new vice-president being up to his armpits in Exxon
I fear greatly for the survival of the EPA as guardian of the
environment and the hope of posterity.
•el*. -' ^
/?
Victor Skorapa, Jr.,M.D. ^
-------
644
Hudson Valley
on Nuclear Safety
P. O. Box 472, New Paltz, N. Y. 12561
January 21, 1975
Dr. W.D.Rowe
Radiation Programs
B.P.A.
Washington DC 20460
Dear Dr. Rove,
At the suggestion of Franklin L. Gage, Viashigton
coordinator of the Task Force against Nuclear Pollution I
as sending you the enclosed article by Dr. Arthur Tamplin
which deals with the problems of Plutonium in the environ-
ment.
I am sure you are familiar with other sources on
the subject by Dr. Gofman and others.
Tours sincerely,
Ji - /f.
HL:js
eacl.
Ned Lehae
Secretary
-------
(Reprinted with permission from The Living Wilderness. Copyright (c)
1974 by The Wilderness Society.)
The Nuclear Gamble:
What Are the Odds?
No adequate system exists to regulate expanding industry
by Arthur R, Tamplin
645
a
£
AN unfortunate thing happened on our way
to the present energy shortage—the Atomic
Energy Commission had a vision. This vision
was a program for the development of nuclear
reactors for the generation of electricity. It was
some 25 years ago when the AEC embarked
upon this long-range reactor program. At the
outset of this grand program, we were told by
its high priests that they would develop a tech-
nology that would supply us an abundance of
cheap power—so cheap that in most cases it
would not be worthwhile to meter it.
Now some 25 years later we find that the
cheapness prophecy was quite wrong and,
equipped with today's hindsight, it is not at all
clear that we should want an abundance of power
to drive an ever-increasing gross national prod-
uct with its attendant resource depletion and
environmental pollution. Moreover, it is obvious
today that the policy over the past 25 years has
led to serious diseconomies. We put 85-90 per-
cent of our energy research and development dol-
lars into the fission reactor program and thereby
preempted research on alternative sources of
electrical energy that are both necessary and
more acceptable. As a consequence, we now find
ourselves confronted in an arrogant fashion by
this bureaucratic fait accompli: we are told that
we can have either clean nuclear or dirty fossil
fuel plants. However, it is abundantly clear to-
day that fossil fuels, primarily coal, will form
the backbone of our generating capacity through-
out this century and into the next. If we had
spent our research dollars differently, we could
have had clean fossil fuel plants years ago, and
most likely we would be well on the way to
obtaining all our energy needs from the sun.
Yet we find our political leaders and our
bureaucracies proceeding under the same old
guidelines of the past. Witness the following
quotation that has now become a new command-
ment in the catechism of the AEC:
In his June 4, 1971 Message on Energy to the Con-
gress of the United States President Nixon pre-
sented a program which included "... A commit-
ment to complete the successful demonstration of
the liquid metal fast breeder reactor [LMFBR] by
1980." He further states that ". . . Our best hope
today for meeting the Nation's growing demand for
economical clean energy lies with the fast breeder
reactor. Because of its highly efficient use of nu-
clear fuel, the brooder reactor could extend the life
of our natural uranium fuel supply from decades
to centuries, with far less impact on the environ-
ment than the power plants which are operating
today."
The present generation of nuclear reactors,
the light water reactors, are a techti•>!«-»ical
cul-de-sac. The difficulty facing them derives
from their use of uranium-235 as a fuel. Accord-
ing to the AEC the economically recoverable
supply of this fuel will last only a few decades.
The fast breeder reactor would utilize uranium-
238, the predominant uranium isotope which is
not fissionable under conditions present in reac-
tors. In the fast breeder, however, it will be
transmuted by nuclear process into plutonium-
239 which can undergo fission in a reactor. The
breeder will actually create more fissionable fuel
than it will consume (it will create fuel or
"breed"). By using uranium-238 in this manner
the breeder reactor will, as the President said,
"extend the life of our national uranium fuel
supply from decades to centuries." With just this
information as evidence, the President's decision
to make the LMFBR our priority energy program
would appear to be sound.
However, the serious nature of this nuclear
energy decision was exposed by Dr. Alvin Wein-
berg, director of the Oak Ridge National Labora-
SPRING 1974
17
-------
646
tory and a proponent of nuclear power, when he
wrote in the July 7, 1972, issue of Science:
We nuclear people have made a Faustian bargain
with society. On the one hand, we offer—in the
catalytic nuclear burner—an inexhaustible source of
energy. . . . But the price that we demand of
society for this magical energy source is both a
vigilance and a longevity of our social institutions
that we are quite unaccustomed to.
Dr. Hannes Alfven, Nobel Laureate in Physics,
had earlier described this "Faustian bargain" in
the May, 1972, issue of Bulletin of the Atomic
'Scientists:
Fission energy is safe only if a number of critical
devices work as they should, if a number of people
in key positions follow all their instructions, if
there is no sabotage, no hijacking of the transports,
if no reactor fuel processing plant or reprocessing
plant or repository anywhere in the world is sit-
uated in a region of riots or guerrilla activity, and
no revolution or war—even a "conventional one"
—takes place in these regions. The enormous quan-
tities of extremely dangerous material must not get
into the hands of ignorant people or desperados.
No acts of God can be permitted.
In his article in Science Dr. Weinberg stressed
the need ". . . of creating a continuing tradition
of meticulous attention to detail." He stated:
In a sense, we have established a military priest-
hood which guards against inadvertent use of
nuclear weapons, which maintains what a priori
seems to be a precarious balance between readiness
to go to war and vigilance against human errors
that would precipitate war. Moreover, this is not
something that will go away, at least not soon.
The discovery of the bomb has imposed an addi-
tional demand on our social institutions. It has
called forth this military priesthood upon which in
a way we all depend for our survival. It seems to
me (and in this I repeat some views expressed very
well by Atomic Energy Commissioner Wilfred
Johnson) that peaceful nuclear energy probably
will make demands of the same sort on our society,
and possibly of even longer duration.
The President's decision to guide us along the
path to a nuclear future was a monumental deci-
sion. But was it the correct one? It is instructive
to look at some of the highlights of past history
of this nuclear priesthood which is the AEC.
A nuclear reactor offers the possibility of in-
dustrial accident far beyond anything past his-
tory has known. Such an accident could result
from the meltdown of the reactor core with the
consequent breaching of its containment struc-
tures and the release of vast quantities of lethal
radioactivity into the atmosphere. An AEC study
Dr. Arthur R. Tamplin, a biophysicist on the staff of
the Atomic Energy Commission's Lawrence Radiation
Laboratory at the University of California, is on leave
working with the Natural Resources Defense Council on
environmental questions concerning the AEC's liquid
metal fast breeder reactor program. With Dr. John W.
Gofman he wrote Poisoned Power: The Case Against
Nuclear Power Plants.
indicated that such an accident could cause the
immediate death of 3,000 to 4,000 individuals as
a result of exposure to radiation. Another 30,000
to 40,000 people would be exposed to levels of
radiation sufficient to cause a substantial num-
ber to die prematurely from cancer. The genetic
consequences of such an accident would affect
many future generations. Expectable property
damage losses were estimated at approximately
$7 billion.
To minimize the risk of such accidents in the
present light water reactors, the AEC and the
industry are relying heavily on an Emergency
Core Cooling System (ECCS) intended to pre-
vent meltdown. The ECCS, however, has never
been fully tested and the facilities for performing
such tests are not even scheduled for completion
until 1975. Six small-scale tests of the ECCS
have been performed and the ECCS failed all six
of these tests. There is thus a strong possibility
that the ECCS will not work.
In 1971 a group of scientists from the univer-
sities in the Boston area (the Union of Con-
cerned Scientists) investigated this overall prob-
lem of core meltdown and the possible effective-
ness of the ECCS. In its published report the
group concluded that the situation was so
perilous as to warrant a halt to the construction
of nuclear reactors.
In testimony presented to the Congressional
Joint Committee on Atomic Energy, Ralph
Nader and the Union of Concerned Scientists
last January 29 made public a secret report by
an AEC task force dated last October. On page
14 of that report was the following:
Review of the operating history associated with 30
operating nuclear reactors indicated that during
the period 1/1/72-5/30/73 approximately 850 ab-
normal occurrences were reported to the AEC.
Many of the occurrences were significant and of a
generic nature requiring followup investigations at
other plants. Forty percent of the occurrences were
traceable to some extent to design and/or fabrica-
tion related deficiencies. The remaining incidents
were caused by operator error, improper mainte-
nance, inadequate erection control, administrative
deficiencies, random failure and combinations
thereof.
Regarding these incidents, on page 16 the task
force stated:
The large number of reactor incidents, coupled with
the fact that many of them had real safety signifi-
cance, were generic in nature, and were not identi-
fied during the normal design, fabrication, erection,
and preoperational testing phases, raises a serious
question regarding the current review and inspec-
tion practices both on the part of the nuclear
industry and the AEC.
There is good reason to suggest that, because
of the meticulous attention to detail that is re-
18
THE LIVING WILDERNESS
-------
quired at every step during construction and
operation of nuclear reactors, it will be impos-
sible to develop an adequate system of regulation
and inspection. The expanding nuclear industry
is most likely unmanageable.
But even after setting aside the technical argu-
ments over engineered safety and the ECCS, it is
important to recognize that in our troubled
world terrorist activities are almost daily occur-
rences. Sabotage of a nuclear power plant is a
real possibility. Aircraft hijackers have already
made such a threat against the reactor at the
Oak Ridge National Laboratory. The December
21, 1972 issue of Nucleonics Week carried a
news item concerning threats against nuclear
plants in England by the Scottish Nationalists
and by the Irish Republican Army. An Asso-
ciated Press dispatch dated March 27, 1973 from
Buenos Aires stated:
fi£ 7
a thousand years. The Atomic Energy Commis-
sion's long-intended answer to the radioactive
waste problem involved the use of abandoned
salt mines at Lyons, Kansas, as a repository for
the lethal fission products. In 1970 an investiga-
tion of the site by the Kansas Geological Survey
found it to be the leakiest salt mine in the
world. Their findings presented the strong pos-
sibility that radioactive wastes in the salt mines
could contaminate ground water supplies and,
accordingly, the AEC was forced to abandon its
plans. The government's present interim plan is
for above-ground engineered storage of the waste
for an interim period of at least 25 years in the
hope that by then some solution to this problem
will have been found.
In May, 1966, the National Academy of Sci-
ences' Committee on Geological Aspects of Ra-
dioactive Waste Disposal submitted a report to
... it is important to recognize that in our troubled world
terrorist activities are almost daily occurrences. Sabotage
of a nuclear power plant is a real possibility. Aircraft
hijackers have already made such a threat against the
reactor at the Oak Ridge National Laboratory.
Troops and police searched yesterday for a team
of guerrillas who seized an atomic plant under con-
struction and made off with the weapons of its
sentries.
The real possibility of a catastrophic accident
was well recognized by the AEC and the Joint
Committee on Atomic Energy in the fledgling
years of the nuclear industry. Rather than push
for the certainty of safety, they pushed to pro-
tect the industry, not the public, by sponsoring
the Price-Anderson Act. This act limits the
liability of a nuclear plant to only $560 million of
the potential $7 billion of damage (seven cents
on a dollar). And, Mr. or Ms. Citizen, you have
no other recourse, because your homeowner's pol-
icy contains a nuclear exclusion clause. Eighty-
five percent of this limited liability has to be
underwritten by the United States government
because of the timidity of the private insurance
industry.
The operation of a nuclear reactor produces
vast quantities of lethal radioactive fission prod-
ucts, the same materials that constituted the
fallout from nuclear weapons tests. These radio-
nuclides remain dangerous and must be isolated
from the environment for a period of more than
the AEC critical of various aspects of AEC prac-
tices. For example, the committee stated that
none of the AEC radioactive waste storage sites
was in a satisfactory geological location. The
committee also criticized the practices related to
low- and intermediate-level liquid wastes and all
kinds of solid waste.
The AEC has done little in response to this
critical report. In fact, this nuclear priesthood
suppressed the report for three years until Sena-
tor Frank Church (D-Idaho) in a floor speech
demanded that it be made public. Just last year,
115,000 gallons of high level radioactive wastes
leaked into the ground at the AEC's Hanford,
Washington, facility over a period of 51 days
during which the staff failed to monitor the
tanks. We are now some 30 years into the
Atomic Age but have yet to devise a safe means
for handling these radioactive wastes which must
be guarded for a thousand years.
The most pernicious product of the nuclear
industry is plutonium-239. This element is not
native to Earth. The entire present-day inven-
tory is man-made. Plutonium-239 will remain
deadly not for 1,000 years but for some 500,000
years. Plutonium is also the most toxic material
SPRING 1974
19
-------
, known to man. One millionth of a gram (there
4 O are 28 grams to an ounce) of plutonium has been
shown capable of producing cancer in animals.
The biological evidence suggests that the radia-
tion protection standards of the AEC for plu-
tonium are far too lax. Last February 14 the
Natural Resources Defense Council petitioned
the AEC to reduce its present maximum permis-
sible plutonium exposure levels by a factor of
115,000!
Besides being extremely hazardous because of
its radioactivity, plutonium is also a substance
from which atomic bombs can be made without
elaborate technology. In the projected breeder
reactor economy there will be some 10,000 tons
of plutonium in the commercial sector of society
and tons of plutonium would be in transit every
day. Just some 10 pounds would be sufficient to
fashion a crude atomic bomb in a basement work-
shop. The information required to fabricate such
a bomb became unclassified years ago. In an age
The breeder reactor decision is lit-
erally a decision for all men and all
time. It is far too important to have
been made with so little public and
congressional awareness.
of aircraft hijacking and the ransom of diplomats
and Olympic athletes the risks of such diversion,
and consequent nuclear blackmail, are not mini-
mized even by ardent nuclear energy supporters.
Thus, Atomic Energy Commissioner Clarence
Larson recently stated:
Once special nuclear material is successfully stolen
in small and possibly economically acceptable
quantities, a supply-stimulated market for such
illicit material is bound to develop. And such a
market can surely be expected to grow once the
source of supply has been identified. As the market
grows, the number and size of thefts can be ex-
pected to grow with it, and I fear such growth
would be extremely rapid once it begins. . . . Such
theft would quickly lead to serious economic bur-
dens to the industry, and a threat to the national
security.
The history of the peaceful nuclear priesthood
is certainly no formula for the future. Its
present-day light water reactor safety program
was allowed to be preempted by commercial in-
terests and budgetary restrictions. The decision
to commit this nation to the fast breeder reactor
may prove to be the most significant technologi-
cal decision since the Manhattan Project. Its im-
portance notwithstanding, this commitment was
not the end product of a rational and public
decision-making process. Rather, it evolved over
25 years of increasing industrial and govern-
mental effort to develop an inexpensive and un-
limited source of energy. The commitment was
made, moreover, in the face of mounting appre-
hension within the scientific community concern-
ing the human and societal hazards of fission
reactors, apprehension which would only be
compounded by the liquid metal fast breeder
reactor program.
As evidence of this apprehension among scien-
tists, a statement of concern over the environ-
ment and world peace (the Menton Statement)
was signed by 2,200 scientists. The statement
included a call for an end to the proliferation of
nuclear reactors. It was presented to U. N. Sec-
retary General U. Thant and published in the
U. N. Courier for July, 1971. Scientists from all
nations at the 23rd Pugwash Conference on Sci-
ence and World Affairs last September con-
cluded:
1. Owing to potentially grave and as yet unresolved
problems related to waste management, diversion of
fissionable material, and major radioactivity re-
leases arising from accidents, natural disasters,
sabotage, or acts of war, the wisdom of a commit-
ment to nuclear fission as a principal energy source
for mankind must be seriously questioned at the
present time.
2. Accordingly, research and development on alter-
native energy sources—particularly solar, geother-
mal and fusion energy, and cleaner technologies for
fossil fuels—should be greatly accelerated.
3. Broadly based studies aimed at the assessment of
the relation between genuine and sustainable en-
ergy needs, as opposed to projected demands, are
required.
The problems associated with the present
reactor program strongly suggest that we are
only perpetuating and compounding a bureau-
cratic blunder by pursuing the LMFBR program.
The breeder reactor decision is literally a deci-
sion for all men and all time. It is far too impor-
tant to have been made with so little public and
congressional awareness.
As a result of a lawsuit brought by the Natural
Resources Defense Council on behalf of the
Scientists' Institute for Public Information, the
AEC is now preparing an environmental impact
statement on the LMFBR program. This will
undoubtedly increase the tempo of the growing
national and international debate over nuclear
reactors. It is to be hoped that at the very least
this debate will result in much more substantial
funding of research and development on the
alternative energy sources mentioned by the Pug-
wash Scientists as well as on programs of energy
conservation.
20
THE LIVING WILDERNESS
-------
649
N. Y. TIMES EDITORIAL 1/10/75
TOXIC CARELESSNESS
In dealing with a substance as deadly as plutonium,
it is not enough merely to minimize the risks. The Atomic
Energy Commission and its successor agency, the Nuclear
Regulatory Commission, have the urgent task of tightening
controls over the use and disposition of this toxic by-
products in the nation's installations.
The dangers from plutonium are infinite. Carelessly
handled, even in minute quantities, it can cause death
and disease. With only modest expertise, a few pounds of
the lead-like element can be fashioned into a crude but
highly explosive nuclear weapon. In the light of these
potentialities, reports that thousands of pounds of highly
enriched uranium and plutonium are missing from the
inventories of the nuclear industry require something more
than generalized denials. A more dozen pounds, which in-
dustry executives concede may have been unaccounted for
from time to time in the past year, would be devastating
in the hands of a terrorist group of hostile government.
Pressure is building up inside the nuclear industry
for a Federal decision to authorize the use of plutonium
as a fuel for civilian power plants to augment the dwind-
ling supply of uranium fuel. It is inconceivable that
responsible policymakers could permit wider dispersal of
plutonium for any purpose as long as even marginal dangers
of nuclear theft remain.
"(C) 1974/1970 by the New York Times Company. Reprinted by permission."
-------
650
January 21, 1975
232 Rowland Canal
P.O. Box 2U9
Venice, California 90291
Dr. William A. Mills, Director of
Criteria & Standards Division (AW-560)
Office of Radiation Program
Environmental Protection Agency
Washington, B.C. 20U60
Dear Dr. Mills:
Please make the following statement of my concern for plutonium emission standards
a part of the official hearing record on these standards.
I am a former nuclear physicist who did some of the first work on the Liquid Metal
(sodium) Fast Breeder Reactor while employed at Atomics International, Canoga Park,
California, in the early 1960s. I am more aware than most of the terrible and- in-
tolerable dangers that even minute amounts of plutonium present to life on this
planet, as we know it, when released into the planetary environment. Plutonium
is one of the most toxic of all of the environmental poisons in minute amounts,
and is extremely long lived by human time standards.
.A
A very smallxof plutonium could fairly easily be fashioned into a crude fission
device. It seems to me inevitable that someday in spite of all possible precau-
tions, we will be faced with world wide nuclear terrorism if we continue to man-
ufacture this substance.
I strongly urge that not only should EPA rule th;
-------
651
7500 g Terrace View Apts.
Blacksburg, Virginia 2Zf060
January 22, 1975
Dr. William A. Mills
Director of Criteria & Standards
Division (A-W-560)
Environmental Protection Agency
Washington, D.C. 20^60
Dear Dr. Mills:
I would like you to make the following comments to be
part of the hearings on environmental plutonium standards
which are being held by the E.P.A. in Denver, Colorado.
I would like to go on record as being opposed to Nuclear
Fission plants in light of their potential dangers to the
environment and mankind. From what I understand, I do feel
that they are immune to the possibility of causing nuclear
explosion, however my main concern deals with the dangers
posed by their lethal wastes. Many questions come to my mind
when considering th« problem of transportation and disposal
of such wastes. A substance which has a half life of 2/t,000
years and is as dangerous as Plutonium is too hazardous to
fool around with. I know that I do not want this substance
transported through my town via truck, train, or any oth«r
means of transportation which is subject to an accident.
Nor do I want it to be disposed of anywhere near my place of
residence, work or recreation.
It is my undeestanding that the number one cause of death
among children under ag« fifteen is cancer. I just hope that
the nuclear fission plants that have existed in the past are
not a contributing factor to this statistic.
Sincerely,
''.•-••"I J'f /- Lf'r+
Vincent Pedicini
-------
652
3667 Summit, Apartment 3
Kansas City, Missouri 64111
January 24, 1975
Dr. William A. Mills, Director of
Criteria and Standards Division (AW-560)
Office of Radiation Program
Environmental Protection Agency
Washington, D. C. 20460
Dear Sir:
As concerned citizens, we should like to submit the following
comments on nuclear power plants and plutonium emission standards.
We appreciate the opportunity to air our views, but we feel that
the hearings on plutonium emission standards, and on other nuclear
power issues, should be more widely publicized since nuclear power
is a considerable threat to all Americans. The Environmental
Protection Agency is the logical governmental agency to perform
such a vital function. In the future, we hope that the EPA will
live up to its information dissemination responsibilities.
Plutonium is the most toxic substance known to man. Atomic
Energy Commission nuclear power plants have a well-deserved
reputation for nuclear "accidents" involving plutonium emissions;
Rocky Flats, Detroit's Fermi fast breeder, the Northeastern
Utilities Connecticut Yankee plant, the Vermont Yankee plant, and
the plant near Hanover, Washington, to name a few. A moratorium
must be declared until nuclear technology has advanced to the
point that plutonium emission accidents are no longer possibilities,
much less probabilities.
The emergency core cooling system, the only system that might
prevent a complete core meltdown, has never been effectively tested.
With the advent of the liquid metal fast breeder reactor, which the
Atomic Energy Commission is pushing so strongly, and the subsequent
plutonium-recycling program, the possibilities of a core meltdown
become truly horrifying. Even the AEC's damage estimates, when it
concerns itself with the reality of a complete meltdown, concede
that human and property losses will far exceed the limits established
by the Price-Anderson Act. We feel that, if for no other reason,
a moratorium should be established until full insurance coverage
will be provided in the event of any loss-of-coolant accident and
subsequent meltdown.
-------
653
Dr. William A. Mills
January 24, 1975
Page 2
All of the factors involved in a possible accident can be
expected to increase in potential, given the current goals of the
AEC and the major utility companies. A core meltdown, with the
right weather conditions, near a large city, could ""produce the
worst casualty in the history of the United States.
We feel that, with plutonium, there are no acceptable
emission standards.
Sincerely,
Robert D. Haun
Diane Ezell
-------
654
COLORADO DEPARTMENT OF HEALTH
4210 EAST 11TH AVENUE - DENVER, COLORADO 80220 • PHONE 388-6111
Edward G. Dreyfus, M.D., M.P.H. Executive Director
January 23, 1975
William Mills, Ph.D., Director
Standards and Criteria Branch (AW-56)
Office of Radiation Programs
U.S. Environmental Protective Agency
Washington, D.C. 20^60
Dear Dr. Mills:
During the presentation of the Colorado Department of Health's testimony before
the hearing panel in Denver, you requested that references be submitted regard-
ing statements made in testimony. In this regard the following is submitted:
1)
2)
3)
"The Problem of Large-Area Plutonium Contamination" from Selected
Papers from the Bureau of Radiological Health Seminar Program.
Seminar Paper No. 002 DHEW, PHS, CPEHS, ECA. (1968 paper of
W. H. Langham, Ph.D.)
"Biological Considerations of Nonnuclear Incidents Involving
Nuclear Warheads" Lawrence Radiation Laboratory publication
UCRL-50639 (1969 paper of W. H. Langham, Ph.D.)
"Toward Interim Acceptable Surface Contamination Levels for
Environmental Plutonium Oxide" by R. L. Kathren, April, 1968,
BNWL-SA-1510.
"A proposed Interim Standard for Plutonium In Soils" by
J. W. Healy, Los Alamos Scientific Laboratory LA-5483-MS
Informal Report UC-41 , January,
5) Transcript of hearing before the Colorado State Board of Health
held February H», 1973, and continued March 21, 1973.
As the representative from the city of Boulder and Dr. Carl Johnson, Jefferson
County Health Department, were concerned with emergency response plans for the
U.S.AEC's Rocky Flats Plant, please find enclosed a copy of a portion of the
state plan for such a contingency. As this plan is under revision, a copy of
the draft revision is also enclosed. Copies have been provided to these two
individuals.
-------
655
William Mills, Ph.D.^Director
January 23, 1975
Page 2
Questions were asked of me by Dr. Morgan and you relating to resuspension of
the plutonium soil contamination. In this regard, the following is provided:
1) Tables of monthly average plutonium 239 and 2kO air concen-
trations observed at CDH on-site sampling stations.
2) Maps locating air sampling stations on-site and in the Denver
metropolitan area.
3) A graph depicting the annual average plutonium 239 and 240 air
concentrations versus time observed at CDH on-site sampling
stations.
The graph illustrates that revegetation and traffic curtailment have been effec-
tive in the D-3 and k area (immediately adjacent to the oil spill area where the
approximate "average" soil concentration is 1 microcurie Pu per square meter
soil surface). The highest contaminated areas are to be removed later this year.
The levels observed over this time period at APG-56, D-l and 2 identify that
soil disturbances in this area (construction of waste water handling facilities
in 1972), did indeed affect air concentrations.
Manipulation of the data provided in the tables identifies an air concentration
half-life for this "old" deposition at station D-5 (0.1 microcurie Pu per square
meter, soil surface) of between k.k years, for world-wide fallout Pu plus re-
suspension to 1.5 years, for resuspension only, using one concentration for
world-wide fallout Pu for the entire period of time involved. The most reason-
able air concentration half-life would approximate 2.7 years for resuspension
only, using a 9.6 year half-time for world-wide fallout. From the above data
a resuspension term, based on annual average air concentrations and the so!)
concentrations associated with stations D-3 and k and D-5, of 5xlO"9 to 5xlO"'0/M
is Identified.
The testimony provided by Mr. Earl Bean, USAEC-RFAO referenced world-wide fallout
Pu levels for all their air sampling stations, which Is what Is being observed
now (off-site). However, it must be pointed out that two stations located east
of the plant site (SS-32 and SS-33) are located on "clean ground" in the wind-
strewn field of the plutonium contamination. Station SS-32 is located at the
intersection of Indiana Street and the Plant's east access road. The surrounding
soil has been redistributed and reworked, and the major wind pattern corresponds
to the layout of the east access road. Station SS-33 is located adjacent to a
plowed agricultural field. Therefore, it would be expected that these stations
would observe world-wide fallout levels. These stations cannot be justifiably
use • ili's'rat.3 that there is n£ resuspension of contaminated soil to an alr-
bot ;-, ^; :r -h-i* r* world-wide fallout.
-------
656
William Mills. Ph.D., Director
January 23, 1975
Page 3
Also enclosed is a retyped version of the Department's presentation of Jan-
uary 10, and a letter the Department received from Shelley Barthel.
Again, the Department wishes to express its appreciation for the bringing of
the hearing to Denver and the privilege of participation. The efforts of EPA,
both the Regional office and the Las Vegas facility, in identifying various
situations at the Department's request is appreciated.
Should you require additional information or need clarification on items al-
ready provided, please advise.
Sincerely,
Albert J. *f)azle
Director
Occupational and Radiological
Health Division
AJH:bs
Enclosures
cc: Paul B. Smith, EPA, Region VIII
-------
657
239 + 240
Pu pti/m3
ON-SITE'LOCATIONS
JANUARY
FEBRUARY
MARCH
APRIL -
MAY
JUNE
JULY
AUGUST
SEPTEMBER
.OCTOBER
NOVEMBER
DECEMBER
AVERAGE
1970
•*••••
___
.00042
.00039
.00019
.00008
.00024
.00020
.00017
.00025
.00024
1971
.00020
.00029
.00030
.00034
.00045
.00051
.00020
.00022
.00038
.00019
.00032
.00027
.00031
1972
D-l
.00020
.00018
.00035
.00021
.00177
.00277
.00133
.00189
.00351
.00258
.00066
.00183
.00144
1973
.00119
.00034
.00046
.00051
.00101
.00322
.00014
.00059
.00017
.00059
.00038
.00027
.00074
1974 1975
.00037
.00022
.00015
.00042
.00058
.00035
AVERAGE
.00037
D-2
JANUARY
FEBRUARY
MARCH
APRIL
MAY
JUNE
JULY
AUGUST
SEPTEMBER
OCTOBER
NOVEMBER
DECEMBER
.00091
.00042
.00025
.00024
.00021
.00019
.00046
.00031
.00010
.00045
.00036
.00036
.00063
.00048
.00031
.00032
.00019
.00027
.00010
.00055
.00020
.00022
.00030
.00016
.00024
.00047
.00073
.00175
.00126
.00178
.00045
.00067
.00053
.00079
.00016
.00365
.00026
.00038
.00016
.00012
.00049
% .00062
.00010
.00018
.00007
.00044
.00046
.00046
.00071
.00269
.00034
.00069
.00062
-------
658
PAGE 2
1970
239 + 240 „
Pu pCi/m
ON-SITE LOCATIONS
1971 ' 1972
1973
1974
1975
JANUARY
FEBRUARY
MARCH
APRIL
MAY
JUNE
JULY •
AUGUST
SEPTEMBER
OCTOBER
NOVEMBER
DECEMBER
AVERAGE
.03300
.00530
.00650
.00160
.00100
.00097
.00051
.00110
.00625
.00689
.02048
.00552
.00768
.00844
.00592
.03742
.00418
.00316
.00534
.01639
.00202
.01029
D-3
.00240
.00522
.00367
.00138
.00245
.00655
.00299
.00458
.01410
.00652
.00094
.00096
.00470
.00203
.00439
.00326
.00128
.00210
.00522
.00325
.00477
.00317
.00154
.00229
.00201
.00294
.00010
.00128
.00130
.00257
.00748
.00442
JANUARY
FEBRUARY
1-iARCH
APRIL
MAY
JUNE
JULY
AUGUST
SEPTEMBER
OCTOBER
NOVEMBER
ISCEhrtSR
AVERAGE
1969
.00900
.00490
.00299
.00310
.00650
.00124
.00071
.00166
.00115
.00037
.00057
.00057
.000273
1970
.00051
.00328
.00049
.00076
.00079
.00330
.00051
.00086
.00026
.00102
.00210
.00058
.00120
1971
APC-56
.00163
.00207
.00388
.00069
.00043
.00092
.00043
< .00008
<„ 00008
.00859
.00223
.00025
.00177
1972
.00053
.00054
.00353
.00039
.00037
.00040
.00035
.01678
.00128
.00230
.00019
.00071
.00228
1973
4.00008
<. 00008
.00090
NA
.00030
.00047
.00032
. .00114
.00020
.00011
<. 00008
<. 00008
.00037
1974 1975
.00003
.00015
.00015
.00011
.00048
.00036
-------
1970
239 +240
Pu pCi/m
ON-SITE LOCATIONS
1971 1972
1973
659
1974
AVERAGE;
D-4
JANUARY
FEBRUARY
MARCH
APRIL
MAY
JUNE
JULY
AUGUST
SEPTEMBER
OCTOBER
NOVEMBER
DECEMBER
.00440
.00082
.00091
.00660
.00107
.00067
.00152
.00170
.00076
.01242
.00893
.00369
.02758
.00419
.00334
.00506
.00731
.02485
.00758
.00236
.00211
.00211
.00243
.00164
.00152
.02256
.00575
.00784
.00613
.01378
.00153
.00322
.00263
.00742
.00690
.00144
.00220
.00428
.00238
.00391
.00191
.00197
.00095
.00287
.00044
.00061
.00128
.00159
.00338
.00223
,00734
.00588
.00324
-------
PAGE 4
660
239 + 240 3
Pu pCi/m
OFF-SITE LOCATIONS
D-5
JANUARY
FEBRUARY
MARCH
APRIL
MAY-
JUNE
JULY
AUGUST
SEPTEMBER
OCTOBER
NOVEMBER
DECEMBER
AVERAGE
.00022
.00014
.00011
.00016
.00008
.00011
.00020
.00015
.00024
.00024
.00013
.00012
.00016
.00009
<. 00008
.00005
.00013
.00008
.00007
.00007
.00006
.00013
.00009
.00015
.00010
.00047
<. 00002
.00009
.00036
<. 00002
.00011
.00010
.00010
.00013
.00005
.00017
.00010
<:. 00002
.00003
<. 00002
.00008
.00003
.00008
.00013
.00019
.00036
.00013
.00012
.00010
-------
PAGE 5
239 +240 '
Pu pCi/m
OFF-SITE LOCATIONS
661
1969
1970
" "• ' m* • •• *.* 1 1. i -» i •« ir^^f ir/j
APC-2 DENVER (EPA nATA^
QUARTERS
FIRST .00007
SECOND .00011
THIRD .00006
FOURTH .00004
AVERAGE .00007
FIRST
SECOND
THIRD
FOURTH
AVERAGE
FIRST ' .00013
SECOND .00010
THIRD .00006
FOURTH .00004
.00006
.00013
.00009
.00003
.00008
.00018
.00017
.00022
.00005
.00016
.00008
.00025
.00008
<. 00003
.00006
.00013
.00007
.00002
.00007
APC-15
.00006
.00019
.00006
<. 00002
<•. 00008
APC-16
.00005
.00017
.CC008
<. 00002
.00006
.00006
.00002
.00002
.00004
ARVADA
.00003
.00005
. .00003
.00012
.00006
GOLDEN
<. 00002
.00008
.00003
.00012
.00002
.00003
.00001
.00001
_. 00002
<. 00008
<. 00002
.00014
<.. 00006
<. 00002
.00016
' .00004
<. 00002
.00004
.00045
.00010
.00013
AVERAGE
.00008
.00011
<;. 00006 x. 0000 6
-------
662
PAGE 6
1969
239 + 240
Pu pCi/m3
OFF-SITE LOCATIONS
1970 1971 1972
1973
1974
1975
FIRST
SECOND
THIRD
FOURTH
AVERAGE
APC-19 BOULDER
.00012 .00005 <".00002 <.00002
.00018 .00013 .00005 .00005
.00013 .00007 <.00002 .00014
.00010 '<.00002 .00010 <.00002
.00013 < . 00007
-------
PAGE 7
1969
1970
239 + 240
Pu pCi/m
OFF-SITE LOCATIONS
1971 1972
1973
663
1974
1975
APC-42 FT. COLLINS
QUARTERS
FIRST
SECOND
THIRD
FOURTH
AVERAGE
C. 00002 C.00002
.00004 .00006
.00007 <'. 00002
<.00002 .00019
<•_._ 00004 <•• .00008
.00015
.00015
FIRST
SECOND
THIRD
FOURTH
AVERAGE
> f- *»r;;JA
APC-81 WALSENBURfi '
.00006
.00011
.00008
.00003
(.00002
.00074
.00003
.00014
.00014
.00017
...00007 ^00006
FIRST
SECOND
THIRD
FOURTH
AVERAGE
APC-108 RANGELY
.00006
.00008
.00008
.00020
.00010
C00002
.00009
.00017
<. 00002
.00016
.00016
-------
•y.
1972
664
KK-SIXi; AIR PAUTICUtATK
SAMPLING LOCATIONS
19
•
2
5
7
8
9
11
13
15
16
19
22
96
57
58
59
f
State Health Department
Denver School Advnn. Bldg.
Aurora
Adams City
Englewood
Cherry Creek Dam
Jefferson County Health Dept.
Arvada
Colden
Boulder
Sloan's Lake
Littleton
Brighton
Edgev;ater
N
ON-Sl-'IE ©
V '°~5
•1 ,
j
• 16
\
\
\
\
\
JEFFERSON
\
^DENVER \
D-5 Woman Creek & Indiana Ave.
o
o
V)
O
10
_!
miles
MAP 1
-------
1972
ON - SITE AIR SAMPLING STATIONS
a
e rs^r- :^ \
MAP 2
-------
SEMI-LOGARITHMIC 359-7O
KEUFFEU ft 6SS6R CO. KAOE IN u. I. A.
3 CYCLES X 60 DIVISIONS
r<
HJ
cr>'
05
-------
667
1380 - 19th Street, #3
Boulder, Colorado 80302
January 8, 1975
Mr. Albert J. Hazle, Chief
Occupational and Radiological Health Division
Colorado Department of Health
4210 East 11th Avenue
Denver, Colorado 80220
Dear Mr. Hazle:
Because I must work, I am unable to attend the public hearing to be held
Friday, January 10th regarding the Rocky Flats nuclear installation.
As^a concerned citizen, I therefore respectfully request that the following
brief statement be entered into the record on my behalf.
I am an eight year resident of Colorado, age 31. I am a certified elementary
school teacher, planning to marry this year and to raise our children here.
I oppose and protest the philosophy which causes the existence of Rocky
Flats. The United States does not need to produce or possess nuclear bombs
-—especially since we intend never to use them. We already possess a
more-than-adequate stockpile of conventional weapons and bombs for use as
a deterrent. Nuclear bombs as deterrents are dangerous, and serve no
rational purpose. The vast resources which are now wasted on these nuclear
bombs should rather be spent toward solving our serious, present social
and economic problems.
I appreciate the opportunity to express my opinion; and, hope that someday
behalf^Thank ou ^ °f ^ ^^ ^ dec!slons made in the public's
Shelley Barthel
-------
o -
17 L b V O)
0
899
-------
669
-------
670
»^
^:
4
^
b
VI
^° ^ (S ^ °o
o^
*
M
4
v»
, -\
V;
3
r\
P?
Vj
: . 0 o —
fj """ ^
O
b
iki
— r
& £
^
3
)
10 A
* I
-------
671
take peace
Mr. & Mrs. C. A. Webber Jr
j 610 S. Elm Street
Greenville, N. C. 27834
t
*""
v
-------
672
49 South Ifein Street
Southampton,' I:IY 11968
January 2? 1975
Dr W D Rowe
.Radiation Trograas
V 1' A
"ashington, DC 20460
T)ear Dr Rowe,
I learn fron the Task Force "gainst Nuclear Po-ilution, Inc,
that you are' asking for "viewpoints of concerned citizens as they
pertain to the problems of plutonium in the environment".
My viewpoint is that the most important challenge to civilization
end to life on this earth is ;resented to everybody by the
proposal of government and industry to build nuclear energy plants.
Dr Gerald A ^rake, of letos.'-iey. MI, says, and is worth quoting,
"If the tubercle bacilus, or virus of a potentially fatal form
of encephalitis packed tremendous energy for fueling electrical
plants, would it be rational to culture these organisms by the ton
and ship them around the nation and the world for such e purpose?
Hardly, and yet they are not nearly as deadly as plutonium 239<>"
Ve need energy. V'ell pretty soon we will need food. How about
solving famine and the population explosion at one stroke by
killing and canning the surplus population and shipping the meat to
the famine striken areas of the world?
I think the U S and the whole world is at the mercy of and in the
power of the insane.
The insane are,among others, but chiefly, the proponents of nuclear
energy.
There is nothing left but hope.
Sincerely yours,
^airfield Porter
-------
470 Windridge Drive
Racine, Wis. 53402
February 1, 1975
673
Dr. William A. Mills
Dir. of Criteria and Standards Div. (AW-560)
Office of Radiation Program
EPA
W3shington, D.C. 20460
Dear Dr. Mills:
This letter is in response to requests for comments on the
amount of Plutonium to be allowed in our environment.
For several years our group has been concerned with the
environmental and health hazards of nuclear power plants. So me
of our main concerns are those involving the use of Plutonium.
We feel that the use of this element should be stopped completely
until all safety problems connected with its recycling and
storage are solved. With the worldwide proliferation of nuclear
plants, the possibilities for theft and blackmail become so
numerous that it is only a question of time before terrorists
carry out some tragedy. This could occur with a bomb or just
by threatening to disperse a small amount of Plutonium into
the air, causing cancer in millions of people.
Any substance as hazardous as Plutonium should not be put into
our world for all future generations to guard. The possibility
of armed fortresses and convoys necessary to guard the manufacture
and transportation and storage of Plutonium should make any
responsible informed person reject nuclear power plants and all
they involve. It is morally wrong and incomprehensible to us
that a supposedly civilized society is even debating the issue.
With any real commitment to alternate power sources and needed
changes in our housing codes, air-conditioners, automobiles,
and with recycling of our resources, there would be no need for
these hazardous plants. The result of positive action on the
above would help the people in this country regain some
confidence in the future,
ours truly
CC: President Gerald Ford
Nelson Rockefeller
Gaylord Nelson
William Proxmire
Les Aspin
Frank Zarb
t.
Reid
Edee Sobel , Co-Chairmen
Racine-Kenosha Citizens for
the Environment
-------
574 w (6 i P National Council on Radiation Protection
and Measurements
791OWOODMONT AVENUE, SUITE 1016, WASHINGTON, D. C. 20014 AREA CODE (301)657-2652
LAURISTON S. TAYLOR, President
E. DALE TROUT, Vice President
W. ROGER NEY, Executive Director
February 7, 1975
Dr. William A. Mills, Director
Division of Criteria and Standards
Radiation Office
Environmental Protection Agency
Waterside Mall E-635
hOl M Street, S.W.
Washington, D.C. 20^60
Dear Bill:
Referring to your telephone conversation the other day, I suggested the
possibility that a study of the hot particle problem by the NCRP might be
submitted for record relative to the EPA hearings which were completed in
Denver on January 10th.
It now appears that this report may not be ready for release within the
prescribed time for "open record".
As you know, any report prepared by a committee of the NCRP has to be
reviewed by the total Council membership and all comments considered before
the report is released. Our committee has completed a report entitled,
"Alpha Emitting Particles in the Lung" and this is now under review by the
Council. While some two-thirds of the members have approved the report and
none have disapproved it, we still feel compelled to receive positive re-
plies from the remaining members. For this reason it is impractical to
have this in your hands by February 10th. We expect the report to be
published soon after that date and we will, of course, make copies available
to you.
You are no doubt aware that this report is one of several that we have in
various stages of completion at the present time and dealing with certain
problems of environmental and occupational exposure to radiation. Another
report dealing with plutonium in occupational exposure situation is also
under review, having been completed by the Scientific Committee that prepared
it.
Other studies less far along are having to do with problems of surface
contamination and removal of contaminated materials.
Since we cannot have the report in your hands by the required deadline,
I would appreciate it very much if you could make this letter a part of the
record so that there will be knowledge of the early availability of the other
reports.
Sincerely yours,
Lauriston S. Taylor
-------
675
STATEMENT PELATING TO THE PROBLEMS OP PLUTONIUM IN THE ENVIRONMENT
The United States is moving into an era wherein plutonium-239
is to be a major source of electrial energy in nuclear fission re-
actors. Thus plutonium-239 will be a major material of national
and international commerce. As much as 200 million kilograms of
Pu-239 is projected as moving through the nuclear fuel cycle over
the next \& years.with many opportunities for accidental release
of Pu02 as aerosols occuring over that period of time.
This radioactive substance which is to be our major fuel is
among the most potent of carcinogens. As little as 3 micrograms
has consistently produced lung cancer in dogs. Plutonium has a
half life of 2lj., lj.00 yearsso that it must be isolated from the bio-
sphere for literally a half million years.
nuclear
Plutonium-239, the material of which/weapons are made will be
moving in progressively increasing volume by highway, rail and wa-
ter. As such it will pose not only a severe public health hazzard
but also portends of a threat to the survival of political freedom.
The necessity of stringent measures to prevent the diversion of
Plutonium and its destructive use against the public by extremist*
groups was discussed in the Senate by Senator Ribicoff on April 30, 7^
in reporting the findings of an AEC study group reviewing the then
current AEC safeguard system. The organization of a national police
force has been discussed and recommended. This does not bode well
for the democracy.
Dr. Alvin Weinberg, former head of the AEC's Oak Ridge Nation-
al Laboratory, one of fission power's chief supporters has neverthe-
less acknowledged the serious social implications of accepting
-------
676 (2)
nuclear fission technology. His reference to the "Paustian bargain"
implied in national commitment to nuclear fission power is well known.
Dr. Chauncy Starr, president of the Electric Power Research Insti-
tute, commenting on leaving future generations the burden of guard-
ing high level radioactive waste for literally hundreds of thousands
of years at the World Energy Conference in Detroit last September,
acknowledged that this was a sociological problem. Yet it is incre-
dible that most of the highly intelligent persons in the commercial
and scientific communities who are promoting nuclear power, are un-
able or unwilling to percieve the great social problems which this
technology entails. This (plus AEG ground rules pertaining to in-
tervention) is a major factor in the lack of any significant public
input into this question which so seriously af'ects its welfare.
Indeed, the public has had very little education in the ramifications
of commitment to nuclear power beyond the PR efforts of the electric
utility industry and of the AEG in behalf of the utility industry.
This public hearing relating to the potential adverse environ-
mental impact of release of plutonium and other trans-uranium ele-
ments with the objective of determining whether or not new and/or
additional standards are required is a fragment in the regulatory
process pe^taininp to nuclear fission technology. As such it is
a worthy but quite insufficient effort. What is needed is an in-
tense educational campaign relating to all phases of comnitmwnt to
nucleai fission power preferably conducted by the EPA which hope-
fully has no vested interest in this technology. This should be
-------
(3) 677
followed by a national referendum on the issue of whether or not
the United States should commit itself to nuclear fission power,
such as is to be held in Sweden later this year,
rictor Skorapa, Jr., M.D.
^300 Lakehaven Drive, N.E.
Atlanta, Georgia 30319
February 8, 1975
-------
678
EMMA HARTZLER
202 South Sixth Street
Goshen, Indiana 46526
-------
679
Paul B. Smith
Air and Hazardous Material Division
1860 Lincoln Street
Denver, Cot 80203
Sir,
I am writing this letter as a concerned Coloradoan, living between two potentially
hazardous operations, one of which is located at Platteville and the other at
Rocky Flats.
Being uneducated in the field of metallurgy and radiation, I can not communicate in
technical terms, I can only ask why!
Why do we as American citizens have to be the recipients of the ABC's experimental
blunders i.e. "accidental and programmed" releases of plutonium into our water,
soil, and air at the Rocky Flats Plant, "unexpected problems" at the Rio Blanco
site, and the "accidental loss" of containers having once carried radioactive
materials, onto our main highway system, I 25!
There are too many of these "accidental happenings" in the name of nuclear progress
and the AEC! Is the AEC oblivious of the future environment???? Is it because of
national security and/or fattening the purse of many who seem to be unconcerned about
our environnwit for future generations?
Please consider actions which will make it more difficult for the AEC to continue
their present experimental programs with hazardous materials,
Sincerely,
A most concerned citizen
-------
680
Form 365
UNIVERSITY OF COLORADO MEDICAL CENTER
Inter-off ice Communication
TO Robert Siek. Chairman
Lamm-Wirth Task Force on Rbcky Flats
FROM John C. Cobb, M.D., M.P.H.
SUBJECT: Plutonium in Dust at Rocky Flats
EJATfi . January 14. 197S
I urgently request that our Task Force make a detailed study of the circumstances
surrounding the contamination of soil from leaking drums containing plutonium in
cutting oil at Rocky Flats. I have heard from various sources that there may be
even hundreds of curies of plutonium in the soil where the bil drums leaked and
that the soil samples from the area immediately east of the spill have been recorded
at levels as high as 40,000 disintegrations per minute per gram of soil. I also
understand that the AEG is planning to dig up this contaminated soil for shipment
elsewhere.
I am concerted about the present danger to employees at the plant and to citizens
of Colorado from wind-blown dust containing plutonium coming from this source. I
understand from reading the Reports CER 71-72 RNM-FC-45 and CER 72-73 RNM-JAP-TGH-
16, dated May 1972 and March 1973, "Wind Tunnel Site Analysis bf Dow Chemical Facil-
ity at Rocky Flats," that the winds up there are frequently so strong that cars
in the parking lot need protection "...from high velocity wind action assaulting
vehicles with abrasive particles..." (Part II, p.ii). Wind tunnel studies were
done to find ways of sheltering parked cars from this sand-blasting which had
evidently become a problem.
Wind tunnel studies were also done to find out whether the monitoring stations
around the perimeter of the Rocky Flats plant were spaced optimally. Conclusion
#4 of this study (Part I, p. 37) reads as follows:
"An array of monitoring devices arranged along the north-south road which
exists to the east of the plant site should intercept plumes if they are
placed at 500 ft. intervals or closer"
This implies that monitoring stations at intervals greater than 500 ft. along
Indiana Street could miss detection of a plume of contaminated air coming from a
point source in one of the buildings at Rocky Flats. From my study of the map
published on pg. 29 of the Annual Environmental Monitoring Report of Rocky Flats
Plant, (REP-ENV-73), dated April 26, 1974, I conclude that the four monitoring
Stations are placed approximately 5,o6o to 7,000 ft. apart along this road. That
is, according to the wind tunnel studies, there would need to be at least ten times
as many monitoring stations as now exist in order to be sure to detect a plume of
contaminated air coming from a point source. To be sure to detect a plume coming
from a contaminated area approximately 500 ft. in diameter like the oil-dpill area,
one would need monitoring stations at least every 1000 ft. along Indiana Street.
What I conclude from this rough preliminary analysis is that a strong gust of wind
from the west could pick up a lot of dust from the contaminated area and blow it
past the monitoring stations in such a way that very lititle, if any, abnormal rise
-------
681
Robert Siek, Chairman /
Page Two
January 14, 1975
in radioactivity would be detected. This is particularly true because the monitors,
I understand, measure only the total amount of radio-activity accumulated over a
24-hour period. A brief gust or dust devil containing a large amount of plutonium
and seriously contaminating the residential areas east of Rocky Flats might there-
fore escape detection completely by the present monitoring System.
It is my urgent recommendation that our task force should get the whole story on
this from Rocky Flats. If the measurements we need have been classified, we must
force them to be released because the health of the residents of this area is at
stake. If the soil was indeed contaminated to the extent of 40,000 dpm/gm, as*
alleged, then a dangerous amount of plutonium has almost certainly been dispersed
into the residential areas all the way from Boulder to Golden, including Denver,
generally undetected by the monitoring system. We have no assurance that this is
not continuing today. Some evidence suggests that it is.
The suggestion by Lauriston Taylor at the EPA Hearings on January Ipth, that soil
standards may not be needed because air standards are satisfactory protection,
evidently does not apply under the particular conditions of strong gusty winds and
inadequate air monitoring at Rocky Flats. At the same hearings, the questions by
Prof. First regarding the relationship o£ contamination in the soil to inhalation
of plutonium are pertinent. We need studies done on site at Rocky Flats under
conditions of very high velocity gusty winds and twisters or dust devils in order
to find out what is the actual situation regarding resuspension of plutonium from
contaminated soil and how much of it is getting into the air breathed by residents
of the area. When the winds are strong enough to sand-blast the paint and pit the
windshields of cars at Rdcky Flats, I suspect we have enough plutbhium in the air
to be dangerous to those who breathe it.
cc: Members of L*»«nm-Wlrth Task Force (15)
Dr. Lauriston Taylor, President
National Council on Rddiation Protection
Prof. Melvin First, Harvard School of Public Health
Dr. Paul Smith, EPA, Denver
-------
382
COLORROO ORGRN1C GROUERS'flNO
To "»hom It vay Concerns
2555 W.3T" fIVC
Effcglfl.ffkB
477-6211
Recent nuclear related accidentsf?) Involving Dow Chemical's Hooky wlate instal-
lation serve as a strong indicator that the ficility threatens the lives of thousan
&B in the surrounding area.
Brocmfield and '"estminstsr are now plagued with traces of Tritium in their H20
supplies as a result of Hooky Flats dumping radioactive effluents into 'lalnut Creek
The Colorado "ublic Health T>oartment has recently deemed development lands in
Arvtida unsuitable building sites due to highly radioactive traces of plutonium ox-
ide dust in the ooll. MOt IS TH? TIM? TO TAKE ACTION rather than allow these atro-
cities to continue.
If nuclear plants are as safe as the Atomic Energy Commission (A^C) and utility
companies would have us believe, then why do they need the protection of the Price-
Anderson Act.
In the event of a nuclear catastrophe at Rocky Flats the ASC admits to losses
as high as J2SO-billion. In accordance with the Price-Andereon Act the utilities
and the /EC (us) would be responsible for a relatively small portion (J560million)
of this loss while the remainder (?) of the burden would be taken out of the Ameri-
can taxpayer's Docket.
As citizens and taxoayers whoee money and property is used in financing this in-
sanity, we urrre you to take action toward shutting down the Rocky Plats nuclear
plant, a warhead trigger manufacturing installation and to petition against the re-
instatement of the Price—Anderson -\ct when it comes up for reconsideation in early
1Q74. '
_--
^&^
5^jirL-_^^_^o^v
-------
683
f AM 8:26
COLORflDO ORGRNIC GRDUERS'RND MRRKETERS'BSSOCffll^-'DENck'CONTROL
To ''horn It ''ray Concerns
477-6211
Recent nuclear related accidental ) involving Dow Chemical's Hocky ?lats Instal-
lation serve as a strong indicator that the facility threatens the lives of thouean
els in the surrounding area.
Brocmfield and "'estminster are now plagued with traces of Tritium in their H20
supplies as a result of Hooky Flats dunmlng radioactive effluents into Walnut Creek
The Colorado Public Health Department has recently deemed development lands in
Arvada unsuitable building sites due to highly radioactive traces of plutonium ox-
ide duet in the soil. TO? IS TH1! TIM TO TAKE K3TION rather than allow these atro-
cities to continue.
If nuclear plants are as safe as the Atomic Energy Commission (A^C) and utility
companies would have us believe, then why do they need the protection of the Price-
Anderson Act.
In the event of a nuclear catastrophe at Rocky Flats the AEC admits to losses
as high as $280 billion. In accordance with the Price— Anderson Act the utilities
and the /EC (us) would be responsible for a relatively small portion ( J560million)
of this loss while the remainder (?) of the burden would be taken out of the Ameri-
can taxpayer's pocket.
As citizens and taxpayers whose money and property is used in financing this In-
sanity, we urge you to take action toward shutting down the Rocky Plats nuclear
plant, a warhead trigger manufacturing Installation and to petition against the re-
instatement of the Price— Anderson *,et when it comes up for reconsideatlon in early
si^JUfis
r
/?
Labor Donated
-------
684
26
COLORRDO ORGRNIC GROUERS'flNO MflRKETERS'fiS50C]fl]ll^;CN
CCiV'iiSPONDENCE CONTROL
To '"horn It "ay Concern: 4^-octi
Recent nuclear related accidental?) Involving Dow Chemical's Hocky ?lats Instal-
lation serve as a strong Indicator that the facility threatens the lives of thousan
<5s in the surrounding area.
Broomfleld and '"eetmlnster are now plagued with traces of Tritium in their H20
supplies as a result of Hocky Flats dumping radioactive effluents into falnut Creek
The Colorado "ublic Health department has recently deemed development lands In
Arvada unsuitable building sites due to highly radioactive traces of plutonlum ox-
ide dust in the soil. 50'? IS 7A? TIW TO TAKE ACTION rather than allow these atro-
cities to continue.
If nuclear plants are as safe as the Atomic Energy Commission (A^C) and utility
companies would have us believe, then why do they need the protection of the Price—
Ande raon Act.
In the event of a nuclear catastrophe at Rocky Plats the AEC admits to losses
as high aa $2£0 billion. In accordance with the Price-Anderson Act the utilities
and the /EC (us) would be responsible for a relatively email portion ($560million)
of this loss while the remainder (?) of the burden would be taken out of the Ameri-
can taxpayer's Docket.
Aa citizens and taxoayers whose money and property Is used In financing this in-
sanity, we urge you to take action toward shutting down the Rocky Flats rwclear
plant, a warhead trigger manufacturing Installation and to petition against the re-
instatement of the Price-Anderson Act when it comes up for reconsideatlon in early
AT^TFWZIF t * <\ rnuj",
™_J_^£2_^JH*Z^^
r^f __S^^d.^&t.^MJ_J^^f^f^^/£2_^^^oe;:)^
^
__^^^^.
^j^fM£^-~{L^-Ld^
a_L^lJilJ^^±^_J^^^_^__^S^-^/
Labor Donated
-------
685
* ^~/
-------
586
-------
£87
/V-rti-za^iy >2j*e&<*o/ <-'^r&&&z/'*<$L#*u^<£ ^cy~
, (/ £/y / ' ^ j/ '
^tsyh&Pft *^-^r.^ ^k^*C£ ^xc^i '^X<^ O**
-------
688
&£&*&/; <3su&r / IL
U
-------
••^^i^^Z^.^.^ ^*&-fv
/ ^ •
JVT
/ £ ' /
°^? ?T?77tC<' ^^
689
-------
90 ^S^fe>* THE DOW CHEMICAL COMPANY
ROCKY FLATS DIVISION
P. O. BOX 888
GOLDEN. COLORADO 80401
January 3, 1975
Mr. Paul B. Smith
Air and Hazardous Materials Division
Environmental Protection Agency
Region VIII, Suite 900
186t Lincoln Street
Denver, CO 8«2t3
Dear Mr. Smith:
Attached is a written comment which we would like to submit
to the EPA Committee considering standards for plutonium.
M. A. Thompson
Manager of Environmental Sciences
cc:
E. W. Bean - RFAO, USAEC
H. E. Bowman - Dow, Rocky Flats
A prime contractor for the U. S. Atomic Energy Commission CONTRACT AT(29-11-1106
-------
STATEMENT FOR THE EPA COMMITTEE 691
CONSIDERING STANDARDS FOR PLUTONIUM
ON THE HISTORY AND PERFORMANCE OF ROCKY FLATS
Submitted by
M. A. Thompson
DOW CHEMICAL U. S. A.
Rocky Flats Division
Following is a brief summary of the history and performance of the
Rocky Flats Plant as related to the handling and release of plutonium.
Announcement of the construction of the Rocky Flats Plant by the
Atomic Energy Commission was made in March 1951 and initial
construction was completed and operations started in 1953. By the
end of fiscal year 1974, the acquisition costs for the plant have
totaled 222 million dollars. This includes about 91 million dollars
for equipment and 131 million dollars for land, buildings and facilities.
Over 90 major structures containing approximately 1. 7 million square
feet of building area are included on the plant site. About 2900 people
are employed at the plant. The plant is situated on about 2500 acres
of government owned property approximately 15 miles north and east
of Denver. The government is purchasing an additional 4000 acres
around the perimeter of the currently owned federal land to act as a
buffer zone. The site for the Rocky Flats Plant was selected because
it best met the following criteria:
1. Located in Nebraska, Kansas, Oklahoma, Mississippi
Arkansas, Colorado, or the Texas Panhandle.
2. Area requirements of two miles by two miles square.
3. Supporting population of at least 25, 000 no less than
five or more than 25 mile distant.
4. Minimum displacement of homes.
5. Dry, moderate climate within 10 miles of a railroad
near good major highways, and a community airport
served by north-south and east-west airlines.
6. Large military air field within 50 miles.
7. 12, 000 KW electricity.
8. 1, 000, 000 gallons of water per day.
-------
692
Since the initial plant construction, several major changes have
occurred in the surrounding communities of significance to the
plant operation. These include a significant increase in the
population of the Denver area; population growth in the general
direction of the plant; the establishment of the City of Broomfield
approximately six miles northeast of the plant; the establishment
of the Jefferson County Airport approximately four and a half miles
northeast of the plant, and the acquisition of Great Western
Reservoir in 1955 by the City of Broomfield for use as a community
drinking water supply. The reservoir, which is on the water course
carrying the Rocky Flats aqueous effluents, was originally built in
1903 and enlarged in 1958. Nonradioactive releases from the plant
are controlled to conform with EPA regulations and discharge
permits. Radioactive discharges are controlled according to AEC
regulations.
The plant is part of the production complex of the Division of Military
Applications of the Atomic Energy Commission. It has been operated
since originally built by The Dow Chemical Company. The primary
function of the plant includes research and development, metal
working and chemical recovery. Plutonium is one of the primary
materials handled at the plant. Since the original plant operation,
extensive control techniques have been utilized to insure that
plutonium in liquid and gaseous effluents leaving the plant site are
below allowable standards and at the minimum practical level.
Improvements have continually been made in these control techniques
so that plutonium concentrations in air and water leaving the plant
site have been reduced and have been significantly under currently
accepted concentration guides.
Small amounts of plutonium have been released in the air and water
due to normal plant operations and due to accidental releases. Two
major fires have occurred at the plant site, in 1957 and 1969, in
which small amounts of plutonium were released to the plant site,
but no off-site releases were detected. Plutonium has been released
from the plant site over a period from 1958 to 1968 because of
leaking 55-gallon drums containing plutonium-contaminated lathe
coolants. Winds which occasionally exceed 100 miles per hour at
the plant site carried an estimated 0. 47 curies (7. 5 grams) of
plutonium over 1390 acres outside the federally owned property.
As a result, plutonium contamination exists in the soil outside the
currently owned federal land and the land presently being purchased
as a buffer zone in concentrations up to 10 d/m/g as compared to a
background from fallout of about . 05 d/m/g. Isolated spots may
exceed the 10 d/m/g.
-2-
-------
693
Since the original construction and operation of the plant, an extensive
environmental monitoring program has been conducted to insure that
all plant discharges were well within applicable standards. Air
water and soil are routinely analyzed for plutonium within the plant
site, at the plant boundary, and in the community surrounding the
plant. Background radiation measurements are made at various
Colorado locations up to 20 miles from the plant. All water discharged
from the plant is held in plant ponds and analyzed prior to release.'
In addition, vegetation and wildlife are also occasionally analyzed
for plutonium. The results of the environmental monitoring are
reviewed monthly with the Colorado Department of Health, the EPA,
and other state and local officials. In general, plutonium concentrations
in plant effluents have been less than 1% of the allowable standards--
for instance, during 1974, the average plutonium concentration in
water leaving the plant site was only . 05% of the standard and the
plutonium in the air at the downwind site of the buffer zone (which is
currently being purchased) was less than . 4% of the currently
accepted standard. This compares to the maximum measured
background concentrations of plutonium in water of . 03% of the
standard and plutonium in air of . 4% of the standard. During 1974
plutonium in Great Western Reservoir, which is the drinking water
supply for the City of Broomfield, averaged only . 002% of the standard
and plutonium in the Broomfield air averaged . 4% of the standard.
Both values are the same as found for background.
In addition to monitoring the surrounding community, an extensive
monitoring program is conducted at the plant. This program includes
monitoring the air in all of the working areas; multiple samplers and
continuous alarms at gaseous release points; periodic soil, vegetation
and animal analysis; monitoring of ground water through a series of
wells and periodic employee health examinations. An extensive quality
control program is included as part of all monitoring activities.
Although a few employees have obtained a plutonium body burden or
lung burden greater than the recommended amount, there is no
indication that any employee has suffered any health effect because
of this exposure or that there is any health hazard to the general
population because of plant operations. It is recognized that our
population is small and that sufficient time may not have elapsed for
health effects to appear, but to date, the record has been excellent.
In addition to the routine monitoring activities, several long term
research studies are under way to determine the movement and effect
of plutonium in the ecosystem. Several studies are being conducted
by the University of Colorado and Colorado State University to
understand the behavior of plutonium in the aquatic and terrestrial
environment. Other studies conducted by the USGS, AEC laboratories,
-3-
-------
694
and private consultants have been concerned with resuspension
and disposition of plutonium, the meteorology of the Rocky Flats
area, and possible movement of plutonium through ground water
and soil. Other long term studies are being conducted by Rocky
Flats employees including the chemistry of plutonium in soil,
methods of removing plutonium from soil by attrition scrubbing
and high gradient magnetic field techniques, particle size character-
ization in air, water and soil by fission track techniques, and
plutonium ecosystem modeling. The modeling includes an attempt
to quantitatively determine the amount of plutonium in each environ-
mental compartment, the rate of movement between compartments
and the long term dose commitment to human beings as a result of
the plutonium behavior. The difficulty in establishing this type of
model is in simplifying the very complex ecosystem into meaningful
compartments and assigning quantitative values to the various
compartments and the intercompartmental rates. Results of all
the studies to date have not identified any problem for man or
biological systems in general in spite of the above-background
concentrations of plutonium in the ecosystem near the plant.
In summary, the Rocky Flats Plant has been operated for about
22 years, during that time normal operations, two fires, and leaking
drums containing waste liquids, have discharged small amounts of
plutonium into the environment. There has been no demonstrated
hazard from past or present operations based on currently accepted
standards and the amount of plutonium in the air and water of nearby
communities is the same as found in background measurements.
Changes and improvements in operational procedures have continually
reduced the amount of plutonium released from the Rocky Flats Plant
due to normal operations and minimized the chance for further
accidental release.
I believe that it is important to establish credible standards for
plutonium because of the increasing concern of the public for
possible hazards associated with plutonium. In establishing these
standards, I believe the public must be assured that the standards ,
which are adopted are adequate for their protection. I believe that,
presently, nuclear materials are considered by the general public
to be a particular hazard. It is important for the public to recognize
that all of us are exposed to background radiation continuously and
that with proper handling and adequate standards, releases from the
nuclear industry will not appreciably increase the risk to their health
and well being.
I believe you have a difficult and complex task; however, one that is
exceedingly important to the nuclear industry and to the general
population.
M. A. Thompson
1-3-75
-------
695
CAS^ (Citizens Association For Sound Energy)
212.5 V. Clarendon Drive
Dallas, Texas 75208
Dr. William A. Mills
Director of Criteria & Standards Division
Office of Radiation Program
Environmental Protection Agency
Washington, D. C. 20^60
Gentlemen:
The following suggestions are submitted regarding setting of standards
for the transuranium elements. The remarks are general in nature and apply
to standard setting of all polutants for the most part as well as the
transuranium elements specifically.
1 ) Set "basic" standards based on biological evidence. Present standards or
recommendations are the results of groups of scientists trying to balance
societal needs against biological risks. A crisis of considerable proportion
is evolving concerning the public's confidence in technology and scientists.
This is largely due to past examples of a lack of professionalism and it is
suggested that the group of scientists be charged simply with determining the
biological risk which in turn is used in setting "basic" standards. After
"basic" standards (including air, water and soil permissible concentrations)
have been determined, a cost- benefit analysis may be employed to set "general"
standards for a given segment of our society.
2) Establish a 95& confidence level that the risk does not exceed a specified
value when evaluating experimental data. Much confusion has been caused in the
past because of the lack of a rigorous approach when making statements about
p
risks. Part of this confusion has arisen due to statements by Professor SternglassV
If he and groups such as yours would emoloy a rigoroas approach, much confxision
would be removed. And if extrapolation of experimental data is required, it
should be done in the most conservative manner and clearly labeled as an
extrpolation (or guess).
-------
2.
3) Adopt a criteria based upon the most susceptible person in the general
society when setting the "basic" standard. Sufficient research should be
conducted to determine the possible dosage to the most susceptible person
as a consequence of setting a given "basic" standard (and marginal consequences
should be simultaneously determined). All modes of transport and accumulation
(including water, air and soil) should be considered to determine where all
possible sinks of pollution may exist. Sufficient research to determine the
o
health effects (on all parts of the body ) of relevant dosages should also
be conducted. The "basic" standard should be set such that the most susceptible
person in the general society has a small chance of being affected deleterlously.
All persons not employed in an associated industry in a manner which insures
that they are entitled to full life and health insurance as well as retirement
benefits should be considered to be persons in the general society. The most
susceptible person concept does not eliminate a child, a fetus (unless lawfully
declared not to be a person) or a transient from consideration.
^) The rate of allowable additions of pollutants to the environment should
be limited in a manner consistent with the assumption that equilibrium
conditions have been attained. The present ambient conditions should be
evaluated in terms of both health effect and ecological (ability of the
environment to feed and, in general, allow the most susceptible person to
harmoniously exist) consequences. If additional releases are allowable,
conditions which assume that the release rate under consideration has been
taking place for a sufficiently long period of time to reach an equilibrium
state should be adopted. This criteria would limit the yearly rate of release
of PU-238 to approximately l/125th of the allowable ambient and PU-239 to
approximately l/35000th of the allowable ambient. Other approaches would not
be conservative.
5) Allowable release rates of each eligible portion of our society should be
apportioned. T-ftien making these allotments, the possibility and consequences
of accidents both on the plant site and in transit should be considered as well
as normal releases in determining the relative demand of ecah segment of our
society. These allotments should be made by EPA and the-possiBilitjr'of including
additional segments should be planned for by reserving an uncommitted portion
for such contingencies.
-------
3.
697
6) A cost-benefit consideration should be utilized at this point - not before.
If it is determined that the value to society of increasing the allowable
release rate of a segment outweighs the risk to society, zoning of areas where
the most susceotible persons are located should first be considered. If this
approach does not yield a suitable solution by itself, an appropriate increase,
which cannot be avoided by zoning, in the allowable release rate for that
segment should be granted. It should be required that all analysis take into
consideration health effects and/or ecological costs and that a common
measuring base be used, for all costs and/or benefits. A cross section of
disciplines should be used tc conduct the cost-benefit analysis under the
auspices of the EPA. All cost-benefit decisions should be periodically
reviewed to evaluate changes.
?) Application to EPA for point source releases should be required. The applicant
should assume that all other segments are operating at their maximum allowable
release rates when justifying his proposal. The applicant should show that
his point source addition rloes net cause any deleterious effects to the most
susceptible person - taking all spatial aspects into consideration with, regard
to all other point source emissions within the same segment which might interact
with his emission to the detriment of the most susceptible person. The consequences
of the proposed dosage to the most sensitive portions of the body should be
evaluated and justifyed. The decision as to which point sources are the most
desirable to society should be a joint decision between the SPA and the
cognizant body of the associated segment (the NRG, AKA, or Department of Defense).
8) Timely reporting of all releases should be required. Criminal laws to
protect the general public should make the user responsible to monitor all
possible release paths and report in a timely manner all releases whether
planned or unplanned - at the site or in transit. Similar laws should apply
to individuals within governmental agencies. A criteria should be established
whereby an accidental release rate which exceeds a predetermined value causes
the user to be automatically penalized. An effective program of continuous
govermental monitoring to assure compliance should be established. Until such
time that proven sufficiently accurate measurement techniques and instruments
become generally available! EPA should monitor at the source where much higher
concentrations exist.
-------
References
638
1 National Academy of Sciences, Biological Effects of Atomic Radiation,
Washington, D. C., 1956
National Academy of Sciences, Radiological Effects of Ionizing Radiation,
Washington, D. C., 1972
National Council on Radiation Protection and Measurements, NCRP Report No. 39,
1971
International Commission on Radiological Protection, ICRP Publication 9
2 Hull, A. P. and Shore, F. J.."Sternglasst A Case History", BNL 16613,
March, 1972
3 Blair, W. J., Richmond, C. R. and Wachholz, B. W.,"A Radiobiological Assessment
of the Spatial Distribution of Radiation Dose from Inhaled Plutonium",
WASH-1320, Sept., 1974
Tamplin, A. R. and Cochran, T. B., "Radiation Standards for Hot Particles",
Natural Resources Defense Council, Washington, D. C. 20036
22 +
Petkau, A., "Effect of Na on a Phospholipid Membrane", Health Physics,
, Vol. 22, pp. 239-244, March, 1972
4 "Reactor Safety Studyt An Assessment of Accident Risks in U. S. Commercial
Nuclear Power Plants", WASH-1400, August, 1974
"Comments by the Environmental Protection Agency on Reactor Safety Studyi
-. An Assessment of Accident Risks in Commercial Nuclear Power Plants", EPA,
November, 1974
Shappert, L. B., Brobst, W. A., Langhaar, J. W., and Sisler, J. A.,
"Probabilities and Consequences of Transportation Accidents Involving
Radioactive-Material Shipments in the Nuclear Fuel Cycle", Nuclear Safety,
Vol. 14, No, 6, Nov.-Dec., 1973
Rowe, W. D. and Holcomb, W. F., "The Hidden Commitment of Nuclear Wastes",
Nuclear Technology, Dec., 1974
Willrich, M. and Taylor, T. B., "Nuclear Theftt Risks and Safeguards",
Ballinger Publishing Co., Cambridge, Mass., 1974
"Environmental Analysis of the Uranium Fuel Cycle", U. S. Environmental
Protection Agency, EPA-520/9-73-003, 1973
5 Jarvis, A. M. and Easterly, D. G., "Measuring Radioactivity in the Environment -
The Quality of the Data", Nuclear Technology, Dec., 1974
-------
Commonw th Edison
One First Nalioi.oi Plaza. Chicago, Illinois £ Q Q
Address Reply to: Post Office Box 767 ^
Chicago, Illinois 60690
February 10, 1975
Director
Criteria and Standards Division
Office of Radiation Programs (AW 560)
U.S. Environmental Protection Agency
401 Main Street S.W.
Washington, D.C. 20460
Dear Sir:
On September 23, 1974, the United States Environmental
Protection Agency (EPA) published a notice of intention to
evaluate the environmental impact of transuranic elements and
to consider whether guidelines or standards were needed to assure
adequate protection of the public health and the environment.
(39 F.R. 34098) On October 24, 1974, EPA published a notice of
public hearing on this subject. (39 F.R. 37810) Commonwealth
Edison Company (Commonwealth) is in general agreement with the
statement submitted and the oral presentations by the Atomic
Industrial Forum and the United States Nuclear Regulatory
Commission in response to these notices. However, Commonwealth
believes that specific information should be added to the record
which delineates the actual impact of plutonium and other transuranic
elements which result from the operation of Commonwealth's seven
light-water reactor units. The following comments are submitted
by Commonwealth to provide this information.
Uranium fuel for light-water reactors usually consists of
high strength uranium-dioxide ceramic pellets. At fuel fabricating
plants, these pellets are hermetically encapsulated in zircaloy
cladding tubes; thereafter, fixed arrays of these completed fuel
rods are shipped, stored, and otherwise normally handled at individual
light-water reactors as integral assemblies. Rigorous quality control
and quality assurance procedures are conducted at each manufacturing
stage by the fuel fabricators to ensure the leaktightness and
integrity of the zircaloy cladding throughout the fuel's lifetime.
In addition, Commonwealth conducts quality assurance audits of each
of its fuel fabricators.
Prior to irradiation, normal uranium-dioxide fuel contains
no transuranic isotopes. However, during irradiation of the uranium-
dioxide fuel in the reactors, plutonium and other heavy elements
-------
700
Director
Environmental Protection Agency
Page 2
February 10, 1975
are produced through a variety of transmutation and radioactive
decay schemes. These transuranic atoms remain within the ceramic
fuel matrix and thus within the zircaloy cladding and under normal
conditions are not released to the primary reactor cooling water.
However, perforations develop in the zircaloy cladding during
commercial operation of light-water reactors, and test reactors
have been operated with intentionally defected fuel rods. The
data from both of these types of operations indicate that fuel
washout (the physical or chemical erosion of the fuel pellet and
subsequent release into the primary cooling water) is insignificant
in either uranium-dioxide or mixed-oxide fuel pellets. In fact,
the excellent chemical stability of uranium-base oxide fuels in
water coolant environments was an important consideration in their
selection for use in light-water reactors. Should the zircaloy
cladding perforate and fuel washout occur, transuranics could be
released into the primary coolant. Our measurements, to date,
show that Neptunium-239, a beta emitter, has been present in the
primary coolant. When Neptunium-239 in the primary coolant is
measurable, the concentration has ranged from 10~4 to 10~2 uCi/ml.
However, the measurements of Neptunium-239 in the radwaste system
storage tanks range from 10"^ to 10~^ uCi/ml. This reduction in
concentration could be the result of dilution by additional water,
decay of the Neptunium-239, the plating out on the reactor
"internals" or retention in the demineralizer resins or other
solid wastes from the radioactive waste treatment system.
The operational difficulties confronting a utility which
proposes to use plutonium-recycled mixed-oxide fuels are basically
the same as those associated with uranium-dioxide fuels. Criticality
considerations and the safeguard regulations must be observed for
both types of fuel. The basic difference is that the radiation
levels, particularly neutron radiation, associated with new mixed-
oxide fuel assemblies are increased, and thus, higher exposures to
workers may result from handling recycled fuels containing plutonium
as opposed to exposures resulting from handling uranium-dioxide
fuel. Nevertheless, it is still possible to maintain personnel
exposure well within acceptable levels. All experiments and
-------
701
Director
Environmental Protection Agency
Page 3
February 10, 1975
demonstrations to date indicate that utility operators can safely
receive, store, and handle mixed-oxide fuels. Irradiation in a
light-water reactor of either type of fuel assemblies causes the
assemblies to become intensely radioactive and thus the same
careful handling procedures are followed for both uranium dioxide
and mixed-oxide fuel assemblies. In essence, both types of fuel
assemblies are moved from the reactor core underwater by remote
handling equipment to storage locations outside the reactor
pressure vessel and the short lived radioactive isotopes are
allowed to decay. Since facilities do not exist at Commonwealth
Edison's nuclear power stations to reprocess or fabricate nuclear
fuels, the complete assemblies are shipped from the stations in
massive casks to a reprocessing plant where the plutonium and
uranium can be recovered for recycling into new fuel assemblies.
While large amounts of potentially valuable plutonium
can exist in depleted uranium fuel pellets, the exact amount
depends on many factors, including the type and capacity of the
reactor, the fuel design, and the extent of fuel depletion. At
the beginning of a typical operating period of Commonwealth Edison's
Dresden 1 reactor, 175 kilograms of plutonium would be present in
the reactor core. By the end of a 12-month operating period, 250
kilograms of plutonium would exist in the reactor core. The fuel
assemblies which would normally be removed from the core at that
t ime would contain 75 kilograms of plutonium, and 72 per cent of
this would be fissionable in thermal reactors. As another example,
at the end of June, 1973, Commonwealth Edison's Dresden 2 nuclear
unit, which is four times as large as Dresden 1, had 460 kilograms
of plutonium in the reactor core. By the end of June, 1974, the
reactor core contained 650 kilograms of plutonium and 80 per cent
was thermally fissionable. Finally, within four or five years,
each of Commonwealth Edison's new, larger, Zion units are expected
to have fuel assemblies removed each year which contain 155 kilograms
of fissionable plutonium. If Commonwealth Edison is allowed to
recycle the fissionable plutonium, an equivalent fuel saving of more
than 58 million gallons of oil or about 460,000 tons of coal can be
obtained per unit per year.
-------
702
Director
Environmental Protection Agency
Page 4
February 10, 1975
The capability of utility nuclear plant operators to
safely handle, store, and extract energy from nuclear fuels
containing encapsulated plutonium in light -water reactors with
no local impact on the environment has been demonstrated. This
experience provides a reasonable basis for the continued use of
uranium-dioxide fuel assemblies and the use of mixed-oxide fuel
assemblies using the present standards for light -water reactors
now set by the Nuclear Regulatory Commission in this area.
Very truly yours
Byrop Lee , Jr .1
Vice-Presiden
*US. GOVERNMENT PRINTING OFFICE:1975 630-513/794 1-3
-------
AW-560
U.S. ENVIRONMENTAL PROTECTION AGENCY
Washington. D.C. 20460
OFFICIAL BUSINESS
Return this sheet to above address, if you
do NOT wish to receive this material l~t
or if change of address is needed Q (indi-
cate change, including ZIP code).
POSTAGE AND FEES PAID
U.S. ENVIRONMENTAL PROTECTION
AGENCY
EPA-335
THIRD CLASS BULK RATE
------- |