U.S. DEPARTMENT OF COMMERCE
National Technical Information Service
PB-281 041
Natural Radioactivity
Contamination Problems
Conference of Radiation Control Program Directors, Inc
Prepared for
Office of Radiation Programs, Washington, D C
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PB 281 041
Published by
Office of Radiation Programs
^8§hingt@n, D.C. 204G0
&
REPRODUCCt) 8V
NATIONAL TECHNICAL
INFORMATION SERVICE
U S DEPARTMENT OF COMMERCE
SPRlNGFltlD VA 221GJ
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ORP Technical Publications
Publications of the Office of Radiation Programs are available in
paper copy from either the National Technical Information Service (NTIS),
Springfield, VA 22161 or from the Office of Radiation Programs.
Publications with PB numbers are available from NT IS; all others are
available from the Environmental Protection Agency, Office of Radiation
Programs (AW-460), 401 M Street, S.W., Washington, D.C. 20460.
EPA Technical Reports
520/1-76-001 Potential Radiological Impact of Airborne Releases and Direct
Gamma Radiation to Individuals Living Near Inactive Uranium
Mill Tailings Piles (PB-258 166)
520/5-76-005 Radionuclide Accumulation In A Reactor Cooling Lake
520/7-76-007 ORP Program Statement (PB-258 159)
520/2-76-008 An Examination of Electric Fields Under EHV Overhead Power
Transmission Lines
520/3-76-009 Reactor Safety Study (WASH-1400): A Review of the Final
Report (PB-259 422/AS)
520/1-76-01C Radiological Quality of the Environment (PD-254 615/AS)
'520/3-76-011 Significant Actinide and Daughter Activities from the
HTGR Fuel Cycle (PB-258 150/AS)
520/4-76-012 Recommendations Or. Guidance For Technic To Reduce Unnecessary
Exposure From X-Ray Studies In Federal Health Care Facilities
(PB-259 866)
520/4-76-013 Health Effects Of A1 pha-Eirittirg ^articles In The
Respiratory Tract
520/5-76-014 Radiation Dose Estimates to Phosphate Industry Personnel
520/5-76-015 Air Pathway Exposure Model Validation Study At The
Monticello Nuclear Generating Plant
520/4-7G-016A Environmental Radiation Protection Requirements For Normal
Operations Of Activities In The Uranium Fuel Cycle,
^ Volume I
520/4-76-016B Environmental Radiation Protection Requirements for Normal
Operations Of Activities In The Uranium Fuel Cycle,
Volume II
520/4-76-017 Environmental Analysis Of The Uranium Tuel Cycle (PC-25S 857)
520/4-76-018 A Preliminary Evaluation Of The Control Of Indoor Radon
Daughter Levels In New Structures (PB-252 670)
520/4-76-019 Federal Guidance Report No. 9: Radiation Protection
Guidance for Diagnostic X-Rays
520/5-76/020 Radiological Measurement At The tfaxey Flats Radioactive
Waste Burial Site - 1974 to 1975
600/4-76-027 Radioactive Prediction Model For Nuclear Tests
6C0/4-76-035 Factors Affecting The Use Of CaF :mn Thermoluminescent
Dosimeters Tor Low-Level Environmental Radiation Monitoring
520/E-77-001 Radiological Survey Of Puget Sound Navel Shipyard, Bremerton,
Washington and Environs
520/4-77-003 Considerations of Health Benefit-Cost Analysis for Activities
Involving Ionizing Radiation Exposure and Alternatives
520/4-77-005 Radiation Protection Activities 1976
52C/3-77-006 Summary of Radioactivity Released In Effluents From Nuclear
Power Plants Frorr. 1972 thru 1975
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BIBLIOGRAPHIC DAT A '¦ Hrpmi No. 1.
sheet EPA 5?P/i»-77-!I3
3. Mri ij»u hi'•. 'NrrriMni1 N,».
4. 1 il le uin! n 1e
NATURAL RADIOACTIVITY CONTAMINATION PRO BUM
5. Rrpoti ll.ur
February ]°7o
6.
7. Anfhor(s)
8. 1 'rriorntmg "ip,,int/.i(iiin Kept.
No.
9. I'erfuiining Organization Name and Address
A REPORT OF THE TASK FORCE
Prepared by
Conference of Rndiat.ion Central Program Directors. Inc.
10. I'rnject / I .i sk/tt ork Unit No.
M. (.ontfuci Airant No.
PHS 223-76-6018
EPA D7 -OC16S
12, Sponsoring. Organization Name and Address
U.S Environmental Protection Agency
Office of Radiation Programs (AW-^^S)
Washington, D.C. 20^60
13. !>pc of Report fc Period
Covered
14.
15. Supplementary Notes
16. Abstracts
Naturally-occurring radionuclides are ubiquitous in the environment. Under
various circumstances these radionuclides primarily from the uranium and thorium
decay series can contaminate the environment to the extent that they pose real
or potential public health risks. The investigation and regulatory control of the
impacts of most of these -sources have been greatly overlooked by Fededernl and State
agencies in the past.
This report provides an Initial assessment of the scope of the contamination
problems, the priorities for radiation control efforts, and recommendations for
problem resolution and implementation of effective control measures. Ibis report
is intended to assist those persons or agencies interested in the protection of
public health from naturally-occurring radionuclide contamination.
17. Key Words and Document Analysis. 17a. Descriptors
17b. ldcnt if icrs/Open-H nded Terms
Natural radioactivity
Radiological problems
Radi&tion contamination
Fossil fuels
Ground ¦water
Mineral extraction
17c. CIOSATI Held Group
Mineral processing Radon
Consumer products. Lead
Construction materials Polonium
Phosphate industry Zirconium
Uranium
Radium
18. Availability Statement
19. Sri urity ("lass (this
Report)
UM.I.ASSiril.P
21. No. o( Pages
f/°
20. Security la^s ( 1 hi*-
I'-ige
l!Nf I A^ll H
i7. I'rice /
pcfioyplfW
FORM NTIS-11 (REV. 10 731 | N[*1|
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EPA-520/4-77-015
NATURAL RADIOACTIVITY
CONTAMINATION PROBLEMS
A REPORT OF THE TASK FORCE
Prepared pursuant to
PHS Contract Number 223-76-6018
which is partially funded through
EPA Interagency Agreement D7-0968
Printed February 1978
Prepared by
Conference of Radiation Control Program Directors, 8ne.
With the cooperation of
U.S. Nuclear Regulatory Commission
U.S. Department of Health , Education and Welfare
Bureau of Radiological Health
and
(9
U.S. Environmental Protection Agency
Office of Radiation Programs
Washington, D.C. 20460
' *
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TABLE OF C_fWTE!-:T5_
P?.gt
Foreworc /
Preface v 1 '
Task Force Participants 1X
History and Purpose of Task Force 1
Phosphate Industry 8
R<-vi-;qica1 Aspects o' Thorium ar.d Ooahtpr Products ?'
Radio-activity in Fossil 29
Radium ana Radon in Ground Water 40
Mineral Extraction nnG Processing Activities 4*
Raoo'i in Csvos
Standards and Guidelir.es Radioactive Material in Consumer
and Cor.':truction Products 04
Radioactivity in Construction Materials 51
Related EPA-Task Force Activities 73
Statutory Authority of States to Regulate Naturally-Occurring
Radioactive Materials 76
P.ecor.i.iendfl tions 78
Attachments
Attachment A 8?
Attachment B C5
Attachment C 90
Attachment 0 92
Attachment E 94
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FOREWORD
The Conference of Hadiatior Conti-ol Program Directors is an organization
whose membership is comprised of all directors of radiation control programs
in the 50 States, the Territories, and some large municipal agencies.
The Conference was formed to serve as a mechanism for providing a more
functional means of exchanging information between State and Federal agencies
as well as between States themselves in areas of mutual concern or interest.
Additional objectives and purposes of this Conference are to:
(1) Promote radiological health in all aspects and phases.
(2) Encourage and promote cooperative enforcement programs with
Federal agencies and between related enforcement agencies
within e^ch State.
(3) Collect and make accessible to all radiation control program
directors such information and data as might be of assistance
to them in the proper fulfillment of their duties.
(4) Foster uniformity of radiation control laws and regulations.
(5) Support programs which will contribute to radiation control.
(6) Assist members in their technical work and development.
(7) Exercise 1 eadership witn radi.vJor, control professionals and
consumers in radiation control development and action.
The Office of Radiation Programs of the Environmental Protection Agency
carries out a National program designed to evaluate public health impact
from ionizing and nonionizing radiation, ana to promote development of
control necessary to protect the public health and ensure environmental
quality. In this regard, the Environmental Protection Agency (1) develops
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radiation orotec.tion standards, criteria, and guidance, {?.) conduct
special '.tvirc-nnsctital studies, (3) evaluates radiation exposure trends,
(4) assesses radiation control technology» and (5) provides technical
assistance to State and local agencies responsible for radiation control.
The Office of Radiation Program:., through funding and direct technical
assistance, supports the Conference of Radiation Centre 1 Program Directors,
Inc., in its objectives and activities to assure an effective federal/
State partnership ir. limiting unnecessary environmental and public radi-
I
ation exposure. Selected Conference reports are published by the
i
Environmental Protection Agency and are distributed to Federal , State and
lees! radiation protection personnel, industry, libraries, laboratories,
and other concet nod grcups ant', individuals. These publications are for
sale by the Government Printing Office and/or the National Technical Infor-
mation Service.
Reader:; 3i*c encouraged to rep-.-rt errors or omissions to the
Conference or the Office of Radiation Programs.
X . /
• I- O,
. P,
Gerald i. Parker V.'. ft. Kowe, Pli.D.
Chairiran Deputy Assistant Administrator for
Conference of Radiation Control Radiation Programs
Program Directors, Inc. environmental Protection Agency
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PREFACE
Naturally-occurring radionuclides are ubiquitous in the environment.
Under various circumstances these radionuclides primarily from the
uranium and thorium decay series can contaminate the environment to the
extent that they pose real or potential public health risks. The
investigation and regulatory control of the impacts of most of these
sources have been greatly overlooked by Federal and State agencies in
the past. In order to initiate effective control measures in this
radiation protection problem area, the Conference of Radiation Control
Program Directors, Inc., established a Task Force to assess contamination
by naturally-occurring radionuclides and assist the States and Federal
agencies in devloping appropriate radiation protection guidance and
criteria. The Tas'k Force consisted of representatives from several
State radiation control programs with resource persons from the Environmental
Protection Agency.
This report provides an initial assessment of the scope of the
contamination problems, the priorities for radiation control efforts,
and the Task Force's recommendations for problem resolution and implemen-
tation of effective control measures. This report is intcnted to assist
those persons or agencies interested in the protection of public health
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This document should be of special interest to State, local, and
Federal radiation protection personnel in the United States and,ot:-.er
countries.
L. Hall Bohlinger, D.Sc.
Nuclear Projects Coordinator
Nuclear Energy Division
Division of Radiation Cortrol
Richard J. Guimond
Criteria l< Standards Divinon
Cffice of Radiation Programs
Environniental Protection Agency
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TASK FORCE PARTICIPANTS
Task Force No. 7 consists of the following membership:
L. Hall Bohlinger, Chairman
Nuclear Energy Division
Louisiana Department of Natural Resources
Gary F. Coothe
Radiation Control Service
Oregon Department of Human Resources
Oayne H. Brown
Radiation Protection Branch
North Carolina Department of Human Resources
Michael Christie
Radiation Control Section
Idaho Department of Health and Welfare
Ulray Clark
Radiological and Occupational Health Program
Florida Department of l-'ealth & Rehabilitative Services
In addition, the following individual served as a resource person to the
Task Force;
Richard J. Guimond
Office of Radiation Programs
U. S. environmental Protection Agency
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H'STORY AND PURPOSE OF THE TASK FORCE
Task Force No. 7 on Natural Radioactivity Contamination Problems
was established by the Executive Committed of the National Conference
of Radiation Control Program Directors in 1975 as an extension of Workshop
No. 5 of the 1974 Annual Meeting of the N'CRCPD.
The charge to this task Force is to:
(1) Provide assistance to the Conference, individual States,
and Federal agencies in scoping the problem of contamina-
tion by natural radioactivity;
(2) Assist in developing appropriate radiation protection
guidance and criteria;
(3) Assess the impact of naturally-occurring rr.dioactivity
c.ontarcri nation in the gene-al environment ar,:! the Conference
member States; and
(A) Serve as a "focal pc'nt for State input to the progr?^s of
$ Federal agencies.
The charge given necessarily implies certain resDonsibilitic-s in
which the Task Force must assist the appropriate State and Federal
agencies. These include the following:
(1) Defining the radiation level or concentration or stag? of
ri i< .3 v.h' ,u rrti';"?"! V'-.-cciirri n j radio native naterinl
b'lC'j.'t1; a ¦. >¦: <¦ j t'i--:1. l.n Lh? en v. ".;r,r,K;.t;
(?) Tying i-;hu Vjs ujlhc-ity tu d^/elj; ar.d implement
guidelines and criteria for enforcement action;
(3) Identifying the impact that naturally-occurring radioactive
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(A) Examining the need for control on the use of products and
byproducts containing fIGRM and the associated economic, impact
of such control;
(5) Defining the sources currently known or suspected to contain
possibly hazardous amounts of NORM and describing other
potential problem areas; and
(6) Recommending priorities for control programs to address NORM
problems.
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INTRODUCTION
Natural radioactivity and its associated radiological impacts have
generally been overlooked in the past. Although there have been strict
controls on other sources of radiation such as byproduct material, X-ray
machines, special nuclear material, etc., natural radioactivity control
has been minimal, perhaps due to the fact that it is "natural" rather
than "man made" radioactivity. This lack of strict controls has been
due in part to the fact that the Federal Government has limited juris-
i
diction over naturally-occurring radioactive material, and control was
left previously up to the States, who often times did not have adequate
programs to deal with.radiation. While there are over 100 naturally-
occurring racicmuclides, public health problems are usually limited to
the 30 or more rsdionoc.lides in the uranium and thorium decay series
became of their relative abundance and toxicity. The increased incidence
of bone cancer in radiur. dial painters and lung cancer in fluorospar and
uranium miners are examples of undesirable health impacts due to exposure
&
to these radionuclides. Other examples of increased population exposure
to .NORM include the radon problems in several Western States due to the
use of radioactive tailings and the use of reclaimed phosphate wining
'land in Florida.
The majority of the work of this Task Force does not deal with what
is usually, referred to as truly natural radiation exposure, but pore
appropriately is concerned with exposure to radiation occurring as a
result of alteration of the natural sources by technology. This new
;ategory for human radiation exposure, introduced by Gesell and Pritchard,*
is termed "technologically enhanced natural radiation" (TENR), and is
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defined as "exposures to truly natural sources of radiation (i.e.,
naturally-occurring isotopes and cosmic radiation) which would not occur
without (or would be increased by) some technological activity not expressly
designed to produce radiation." This exposure to increased radiation
from living in a structure constructed over phosphate nining reclaimed
land would const:-tute a TENR exposure; however, an exposure from a
radium needle would not, since the latter is expressly designed to
produce rat'iatio.n. It is interesting to note the EPA in their May, 1976
report, "Radiological Quality of the Environment", has estimated from the
sketchy data available, that for individuals, the largest radiation dose
received from all sources is derived from TENR. This results'in 140-
14,000 millirers per year to the tracheobronchial surface tissue of the
(¦cinq, mainly a.; a result of innalation of radon daughter products from
nr.-.:/ur :ril" i.e. i 1 \r-. . AdcHi onal I v : T he tt-.ir;', largest calory of
population Jose is estimated ic be from TEIJR which contributes approximately
2 pillion pers-!-;en per yea; internal exposure. This internal dose
results- fro;i exposure to ore r,.ning and Milling, radon in potable water,
naLdral 'jas, LPG, (r.i nes, caves, and in geothermal enei gy procuctior,, and
radioactivity ir. construction materials. Tin's is comparable to the dose
received -from the use of radiopharmaceuticals , which is the scccnd
largest category cf population dose cor.tr i cuti r.g slightly greater than
3 "-illiori person-Pern per year.2
It is the objective of liris Task force to collect and study available
information and data on naturally-occurring radioactive materials in the
envi rennent and to rr.dke recommendations to the Conference regarding the
need for evaluating, monitoring, and controlling natural radioactivity.
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The problem areas examined by the Task Force are as follows:
A. The phosphaie industry
C. The radiological aspects of throium and daughter products
C. Radioactivity in focsil fuels
D. Radium and radon in ground v/ater
E. Mineral extraction and processing activities
F. P.adon in caves
G. Standards and guidelines for radioactive material concen-
I
trations in material and consumer products
(i. Radioactivity in construction materials
I. Statutory authority of States to regulate naturally-
occurring radioactive materials.
The Task Force has developed a series of recommendations based on
findings and conclusion of data, and mod?l State regulations have been
developed for potential incorporation into the CSG model State regula-
tions and adoption by-those States where such action may be warranted.
In November 1375 , the first formal meeting of the Task Force was
held in Orlando, Florida. During this time, the members toured the base
phosphate mining area of Central Florida and visited several housing
projects built on reclaimed land in order to obtain a perspective on th«?
magnitude of the problem. Radiation surveys were taker, using a Micro-R
meter over reclaimed land and hnusing projects, near slag piles, and
over roads constructed wi-:i phospnate byproduct material. A report of
ihiL reetir-g was sut-mitted to the Conference in January 1976 and can
be made available to interested parties. Later in September, 1976, a
fo!low-jr> meeting was ^eld in Baton Rouge, Louisiana, at which time Task
Horce members toured a wet process phosphoric acid production plant,
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prepared a working outline for preparation of the final report, assigned
specific areas to be completed by the members, and established preliminary
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REFERENCES
1. Gesel] , T. F. and Prichard, N. M.< The Teclmolepical Iv Enh.inced
Natural Radiation Envirom.ent:' Health Physics, V. 28, Mo. 4, ]97f>.
2. RiidioJojrica] (Quality of the Environment, U. S. EPA, QRP,
EPA-52/1-70-010, 1976.
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PHOSPHATE KJDUSTRY
The radioactivity of phosphate rock was probably first observed in
1908 when the British physicist R. Strutt (1908) found that samples of
phosphorite were several times more radioactive than the average rocks
of the earth's crust. More recent studies of the concentrations of
I
natural uranium and thorium in phosphate ores produced in the United
States indicate that concentrations of these natural materials range
from about 10 to 400 ppm (5.4-267 pCi/gm) and 2 to 20 ppm (0.4-4 pCi/gm),
1 7
respectively. 'c Uranium daughters in the phosphate ores, at least
through radium-226, are usually in secular equilibrium.
Industrial Operations
In 1974, the total U. S. production of marketable phosphate rock
was about 46 million tons.^ At present, the domestic marketable phosphate
rock production accounts for about 40 percent of the total world pro-
duction. The Florida phosphate industry produces about 80 percent of
the total domestic phosphate rock output. The remaining output originates
from several Western States. Consequently, the large scale operations
of this industry in one regional area may lead to.several types of
impact on the environment including that ;.ne i ¦K'ieociiv" imp-,"-i
in the ores, v;astes, and other ire-toria 1 s.
The standard mining practice in Flor'rii to ••trip t1'? overburden
and mine the phosphate matrix. This overburden is slacked on 'ir.ir.itied
ground adjacent to the irining area. Approximately 50t;o acres of land
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arc mined per year in Florida, removing about 163 million cubic yards of
overburden, and extracting 112 million yards of matrix. In the Western
U.S., dry mining technics are used extracting the ore with power shovels
and shipping it to manufacturing facilities in trucks and rail cars.^
At the beneficiation plant, the matrix is processed to upgrade its
concentration. The output materials from this operation are
marketable phosphate rock, sand tailings and slirnes. These materials
are produced in a ratio of about one to one to one. Table 1 lists the
uranium, thorium, and radium-226 activities for these materials.
TABLE 1: Natural Radioactivity Concentrations in Florida
Phosphate Mine Products end Wastes ipCi/gni)^
Mate-- 1 Ra-226 U-23S Th-230 Th-232
l-'arV.etnble Ruck 42 4?, 3 0.44
Slimes 4L <14 48 l.£
Sand Tciiinas 't.'j C.3 4.2 0.89
In beneficiation, water is used for processing in addition to
bei'-o used as a transportation medium, 'lined-out areas are used for the
disposal of sand tailings and slirr.es, in addition to overburden. Several
Florida slime ponds have discharges to t/>c eivironnei't, and br-neficiaticn
wastes are present in the slimes. The concentration of rhssolved radi-ji7.-226
in sliine discharges was less than 5 pCi,'liter at all facilities. The
..nniss^l ved radiun:-2?6 concentration ranged from 10 to .1000 pCi/liter
*:id v/as hiyhly dependent on the total suspended solids in the slimes.
Although no chemical process is used to treat the discharge from the
slime ponds, concentrations of radium-226 in effluents were all less
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than 3 pCi/liter. The reduction of total radiuin-226 from the raw slime
discharge to the effluent discharge ranged from 92 percent to greater
than 99.9 percent. This was primarily due to the removal of suspended
solids by settling. Consequently, effective solids removal technics are
necessary to insure minimal release of radium-226 to receiving waters.
Marketable phosphate rock is processed into two major products,
fertilizers and elemental phosphorus. Processing for these products
takes place in "wet process" phosphoric acid plants and electric furnace
plants, respectively.
I
In the "wet process" phosphoric acid plant, the raw materials are
ground phosphate rock, 93 percent sulfuric acid, and water. Phosphate
rock is mixed with the sulfuric acid. This reaction produces phosphoric
acid and gypsum. Following the reaction in the attack vesso., the
nnxture is riltered to the gypsum from the pho~phcv'ir. acid.
T!i^ gypsum is pumped as a slurry to a large pile near the facility where
it is allowed to dewater. 5ince eppro>imately 4 metric tons of cjypsor,
are produced per ton of phosphoric acid, a largo phosphoric acid plant
t.
would produce about 2.5 million i.ietric tons of yypsum per year."
•".pproximc t*-i y cms percent of the r^diu.n-^b, 60 to 80 percent of r.ne
i,,;i.cr iurn-2 V: fsf) pe'Tcof the i;ranur: in phosphate rock are dis-
•.O: ^ - iO t '• >.'i i.n sulfuric aci'!.
Tab":"- '.:ts the "'.verage radioacti v; ty coneyurat'.cns foi' i: e
f,T.' i 1 lzc" "irn-: ts ana p'ost'-t-ciiyps^R byproduct of sc-ve rd'l v.'et-prucess
f3._1l1i.icj m Florida. Phosphoric acid sar-ples w*-re fc;i:d io
conuin fro-' 50,000 to 10C.CSG pf:/liter iiraniuni-236 and about 1000
pCi/litef radiuM-22'L-. The concentration of uranium appears to vary
:ir"c;.'v .vith the cci' ,-ntrat ion of P?0._.
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TABLE 2: Natural Radioactivity Concentrations in
Materials Produced from Florida Phosphates (pCi/gram)
Material P.a-226 U-238 Th-230 Th-232
Normal Superphosphate
21.3
20.1
18.0
0.
.6
Diammonium Phosphates
5.6
63
65
0.
.4
Concentrated Superphosphate
21
58
48
1.
3
Monoammonium Phosphates
5
55
50
1.
.7
Phosphoric Acid*
1
25.3
28.3
3.
.1
Gypsum
33
6
13
0.
.3
*29 percent acid.
Each "wet process" phosphoric
acid plant
incorporates a large
cooling pond (¦*¦ 500 acres) of contaminated water for recycle in the
facility. During periods of excess rainfall it becomes necessary to
discharge water from these ponds to nearby streams. Field studies at
several Florida facilities indicate raw process water contains approximately
50 to 90 pCi total radium-226 per liter and approximately 400 to 2000
pCi/liter of uranium-238.
To prepare process v/ater for discharge to the environment, the pH
must be increased from 1.5-2.0 to 6-9. To accomplish this, slaked lime
is normally added to the discharge water in a step called "double liming."
Studies have shown that this treatment is highly effective in removing
radionuclides from the effluent. P.adium-226 reductions of greater than
96 percent we re observed in all situations studied. Similar reductions
in uranium and thorium were also observed. As a result of the effective-
ness of this treatment, EPA discharge permits usually stipulate an
acceptable pH range of 6-9 for treated effluent to ensure minimization
of radioactivity ir phosphoric acid plar.t discharges.
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In the thermal processing of phosphate rock, silica and coke are
added; this mixture is electrically reduced to form elemental phosphorus.
Ferrophosphorus and calcium silicate slag byproducts are also formed in
the process. Data from analyses of these samples indicated that most of
the uranium and radium-226 present in the input phosphate rock is trans-
ferred to the slag during the process.
Reclaimed Land Use
Approximately 100,000 acres of land have been mined for phosphate
rock in Florida. To date, about 25.000 acres of the mined lands have
been reclaimed for residential and commercial development, farming, and
grazing. It is estimated that about 1000 structures have been built on
these lands. Since reclaimed lands are composed of overbjrden, leach
zone material, matrix, sand taiMngs, and/or slices, they frequently
contain radiu'n-226 concentration substantially higner than the 0.1 to ?.
pCi/gram typical of U.S. soils. Concentrations u:j to 93 pCi/gram have
been measured in these roc'aimed soils. However, radium-226 concen-
trations in the reclaimed land soils generally range between 10 to 30
pCi/orarn. Such radium-226 concentrations often persist to soil depths
greater than 20 feet. Due to the elevated soil radium-226 concentra-
tions, a considerable quantity of radon-222 is produced. This racion-?22
diffuses to the ground sfrfocc ar.o th»-c.i."jh t;:-.-r-;onc r ? ?.»
where it can lead to the biiilcur; of short-; i" .->J f.i....... -;«r
indoor environment. Data on avc-rag; gross " >c- -••i" -=
over a one-year period wore obtained for several st*-::.-:1.v.-c--. ',elLr'.eJ .:L
radom ori reclaimed 1 nd and on land distant from the Florida phosphate
region. The data from these structures are summarized in Ta:;'le 3.
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TABLE 3: Percentage Range of Radon Daughter Levels
Reclaimed Land (rvf!3)
Nonreclaimed_ Land_(n=9^
0.05 to 0.1 WL
0.01 to 0.05 WL
0 to 0.01 WL
38«
w> J 'j
31%
0.05 WL
0.01 to 0.05 WL
0 to O.Ul WL
-0-
22*
From the data obtained to date, it is believed that >:he potential
excess lung cancer risk associated with the higher levels, warrant
additional studies to delineate more fully tne scope and magnituae of
this problem. Based on the assumption thit c-xcoss lung c-'inccs will
double per 60 CWLM exposure, we con associate the highest annual average
working level observed of 0.1 k'L for continuous occupancy :nv an avenge
lifetime (70+years), with a 6 to 10 times increase in l'jn
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{.c-eal d i:>c.h;:rqes to surface waters to loss than 3 to 4 pCi/nter.
two principal : ivers in 1:10rido recoiviny such effluents are the
tVocr* fiivei s. L'st i.i:j ii o-i cf the- population dose resiil 1. i :in
fnv, .'J I schanjes to the sr.- rivers depends 0:1 the total discharges, i.he
1' '¦ vo1" crn.",... the lumber of mines ciischorgii»g, and iho licv.ns tr c-air
"¦or'.;.la! io 1 /VI of lhes° factors arc quite variable froi'i •.'.¦¦¦ ar to yc-e*'
and season to season in Florida. However, it is high1> unlikely that
nonral discharges fVom mines and phosphoric acid plants to these Rivers
would result in -a 01 c. n-?^6 concentrations greater than 0.5 pCi/liter
above norp-a! to downstream users. However, accidental failure of sliine
pond dikes could s^nificantly increase the radium-226 concentrations in
vhe ri-.'ers since slices contain greater than 2000 pCi/liter total
rad i i'lir i.2v-.
i'y shallow wel'i water supplies in the (Jentr-ii Florida. area have
'. ¦ e: £sbr/.n to contain rad i ;i>n-?26 coneentra L ions greater than the lin-it
of 5 pCi/liter i^d i ¦./.-•¦i- XP6 arid rad iui;i-22o established by M10 Lnvironiritntal
Protection Agency's Safe f)-'inking Water Regulations of 1975. rlov.-eve^,
since no asscss-nent '.-as made of these ground waters prior to extensive
mining, it is presently uncertain to what extent the levels are due to
the natural presence of uranium in pnosohato ores or the operations of
the industry. Additional work is underlay to investigate this Question
further.
Data collection and evaluation of a1?- emissions 1vot e~e::;;i!f :.l
phosphorus and uhospberic acid plants are incomr.lete. Havener. there
are sore peellminjry indications that signif icant cuan(.i ries of Po-210
-------
.-ay he edited ¦">,om these facilities due to voldtization durinc calcining
or furii'jre opera tioris.
Workers in the phosphate operations come in close contact with
large amounts of phosphate ores, products, and wastes along with inru 1 ,'tion
of Just generated by unloading, crushing, drying, and other acti-i tier..
, i
The worst exposure situations were observed in areas of high dust con-
centrations and in or around the phosphoric reactor vessel and its
associated equipment. Based on normal worker occupancy and radiation
levels measured in Florida facilities, it has been estimated that direct
gatnnia dose, equivalents for workers ir> piiOi>phoric acid or elemental
r
phosphorous plates range from 30 to 300 mrein per year.' fhe annual
dose ecHivdlenl rate to the tracheobronchial region of the lung, due to
inV. labor. of radon daughters, has been estimated to be a high r.s 5
re.n/yr {those workers. Estimates of the avenge lung dose wot!Id of
course oe very much lower.
Fro;:! the data collected and analyzed to date, population exposures
to ttif Indoor radon daughters ii: structures appear to be the most signi-
ficant public health problem, and efforts are being made to develop
r?ch?tion protection guiCL-iines to evaluate and control exoosurc-s to
\>.is source. As an interim measure, the CPA has provided i.he State o<
Florida a screening level v;hieh allows continued land development without
a significant health impact. This interim guide-line is based on a gaiwa
exposure of less than 10 uR/hr (including background) v.hirh can be
associated with a estimate of o radon daughter level less than 0.0! WL.
Other aspects of tMe industry which require Further sti.dy incl^-.c-
trio impact of using byproduct slag aMd gypsum for construction :To;.er :als.
-------
tie uptake* of '-ad icnucl ides by crops due to fertiliser use c; growing on
reel air.eci iao-v.-, evaluating control technulog i es to limit indoor radon
dfli; ghter levols, assessing the impact of recovering u rani urn fuel from
phos::hp'Viteri.ils, and the use of cef 1 uorinV.td phosphate as a livestock
feed supplement.
Phosphates as Livestock Feed Supplements
The presence of uranium (2-130 ppm) in livestock feed supplements
has been reported in proportion to their phosphorus content. This is
due aDparerr.ly 10 the transfer of uranium with phosphorus from the
original rock phosphate to the feed regardless of whether the mineral
has been chemically processed or used more or less directly. The occurrence
of radium-2?6 in the feed supplements falls into two groups depending
upon the type of phosphate material used, and is either 70% of the
equilibriun: amount or 67. of the equilibrum amount. Beneficiated defluori-
nated phosphate rod: has been shown to contain the higher an.ount of
radium-<:¦?6 winle feed supplements utilizing fertilizer phosphate as s
; rivalry source for phosphorus exhibit the lower radium concentration.
'3as(-d cn mr t;;Dcl ic studies of uranium ingested by dairy cattle with
iiorirv.i diet, and assuming the maximum transfer of uranium (0.2")
the highest U:P ratio feedstock directly to the cow's milk, the
following data is derived.
elemental phosphorus requirement for 600 Kg lactatiny dairy
cow - nn/day
Daily ingestion of uranium if supplement prov.ides 257 P -
0. Q]G on
Concern:at 'Ois of uranium in milk assumino ?0 liters per
H^y ].f_. y+v/1
-------
Thus it appears that the uranium content of feed supplements should
not bo cf great realth significance to the cow or mar. based 011 current
yjkiol ines.
C.' --reaver concern v.as the radium in the supplemenis. Using the
i.'Oii ;Vj cow and assuming (1) that 0.G2'.- of the dose of ingested radium-226
is secreted into the cow's milk per liter and (2) that the highest Ra:P
ratio fee-'i was used to provide 25% of the cow's P requirement, then the
contribution of the supplement to the radium content of milk is calculated
1
to be 0.7, pCi/l. The cow's daily ingestion from the supplement would be
i.'.pjj'V'v^tely 3?r.i3 pCi. Publ ished volumes for rndiuri in milk ranee from
O.G'J-O.j pCi/l. The TRr. recophvended ma/.in.um periv.i^sibie radium-226 dose
lor a huiTian being is P.G pCi/day. In order to achieve this ingestion
rate, one w.-uld have to censure approximately 29 liters of milk per day.''
As >-esult of the foregoing, the radium corvi.ent. of feed supplements
does not appear sufficient to result in a significant Transfer to human
beings; however, more data would be desirable to confirm this conclusion.
One additional item of consideration with respect to natural radio-
activity in feed supplements concerns the storage of large quantities of
material in warehouses andthe possibility of radon buildup resulting in
occupational exposure. Data is currently unavailable for evaluation of
this potential exposure, however research is currently on-yoing.
This Tisk Force does not consider the radioactivity in livestock
feed supplements to be high priority at this time and will not include
specific recommendations; however, we will continue to evaluate related
studies and will defer any conclusion until such time that additional
research in this area can be completed.
-------
Uranium Recovery
Uranium foe use as a fuel in nuclear power plants has historically
been extracted from Western ore;; containing high concentrations of the
element. At present, Western ores mined for their uranium values average
about 0.2 percent uranium. With the existence of high grade ores waning
and the price of uranium drastically increasing from $8 per pound to over
$40 per pound, UjOg low grade deposits are becoming more important.®
Two types of ore which contain uranium in economically recoverable con-
centrations based on today's technology and economic climate are phosphate
and copper.
The production of phosphoric acid results in dissolving about 80
percent of the uranium in the ore.^ Through technology developed at Oak
Ridge National Laboratory (ORNL) and several industries based upon
solvent extraction .methods, it is now possible to recover 90% or more of
the uranium from the phosphoric acid.^ Present estimates indicate that
uranium can be recovered from large wet-process phosphoric acid plants
for about $8 - SI5 per pound U3O3 using variations of the basic ORNL
process.^
-All present practicable uranium recovery techniques for phosphates
apply only to phosphoric acid. Further, recovery from lower production
volume plants may be ir.ore risky and costly than others. While recovery
from facilities with the capacity of 200,000 tons P2O5 per year nay
become practicable, initial recovery efforts will probably te restricted
to larger facilities. In 1976, the capacity of wet-process phosphoric
acid plants (greater than 200,000 tons Per year) was about 7 million
-------
tons P.Or- This oi:iourit of phosphoric acid would contain about 10 million
£ j
pounds of Uo0o which is e^ouwh to fuel about 20 one thousenn i'fioaw,itt(e)
o O
nuclear power plants per year.
The U.S. Environmental Protection Agency is presently conducting
studies to determine the envi.'Cin;or.tnl impact, of uranium recovery from
' 2
phosphoric acid.' In cenoral, potential e.vposurrs are anticipated
to result fron emissions, effluents, dust in calcinmci and packaging
operations, and transportation. At this tine, it is di f-^r >:i t to esti-
mate the potential impact although it is not expected to be of major
sicr- i ficanre.
L'rjniu:'! >"0cc>very f.-c:- i.ocr leach solutions tnrc.r.h lun r-xc'ianrje
is i\ Hi:' considered il several n'ine-nill operat ions. "hi. potential
radi;, ic-jicil '"'peri ;t> ttr:recover/ rs 'j'• r.¦ 'w:¦ -;i p^ese; although it
shon"!!.e si:'"lt.r t'.> .on r-xchdnq-j i.pera?.af preser.s i.icnt.M '.'ir.es.
-------
REFERENCES
1. Menzel , R.G. "Uranium, Radium, and Thorium Control in Phosphate Rocks
and their Possible Radiation Hazard," J. Agr. Food Chenu, Vol. 15, No.
2, pp 23i-?3£ (1963).
2. Guimond, R.J., Windham, S.T. "Radioactivity Distribution in Phoipi.f^e
Products, Byproducts, Effluents, and Wastes, 0RFJ/CS0-7fj-3, U.S. environmental
Protection Agency, Washington, D.C. (August 197'6).
3. Stowasser, W.F. "Phosphate Rock," 1964 Bureau of Mi ties Mi_noraT_ Yearbook,
preprint, IJ. S. Department of Interior, Washing tori, D.C." f 1976X-
4. Office of Radiation Programs: ''Prel i mi nary Findings - Radon Daughter
Levels in Structures Constructed on Reclaimed Florida Phosphate Land,"
Technical Note ORP/CSC-7^-4, U.S. Environmental Protection Agency
(September 137L;).
1
5. Slack, A.V.; ed. "Disposal or Use of Gypsum," Phosphoric Acid, Vol. 1,
Part 111 (196?-).
6. Windham, S.T., Partridge, J.. Horton, T. "Radiation Dose Estimates to
Phosphate Industry Personnel," EPA-5^0/5-76-014, U.S. Environmental
Protection Agency. Montgomery, Alabama (1976)
7. Reid, D.F., Sackett, W.M., and Snalding, R.F., "Uranium and Radium in
Livestock Feec Supplements", Health Physics
S. U.S. Congress Joint Committee on Atomic Energy Hearings before the
Subcommittee- on Legislation of the Joint Comir,;ttee on Atc-mic Energy on
Physical Research; Nuclear Materials, 94rh Congress, 1st session,
9. Guimond, R.J. and Uindham, S.T. Radioactivity Distr but.ion in Phosphate
Products, By-products, Effluents, and Wastes, Office of "Radiation
Programs, Envi ronrner.tai Protection Agency, "echnical Note ORP, CSD-75-3,
August 1975.
10. Hurst, F.J. and Crcuse, D. J., Recovery of uranium from wet-process
phosphoric acid by extraction with octylphery1 phosohonc acid, jndustrjal_
Engineering Chemi ca 1 Process 0escrj ptions a_n_d Developments , Vol. 13,
pp. 285, July 1974.
11. Bieniewski, C. L., Persse. F. H. and Branch E. F., Avai 1 ab'i 1 i ty of
Uraniuni at Various Prices from Resource_s_in the United States , Inforniation
Circular 8501, United States Department of the Interior, Bureau of Mines,
1971.
12. Davis, W. , Haywood, F. F, and Walsh, P. J., Progress Report for March, 1977
on EPA sponsored Project - "Control of Radiological Impacts from Kecovery
of Uranium from Phosphate Ores, Products. By-Products, and Wastes,"
Cak Ridge National Laboratory, April, 1977.
-------
RADIOLOGICAL ASPECTS OF THORIUM AMD DAUGHTER PRODUCTS
Thorium-232 is the 35th most abundant element in the earth's crust,
0.001 to 0.002 percent being most generally accepted. It is about three
times more plentiful than uranium-238.
Uses
In addition to the thorium fuel cycle which is currently under
investigation, thorium has long been used in the following non-nuclear
applications:
A. Before the advent of nuclear energy, thorium was used chiefly
in the manufacture of gas mantles because of the brilliant
light-emitting qualities of their oxides. Even to this day,
the Coleman gasoline cam,) lanterns find continued use with the
mantles.
B. Thorium coated tungsten wire has been used for a long time as
cathodes in vacuum tubes. Because of the low thermionic tork
function, the thorium can produce high electron emission.
Where size of the focal spot is not vitally important (for
example, water or oil-cooled therapy tubes), ana in uses
demanding high X-ray emission efficiency, thorium may replace
tungsten to increase X-ray production and strength.
C. Tungsten-thorium alloys increase the efficiency of filaments
for incandescent electric lamps.
-------
P. Thorium finds increasing use in heliarc welding of tungsten
electrodes because it offers the advantage of instant arc
starting and arc stability. Welds made with 10 percent Th-Ko
filler are ductile even at room temperature.
E. Thorium is an important alloying element in magnesium, imparting
high strength and creep resistance at elevated temperatures.
Thib is because of its high melting point (3220°C). Many
aircraft structural parts contain this alloy with magnesium.
F. Thorium oxide is the most stable of the refractory oxides and
has been used to a limited extent in specialized melting
operations as crucible construction material and in other
ceramics.
G. Highly purified thorium in small amounts goes into special
optical glass giving it a high refractive index and a low
dispersion. Consequently, they find application in high
quality lenses for cameras and scientific instruments.
H. Thorium oxide also has industrial use as a catalytic agent for
oxidizing sulfur dioxide to sulfur trioxide in the production
of sulfuric acid, in the conversion of ammonia to nitric acid,
in the making of water gas from carbon monoxide and in petroleum
i.- 1
cracking.
Sources
As a consequence of its inability to form soluble higher valency
compounds, only six minerals containing thorium as an essential con-
stituent are known, compared with about seventy uranium minerals.
-------
Unlike most other rocks and minerals, thorium-bearing minerals are not
soluble in water, and so are not destroyed during erosion. Instead,
they accumulate as placer deposits in riverbeds and in sand on ocean
beaches. There are thorium veins known to exist in thi.s country and
other places in the world just recently discovered. Should there be a
heavy need for thorium in the future, these veins could be exploited.
The three most significant minerals from which thorium has been recovered
are nionazite, thorianite, and thorite. The world's supply of thorium
\
has been obtained most entirely from monazite. Monazite, ThPO^, a
phosphate, is very brittle, fractures unevenly and is radioactive. It
is sufficiently magnetic to concentrate electromagnetically in a strong
field. It occurs characteristically as a very minor accessory constituent
in granitic and syenitic igneous rocks. These rocks seldom contain
enough monazite to warrant recovery, but the natural process of erosion
concentrates the monazite sand?, in the beach and stream deposits:
Monazite occurs typically as small but distinctive round, glassy grains,
colored honey-yellow to yellowish-brown. Thorium occurs as a trace
element in various mineral deposits including rare earths.
The principal monazite sources have been the beach sands of India
and Brazil. Monazite concentrations in commercial or near-commercial
quantities can be found in numerous geographic areas within the continental
U.S. On the East coast are stream placers or old beach deposits in the
Carolinas and Florida (Jacksonville Beach). The most important commercial
deposits are found in Idaho, particularly along stream and river placers
on the western edge of the Idaho batholith, a large granite area in the
-------
central part of the State. Thorianite, ThO^, is soluble in sulfuric
acid and is slightly less radioactive than pitchblende. Thorianite
deposits in Madagascar are now being commercially worKed for thorium.
It is also being processed in Siberia and in New Zealand. Deposits have
also been reported in sand and gravel beds in Canada, California and
Montana. Thorite, ThSiO^, the third major mineral containing thorium,
is principally found in the beach sands in South Island, flew Zealand.
Similar deposits u<~e found in Central California gold placers, especially
along two rivers, the Tuolumne and Consumnes. As mentioned above,
recent discovery of thorium veins in the U.S. containing either monazite,
thorionite, thorite or all three, could provide a great resource for
this country easily exploitable in the near future J
Preparation
The established thorium extraction process starts from monazite,
the chief conmercial ore. Monazite is chemically inert, and the dissoluti
or "opening" process must be drastic; highly concentrated solutions of
sulfuric acid or sodium hydroxide at HO^-IGO0 C are used. The thorium
phosphates are rapidly converted to sulfates with the liberation of
phosphoric acid. Dissolution of thorium sulfate in water and basic
separation by addition of ammonia gives essentially thorium hydroxide.
The thorium hydroxide is dissolved in nitric acid and the slurry is
allowed to go through an evaporation process. Another breakdown with
sodium hydroxide-followed by water washing produces the oxide. Also
use is made of the oxide's magnetic quality allowing further magnetic
-------
the radioactive inert gas daughter thoron, which is liberated from the
mineral or breakdown. The oxide, like the mineral thorianite, can then
be reduced with calcium to form tie pure metal.(2,3)
Radiological Problems
The extraction of thorium from its ores leaves thorium-238 in the
purified material which decays directly to the short-lived (T'5 3.64 days)
/'
parent of thoroii. Even outside of the mining and extraction of thorium,
commercial non-nuclear usage, i.e., in mantle making, ceramics, electronic
tube filament making and other such industrial handling, there is the
hazard f"'om the inhalation of thoron (radon-220), a daughter product of
thorium. There are not near as many epidemiological studios compared to
radon-222 in the providing of evidence for an exposure-risk rel-ationship.
Although natural levels of thorium in soil and construction materials
are comparable to and in many cases exceed those of radium and uranium
in the source form of monazite sands or thorite ores, there is not the
seepage problem ,~:,sociated with thoron (T-'s = 55 seconds) as v/i th
radon-222 (T'i =¦ 3.!i days). The short half-life of thoron means that the
air concentrations are generally much lower than Lho^e for radon whose
diffusion period through the ground is comparable to its half-life.
Thus the prime concern for the hazards relating to the daughter products
of thorium are narrowed around the extracting processes and the industrial
A
machining and usage of the metal.
The deposition of the thoron decay products depends mainly or. (1)
the fraction of inhaled uncombined radioactive atoms; (2) the particle
size distribution of the carrier aerosol of the combined radioactive
-------
atoms; (3) the concentration of thoron daughters in the local atmniph?>~e;
and (4) the degree of attachment of these daughter ions to the aerosol
particles. The consequent lung dose further depends or. the deposition
distribution in the tracheobronchial tree and within the various mucous
layers. The "working level" concept originally applied only to radon
daughters (MPC's). This lias, however, been extended to include thoron
daughters.- A thoron working level used to be defined as equivalent to
the potential alpha energy released due to the complete decay of 100 pCi
of eac!i of the thoron daughters per liter of air as was done for radon.
However, now the preferred definition is merely any combination of radon
daughters including thoron which on ultimate decay will liberate 1.3 x 10^
MeV of potential alpha energy per liter of air. In light of the original
definition, the thoron WL appears to be 13.5 times greater than the
radon WL.^ This all usion does not, however, mean that the dose to tho
respiratory tract on exposure to one thoron WL is also 13.5 tines
greater than that due to an exposure to 1 WL of radon daughter. The
radon daughter elements deposited in the lungs undergo radioactive decay
at the site of deposition because of the short half-lives involved,
whereas the thoron daughters, having comparatively longer half-lives,
are partially eliminated by biological processes. In fact, calculation
shows that approximately 43% of the thoron daughters only remain with
the lungs and decay. This translates to a lung dose of only about 5.8
times that delivered by an equivalent concentration of radon daughters,
all other conditions being identical.
The latest radiological activity surrounding thorium-thoror, and the
daughter products has been a decision on the most correct lung model to
-------
be used in describing inhalation doses. There has been a preponderance
of models from different authors all producing widely uncomparable
results. In spite of the differences, the studies all agreed in conclusion,
that the highest alpha dose should be expected in the upper and medium
bronchial region. This result is of great importance in the inter-
pretation of the enhanced lung cancer mortality.
The current problems, concerns and activities surrounding the
radiological aspects of thorium, thoron and the daughter products seems
to be centered around the determination of doses to the various respiratory-
related organs as a result of inhalation of the daughter products. In
summary thorium seems to present just as much of a problem as does
radon and its daughters, but perhaps of a slightly less hazardous nature.
-------
REFERENCES
1. Staat?, M.H., "Thoriur, Veins in the United States', Ccon. Geol., Vol. 69,
1974, pp. 444-507.
2. Nininqer, R.D., Minerals Per Atomic Energy, D. Van Nostrand Co., Princeton,
N.J., 1956 2nd Ed.
3. Smith J.F., Carlson, O.N., Peterson, D.T., Scott: T.E., Thoriurn: Preparation
and Properties, The Iowa State University Press, Ames, Iowa, 1975.
4. .Jaccbi, W., "The Dose to the Human Respiratory Tract by Inhalation of
Short-Lived Rn-222 and Rn-220 Decay Products," Health Physics, Vol. 10,
1964, pp. 1163-1174.
5. Khoru A.M., Dhendayuthem, R., Raghavayya, M., and Nambiar, P.P.V.J.,
"Thoron Daughter Working Level," Paper delivered by the Health Physics
Division, Bhahha Atomic Research Centre, Bombay, India.
-------
RADIOACTIVITY IN FOSSIL FUELS
Description of the Problem
It is generally known that fossil fuels contain trace quantities
of naturally-occurring radioactive materials in the uranium and thorium
decay series! The U. S. consumes vast quantities of fossil fuels. For
i
example, a single 1000 MWe coal-fired power plant would consume about
560 tons of coal each hour, and would produce about one-half million
tons per year of ash. Even with only trace quantities of radioactive
materials in these fuels, the large volumes of fuels consumed would
involve the re-distribution of significant amounts of radioactivity into
the envirorment. The problem addressed in this section of the report is
what the States, EPA and other members of the Conference should do in
evaluating, monitoring, or controlling radioactivity from the utiliza-
tion of fossiI fuels.
Activities to Date
The radiological impact of natural gas as a source of radon has
(1 2 31
been evaluated by several investigators. ' ' ' The Bureau of Radiological
4
Health has conducted a radiological survey of an oil-burning power plant,
and the EPA has conducted a similar stud'. around a coal-fired power
plant utilizing Eastern coal.D The Oak Ridge National Laboratory has
measured trace elements rt the- Allen coal-fired steam plant which also
utilizes Eastern co.il.^ The Idaho Department of Health and Welfare,
Radiation Control Section has performed an evaluation of a proposed 10C0
MWC coal-fi^ed power plant which would utilize Western coal.''
-------
The conclusions and recommendations in this report are based in
part on the resufts of the above studies.
Areas of Concern
A. "Natural Gas
Natural gas contains radon which emanates from radium-bearing
geological strata. Doses to the bronchial epithelium from
radon in natural gas consumed in homes have been estimated by
8
the EPA. The annual dose committment from radon in natural
gas has been estimated to be 2.73 x 10^ man-rein. This dose
committment is based on radon concentrations in natural gas
being 20 pCi/1.
The annual dose committment appears to be insignificant when
compared to background and other sources of radiation. In
view of the limited future use of natural gas due to depleting
supplies, the total environmental dose committment becomes
even less significant.
It appears there could be a localized problem with natural gas
if concentrations of radon in gas approached 357 pCi/1. This
may be possible for users close to the well head. Such levels
could result in radon concentrations in houses on the order of
1.0 pCi/1 which might cause indoor radon daughter levels to
approach .01 WL.
In view of the small potential dose committment from radon in
natural gas and the high radon concentrations in natural gis
-------
necessary for a local radon problem, no recommendations are
made here regarding the continuous evaluation or monitoring of
radon gas exposures from the use^of natural gas. However,
evaluation of specific uses, especially those close to well
heads may be warranted.
B. Oil
Oil contains trace quantities of uranium, thorium and their
daughters. No environmental distribution of radioactive
material around an oil-fired power plant was observed by
Gordan. The radium-226 content of fly ash from oil-fired
plants is 21 times less than the rodium-22fi content of fly ash
Q
from coal-fired plants. It would appear then, that the
radiological impact from oil-fired plants would be insigni-
ficant. Therefore, no recommendations are m^de here regarding
the continuous evaluation or monitoring of oil-fired plants.
C. Coal
It is generally known that coals contain varying concentra-
tions of uranium and thorium and the radioactive daughters of
these elements.
According to a paper by J. D. Vine^, large potential reserves
of urani;i.i; are contained in ccal and lignite, and the con-
centration of uranium in the ash of coal provides a oossible
means of recover^ ig uranium as a byproduct. Uranium bearing
lignite occurs in the Fort Unio.-, formation of Paleoceno age in
the Northern Great Plains, in tnc- Salt Lake forn:.;tion of
-------
Pliocene age in Southern Idaho, and in Tertiary sediments in
Nevada and Southern California. Uranium-bearing coal is
present in the Wasatch formation of Focene age in Wyoming, in
the Laramie formation of Cretaceous age in Colorado, and in
the Bear River formation of Cretaceous age in Idaho. Bituminous
coal and anthracite in North Central and Eastern United States
contain only very small quantities of uranium.
Vine reports that the uranium content of Western lignite
varies from 0.001 to about 10 percent and averages 0.008 percent..
Western coal samples from Wyoming and Idaho range from about
0.001 to 0.05 percent uranium with averages being about 0.003
percent for Wyoming and 0.05 percent for Idaho. The author
points out however, that hinh rank, low ash coals of the type
most des-ired for fuels are rarely uraniferous.
In a paper by Stocking and Page^ , the uranium content of
coals, especially Western coals, is reported. The difference
in the uranium content of different types of coals is not
entirely a consequence of the availability of uranium.
Laboratory experiments demonstrate that peat, lignite, and
subbituminous coal extract 98" of the contained uranium from
aqueous solutions, while bituminous and anthracite (the 'jpe
of coal most suitable for fuel) capture less tnan a fifth and
slightly more than a tnird, respectively.
1 7
In a report by Aberncthy :i-d Gibson , values of the uranium
concentrations in Western coal are, on the average, 2 to 1C0
times higher than in Eastern coal.
-------
The radiological implications of the extensive combustion of
fossil fuels has been briefly dealt with in past literature.
The radium-2?6 concentrations in European coals, in fly ash
from power plants, and in contemporary fossil snows have been
documented. Trie radium-226 releases into the atmosphere as a
14
result of burning Appalachian coal have also been discussed.
There has apparently been very limited radiological surveillance
conducted around fossil fuel power plants. Two such studies
were conducted by the Oak Ridge national Laboratory and the
15
U.S. Environmental Protection Agency. Both studies concluded
that the utilization of fossil fuels for power generation does
not present a significant radiological health concern; however,
it has been pointed out by Rowe that these conclusions may
reouire modifiration for the utilization of Western coal,
since both studies add-vjssed only low uranium content Eastern
i 16
coal.
The Stcte of Idaho has evaluated the radiological impact from
a proposed 1000 MWe coal-fired plant to be constructed near
Boise.^ The proposed plant, called Pioneer, was to utilize
Western coal from l:yomi ny.
IdUe yiv;>s the estimated releases from such a plant and
conparts these releases to maximum permissible release con-
Tvn'crcino'is to unrestricted areas. The assumptions used in
-------
Table. For example, it was assumed that the concentrations of
uranium and daughters was 0.23 pCi/g and the concentration of
thorium and daughters was 0.18 pCi/g. The efficiency of the
electrostatic precipitators was assumed to be 99.7". It
should be emphasized that if lower grade coals containing more
radioactivity are used, and if the efficiency of effluent
controls goes down, then radioactivity releases could be much
higher for a specific power plant.
Table 2 gives the results of fly ash analysis taken from the
Idaho report. The fly ash samples were from the Jim Bridget'
coal-fired plant in Wyoming, which utilizes Wyoming coal from
a different deposit than the proposed Pioneer coal. It can be
seen from Table 2 that radium concentrations in fly a^h average
about 3.1 pCi/g. It appears possible that radon levels in
houses constructed in fly ash disposal areas could be elevated.
In view of the Idaho report and other papers cited here, the
following recommendations are made regarding coal-fired plants:
(1) The radiological aspects of each proposed coal-fired
plant should be evaluated by the appropriate agencies.
Radioactive releases should be estimated from an analysis
of the coal to be consumed and the operating characteristics
of the proposed plant. This recommendation is especially
pertinent to any proposed plant that intends to derive
its fuel from low-grade, uraniferous Western coals.
-------
(2) The States, the EPA, or other appropriate agencies should
proceed to measure radon levels on fly ash piles and in
structures built in fly ash disposal areas, if there are
any.
(3) The EPA and appropriate Slates should study and evaluate
uses of fly ash from coal-fired plants, particularly
those uses which are likely to cause elevated radon
levels in habitable structures.
-------
TABLE 1
ESTIMATED AVERAGE AIRBORNE 'RADIOACTIVITY RELEASES FROM PIONEER - TWO UNITS, 500 Mw„ EAChO)
RELEASE CONCENTRATION
MAX. PERMISSIBLE RELEASE
f(2)
TOTALS
(1) Assumes:
% RELEASE
I_S_0_I0_P_E
—iiiijM-iLJAjii
CONCENTRATIONS (uCi/ml -x 1014)
STANDARD
Uranium Series
23Su
4.63
200
2.31
234(j
4.63
400
1.15
230Th
4.63
30
15.43
226Ra
4.63
200
2.31
222Rn
1545
300,000
0.52
210po
1545
700
220
210Pb
4.63
800
0.57
Thorium Series
232Th
3.63
100
3.63
228Ra
3.63
100
3.63
228jh
3.63
20
18.15
3.63
2,000
0.18
212Pb
3.63
70,000
0.01
267.89 %
RELEASE/YR
(Ci)
0.0031
0.0031
0.0031
0.0031
1.0280
1.0280
0.0031
0.0024
0.0024
0.0024
0.0024
0.0024
2.083 Ci
(a) 0.3% release of all trace elements in coal except 210po and 222pn (i00% release).
(b) Uranium and thorium are in equilibrium with daughters.
(c) Coal contains 0.23 pCi/g U and 0.18 pCi/g Th.
(d) Total effluent is 4.48 x 10^ ft^/rnin.
(e) b62 tons of coal is consumed per hour.
(2) Maximum permissable releases of airborne radioactive materials to unrestricted areas - Idaho Radiation
Control Regulations, Part C, Appendix A, Table II. Assumes radioactive materials particulates are
-------
TABLE 2
Jim Bridger Fly Ash
ANALYZ1T) BY
ISOTOPE
Uranium Series
F.lv Ash £1
(12/75)
pC: /^ ) * o<2>
NOTES:
(1) Based on dry weight.
(2) o is one standard deviation due to counting statistics.
Fly Ash #2
(11/75)
pCi/gyl) o(2)
LFE
23Su
8.5S
- 1
2.57
1 .3
lit:
230-^
7.0
1 .4
3.3
.2
if]';
22(>
¦1.9
i .2.
2.4
- J
rc:s
226^
3.8
1 .3
ijt:
21°pb
18.0
i 1
3.0
; .2
CO
Thorium Series
1 ijt;
232Th
4.7
1 .3
2.8
-------
REFERENCES
1. Johnson. K.II. , Jr., Bernhardt, O.K., Nelson, N.S., Gil Icy, 11. W., Jr.,
1973. Asses^Tioni of l\>tential Radiological Health Effects l'ro;n Radon
mi Natural Gas, EPA-520/1-73-001Wa;-!unf;ton. D.C.
2. Gesel 1, T.I'.. 'kj'jJJr'i ^''pl i cat Ions of [^idon iH Natural Gas
and Na 111ra 1 Gas PnxU'.cl s - Final Report. A rojxjrt of lho University
oi Texas Health Science Center at Houston, School of Public Healtti, 1973.
3. Barion, G.J., et.. al . , Contribution of Radon in Natural Gas to the
Natural Rndioacfivitv in Homes. Oak P. i dice National laboratory Report
'IV-1154, 1973] " ~ "" '
4. Gordon, J.A., 19G8. In tori ri Pnport of t_he Slrrtv of Pub He Ilea 1 th Ascpcfs
oi' Fossi 1 Euo 1 and Nuclear Pov.er Plants. Southeastern Hadjological Health
Laboratory, Bun.--a 11 of lladio logical Health, U.S. Public Health Services.
5. P/xiresian, P.H. , Easterly, D.C-., Cunmin^s, S.L., 1970, "Radiological Survey
Around Power Plants Usinj; Fossil Fuel", Office of Research and xV)tiitorjng,
U.S. llnv 1 ronnx.'ntal Protection Agency, EERL 71-3.
6. 13o 1 ton, N.E. , 1974, ^race Elanent Measurements at. the Coa"i-l-'i red Al len
Stream Plant, Progress Rejiort, June 1971-1973, Oak P.id^e Nati.onal laboratory,
ORNI^-NSF-EP-43."
7. Boothe, G.F. , 1976. An Evaluation of the Radiological Asjjects of the
Projxrsed Pioneer Cnal-Fired Plant. Radiation Control Section, Division
of' Lnvi ronment. IdaTx) Department of Health and Welfare, Boise, Idaho.
8. Reference No. 1
9. Reference No. 4
10. Vino, J.D., &956, "Uranium Dearinjx Coal in the United States", Con I ribut ion
by 1 he United St_a_tes Geological Survey aiid At^innc¦ Energy Coiinission for
j he L'ni ted Nat. 1011 's International" Conference (in Peaceful Uses of At/«vic
Li^vi'gy, C>« a. > logical 8ur\ey Proiessional Paper 300, U.S. Government Printing
"Ofl'ice, Washington, D.C.
11. Stocking, H.I:. and Page, L.R., 19f>6, "Natural Occurrence of Uranium in
tin? United States—A Simnary", Contributions to the Grology of Uranium
and Thorium by the Un:,tec! States Geological Survey and Atonic Energy
Conroission or the United Nation's International Conference on Peaceful
Uses of Atonic Ijierj^-, Glopjea 1 Survey Profess .on;:1 Paper 300, U.S.
Govenm-nt Printing Office, Y:a.shingtO'i I.C.
12. Abernethy. H.F. and Gibson, P.H. , 1973, 'Trace Elonents in Coal", U.S.
Department o! Interior, 3ureau of Mines IC 8163.
-------
13. Jauorowski, Z., Bilkiewicz, J. and Zoylica, E., 1971, "Ra-226 in Contemporary
and Fossil Snow', Health Physics, 20, 449.
14. Reference No. 6
15. Reference No. 5
16. Rowe, W.D., 1975, A letter to Ms. Margaret Reilly, Department of Environmental
Resources, P.O. Box 2063, Harrisburg, Pa., Deceriber, 1975.
17. Reference No. 7
-------
radium and radon m ground water
Description of the Problem
It is common for ground water in areas throughout the United States
to have widely varying concentrations of radium, radon and radioactive
daughter products. Radium may range from trace ouantities to over 50
pCi/1, while radon (both in the presence and absence of significant
radium concentrations) may oe found in concentrations greater than
50,000 pCi/1 - ^ •>2,3) nobia gas> ration in water is readily released
with mild aeration. However, the radioactive dauqhters in various
stages of equilibrium will remain in the water. Because of the potentially
high levels of radon in water, it is oossible iri private and commercial
uses to create significant working levels in air.
Radium in water and radon in air have been the subjects of much
Federal interest and research, resulting in appropriate standards.
However, inadequate attention has been devol.ed to the health signifi-
cance of ingested and inhaled radon and radon daughters from notable
water supplies. A large segment of our population is subjected to
exposure to all of these naturally-occurring radioisotopes through the
use of private, commercial, agricultural, public, and community ground
wa^er supplies. In addition, geothermal water may become another sig-
nificant source of highly contaminated water.
Activities to Date
After extensive study and deliberation, Federal regulations have
been established for radium in drinkinq water.^ Additionally, several
-------
States have initiated and/or completed studies of radium and radon
concentrations in their ground water supplies. However, only a limited
amount of research has been done on the health effects of ingesting
radon and its daughters. Much of what has been done is through uncoordi-
nated efforts and has been inconclusive. Researchers have evaluated the
radium decontamination characteristics of conventional water treatment
techniques and have also developed and evaluated special radium removal
techniques.^
Area of Concern
If the EPA drinking water regulations are to be enforced, there
will be a large number of ground water supplies which will be required
to undergo radium removal procedures. As this occurs, consideration
wi 11 have to be giver, to the disposition and disposal of radium con-
taminated water treatment residues.
While much work has been dor.e on the health effects of raden in
air, very little has been done to quantitatively evaluate the health
significance of high radon levels in water as a source of airborne
concentrations. ^Judging from the high levels which are seen in water
and from the private and commercial uses of water in poorly ventilated
areas, airborne radon due to aeration cf water may have significance.
Duncan,, et. al. have calculated that water w'th 1000 pCi/1 radon-22? could
6
result in air concentrations of 1 pCi/1 due to normal residential use.
Further, they have estimated that if a population uses potable water with
a radon concentration of 500 pCi/1, 20 health effects per year might
result from inhalation for every one million people exposed.
Because of the comparatively large concentrations associated with
radon and its daughters in arinking water, it is des'raule to better
-------
understand the health significance of these radioisotopes from the
viewpoint of ingestion. Little work has been done in this area, yet it
is not uncommon for individuals over their entire lifetimes to daily
ingest radon and its daughters, as well as radium, from highly con-
taminated supplies. Further, since contaminated around and geothermal
waters may be used for food crop irrigation, there are ouestions which
r:ust be answered regarding human exposure through the food chain.
Before the public health impact of the sources can be determined, con-
siderable laboratory study is needed in the area of radium and radon
daughter transport and dosimetry in the environment and man.
-------
REFERENCES
1. Grime, W.N., Higgins, F.B., Smith, B.M., f-ehaffey, J.R., Jr., "Natural
Radioactivity in Ground Water Supplies in Maine and New Hampshire",
Project No. A-473, Georgia Institute of Technology! Atlanta, GA (October 1960).
2. Golden, J.C., Jr., "Natural Background Radiation Levels in Florida",
SC-RR-68-196, Sandia Laboratories, A1 buqueroue, N.M. (May 196R).
3. Fong, S.W., Mantiply, E.D., "Environmental Radiation Surveillance 1974-1975
Report", DFS-i863, N.C. Department of Human Resources, Raleigh, N.C. (1975).
4. Environmental Protection Agency, "Drinking Water Regulations - Radionuclides",
Federal Register, Vol. 41, no. 133, pp. 28402-28409, J-.iy 9, 1976.
5. Brinck, W.L., Schliekelman, R.J., Bennett, D.L., Bell, C.R., Markwood, I.M.,
"Determination of Radium Removal Efficiencies in Water Treatment Processes",
ORP/TAD-76-5, U.S. Environmental Protection Ayenc", Washington, D.C. (December
1976).
6. Duncan, D.L., Gesell, T.F., and Johnson, R.H., "Radon-2?2 in Potable
Water," Conference Proceedings, Health Physics Society Tenth Midyear
Topical Symposium: Natural Radioactivity in Man's Environment, October
12-16, 1976, Saratoga, New York.
-------
'MINERAL EXTRACTION AMD PROCESSING ACTIVITIES
N-ji'iorous industries such as copper, fluorospar, vanadium, bauxite-,
litc'iium, and r.-re earth's mining and processing, extract ores which
often occur in strata containing above-average concentrations of uranium,
thorium, and their daughter products.
Unfortunately, liit.le investigation has been done to assess the
radiological impacts from these industries. However, sufficient data is
available to provide an overview of the copper mining and processing
iidu?;.ry and Lhc zirconium extraction process.
Major copper deposits occur generally in three regions of the
United States. These are tne Appalachian Province, Keweenaw Peninsula
(upper Michigan), ard the Cordilieran Province (southwest United States).
The latter region, consisting of Arizona, Ulan, IJew Meyico, and Nevada,
encompasses the largest deposits.
Open pit mining accounted for 89 percent of the cooper extracted in
the United States in 1973 with underground mining method supplying the
remainder. There are three broad methods of beneficialion utilized in
the copper industry. They are hydrometallurgical processing, physical-
cnemic?! separation, and 1each-precipitation-floatation.
The processing activities involve the production of solid wastes,
effluent streams and emissions.
As Figure 1 details, four areas of potential occupational and/or
public radiation exposure have been identified for the copper industry.
For underground mining, hazardous occupational radon levels could result
*This subject was excerpted from the following paper: Fitzgerald,
Joseph, "Radioactivity in liie Copper Or-1 Mining and Dressing Industry",
Proceeding of the Tenth Midyear Topical Symposium of the Health Physics
Society, pp. 58-80, October 11-13, 1976, Saratoga, New York.
-------
from the presence of a uranium co-ceposit. With open pit mining, the
disposal, storage, or utilization of waste rock from a uraniferous
deposit could have a public health impact if not controlled. Likewise,
the discharge of large volumes of pumpout water and seepage frcm tailing
ponds could have an impact on public water supplies in the area. Efforts
have been made to collect radiological data, when available, for each of
these effluent pathways.
Still provides a detailed analysis of the uranium and thorium
occurrence in porphyry copper deposits.^ his geological surveys at the
Copper Cities and Castle Dome open pit mires in Arizona have shown a
positive relationship between the deposition of uranium and the occurrence
of porphyry copper. Assay data from the Copper Cities mine showed
uranium concentrations in the ore body to exceed that of normal igneous
rocks of the same composition in this region (about -1 ppro) by a factor
of 11 to 38. An average concentration of up to 100 ppm is estimated
for the primary copper zone of this nine.
Similar surveys performed at Castle Dome also showed evidence of
this geological co-occurrence, although at lower uranium concentrations
of about 20 ppm. Frequency distribution graphs for the uranium assay
data obtained from 45 feet bench composite samples, are provided for the
two mines in Figures 2 and 3.
Still concludes that uranium exists in commercially extractable
concentrations in a number of porphyry copper deposits. The author
notes, however, that assays at other mines showing relatively low uranium
content indicate that the occurrence of uranium with copper is a site-
specific phenomenon associated with certain geological conditions.
-------
STANDARD DEVIATION = 0.0029 %
MEAN = 0.0055 ^
-4-
u
¦4—T—j l I
I
01234567S9 10 Id 20
£ CHEMICAL U3Q8 x 1C00
(.. c. 7 = 0.007)
FREQUENCY DISTRIBUTION GRAPH
URANIUM CHEMICAL ASSAY DATA,COPPER CITIES
Ml SAMPLES
FROM STILL. A P . URANIUM AT COFFER C'TICS AND OTMHR PORPHYRY
COPPER DEPOSITS, MIAMI DISTRICT, ARIZONA (UNPUB. THESIS), HAP.VAR
-------
Moxhan, et aK_ measured the radiation levels of hydrothennally
altered rocks in the vicinity of several copper and copper-lead-zinc
2
deposits in Arizona. The study sites were the Bagdad porphyry copper
deposit, the United Verde sulfide copper deposit, and the Old Dick and
Iron King copper-lead-zinc sulfide deposits. The survey measurements
obtained for the Bagdad deposit are graphed in Figure 4.
A recent geological survey of uranium concentration is reported by
Davis and Guilbert for several open pit porphyry copper mines in Arizona
and fiew Mexico. Their results are tabulated in Table 2. These levels
are not consistent with background levels, which are on the order of 4
ppm for igneous rocks of this region. One explanation for these observations
is t'.at the ore samples analyzed are not from the highly mineralized
primary ore zone, but from associated zones. Assuming, though, average
concentrations in the mineralized zones an order of magnitude higner than
they observed, the low levels still resulting would also lend support to
the premise of site-specificity for uranium occurrence.
Another source of radiological data is the pumpout waters of mines,
both open pit and underground. The Office of Radiation Programs, EPA,
undertook a survey of radioactivity levels in such effluent for copper
mines in Michigan, Montana, and Arizona.4 The mine operations surveyed
are the u'mt.e Pino (Michigan), Butte Montana), the Old Reliable, and
Bagdad (both A> icria). The radioacti vity levels measured are tabulated
in ~cb.s 3.
In several underground copper mines, radon daughter concentration
levels have posed potential health hazards to mining personnel. As part
-------
TABLE 2
Average Abundances of Uranium in Porphyry Copper Intrusions
and Barren Intrusions of Similar Composition*
Average
Range
Location
Occurrence
Sampies
ppm
ppm
Urani um
Uranium
New Cornelia Nine
mineralized stock
17
1.25
2.1-0.4
New Cornelia Pluton
barren intrusion
12
0.68
1.3-0.2
Mineral Park Mine
mineralized stock
25
0.79
3.5-0.1
Gross Peak-Martin Ridge
mineralized stock
13
0.46
0.9-0.2
Turquoise Mountain
mineralized stock
23
1.27
2.4-0.6
Morenci Pit
mineralized stock
23
0.71
2.5-0.2
Morenci Stock
barren stock
-
—
—
Santa Rita Deposit
mineralized stock
32
1.24
4.7-0.3
Fierro-Hanover
barren stock
6
0.52
0.3-0.8
*Uraniun spectromctrically analyzed. All analyses are from whole-rock
samples except for soil samples of uranium at New Cornelia Pluion, Gross
Peak-Martin Ridge, and Turquoise Mountain.
-------
TABLE 3
RADON-DAUGHTER SAMPLE CONCENTRATIONS
-UNDERGROUND COPPER MINES BY STATE1
Average Radon Range of Radon
Approx. Avg.
Existing
Mi no
Location
No, of
Samples
Daughter ronc.
(WL)
Daughter Cone.
' (WL)
Ventilation
(CFM)
Indian Creek"
M i ssouri
8
0.023
.004 -0.116
Not Available
V i rurnum*
Missouri
8
0.065
.002 -0.117
Not Available
Eagle Mine**
Colorado
IP
Less than .1
Not Available
Not Available
85 Mine
New Mexico
10
0.130
0.060 -0.280
10,000
White Pine
Michigan
11
0.030
0.01 -0.04
330,000
Cal1oway
Tennessee
11
Negligible
Negligible
Not Available
Copper Queen
Arizona
42
0.330
0.02 - 1.7
5,000
*Lead, Zinc Copper
**Lead, Zinc, Copper, Gold, Silver
^Data provided by U.
Denver, Colorado.
-------
of its program to determine which mines require control technology, the
Mining Enforcement and Safety Administration (MESA) of the Department of
the Interior has surveyed a number of underground mines for radon daughter
5
activity levels. High activity is a strong indication that above
background concentrations of uranium exist within the copper matrix.
The radon daughter concentration data for underground mines in Arizona,
Mew Mexico, Michigan, Colorado, Missouri, and Tennessee are given in
Table 4.
As the data shows, the highest levels were recorded in the Arizona
and New Mexico mines (average radon working levels of .33 and .18,
respectively), which correlates with data showing uranium concentrations
in soil ranging from 2 to 10 times background levels. The Michigan,
Colorado, and Missouri mines all showed radon daughter levels less than
.1 WL. while the cooper mine sampled in Tennessee showed a negligible
concentration of radon daughters. The amount of mine ventilation has a
direct effect on the radon daughter concentration. Although ventilation
information was only available for three mines, the average amount of
air circulated in those mines varied by as much as a factor of 60.
The potential for radiation exposure from the products, by-products,
and wastes of the copper industry may be addressed for two groups - the
general population and those occupationally exposed. For the former
group, the potential environmental interfaces would include exposure due
I
to: 1) utilization of copper mill tailings; 2) construction on reclaimed
urai'iiferous mining land; 3) seepage from tailing ponds; and 4) radon gas
emanation and dust from waste piles.
-------
TABLE 4
RADIOLOGICAL ANALYSIS OF COPPER MINE
PUMPOUT WATER*
TOTAL
MINE SOURCE Ra-226 (pCi/1) URANIUM (mg/1)
White Pine (Michigan)
Mine Water Discharge *3
13.6
<0.1
Mine Water Discharge "2
4.2
<0.1
Mine Water Discharge £3
27.3
< 0.1
Butte (Montana)
Kelley Operation Mine Water
4.8
<0.2
Berkley Pite Mine Water
1.5
< 0. T
Continental East Mine Hater
3.0
< 0.1
Input to Emergency Pcnd
1.7
<0.1
Old Reliable (Arizona)
300' Level Mine Drainage
2.6
<0.1
Bagdad (Arizona)
East Pit Mine Water
1.6
< 0.1
West Pit Mine Water
12.7
0.25
-------
Utilization of copper mill tailings has been of a negligible scope
despite the vast amounts available. While other mineral tailing wastes
find suitable applications, there are a number of reasons why copper
mi I ! La i 1 inqs have not:
1. The projected growth for building construction in the Southwest
and Mountain States is the lowest in the country.
2. Transportation costs would n;ake its use uneconomical outside
of the immediate vicinity of the nine.
3. Duo to its high silicate content, impaction is difficult
ipaking its use as a construction or fill material unsuitable
ir. many cases.
At several mines rear population centers, however, tailings have
been utilized "in road construction and as general land-fill material
(after :: i x ;: i o wit'", othnr soils to imprr-ve impaction). As no records are
Maintained concerning the amounts of tailings removed for these purposes,
only estimates are possible, for a mine near Tucson, Arizona, for
example, approximately 100 thousand tons of tailings were utilized for
road construction. A small but indeterminable amount of tailings from
this mine we>*e also usc-d for land-fills and construction material.^
Pigott, et al_. demonstrated tne suitability of tailings materials
in the nrodurtion o* dry-pressed building bricks.' Pilot-plant production
illustrated that bricks of superior quality were possible. A barrier to
commercialization, however, was again, the distance between the source
material and the 'uarl.Gt. If the price of construction materials continues
to climb at the present rate, though, these bricks may become competitive.
-------
The potential radiation problem associated with the use of these
tailings which contain an, as yet, undetermined amount of uranium is at
best conjecture. If uranium concentrations do prove significant (at
least an order of magnitude higher than background), then the potential
hazard would be greatest ir homes either built with materials constructed
from the tailings, or where tailing material has been used for fill or
grading. The radiation exposure from construction materials and land-
fills would be a result of direct gamma radiation and lung exposure due
to radon daughter alpha radiation.
In the University of Arizona's 'ubl ication "A Balanced Approach to
Resource Extraction and Creative Land Development", the task force
involved proposed the long-term development of copper waste heaps and
g
ponds for residential and commercial use. Their plans called for
"satellite" communities to be built on the terraced piles with agriculture
and commercial zones. Although use of reclained copper mining sites is
very small at present, the proximity of cities such as Butte, Montana,
Salt Lake City, Utah, and Tucson, Arzona, to large mining operations
makes future development a possibility. This potential is further
enhanced with the ongoing environmental drive to eliminate such eyesores
as mirier-out open pit areas and abandoned waste piles.
The potential exposure from uranium and its daughter products is
ao<:in, difficult to ascertain without measuring the levels of the waste
Materia!. There po'.-sibil ity that hoires built on, or adjacent to,
fO'i'ier Sr-ttJing ponds woclr- experience even greater radiation exposure
du-: to higher residual unmiji,: corxentra ti cr;s . fom the dewatered slimes
and tailinos.
-------
It is evident that elevated radioactivity levV^.Jiave been found to
be associated with some copper mine pumpout waters. As an "active mine
must be continuously pumped, this effluent presents a potential groundwater
contamination, particularly at the volume typical of a mining operation
(1-10 million gpd). Likewise, as a high sulfur content is often associated
with copper tailings, sulfuric acid produced with rainwater can gradually
leach but uranium and its daughter products from storage piles. These
effluents should meet Federal and State discharge standards where applicable
I
before such releases are permitted.
Radon gas emanation and blowing dust are potential problems associated
chiefly with tailing piles and dry evaporation ponds. While radon gas
would be given off as a daughter product of the radium in the waste
material, any potential hazard would be that associated with emanation
and diff--i";on into closed structures.
Occupational exposure to natural radiation in the copper mining and
dressing industry can be divided into two sectors, the mine and the
mill. In an underground mine, exposure would be primarily due to radon
daughter products and the critical organ would be the lung. However, as
most mining is open pit (42 of 56 active mining operations), exposures
would only be of concern on an individual mine basis. In the mill,
radiation exposure would be dependent upon the type of beneficiation
being performed. For enclosed areas, radioactive particulates may pose
a problem. However, as no data has been collected concerning occupational
radiation levels in copper mills, no conclusions can be made at this
-------
time. Additionally, uranium recovery operations utilizing copper leachate
solutions could result in some occupational exposure. Such operations
would involve the handling and processing of concentrated leachate, and
the handling, transportation, and storage of the yellow cake.
The obvicus conclusion from this preliminary evaluation is that
there is a paucity of available radiological data concerning copper
mining and milling wastes. Although it is apparent that the generally
low concentrations of uranium found in primary ore has discouraged such
investigation, significantly elevated radionuclide concentrations in
underground mine atmospheres, mine runoff effluent, and leaching solutions
tends to refute the conclusion that a potential source of radiation
exposure cannot exist. There are numerous chemical and physical processes
by which the uranium concentration of waste materials can be increased,
including dewatering, Teaching, and precipitation. From a review of the
beneficiation processes, experience from EPA's current phosphate industry
study, and taking into consideration the chemical properties of uranium,
it is likeOy that a large fraction of the uranium is ultimately discharged
with the tailings. A need exists for a radiological impact assessment
of this and other mining and milling effluents. This analysis should
include primary ore, waste rock, beneficiation solutions, tailings, and
all effluent streams.
There is a growing consideration given to the utilization of these
waste materials fcr construction e:.d landfill purposes which could lead
to an increased public exposure. With the 1 miner.so amount, of waste
materials being generated, the likelihood of reclanation and >.jti 1 itior.
is beccr.irg greater. As the most significant potential exposure prowler
is the construction of homes or. urvwiiferous reclaimed land, the pattern
-------
of population growth is critical. At the present time, the lack of
development in the irrmediate copper mining areas of the Southwest make
such reclamation less of a concern. However, at present growth rates in
these "sunshine" States, this situation could change dramatically.
Occupational ly hazardous radon working 'levels have been measured in
a number of underground copper mines. Although measures are being taken
to rectify this problem, there are other facets of the mining and milling
process which have a potential for occupational exposure which deserve
scrutiny. Enclosed structures in which beneficiation solutions are
exposed to open air, for example, should be monitored to determine the
working level exposure to radon daughters.
Similar preliminary assessments are needed for other mining industries
to determine their potential radiological impact and the need for field
studies to document impacts.
ZIRCONIUM EXTRACTION' PROCESS
In the zirconiun extraction process, zircon ore (sand) is dressed witn
coke in a ball mill to a very fine consistency. This step may be preceded
by a magnetic separation to remove some thorium contamination from the sand.
The coke-zircon mixture is introduced into a chlorineticn reaction
chanber, the temperature elevated to 1200°C, and chlorine gas is reacted
v.'ith the mixture. The primary reaction is:
ZrC?.Si'V 2C + 4C1-, _j_J _ __ Zr C1.-+ Si2CC,
T^OO^C"
A two-stage condenser (lioOiSiC'i/) separates crude "J:- ff) C. 4 frcrr. j '¦ C4
which is processed for sals.
The process now proceeds to the Zr-Hf separation. This is a soiv-rnt
extraction process using methylisoL^ly!ketone and an aqueous solution of
-------
ammonium thiocyanate. The Hf is carried into the MIBK fraction and the
completeness of this separation is measured by activiating the natural Hf-180
to radioactive Hf-181 using Cf-252 sources. The Zr is carried into the
aqueous phase as zirconium oxychloride (ZrOCl2) and is precipitated as the
sulfate with the NH^Cl being further processed to recover NH4OH. The
Zr (504)2 repulped with aqua ammonia (NH^OH) to form Zr(0H)^and ammonium
sulfate which is boiled down and can be used as fertilizer. The zirconium
hydroxide (Zr^H)^) is filtered and sent to the calciner where it is fired
to the oxide (ZrOj).
The zirconium oxide is then remixed with the coke and sent through a
pure chlorinator to yield ZrCl^ free of Hf. The zirconium chloride is con-
densed and goes to the magnesium reduction process (known as the Kroll
process). Here, magnesium metal is reacted with ZrCl^ to produce magnesium
chloride (MgC12) and zirconium sponge (metal). A flow chart illustration
is presented in Figure 6.
The first residue generated by this process is the sand chlorinator
residue (tailings). This residue is primarily coke (90%), unreacted silicates,
and non-volatile chlorides. There is a significant amount of Ra-226 and
daughters in soluble form in this residue (ranging from 150-1300 pCi/g(dry)).
The chlorinator residue ends up in a pile as indicated in Figure 6. There
are also drains and general waste from this process that are sent to pond 1A,
which is a holding pond for the clarif7>r. There 1s a turnover in the caustic
alkali scrubbers used here that is partially recovered and partially sent
to the clarifier.
The sludge coming from the clarifier comprises the largest volume of
waste generated in the zirconium extraction process. Radiurr-226 concentra-
tions in sludge have been measured between 87 and 15*1 pCi/g(dry).
-------
j*. SEPARATIONS
Zr(llf)tl'-4 from CHLORINATOR
Unreactrd Sand
Drains to Cl.irificr
— ZrOC12 • GOu—«
CaOH
lORIN'ATOR
p.rsinur. mc
MI^Cl 'to
Airmonm .Recovery'
Zr(SO~rK-NMuO!l
SO Rcc
" cJ
(N'!iu) ? 50., 1'ortil.l
vr Kl-s i-J.i.0———
1 nor Drains*-,
NaOH cr HjSO,
liOLD IN'G POND IA
Scruhbcrs
ZrO
SiCl
Coke
Liquid
Fertilizer
Underflow
CC
WM-SIUM
".'CTION fURNACE
j liOI.DIVQ -'ON? IE
Supcr:i3lu
FIGURE 6
ZIRCONIUM EXTRACTION'
PROCESS
''::iins G. Scrubbers
Zr Sponge—*-'
pi! Cortiol
CO-,, NnC.I, JI,SO;
¦To Mill
¦^-Liquid Effluent to Tmax Creole
soi.vr.sr
rXTR-\CTIO.V
HOLDING POND
i i i.'i i:r
TV: r.O MAKE-UP
K11.~ FP. CAKE
V3-V4 FII.THR
TURE Zr02
ClIi.OR INATOR
VI .TANK
-------
In the sulfate precipitation (Vo) ammonium chloride is generated and
is sent to a recovery site to recover ammonia. The arnTOniurn chloride is
operated by the neutralization of HC1 with ?IRH OH (amronia).
The Zr(SO^)2 is repulped v;ith ammonium hydroxide to form Zr(0H)/|. This
process yields ammonium sulfate ((NH/j)2SO4) which is further processed tc
liquid fertilizer.
There are scrubbers associated with the final three (3) steps: the
calci.ier, the pure chlorinator, and the Kroll process magnesiurn reduction
furnaces. These scrubbers are vented to the clarifier. In addition to
this, there is a pure chlorinator residue that is also dumped on the
residue pile. The pure chlorinator residue contains about 200 pCi/g P.-2Z6.
The most significant radiological problem presented by the zi rcCni ur„
extraction process appears to be the potential contamination of surface cr
ground water from the chlorinator residues. It has been demonstrated that
the radium in these residues is extremely soluble. Radium-225 concentration
in water under a chlorinator residue pile has been treasured to be as high
-------
REFERENCES
1. Still, A.R., "Uranium at- Copper Cities and other Porphyry Copper
Deposits, Miami District, Arizona," Unpub. Ph.D. Thesis, Harvard
University (1962).
2. Moxhatn, R. M., Foote, R.S., and C. M. Bunker, "Gamma-ray Spectrometer
Studies of i (ydrothermally Altered Rock," Economic fieology, 60(4)
(June-July 1965).
3. Davis, J.D. and J. M. Guilbert, "Distribution ;jf the Radioelenients
Potassium, Uranium, and Thorium in Selected Porphyry Copper Deposits,"
Economic Geology, 68(2) (March-April 1973).
4. "Radioactivity Analyses Performed on Water Samples from the Ore
Mining and Dressing Industry," Calspcn, Inc., Buffalo, IiY, Office
of Radiation Programs, U.S. Environmental Protection Agency (1975).
5. U.S. Department of the Interior, Mining Enforcement and Safety
Administration, Denver, Colorado, private communication (October
28, 197b).
6. Rabb, D., University of Arizona, College of Mines, private
communication (August 7, 1975).
7. Pigott, P.O., Valdez, E. G., and K. C. Dean, "Dry-Pressed Building
Bricks from Copper Mill Tailings, RI-7537, U.S. Department .of the
Interior, Bureau of Mines (1971 ).
8. "A Ralanced Approach to Resource Extraction and Creative Land
Development," University of Arizona, College of Architecture and
College of Mines (joint project) (1974).
-------
RADON IN CAVES
It has recently ccme to the attention of State radiological health
officials that potential radiation hazards may exist in a number of
National Park Service caves and "cave air" conditioned buildings as
indicated through field measurements of radon and radon daughter levels
performed by the Minir.g Enforcement and Safety Adninistratio;i. A parti-
cular concern is during the summer months v:hen visitor use is the greatest
and the interchange of interior air with exterior air is at a minimum.
This situation would result in the working level exposure being maximized.
Since there are a number of State and privately owned caves and "cave
air" conditioned buildings, it will be strongly recommended that furtner
investigation in this area be undertaken.
During a three or four hour underground visit, the individual
exposure probably would not be large; however, a significant population
person-P.em dose per year, may result from the approximately or-e million
persons visitinq caves operated by the l1. S. National Park Service each
year. At the request of the National Park Service EPA made ir.terin
recommendations on exposure limits for persons employed in the Carlsbad
Caverns. On June 3, 1976, EDA recommended a 4 V.'LK annual limit for
workers in these caverns as an interim recommendation and requested
public comment on the general applicability of these recommendations
to other caves and cav~rrs coen to the public (41 F.R. 2?4Q9).
LPA further recommended that erasures be implemented to keep exposures
below the 4 l.'LK annual li'nit where feasible. !!o limit was set for visitors
to the caverns. FiJA also stated that the individual exposure 1 in~.it
-------
of 4 WLM per year cannot be characterized as safe since the risk of
lung cancer would expect to double after 10 to 20 years of employment;
therefore, it might be advisable to rotate long term employees working
in elevated radon areasJ
This Task Force recommends that a more thorough evaluation be
performed on this source of possible radiation exposure in State and
privately owned caves. If control methods are found to be necessary,
ventilation has been suggested as a corrective measure, but in such a
way. as not to eventually destroy the cave features and ecology that
persons came to view. It is recommended that representatives of this
Task Force, EPA, NIOSH, and MESA meet to discuss the preliminary inves-
tigations and measurements and determine what other studies should be
undertaken to properly evaluate this situation. Additionally, the
interim recomnendations made on the basis of existing Federal guidance
for the protection of underground uranium miners should be evaluated as
additional information and data are obtained.
-------
REFERENCES
1. Radioloqical Quality of the Environment, U.S. EPA, ORP.
EPA-52/1-7 6-010, 1976
-------
STANDARDS AHD GUIDELINES FOR RADIOACTIVE MATERIAL
iU CONSUMER AND CONSTRUCTION PRODUCTS
The NHC arid some of the States currently have regulations controlling
the use of uranium mill tailings for construction rind other purposes.
The question immediately arises as to the need for similar controls on
other industrial product:, or byproducts that contain radioactivity, such
as slag, gypsum, and other materials from phosphate plants, or tailings
from other typos of mining and milling operations. Idaho has proposed a
regulation prohibiting the use of slag under or within habitable structures,
but this sane- regulation authorizes the use cf slag outdoors, i.e., for
road cons (.ruction, railroad ballast, etc. (This regulation appears as
Attachment A in this report.) Controls on the use of other radioactive
material? will be difficult in the future without standards and guide-
lines fcr radioactivity concentrations". For example, what concentration
of rad • P.L:'G in slag is acceptable for the use of slag under or within
houses, and what is the maximum permissible concentrations of radium-226
in gypsum that, could be tolerated for use in wallboard? Also, what
level of radioactivity is permissible in materials used for road con-
struction, general fill, and otner uses?
There is an obvious need for answers or at least guidelines pertaining
to questions like these above. It is therefore recommended that the EPA
virvolep standards and guidelines for the use, distribution, and disposal
~strial products and byproducts containing r.atura'ily-occurring
radioactive materials.
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RADIOACTIVITY IN CONSTRUCTION MATERIALS
It is estimated that the average person in the United States spends
95'i of his time indoors. Over 78/.' of this time is spent in the home J
Selected members of the population, such as the very young, the elderly,
and the chronically ill, spend an even higher percentage of their time
indoors. Yet, knowledge of the radiation exposure which, occupants
within buildings receive as a result of naturally-occurring radionuclides
present in construction materials is far from complete. This situation
exists in spite of the fact that estimates show that the radiation
exposure to the population from natural background (including the dose
equivalent from radionuclides in building materials) is greater than
that from any other source.
Radionuclide Content of Building Materials
Tie literature review by Eadie notes the paucity of significant
published data relating to radionuclide concentrations in specific
2
building materials. No comprehensive surveys of the radionuclide
content of construction materials in the United States are available at
the present time. However, analyses of radionuclide concentrations of
commonly used building materials have been conducted in the United
Kingdom, the Soviet Union, the Federal Republic of Germany, the German
Democratic Republic, Taiwan, Sweden, and Hungary. These studies indicate
*This Section contains excerpts from the following report sponsored
by the EPA: Moeller, D.W. and Unrierhill, D.W., "Final Report on the Study
of the Effects of Building Materials on Population Dose Equi valents':,
Harvard School of Public Pealth, December, 1976.
-------
that large variation in the radionuclide content exists among different
types of building materials. Generally, wood products, natural plaster,
metals, and cement display the lowest concentrations. Highest concentrations
are observed in materials such as granite, pumice stone, and clay brick
and in some byproducts of industrial processes such as artifical gypsum
and concrete composed of coal-tired power station fly ash.
The most comprehensive studies published to date dealing with the
natural radioactive content of building materials are those of Krisiuk,
et al., using gamma spectrometic analysis, determined the radium-226,
thorium-232 and potassium-30 concentrations of over 300 samples of
3
building materials from many regions of the U.S.S.R. Materials of
volcanic oricin including granite, tuff, and facing materials composed
of tinguaite and endialite, as well as materials manufactured from
industiial wastes such as boiler slag, blast furnace slag, and coal fly
ash exhibited high radionuclide content. In contrast, materials comprised
of natural gypsum, chalk, lime, and cement showed relatively low radionuclide
content. Radionuclide concentrations in some of these materials are
presented in the Table, along with estimates of the air-absorbed dose
rates the mate$als would produce if they served as the wall, ceiling,
and floor of a room of standardized dimensions. The data on radionuclide
concentrations in many construction materials showed large variability
from region to region.
Situations which result in the use of high radioactivity materials
in structures in the U.S. include uranium mill tailings used as backfill
and construction material made from byproducts of the phosphate mining
and milling industry in Florida/1'^ The radionuclides of primary concern
in both of these cases are uranium and its daughter products. Another
-------
radionuclide of probable importance in the U.S. is potas1"i.ti-40.
Lowder, et al., have stated that concrete blocks manufactured from
Conasauga shale deposits in Eastern Tennessee, for example, may con-
tribute to elevated exposures due to the potassium-40 content of the
micaceous clay commonly associated with this type of shale.^
Radiation Exposure
Building materials constitute both a source of and shield from
external radiation exposure. The source characteristics result from
naturally-occurring radionuclides in the building materials themselves,
and shielding characteristics are determined by the degree to which
natural terrestrial and cosmic radiation sources are attenuated by these
materials. In general, wood fra~;e buildings have low source qualities
and are relatively poor shields fo * terrestrial and cosmic "-.'didtion.
Masonry buildings are often significant sources hut provide good shielding
for terrestrial b^ckcruuni r-j J :at.i:.n.
Hadon and radon daughter conccntrations inside buildings have been
measured by several investigations. Yeates, et al., measured radon
daughter concentrations in several frame dwellings and mul ti-story
masonry buildings in the Roston, Massachusetts, area.1 In single family
frame dwellings, radon daughter concentrations were of the same order
for outside and first floor measurements. Basement concentrations were
from 4 to 23 times higher than first floor concentrations. Daughter
concentrations in masonry office buildings tended to be slightly higher
than first-flcor concentrations in residences, but the concentrations in
-------
offices showed little variation with building height. Home ventilation
rates varied between 1 to 3 air changes per hour, while measured office
rates ranged from 5 to 14 per hour.
According to Auxier the overall dose to the bronchi of people
occupying homes built of uranium bearing materials (e.g. some granites,
low density concretes, and gypsum boards) over a fifty year period at an
average of 15 hr/day would approach that at which the incidence of lung
cancer in miners is doubled. I p. a poorly ventilated basement laboratory;
Parthaserathy found the background concentration of polonium-218 to
range from 955 to 1915 pCi/1.^
It appears that the average contribution from radionuclides in
building materials to the external dose equivalent rate to occupants in
brick and masonry houses is about 10 to 20 mRem/yr. For some population
groups, values range up to 100 mRem/year or more. Dose equivalent r^tes
to the lungs may be even higher,and it would appear that control ^sures
should be considered. Such measures include (1) material substitution,
(2) improved manufacturing standards, (3) changes in basic building
designs, (1) application of surface sealants, and (5) increased ventilation
accompanied by processes for the adsorption and/or filtration of airborne
radionuclides. Economic analyses show that several of these measures
appear to be justified if one applies the cost-effectiveness guidelines
proposed for nuclear pov/er plants by the U.S. Nuclear Regulatory Commission
of SI000 per person-Rem.
-------
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-------
Radioactive Phosphate Sfag in Outdoor Construction
Phosphite slog, a calcium fluorosi1icate byproduct of the thermal
phosphate industry, has been coircuonly used throughout Southeastern Idaho
for many years. Its rock-like qualities make it an ideal substitute for
common gravel in many outdoor construction projects, i.e., highway
sidecasting, asphalt and concrete aggregate, road fill, stabilization
material in feedlots, and as railroad ballast. Since 1971, all asphalt-
coated surfaces in one Idaho city have included the use of phosphate
slag, i.e., all city streets, all parking lots, elementary school playgrounds,
etc.
Radioassay of phosphate slag shows a r-'dium-226 content of 35 pCi/gram.
This may be contrasted to the radium-226 assay of common gravel at 0.40
pCi/gram. The direct gamma exposure rate measured at 3 feet over the
surfaces of city streets, parking lots, playgrounds, etc. built with
phosphate slaq was 15 to 40 -nR/hour. Measurements made over similar
surfaces constructed with common gravel showed gamma levels of between
6 and 10 R/hour.
it is anticipated that the continued use of phosphate slag within a
city's boundaries will eventually result in a human population living
within a network of streets measuring two to seven times above the
natural gdnma radiation background. Although not defined, the increased
radon-222 concentrations in the city's environment will pose an additional
radiation exposure to the population. Additionally, upon removal of
worn-out asphalt surfaces from the city's streets, there is no perpetual
assurance that the radioactive slag will not be used as a fill material
under habitable structures.
-------
The problems indicate a thorough evaluation of the environmental
consequences of continuing to use phosphate slag in outdoor construction
is warranted.
-------
REFERENCES
1. Oakley, D.T., "Natural Radiation Exposure in the United States,"
U.S. Environmental Protection Agency, Washington, D.C., Report
0RP/SID72-1, 1972.
2. Eadie, G.G., "Radioactivity in Construction Materials: A Litera-
ture Review and Bibliography," U.S. environmental Protection
Agency, Technical Note ORP/LV-75-1 (April, 1975).
3. Krisiuk, E.M., Tarasoc, S.I., Shamov, V.P., Shalak, N.I.,
Lisachenko, E.P., and Gomel sky, "A Study on Radioactivity of
Building Materials," Leningrad Research Institute for Radiation
Hygiene, Ministry of Public Health of the U.S.S.R. Leningrad (1971a).
4. Culot, M.V.J, and Schiager, K.J., "Radon Progeny Control in
Buildings," Final Report on research supported by EPA Grant
ROT EC00153 and AEC Contract AT(11-1 )-2273, Colorado State
University (May, 1973).
5. Guimond, R.J. and Windham, S.T., "Radioactive Distribution in
Phosphate Products, By-Products, Effluents, and Wastes," U.S.
Environmental Protection Agency, Office of Radiation Programs,
Technical Note ORP/CSU-73-3 (August, 1975).
6. Lowder, W.M., George, A.C., Gogolak, C.V. and Blay, A., "Indoor
Radon Daughter and Radiation Measurements in East Tennessee and
Central Florida," Health and Safety Laboratory, U.S. Atomic
Energy Commission, KASL TM-71-8 (1971).
7. Yeates, D.B., Goldin, A.S., and Moeller, D.W., "Natural Radiation
in the Urban Environment," Nuclear Safety, Vol. 13, No. 4,
pages 275-286 (July-A',;gust, 1972).
8. Auxicr, J.A., "Respiratory Exposure in Buildings Due to Radon
Progeny Health Physics", Vol. 3]_, pages 187-188, (1976).
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RELATED HPA—TASK FORCE ACTMTIES
The United States Environmental Protection Agr-r.cy is presently
conducting several programs to determine the need for -voidtioo pro-
tection standards, guidelines, and criteria with resoect to exposures
from naturally-occurring radionuclides. Tho following problem areas
have been identified for initial efforts because r,f their public health
importance :
1) The development of roc attend; t ions to the State of Florida ft <•
the control of radiation exposures associated with phosphate
materials. These recommendations will exclude acceptable
indoor radiation level cuidelires arcl criteria for oval uati nv;
undeveloped land to preclude ra«iiat'on problems i'i homes thdt
might be constructed on the land.
2) Land contamination problems exist in several States in addition
to Florida, because of uranium mine and milling and other
mineral processing activities. Tnerefore, the Agency is
evaluating the need to develop national guidelines for acceptable
land use of areas containing elevated concentrations of naturally-
occurring radioactive materials.
3) Construction materials such as phosphate slag, pumice, fly
ash, and phosohogypsum can contribute significant radiation
exposure to occupants of structui rs !M<5e frop th•?.-.£ materials.
To provide adequate public health protection ft en these
-------
materials, the Agency is assessing the need to develop national
guidelines for acceptable radiation concentrations in con-
struction materials used in structures.
4) These same cons (.ruction materials are frequently used for road
pavement, railruad ballast, bacM'ill, and other applications.
While the public health significance of these uses aie probably
not as great as when used in structures, it is not clear that
such practices are prudent and in the overall public interest.
The State of Idaho has requested the Agency to provide guidance
for a np T,irri ate tadiation protection criteria for these applications.
In conjunction vHh the Scate of ;dr.l.o's request, ana because
such problems are of national interest, the Agency is considering
national radiation protection recommendations for such applications
of natura11>-cccurring radionuclides.
All of the proulems'noted above are of significant, importance to
one or more Stales Further, existing 1 egis 1 atiori provider, many States
with some authority to control such exposures. Therefore, it is recommended
that this Task Force, or: behalf of the Conference, work closely with the
L'nvironmental^PrGtection Agency in then efforts !.o develop the criteria
and guidelines described above. The Task Fe'ce would interact, with FPA
in the following manner:
1) Feview and evaluate any technical support documents developed
by the Agency.
2) Evaluate the practicality and overall Quality of standards,
criteria, and guidelines developed by the Agency including
assessiriy their compatibility with existing State regulations.
-------
Provide EPA with input in the development of criteria and
guidelines including any data and information available from
the "States.
Any other coordination that its determined to be appropriate.
-------
STATUTORY AUTHORITY OF STATES TO REGULATE
NATURALLY-OCCURRING RADIOACTIVE MATERIALS
The Task Force recommends that all States adopt uniform regulations
pertaining to the control of radioactive mineral tailings and industrial
byproduct piles. Louisiana, for example, has adopted such a regulation
(See Attachment D). These regulations should not be simply limited to
"uranium ;mll tailings", because it is clear that other types of radio-
active piles must also be controlled.
The States, in some instances, should investigate their statutory
authority to control naturally-occurring radioactive material. There is
the belief in some States that Agreement State radiation control agencies
have authority only over byproduct or agreement material, and not over
natural ly-OT-urri nn radioactive materials. Consequently, there may be a
need i'or additional statutory authority to control naturally-occurring
radioactive materials.
The obvious method of achieving the needed control program would be
through specific radioactive materials licensing.
Specific licenses could be issued for the naturally-occurring
radioactive materials in the uranium decay series. The mining, bene-
ficiating, processing, and crushing operations could be licensed to
possess, use, and store this radioactive material. Specific licensing
could provide for:
-------
(1) Restricted use of industrial byproducts such as slag.
(2) Long-term control of slag arid gypsum piles.
(3) Periodic radiation monitoring in order to continuously define
and assess radiological problems.
(4) Imposition of radiation regulations and standards.
Safe uses of slag and other radioactive industrial byproducts could
be provided for by a license. A license could:
(1) Restrict the use of those materials to road construction,
other outdoor uses, and other uses authorized by the reg-
ulatory agency.
(2) Prohibit the use of these materials for any purpose that would
result in or would likely result in slag being under, incor-
porated into, or within dwellings.
Examples of specific licenses that could be issued t.o phosphate
industries are given in Attachment 8 of this report. Attachment C is
a licensing-guide for a phosphate industry application for a radioactive
material license.
Other industries with significorit radiological aspects such as
zirconium recovery plants and rare earth mills and processing plants
should also oe licensed in order to insure adequate controls over the
naturally-occurring radioactive material. The State of Oregon presently
licenses a zirconium plant and requires the plant tc transfer all
radioactive tailings containing thorium to the waste disposal site near
Hanford, Washington.
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RECOMMENDATIONS
A. Pending the establishment of appropriate standards, the use- or
phosphate mining and milling byproducts in occupied structure'.;
should be discouraged if they contain elevated levels of radium-226.
EPA should place high priority on evaluating + nis application cf
these byproducts and balancing this against the environmental
problems associated with waste storage of th:- nvterials.
B. Phosphate byproducts, particular gypsum, are |resently used to a
limited extent as an agricultural soil conditioner. Although
little is specifically known regarding the environmental i.-p.jct of
this use, and considering the small addition of radioactiviry to
the environment, it is unlikely that this appl icatior: woulo result
in significant radioactivity uptake in crops. It is riot >"eco,
that this use of the byproduct materials be discouraged at >;his
time. Additional controlled studies should be performed to dacunc-n:;
the anticipated minimal environmental impact of this use.
C. Slag from thermal process phosphorus acid plants should not be used
for any purpose that results in its being under or within an enclosed
structure. Any other use of slag should be thoroughly evaluated.
0. States, where applicable, should adopt regulations pertaining to
control of radioactive mineral tailments and industrial byproduct
piles. States should investigate their statutory authority over
naturally-occuring radioactive material and if necessary, enact
appropriate legislation.
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E. The States should perform additional radiological air monitoring .
inside and outs— r phosphate plant areas.
F. States should inventory mineral mining and processing operations
referred to in Part VI of this report, and examine potential radio-
logical aspects of their effluent, emissions, products and wastes.
A report of the inventory and other findings should be submitted to
Task Force -7 with any pertinent recommendations.
G. This Task Force as a representative of the Conference, should meet
with EPA, NIOSH, OSHA and MESA and discuss their respective /jurisdictions
and activities regarding occupational radiation exposure in the
phosphate industry.
H. EPA should study the uptake of naturally-occurring radionuclides in
food crops from irrigation water, fertilizer, and radiation-bearing
so i 1.
I. EPA should study the whole body and organ doses resulting from
ingestion of radon daughters in drinking water.
J. EPA should evaluate the inhalation hazard which may result from the
release of radon from water containing high concentrations of
naturally-occurring radioactive material during certain home and
commercial uses.
K. CPA should develop national crito^ia ar.d guidelines concerning the
use and distribution of industrial byproducts containing naturally-
occwiT ir.3 radu.:,CLi ve i-iatoria i. The EPA snould consider seeking
appropriate autnority tc promulgate such guidelines as national
standa rds.
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L. EPA and appropriate States should study and evaluate oil uses of
fly-ash from coal-fired plants, particularly related to construction
materials.
M. lhe radiological aspects of each proposed coal-fired plant should
be evaluated by the appropriate agencies. Radioactive releases
should be estimated from an analysis of the coal to be consumed and
the operating characteristics of the proposed plant. This recommendation
is especially pertinent to any proposed plant that intends to
derive its fuel from low-grade, uraniferous Western coals.
N. The EPA should develop standard procedures arid guidelines for
sample collection and analysis of naturally-occurring radioactive
material to ensure the acquisition of uniform arid comparable data
by State and Federal programs. The EPA should expand their cross-
check quality assurance-program in conjunction with the standard
analytical procedures arid to include .NORM.
0. The States, the EPA, or other appropriate agencies should proceed
to treasure radon levels on fly ash piles and ir> structures built in
fly ash disposal areas, if such case exists.
P. It is recommended that representatives of this Tas^. F.\~ce, EPA,
IJIOSH, and MESA meet to discuss the preliminary investigations t;nd
measurements of r^don-222 in caves and determine what ether studies
should be undertaken to properiy evaluate this situation. Add-tiona!!y.
tne interim recommendatic-ns made on tl'.o basis of existing lederal
guidance for the r;rnt.eciion underground uranium miners should be
evaluated as additional information and data are obtained.
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Q. This Task Force recommends that a thorough evaluation be undertaken
concerning the occurrence of radon-222 as a source of possible
radiation exposure in State and privately-owned caves.
R. In view of the measured high concentration of radium-226 in oil
brines, the impact of uncontrolled discharge of these brines on the
biosphere should be evaluated by appropriate State and Federal
agencies. The proposed study in Attachment E to investigate this
impact should be considered for funding by EPA or other appropriate
agencies.
S. Phosphate industries and all other industries having signified!
radiological impacts should be licensed in order to assure adequate
controls over naturally-occurring radioactive materials.
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ATTACHMENT A
Exploration of the Proposed Revision
of Part I
Idaho Radiation Control Regulations
It is generally known that when radium-bearing material is placed under
houses or other structures, radioactive radon gas emanates from the
radt..hi; and may diffuse into the structures causing internal radiation
exposures tc- occupants.
The Radiation Control Section has established that slag from thermal
phosphate plants is radioactive and contains radium as well as other
radioactive materials.
The Radiation Control Section has determined that radon concentrations
in houses constructed with slag as aggregate in concrete can exceed the
Surgeon General's recommended radon concentration guidelines.
Since slag is radioactive, the provisions of Part I, "Radiation Safety
Requirements for Radioactive Mineral Mill Tailings", Idaho Radiation
Control Regulations, can be applied. Section 1.2(f) prohibits the removal
of tailings material from the slag pile without specific written approval
of the Agency.
Slag has been used for a number of years for various purposes, including
as aggregate in asphalt, as railroad ballast, as aggregate in drain
fields, as stabilization material in cattle yards, and as aggregate in
concrete. It is f>e purpose of these proposed revisions to Part I to
(a) provide for the limited use of slag where no hazard has been established,
e.g. road construction and (d) to prohibit the use of slag where a hazard
has br>en established, i.e., unde^ or within habitable structures.
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Sec. 1.2 Maintenance of Piles and Ponds at All Mills.
(f) Except as provided in Sec. 1.5 of this Part and for reprocessing at
the site, prior written approval of the Radiation Control Agency must
be obtained before any tailings material is removed from any active or
inactive mill site or tailings pile.
Sec. 1.5 General License.
(a) A general license is hereby issued to transfer, receive, acquire, own,
possess, and use licensable concentrations of naturally-occurring
radioactive material in slag from thermal process phosphate plants
provided that:
(1) A written notice containing the following statement or substan-
tially similar statement shall accompany each transfer of slag:
NOTICt - SLAG FROM THERMAL PROCESS PHOSPHATE PLANTS
CCNTALM5 TRACE QUANTITIES OF RADIUM, A RADIOACTIVE
MATERIAL. SLAG IS HOT SUITABLE FOR USE UNDER OR
WITHIN HABITABLE STRUCTURES. THE IDAHO RADIATION
CONTROL REGULATIONS PP.OHIEIT THE USE OF SLAG AS
FILL OR AS AGGREGATE IN CONCRETE THAT WILL BE UNDER
OR WITHIN HABITABLE STRUCTURES.
(2) Slaq containing liccns3ble concentrations of naturally-occurring
radioactive notorial shall be used for only the following purposes:
(i) For road construction, either as aggregate in asphalt
"or concrete, as fill, or as sio'ecasting.
(ii) For railroad grade? as ballast.
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(in) Tor parking lots, driveways, sidewalks, bridges, or
other outdoor structures, as aggregate in asphalt or
concrete.
(iv) For stock /ards as fill or as stabilization material,
(v) for other purposes specifically authorized in writing by
the Radiat ion Control Agency.
(b'; it shall be specifically prohibited to use slag containing licensable
concentrations of naturally-occurring radioactive material for the
following purposes:
(1) As aggregate m concrete or other notorial that will be under
or within habitable structures.
(2) For ory purpose that will result or likely to result in slag
being under, mrorpoi ated into, or within habitable structures.
{3; Ft"' a¦ >y other ?-. cost c/.ccpt ,-.s antl>Grizee! in Sec. \.5{o)[?).
(c) Persons who transfer, receive or acquire slag 1 roi:i thermal process
phosphate plants pursuant to the general license contained in Section
1.5(a)- shall be e/cmpt from the requirements of Part C of the^e
regulations.
Sec. i .20 DefiniT.ir.ns. As used m this part:
(a) "H'abi tchl e structure" neons any dwelling, reuse, garage, building
or other ceclnsed structure Ihdl is lii-.oly to be occupied by an
indiviriu-il.
(b) "Licensable concentrations of natural 1y-occurring radioactive material
;;eans concentrations of the uranium or thor",w\ series radioisotopes
greater than those concentrations listed in Part B, Schedule A, Exempt
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(c) "Mill" means any ore processing plant, a thermal or wet phosphate
processing plant, or any ether processing or manufacturing plant.
(d) "Slag" Hiearis that tailings material of the thermal process phosphate
plants.
(e) "Tailings material" means any residue separated in the preparation
of various products.
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ATTACKMEHT B
Elemental Phosphorus Plant
Ni['kl/U|U
ciriHtooN iiiti
INItlAl LICtH*(
frcflcut Amc
Ait V«
iNti ifttt.ro ru»tu'HT to t
'.co«o«hc( Mirx
Q ApplicoiioT Q Idler Q Tclfiprom CD-
ILOINI 1 H>l| KO
©» Ol-'XIHT J
H""
AUlHO«l/fD OSC
Naturally occur-
ring radioactive
materials in the
uran iir,i and
thoriun series.
Natura^Ly occur-
ring radioactive
materials in the
uranium and
thorium series.
As necessary for
mininp;, process-
ing, and recovery
of elemental
phospliorus.
As necessary for
mining, process-
ing, and recovery
of elemental
phosphorus.
Pto.sphcrus bearing
sl\rs.le or ore containing
licensable concentra-
tions of radioactive
materials.
Industrial jy-pixxiucts
containing icer.sable
concentrations c. radio-
active naterials.
Phosphorus bearing shale or
ore containing licensable
concentrations of radioactive
material may be mined,
beneficiated, ar.d processed
for the purpose of extractirg
elemented phosphorus.
Unless otherwise provided by
the Conditions of this license,
ind> jtr'al by-products containing
li^ensable concentrations of
tadioactive naterials shall be
for storage only.
1. All industrial by-products containing licensable corjentratiurs of radioactive rmterials
shall be stored at the licensee's phospliate plant :iear .
2. Radioactive furnace slag may be transferred tc slag crushing operations which hold
a specific license issued bv the State of or another State which authorizes
the receipt and use of such material, rvushed slag sliall be used only for (specify
uses).
3. The licensee shall maintain records of all furnace slag transfers utiich indicate the
amount of slag transferred to each slag crushing operation. Records shall be made
available for inspection by the Radiation Control Agency.
4. FEP may be transferred or used by the licensee and is cxrrpt frcni the provisions of
this license and the Radiation Control Regulations.
- 86 -
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""
" ~ "" ' . |""
¦ ¦¦ •« |nn»»iiO» o«il
j G INITIAL UIC LHVC j
Vinvjv f_ ) '»*' • 0 >0<
» 0* 01 »i( 1 |
| «
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RADIOACTIVE
MATERIAL LICI.-.NSE
Wi.'t Process Plant
lOIO'C I
!•«*«» n> t«
j App!icof«o« | "J I rlter £3 Ttlrgiom C3-
rie*TiO>4 1 HO0K.I I.ONIAINI* oa ( OlV'Cl |
AU1 HOPli I O use
Naturally occur-
ring radioactive
materials an tlie
uranium and
tlK^nmn series.
Naturally occur-
ring radioactive
materials in the
uranium :ind
thorium series.
As ncxie^sary for
mining, process-
ing, and pro-
duction of
pliosphoru acid
aiid fertilizer.
As necessary for
mining, proof-
ing1, and pro-
duction of
phosphoric acid
and lorijli-ser.
Ptio.cjphorus bearing
shale or ore containing
licensable concentra-
tions oT radioactive
materiais.
Industrial by-products
containing ljconsable
ix;ncentrat ioits of radio-
active materials.
Phosphorus bearing shale or
ore containing licensuhlr
concent nit ions ol' radioactive
material?. ni\ bi mir.fxi,
Ijenol jcluted, and pn.xiosse* storxxi at the ! iconic' r, chi.!»b <0 pi.Lit near _
2. Th«-» noens»-'-* sh^l i rv*r^ly with I i;r pnjv: xions of I'art Tn piles and oilv^r industrial
by-product piles containing } i(.rnr.ahlr,concent r:\tJi-r.s of r-CJ.i- •«i- 11 .•*> iniicrial.-.
3. Pi*>sphoric acia :m provisions
oi this i ic» cu<.' emd Uic Radial ion Cuarol H*frulai ions.
•1. The license i-;hal 1 cxrply with statements, u-present ntions ancl procedures contacted
in jns ,tji|>i ic.it.ion dated and signed by
-------
RADIOAC I IVI-:
©
MATKRIAl- UCKNGII
Slag Crushing Ccrrpary
~
Prcifwi S, mi-Mmi n»i
Art Vol d
IHIt KClMf I
PU*lU>S< fO »"8 •
Appllcoiiort Q lelttf Q Telegram Q---
IIGNID »Tl
•-u-.« I
¦T-^.y-rr.\o"j-'.v.^.j p.-Tc.TT,^'.. ..
Naturally occur-
ring radioactive
materials in the
uranium and
thorium series.
As necessary for
the carrierciaL
uses of slag
authorized by
this license.
Furnace slag contain- Unless as otherwise provided
ing licensable concen- by the conditions of this
trations of radioactive license, slag containing
materials from phosphate licensable concentrations of
industries utilizing a radioactive material shall be
thermal process. for hauling, crushing and
storing only.
1. Slag containing licensable concentrations of radioactive iraterial shall be crushed and
stored at the licensee's facility near .
2. Slag containing licensable concentrations of radioactive material may be used by the
licensee for purposes of and in any other
State where such use is not prohibited.
3. The licensee shall nraintain records of all uses and all transfers of slag containing
licensable concentrations of radioactive materials which indicate the specific use,
location, prid amount of slag used or transferred. Recoixis shall be nude available
for inspection by the Radiation Control Agency.
4. The licensee shall ocmply with statements, representations and procedures contained
in his application dated and signed by .
l0t «V
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attachment c
INSTRUCTIONS
Application for Radioactive Materials License
1. (a) Name and Street Address of Applicant. Give name and address of
company.
(b) Street Address(es) at Which Radioactive Material will be Used. Must
include all locations where ore, products, or industrial byproducts
containing licensable concentration of radioactive material are mined,
processed, stored, or distributed from. (Also, list names and
locations of all underground mines.
2. Department, to Use Radioactive Material. Self explanatory if applicable.
3. Self explanatory.
4. Individual User(s). Not applicable.
5. Radiation Protection Officer. Name of person designated as the individual
responsible for insuring compliance with all license conditions -.cij all
applicable radiation regulations.
6. (a) R^d loa^ti ve_M:i_t,sria 1 . !:jv:ify naturally-occurrina radioactive
material in the uranium and thorium decay series.
(b) Chemical and/or Physical Form and Maximum Quantity of Fach Chemical
and/or Physical form That You '..'ill Posess at Any One Time-. Tor the
form of material specify: (T) phosphorus bearing shale or ore con-
taining licensable concentrations of radioactive material and/or {?.}
inuustrial byproducts containing licensable concentrations of radio-
active material including slag, gypsum, fluid dust material, etc. (make
1:s L complete; and/or '3) industrial products containing licensable
coiv;entrai luri of radioactive material including phosphoric acid,
fertilizer e!] phosphorus, FFP, etc. (ma^e list complete).
kic! :c'icti'. " s (aii'borno c~ liquid effluents) should not be
ir:<: 1 ,fl i.1..
For rnaxi:'iii¦: i;i:.-;r,f.ity simply specify: (i) As necessary for mining,
p roc ess in.-, :.r.d manufacture of elemental phosphorus, phosphoric
acid, fertiliser, etc. and/or (2) As necessary for the commercial
'1 z' o" - i n f1 a c a i *'»::); -f. d by t * 11 s 1 ^ t. c-n s-.r.
7. Destr iK: •'•jrjiose for _Wh i cji Radioactive Material Will ysrj. Sr><><. i fy a:;
uses of or-'1, products, arid industrial byproducts containing licensable
concentrations of radioactive material that yom want to be authorized for,
including but not liuitec! to such things as: (1) mining, (2) beneficiating,
-------
(3) processing, (4) transfer to slag crushing operations, (5) transfer to
vanadium extraction companies, (C) transfer to asphalt companies for road
construction, (7) transfer to railroads for railroad grades, (8) all other
transfers (specify ultimate uses), (9) storage, (10) all other uses.
8. Type of Training. Applies only to the Radiation Protection Officer.
Individual should have training that will simply enable him to understood
license requirements and applicable radiation regulations.
9. Experience with Radiation. Applies only to the Radiation Protection Officer.
10. Radiation Detection Instruments. List of instruments should include all
survey meters, air samplers, and laboratory equipment necessary to measure
radiation levels (including airborne radioactivity) in order to determine
and insure compliance v/ith license conditions and applirable radiation
regulations. (Do not include personnel monitors). Or alternatively,
describe facilities or consultant firms to be used or employed for radiation
measurement purposes.
11. Method, Frequency, and Standards Used In Calibrating Instruments Listed
Above_. Self explanatory.
12. Film Badges, Dosimeters, and Bio-3Ssay Procedures Used: The requirements
for personnel monitoring are specified in Section of the
Radiation Control Regulations. (See also. Section )
13. Facilities and Equipment. Self explanatory.
14. Radiation Protection Program. See Sections C.l, C.101, C.102, C.103,
C". 104, C. 105, C.106, C.201, C.?05 of the Radiation Control
Regulations.
15. Waste Disposal. Must include a description of all airborne and liquid
radioactive effluents, if any. See Section of the
Radiation Control Regulations.
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ATTACHMENT D
PART _
RADIATION SAFETY REflUI REPENTS FOR RADIOACTIVE
MINERAL TAILINGS AND INDUSTRIAL P.Y-PRODUCT PILES
Set,. .1 SOOPK. The reflations in this part establish requirements for
radioactive; mineral tailings, piles and ponds and by-product piles containing
radioactive material from Industrial processes in concentrations in excess of
Ixjrr'' microcurie per ^ram1. As used in this part "by-product" trc-ans any
material produced, other than the primary product, in an industrial process.
Tin? provisions of this pari are in addition to, and not in substitution for,
other applicable; provisions of: (a) these regulations and (b) any specific
license issued pursuant to Set;. C.30 of Part C of these regulations.
Sec. .2 SPECIFIC TOR TAILINGS. PILES AND J-ONDF.. Unless specifi-
cally provided otherwise by the Division, the following requirements for tailing,
pile and pond areas shall be fulfilled:
(a) Ac<^;ss to such areas shall be controlled and posted as specified by the
Division.
(b) Those areas shall be maintained! in such a injure;' that excessjve erosion
ol , or environmental l"iartards I rot:., r:.;'ior > ovrsc
shall be stabilise! to prevent erosion.
'i:Ci/rr.l lor liquids
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(2) Drainage ditches .sufficient, to proven! erosion from surface runoi I
water .shall be provided.
(c) Prior written approval of the Division shall be obtained beiore the
surface area of the land .shall be put to use.
(d) With the except ion of reprocessing at the site, approval by the Division
must be obtained prior to rejroval of any material f)\fn these areas.
Sec. .3 SALE OR TRANST'TP. OF TIE SITE. The Division shall be- j'.iven wit ten
notice thirty (30) days in advance of any contemplated transfer of right, litle
or interest in the site by deed, lease or other conveyance. The written notice
shall contain the name and address of the proposed purchaser or transferee.
Sec. .4 ABANDONMENT OF HIE SITE. Prior to abandonment, of the site, the
requirements of this section shall be fulfilled.
(h) Piles shall be staluli','ed against wind and water erosion ;ind. rontoured m
a tnanner which will prevent col lection of water.
(b) )n addition to the above requiranents, any material which has been
removed from the pile by natural forces shall be returned to fhc pile.
(c) Ponds shall be drained and covered with materials that prevent blowing of
dust. Water drained Iran the ponds shaiL be disposed of in a manner
approved by thr Division.
(d) Dotr.iled plans lor appliance with paraprrnpl'iS .'l(a). (b) and (e) shall
be suumtLed to the Division, for review rind approval.
See. _ .5 Vi/UVrjt. Dpon application to the Division, certain rcxiuirc-Tnonts of
this part may be waived or modified if it. can be si * ;wn that the rt-qui rcrr>?nts are
unnecessary or impractical in specific cases.
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ATTACHMENT IE
IN 1 kODllC'.nON'
Tic occiin cncc of environmentally h i j;li concern rat. i ens of r.uliun iso-
topes in oil fic-ld production waters (also called oil field brines, pro-
duced water, produced i a s t c-wa t er , or forr:aj_i_on r) iuei! document ed
(Km oiin, 1V 3; Got t and Mill, 1955; Armbiust and Kuroda, 1950). Arnbrust
and Kuroda (1950) reported Rn-22<"t, Ra-226, and Ra-22S in pi odnc t i on i-.ilcrs
fiom oil fields in Oklahoma and Arlansas, with activities ranging from
100-1 j 00 pCi/1 f, a-a:: , 1-1600 pCi/1 Ra-226, and lip to J00 pCi/1 Kj-.TJS.
They also found S pCi/1 Th-228 and 0.5 pCi/1 Th-227 in one well sar.pl e.
Gott and liill (1955) reported en vi ronment a 1 1 y high conceit i at ! ons o!" ra-
dium in proc i pi t a t cs collected from the bottom of oil-water separators,
and from ditches and ponds used for disposal of the production water.
The Mississippi, Louisiana, and Texas Gulf Coasts cither arc, or have
the potential to> become :rajor oil-producing areas of the United States.
Texas and Louisiana have numerous producing ve! Is both on- and off-shore.
During the period November 1972 to October 19/3, app ro.\ i ma t c 1 y 1.7 x 1015
liters of production i-ater were discharged to the Gulf of Mexico from
operations on federal Outer Continental Shelf (OCS) leases outside the
three-mile limit (data furnished by U. S. Geological Survey, 11)74). Rec-
ords of discharges inside the three-mile limit and on-shore are maintained
by the states in which the discharges occurred. Data provided by the De-
partment of Ccr.scrv'at i on , State of I.oui si ana , show that for the year 1975
a state total of S.J x 10!0 liters of formation waters were discharged into
the surface environment, 17.5° off-shore (presumably inside the th roe - rci ! c-
limit), and 82.3% or 6.7 x 1010 liters on-shore. Of the latter, 6.0 x 10!u
liters verc discharged into non-potable water bodies, -5.3 x 10s liters wore
discharged in jo streams and rivers, and 2.4 x 109 liters '..ere disposed of
in open holding pits f i o:r, which gradual loss occur's via e vapo rat i on a.id
seepage into tlie underlying ground. Similar data should be available f,-om
the Slate of Texas upon icquest. In 19/4, several samples of formation
waters from the Gulf Coast production region were obtained and anaiy.-cd
for Ra-226. The results are presented in Table 1.
The data in 'I able 1 show that envi ronmcntal ly high levels of Ra-226
are common in production waters from th.c Gulf Coast oii fields. For com-
parative purposes, it is noted that average open ocean surface waters con-
tain about 0.05 pCi/liter; coastal waters probably do not generally get
r.iuch higher than about 1 pCi/liter, except in very restricted environments;
drinking water standards restrict the permissible R.itonteuL to less
than 5 pCi/1 :ter; and agreement state and r'iiC regu)ations governing t. he-
operations of licensees permit no more than 30 pCi /'! t c i in liquid diicvarg
to unrestricted access areas According to Louisiana state officials, po-
duction waters do not come under these regulations at the present tim., but
it is notable that the;' contain up to <100 pCi/liler,or 10 tin.es the per-
missible regulated inputs.
To our 1-nowlcdge, there have been no scientific studies of the input
]cvels, speciation (in terns of dissolved vs. particulate forms) cr iiiiimat
disposition (fate) of such naturally occurring radium being disehaiged into
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loc;rl cm uar i tic- environments (marshes, stream-,, rivers). The occurrence
of '~;.vi ronnentaI ly high levels of radium in production waters docs not
appear to be a widely known fact, as evidenced by conversations with both
slate officials and oil company officials, although such discussions have
not been exhaustive.
THE LKUVI LLE OIL FIELD
The l.eevillc Oil Field is a producing field covering abovt 62 km2 (2'
rr.i2) in Lafourche Parish, Louisiana, centered near 29°14'N, 90J12'W (see
Fig. 1). This field uas discovered in 1928, and is operated by Texaco, Inc.
By Texaco's estimates (in a letter to Dr. T. Whelan dated 30/13/76),
production is expected beyond the year 2000. The Lc-cville Oil Field is in
and surrounded by a salt marsh complex typical of southern Louisiana. The
annual average salinity of the marsh water is 13.3 %„ (Whelan et al., 1976),
and the hydrology is seasonally controlled. There are three primary hydro-
]oj;ic conditions: in the winter, the winds are from the north and push the
marsh water toward the south, resulting in seasonally low water levels in
the marsh, and biologically, the marsh is least active; in the spring, a
"spiing tide" or "flood tide" reverses the prevailing condition, and sea-
sonally deep water levels occur; and during the summer, the hydrologic
conditions are nost stable, -with only small diurnal tides affecting the
medium water level oy a few tens of centimeters, and the marsh is biologi-
cally quite active. The predominant vegetation find primary producer is
SjM'Ltc'ui fit' eA>i-i£Zu-ia, a marsh gross. There are also abundant mussel arid
clam banks, and coru.ierc i a 11 y harvested oyster beds; benJiic organisms,
primarily r.nrphipods and crabs, abound; pelagic biota include grass shrimp,
the (iiii f Killifisli" (F. OKandiLi) , ar.d the Sheepshead Minnow (C. vci-ligcvtuA) .
Figure 2 is a p rticn of a topographic map of the area. Oil it are plot-
ted the Leeville Oil Field tank batteries which are reported to be discharging
production waters into the surrounding surface environment. These production
waters '.say properly be classified as brines since thei; average annual "salin-
ity" d^cs not vary much from lS0°/o(> (T. Whelan, personal communication).
Although this field has been producing for several decades, records of volumes
of production water discharges have only been maintained in recent years.
Table 2 Minima ri zes .the five-year (1971-1975) production water discharge his-
tories for the 11 tank batteries reported by Texaco to the Department of Con-
servation, State of Louisiana.
The total five-year discharge was 6.3 x 10® liters; the 1975 volume dis-
charge of 1.03 x 109 1.vers was ~1.6% of the total on-shore discharge in the
State of Louisiana. In October 1976, brine samples from the discharges at
TB #'1. in nid-field, and TB US, in the northern, less built-up area of the
field, were*san;plcd and analyzed for Ra-226 in our laboratory. The results
are presented in Table 3, and indicate that both tank batteries are discharging
water with environmentally high concentrations of Ra-226.
Based on the data in Tables 2 and 3, in 1975, TC fM discharged approximatc-
ly C.2 Curies Ra-226, and TB n'8 discharged approximately 0.016 Curies R.i-?26
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in* cj the local salt mais1: complex. If it is p.? :-u:,!i'ci that tin.; average pro-
duction inter from the leeville Oil Field cont .*i i :i s about 2R0 pCi/1 Ra-2?6,
thtn over the five-year period of record, up to 1.76 Curies Ra-226 were
r.'!df d to the- ii.i r;".ii around the field. At this ti-e, we have no data by
:.!.ich to predict the ultimate fate of that radium. We also do not know if
;:i:y utlici isotopes fjvin the u ra n i urn -1 hor i um series a i e piesent in er.viron-
rientally s i g.i j f i c.i nt concintrations in the i oduc t i on waters.
We arc prepared to design and implement a program which wi i ] .insider
some of these <[uc--.tiens. We anticipate that such a program would involve
collection and analyses of production i.ater (brine") :.-:;ples, marsh-water
samples, and various biological samples from the sti.dy site. The number
of each type of ;w,)rle will have to be determined hy tic crivi roni;.e»t a 1 < or.-
ditions at the study site, but may be estimated as up to 75 each. The
resulting data v. 1 11 be con-pi led, interpreted, and discussed in a final re-
port, to be delivered v. i t h up to six (6) copies to the sponsor approx i i.-.a t c-1 y
16-20 months after project initiation. It is 3 3 so expected -.!iat om? -. r - ore
professional papeis to be published in reputable scientific jourr.ajwill
ic.sult, ai.d -:i:ese v.-ill acknowledge the sponsoring agency.
RliFF.RFN'CFS
'>! ipb rus* , C. F. and I'. K. Kuvoda. On the Tsotopic Const i tut ior. of Radium
(.-
-------
1ABLF. ]
r.1-226 in sri.i.cir.n sA.'ir'i.is or formu ion wailks from
'11II. GULF COAST I'KOIHICTION KF.GION
1 CAJn OM
ARCO, High Island Plat-
form B, ~ 12 ;ni 1 cs offshore
Galveston, TX
Tfth'ATMLN'T
Rough fi1tcred ,
fi lira to acidi-
fied
MTUACTIVr;
SALINIIY
QtO
121
Ra-226
.('"J/.1!
:>:i ^ 4
K,".XON, Grand Isle Terminal,
Grand Isle, LA
No trcalPicnt
99
1 <13 ~ 3
KXXON, No location dat3
provided, shi pped from
Lafayette, LA
No treatment
Acidified, but
not filtered
98
291 +_ 3
2i)8 + 2
r.XXON', Pelican Island
Term., Pelican Island, TX
No treatment
Filtered, Acid,
llnfi 1 tcrcd, Acid.
100
22 + 1
16 '£ 5
46 + 2
Tf'^CO, Bay dc Chene,
J- ffcrson £j Lafourche
Parishes, LA
IJnf i It cred , Ac i d.
Filtered, Acid.
128
335 *_ 10
327 + 5
TF.XACO, Garden Island Bay,
Plaquemines Parish, LA
Unfiltcred, Acid.
Filtered, Acid.
110
397 t 8
393 + 6
TF;XAC0, No location,
originate llounia, LA
Unfiltcred, Acid.
Filtered, Acid.
276 +_ 3
131 + 2
NOTE: F.rrors indicate precision (lc) of replicate analyses; overall tech-
nique error is ^7%.
-------
1971
1972
1975
1974
1975
T? »:
73 HA
TS fS
T/ui'.f 2
lf.f.villf. salt wvrru disposed of
IN NON-POTABLH WATER
TB T3 n TP "IS T3 »0
TB f 10 TB «!1 T3 *12 T3 Hs;2
TOTA!.
4.6.!xt07 7.71x10s 1.91xl08 5.80x10s 3.19x10s 1.51x10"
5.SOxlO1 3.48x10' 4.64x10' 5.60x10s 1.59x10'
4.6.:xl07 7.71x10° 1.91x10° 5 - S 0 x X 05 3.19x:0e l.SlxlO6 S.90x10s S.EOxlO7 1:76x10'' 4.64x10s S.SOxlO5 l.S° '0'
3.SSxlO7 6.93x10° 1.63xl06 2.58xl07 3.19x)03 S.46 <107 1.47xl06 6.2?\107
4.38x107 4.53x10® 4.52x107 4.88xl07 l.llxJO8 8.03xIG7 2.S6xlOf 5.74xl07
5.4 7x107 S.StJxiO8 8.36xl07 2.0.10' 3.74x10"
1 .08x107 7.73x10s 1.03x10'
( TAF1LC 3
^ Ra-226 IK BRINE PROM TB »4 AND TB *$, LEEVILLE OIL FIELD
c»
I
TB Hi No Treatment 377 ~ 20 pCi/1
Acidified 319 9 pCi/1
Filtered and Acidified 313 5 pCi/1
TB iiS Acidified 260 +_ 8 pCi/1
-------
fOstCH«» > * tf*
iOJ'I'asa
V7 Gb'F.c 1
iliu1 \i l opose d study site
- 99 -
-------
EPA Technical Notes
ORP/CSD 76-1 A Statistical Analysis Of The Projected Performance Of
f'ulti-Unit Reactor Sites
ORP-CSD 76-2 Estimate of the Cancer Risk Due to Nuclear-Electric Power
Generation
ORP/CSD-77-1 Proceedings: A Workshop On Issues Pertinent To The Development
Of Environmental Protection Criteria For Radioactive Wastes
ORP/CSD-77-2 Proceedings: A Workshop On Policy And Technical Issues
Pertinent To The Development of Environmental Protection
Criteria For Radiaoctive Wastes
ORP/CSD-77-4 Plutonium Inhalation Dose (PAID) A Code For Calculating Organ
Doses Due To The Inahlation And Ingestion Of Radiaoctive
Aerosols
ORP/EAD 76-4 A Computer Code (RVRDOS) to Calculate Population Doses from
Radioactive Liquid Effluents and an Application to Nuclear
Power Reactors on the Mississippi River Basin (PB-261 322/AS)
ORP/EAD 76-6 Area Source Radiological Emission Analysis Code (AREAC)
ORP/LV 75-84 Radioactivity Associated with Geothermal Waters in the
Western United States - Basic Data (PB-251 971/AS)
ORP/LV 76-1 Radiation Survey in Beatty, Nevada, and Surrounding Area
(PB-252 670/AS)
ORP/LV 76-2 Parameters For Estimating The Uptake of Transuranic Elements
By Terrestrial Plants (PB-254 029/AS)
ORP/LV 76-3 Review Of State Licenses For Disposal Of Low-Level Radio-
active Waste By Shallow Land Burial
ORP/LV 76-4 Report of Ambient Outdoor Radon and Indoor Radon Progeny
Concentrations During November 1975 At Selected Locations
In Tfie Grants Mineral Belt, New Mexico (PB-258 257/AS)
ORP/LV 76-5 Evaluation Of Sample Collection And Analysis Techniques For
Environmental Plutonium (PB-253 960/AS)
ORP/LV 76-9 Sampling and Data Reporting Considerations for Airborne
Particulate Radioactivity
ORP/LV 77--1 Outdoor Radon Study (1974-1975): An Evaluation of Ambient Radon-222
6 Concentrations In Grand Junction, Colorado
ORP/TAD 76-1 Determination of Radium Removal Efficiencies in Iowa Water
Supply Treatment Processes
ORP/TAD 76-2 Determination of Radium Removal Efficiencies in Illinois
Water Supply Treatment Processes for Small and Large
Populations
ORP/TAD 76-3 Public Health Considerations Of Carbon-14 Discharges From
The Light-Water-Cooled Nuclear Power Reactor Industry
ORP/TAD 76-4 Available Methods Of Solidification For Low-Level Radioactive
Wastes In The United States
ORP/TAD 76-5 Determination Cf Radium Removal Efficiency In Water
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