U.S. DEPARTMENT OF COMMERCE
Rational 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
Feb 78
-------
NATURAL RADIOACTIVITY
CONTAMINATION PROBLEMS
rHBmnM Bf
Agency
Offles of RaflattM Programs
WattltatftM, DX. 20410
-------
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 NTIS; all others are
available from the Environmental Protection Agency, Office of Radiation
Programs (AW-46C), 401 M Street, S.W., Washington, D.C. 20460.
EPA Technical Reports
520/1-76-001
520/5-76-005
520/7-76-007
520/2-76-008
520/3-76-009
520/1-76-010
520/3-76-011
520/4-76-012
520/4-76-013
520/5-76-014
520/5-76-015
520/4-76-016A
520/4-76-016B
52C/4-76-017
52C/4-76-018
520/4-76-019
520/5-76/02C
600/4-76-027
600/4-76-035
520/5-77-001
520/4-77-003
520/4-77-005
52C/3-77-006
52C/1-77-009
Potential Radiological Impact of Airborne Releases and Direct
Gamma Radiation to Individuals Living Hear Inactive Uranium
M111 Tailings Piles (PB-258 166)
Radionuclide Accumulation In A Reactor Cooling Lake
ORP Program Statement (PB-258 159)
An Examination of Electric Fields Under EHV Overhead Power
Transmission Lines
Reactor Safety Study (WASH-1400): A Review of the Final
Report (PB-259 422/AS)
Radiological Quality of the Environment (PB-254 615/AS)
Significant Actlnlde and Daughter Activities from the
HTGR Fuel Cycle (PB-258 150/AS)
Recommendations Or Guidance For Technic To Reduce Unnecessary
Fxposure From X-Ray Studies In Federal Health Care Facilities
;?B-259 866)
Health Effects Of Alpha-Eir1tt1ng Particles In The
Respiratory Tract
Radiation Dose Estimates to Phosphate Industry Personnel
A1r Pathway Exposure Model Validation Study At The
Monti cello Nuclear Generating Plant
Environmental Radiation Protection Requirements For Normal
Operations Of Activities In The Uranium Fuel Cycle,
Volume I
Environmental Radiation Protection Requirements for Normal
Operations Cf Activities In The Uranium Fuel Cycle,
Volume II
Environmental Analysis Of The Uranium Fuel Cycle (PC-259 857)
A Preliminary Evaluation Of The Control Of Indoor Radon
Daughter Levels In New Structures (PB-252 670)
Federal Guidance Report No. 9: Radiation Protection
Guidance for Diagnostic X-Rays
Radiological Measurement At The Maxey Flats Radioactive
Waste Burial Site - 1974 to 1975
Radioactive Prediction Model For Nuclear Tests
Factors Affecting The Use Of CaF :mn Thermoluminescent
Dosimeters For Low-Level Environmental Radiation Monitoring
Radiological Survey Of Puget Sound Navel Shipyard, Bremerton,
Washington and Environs
Considerations of Health Benefit-Cost Analysis for Activities
Involving Ionizing Radiation Exposure and Alternatives
Radiation Protection Activities 1976
Summary of P.acioactivlty Released In Effluents From Nuclear
Powor Plants From 1572 thru 1975
Radiological Quality of the Environment In The United States 1977
-------
BIBLIOGRAPHIC DATA
SHEET
I. Mrpori No,
KPA 5Pr>A-77-15
3. Krci|i|rni'i Acfflii'M' N ».
4. l it If and Snl-1 >i lr
NATURAL RADIOACTIVITY CONTAMINATION PROBLEMS
5. Krport
February 1
6.
7. Aufhor(«)
8. Performing Orgnni/ittion Kcpr.
No.
9. Performing Organization Name and Addrc«.n
A REPORT OF THE TASK FORCE
Prepared by
Conference of Radiation Control Program Directors. Inc.
10. Project/Task/Work Unit No.
11. (lontrnct/(»rnnt No.
PUS 223-76-601H
EPA D7-0Q68
12. Sponsoring Organization Name and Address
U.S Environmental Protection Agency
Office of Radiation Programs (AW-h'jP)
Washington, D.C. 20^+60
13. I'ypr of Heport 8t Period
(!overe«!
14.
1
15. Supplementary Notes
16. Abstracts
Naturally-occurring radionuclide:; are ubiquitous: in t.he environment. Under
various5 circumstances these radionuclides primarily from the uranium arid thorium
decay series can contamiriar.e the environment to the extent that they pore real
or potential public health risks. The investigation and regulatory control of' t.he
impacts of most, of these 'sources have been greatly over]ooked by Fedederal and Ctate
agencies in the pant.
Thi:: report. provider, an initial asr.ecsment of the scope of the? contamination
problems, the priorities; for radiation control efforts, and recommendations for
problem resolution and implementation of effective control measures. Thin report,
is intended to assist those persons or agencies interested in the protection of
public health from naturally-occurrinp radionuclide contamination.
17. Key Word* and Document Analysis. 17a. Descriptor*
17b. Identifiers/Open-Ended Trtms
Natural radioactivity
Radiological problems
Radiation contamination
Fossil fuels
Ground water
Mineral extraction
17c. COSATI I ie IJ Group
Mineral processing Radon
Consumer product:.: I/ead
Construction materials Polonium
Phosphate industry Zirconium
Urani urn
Radi um
18. Arailability Statement
19. Security C lass CI his
Report)
IINC l-ASSIHl-D
20. Serunty < lass (This
I INC I.ASSII II P
21. No. of Pages
I/O
22. Price /
pcfibk/filFffO)
roRM ntihb mev. iotji KNDORSH) MY ANSI ANI> I'NfM t)
THIS HIRMUIV PI- RH'HuniK M>
l*rOMM.OC «?M.P74
-------
EPA-620/4-77-016
NATURAL RADIOACTIVITY
CONTAMINATION PROBLEM8
A REPORT OF THE TASK FORCE
Prepared pursuant to
PHS Contract Number 223-76-6018
which it partially funded through
EPA Interagency Agreement 07-0968
Printed February 1978
Prepared by
Conference of Radiation Control Progrs«n Directors, Inc.
With the cooperation of
U.S. Nuclear Regulatory Commission
U.S. Department of Health , Education and Welfare
Bureau of Radiological Health
and
U.S. Environmental Protection Agency
Office of Radiation Programs
Washington, D.C. 20460
-------
IABLE_OF _ C ONTF WT3
P'j
Forewort '
Preface v 1 •
Task Force Participants ix
History and Purpose of Task Force 1
Phosphate Industry B
H«-, cd! Aspects of Ihor'Mr- sr.d f?.:-t«hter Prr 2!
ka.iiuacti vi ty in Fossil l'ue'N
Radium ana Radon in Ground Water 40
Mineral Extraction an,a Processinq Act!vit.es 44
R3-.W in C;vg*> . . > ;
Standards and Guidelines Radioactive tfalfct ia- in io'^wr^y
and Construction Products . . ¦/,
Radioactivity in Construction Materials 65
Related EPA-Task Force Activities 73
Statutory Authority of States to Rf^jlate Natural ly-Occurrir.;
Radioactive Materials
Recof.iwndations 78
Attachments
Attachment A p.;
Attachment B PC
Attachment C »C
Attachment 0 92
Attachment F •"><
111
-------
FOREWORD
The Conference of Radiation Control Program Pirectors 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 1n 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 each 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 leadership with radiation 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, and to promote development of
control necessary to protect the public health and ensure environmental
quality. In this regard, the Environmental Protection Agency (1) develops
Preceding page blank
-------
radiation protection standards, criteria, and guidance, (2) conduct
social ervironmer.tal studies, (3) evaluate? radfatfon 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 Programs, through funding and direct technical
assistance, supports the Conference of Radiation Control Program Directors,
Inc., in its objectives and activities to assure an effective federal/
State partnership ir limiting unnecessary environmental and public radl-
a'i.m exposure. Selected Conference reports are published by the
t"r.vi»r.'.rr*ntal Protection Agency ard erv distributed to Federal, State and
leva! radiation protection personnel, industry, libraries, laboratories,
other concerned gn upi, and individuals fnese puh'ication; «re for
sale by the Government Printing Office and/or the National Technical Infor-
mation device.
°csder', are (ntouraged to «-#pgrt errors cr emissions ic th»;
Conference or the Office of radiation Program;.
Gerald . Parker
Chdi rran
Conference of Hadiatfon Control
v,'. D. f'.owe, Ph.D.
Deputy Assistant Administrator for
Radiation Programs
Environmental Protection Agency
Program Directors, Inc.
vl
-------
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 Task Force consisted of representatives from several
Stat? 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 intented to assist
those persons or agencies interested in the protection of public health
from naturally-cccurring radionuclide contamination.
v11
-------
This document should be of special interest to State, arui
Federal radiation protection personnel in the United States snd.otiier
countries.
L. Hall Bohllnger, D.Sc.
Nuclear Projects Coordinator
Nuclear Energy Division
Division of Radiation Control
y/w*
/
Richard J. Guimond
Criteria & Standards !?1 vision
Office of Radiation Programs
Environmental Protection Agency
vi 11
-------
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. Boothe
Radiation Control Service
Oregon Department of Human Resources
Dayne H. Brown
Radiation Protection Branch
North Carolina Department of Human Resources
Michael Christie
Radiation Control Section
Idaho Department of Health and Welfare
U1ray Clark
Radiological and Occupational Health Program
Florida Department of Health & 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
-------
HISTORY ANO PURPOSE OF THE TASK FORCE
Task Force No. 7 on Natural Radioactivity Contamination Problems
was established by the Executive Committed of th •> National Conference
of Radiation Control Program Directors in 1975 as an extension of Workshop
No. 5 of the 1974 Annual Meeting of the NCRCP0.
The charge tc 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;
Asses* the Impact of naturally-occurring radioactivity
cor lamination in the general environment and the Conference-
member States; and
(4) Serve as a focal point for State ;nout to the program:. cf
Federal agencies.
The charge given necessarily implies certain ressonaibill ties in
which the Task Force must assist the appropriate State and Federal
agencies. These include the following:
(1) Defining the rr.diat-ion level or concentration or stage of
urtceti 1 :'-3 .:V ret;-! *1 «/-•:. ccur ring r.vj; oak t i ve pateri"!
{-'0*-:) lo the f.r.virvnuei-t;
{<) Tying **ho uaihority to de/eloj) and implement
guidelines and criteria for enforcement action;
(3) Identifying the Impact that naturally-occurring radioactive
contalmlnation has on the general population;
-------
(4) Examining the need for control on the use of products and
byproducts containing NORM 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.
- 2 -
-------
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-
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 radionuclides, public health problems are usually limited to
the 30 or more radionuclides in the uranium and thorium decay series
because of their relative abundance and toxicity. The increased incidence
of bone cancer in radium 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 " -adioactive tailings and the use of reclaimed phosphate mining
lan. u 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 more
appropriately is concerned with exposure to radiation occurring as a
result of alteration of the natural sources by technology. This new
category for human radiation exposure, introduced by Gesell and Pritchard,*
is termed ' ' ologically enhanced natural radiation" (TENR), and is
- 3 -
-------
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 1n a structure constructed over phosphate mining reclaimed
land hould constitute a TENR exposure; however, an exposure from a
radium needle would not, since the latter is expressly designed to
produce radiation. 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 niillirens per year to the tracheobronchial surface tissue of the
"jng, mainly a; a result of inhalation of radon daughter products froni
ar.i-:.
-------
The problem areas examined by the Task Force are as follows:
A. The phosphate Industry
D. The radiological aspects of throlum and daughter products
C. Radioactivity 1n fossil fuels
D. Radium and radon 1n ground water
E. Mineral extraction and processing activities
F. Radon In caves
G. Standards and guidelines for radioactive material concen-
trations in material and consumer products
H. 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 model 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 1975, 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 the
magnitude of the problem. Radiation surveys were taken using a M1cro-R
meter over reclaimed land and housing projects, near slag piles, and
over roads constructed with phosphate byproduct material. A report of
tMs meeting was submitted to the Conference in January 1976 and can
be made available to interested parties. Later in September, 1976, a
follow-iip meeting was held in Baton Rouge, Louisiana, at which time Task
Force members toured a wet process phosphoric acid production plant,
- 5 -
-------
prepared a working outline for preparation of the final report, assigned
specific areas to be completed by the members, and established preliminary
recommendations.
- 6 -
-------
references
Gesel 1, T. F. and Prichard, N. H*-, 'The Technologically Flthancod
Natural Radiation Environment, Health Physics, V. 28, No, 4, 197
Radiological Quality of the Environment, U. S. EPA, CMP,
EPA-52/1-70-010, 1976.
-------
PHOSPHATE MDUSTRY
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
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 p
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 rarketable 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 envirorurent mc ? u ! 'ha; : ry* • i ia:
in the ores, wastes, and ot her materia !•...
The standard mining practice in Florida ~c tn ovorhi;rd*»r>
and nnne the phosphaie nu.triy.. Thi'j overburden i:> .,Uckeci -.»r» uf-ii.i»ei:
ground adjacent to the mining area. Approximately £>UOG acres of land
- 8 -
-------
are 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
P2C5 concentration. The output materials from this operation are
marketable phosphate rock, sand tailings and slimes. These materials
are produced in a ratio of about one to one to one. Table 1 lists the
uranium, thorium, and radiuir-??6 activities for these materials.
TABLE ): Natural Radioactivity Concentrations in Florida
Phosphate Mine Products and Wastes (pCi/gm)^
Mate- . Ra-226 U-238 Th-230 Th-232
/ XdrW'tiLle f-.ock 4i 4' 3 0.'4
Siimes 41 44 4t 1.4
Saricf Tailings 7£.3 0.,-s^
In beneficiation, water is used for proce^ing in Addition *o
bev.o "jscd ac. a transportation medium. Minen-out areas ar" usf-d f'>r the
disppsal of sand tai'.ings and slimes, in addition to overh'jrd'»r.. Several
Florida slime ponds have discharge' Ic the ervironnenr,, ?irr.*>f fciatim
wastes arc present in che si Th 1 ioe discharges was le'.s than 5 pCi/l'ter nt al1 facilities. The
..•r.nis'.alvcd radiw"- 2?6 ropi.«»»lrat ion r^n^el '*m 10 t, ; jO" i/1 i ter
^fid was Mghly dependent on the total suspended solids in the slimes.
Although no chemical process is used to treat the discharqe from tie
slime ponds, concentrations of radium-226 in effluents were all less
- 9 -
-------
than 3 pCi/1iter. The reduction of total radfum-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 pla-e in "wet process" phosphoric acid plants and electric furnace
plants, '¦•"-.pectively.
In the "wet process" phosphoric acid plant, the raw materials are
yround phosphate rock, 93 percent sulfuric acid, and water. Phosphate
rory is mixed with the sulfuric ac id. This reaction produces phosphoric
arid and gypsum, following the reaction in the attack vess'1 . the
^i.xturo ifiltered to '.he oypsurr frvjir the nhoreboHr vid.
T'; ¦ qyp,>iii' i • pumped as a slurry to a 'large pile near the facility where
i* I:, allowed to aewater. iince approximately 4 netric tons of gyroum
arc >cduced per ton of phosphoric Kid, -i >.r, sul t'.or. id.
Tab!- is the .-.verage radioactivity conr»>tcMti' ns f-<>
f>-r i 1 i^er ;md oh ispbc;)ypv:jip •syfJS'oduct of several wet-procs«..r,
-• ¦. f3vi: it ic i
-------
TABLE 2: Natural Radioactivity Concentrations in
Materials Produced from Florida Phosphates (pCi/gram)
Material
Ra-226 U-238 Th-230 Th-232
Normal Superphosphate
Oianinonium Phosphates
Concentrated Superphosphate
Monoanmonium Phosphates
Phosphoric Acid*
Gypsum
21.3
5.6
21
5
33
20.1
63
58
55
25.3
6
18.0
65
48
50
28.3
13
0.6
0.4
1.3
1.7
3.1
0.3
*29 percent acid.
Each "wet process" phospf ; .id 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 water for discharge to tne 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
'odionuclides from the effluent. Radium-226 reductions of greater than
96 percent were 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 in phosphoric acid plant discharges.
- 11 -
-------
In the thermal processing of phfphate rock, silica and cok« ,j<-e
added; this inixture is electrically reduced to form elemental phosphorus.
Ferrophosphorus and calcium silicate slag byproducts are also formed in
the process. Data from analyses of these sa^pV-. 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 Utt
Approximately 100,000 acres of land have been rined for phosphate
rock in Florida. To datt, about 25,000 acre;, of the- mined laid', hcv
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 overburden, leach
zone material, matrix, sand tailings, and/or slimes, fre';.jpntly
contain radiL""-226 concentration substantially higne»- tnan the 0. i to
pCi/gram typical of U.S. so* •<. Concentrations ».;r> to 99 DCi/s fm>*
been measured in tnese reclaimed soils. However, radium-?26 concen-
trations in the reclaimed land soils generally range between 10 to 30
pCi/gram. Such radium-226 concentrations often persist to soil depths
greater than 20 feet. Due to the elevated soil radiun-226 rnncentra-
tions, a considerable quantity of radon-222 is produced, This radon-???
diffuses to the ground =!!:« ri.~-i.iv.jr. tv *• • •. •: .re. ...
where it can lead to the buil.iuo of short-i • .r,v.. : . k
indoor environment. Data on average crosr- *ru'..-r --..j - h tv-
over a one-year period were obtained for several \tr:;:. e- * :
radom on reclaimed land and on land distant fro*, the Hor-ida phosphate
regior. The d;»ia frof- these structures are vjmnarizej in Tat/le 3.
- 12 -
-------
TABLE 3: Percentage Range of Ra-ion r>*i3*t
Reclaimed Land (n=13) L?«-d i••>-'>}
0.0b to 0.1 WL : 38% 0,05 5# r -l-
n-01 to 0.05 WL : 31% %':? H: kl : 22'.'
0 to 0.01 Wt : 31% 6 »o li.Ul WL :
From the data obtained to date, it is teiiev?d -> .«.r: '»•;
excess lung rancer risk associated with the higher levels, warra;-..
additional studies to delineate more fully the scope and magnitude of
this problem. Based on the assumption thit fxcesr- lw lonvr
a general population, the estimated neaith risk would be proportionately
greater, possibly by as much as a factor of ?. *?e rengn ?*•:>. •:^>irr,e,
the need for further efforts to reduce the large imo?rt?inrie*- in these
risk estimates.
Principle Exposure Pathways
There are numerous pathways which could cause exposure -.a re-
public due to operation of the phosphate industry. These include txposjres
r.ir.9 from eft iu«a%. em is*-ions, around wafvrs, .» • a ?:.< -.j.r,-
j.rocutts and byproducts, living and working on reclaimed land, arc
working in industry.
As shown by the data presented, the effluent'- rem •-.hoiph.-ite "int
slime ponds and phosphoric acid plants are readily controllable to limit
- 13 -
-------
ir.r.'il r.sdIdischarges to surface waters to less than 3 to 4 pCi/liter.
•'=•'? two principal >•» ;ers in Honda receiving such effluents are the
••••»> i'i '3 ?("•.p'! to down'cream users. However, accidental failure of slime
¦unci dikes could significantly increase the radium-226 concentrations in
Mie rivers since slimes contain greater than Z00O pCi/liter total
v j j i! ¦ i c*:.
m "hjllovn we I'i water supplies in the Central Florida area hje»e
;o >:-5.!ta«« racJium-226 concentrations greater than ::he lir.rit
of pfi/l iter i-,idiuw-;C(t and radium-220 established by the Fnvironmental
Pretect;or Agency's Safe !V inking Water Regulations of 1975. Howeve>\
since no •• .;.ev: :ieot '.a*; made of these around waters prior to extensive
minimi, >. ipresently uncertain to what extent the levels are due to
thn presence of uranium in phosphate ores or the operations of
Uie i'l'-sfy. Additional work is underway to investigate this question
further.
Da ta collection end evaluation of a*r em is?.-; or..-; from <*'wntrt
phosphorus and phosphoric acid plants are incomplete. He.••ever, there
are sor;c preliminary indications that significant quantities of Po-210
- 14 -
-------
may he emitted *rom r.hese facilities due to volatizdtion d'.irinc ^alcinino
or furnace operations.
Workers in the phosphate operations come in close contact, with
large amounts of phosphate ores, products, and wastes along with i'-.r. : Tt.i::n
or dust generated by unloading, crushing, drying, ana other activ t.
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
namrria doso. equivalents for workers in phosphoric acid or elemental
r
phosphorous plants range from 30 to 300 mrem per year. Tne annua;
dose ecuivdlent rite to the tracheoL'rcnchial region of the luiq, due to
inhalation oi radon daughters, has been estimated co d.: a hicjn as 5
rein/yt 1'c.r those workers. Estimates of the average lung dose wo:.ic > .. f
course be very much lower.
fro:;: 'he data collected and analyzed to date, population txposurrs
to the indoor raooii slaughters in structures appear to be the most, -.igni-
iicant public health problem, and efforts are being made to develop
radiation protection guidelines to evaluate and control exposures to
this source, As an i titer i>n measure, the EPA has provided the SUte . f
Tio.-ida a screening level which allows continued land development without
a significant health impact. This interim guideline is based on a quiwa
exposure of less than 10 uR/hr (including background) v#hich can he
associated with a. estimate of a raden daughter level less than 1.1.01 WL.
Other aspects of the industry which require farther study .
tie impact of using byproduct slag and gypsum for construction .• uls
- 15 -
-------
the uptake of radionuclides by crops due to fertilizer use or growing on
reclaimed lands, evaluating control technologies to limit indoor radon
daughter levels, assessing the impact of recovering uranium fuel from
phosph*tfc i aterials, and the use of defluorinated phosphate as a livestock
feed supplement.
Phosphates as Livestock Feed Supplements
The presence of uranium (2-180 ppm) in livestock feed supplements
has been reported in proportion to their phosphorus content. This is
due apparently to the transfer of uranium with phosphorus fror, the
original rock phosphate to the feed regardless of whether the mineral
has beef', chemically processed or used mor~ or less directly. The occurrence
of radi't
-------
Thus it appears that the uranium content of feed supplements should
not be of great .-.eaith significance to the cow or man based on current
guidelines.
Of greater concern was the radium in the supplements. Using the
60U K«j cow and assuming (1) that 0.02% of the dose of ingested radium-226
is secreted into the cow's milk per liter and (2) that the highest Ra:P
ratio feed 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
to be 0.7 pCi/1. The cow's daily ingestion from the supplement would be
dp-iri'iy.wlately 3^53 pCi. Published volumes for radium in milk range from
O.Cs-C.3 pCi/i. The FRC rc'cocunended maximum permissible radium-226 dose
1or a human being is 20 pCi/day. In order to achieve this ingestion
rate, one would have to consume approximately 29 liters of milk per day.^
A- a result of the foregoing, the radium content 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 and the possibility of radon buildup resulting in
occupational exposure. Data is currently unavailable for evaluation of
this potential exposure, however research is currently on-going.
This Task Force does not consider the radioactivity 1"n 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 bfe completed.
-------
Uranium Recovery
Uranium for use as a fuel in nuclear power plants has historically
been extracted from Western ores 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, U3O0 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 phosphates
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 - $15 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 more risky and costly than others. While recovery
from facilities with the capacity of 200,000 tons per year nay
become practicable, initial recovery efforts will probably be restricted
to larger facilities. In 1976, the capacity of wet-process phosphoric
acid plants (greater than 200,000 tons P205 per year) was about 7 million
- 18
-------
tons ^2%' dmount- phosphoric acid would contain about 10 million
pounds of UjOg which is enough to fuel about 20 one thousand wqaw«tt(e)
nuclear power plants per year.
The U.S. Environmental Protection Agency is presently conducting
studies to determine the environmental impact of uranium recovery from
12
phosphoric acid. In general, potential exposure*, are anticipated
to result from emissions, effluents, dust in calcininq and packaging
operations, and transportation. At. this time, it is dif'f'iit to esti-
mate the potential inpact although it is not expected to be of major
sicnif icanct'.
biMji recovery tYw ec.per solutions throve r. ion i--y change
is rvi-'-ft ; on?idered at M-v^ral mine-will op*rat ion'-.. "h-. potential
rart'olo'iical rnpft ?f th-;:, recovery *s jrkr. ¦¦*/!: <;l p* ~ ?. 1 though it
-.-e s'^Ur to ion r-xefcarnje i^era " ".->:.*r,t ^ines.
- 19 -
-------
REFERENCES
1. Menzel, R.G. "Uranium, Radium, and Thorium Control in Phosphate Recks
and their Possible Radiation Hazard," J. Agr. Food Chem., Vol. 16, No.
2, pp 231-?34 (1968). ~
2. Guimond, R.J., Windham, S.T. "Radioactivity Histribution in Pho*-..Loft-
Products, Byproducts, Effluents, and Waster,, ORP/CSO-76-3, U.S. Environmental
Protection Agency, Washington, D.C. (August 1975).
3. Stowasser, W.F. "Phosphate Rock," 1964 Bureau of Mines Mineral Yearbook,
preprint, U. S. Department of Interior, WPiTngtonr~D.C. ' "0*9767."
4. Office of Radiation Programs: "Preliminary Findings - Radon Daughter
Levels in Structures Constructed on Reclaimed Florida Phosphate Land,"
Technical Note 0RP/CS0-7£j-4, M.S. Environmental Prot
-------
RADIOLOGICAL ASPECTS OF THORIUM AND DAUGHTER PRODUCTS
Thorium-232 is the 35th most abundant element in the earth's crust,
O.OOl to 0.002 percent being most generally accepted. It is about three
times more plentiful than uranium-238.
Uses
!n 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
Iight-emitting qualities of their oxides. Even to this day,
the Coleman gasoline camp 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 work
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), and 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.
- 21 -
-------
D. 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-Mo
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.
This 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
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.
- 22 -
-------
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 this 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 monazite, 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 sands 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 cotimercial 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 cornnerdal
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
- 23 -
-------
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
aiso 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, New Zealand.
Similar deposits are found in Central California gold placers, especially
along two rivers, the Tuolumne and Consumnes. As mentioned above,
recent discovery of thorium veins in the iJ.S. containing either ronazite,
thorionite, thorite or all three, could provide a oreat resource for
this country easily exploitable in the near future.'
Preparation
The established thorium extraction process starts from monazite,
the chief commercial ore. Monazite is chemically inert, and the dissolution
or "opening" process must be drastic; highly concentrated solutions of
sulfuric acid or sodium hydroxide at 140°-150° 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
separation from impurities. Good ventilation is necessary to carry away
- 24 -
-------
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 the pure metalJ2»3)
liadtoto^eal PrtWems
The extraction of thorium from its ores leaves thorium-235 in the
purified material which decays directly to the short-lived (TS = 3.64 days)
parent of thoron. Even outside of the mining and extraction of thorium,
conmercial non-nuclear usage, i.e., in mantle making, ceramics, electronic
tube filament making and ether such industrial handling, there is the
hazard from the inhalation of thoron (radon-220), a daughter product of
thorium. There are not near as many epidemiological studies compared to
\
radon-222 in the providing of evidence for an exposure-risk relationship.
\
Although natural levels of thorium in soil and construction materials
'v
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 associated with thoron (P, = 55 seconds) as wi th
radon-22? (T'a = 3.8 days). The short half-life of thoron means that the
air concentrations are generally much lower than tho'-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
machining and usage of the metal.*
The deposition of the thoron decay products depends mainly on (1)
the fraction of inhaled uncombined radioactive atoms; (2) the particle
size distribution of the carrier aerosol of the combined radioactive
- 25 -
-------
atoms; (3) the concentration of thoron daughters in the local atmosphere;
and (4) the degree of attachment of these daughter ions to the aerosol
particles. The consequent lung dose further depends on t^e deposition
distribution in the tracheobronchial tree and within the varioi:: mucous
layers. The "working level" concept originally cpplied only to radon
daughters (MPC's). This has, 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 each of the thoron daughters per liter of air as was done for radon.
However, now the preferred definition is merely any combination of ra
-------
be used in describing inhalation doses. There has been a preponderance
of models from different authors al i producing widely uncomparable
result's. 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.
- 27 -
-------
REFERENCES
1. Staatz, M.H., "Thorium Veins in the United States", Econ. Geo!., Vol. 69,
1974, pp. 444-507.
2. Nininqer, R.D., Minerals for 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., Thorium: Preparation
and Properties, The Iowa State University Press, Ames, Iowa, "1975.
4. Jacobi, 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. Khan, A.H., Dhendayuthem, R., Raghavayya, M., and Nambiar, P.P.V.J.,
"Thoron Daughter Working Level," Paper delivered by the Health Physics
Division, Bhabha Atomic Research Centre, Bombay, India.
- 28 -
-------
RADIOACTIVITY M FOSSIL FUELS
Description of tli« 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 fessil fuels. For
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 environment. 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 fossil fuels.
Activities tc Date
The "ddiological impact of natural gas as a source of radon has
(12 3)
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 study around a coal-fired power
plant utilizing Eastern coal." The Oak Ridge National Laboratory has
measured trace elements at the Allen coal-fired steam plant which also
utilize" [.astern coal/' The Idaho Department of Health and Welfare,
Radiation Control Section has performed an evaluation of a proposed 1000
MWe coal-fired power plant which would utilize Western coal.''
- 29 -
-------
The conclusions and recommendations in this report are based in
part on the resuTts.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 hy
g
the EPA. The annual dose committment from radon in natural
gas has been estimated to be 2.73 x 10^ man-rem. This dose
conmittment 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 deplecing
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 gas
- 30 -
-------
necessary for a local radon problem, no reconmendations are
made here regarding the continuous evaluation or monitoring r.f
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 hy
Gordan. The radium-226 content of fly ash from oil-fired
plants is 21 times less than the radium-226 content of fly ash
g
from coal-fired plants. It would appear then, that the
radiological impact from oil-fired plants would be insigni-
ficant. Therefore, no recommendations are made 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. Vine10, large potential reserves
of uraniun: are contained in coal and lignite, and the con-
centration of uranium in the ash of coal provides a oossible
means of recovering uranium as a byproduct. Uranium bearing
lignite occurs in the Fort Union formation of Pal eocene aqe in
the Northern Great Plains, in the Salt Lake formation of
- 31 -
-------
Pliocene age in Southern Idaho, and in Tertiary sediments in
Nevada and Southern California. Uranium-bearing coal is
present in the Wasatch formation of Eocene 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 high rank, low ash coals of the type
most desired 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 type
of coal most suitable for fuel) capture less than a fifth and
slightly more than a third, respectively.
10
In a report by Abernethy ^nd r;ib:-on ' , values of the uranium
concentrations in Western coal are, on the average, 2 tc IOC
times higher than in Eastern coal.
- 32 -
-------
The radiological implications of the extensive combustion of
fossil fuels has been briefly dealt with in past literature.
The radium-226 concentrations in European coals, in fly ash
from power plants, and in contemporary fossil snows have been
documented. The 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
require modification for the utilization of Western coal,
since both studies addressed only low uranium content Eastern
coal.^
The State 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 Wyoming.
1 -iL1 e 1 yives the estimated releases from such a plant and
compares these releases to maximum permissible release con-
centrations to unrestricted areas. Tho assumptions used in
calculating the releases are listed in footnote (1) of the
- 33 -
-------
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 Bridger
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 ash 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 recotrmendations 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.
- 34 -
-------
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.
The EPA and appropriate States 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.
- 35 -
-------
TABLE 1
STIMATED AVERAGE AIR30RNE RADIOACTIVITY RELEASES FROM PIONEER - TWO UNITS, 500 Mwp EACH^1)
ISOTOPE
Uranium Series
238u
234u
230jh
226Ra
??SR"
210po
210Pb
Thorium Series
232jh
228Ra
22?Th
Ra
U>
224
212pb
RELEASE CONCENTRATION
(iCi/ml x 10") _
4.63
4.63
4.63
4.63
1545
1545
4.63
3.63
3.63
3.63
3.63
3.63
MAX. PERMISSIBLE RELEASE^ ? RELEASE
CONCENTRATIONS (uCi/ml x 1014) STANDARD
200 2.31
400 1.15
30 15.43
200 2.31
300,000 0.52
700 220
800 0.57
100 3.63
100 3.63
20 18.15
2,000 0.18
70,000 0.01
RELEASE/YR
0.0031
0.0031
0.0031
0.0031
1.0280
1.0280
0.0031
0.0024
0.0024
0.0024
0.0024
0.0024
TOTALS 267.89 r' 2.083 Ci
(1) Assumes: (a) 0.3£ release of all trace elements in coal except 210po an(j 222Rn poos release).
(b) Uranium and thorium are in equilibrium v.'ith daughters.
(c) Coal contains 0.23 pCi/g U and 0.18 pCi/g Th.
(d) Total effluent is 4.48 x 10® ftVmin.
(e) 562 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 I!. Assumes radioactive materials particulates are
insoluble.
-------
TABLE 2
Jim Bridger Fly Ash
GJ
ANALYZED BY
LFE
LFE
LFE
IJT.
ISOTOPE
Uraniun Series
238u
230^
226^
22®Ra
210ft,
Thorium Series
23%,
Ply Ash #1
(12/75)
pCi/gU) , g(2)
4,7
.3
LIE
NOTES:
(1) Based on dry weight,
(2) o is one standard deviation due to counting statistics.
Fly Ash #2
(11/75)
c<2)
8.58
* 1
2.57 «
.3
7.0
1 .4
3.3 *
.2
4.9
! .2
2.4 «
.1
3.8
« .3
__
18.0
i 1
3.0 *
.2
2.8
-------
REFERENCES
1. Johnson. R.H. , Jr., Bernhardt.. U.K., Nelson, N.'-',, Calley. H.W., Jr.,
I!>73. Ass* ¦si-ineiM of !_*>( ent. iaj_ Pad if > I oyi <-a_l HcaUh Effects from Radon
in datura I Gas, EPA-f>20/lI (X>1, Wsivhi n*rt< »n ,~R .C. " * ~
2. (a >s« • i 1, T.F.. Radiologica 1 HeaUh lnpl i cat ions of Radon in NaturaJ Oas
;,r"' ">,aiu.riil G>as j^xxTticTs - Final Rejxrt. A report, of the University
ol Texas Health Sri ewe Otiter at Houston, Schrt of Uie SJudv «>f Publjc Hrsil Ui Asepct s
o_f F'ossil Fuel :md Nue I ear PtnwT Plants. SouC beast om Itidiolonical Health
Ialjoratory, jSireau of Radiological Health, U.S. Public Health Services.
.r>. Hedrosian, I'll., Easterly, D.G., Cunning, 8.L., 1970, "Radiolr>gical Survey
Around hwer Phuits Using Fossil Fuel", Office of Rei-warch ;>nd *lt>nitoring,
U.S. Km irnnmental Protection Agency, KERI, 71-3.
<1. Hoi ton, NIW , 7Yace >nt Measurements at t he Coal -Fi re<1 AHen
Stream Plant, Process Report, June 1971-1973, C\ik Ridge National i afx >rat.ory,
01M^NSK-ij>-13. " ~ "
7. Boothe, n.F., 1976. An Evaluation of U*» Radiological Aspects of the
Proix^sed Pioneer Coal-Fired Plant. Radiation Qmtroi Section, Division
of I jivi ronment., Idalx) Detriment of Health and Welfare, Boise, Icfciho.
8. Reference No. 1
!). Reference No. <1
10. Vine, J.D. , 195f>, "Uranium Hearing Q>al in the United States", Contribution
the Unitod Staters Geological Survey and Atomic Energy 0t amission for
the L'ni t
-------
13. Jaaorowski, Z., Bilkiewiez, J. and Zoylica, E., 1971, "Ra-226 in Gcntanporary
and Fossil Snow", Health Physics, 20, 449.
14. Reference No. 6
15. Reference No. 5
16. Bcwe, W,D., 1975, A letter to Ms. Margaret Reilly, Department of Fhvironmental
Resources, P.O. Box 2063, Harrisburg, Pa., Deeenfcer, 1975.
17. Reference No. 7
- 39 -
-------
RADIUM AND RADON IN 6R0UND 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 ana 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 be found in concentrations greater than
50,000 pC i/1.^ a n0k]e cds, radon in water is readily released
with mild aeration. However, the radioactive daughter! in various
stages of equi1ibr!jm wi11 remain in the water. Because of the potentially
high levels of radon in water, it is possible in 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 devoted to the health signifi-
cance of ingested and inhaled radon and radon daughters from potable
water supplies. A large segment of our population is subjected to
exposure to all of these natu^ally-occurring radioisotopes throuqh the
use of private, commercial, agricultural, public, and community ground
water 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 drinking water.^ Additionally, several
- 40 -
-------
States have initiated and/or completed studies of rarMun and r?.¦-!»r
concentrations in their ground water supplies. However, only a limited
amount of research has been done on the health effects of ingestina
radon and its daughters. Much of what has been -lone 13 through ur~rdi-
nated efforts and has been inconclusive. Researchers h^ve evaluated the
radium decontamination characteristics of conventional water treatTOn*
techniques and have also developed and evaluated special radium removal
techniques.^
Area of Concern
If the EPA drinking water regulations are to be enforces, there
will be a large number of ground water supplies which wi' 1 be '"c.;u> rc-r.
to undergo radium removal procedures. As this occurs, consideration
will have to be giver, to the disposition and disposal of r:ate 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 with 100C pCi/1 radon-2P? could
e
result in air concentrations of 1 pC.i/1 due to normal residential use.
Further, they have estimated that if a population uses potable water witr.
a radon concentration of 500 pCi/1, 20 health effects per year 1,light
resu from inhalation for every one million people exposed.
Bfc-ause of the comparatively large concentrations associated with
radon and its daughters in drinking water, it is tpsirable to better
- 41 -
-------
understand the health significance of these radioisotopes from the
viewpoint of ingestion. Little work has been done in this area, yet it
is not uncomnon 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 ground and geothermal
waters may be used for food cro/> irrigation, there are ouestions which
nust 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.
- 42 -
-------
REFERENCES
1. Grime, W.N., Hioglns, F.B., Smith, B.M., Mehaffey, 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).
?. Golden, J.C., Jr., "Natural Background Radiation Levels in Florida",
SC-RR-68-196, Sandia Laboratories, Albuqueroue, N.M. (May 1968).
3. Fong, S.W., Mantiply, E.D., "Environmental Radiation Surveillance 1974-1975
Report", DKS-5863, 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, July 9, 1976.
5. Brinck, W.L., Schliekelman, R.J., Bennett, D.L., Pell, C.R., Markwood, I.M.,
"Determination of Radium Removal Efficiencies in Water Treatment Processes",
ORP/TAD-76-5, U.S. Environmental Protection Agency, Washington, D.C. (December
1976).
L>. Duncan, D.L., Gesell, T.F., and Johnson, R.H., "Radon-222 in Pntabli1
Water," Conference Proceedings, Health Physics Society Tenth Midyear
Topical Symposium: Natural Radioactivity in Man's Environment, October
12-16, 1976, Saratoga, New York.
- 43 -
-------
MINERAL EXTRACTION AND PR0CESSIN6 ACTIVITIES
Numerous industries such as copper, fluorospar, vanadium, bauxite,
"itanium, and rare earth's mining and processing, extract ores which
often occur in strata containing above-average concentrations of urar,,; 'jrr,
thorium, and their daughter products.
Unfortunately, little 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
•iiidij?'~ry arc! Lhc zirconium extraction process.
Major copper deposits occur generally in three regions of the
¦irited States. These are the Appalachian Province, Keweenaw Peninsula
(upper Michigan), and the Cordilleran Province (southwest United States).
The latter region, consisting of Arizona, Utah, New Mexico, and Nevada,
snconiposses 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 beneficiation utilized in
the copper industry. They are hydrometal1urgical processing, physical-
chemical 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 the Copper Ore 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.
- 44 -
-------
from the presence of a uranium co-deposit. 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 from 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 mines 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 ppr:) by a factor
of 11 to 38. An average l^Og concentration of up to 100 ppm is estimated
for the primary copper zone of this mine.
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.
- 45 -
-------
80-
STANDARD DEVIATION = 0.0029 %>
MEAN - 0.0055 £
u
til,!
0123456789 10
15
20
4 CHEMICAL U3Qg x 1000
(t. e. 7 - 0.007)
FREQUENCY DISTRIBUTION GRAPH
URANIUM CHEMICAL ASSAY DAT A, COPPER CITIES
441 SAMPLES
f POM STILL. A.P. . URANIUM AT CO^KP CUinS AND OTHER PORPH Yr.Y
COPPER OK POSIT S, MIAMI JM:.Tr»;C T. ARIZONA (UNPUB THESIS), HAHV."- R D
UNIVERSITY. CAMBRIDGE. MASSACHUSE VTS »19o2). REPRINTED BY PERMISSION.
-------
Moxhan, ejt aj^ measured the radiation levels of hydrothermal1y
altered rocks in the vicinity of several copper and copper-lead-zinc
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
obflined for the Bagdad deposit are oraphed 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 Mew Mexico. Their results are tabulated in Table 2. These levels
are not consistent with background levels, which are on the order of 4
ppn for igneous rocks of this region. One explanation for these observations
is that the ore samples analyzed are not from the highly mineralized
prinary ore zone, but from associated zones. Assuming, though, average
cor.cenrrations in the mineralized zones an order of magnitude higher 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,
bot* 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.'' The mine operations surveyed
art- t'if; Wh i t.e Pine (Michigan), Butte (Montana), the Old Reliable, and
Bagdcd (both Ar i,:o?ia). The radioactivity levelr, measured are tabulated
In several underground copper n:ines, radon daughter concentration
levels have posec' potential health hazards to rrining personnel. As part
- 47 -
-------
TABLE 2
Average Abundances of Uranium in Porphyry Copper Intrusions
and Barren Intrusions of Similar Composition*
Average
Range
Location
Occurrence
Samples
ppm
ppm
Uranium
Uranium
New Cornelia Mine
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.?
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
*Uranium spectrometrical1y analyzed. All analyses are from whole-rock
samples except for soil samples of uranium at New Cornel ia P'luton, Gross
Peak-Martin Ridge, and Turquoise Mountain.
- 48 -
-------
TABLE 3
RADON-DAUGHTER SAMPLE CONCENTRATIONS
IN UNDERGROUND COPPER MINES BY STATE
Mine
Location
No of
Samples
Average Radon
Daughter Cone.
(WL)
Range of Radon
Dauqhter Cone.
(WL)
Approx. Avg.
Existing
Ventilation
(CFM)
Indian Creek'
Missouri
8
0.023
Virurnum*
Missouri
8
0.065
Eagle Mine**
Colorado
10
Less than
85 Mine
New Mexico
10
0.180
Wh.ite Pine
Michigan
11
0.030
Calloway
Tennessee
11
Negligible
Copper Queen
Arizona
42
0.330
*Lead, Zinc Copper
**Lead, Zinc, Copper, Gold, Silver
.004 -0.116
.002 -0.117
Not Available
0.060 -0.280
0.01 -0.04
Negligible
0.02 - 1.7
Not Available
Not Available
Not Available
10,000
330,000
Not Available
5,000
^Data provided by ll. S. Dept. of the Interior, Mining Enforcement and Safety Administration,
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
activity levels.^ High activity 1s a strong Indication that above
background concentrations of uranium exist within the copper matrix.
The radon daughter concentration data for underground mines 1n Arizona,
flew Mexico, Michigan, Colorado, Missouri, and Tennessee are given in
Table T
As the data shows, the highest levels were recorded 1n 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 copper mine sampled in Tenriessee 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 foi er
group, the potential environmental interfaces would include exposure due
to: I) utilization of copper mill tailings; 2) construction on reclaimed
uraniferous mining land; 3) seepage from tailing ponds; and 4) radon gas
emanation and dust from waste piles.
- 50 -
i
/
-------
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 t>3 27.3 <0.1
Butte (Montana) Kelley Operation Mine Water 4.8 <0.2
Berkley Pite Mine Water 1.5 <0.1
Continental East Mine !\'ater 3.0 <0.1
Input to Emergency Pond 1.7 <0.1
Old Reliable (Arizona)
Bagdad (Arizona)
300' Level Mine drainage
East Pit Mine Water
West Pit Mine Water
2.6 <0.1
1.6 <0.1
12.7 0.25
*Performeci under contract to U.S. Environmental Protection Agency, Effluent Gulielines Division
-------
Utilization of copper sn'l failings has been of a negligible scope
itrsr ifp th" vast amounts available. While other mineral tailing wastes
find suitable ipplicatiens, there are a number of reasons why copper
' I tdi> i'.yi >ave not:
i. The projected growth for building construction in the Southwest
¦jnil fountain !-itaN-s is the lowest in the country,
i. ra'isyortat ion >.osts would its use uneconomical outside
the i»nnedi'itc vicinity of the i ine.
'-'(i" ") its hi'jh filir.Ue content, impaction is difficult
•'aki.ij ;ts use as ? construction or fill r«terial unsuitable
A; •.! t.irc rp.ir :,or;iii»tion centers, however, tailings have
bet.-" in roa f •..-•-v.itrue*.ion and qerieral land-fill material
i is" vi •. ¦•!...» 'Hpr 'on' l':¦ tin records are
' i 11 * a ¦ nt-fi the ai>.;u':V of tailings removed for these purposes,
cr,:,. 7 r-i'i- tJtssif If-, ' or a mine near Tucson, Arizona, for
: , 'jppro/. i c n t.c' v i:if! thousand tons of tailings vere utilized for
c-'.-rr,fruction. A small but indeterminable amount of tailings from
C
r::ir-v.- rt< a 1 \c used foi land-fill? and construction material.
P I •, ft •!!. stated the suitability of tailings naterials
f
'(€ rro'lur :.i'in ->*• i'i:.st'-ited th»r hrv-Vs of superior quality were possible. A. barrier to
co^iercial i/ation. •v-«w<-ve»', was again, the distance between the source
material o>=d the -;«ark»t. If the price of construction materials continues
to el in,!; at the iresent rate, though, these bricks nay become competitive.
- 52 -
-------
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 in 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 aipna radiation.
In the University of Arizona's ufclication "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 .;se, Their plans called for
"satellite" communities tc he built on the terraced piles with agriculture
and commercial zo'ie ,. Although use of reclaimed copper mining sites is
very small at present, the proximity of cities such -v, fcutte, Montana,
Salt Lake City, Utah, arid 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 mined-out open pit areas and abandoned waste piles.
The potential exposure from uraniur. and its daughter products is
i\¦ n, d! rf i''sceriftin without measuring the levels of the waste
n.a*"ri.:!, Ihorr- i« ¦ ¦ pc*-•;ib111 f..y that hones built on, or adjacent to,
lo-mtr s.-tt: >i-3 pond-: wo^ri »>x3eri*-nce even greater radiation exposure
du«> to higher residual uioniui:: cenantratiens from the dewatered slimes
and tailing'*.
- 53 -
-------
It is evident that elevated radioactivity levWs^have 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 associate*4
with copper tailings, sulfuric acid produced with rainwater can gradually
leach out uranium and its daughter products from storage piles. These
effluents should meet Federal and State discharge standards where applicable
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 diffusion into closed struct'/res.
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
- 54 -
-------
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 obvious 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 cranium concentration of waste materials can be increased,
including dewatering, leaching, and precipitation. Frc-n 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 likely that a large fraction of the uranium is ultimately ;ii scharged
with the tailings. A need exists for a radiological impact assessment
of this and other mining and milling effluents. This analysis should
include prircary ore, waste rock, beneficiat:on solutions, ta')i.'i';s, r.-nci
all effurnt streams.
Ther-.; is s growing consideration given to the utilization tm-M:
waste i.icterials U.r construction <;v.1 landfill purposes which co-;j".d
to an ir-creased public exposure. With the i»!ircnsy amour*, of wast'..-
materials Vj'ir<, -trier.-!cert, the likel ibood of rec!ar:at- .»n err. ;t : '1 ,\<: -<¦
is becou-W'i; greater. As the nost significant notemial expcsu," p.v~i.-.i-
is the construe::ion of homos on uraniferous reclaimed land, fir „-.if.terr
- 55 -
-------
of population growth is critical. At the present time, the lack of
development in the immediate 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.
Occupationally 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 zirconium extraction process, zircon ore (sand) is dressed with
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 1s Introduced into a chlorination reaction
chamber, the temperature elevated to 12Q0"C, and chlorine gas is reacted
with the mixture. The primary reaction i«.;
ZrC,.S10„+ 2C + 4C1 7 H S i' ~ :CC9
' ' * "1BT '
A two-stage condenser {01Ci4) separates crudf 5-f4. frcr "-CI4
wh'ch is processed for sale.
The process now proceeds to the Zr-Hf separation. This is a solvent
extraction process using methyl 1sorvjtyiketone and an aqueous solution of
- 56 -
-------
ammonium thlocyanate. The Hf 1s carried Into the MIBK fraction and the
completeness of this separation 1s measured by act1v1at1ng the natural Hf-180
to radioactive Hf-181 using Cf-252 sources. The Zr 1s carried Into the
aqueous phase as zirconium oxychlorlde (ZrOCl2) and 1s precipitated as the
sulfate with the NH4CI being further processed to recover NH4OH, The
Zr ($04)2 1s repulped with aqua ammonia (NH4OH) to form Zr(0H)^and ammonium
sulfate which 1s boiled down and can be used as fertilizer. The zirconium
hydroxide (Zr(OH)^) is filtered and sent to the calclner where it 1s fired
to the oxide (ZrC^).
The zirconium oxide 1s then remixed with the coke and sent t..rough a
pure chlorlnator to yield ZrCl4 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 ZrCl4 to produce magnesium
chloride (MgCl2) and zirconium sponge (metal). A flow chart Illustration
is presented in Figure 6.
The first residue generated by this process 1s the sand chlorlnator
residue (tailings). This residue 1s 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 chlorlnator residue ends up 1n a pile as indicated in Figure 6. There
are also drains and general waste from this process that are sent to pond 1A,
which 1s a holding pond for the clarifier. There 1s a turnover in the caustic
alkali scrubbers used here that is partially recovered and partially sent
to the clarlfier.
The sludge coming from the clarifier comprises the largest volume of
waste generated in the zirconium extraction process. Rad1um-226 concentra-
tions in sludge have been measured between 87 and 154 pCi/g(dry).
- 57 -
-------
en
00
FTEP MAKE-UP
KILTER CAKE
Monaz i'.c
ro NF.ro
nu.^t r
Unreaoted Sand
r res
ilORINATOR
RESIDUE PILE
)1 Residue.
j_ Floor Grains*.
Volatile*
Che ; M
How Dc
NaOH or.H.SO,
SiCl
10 Separations
To Market
Siipernatc
Underflow
CO
¦Reparations
Sump
(CooZing Hater
SLUDGE POND
HOLDING POST; IB
pH Control
HOLDING POND 2
HOLDING POND 1A
CLARIFIER
SEPARATIONS
Zr(Hf )CK from CHLORINATOR
ZrOC 1 2 ~ SO;,
CaOH
NHuCl 'to
Anmonia .Recovery-
Zr(SOiT) NHuOil
So Recycle
(NH,,) 7 SOi, Fart i 11 zer.
Scrubbers
r
ZrO, ~ Coke
Liquid
Fertilizer
FIGURE 6
'rains 6. Scrubbers
SOLVENT
EXTRACTION
V2 FILTER
MAGNESIUM
: :r'Ction furnace
VS-V4 FILTER
CALCINER
V2 POND
.1 TANK
PURE Zr02
CHLORINATOR
- Residue
Scrubbers
ZrCl
Zr Sponge ~¦To Mill ZIRCONIUM EXTRACTION
PROCESS
Liquid Effluent to Truax Creek
-------
In the sulfate precipitation (V2) ammonium chloride is generated and
1s sent to a recovery site to recover ammonia. The ammonium chloride is
operated by the neutralization of HC1 with NRH OH (ammonia).
The Zr($04)2 repu^ped with ammonium hydroxide to form Zr(0H)4. This
process yields ammonium sulfate ((^4)2504) which is further processed tc
liquid fertilizer.
There are scrubbers associated with the final three (3) steps: the
calciner, the pure chlorinator, and the Kroll process magnesiur, 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.-226.
The most significant radiological problem presented by the zirconium
extraction process appears to be the potential co-^tamina t-'or of surface cr
ground water from the chlorinator residues. !t has seen demonstrated that
the radium in these residues is extremely soluble. Radiuir-226 concentration
in water under a chlorinator residue pile has been measured to be as nigh
as 45,000 pCi/I.
- 59 -
-------
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. Moxham, R. M,, Foote, R.S., and C. M. Bunker, "Gamma-ray Spectrometer
Studies of Hydrotherma1ly Altered Rock," Economic Geology, 60(4)
(June-July 1965).
3. Davis, J,D. and J. M. Guilbert, "Distribution of the ftadioelemer.ts
Potassium, Uranium, and Thorium in Selected Porphyry Cooper Deposits,"
Economic Geology, 68(2) (March-April 1973).
4. "Radioactivity Analyses Performed on Water Samples from the Ore
Mining and Dressing Industry," Cal span, Inc., Buffalo, f.'Y. 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, 1975).
6. Rabb, D., University of Arizona, College of Mines, private
communication (August 7, 1975).
7. Pigott, P.G., 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 Balanced Approach to Resource Extraction and Creative Land
Development," University of Arizona, College of Architecture and
College of Mines (joint, project) (1974).
- 6C -
-------
RADON m CAVES
It has recently come 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 fiinir.g Enforcement and Safety Administration. A parti-
cular concern is during the summer months when 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 nur.ber of State and privately owned caves and "cave
air" conditioned buildings, it will be stro.igly 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-Rem dose per year, may result from the approximately one million
persons visiting caves operated by the U. S. National Park Service each
year. At the request of the National Park Service EPA made interim
recommendations on exposure limits for persons employed in the Carlsbad
Caverns. On June 3, 1976, EPA recommended a 4 WLM annual limit for
workers in these caverns as an interim >^commendation and requested
public comment on the general applicability o* these recommendations
to other caves and caverns ooen to the public (^1 F.R. 22409).
EPA further recommended that measures be implemented to keep exposures
below the 4 WLM annual limit where feasible. Mo limit was set for visitors
to the caverns. EPA also stated that the individual exposure limit
- 61 -
-------
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, 1t might be advisable to rotate long terr> employees working
1n elevated radon areas J
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 1n 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 recommendations 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.
- G2 -
-------
REFERENCES
1. Radiological Quality of the Envlronwent, U.S. EPA, ORP,
EPA-52/f-76-010, 1976
- 63 -
-------
STANDARDS AND GUIDELINES FOR RADIOACTIVE MATERIAL
IN CONSUMER AND CONSTRUCTION PRODUCTS
The NPO and some of the Stales currently have regulations control 1 inq
the use of uranium mil] tailings for construction nd other purposes.
The 11->n iwrediat.el y arises as to the need for similar controls on
other itria; product" or byproducts that contain radioacri vity, such
as s idti, gyp vjt'i, and other materials from phosphdte plants, or failings
froin otter ty;:,.-- of mining and milling operations. Idaho h.v, pro:.c:>ed a
re'.;.! a t;on prv.hib'- ting the use of slag under or within haM t.at.i" tryctu*-es,
hut t.'i'::' regulation authorises the iise cf slag outdoors, for
: vy, \ rue lion, railroad ballast, etc. (This regulation aj-pear-, as
.';ttachi.,^!i:. <¦ in thh report.) Controls on the use of et.h{r r ci-io> r.ti. e
materia I •, .; 111 he difficult in the future without, standards and -ij Mr--
linos ft.. radioactivity concentrations. For example, what ujncmtrjt.ion
<-f r fici (•<-. ¦?,.:( 'ri s' acj is acceptable for the use of s 1 6 standards and guidelines for the use, distribution, and disposal
t.: :-.-i.,';;*riu' products and byproducts containing natural l,y-occurring
r.-dioacV! ve witerial s.
- 64 -
-------
RADIOACTIVITY IN CONSTRUCTION MATERIALS
It is estimated that the average person in the United States spends
95'- of his time indoors. Over 78' of this time is spent in the home.'
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 dese
equivalent from radionuclides in building materials) is greater than
that from any other source.
Radionuclide Content ef Building Materials
The literature review by Eadie notes the paucity of significant
published data relating to radionuclide concentrations in specific
? ~
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
oy the EPA: Moeller, O.W. and Underbill, D.W., 'Tina' Report on the Study
of the Effects of Building Materials or Population Dcc;e fqui valents ,
Harvard School of Public Health, December, 1976.
- 65 -
-------
that la roe 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
.ire observed in materials such as granite, pumice stone, and clay brick
and in some byproducts of industrial processes such as artifical gypsum
.t'c; concrete composed of coal-fired power station fly ash.
The most comprehensive studies published to date dealing with the
natural radioactive content of building materials are those of Krisiuk,
el ul., using gamma spectrometic analysis, determined the radium-226,
f.horium-23? and potassium-30 concentrations of over 300 samples of
3
building materials from many regions of the U.S.S.R. Materials of
volcanic origin including granite, tuff, and facing materials composed
of tinguaite arid endialite, as well as materials manufactured from
industti«i! 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
-,on»:ent. Radionuclide concentrations in some of these materials are
presented in the Table, along with estimates of the air-absorbed dose
rates the materials 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
arte construction ^aLerial made from byproducts of the phosphate mining
4 S
arid mi!liny industry in Florida. The radionuclides of primary concern
!• of th.-;se cases are uranium and its daughter products. Another
- 66 -
-------
radionuclide of probable importance in the U.S. is p^f as-; -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 sh4e?d from
external radiation exposure. The source characteristics result from
naturally-occurring radionuclides in the building mater-jls themselves,
and ir,< shielding characteristics are determined by tr- to which
natural terrestrial and cosmic radiation sources ere bt*--_-mated by these
•materials. In general. wood frame buildings have low qualities
j',J :,(i; relatively poor shie'ids fo~ terrest.ri«i and cosmic • >:*ir!tion.
Masonry buildings are offer- sijoif scant sourer-,; rut provide nood shi"iding
fur .-"Testrii:! • ut i •-«.
Hadon and radon daugnt.e,- concentration:, inside bui idings have been
pleasured by several investigat'uns. Yeates, et al., ••*.;?>»$-J red ruden
daughter r -.ncentrations in several frfv;,e dwelling:; <-.nd rulti-story
nasonry buildings in the Boston, Massachusetts, area.' Sr. single family
franco dwellings, radon daughter concentrations v.-ere of the sare order
tor outside and first floor measurement?. Casement concentrations were
from 4 to 2s times higher than first floor concentrations. Daughter
concentrations in masonry office buildings tended to be slightly higher
than first-floor concentrations in residences, but the concentrations in
- 67 -
-------
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 o/erall 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. Tp a poorly ventilated basement laboratory,
Parthaserathy found the background concentration of polonium-218 to
O
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 rates
to the lungs may be even higher,and it would appear that control measures
should be considered. Such measures include (1) material substitution,
(2) improved manufacturing standards, (3) changes in basic building
designs, (4) 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 power plants by the U.S. Nuclear Regulatory Commission
of $1000 per person-Rem.
- 68 -
-------
RAmoAcrm onmxr ok u'iuhnc materiaus*
Ty|*- of building nnterial
liriife, clinker
Clay bricks
bricks
Bricks
Heavy concrete
Light concrete
Concrete
Concrete without alum sha ie
Concrete containing alur: sliali
Cement
Cftiitnl
. C>nent
L>i;u'..-;lone and s;uid
Natural sand :uid sand rojei.'l.s
'Natural plaster
I Natural plaster
| Plaster
' ONimcul plaster
OirmiojiJ piaster
Gi':ini to
' Hninite bricks
Tuff
Pumice store.'
i S'an pimice
Rock uiapepilo
Lime
Phosphorus -1 :i^'s
: Facing mil• naIs
(V.iuitrv
Kul. Pit. of (jemany
I. ti11< ti Kiniztiri
iv iet t'nion
Sweden
j \vera^re activity concentration
Nuaher of (jtCI )
san?)les
2:s
55
109
Soviet Union
Soviet !.'nion
l-ni i.ixl Kintxkxi
Sttixlen
Sweden
Fed. Rep. of Ciormany
Swixii 'ii
Siviet Union
Fed. Hep. of Oonnany
Soviet l.'nion
I'nit.iii KinKtlrm
Fed. Rop. of (lemony
Soviet t'nion
Fed. Rep. ol Ciemur.
Un1ti.il KinKd'-m
K7
29
10
..J...
Seviot Lnton
I'nilod Kintfriom
Sovirt Union
F<-d. Hfi>- Cuntuny
Srvii-i t'nion
CniU-d Kinfidiin
Swrxit'n
Sovirt I'n it >n
Soviet I'n ion
69
1
1
ir»
•it*
17
:-:o
15
it
11
t
6
<»
7.1
- —
Air dosr
rat*
4
2.1
10
"1-
i
•10
2K
IK
21
1.'.
22
i
an
•Ueninson, i't u 1. , 1975
**The absorlxii dose rates
i
...1.
1 .1
1.2
o. 17
0.5
0.5
L\'>
I(>
in
12
15
15
II
50
70
1.5
16
2.:i
28
:'.o
2-1
. n
2*'.
i .5
21
0. 1
12
2
o ! ¦;
¦ *
21
2.:i
HO
in air' liave Ux'ti
cub
siriiIV :> 1 ::''«»;ry and an Infinite thickness
-------
Radioactive Phosphate Slag in Outdoor Construction
Phosphate slag, a calcium fluorosilicate byproduct of the thermal
phosphate industry, has been commonly 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.
R?dioassay of phosphate slag shows « radium-226 content of 35 pCi/gram.
This nay 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 slag was 15 to 40 wR/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 gamma 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.
- 70 -
-------
The problems Indicate a thorough evaluation of the environmental
consequences of continuing to use phosphate slag in outdoor construction
is warranted.
- 71 -
-------
REFERENCES
1. Oakley, D.T., "Natural Radiation Exposure in the United States,"
U.S. Environmental Protection Agency, Washington, O.C., Report
ORP/SI072-1, 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
?R01EC00153 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/CSD-73-3 (August, 197b).
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, HASL TM-71-8 (1971),
7. Yeates, O.B., Goldin, A.S., and Moeller, D.W., "Natural Radiation
in the Urban Environment," Nuclear Safety, Vol. 13, No. 4,
pages 275-286 (July-August, 1972).
8. Auxier, J.A., "Respiratory Exposure in Buildings Due to Radon
Progeny Health Physics", Vol. 31, pages 187-188, (1976).
- 72 -
-------
RELATED EPA-TASK FORCE ACiiVmbS
The United States Environmental Protect?on Are.-ry •'? pr-scRtly
conducting several programs to determine the n«ed fur .-vriidtKm pro-
tection standards, guidelines, and criteria with resucct to exposures
from naturally-occurring radionuclides. The following problem areas
have been identified for initial efforts because of the it f,y!<1U heal ;.h
importance:
1' The development of rcn.onimi-r;riiJ-ions tc the State o: F'cicu *•••
the control of radiation exposures associated with pr.ospnate
materials. These recommendations will exclude accrot^r-le
indoor radiation level uuide1ines and enter'"* for t c.,1 u::r; <
-------
materials, the Agency is assessing the need to develop national
guidelines for acceptable radiation concentrations in con-
struction materials used in stnir.tures.
4} These same construction materials are frequently used for road
pavoiwnt, r^-lrujd ballast, backfill, and other applications.
While the public health significance of these uses are probably
not as great as when used in structures, it is not clear that
such prar.f.'<•.
-------
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.
. 75 -
-------
STATUTORY AUTHORITY OF STATES TO REGULATE
NATURALLY-OCCURRING RADIOACTIVIE 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 riot be simply limited tc
"uranium »nll 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
rVi belie' in some States that Agreement State radiation control agencies
have authority only over byproduct or agreement material, and not over
:i.-; tu r'o 11 y -ofTurri no radioactive materials. Consequently, there may be a
need for additional statutory authority to control naturally-occurring
nidi oat*i ve 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
radio-active materials in the uranium decay series. The mining, bene-
fit iating, processing, and crushing operations could be licensed to
possess, use, and store this radioactive material. Specific licensing
could provide for:
- 76 -
-------
(1) Restricted use of industrial byproducts such as slag.
(2) Long-term ontrol of slag and 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 these 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 to phosphate
industries are given in Attachment B of this report. Attachment C is
a licensing guide for a phosphate industry application far a radioactive
material license.
Other industries with significant radiological aspects such as
zirconium recovery plants and rare earth mills and processing plants
should also be 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 to transfer all
radioactive tailings containing thorium to the waste disposal site near
Hanford, Washington.
- 77 -
-------
RECOMMENDATIONS
A. Pending the er.tabl ishment of appropriate standards, the us;- „•
phosphate mining and milling byproducts in occupied structures
should be discouraged if they contain elevated levels of rniiiur-?.?^
EPA should place high priority on evaluating ~his application cf
these byproducts and balancing this against the envirender'm!
problems associated with waste storage of the- material-..
B. Phosphate byproducts, particular gypsum, .-ire present!-• used ?<.. «
limited extent as an agricultural soil conditioner, AUhc.-nh
little is specifically known regarding the ervi roriii.en4 rr o;
this use. and considering the uital 1 addition of radioJCt ivi-y t,o
the environment, it is unlovely that th is application wou!" >•*••>» t L
in significant radioactivity uptake in crops, it is no? r?r.o'.;\.»ci.-i
that this use of the byproduct materials be discouraged at this
time. Additional controlled studies should be porferred to dscunen '
the anticipated minimal environmental impact of this use
C. Slag from thermal process phosphorus acid plants should not he used
for any purpose that results in its being under or within an enclosed
structure. Any other use of slag should be thoroughly evaluated.
D. 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.
- 78 -
-------
The States should perform additional radiological air monitoring
inside and outside phosphate plant areas.
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 #/ with any pertinent recommendations.
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.
EPA should study the uptake of naturally-occurring radionuclides in
food crops from irrigation water, fertilizer, and radiation-bearing
soi 1.
EPA should study the whole body and organ doses resulting from
ingestion of radon daughters in drinking water.
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.
EPA should develop national criteria and guidelines concerning the
use and distribution of industrial byproducts containing naturally-
otcun-ir.-i radioactive material. The EPA should consider seeking
appropriate authority to promulgate such guidelines as national
standards.
-------
L, [PA and appropriate States should study and evaluate all uses of
fly-ash from coal-fired plants, particularly related to construction
materials.
M. The radiological aspects of each proposed coal-fired plant should
be evaluated by the appropriate agencies. Radioactive releases
should be estimated frou 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 and guidelines for
sample collection and analysis of naturally-occurring radioactive
material to ensure the acquisition of uniform and roinparable data
by State and Federal programs. The EPA should expand their cross-
check quality assurance program in conjunction with the standard
analytical procedures and to include NORM.
0. The States, the EPA, or other appropriate agencies should proceed
to measure radon levels on fly a^h piles and in structures built in
fly asn disposal areas, if such case exists.
P. It is recommended that representatives of this Task Force, KPA,
NIOSH, and MESA meet t.o discuss the preliminary investigations and
measurements of radon-2.?.? in caves and determine what ether studies
should be undertaken to properly evaluate this situation. Adclitiona:ly,
the interim recommendations 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.
- 30 -
-------
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 urcontrolled 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 f1 iding by EPA or other appropriate
agencies.
S. Phosphate industries and all other industries having significant
radiological impacts should be licensed in order to assure adequate
controls over naturally-occurring radioactive materials.
- 81 -
-------
ATTACHMENT A
Explanation 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
radium and may diffuse into the structures causing internal radiation
exposures to 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" taiTingV inVter'ial 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 the 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 (b) to prohibit the use of slag where a hazard
has been established, i.e., under or within habitable structures.
- 82 -
-------
Shc. 1.2 Maintenance of Piles and Ponds at All Mills.
(f) Except as provided in Cec. 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 licensabie 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:
NOTICE - SLAG FROM THERMAL PROCESS PHOSPHATE PLANTS
CONTAINS TRACE QUANTITIES OF RADIUM, A RADIOACTIVE
MATERIAL. SLAG IS MOT SUITABLE FOR USE UNDER OR
WITHIN HABITABLE STRUCTURES. THE I0AH0 RADIATION
CONTROL REGULATIONS PROHIBIT THE USE OF SLAG AS
FILL OR AS AGGREGATE IN CONCRETE THAT WILL BE UNDER
OR WITHIN HABITABLE STRUCTURES.
(2) Slag conta<"4ng licensable concentrations of naturally-occurring
ra
-------
(in} To" parking lots, driveways, sidewalks, bridges, or
other outdoor structures, as aggregate in asphalt or
concrete.
(iv) For stock yards as fill or as stabilization material.
(v) For other purposes specifically authorized in writing by
the Radiation Control Agency.
It shall be specifically prohibited to use slag containing licensable
concent rations of naturally-occurring radioactive material for the
following purposes:
(I.) As aggregate in concrete? or other material that will be under
or within habitable structures.
(?) For any purpose that will result or ?s likely to result in slag
being under, incorporated into, or within habitable structures,
i o>" any other ennest except a"t.hcr"; reel in ^ec. 1.5(a)'.2).
Persons who transfer, receive cr acquire slag from thermal process
phosphate plants pursuant to the general license contained in Section
1.5(a) shall be exempt from the requirements of Part C of these
regulations.
Definitions. As used in this part:
"Hobitc1"1 e structure" frear.s any dwell ing, reuse, garags, building
or other enclosed structure that is 'likely to be occupied by an
ind i vidual .
"Licensable concentrations of nature 11 y-occurring radioactive material"
means concentrations of the uranium or thorium series radioisotopes
greater than those concentrations listed in Part B> Schedule A, Exempt
fc-ncentra tions , of these regulations.
- °A -
-------
"Mill" means any ore processing plant, a thermal or wet phosphate
processing plant, or any other processing or manufacturing plant.
"Slag" means that tailings material of the thermal process phosphate
plants.
"Tailings material" means any residue separated in the preparation
of various products.
- 35 -
-------
ATTACHMENT B
Elemental Phosphorus Plant
ICCK NUMftCA
~
o*»«
proleui AmeAdmentt
Ar« Vd4
~ AppKcoilon ~ l*"" ~ teleflrort* Q_
iiOHto art
MAOlO'fOTOM 1 ]hUi«W« *Q»«*•»»•]" IliUO lOUKCI IOl*T«H«AtlOM jsTO*«6f <
, | ,v.tii I e* ew<*>tiir I— — f"
ho)o- »»»¦««•[ -t» >Q>»C» jcnt«.CAL »TAT«|
CONT4(*C* OH f l^OtVd OVVICi
IT
AUTHORtrCO use
Naturally occur-
ring radioactive
materials in the
uranium and
choriun series.
Naturally occur-
ring radioactive
materials in the
uraniun and
thorium series.
As necessary for
mining, process-
ing, and recovery
of elemental
phosphorus.
As necessary for
mining, process-
ing, and recovery
of elemental
phosphorus.
Phosphorus bearing
shale or ore containing
licensable concentra-
tions of radioactive
ti' trials.
Industrial by-products
containing licensable
concentrations of radio-
active materials.
Phosphorus bearing shale or
ore containing licensable
concentrations of radioactive
material may be mined,
beneficiated, and processed
for the purpose of extracting
elementeci phosphorus.
Unless otherwise provided by
the Conditions of this license,
industrial by-products containing
licensable concentrations of
radioactive materials shall be
for storage only.
1. All industrial by-products containing licensable concentrations of radioactive materials
shall be stored at the licensee's phosphate plant near .
2. Radioactive furnace slag may be transferred to slag crushing operations which hold
a specific license issued by the State of or another State which authorizes
the receipt and use of such material. Crushed Slag shall be used only for (specify
uses).
3. The licensee shall maintain records of all furnace slag transfers which indicate the
amount of slag transferred to each slag crushing operation. Records shall be made
available for inspection by the Radiation Control Agency.
FEP may be transferred or used by the licensee and is exarpt frcm the provisions of
this license and the Radiation Cbntrol Regulations.
- 86 -
-------
O LifCMtl I
J^CHOH 1 w*J.«u»T 1 imilBHfrKI ¦«>'.. {»'}» | $'0«*Gt £M*H* |
I "A^&Wci I '0** *"VE«I i'«»t | "
The licensee shall aonply with the provisions of Part of the
Radiation Control Regulations, as they apply to furnace slag piles and other industrial
by-product piles containing licensable concentrations of radioactive materials.
6, The license shall comply with statements, representations and procedures contained
in his application dated ; and signed by .
- 87 -
•yC i-Mk'OCuot; Cl-CuM*
-------
RADIOACTIVE
MATERIAL LICENSE
Wot Process Plant
N ft C NUHIO
¦ ¦DHIHI liwHtta
~
Prc*«out
Ar« Vcii
llfl IICINK ItlWIO fV«tu'XT tO «**0 >
• mi t
|J Appficot'on * "f*r J J TeJf Q'om O
AICNIO •*.
««oio-»oro»t ] M»HOiOWU .im.tlf.CM.ON j»
,«tN J„.ft, MOJO'VonT-C.#^ jcHIM.CAt #0««
»tO**«C COM
i>m« o« Ii'mum oivcij
AUlMOAtKO use
Naturally (x:cur-
ring radioactive
materials in the
uranium and
thoriim serifK.
Naturally occur-
ring radioactive
materials in the
uranilm and
thoriun series.
As necessary for
mining, process-
ing, and pro-
duction of
phosphoric sic id
and fertilizer.
As necessary lor
mining, process-
ing, and pro-
duction of
phosphoric acid
and fertilizer.
Phosphx is bearing
shale or ore containing
licensable concentra-
tions of radioactive
materials.
Industrial by-products
containing licensable
ooncentratioas of radio-
active iraterials.
Phosphorus bearing shale or
ore containing licensable
concentrations of radioactive
rraterials ray be mined,
beneficiated, and processed
for the purpotx of producing
phosphoric aeid and fertilizer.
Unless otherwise provided by
the Conditions of this license,
industrial by-products containing
licensable concentrations of
radioactive materials shall be
for storage only.
1. Al l indu.str.iaJ by-producis <.x>nlainini; 1 wionsMbl.t- o' ncenirations ratikuctn-e UMTials
shall be stored at the ! ierr..-:i < 'cfKmicaJ plant. m•::r _
2. The iincrpt rat ii •;!' i ;<) !¦ u« .1 ¦. 'tti provisions
this iicen.-vO and Die Radiation Control Rtigulationx.
•I. Hie lieensi*' shalj cxifyly with statements, representations and procedures contair.cd
in his application dated :ind sif^ned by .
53 -
'lOu'tio'*l*
-------
RADIOACTIVE
matkwal ucknsg
Slag Crushing Ccnpany
O
N4« HUHII*
• TllitflOn OATg
(>wi Am<
Af« VoU
THIS licthtt lltuto FW»»U»Nl tO
«*>e in t(co*e»Nct w.itn
~ Appticolloo ~ Idler ~ tflfO'om (J
ttCHia avi
HkOlOlftOTO'C
luxlNT
1tt „ m 1hs*rT*f IOU*
-------
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 _beJJsed. 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 rnj all
applicable radiation regulations.
6. (a) Radioactive Material. i;p-: : !fy rwtural ly-otcurring radioactive
material in the uranium and thorium decay series.
(b) ChrjnicaJ and/or Physical rorm and Maximuni^Quantity of_Each Chemical
and/or Physical Form That_You Will Posess at Any One Time. For the
forni of material specify: (V) phosphorus bearing shale or ore con-
taining licensable concentrations of radioactive material and/or (2)
industrial byproducts containing licensable concentrations of radio-
active orial inclining -Jag, gypsum, fluid dust material, etc. (make
coripiete; and/or (3) imustrial products containing licensable
coru;«nt ration of rad'iraor.ive material including phosphoric acid,
Tet'ili/tr e 1 f.-:;ionv.-.i phosphorus, FFP, etc. (make list complete).
B-v! ct*'. - {a< rhorne or liquid effluents) should not be
: 'i I
For ;naxi"!i:. ;; . i ty sinply specify: (i ) As necessary fc-r jriininn,
prncessin.-., . .-.c wanufacture of elemental phosphorus, phosphoric
afio, fertiliser, etc. ancJ/or (2) As necessary for the commercial
< by U.1S I .
7. Descr iK- •'•iqif.'Sf For Which Radio.ir.tive M-ite^ial Will : ; fy .V
uses of ore, products, arid industrial byproducts containing licensable
concentrations of radioactive material that you want to be authorized for,
including but not limited to such things as: (1) mining, (2) beneficiatina,
- 90 -
-------
(3) processing, (4) transfer to slag crushing operations, (5) transfer to
vanadium extraction companies, (6) 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 understand
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 with license conditions and applicable 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-assay Procedures Used. The requirements
Tor personnel monitoring are specified in "Section "of the
Radiation Control Regulations. (See also, Section __)
13. Facilities and Equipment. Self e nlanatory.
14. Radiation Protection Program. See Sections C.l, C.101. C.102, C.103,
C.104, C.105, C.106, C.201, C.205 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.
- 91 -
-------
ATTACHMENT D
PART _
RADIATION SAFETY REQUIREMENTS FOR RADIOACTIVE
MINERAL TAILINGS AND INDUSTRIAL BY-PRODUCT PILES
See. 1 SCOPK. The regulations 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
—7 1
1x10 microcurie per gram . As used in this part "tiy-product" means any
material produced, other than the primary product, in an industrial process.
Tim provisions of this part are in addition to, and not in substitution for,
other appiicable; provisions of: (a) these regulations and (b) any specific
1 icense issued pursuant to See. C.30 of Part C of tiie.se regulations.
Sec. _.2 SPECIFIC RMXJIRfcMENTS FOR TAILINGS, PI1J2S AND PONDS. Unless specifi-
cally provided otherwise by the Division, the following requirements for tailing,
pile anil pond areas shall be fulfilled:
(a) Access to such areas shall be controlled and posted as specified by the
Di vi sion.
Cb) These areas shall be maintained in such a manner that excessive erosion
of, or environmental hazards from, i*;:<
(I) Pile edges adjacent to a river, t*iyou, creek or "-.iier
shall be stabil izwl to prevent erosion.
'iCi/rr.l (or 1 Ujuids
- 92 -
-------
(2) Drainage ditches sufficient to prevent, erosion from surface runotl
water shall be provided.
(c) Prior written approval of the Division shall be obtained betore the
surface area of the land shall be put to aso.
(d) With the exception of reprocessing at the site, approval by the Division
must be obtained prior to removal of any materia] fnn these areas.
Sec. .3 SALE OR TRANSFER OF HIE SITK. The Division shall be given written
notice thirty (30) days in advance of any contemplated transfer of right, title
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. A ABANDONMENT OF THE SITE. Prior to abandonment of the sire, the
requirements of this section shall be fulfilled.
(h) Piles shall be stabilized against, wind and water eros-iev ;mc! contoured in
a manner which wi.ll prevent col lection of water.
(b) In addition to the above requirements, any material which h-is
removed irorn the pile by natural forces shall be returned to rr.n pile.
(c) Ponds shall be1 drained and tx>v«red with materials that, prevent blowing of
dust. Water drained l™m the? ponds shall be disposed of in a manner
approved by the Division.
(d) Detailed plans for onrpl iancc with parcgrapiu-i .1(a) (b) 'md (c) shall
;>e snunit ted to the Division, ior review and approval.
Sec. _.5 WAIVER. Upon application to the Division, certain roqiiiranents of
this part may be waived or modified if it can be sliown that the renuirenents are
unnecessary- or impractical in specific cases.
- 93 -
-------
ATTACHMENT E
INTRODUCTION
The occurrence of environmentally concentrations of milium iso-
topes in oil field production waters (also called oil field brines, pro-
duced k.'.iti r, produced i.jstc-w.rter, or format ion water) is Ve 1 ] \io7u^u iitod
(Kuroda, If 53; Gott and Mill, 1DS3; Ar nib rust and Kuroda, l«)So). Arabrust
and Kuroda (1950) reported Ra-224, Ra-226, and Rn-228 in product i ..m i-.atcrs
from oil fields in O'r.lahona and Arkansas, with activities ranging from
100- I i 00 pCi/1 Ra-22-1, I - 1600 pCi/1 Ra-226, and up to .100 pCi/l Ku-^rS.
They also found 8 pCi/1 Th-228 and 0.5 pCi/1 Th-227 in cue well sample.
Cott ;:';d lii'.l ( !P53) .'.ported <.nv.» rowaenta 1 ly high concent rat ions ot' ra-
dium in precipitates collectvd fro:a the bottom of oi!-water separators,
and from ditches and ponds used for disposal of the product ion water.
The Mississippi, Louisiana, and Texas Gulf Coasts cither arc, or have
the potential to bcco;nc major oi 1 -prcduc i ng areas of the: United States.
Texas and Louisiana have numerous producinguc]Is both on and offshore.
During the period Noveir.ber 1972 to October 19/3, approximately 1.7 x 10la
liters of production water were discharged to tiie Gulf of Mexico from
operations on Federal Outer Continental Shelf (OCS) leases outside the
three-mile limit (data furnished by U. S. Geological Survey, l'_>74). Rec-
ords of discharges inside the three-mile limit and on-shore are 'M intainod
by the staie.s in which the discharges occurred. Data provided by the De-
partment of Censcrvat ion, ^tatc of Louisiana, show that for the year IP'S
a state total of 8.1 x 10!c liters of formation water3 were discharged into
the surface envi ronscnt, 17.5° off-shore (presumably ins; do the th^c-e-ni !e
liniit), and S2.5% or 6.7 x 1013 liters on-shore. Of the latter, 6.0 x j01v
liters were discharged into non-pot able water bodies, .1.5 x 10* lit-rs were
discharged into streams and rivers, and 2.4 x 109 liters v.erc disposed oi'
in oj>en holding pits from which gradual loss occurs via evaporation aid
seepage into the under! yi ng ground. Similar data should be available i \>;;i
the State of Texas upon request. In 1974, several samples of forn.al i or.
waters from the. Gulf Coast production region were obtained and anai
for Ra-226. The results arc presented in Table 1.
The data in Table 1 show that environmentally high levels of Ra-226
arc conji'on in production waters from the Gulf Coast oil fields. for corc-
f.irative purposes, it is noted that average open ocean surface waters con-
tain about 0.05 pCi/liter; coastal waters probably do not generally get
much higher than about 1 pCi/liter, except in very restricted onvi roiur.cnt s:
drinking water standards restrict the porno ssi'i.lc Ka-L'.G ic;.t to '
than 5 j»Ci/I iter; and agreement - state and f-itC !v»i;!,i:iO!is it-; ¦
operations of licensees permit no more than 30 j.'Ci/! iter i:> 1 i;p: i!:-. v
to unrestricted access areas. According to Louisiana state o:T:.:jais, e-o-
duct ion waters do not "come under these regulations at the j > i-" s t ;: .< . !«jt
it is notable that they contain up to 400 pCi/liter, or 10 tines the per-
missible regulated inputs.
To our knowledge, there have been no scientific ste'ics of the ia;"i*
levels, speciation (in tons of dissolved vs. particulate foins) cr tiMate
disposition (fate) of such naturally occurring radium being discharged into
- 94 -
-------
local estuaririe environments (marshes, streams, rivers). The occurrence
of '.i.'.i ionmcnta 1 ly hif.h levels of radium in production waters does not
appear to be a widely known fact, as evidenced by conversations with both
state officials and oil company officials, although such discussions have
not been exhaustive.
THE LEEVILLE OIL FIELD
The Leeville Oil Field is a producing field covering about 62 km2 (24
mi2) in Lafourche Parish, Louisiana, centered near 29°14'N, D0°12'W (see
Fig. 1). This field was discovered in 1928, and is operated by Texaco, Inc.
By Texaco's estimates (in a letter to Dr. T. Whelan dated 10/13/76),
production is expected beyond the year 2000. The Leeville 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-
logic conditions: in the winter, the winds are from the north an-*, 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
"spring tide" or "flood tide" reverses the prevailirg condition, and sea
sonally deep water levels occur; and during, the summ' r, the hydrolcgic
conditions are most stable, with only small diurnal tides affecting the
medium water level by a few tens of centimeters., jno ih;> watr-; 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 10* liters was ~1.6% of the total on-shore discharge in the
State of Louisiana. In October 1976, brine samples from the discharges at
TB #4, in mid-field, and TB #8, in the northern, less built-up area of the
field, were sampled and analyzed for Ra-226 in our laboratory. The results
arc presented in Table 3, and indicate that both tank batteries are discharging
water with environmentally high concentrations of Ra-226.
Ba^ed on the data in Tables 2 and 3, in 1975, TB #4 dischargcu approximate-
ly C 2 Curies Ra-226, and TB #8 discharged approximitely 0.016 Curies Ra-?26
- 95 -
-------
into the l^cal salt marsh complex. If it is ,issu:,ied that the average pro-
duction water from the leevillc Oil Field contains about 280 pCi/1 Ra-226,
then over the five-year period of record, up to l,7f> Curies Ra-226 were
n Ided to the :11a r.-.h a round the field. At this time, wc have no data by
which to predict the ultimate fate of that radium. Ke also do not know if
any other isotopes fi'.im the uranium-thorium series .'sic present in environ-
mentally sigaificant concentrations in the production waters.
Ke are prepared to design and implement a program which will answer
some of those que.tiers. We anticipate that such a program would involve
collection and analyses of production water (brine) r;>,nplcs, marsh-water
samples, and various biological samples from the .tn.iy site. The number
of each type of sv.ipie will have to be determined by the environmental
ditions at the study site, but may be estimated as up to 75 each. The
resulting data will be compiled, interpreted, and discussed in a final re-
port, to be delivered v.ith up to six (6) copies to the sponsor approx inanely
16-20 isonths after project initiation. It is also exported that one or : '¦•re
professional papers to be published in reputable scientific journals will
result, ;;i.d Osose will acknowledge the sponsoring agency.
REFERENCES
Ai i?!»rt;sf , C. F. and P. K. Kuroda. On the Isotopic Constitution of Radium
fUa-224/Ra-2?A and Ra-228/Ra-226) in Petroleum Brines. Transactions,
Am. Ceophys. U., 37f 2), 216-220, 1956.
Hott, G. B. and J. W, Hill. Radioactivity in Some Oil Fields of South-
eastern Kansas. HSf,S Bull. 9SSE, pp. 69-122, 1953.
Kuroda, P. K. Radioactivity Tables of Some Natural Waters. U. of Arkansas,
Inst. Sei. Tech., 58 p., 19S3.
'•¦•'helan, T. , John T. Ishmael, and W. S. Bishop. Long-term Chemical Effects
of Petroleum ir. South Louisiana Wetlands - 1. Organic Carbon in Soiii-
n'.-iits and Waicrs. Mar. Pollut. Bull., 7(8), 150-155, 1976.
- 96 -
-------
TARI.F. 1
Ra-2?6 IN SF.I.IiCST.D SAMPIJ-S OF FORMATION KATfiRS !:ROM
THF. GULF COAST PRODUCTION RF.GION
IDENTIFICATION
ARCP, High Island Pl.it-
form B, ~ 12 miles offshore
Galveston, TX
TREATMENT
Rough filtered,
fil tr.ite acidi-
f i ed
REFRACTIVE
SALINITY
. ._Cep±)
121
Ra-2^6
(pCi/i).
313 * 4
F.XXON, Grand Isle Terminal,
Grand Isle, LA
No treatment
99
143 ~ 3
EXXCN, No location data
provided, shipped from
Lafayette, LA
No treatment
Acidified, but
not filtered
98
291 + 3
298 V 2
EXXON, Pelican Island
Term., Pc-lican Island, TX
No treatment
Filtered, Acid.
Unfiltered, Acid.
100
22 ~ 1
16 1 5
46 + 2
TEXACO, Bay de Chene,
Jefferson 5 Lafourche
Parishes, l,A
Unfiltered, Acid. 128
Filtered, Acid.
335 +_ 10
327 ~ 5
TEXACO, Garden Island Bay,
Plaquemines Parish, LA
Unfiltered, Acid. 110
Filtered, Acici.
397 +_ 8
393 + 6
TEXACO, No location,
originate Houma, LA
Unfiltered, Acid.
Filtered, Acid.
276 +_ 3
131 + 2
NOTE: Errors indicate precision (la) of replicate analyses; overall tech-
nique error is +7%.
- 97 -
-------
! 971
1972
1973
1974
1975
LEEV!Vi.F. SALT WATER DISUSED OF
IN NON-POTABLE WATER
TB «1
TB #4
T3 #5
TB *6
T3 «7
TP <:8
TB »9
TB ^10 TB #11
TB *12
TB Bge
TOTAL
4 , 64 x \ 0 7 7.71x10s 1.91xl08 5.80x10s 3.19x10® 1.51x10s
5.80x10' 3.48x10' 4.64x10' 5.80x10' 1.59x!0'
9
4.64x10' 7.71x10' 1.91x10® 5.80x10s 3.19x10® 1.51x!0® 5.90x10s S.SOxlO7 1.76x10' 4.64x10' S.80x10s 1.5.° '0
4.98x10' 4.64x10s 1.39x10*
3.53x10' 6.93x10® 1.63x10® 2.58x10' 3.19x10s 8.46xl07 1.47x10s 6.29xl07
4.38xl07 4.59x10s 4.59x10' 4.88x10' 1.11x10® 8.03x10' 2.86x10' 5.74xl07
5.47X107 5.89x10® 8.36x10' 2.04xl07 1.44x10® 6.46x10'
5.90x10'
8.61x10' 1. 1S>.10' 8.7qx!0'
1.08x10' 7.73x10' 1.03x10'
TABLE 3
I
Ra-226 IN BRINE FROM TB #4 AND TB #8, LEEVILLE OIL FIELD
CO
i
TB #4 No Treatment 327 _~ 20 pCi/1
Acidified 319 _» 9 pCi/1
Filtered and Acidified 318 5 pCi/1
TB #8 Acidified 260 8 pCi/1
Filtered and Acidified 248 » S pCi/1
-------
toxic*•*** 4*'*
f
W<&WW'. :K
x' Xv'/'y/--
yfc/7/A'/''//4
ivt« «c.
-------
EPA Technical Notes
ORP/CSD 76-1 A Statistical Analysis Of The Projected Performance Of
f'ult1-Un1t 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 Radlaoctive Wastes
ORP/CSD-77-4 Plutonium Inhalation Dose (PAID) A Code For Calculating Organ
Doses Due To The Inahlatlon And Ingestion Of Radlaoctive
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 75-8A Radioactivity Associated with Geothermal Waters 1n 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 The 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
Concentrations In Grand Junction, Colorado
ORP/TAD 76-1 Determination of Radium Remo»al Efficiencies 1n Iowa Water
Supply Treatment Processes
ORP/TAD 76-2 Determination of Radium Removal Efficiencies in Illinois
Vlattr 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 Determinalon Of Radium Removal Efficiency In Water
Treatment Processess
------- |