Ecological Research Series
AVAILABILITY, UPTAKE AND
TRANSLOCATION OF PLUTONIUM WITHIN
BIOLOGICAL SYSTEMS:
A Review of the Significant Literature
Environmental Monitoring and Support Laboratory
Office of Research and Development
U.S. Environmental Protection Agency
Las Vegas, Nevada 89114
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RESEARCH REPORTING SERIES
Research reports of the Office of Research and Development, U.S. Environmental
Protection Agency, have been grouped into five series. These five broad
categories were established to facilitate further development and application of
environmental technology. Elimination of traditional grouping was consciously
planned to foster technology transfer and a maximum interface in related fields.
The five series are:
1. Environmental Health Effects Research
2. Environmental Protection Technology
3. Ecological Research
4. Environmental Monitoring
5. Socioeconomic Environmental Studies
This report has been assigned to the ECOLOGICAL RESEARCH series. This series
describes research on the effects of pollution on humans, plant and animal
species, and materials. Problems are assessed for their long- and short-term
influences. Investigations include formation, transport, and pathway studies to
determine the fate of pollutants and their effects. This work provides the technical
basis for setting standards to minimize undesirable changes in living organisms
in the aquatic, terrestrial, and atmospheric environments.
This document is available to the public through the National Technical Informa-
tion Service, Springfield, Virginia 22161.
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EPA-600/3-76-043
April 1976
AVAILABILITY, UPTAKE AND TRANSLOCATION OF PLUTONIUM WITHIN
BIOLOGICAL SYSTEMS: A Review of the Significant Literature
by
Anita A. Mullen and Robert E. Mosley
Monitoring Systems Research and Development Division
Environmental Monitoring and Support Laboratory
Las Vegas, Nevada 89114
U.S. ENVIRONMENTAL PROTECTION AGENCY
OFFICE OF RESEARCH AND DEVELOPMENT
ENVIRONMENTAL MONITORING AND SUPPORT LABORATORY
LAS VEGAS, NEVADA 89114
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DISCLAIMER
This report has been reviewed by the Environmental Monitoring and Support
Laboratory-Las Vegas, U.S. Environmental Protection Agency, and approved for
publication. Mention of trade names or commercial products does not constitute
endorsement or recommendation for use.
NOTICE
Effective June 29, 1975, the National Environmental Research Center-Las
Vegas (NERC-LV) was designated the Environmental Monitoring and Support
Laboratory-Las Vegas (EMSL-LV). This Laboratory is one of three Environmental
Monitoring and Support Laboratories of the Office of Monitoring and Technical
Support in the U.S. Environmental Protection Agency's Office of Research and
Development.
Effective January 19, 1975, the U.S. Atomic Energy Commission (AEG) was
reorganized into two separate agencies, the Nuclear Regulatory Commission and
the U.S. Energy Research and Development Administration (ERDA).
ii
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ABSTRACT
This report is a selective review of the literature on the availability
of plutonium in the environment and its cycling throughout representative
biological systems ranging from large biomes covering hundreds of miles to
the molecular transformations within individual cells. No attempt was made
to develop a comprehensive bibliography. Rather, references were selected
for inclusion as representative documentation for the vast spectrum of
material that is available on the subject.
Important general references are listed separately. Thereafter the
literature is described in essay form on a subject basis. References
cited by number in the text are listed in complete bibliographic form at
the end of the report together with an author index. The majority of the
material reviewed is limited to relatively recent publications.
111
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CONTENTS
Page
Abstract 1:L1
Acknowledgments v^
Conclusions 1
Introduction *•
r\
Objective
Approach 3
Organization . 3
Bibliographies 3
Potential Sources of Plutonium 5
General 5
Weapons Development "
Weapons in Transport 8
Fuel Processing and Reprocessing 8
Fires 9
Waste Disposal from Plants 9
Shipment 10
Nuclear Reactors and Radioisotopic Generators 10
Transport of Plutonium from Sources to Biosphere 13
Introduction 13
Chemical and Physical States of Environmental Plutonium 14
Soil 14
Air 16
Water 17
Biological Aspects of the Physicochemical Complexities 20
of Plutonium
Mammals 21
Plants 24
IV
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Page
Biological Deposition and Effects 24
Deposition and Effects of Pu in Aquatic Environments 24
Deposition, Effects and Countermeasures of Pu in Soil, 27
Plant Environments
Soil 27
Plants 29
Absorption of Plutonium by Animals 31
Biological Behavior of Inhaled Plutonium in Animals 37
Bone Deposition 39
Biological Effects of Plutonium in Animals 40
Blood 41
Bone 41
Liver 42
Lung 43
Lymph 4 3
Other Effects 44
Countermeasures for Plutonium in Animals 45
Deposition of Plutonium in Man 46
Effects of Plutonium in Humans 49
Countermeasures for Humans Exposed to Plutonium 49
Contamination
Present Analytical Methods 49
General Methods 50
Autoradiography 52
Instrumental Analysis 52
Bioassay for Plutonium 53
In Vivo Measurement of Plutonium 54
Monitoring Instrumentation 55
References 57
Author Index 85
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ACKNOWLEDGMENTS
The computer search of the Nuclear Science Abstracts was provided by
the Nevada Applied Ecology Group, Oak Ridge National Laboratory. Special
thanks to all who aided in the search for material .from 1970 to 1975
inclusive.
Much information was derived from the extensive indexed bibliography
of plutonium documents prior to 1970 that was compiled by Dr. M. G. White,
formerly of EPA and now with ERDA, Nevada Applied Ecology Group, Nevada
Operations Office and R. 0. Houston of EPA, EMSL-LV, who helped research
and organize the documents, and D. Wickman, EPA, EMSL-LV, who ordered many
of the documents referenced.
Special appreciation is due to J. M. Burford, D. D. Wicker and the
many others who sorted and indexed the abstracts and documents.
The efficient typing and preparation of the manuscript by P. A. McGill
and S. F. Forshee are deeply appreciated.
Special thanks to Omer Mullen for assisting with the sorting, editing
and proofing of the material.
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CONCLUSIONS
This review has briefly covered many topics but has addressed only a
small portion of the articles published over the past 25 years.
As additional energy requirements increase the number of nuclear power
generators, processing and reprocessing plants throughout the world, the
potential increases for the distribution of plutonium within a variety of
biomes previously only touched by worldwide fallout. At this time it appears
that more is known of the interactions of plutonium within a desert ecosystem
than in any other system. The largest single group studying plutonium in the
environment is the Nevada Applied Ecology Group (NAEG) which is supported by
the Energy Research and Development Administration. Its main concern has
been the area of the Nevada Test Site and its immediate environs.
Additional studies are needed to determine the physicochemical inter-
actions of plutonium in areas receiving moderate to heavy rainfall, which
results in lush vegetation with its attendant litter and greater quantity
of decomposition products affecting soil chemistry and fertility. Tempera-
ture extremes causing seasonal variations in plant constituents, endemic
and transient wildlife populations, invertebrate community size and average
age of individuals within these ecosystems all must be taken into considera-
tion.
Differing soil types are known to affect the translocation and avail-
ability of plutonium. What is not clearly defined is the effect of adding
amendments to the soil in order to increase fertility. Nitrogen and trace
minerals may be added to soil in many chemical forms, each of which may
change the availability of plutonium for absorption by flora or fauna.
The selectivity of organisms for iron and plutonium present in the
same biomass is not thoroughly understood. This may be affected by
seasons, nutritional needs, altitude and age of the receptor.
Investigations underway by NAEG indicate that the availability of
plutonium may be increased each time it is ingested by an animal, passes
through the digestive processes and is excreted. This may concentrate
plutonium in vegetation growing on plots of ground previously fertilized
by the application of contaminated manure. More work must be done before
these complex interactions can be understood.
Some work has been completed on the behavior of plutonium in aquatic
systems. The reactions of plutonium particulates in fresh and saline water
are just beginning to be understood. Incorporation of particulates within
bottom sediments may isolate plutonium and prevent dissolution for long
periods of time but violent agitation, e.g., storm wave action, mechanical
mixing or erosion and flooding of large land areas and deposition of the
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sediments on farm lands may cause a release of this stored plutonium and
increased uptake by biological systems. This mechanism should be better
understood since most nuclear power plants are located near large sources of
water increasing the potential for low level chronic release in effluent
streams.
The role, microorganisms play in affecting availability of plutonium
in soil-plant relationships is being studied on a limited basis. Little
is known of plutonium interaction with microorganisms present in the
gastrointestinal tract. Work has started on the absorption of plutonium
by algae. Ingestion of this algae by aquatic organisms may lead to further
concentration and transfer up the food chain.
There are many studies underway by the NAEG as summarized by Dunaway and
White2"* in 1974. Many of these studies seek to further information on the
behavior of plutonium in fauna found within a desert environment. These studies
encompass tissue concentration of plutonium in cattle grazing in contaminated
areas, rodents and lizards inhabiting the same area, transfer of various forms
of plutonium to milk by dairy cows, and concentration of plutonium in tissues
and eggs of chickens ingesting differing forms of plutonium.
Many authors have devoted much time to extrapolating the results
obtained with laboratory animals to man. This comparison though perhaps
valid in many instances, may prove to be of limited use when the compli-
cating factors and discriminating mechanisms inherent in man's physiology
are taken under consideration. The effects of chronic plutonium contami-
nation in humans necessary for a true evaluation of its hazards will continue
to be a source of conjecture for many years in the future. Man can only hope
to limit the concentration of this potentially hazardous radionuclide in the
environment until additional knowledge is forthcoming.
INTRODUCTION
OBJECTIVE
The objective of this review is not to develop a comprehensive biblio-
graphy on plutonium, but rather to identify and comment upon the significant
and relevant literature representing the many detailed studies of the inter-
action of plutonium in biological systems. Material included in this review
has been selected to provide an overview of the subject and to indicate
where deficiencies may exist in biological data.
Plutonium, produced for the first time in 1941, has been released and
distributed throughout the biosphere during the last 25 years. The physico-
chemical changes induced by natural processes may enhance the biological
availability and increase the concentration of plutonium in specific biomes
thereby causing greater biological effects and risk to mankind.
The concern then is to limit the production and control the use of
plutonium until such time as the very complex interactions with biological
systems have been investigated and a better understanding of potential
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hazards has been achieved. The need for energy makes It imperative that
mankind make most efficient use of available sources and channel the
potential of plutonium-derived energy to the benefit of all, while mini-
mizing the deleterious effects on man and his environment. Only by an
overall understanding of what has been found in the past can guidelines be
set for the future.
APPROACH
Literature included in this report was selected on the basis of its
significance and relevance from a variety of bibliographies, general
references and abstracts. Where the original reference was not available
to judge the value of the reference, the abstract was consulted to determine
its applicability.
ORGANIZATION
This report lists annotated bibliographies, important general references
and abstracts. Thereafter, the literature is reviewed in essay form on a
subject basis. The subject headings are covered in individual sections
and under each of these, several subsections review literature on a given
topic. The 419 references reviewed are cited in the appropriate subject
divisions of this report and in complete bibliographic form at the end
of the report in the order mentioned in the text. Finally, an author
index of the references cited is included to facilitate the location of
particular material.
BIBLIOGRAPHIES
The following bibliographies are closely related to the subject.
(1) Environmental Aspects of Plutonium - A Selected Annotated
Bibliography, September, 1972, Environmental Plutonium Data Base Group,
Oak Ridge National Laboratory, Oak Ridge, TN, ORNL-EIS-72-21, 387 p.
(2) Ibid (Suppl. 1) August, 1973, ORNL-EIS-73-21, 479 p.
(3) Ibid (Suppl. 2) February, 1974, ORNL-EIS-74-21, 272 p.
These three volumes contain over 2,000 references on the environmental
aspects of plutonium and uranium at the Nevada Test Site (NTS). The litera-
ture was selected to meet the needs of the Nevada Applied Ecology Group (NAEG)
of the Nevada Operations Office, Las Vegas, Nevada.
(4) Environmental Aspects of the Transuranics - Compiled and edited by
Martin, F. M. , Sanders, C. T., and Talmage, S, $. , Oak Ridge National
Laboratory, TN, ORNL-EIS-74-2 (Suppl. 3) December 1974, 226 p.
This bibliography contains 528 references on the environmental aspects
of uranium and the transuranic elements, with a preponderance of material
about plutonium. Indexes are given for authors, subjects, categories,
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keywords, geographic locations, permuted titles, taxons, and publication
descriptions.
(5) Biological Effects of Plutonium. A Bibliography - Compiled
by Suratno, P., CE-BNL-Bib-6, 60 p.
This bibliography was compiled mainly from Nuclear Sciences Abstracts
for the period 1969-1973. It was produced in support of the continuing
work at Berkeley Nuclear Laboratories on the health physics problems
associated with the transuranic elements. Its arrangement is in three
sections: A. Biological Effects (47 refs); B. Physiological Aspects
(110 refs); and C. Techniques of Measurement (60 refs).
General Reference Reviews and Summaries
The following reports or references give reviews and summaries of
available information related to the subject.
(1) Uranium-Plutonium-Transplutonic Elements, Hodge, H, C,, Stannard,
J. N., and Hursh, J. B., Eds., Springer-Verlag, New York, 995 p., 1973.
This book is separated into three broad categories and 21 chapters
which deal separately with uranium, plutonium, and the transplutonic
elements. In general the sections discuss history; chemical and physical
properties; distribution, excretion, and effects; body burdens; bioassay;
health physics aspects; and environmental considerations.
(2) Radiobiology of Plutonium, Stover, B. J. and Jee, W, S. S., Eds.
The J. W. Press, University of Utah, Salt Lake City, Utah, 552 p., 1972.
This book is separated into 25 chapters dealing with general topics
of historical background, metabolism and effects of plutonium as pertains
to beagle studies, metabolism of 239Pu in rodents, use of chelating agents*
and plutonium in man.
(3) The Metabolism of Compounds of Plutonium and Other Actinides,
ICRP Pub. 19, Pergamon Press, New York, 59 p«, May, 1972.
This report reviews literature up to 1972 relating to the chemistry of
plutonium as related to biological behavior, e*g., entry of plutonium
by inhalation, absorption and retention of deposited actinides. Three
tables are given which summarize principal inhalation studies with plutonium
compounds in experimental animals, absorption of actinides from the gastro-
intestinal tract and distribution of actinide compounds in experimental
animals and man.
(4) "A Review of Transuranic Elements in Soil, Plants, and Animals »
J. Environ. Quality 2;1» pp, 62-65, 1973.
Published information concerning the distribution and fate of neptunium,
plutonium, americium and curium in terrestrial ecosystems is reviewed in this
article.
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(5) "Physiopathology of Plutonium Contamination: Fundamental
Concepts," Saenz, M« D. L. and Ramos, E,, translated by Ralph McElroy Co.
for Los Alamos Scientific Laboratory, Los Alamos, LA-TR-74-16, 40 p.,
1973, translated 1974.
Published information concerning the physiopathology of plutonium
was reviewed including internal contamination, effects, dose and therapy.
(6) "Consideration of Reactor Accident Exposure Guides for Plutonium,"
Bair, W. J., BNWL-SA-4968, 23 p., 1974.
This report reviews some of the biological aspects needed to be
considered in establishing an emergency reference dose for plutonium. The
discussion is limited to plutonium entering the body through the respiratory
tract.
(7) "Evaluation of Plutonium-Contamination in Radioactive Waste
Disposal Areas with Respect to Their Potential Hazard and Eventual
Disposition," McCurdy, D. E., M. L. Wheeler, M. D. McKay, and R. K.
Lohrding, Quarterly Report Transuranic Solid Waste Management Research
Programs October-December 1973, Los Alamos Scientific Laboratory, p. 17-55.
This report evaluates the plutonium contaminated waste disposal areas
of the Los Alamos Scientific Laboratory (LASL) and analyzes the risk of
natural and man-made disasters that could be causal events for releasing
stored waste to the environment, the resulting abiotic transfer processes for
movement of the released plutonium-contaminated waste, biological trans-
port mechanisms, radiological assessment of the intake of transuranic
elements and the radionuclide inventory of waste disposal areas at LASL
are also discussed.
(8) The Dynamics of Plutonium in Desert Environments, Dunaway, P. B.
and M. G. White, Eds., NVO-142, 369 p., July, 1974.
This is a progress report of projects of the Nevada Applied Ecology
Group, U.S. ERDA, Nevada Operations Office and contains summaries of
work presently underway as well as preliminary reports of completed
projects. The several topics covered are soils, statistics, vegetation,
animals, resuspension, distribution, and inventory modeling and infor-
mation as applies to plutonium on the Nevada Test Site and surrounding
environs.
POTENTIAL SOURCES OF PLUTONIUM
GENERAL
Plutonium is a radioactive element of increasing importance as the
need for energy sources becomes more acute. It is one of the most toxic
radionuclides because of its biological behavior as well as its physical
characteristics.
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As summarized by Saenz and Ramos1 in 1973, the Importance of plutonium
has been apparent since it was produced for the first time by Seaborg and
others as reported by Weast2 in 1966. Although the existence of plutonium
in nature has been proven, its natural quantities are so low (Levine and
Seaborg3 in 1951 and Hoffman1* et al. in 1971) that the risk comes from
its artificial production.
Of the radioactive plutonium isotopes, 239Pu is the one most used in
the nuclear industry where it is produced by irradiation of 238U in nuclear
reactors. Its high specific activity and long half-life determine its
high radiological toxicity (Saenz and Ramos1).
Increasing use of plutonium in nuclear fuel, industrial, biomedical and
space applications, as well as weapons development, increases the possibility
of accidental releases contaminating the biosphere.
Since 1952, weapons tests and nuclear accidents in space have released
plutonium into the biosphere with resultant fallout over the entire earth
(according to the estimates of Cherdyntsev5»® et al. in 1968 and 1970)
approximating a concentration of 239Pu of 10 12% when mixed in the first
few centimeters of soil. The values of liberated plutonium given by the
Scientific Committee of the United Nations and reported by Norwood7 in 1971,
assumes an activity of 0.5 mCi of 239Pu, equal to eight tons.
Global air activity values for 239Pu were shown to be 10 15 Ci/m3 of
239Pu in 1963 as reported by DeBortoli8 et al. in 1966 and 10~17 to 10~16 Ci/m3
in the USA in 1965 as calculated by Drobinski9 et al. in 1966. These values
appear to coincide in order of magnitude with later maximums arrived at
by Volchok and Kleinman10 in 1971.
Although the risk from weapons testing would appear to be low, the
increasing use of plutonium in industry, medicine and aeronautics has caused
Seaborg11 in 1970 to forecast that these applications will use 60 to 80 tons
of 239Pu in the next few decades and up to 6 tons of 238Pu by the end of the
century.
Environmental contamination as the result of accidents was reviewed by
Eisenbud12 in 1973. The events discussed include: fallout from the thermo-
nuclear detonation of March 1, 1954; the accident to the Windscale Reactor
number one of October 1957; the Oak Ridge plutonium release of November
1959; the Army Stationary Low-Power Reactor (SL-1); the Houston incident
of March 1957; the Fermi fuel meltdown; the abortive reentry of the
SNAP 9-A; and the plutonium fire at Rocky Flats.
WEAPONS DEVELOPMENT
The first formal environmental contamination experiments with plutonium
were carried out under the auspices of the U.S. Atomic Energy Commission
(AEG) at the Nevada Test Site. In 1956 a test (Project '56) was carried
out to study the behavior of released plutonium in air, soil, and the desert
environment. No biological work was included in this experiment. As •'
reported by Stannard13 in 1973, "Operation Plumbbob" conducted in 1957 a
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full scale biomedical program was undertaken by a group from the University
of Rochester (Wilson et al.) along with more elaborate studies of aerosols,
cloud physics, decontamination and area monitoring studies by a group from
Sandia Corp. (Cowan15) and the United States Air Force. The levels of
ground contamination were on the order of 2.6, 40 and 560 micrograms per
square meter of desert soil.
"Operation Roller Coaster" was a. joint United States-United Kingdom
venture and was carried out in a remote area of north central Nevada.
There were four test firings and the emphasis was placed on inhalation
of plutonium from cloud passage according to Wilson and Terry16'17 in
1965 and 1968.
An environmental inventory of the Los Alamos area was reported for the
period July 1, 1972 to March 31, 1973, by Hakonson18 et al. in 1973. Included
in this survey was the Trinity area, scene of the world's first nuclear deto-
nation (July 1945). A similar study of the 2,200 hectares surrounding Los Alamos
was reported by Johnson19 in 1972. These environmental assessments included
careful search of the administrative records to determine the extent to
which the land might have been used or involved in the Laboratory's activities.
Extensive measurements of the radiation levels in the field, and radiochemical
analysis of numerous soil and vegetation samples were completed. Results
showed that all measured values were comparable to reported worldwide levels,
and no radiation or radioactive contamination observations were encountered
that are of radiological health or environmental concern. In a similar
n ft
report by Hakonson and Johnson in 1973, a comparison was made between the
data collected 20 years earlier and that collected in 1972. The major change
observed was an increased migration of plutonium downward through the soil
profile. Concentrations of plutonium in vegetation and rodents were too low
to make valid comparisons.
o i
The comprehensive review prepared by Eisenbud in 1973 of fallout
distributed from nuclear explosion includes the amounts and distribution
of radioactive debris produced in weapons tests; methods of estimating
how radioactive debris is partitioned among the three components of fallout
(the fallout in the immediate vicinity of the explosion, the debris injected
into the troposphere, and the debris injected into the stratosphere); and
the behavior of plutonium released in weapons tests.
In the quarterly reports of the New York Operations Office Health and
Safety Laboratory, Hardy ' tabulates the data from the fallout monitoring
program. The plutonium 'content of atmospheric samples obtained through
Project Air Stream during 1970 and 1971 and the plutonium content of
stratospheric samples obtained through the High-Altitude Balloon Sampling
Program during 1969 and 1970 are included in the report for March-June 1971.
The June-September 1972 report shows plutonium deposition at worldwide land
sites and those collected at Atlantic Ocean weather stations.
Environmental surveys of the main areas of plutonium deposition at the
Nevada Test Site are included in the Nevada Applied Ecology Group Progress
Report edited by Dunaway and White in 1974.
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WEAPONS IN TRANSPORT
American bombers carrying nuclear weapons have crashed in Spain in 1966
and Greenland in 1968. Problems connected with the detection and decontami-
nation of these areas were discussed by Hvinden25 in 1973. The area contami-
nated in Spain was cleared sufficiently after 2 or 3 months to allow agricul-
tural use. In Greenland, measurements of fish, birds, foxes and seals showed
no contamination above allowable limits.
In a follow-up study, Hanson26 in 1972 was able to detect small amounts
of 239Pu and 21*°Pu in lichens collected near the Greenland site during
July-August of 1968. This activity was associated with -particles estimated
to be 0.5 to 1.0 micrometers in diameter containing slightly greater than
background levels of plutonium radioactivity.
FUEL PROCESSING AND REPROCESSING
Increasing utilization of nuclear fuels will result in wide-scale
plutonium recovery processing, reconstitution of fuel, transportation
and extensive handling of this material. According to Paxton27 in 1972,
there have been only six supercritical accidents spread over 20 years of
processing fissile material. None of these was associated with mechanical
processing, storage or transportation. All occurred in recovery plants and
all occurred with aqueous solutions; four involved highly enriched uranium,
and two involved plutonium. One of those involving plutonium occurred at
the Los Alamos Scientific Laboratory - December 30, 1958, and the other at
the Recuplex Plant at Hanford, Washington, April 7, 1962. The results of
these 6 accidents have been 2 deaths, 19 significant overexposures to
radiation, no equipment damage, and negligible loss of fissile materials.
In no case was there any danger to the general public.
Many safeguards are built into facilities used for processing of nuclear
fuels so that confinement of radionuclide release to the environment is kept
to a minimum. It is a well recognized problem that plants handling long-
lived radionuclides may release extremely low levels of radionuclides daily
through filters or other pathways. Although these releases may not be
generally measured in terms of air concentration, after many years of opera-
tion small quantities of the material can be detected outside of the facility.
This has happened at Rocky Flats and other areas according to Biles28 et al.
in 1971.
A study was made of the possibility of hazardous environmental plutonium
releases caused by uncontrolled oxidation of plutonium within the enclosure
at Rocky Flats (Hunt ). The report reviews the existent observed data on
restricted plutonium release and then constructs a release model relating
the free-release source strength (i.e., the source strength outside the
enclosure) and the parameters describing the release. Based on both the
observation data and the model calculations, the conclusion follows that
restricted release is unlikely to lead to dangerous free-releases of a
plutonium aerosol. The model calculations specifically show that the maxi-
mum credible accident assumed, would be safe by about 2 to 5 orders of
magnitude. However, the calculations indicate that maximizing either the
8
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Plutonium release rate or the asymptotic temperature reached in an enclosure
can cause a free-release exceeding the safe rate.
FIRES
The pyrophoric nature of plutonium metal has led to several plutonium
fires. The major fires occurred at Rocky Flats in 1957 and 1969 and resulted
in airborne plutonium being distributed over a wide area surrounding the
facility and resulted in contamination of the soil as reported by Hardy and
Krey30 in 1970.
An analysis of 46 incidents involving plutonium metal or compound under
thermal stress has been reported by Mishima and Schwendiman31 in 1971. These
incidents, occurring in the nuclear industry during the period from 1952 to
1967, are cataloged as to the nature of the material involved, the initiating
event and the consequences.
WASTE DISPOSAL FROM PLANTS
For several decades, transuranic-containing solid waste has been placed
in shallow burial grounds at several of the AEC contractor facilities. The
hazards of the release of this radioactivity from the waste burial environ-
ment at the Los Alamos facility was discussed by McCurdy32 et al. in 1974.
The possible catastrophic events leading to the release of these materials
are addressed and a model is proposed for the movement of these radioactive
materials throughout the environment.
A review of processing of plutonium-contaminated liquid wastes at
Los Alamos was reported by Emelity and Christenson33 in 1971. This report
lists the quantities of liquid wastes processed during the years 1966
through 1970.
Over the past 20 years, the National Reactor Testing Station (NETS) in
Idaho has accepted radioactive waste for burial. Wastes received included
materials contaminated with transuranic elements, primarily from AEC's Rocky
Flats operation, as well as items contaminated with fission products and neutron
activated materials from various onsite operations. Early disposal methods
varied from stacking of drummed and boxed waste into pits to random dumping
of various categories of waste into common trenches or pits. Reassessment of
past disposal practices and concern for long-term isolation of transuranic
wastes led to the establishment of above-ground retrievable storage in
1970. However, about 54,000 cubic meters of alpha waste remains buried at
NRTS. The plan for retrieval of this waste for treatment and storage in
a Federal depository was reported by Hickman3"* in 1974.
Liquid wastes from the plutonium finishing plant at Richland, Washington,
have been discharged to subsurface disposal facilities (enclosed trenches)
since the startup of the facility approximately 22 years ago. The removal
and disposal of this contaminated soil is discussed in AEC Environmental
Statements35*36 of January and April of 1972.
New guidelines for the interim storage of solid transuranic wastes were
proposed by the H-Division staff of Los Alamos37 in 1974. A summary of
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current practices in solid waste disposal is included.
A review of radioactive waste disposal and its eventual pollution of
groundwater from this waste was completed in 1974 by Todd and McNulty
SHIPMENT
A Q
It has been estimated by the U.S. Atomic Energy Commission in 1972
that by the year 2000 the total nuclear power generating capacity in the
United States will be approximately 1200 gigawatts. Over the next 25 years,
the expansion will increase the need for shipping 239Pu (produced in light
water reactors and liquid metal fast-breeder reactors) from fuel reprocessing
plants to fuel fabrication plants where these fissile isotopes can be recon-
stituted into reactor fuel elements.
If aqueous solvent extraction processes are employed for separating
plutonium in the spent fuel, the plutonium will emerge in the reprocessing
plant product streams as nitrates in aqueous solutions. The problems and
hazards inherent in shipping these solutions were discussed by Ulrica1*0 in
1974. In a conference on transportation of nuclear material, Wischow1*1 in
1970 reported case histories of misrouted and misplaced shipments. Corrective
action and regulations pertaining to physical prohibition of fissile materials
were briefly discussed. Hazards associated with transportation accidents in
which plutonium was subjected to gasoline fires were reported by Mishima and
Schwendiman42 in 1973.
Becker"*3 in 1971 reported on steps that LRL was taking to improve controls
over packing of plutonium shipments. Two case histories were cited. The
importance of quality control in packaging Pu(N03)if solution and PuOa powder
was discussed in an article by Brown and Heaberlin'*'* in 1974. An industry-
wide survey was conducted of 775 shipments involving 6,200 packages over a
period of 3 to 4 years. Package closure error could result in breaking of
containment during shipment or a series of errors might release the contents
during normal shipment. A listing of closure faults is provided with the
number of times the faults have been observed.
This is not a complete record of these faults as records on errors were
not kept consistently as required to be kept. Although increased quality
control procedures implemented since 1972-1973 have decreased the frequency
of these errors, they have not been entirely eliminated.
The problems of calculating risk of criticality in transporting fissile
materials were addressed by Thomas1*5 in 1971. Proper packaging and container
sizes are discussed.
NUCLEAR REACTORS AND RADIOISOTOPIC GENERATORS
Plutonium is produced by irradiating uranium with neutrons in a nuclear
reactor. Its isotopic composition depends on the time in the reactor and
the type of reactor. This plutonium may be recycled in light-water reactors.
Utilization in this way will require reprocessing and fuel refabrication.
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The introduction of commercial fast-breeder reactors is not expected to
occur until the mid-1980's according to Pigford and Mann1*6 in 1973. The
fast-breeder reactor has excellent fuel economy. It is fueled with plutonium
and "breeds" plutonium from 238U, creating a surplus for the first fuel charge
of other fast-breeder reactors. The danger from this type of reactor, accord-
ing to Hamilton in 1971 is that the chain reaction can easily run away,
creating a supercritical mass which would eventually be blown apart. The
total radioactivity in the yearly amount of fuel discharge, at the time of
discharge, is greater for the fast-breeder reactor than for the light-water
plant because of the need for more frequent replacement of core fuel in the
breeder. The yearly amount of plutonium in the fast-breeder fuel cycle is
about eight-fold greater than in the light-water nuclear plant. An experi-
mental 1000 Mw(e) fast-breeder reactor will contain about 1.8 to 2.8 tons
of plutonium corresponding to 2.2 to 3.5 million curies of plutonium
according to the U.S. Atomic Energy Commission48 report of 1972. A flow
sheet listing the material and environmental release for a breeder reactor
nuclear power plant was presented by Pigford and Mann1*6 in 1973.
A historical resume of the breeder reactor program and its impact on the
environment was given in a report by Daub49 in 1972. A program plan listing
fuel materials and accident conditions for a liquid metal fast-breeder reactor
(LMFBR) was'presented by the Argonne National Laboratory50 in 1972.
Safety aspects of nuclear fuel cycles were reviewed by Wymer51 in 1971.
Future developments and requirements for the nuclear fuel cycle are also
discussed. Plutonium utilization in boiling water reactors is summarized
in a report by General Electric Company,52 released in 1971. Activities
associated with t;he AEC-sponsored Integrated Safeguards Experiment and
Plant Instrumentation Program are reported. A review of plutonium utili-
zation in thermal reactors was presented by Schmid53 in 1973. Recycling,
fueling, decontamination and safety are discussed. The drawbacks of nuclear
power were discussed by Engstroem54 in 1972. Siting of power plants, radia-
tion hazards and environmental impact are included. .The dangers associated
with nuclear power reactors were described by Lapp55 in 1975. The possibil-
ities of accidents occurring are presented in an analytical diagram called
an "accident tree." Of all the possibilities, the probability of a few
hundred of the most important was determined and of these 15 were judged
to be the major sources of risk. An assessment of accident risks in U.S.
commercial nuclear power plants was reported by Rasmussen56 in 1974.
The health physics aspects of fast-breeder reactors were discussed by
Heine and Hart57 in 1971. The specific aspects are grouped according to
segments of reactor operations. Under certain hypothetical accident
conditions where fuel vaporization could occur, plutonium could be the
dominant hazard.
The results of a radiological environmental survey in the vicinity of
EBR-II were given by Oltman58 et al. in 1973. Measurements were made at
radial distances up to 5 miles from the effluent stack. Soil samples were
obtained and analyzed for plutonium content. No plutonium deposition pattern
could be constructed.
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A series of studies to evaluate the fractional airborne release of
Plutonium under various postulated reactor accident conditions was completed
by Mishima and Schwendiman59 in 1972. Data generated in earlier laboratory
scale studies were also reviewed. Topics dealing with the acceptability of
nuclear fission for energy sources were discussed by Gofman60 in 1972. The
biological problems associated with nuclear fission, the fission product
problem, the plutonium problem and the major accident problems are included.
The University of Washington nuclear reactor plutonium contamination incident
of June 13, 1972, was discussed by Hilborn6l et al. in 1972.
Both major and minor accidents involving the release of aerosols of
sodium are possible during the generation and maintenance of a fast reactor.
These aerosols could be radioactive, involving not only the radioactive
sodium, but also fission products, uranium and plutonium. This problem
was reviewed by Kotrappa62 in 1973. The use of nuclear power generators,
batteries and heat sources for use on land, in space vehicles, ocean diving
equipment and for powering artificial pacemakers, organs, and other medicinal
uses increase the possibility of environmental contamination from these
sources. A detailed nuclear safety evaluation of the SNAP-19 C generator
was conducted by Conway and Dobry63 in 1973. In 1972 Weiner6"* reported on
the safety testing of a 238Pu fueled Radioisotope Thermoelectric Generator
(RTG) for the Navy Transit Satellite. The containment of the 238Pu fuel
was checked for all normal reentry environments and for all accident
environments during prelaunch, launch pad, early launch abort and pre-
orbital insertion abort.
The operating experience and advances in the safety of space nuclear
power systems fueled with 238Pu were reviewed by Dix65 in 1972. The opera-
tional safety experience with eight NASA launches of spacecraft powered
with nuclear energy since 1968 including two Nimbus weather satellites,
the Apollo 12, 13, 14, 15 and 16 lunar landing missions, and the Pioneer 10
Jupiter mission was discussed. The concept of isotopic power generators is
explained in a 1971 article by Penn66. The heart and pacemaker batteries
and the UKAEA RIPPLE (radioisotope-powered prolonged life equipment) generator
is described. In 1971 Williams57 developed models for estimating the extent
to which radioisotopic fuel forms will vaporize if released to the fires
resulting from the catastrophic aborts of rocket booster vehicles. Pad
aborts of both liquid- and solid-propellant systems are considered and aborts
after lift-off are also treated. Estimates are given for the size and
activity spectra of the radioactive particles produced when the vapor
recondenses. Numerical results are specifically calculated for certain
238Pu(>2 fuel forms (microspheres, solid-solution cermet, and plutonia-
molybdenum cermet). Tables for the ingrowth of daughter products from the
decay of plutonium isotopes used in heat sources are given in an article
by Haas and Campbell68 in 1972. The typical composition of the plutonium
metal used in the fabrication of the sources is also listed.
The general considerations of radioisotopic power and its international
aspects were discussed by Cellini and Stadie69 in 1972. The work of the
OECD Nuclear Energy Agency since 1967 in studying radioisotope batteries,
particularly for cardiac pacemakers is discussed. This work includes heat
source development, capsule evaluation, safety assessments of radioisotope
heat sources under normal and accident conditions, radiation hazards
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evaluations, and human implantation of 238Pu fueled pacemakers which began
in April 1970.
Safety tests of plutonium fueled devices for medical applications were
presented by Warner70 in 1972. Results demonstrate that plutonium devices
are suitable for widespread implantable medical applications. The current
status of radioisotope-powered artificial organs was given in 1972 by
Toyoshima and Hart71. The basic problems of energy sources for implant-
type organs and the status of high reliability long-life (10 years) 238Pu
power sources were discussed.
The use of radioactive material as a power source implanted in the
human body such as 238Pu batteries to drive cardiac pacemakers, becomes
more important. In most cases the amount of radioactive material implanted
in the body is considerable and the nuclide hazardous (Hunzinger72).
Bearers of isotopic batteries are not necessarily old people bound to
hospital beds. They include all ages and persons in their full professional
activity. A bearer of an isotopic battery can hardly be confined to a
controlled zone, the establishment of which is a well known principle of
control in radiation protection, nor can the person be treated like a
consignment of radioactive material and be subject to the well established
test procedures for these packages. The safety principles of isotopic
sources implanted in a freely moving human are outlined in this paper.
The focus is on the exposure of other people to penetrating radiation,
on partial loss of the radioactive material, i.e., exposure to contamina-
tion and the total loss of control over the source. Safety in industrial
fabrication of implantable devices powered by radioisotopes was discussed
by Matheson73 in 1971.
TRANSPORT OF PLUTONIUM FROM SOURCES TO BIOSPHERE
INTRODUCTION
The presence of free plutonium in the atmosphere, ground and water can
lead to direct contamination by inhalation or through ecological cycles.
Understanding the transport mechanisms for the various physical and chemical
forms of plutonium from the contaminating source to the biosphere is compli-
cated by the nature of plutonium chemistry. The fate of the released pluto-
nium is uncertain and complex.
Studies have been conducted by several investigators to determine the
problems associated with plutonium cycling in the environment and reported
in 1973 by Carfagno and Westendorf7\ These authors discuss the research
being done to determine the mobility of radionuclides in major segments of
terrestrial environments. Reciprocal transfers of environmental radio-
activity are investigated for three major components—soil, plant, and
animal.
The environmental levels of plutonium at U.S. Atomic Energy Commission
installations were summarized in a report by the U.S. Environmental Protection
Agency75 in 1973. The sources and activities of plutonium found in environ-
mental samples are given.
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The behavior of plutonium in ecosystems and its biological effects on
natural fauna and flora as applied to desert ecosystems at the Nevada Test
Site were presented by Romney and Davis76 in a report published in 1971,
The environmental monitoring program for a nuclear fuel reprocessing
plant (located in the South Carolina coastal plain), as based on a man-
environment ecosystem concept, was described by Platt et al. in 1973. The
principal pathways to man—atmospheric, terrestrial, and aquatic—are each
subdivided into natural, recreational and domestic components. The use of
ecologically defined samples provides rates of movement and bioaccumulation
that lead to ecological models that are transferable to other nuclear
industries.
Research to provide data on the mobility and transport of plutonium
in environments associated with nuclear power production facilities of
the humid eastern United States was outlined by Reichle78 et al. in 1974.
A model for predicting the redistribution of particulate contaminants
from soil surfaces was proposed by Travis79 in 1975. The usefulness of
this predictive tool is demonstrated by calculations involving mixture
of particulate 238Pu02 in highly erodible soils under dust storm conditions.
Time dependent surface concentration and breathing zone exposure isopleths,
evolving from a small contaminated area, show the potential hazard from wind
eroding toxic materials.
Wind distribution of plutonium released by the fires at Rocky Flats
was discussed by Poet and Martell80 in 1974.
CHEMICAL AND PHYSICAL STATES OF ENVIRONMENTAL PLUTONIUM
Since the chemical and physical states of plutonium determine its
transport throughout ecosystems, these states will be discussed separately.
Soil
Soil chemistry mechanisms partially control the biotic availability of
plutonium over long time periods. The chemical form of radionuclides in
soil in the vicinity of Oak Ridge National Laboratory and the character of
secondary reaction products and the availability of nuclides to plants
after weathering under natural environments was included in the report by
Carfagno and Westendorf7>t in 1973.
Miner81'82 et al. in 1972 and 1973 give the results of studies on the
chemical behavior of plutonium in soil-water environments. Plutonium
dioxide and soluble plutonium were shaken with a soil-water mixture and
the plutonium in the various phases was measured.
Isotopic ratios and chemical constituents of plutonium in soils and
sediments of the Argonne National Laboratory were listed in 1974 by Sedlet83
et al.
The chemical nature of waste solutions discharged to the soil of the
Hanford facility and a study of their present form were reported in 1973
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by Swanson81*. The leach behavior of plutonium in these soils was also
investigated.
As stated by Krey85 in 1974 and Poet and Kartell86 et al., the knowledge
of the chemistry of fallout plutonium in soil is not very complete. They
tabulate the mobility of plutonium in soil from Rocky Flats, Rhodes87'88
in two articles published in 1957, pointed out the polymerization known to
occur in soil. The slow rate of diffusion and leaching of plutonium by
groundwater at the Hanford facility was reported by Hajek89 in 1966. Self-
diffusion of plutonium in soils will only occur due to migration of molecular
size particles through soil solutions. He concluded that plutonium could be
expected to move about 85 mm in 2.4 X 105 years by this process. This was
predicted by using soils moistened with 20% water content by volume. This
is a high water content when considering desert environments.
The rate of transport of plutonium out of a waste burial area by
migrating soil moisture is dependent on many factors. The chemical forms
of the isotopes and their respective solubility in water must be determined.
The amount of dissolution of plutonium from waste is strongly affected by
the chemical form of plutonium present, and by the chemistry of the leaching
solution. In general, soluble salts increase the solution rates, as do
organic complexing agents [Los Alamos Scientific Laboratory (LASL)90 in 1974].
In 1974, LASL9"and Patterson91 et al. commented that plutonium leaching
from soil appears to be more affected by solubility than by exchange
reactions.
Plutonium absorption by soils is equally complex, being strongly
affected by pH, as well as the concentrations of other metallic ions.
Plutonium appears to be present as a polymer in most solutions and is
highly sorbed by natural materials. In general, it behaves as a cation
at pH values up to about 12, at which point it exhibits strong anionic
properties.
Dissolution and absorption of plutonium can be quantitatively described
in terms of a distribution coefficient (ratio of material concentration on
solid phase to concentration in liquid phase, Kd), as in Christenson92 et al.
in 1958. A table showing solution percentage and distribution coefficients
for plutonium in waste and soil was given in the LASL90 report.
The distribution and characterization of plutonium in soils from the
Nevada Test Site were reported by Reichle78 et al. in 1974. The leach-
ability of plutonium from soils containing different particle sizes was
also given.
The physical aspects of plutonium in soils affect its solubility and
transport by resuspension. Plutonium resuspension from soil is the subject
of reports by Michels93, Sehmel and Lloyd9"*'95. These reports cover resuspen-
sion of plutonium from the vicinity of Rocky Flats and investigate effects
of particle size and wind speed.
The evaluation of the resuspendable amounts of plutonium-238 in soil
from the vicinity of the Mound Laboratory at Miamisburg, Ohio, was given
in summary reports by Carfagno and Westendorf96,97,98 in 1972 and 1973.
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Results of analysis of silt samples from the Great Miami River were also
given.
Air
The importance of knowing the chemical and physical forms and the uncer-
tainties involved in estimating inhalation exposures from the 239Pu contami-
nation at Rocky Flats were reviewed by Boss" in 1972.
In 1972 Volchok100 et al. investigated the plutonium in the neighborhood
of Rocky Flats as pertains to airborne respirable particles. Experiments
were carried out to determine the respirable fraction of the resuspended
239Pu. The results indicate that in this area, with concentration in excess
of 1 fCi/m3, the respirable fraction is about 0.2 to 0.4.
In 1972 Fish101 et al. discussed experimental data and analytical models
to be considered in assessing the transport of plutonium aerosols following a
hypothetical reactor accident. Behavior of released airborne materials
within the reactor containment system, as well as in the atmosphere near
the reactor site boundaries, were semiquantitatively predicted from experi-
mental data and analytical models.
The results of a simulated airborne release of uranium, representing
plutonium, during the burning of contaminated waste were discussed by
Mishima and Schwendiman102 in 1973. A source term containing both a
fractional release and aerodynamic size distribution is required to evaluate
the potential downwind hazard from a postulated inadvertent release. The
approach taken in this study of a potential accident situation in a radio-
chemical processing plant was to measure the fractional airborne release
and aerodynamic size distribution released using a simple but realistic
situation. The release of uranium (as a stand-in for plutonium) was mea-
sured during the burning of flammable, solid materials containing either
uranium dioxide powder or uranium nitrate solution. The flammable materials
used were representative of the typical types of solid waste generated by
such a process and were packaged in a typical manner.
In 1972 Mishima and Schwendiman103 characterized radioactive particles
in a plutonium processing plant exhaust system. Filter and cascade impactor
samples were taken of the stack gases and various exhaust streams. The aero-
dynamic characteristics, the amount and distribution of particles and their
associated radioactivity were measured. The general conclusion that was
reached was that the plutonium present appeared to be attached to large,
nonactive particles.
A series of studies to determine the fraction of plutonium made airborne
and characteristics of aerosols produced by overheating plutonium metal and
several plutonium compounds was undertaken by Schwendiman!°"* et al. in 1958.
Plutonium in various phases of processing and use commonly appears in three
forms—plutonium metal, plutonium compounds as powders, and liquids contain-
ing soluble plutonium compounds. All three forms can be found in various
atmospheres and configurations. Of the materials studied, plutonium
compounds in the form of powders released the largest amounts of plutonium
aerosol. The chemical compound, temperature and airstream velocity obviously
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had a great effect on the percentage released. The highest rate of release
was from partially oxidized plutonium oxalate, 0.82 wt % per hour at 1000 C
in 100 cfm per second air. Plutonium fluoride release rates were the lowest
for the compounds considered, 0.007 to 0.05 wt % per hour.
Overheating plutonium metal created less airborne material than its
compounds. The size distribution of the oxide produced can vary with the
oxidation conditions and, since the oxide is friable, the mechanical
processes to which it is subjected. The median mass diameter of the
particles airborne during one of the experiments was 4.2 micrometers.
Heating liquids containing soluble plutonium compounds released the
smallest amounts of material. Using slow heating rates, the maximum amount
airborne from a concentrated plutonium nitrate solution over a 2-hour period
was 0.03 wt %. When a greater heating rate and greater volume were used,
the maximum amount airborne was 0.18 wt % during a 63-minute sampling period
at a full rolling boil. Tables are presented in the report giving the results
of the study in greater detail.
In 1973 Clarke105 devised a model for determining dispersion of effluent
from stacks of nuclear installations and evaluated the inhalation doses.
Plutonium isotopes 239Pu, 2I>0Pu and 238Pu have been injected into the
stratosphere as a result of atmospheric nuclear weapons tests and have
reached the ground as particulate fallout. A satellite bearing a Systems
for Nuclear Auxilliary Power generator (SNAP-9A), containing 17 kCi or 1 kg
of.238Pu reentered the atmosphere in the southern hemisphere in 1969. The
resulting burn-up during reentry turned the 238Pu into small particles at
an altitude of about 50 km. The global inventory and distribution of fall-
out plutonium from these and other sources were compiled by Hardy106 et al.
in 1973. The surface air concentrations and characteristics of the SNAP-9A
burnup in the vicinity of Richland, Washington, were also reported in 1973
by Thomas107.
A mathematical model describing the behavior of particulate Plutonium
in the lower atmosphere was proposed by Travis108 in 1973. The model accounts
for particles settling or impinging on the earth's surface as well as particle
re-entrainment or resuspension.
The radioactive fallout rates and mechanisms describing the behavior
and characteristics of radioactive debris from Chinese nuclear weapons
tests were reported in 1973 by Thomas109 et al.
The nature and distribution of radiation to be expected in the strato-
sphere, including that resulting from nuclear tests, contributions from
plutonium released on burnings of SNAP generators, galactic rays and solar
proton flares were included in a report by Webb110.
Water
The dissolution of 238Pu in environmental systems was the subject of a
report by Patterson91 et al. He points out that some experimenters have
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erroneously assumed that the problem of plutonium transport is connected
with the "solubility" of PuOa, whereas the real problem is the rate of
dissolution. Plutonium dioxide reacts chemically with aqueous solution to
release plutonium ions. These ions, in turn, will react quickly with
other agents in the solution to form soluble complexes or will react with
the water itself to form insoluble suspensions. The term "solubility"
does not apply in the thermodynamic sense to the plutonium dioxide water
system. Because the dioxide cannot be formed in the presence of water, no
equilibrium can be achieved between the dioxide and the plutonium ions in
solution. The dissolution reaction for Pu02 is irreversible, the dioxide
continuously goes into solution. In a static system a state of pseudo-
equilibrium may be reached, with the plutonium in solution remaining
constant. The concentration of ionic species of plutonium is controlled
by the solubility product of the hydrous oxides that are precipitated from
solution according to Polzer111 in 1971. The rate of dissolution of the
dioxide is independent of the concentration of the plutonium ions in
solution.
As stated in 1974 by Patterson91 et al., the definition of plutonium in
solution is not well defined. The "solution" may contain fine particles of
undissolved oxide, precipitated hydrous oxide, polymers in colloidal form,
and various complex ions of plutonium.
As shown by Polzer111 and Silver112 in 1971, the rate of dissolution
of PuC>2 is dependent on many factors, including pH, temperature, oxidizing,
reducing, or complexing agents and surface areas of the oxide (particle
size and shape).
The history of the sample is also important , including the duration and
temperature of heat treatment, time, temperature, and radiation history
since treatment. According to Kapshukov113 et al. in 1971, the high specific
alpha activity affects several of these factors, 238Pu(>2 might be expected to
dissolve more rapidly than 239Pu02. The self-irradiation of the 238Pu02
causes damage to the crystal lattice, but this damage may be annealed out
by heat treatment. It was found that the lower the temperature at storage,
the greater the retention of damage.
In 1974 Patterson91 et al. concluded that Pu02 initially rapidly dissolves
or reacts when first placed in contact with a neutral aqueous medium. The rate
may vary from sample to sample under nominally the same conditions but is
generally greater than 100 ng/m2s for 238Pu and on the order of magnitude
of 1 ng/m s for Pu. After a few hours the rate decreases to a value that
generally remains constant, until the concentration of alpha activity becomes
high enough to initiate competing reactions, such as coagulation of suspended
material or precipitation from a colloid. The change in rate of dissolution
after a few hours is unknown but in 1969 Kubose111* et al. speculated that a
hydrous coating may form, protecting the material from further rapid dissolu-
tion.
In an electrochromatographic experiment, Lingren115 discovered in 1968
that the dissolution of high-fired Pu02 in seawater yielded negatively and
positively charged carbonate complex ions as well as neutral colloids. The
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latter may be in the form of very small hydrous oxides as stated by Lloyd and
Haire116 in 1973.
The dissolution of airborne plutonium in water has been measured in
a scrubber in parallel with an air filter by Hayden117 in 1972.
Some investigations have been done on the dissolution of 238Pu02 micro-
spheres in water (Hudson118 in 1968; Adams and Fowler119 in 1974). In 1973
Raabe120 et al. reported on in vitro solubility of respirable particles of
238Pu and 239Pu.
A report by Curtis and Bentz121 in 1972 discusses the chemistry of
plutonium in natural waters. The assumption that the form of plutonium in
natural water would be that of the tetravalent state is questioned. Acci-
dentally released "soluble" plutonium is alleged to form plutonium-polymers,
or becomes solubilized ionic trivalent plutonium.
Nature provides an abundance of organic materials which may act as
reducing agents toward an oxidizing material such as the Pu + 4 ion, so that
were the Pu(IV) polymer to depolymerize, it might yield trivalent plutonium
ions. On the other hand, plutonium dioxide falling into ocean waters may
spend years dissolving. As radioactive decay and natural causes slowly
degrade the oxide, plutonium may be released to the ocean water very slowly
and at such low concentrations that polymer formation may not be possible.
Several things may occur to the released soluble plutonium: it may become
attached to a bit of sediment or organic material and remain so attached in
the tetravalent state; it may be reduced to Pu(III); or it may be oxidized
to a higher form. A computer program for predicting the final form of
"soluble" plutonium in given conditions of acidity, potential, and complexa-
tion factors was proposed by Silver122 in 1971-
In 1972 Dix and Dobry123 summarized some of the environmental phenomena
that modify plutonium reactions in water. They listed the results of Metz
who placed plutonium sulfate solution in synthetic seawater and found that
it "disappeared" from solution with a half-life of about 40 hours. Of the
plutonium recovered, 50% was found in a tan flocculent deposit on the bottom
of the tank, 20% was found on the walls of the tank below the surface and
about 30% was found on the walls above the water line which was exposed to
the spray from air bubbles resulting from circulation and aeration. Metz's
experiments with a fresh specimen of 238Pu02 molybdenum cermet yielded surface
dissolution rates of 0.01 yCi/day per square millimeter of exposed surface
area (0.05 yg/day per g of Pu02) and plate out of an insoluble plutonium
product was observed on .,the,container surface.
In 1972 Langham124 studied the fate of Pu02 following the Thule accident.
He found that particles agglomerated on inactive debris and only about 1% was
suspended as very fine particulates in water derived from melting ice. In
1966 Lai and Goya125 found that plutonium metal chips placed in seawater
reacted completely in about 10 hours, accompanied by the evolution of hydrogen
which served to continuously expose fresh metal surfaces until the reaction
went to completion. The products of the reaction were small particles of black
material (Pu02) that settled to the bottom and a white or pale green gelatinous
product [Pu(OH)iJ of low density which was suspended in the water. The
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solubility of the above products appeared quite low. As stated by Taube126
in 1964 the equilibrium constant for hydrated plutonium oxide in distilled
water is 7 X 1(T56.
In 1971 Aarkrog127 re-examined the area of the accidental release of
plutonium at Thule, Greenland. The investigation included samples of sea-
water, bottom sediments, bottom animals, zooplankton, fish, seabirds, seals,
seaplants, and lichen. The results showed that the levels had decreased
but plutonium was still present in concentrations significantly above the
fallout background. Samples of bottom sediments showed a vertical movement
of plutonium in the sediments down to a depth of at least 10 cm. Bivales
as far as 30 kilometers from the point of impact contained plutonium from
the accident.
In 1968 Kubose128 et al. found that when 238Pu02 microspheres, 100 ym
in diameter, were implanted in situ in the Pacific Ocean on the surface of
bottom sedimets they became encrusted as a result of biochemical action.
The microspheres were clearly visible in each aggregate and appeared to be
little altered by submergence after 5 months in the sea. The aggregates
were composed of sand grains and organic detritus, which was lightly cemented
around the microsphere by a dense matrix of mucilage and small diatoms. This
phenomena lowered the rate of dissolution of 238PuOa markedly. Observations
were also made on microspheres buried within bottom sediments. The plutonium
adsorbed to the sediments and remained localized at the site of the micro-
sphere.
The particulate size and physicochemical state of plutonium in the
Bikini Atoll Lagoon is reported by Nevissi and Schell129 in 1975. They
found that 16 years following the last nuclear test on the Atoll, the
plutonium was neither buried totally in the lagoon sediments nor has it been
discharged completely to the ocean. Small particles and/or ions are released
at the sediment-water interface and are transported by the currents. These
particles and ions agglomerate during transport away from the sediment surface.
In 1972 an evaluation of the potential for concentration and transfer of
plutonium in Lake Michigan was done by Wahgren and Nelson130. The present
levels, distribution and biogeochemical behavior of fallout plutonium are
presented.
BIOLOGICAL ASPECTS OF THE PHYSICOCHEMICAL COMPLEXITIES OF PLUTONIUM
A detailed summary of the chemical and physical properties of plutonium
was given by Taylor131 in 1973. Saenz and Ramos1 also summarize the physical
and chemical aspects of plutonium as applied to physiological interactions
among biological systems. A brief summary of the most important biological
aspects of the chemistry of plutonium in this review concerned its states of
oxidation, its tendency to hydrolyze, and its capacity to form complexes. The
polyvalence shown by plutonium from Pu(III) to Pu(VII), and the proximity of
its oxidation potentials permit equilibrium states in solution among its ions
of different valences. This coexistence brings about a very complex chemistry
of this nuclide in its biological behavior.
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Mammals
If plutonium in ionic form enters the mammalian body, three main types
of reaction may be expected to occur.
Hydrolysis to yield polymeric or colloidal species - Plutonium can hydrolyze
to insoluble hydroxide, passing through intermediate states of polymeriza-
tion with formation of colloidal aggregates. This phenomena can occur at
physiological pH, qualitatively and quantitatively influencing its distri-
bution and deposit in the various systems, organs, and tissues.
Complexing by proteins or other biological macromolecules - Plutonium deposited
in a localized area will complex with structural proteins. Particulate forms
may be removed by phagocytic action.
Complexing or chelation with small molecular weight components of animal cells
and tissues - Plutonium complexes with anions of mineral acids (nitrates,
carbonates, etc.) and of organic acids (citrates, proteinates). Stability
depends on the complexing bonders. Bonders of great chemical stability can
form complexes which dissociate at physiological pH. Other nonbiodegradable
bonders form biologically stable complexes. Thus, the interaction of plutonium
with a broad variety of biological bonders produces simultaneous mechanisms of
dissociation and formation of new complexes which influence retention, excre-
tion and elimination therapy.
Plutonium compounds occurring as airborne contaminants are either very
insoluble in body fluids, e.g., PuOa, or are relatively soluble and trans-
portable in the body, e.g., plutonium nitrate.
Insoluble plutonium translocates from the respiratory tract very slowly,
over many years, and this imparts most of the emitted radiation energy to
lungs and associated tissues such as thoracic lymph nodes. Insoluble pluto-
nium inhaled as particles normally remains in the particulate form in the
body for a relatively long time. The size of the particles determines the
deposition and mobilization in the respiratory tract. The transportable
compounds inhaled are diffused in the blood and organic fluids, and are
transported to be deposited in organic tissues or excreted in the urine.
Of the nontransportable compounds, a fraction of that deposited in
the upper respiratory channels is exhaled and another part is moved by
ciliary action toward the esophagus and gastrointestinal tract. The remain-
ing fraction which is deposited in the lower portion of the lungs is either
localized or is slowly moved either toward the gastrointestinal tract and
eliminated in the feces, or toward the blood and lymph by solubilization of
the particles or by transport through the pulmonary epithelium. The
mechanics of elimination of radioactive particles from the respiratory
tract are basically ciliary action, phagocytoses and transport to the
circulatory system (blood and lymph).
Saenz and Ramos1 presented the kinetics of movement of plutonium parti-
cles in the respiratory tract and Bair132 et al. in 1973 summarized the depo-
sition arid translocation of inhaled plutonium in great detail.
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Diffusion of plutonium in the blood and interaction with proteins
discussed by Saenz and Ramos1 and Taylor131. Plutonium reaching the blood
may be absorbed and excreted in the urine without change, if the compound
is stable; disappear in a few minutes to be mobilized by the liver, if
strongly hydrolyzed; or form complexes with proteins if the compound is
unstable. Approximately 90% of serum protein is protein bound, mainlv^to
the beta globulin (transferrin) to form a very stable complex (Palmer in
1956 and Belliayer131* in 1959). The interactions of plutonium with protein
are influenced by the physicochemical characteristics of the plutonium com-
pound that reaches the blood.
Many authors have studied the interactions of Pu(IV) and serum proteins
to establish that transferrin is the major plutonium binding protein in man
[(Stover135 et al. in 1968; Bruenger135 et al. in 1970); dog (Stevens137
et al. in 1968; Muntz and Barren138 in 1947); horse (Turner and Taylor139 in
1968); rabbit (Taylor1"*0 in 1969); and rat (Boocock and Popplewell1 "*l in
1965 and Turner and Taylor1"*2)].
As summarized by Taylor131, transferrin is a glycoprotein with a molec-
ular weight of about 90,000 in which aspartic acid, glutamic acid, lysine,
leucine and alanine are the most abundant amino acids. The transferrins of
all the species studied bind 2-gram atoms of iron to form a complex which
dissociates in acid solution but is stable up to pH 9 to 10 as reported
by Feenez and Komatsu1"13 in 1966. The effect of pH on the binding of
Pu(IV) to transferrin was studied by Chipperfield and Taylor1"*1* in 1970,
who showed that maximum binding occurred at pH 7. The mechanisms of Pu(IV)
binding by transferrin are not fully understood. In 1968 Stover135 et al.
and Turner and Taylor139, on studying dog and horse sera, concluded the
bicarbonate ions were required for the binding of Pu(IV) to transferrin in
a similar manner to their requirement in the binding of iron (Feenez and
Komatsu143).
Chipperfield and Taylor11*1* question the requirement for bicarbonate
in the binding of Pu(IV) to transferrin. Plutonium can be displaced from
its combination with transferrin by the addition of iron; little plutonium
is found bound to iron-saturated transferrin (Popplewell and Boocock1"*5 in
1968; Stevens137 et al.; Turner and Taylor139; Massey and Lafuma1"*6 in 1968).
Under their experimental conditions, Chipperfield and Taylor11*1* found that
the binding of iron and plutonium to transferrin was similar in that both
increased up to pH 7; above pH 7 the Pu(IV) transferrin complex was less
stable than the Fe(III) complex, but this may be a reflection of the greater
tendency of plutonium to hydrolyze. The results of these studies indicate
that Pu(IV) can bind at the iron binding sites in transferrin but can also
bind at other sites in the molecule.
The stability of the Pu(IV) transferrin complex has not been determined.
Stover135 et al. concluded it had a high stability but less so than Fe(III)
transferrin. Popplewell and Boocock11*5 showed that Pu(IV) can be displaced
by citrate or DTPA.
A small proportion of plutonium may be associated with albumin and with
the gamma and other globulins (Turner and Taylor139; Stevens137 et al.; and
Popplewell and Boocock! "*5) .
22
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As summarized by Saenz and Ramos1 the distribution from the blood and
deposit in the various organs and tiss,ues are determined by the stability
of the plutonium compounds which have passed to the blood or which have
been formed by hydrolysis at physiological pH. In the case of heavily
complexed compounds, deposit takes place preferentially in the bone at a
proportion of about 80% to that in liver. If the compound has been hydro-
lyzed, the deposit takes place preferentially in the liver, at a proportion
of 7Q to 80% to that in bone.
Deposit of plutonium takes place on the surface of the bone as found by
Stover and Eyring11*7 in 1970, mainly in the cells of the endostium, and to a
lesser degree on the periostium. The selectivity for the cells of the endo-
stium is associated with the presence in those cells of a .glyeoprotein,
sialoprotein, to whose carboxylic groups plutonium is joined to form a very
stable complex (Chipperfield and Taylor11*1* and Herring11*8 et al. in 1962).
This incorporation includes mechanisms for the dissociation of the Pu-
transferrin complex at the level of the bone surface and diffusion of the
plutonium from the blood, with the changes of pH derived from the presence
of specific organic acids of the bone (lactic, citric) mainly influencing
this process.
Experiments with different species of animals and in different parts of
the skeleton in 1972 showed the nonhomogeneity in the distribution in the bone
in medullary spaces, and later, according to Jeell>9, at the base of the cranium.
Plutonium can be localized in the red bone marrow before being deposited
in the bone medullary spaces, and later, according to Jee11*9 and Erleksova150
in 1960, the plutonium mobilized from the bone deposits can be found either
recirculating in the blood, or in spaces in the bone marrow, or retained in
cells of the reticuloendothelial system.
The accumulation and retention in the medullary macrophages seem to be
associated with processes of phagocytosis and existence of the iron storage
protein, hemosiderin (Vaughn151 et al.). Their conclusion is that plutonium
reaching the blood by any route of entry, if in monomeric form, is deposited
initially in the skeleton rather than in the liver; if in the polymeric form,
it is likely to be deposited in the liver rather than the skeleton though it
may subsequently translocate to the skeleton. During their research of the
subject they concluded that little is known at present about the mechanisms
and the form in which plutonium translocates from the site of entry to the
blood stream, though experimental results suggest it is initially translocated
in the form of soluble complexes and may later take a more colloidal form.
Initially it can be expected to be deposited primarily in the skeleton rather
than in the liver. Plutonium, from occupational and fallout exposure, reach-
ing the circulation in man after some years, has been assessed as redepositing
roughly half in bone and half in liver (Taylor152).
The fractions of available plutonium which are deposited in the liver
and the characteristics of their distribution are a function of the physico-
chemical state of the compound and of the route of penetration (Saenz and
Ramos1). In general, low relations of liver/bone deposits indicate the
entrance in blood of complexed transportable compounds. High values suggest
the existence of hydrolized plutonium.
23
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By intravenous injection of complexed compounds in dogs and rabbits,
Cochran153 et al. observed in 1962 a diffuse initial distribution in all
liver structures and, later, an irregular redistribution and accumulation
in cells of the endothelial network according to the degree of polymeriza-
tion reached in their interaction with organic fluids.
With easily hydrolyzable compounds, the initial distribution is not
homogeneous, and the plutonium aggregates are localized in macrophages mainly
in peripheral zones of the hepatic lobes (Lindenbaum151f et al. in 1957).
Mechanisms of interchange between plutonium and proteins seem to be
involved in incorporation into the liver, especially processes of phago-
cytosis in redistribution.
In this respect, histological studies of dog livers in vivo (Stover and
Eyring147 in 1970) and in vitro (Bruenger136) show the existence of plutonium
associated with ferritin in the liver. This leads to the supposition that
the incorporation takes place according to the following reaction:
Pu IV-transferrin + ferritin = transferrin + Pu IV-ferritin.
The processes of phagocytosis, on the other hand, facilitate the
mobilization and interchange of plutonium between the hepatic compartment
and the Kupffer cells.
Plants
In the area of plant uptake of plutonium, the determining factors are
plant species and vigor, soil type and chemical form or solubility of the
deposited material (Romney and Davis155 in 1972 and Menzel156 in 1965).
Plutonium is tenaciously held by the soil, preventing plant incorpora-
tion, particularly if salts, acids, detergents and organic compounds are
absent (LASL37 in 1974). Soil characteristics, such as soil structure,
organic content, pH and the amount of clay present, influence the availabil-
ity of plutonium to some extent but probably no more than a factor of ten
(Romney and Davis155).
BIOLOGICAL DEPOSITION AND EFFECTS
DEPOSITION AND EFFECTS OF PU IN AQUATIC ENVIRONMENTS
When plutonium is released to surface or groundwaters it may be concen-
trated by and in plants and in silt sediments and suspended materials in the
water. The concentration of plutonium in sediments or in aquatic organisms
frequently exceeds their concentration in the surrounding water, often by
several orders of magnitude as reported by Sayre157 et al. in 1963. The
plutonium, thus concentrated, may be released suddenly at some future time
in quantities far exceeding their maximum*permissible concentrations.
The available data concerning the dissemination of plutonium in the
aquatic environment were summarized by Noshkin158 in 1971. The most studied
24
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isotope has been 239Pu derived from worldwide fallout. Essentially all the
published work has been concerned with levels in the marine environment where
Plutonium is found widespread among planktonic, pelagic and benthic organisms.
The concentrations are higher in organisms feeding on sediment or on surfaces
than in those drawing on the water itself. There is some evidence that
Plutonium concentrations are increased in organisms of high trophic levels.
Bone and liver are major repositories for plutonium in marine vertebrates
while muscle tissue of both marine vertebrates and invertebrates contain
relatively lower concentrations. In marine sediments, as in soils, plutonium
is more mobile than was originally expected. Fallout 239Pu appears to contri-
bute more than fallout 90Sr or 137Cs to the artificial radiation exposure of
many marine species.
The results of studies of the concentration of plutonium in marine
invertebrates of the North Atlantic Ocean and their ecological relationships
are presented by Noshkin159 et al. Organisms from the near-shore environment
were selected to show effects on plutonium uptake of variations in feeding
habits, association with sediment, or with absorptive surfaces and of trophic
levels. Of the invertebrates analyzed, the mussel clam, oyster and scallops
are filter feeders, subsisting on tiny organisms and organic detritus removed
from suspension. Plutonium-239 concentrations in the mussel body average
51 dpm/100 kg, a level 300 times that in seawater. The shell of the mussel
was found to have, on the average, 64% more plutonium than the same weight of
soft tissue. Fallout plutonium concentration in the mussel has increased by
a factor of 2 in 6 years, as compared to results of Pillar160 et al,,
reported in 1964. Deposition as recorded in Tokyo by Miyake161 et al. in
1970 has increased only by 25%.
The 239Pu concentration in starfish collected as they were feeding on
the mussel beds, although different in each sample, was about four times
that found in the mussel upon which each was feeding (Noshkin159). The
marine worm, Nereis, contained the highest concentration found in marine
invertebrates. This worm is a nonselective deposit feeder and ingests
quantities of surface sediment. Concentrations in other invertebrates are
also given in the report by Noshkin159 et al. Significant concentrations
of 2 Pu were also found in Sargasso weed. This weed may cycle considerable
quantities of 239Pu to specific near-shore regions.
In 1971 Wong162 et al. reported on the plutonium concentrations in
organisms of the Atlantic Ocean. The results showed that 239Pu was concen-
trated in some tissues of each organism so far examined. In fish, 239Pu
concentrations range from 0.2 to 140 dpm per 100 kg fresh weight; in benthic
invertebrates from 23 to 140 dpm per 100 kg; in plankton, from 130 to 340 dpm
per kg and in Sargasso weed, up to 1280 dpm per 100 kg.
In 1971 Patin163 et al. reported on a series of experiments performed
to study the accumulation of 23 Pu by live and dead Misgurnus Fossilis
spawn. The intensity of the accumulation was found to be related to the
phase of embryogenesis because of change in the membranes of the spawn.
The bulk of the plutonium was adsorbed on the membrane of live spawn. In
dead spawn, the adsorption of plutonium was virtually irreversible.
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Wong16"* et al. in 1970 reviewed data from a number of studies of 239Pu
uptake and retention by marine animals and sediments and the content of 239Pu
in seawater from various locations. It was concluded that most of the plutonium
released to the near-shore marine environment concentrates in sand and silts of
the sea floor and beaches.
Hodge165 et al. in 1973 found that repeated measurements of 23aPu in
several organs of albacore tuna suggest that the upper layers of the North
Pacific Ocean can retain large fractions of this nuclide for periods of a decade
or more. During the period from 1965 to 1971 the reported rate of input from
fallout decreased by about one-half in 1 year. During this same period, Z39Pu
concentrations in albacore liver decreased to one-half in about 3.5 years.
In 1974 Adams and Fowler166 placed goldfish in aquaria containing 238Pu02
microspheres. At intervals up to 302 days the fish were analyzed and tables
were presented to show alpha activity in the gills, intestine, muscles, bones,
and total body. Results are also presented for radioactivity in the aquaria
water and for radioactivity of the shell and tissues of inhabitants of the
aquaria after 185 days.
Examples of variations in bioconcentration and concentration factors for
plutonium in aquatic ecosystems are given by Kneip and Lauer167 in 1973. Pro-
blems associated with making general statements regarding concentration factors
are discussed.
Two reports covering the years 1971-72 and 1973 present the data of studies
on the plutonium concentration along freshwater food chains of the Great Lakes
(Ouchi168 et al. and Bowen and Noshkin169). Results indicate that bottom
feeding fish, e.g., shad, sucker, carp, bullhead, and rum, had higher 239Pu
concentrations than predators such as perch or bass.
Results of studies to determine the 239Pu levels in water, sediment, plank-
ton and fish samples collected from Lake Michigan were reported by Marshall170
et al. in 1972.
Gromov and Spitsyn171 in 1974 studied the change in the physicochemical
state of 239Pu due to its assimulation by phytoplankton. The stabilization
of the physicochemical form of 239Pu alters the state of plutonium in the
marine environment, which, in turn, leads to variation in the entrapment of
this element by bottom sediment and by suspended matter.
Gromov and Spitsyn172 also studied the absorption of 239Pu by a culture of
single-cell green algae and by a natural phytoplankton community. It was found
that the natural community concentrated the plutonium to a greater extent than
the pure culture did. At 15 to 17 days, the isotopes are released into the
seawater in a physicochemical form in equilibrium with the oceanic environment.
Folsom173 et al. presented data in 1972 on the concentration of 238Pu,
239Pu, 2"*°Pu in IAEA seaweed samples.
In 1971 Wong171* et al. found that seaweeds concentrate plutonium and that
seaweeds may be a sensitive indicator for the detection of variations of pluto-
nium concentration in the marine environment.
26
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Zlobin and Perlyuk175'176 in 1973, studied the photosynthesis and mecha-
nism of the action of cyanide on cell respiration and 239Pu accumulation by
marine algae. The introduction of this respiratory inhibitor into the
energy system of algae caused a response reaction in the form of a decrease
in plutonium accumulation by plant cells. It is postulated that assimilation
of colloidal particles of plutonium occurs as a result of ultraphagocytosis.
A study of plutonium and polonium inside giant brown algae is reported
by Wong177 et al. in 1972. It was found that large variations occurred
between specific tissue types. Sampling thin parts of brown algae or thin
outer layers should provide great sensitivity for detecting early changes
in the extremely small traces of plutonium that are now anticipated in the
sea from reactor effluents, nuclear fuel processing or fallout.
DEPOSITION, EFFECTS AND COUNTEKMEASURES OF PU IN SOIL, PLANT ENVIRONMENTS
Soil
A great deal of study has been done concerning the deposition, concen-
tration and mobility of plutonium in the soil of the Nevada Test Site (NTS).
Langham178 et al. in 1966 and Langham179 in 1968 assessed the problem of
plutonium contamination at NTS and elsewhere and suggested that the hazard
to man was minimal as long as particles deposited on vegetation and soil
remain deposited. In 1970 Romney180 et al. observed a slight downward move-
ment into undisturbed soil profile at NTS during the 10 years following
deposition. Although the solubility of plutonium fallout particles in the
presence of soil is poorly understood, plutonium infiltration to a depth of
12 cm was attributed to the downward movement of high density particles and
not solubilization. In 1970 Mork181 noted very similar downward movement in
the same sampling area 2 years post-detonation where plutonium was found to
be predominantly associated with >44 y particles. Price182 in 1973 review-
ed the distribution and fate of plutonium in terrestrial ecosystems and iden-
tified areas needing further study.
In 1973 Tamura183 et al., discussed studies characterizing plutonium-soil
interactions at NTS. Samples were taken to provide adequate activity levels
to permit determination of plutonium on different size and mineral fractions.
The soils were then subjected to extraction of the plutonium content by nitric
and hydrofluoric acid.
The ecological aspects of plutonium dissemination in terrestrial environ-
ments at the NTS were covered in a report by Romney and Davis155 in 1972.
Emphasis was placed upon standardization of analytical methods, delineation of
contaminated areas, problems of resuspension and redistribution, food chain
transport and ecological effects.
Anspaugh181* et al. , Eberhardt185 and Gilbert186 gave summaries of test
results and statistical analysis of soil plutonium studies at NTS. Inventory
of 239Pu and 21*°Pu at various depths in surface soil samples was determined
and results of resuspension and redistribution studies were given.
Soils of five areas located on the Test Range Complex at NTS were charac-
terized and soil profiles prepared, identified, and classified by Leavitt187
in 1974.
27
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The plutonium content of soil at Nagasaki, Japan, 24 years after detona-
tion of a nuclear device, was reported by Sakanoue and Tsuji188 in 1971- The
results indicate that plutonium contaminants in soil are not easily removed
by natural forces.
The literature regarding effects of the liquid waste disposal operations
at Hanford on the soil environment was summarized by Rautson18 in 1973. The
summary is divided into studies pertaining to: the vadose zone below a depth
of 6.1 meters (lower vadose zone); the saturated zone; and the vadose zone
above 6.1 meters (upper vadose zone). Migration of wastes discharged to the
lower vadose zone over the past 20 years by the mechanisms of diffusion,
leaching and particulate transport is discussed.
A program to examine soil-actinide relationships in sediments from a
disposal facility and characterization of actinide-bearing soils was covered
in a report by Ames190 in 1974. At least two types of plutonium were found
by autoradiographic and microprobe examination of core samples. Plutonium
particles (up to 10 urn in diameter and 60 wt % Pu02) were the most conspicuous
form. The second form of plutonium occurred in lesser concentration (<0.4 wt %
Pu02) but was found associated with silicate hydrolysis.
The isotopic analysis of soils in the vicinity of the Lawrence Livermore
Laboratory as measured in 1973 was given by Silver191 et al. in 1974.
Mass isotopic analysis of fallout in the soils of north central and
southeastern sections of Utah collected in 1971 indicates that the NTS was
the probable secondary source according to a report by Hardy192 et al. in
1972. Isotopic ratios and composition of the fallout in soil were given.
Environmental monitoring reports by Reynolds Electrical and Engineering
Company, Inc.,193 in 1969 and the National Environmental Research Center19"* in
1973 gave the soil fallout composition from testing activity as determined in
areas surrounding the NTS. Plutonium-239 soil measurements, depth profiles
and physical state were given for the Rocky Flats vicinity by Poet and
Martell86 in 1972.
In 1974 Healy195 proposed an interim standard for the upper limit of
concentration of plutonium in soils in inhabited areas. Available information
on possible sources of exposure of people living in an area where soils are
contaminated with plutonium was analyzed to derive estimates of intake. An
evaluation of protective guidelines was reported by Anspaugh184 et al.
Bliss and Dunn196 reported in 1971 on the results of studies underway to
determine plutonium in soil from areas outside the NTS. Plutonium was detected
in four locations and showed concentrations in the top 3 cm of soil that were
10 to 100 times greater than the concentration of soils in other areas.
The role of soil microorganisms in the movement of plutonium was noted
by Au in 1974. The study was designed to determine the ability of micro-
organisms to absorb plutonium, to quantify the uptake and to determine the
microbial population of soils of the NTS.
28
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The effects of soil heating by 239Pu on field flora were studied by
Krivolutskii and Fedorova198 in 1973. The results indicate a sharp decrease
in the number of soil organisms as a result of heating the medium with239Pu.
The feasibility and environmental impact of cleaning up plutonium contam-
inated areas in Nevada were discussed by Wallace and Romney199 in 1974, It
was felt correction of the damage done to the fragile environment during the
course of decontamination may require greater efforts than the decontamination.
Alternate procedures were discussed.
Plants
In 1973 Francis200 found that a survey of literature associated with the
movement of plutonium in soil and uptake in plants reveals that a major portion
of the investigations pertains to soils developed under arid or semiarid
climates.
Short-term studies summarized by Price182 in 1973 indicate less than 10%
plutonium uptake by plants. Fallout plutonium uptake by plants was studied
by Nishita2 l et al. in 1965 who reported that ladino clover uptake was very
low. Another study by Selders202 et al. in 1955 found that only trace amounts
of alpha activity were detectable in tomato plants grown in fallout-contaminated
soil, and no uptake was recorded for bean, barley or tumbleweed. In 1948
Jacobson and Overstreet203 reported that plutonium uptake by barley from
clay suspensions was greatest for tetravalent plutonium. That the sorption
of tetravalent plutonium to root surfaces from culture solutions was linear
with respect to concentrations, whereas, leaf concentrations appeared to be
curvilinear, was also noted in 1955 by Rediske2"*0 et al. The uptake into
shoot tissue by tumbleweed from solution cultures was slightly less than for
bean, barley or tomato.
In 1971 Cummings and Bankert205 used pot culture to compare the uptake
by plants of 238Pu from nine different soils. Plutonium uptake was found to
be 7 X 10~6% to 280 X 10~6% of plutonium applied.
In 1963 Wilson and Cline206 compared the uptake of plutonium from soil
by barley with that of tungsten and lead. Using a modified Neubauer technique,
it was found that uptake of Pu(IV) from an acid soil was greater than uptake
from alkaline or calcareous soils, and plutonium uptake was less than tungsten
or lead. Cline207 in 1967 reported the uptake of americium and plutonium from
two of the same soils and indicated concentration factor (CF) values [CF =
yCi/g acceptor (e.g., plant)/yCi/g precursor (e.g., soil)] of 0.003 for ameri-
cium uptake from either soil and 0.0002 and 0.0001 for plutonium uptake from
acid and alkaline soil, respectively.
Neubold and Mercer208 and Neubold209 reported that although plutonium
uptake by perennial ryegrass was low, it increased over the 2-year period
of study. It'was detectable in the third harvest of the first growing season
for one of the three soils studied (an acid soil) and the fourth harvest
showed barely detectable uptake from all three soils. Results from the next
growing season indicated that uptake from the acid soil was nearly four times
greater than the previous year's maximum. In 1970 Romney et al. studied
29
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the uptake of fallout plutonlum by clover over a long period under greenhouse
conditions. A substantially greater foliage uptake of plutonium, a seven-
fold increase, from a highly contaminated soil occurred after 5 years of
cropping as compared to the first year. It was postulated that the increase
in uptake was due to either more perennial roots coming into contact with
Plutonium particles as the plants aged or that natural organic materials
resulting from root tissue decay complexed with the plutonium and resulted
in increased uptake.
As chelates enhance plant uptake of heavy metals, the influence of
chelating agents on the uptake of plutonium was studied by Hale and Wallace
in 1970. They compared the effects of chelating agents DTPA, EDDHA and Fe-
EDDHA on the uptake of heavy metals from soil by bush beans.
Romney212 et al. reported results from studies of perennial vegetation
growing in Area 13 of NTS. Relatively uniform distributions of 239~21*0pu anci
2ttlAm were found among individual samples of the same plant species. However,
there were considerable variations in the contamination levels between differ-
ent species, presumably from superficial entrapment of resuspended particulate
material. Concentrations in Eurotia lanata were three to five times higher
than in other species sampled from the same study site. Additional studies
by Romney213 et al. were reported in 1975.
Price2lk studied tumbleweed and cheatgrass uptake of plutonium and demon-
strated that shoot uptake is clearly influenced by the chemical form of the
transuranic. Test results indicate that organic acid complexes of plutonium
such as oxalate or citrate can increase plant uptake when added to soil as
compared to uptake from dilute nitric acid solutions.
In 1972 Smith215 et al. studied the radionuclide content and botanical
composition of the diet of beef animals grazing on the Area 18 range of the
Nevada Test Site by analyzing rumen samples collected from fistulated steers.
The radionuclide concentrations were generally low with periodic increases
in individual isotope levels which could be traced to a specific contaminating
event.
Klepper and Craig216 in 1973 report studies of the interactions of pluto-
nium aerosols with plant foliage. The studies include exposure of 2-week-old
bean seedlings to 239Pu nitrate aerosols of 1 to 3 U size at wind speeds of
16.4 m/min.
When samples of foliose and fruticose lichens were collected from 27
sampling sites in the Thule, Greenland, region following the crash of a bomber
carrying nuclear weapons aboard, Hanson26 found slightly higher than back-
ground amounts of 239Pu and 21ft)Pu associated with particles of estimated 0.5 to
1.0 ym diameter.
In 1969 Alvarez-Ranies and Santos217 studied the contamination of terres-
trial gastropoda feeding on plants exposed to the plutonium aerosol from the
collision of planes carrying atomic weapons over Palomares, Spain. Plutonium
values in soil, plants and the gastropoda flesh and shell were tested and the
interacting relationships noted.
30
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ABSORPTION OF PLUTONIUM BY ANIMALS
Several possible routes of entry exist by which terrestrial animals can
incorporate plutonium into their bodies. Herbivores and small animals may
ingest radioactivity by foraging on contaminated vegetation, drinking contami-
nated water or consuming radioactive soil while eating or grooming the fur.
Inhalation may also represent an important avenue of intake for burrowing
animals and for animals living in an environment where considerable resuspen-
sion is evident. Predators, however, would probably derive most of their
intake from the consumption of smaller prey animals which contain plutonium
in their internal organs or on their pelts. Man enters into this terrestrial
food web by consuming the meat from certain sport game and domestic grazing
animals and the milk from dairy herds (LASL37). Ingestion has been considered
to be the primary route of entry involved in the food chain transport of resid-
ual plutonium in the environment (Olafsen and Larson218).
Ershov219'220 et al. in 1970 and 1971 studied the penetration of 239Pu
through the epidermis during superficial contamination using piglets. The
results, shown graphically, indicate that at the beginning, activity penetrat-
ing the skin at any fixed depths very rapidly increased. After 12 hours of
contact the amount taken up per unit time decreased and became balanced, i.e.,
the amount of the absorbed and expelled radioactive preparation was equal.
The kinetics of microdistribution in the skin and the dose distributions in
structural layers of skin are also given.
An early work by Finkle221 in 1945 considered the distribution of pluto-
nium in a dog 16 days after administration of a lethal dose of plutonium
nitrate. The skeleton contained 25% of the injected dose, liver 31%, muscle
8% and spleen 3.5%; 10% was excreted. The plasma fraction of the blood con-
tained 80% of the plutonium found therein. Studies with intravenous injec-
tion of plutonyl nitrate into mice found concentration of 27% of the dose
after 64 days. When plutonyl citrate was injected the liver content fell
from 35% to 14% on the 31st day and to 7% on the 64th day showing a half-time
value of 20 days. Mice receiving plutonyl nitrate intramuscularly had liver
retention that showed the same 20-day half-time. Plutonyl citrate injected
into the peritoneal cavity of mice was slowly absorbed with a concentration
occurring in the femur and liver; plutonyl nitrate, intraperitoneally, behaved
similarly but was somewhat more slowly absorbed and therefore, was retained
longer by the liver.
In 1948 Hamilton222 noted that plutonium is not absorbed to any signifi-
cant degree by way of the digestive tract. The metabolism of plutonium follow-
ing intramuscular injection is essentially the same after administration as
Pu , Pu+tf and Pu+6. He suggests that plutonium is converted by the body into
one valence state regardless of the valence administered.
Results of the biomedical program in conjunction with the 1957 "Operation
Plumbbob," were reported by Stannard13 in 1973. The primary purpose of the
program was the direct determination of the uptake and retention of plutonium
by a variety of animals as a function of time of exposure and the relation
of the amounts found to air and ground levels. There were two major phases
and groups of exposed animals—those exposed during cloud passage and those
31
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exposed during long-term post-event periods. Rats and dogs were used in the
former; dogs, sheep and burros for the latter. For the cloud passage phase,
animals were placed from 164 to 656 meters downwind from Ground Zero. For the
resuspension phase the animals were placed in areas with levels of ground
contamination of 2.6, 40 and 560 micrograms per square meter of desert floor
soil. The animals remained in place for periods ranging from 4 to 160 days.
The plan was to measure the accumulation of plutonium in the lung and other
tissues as a function of time and various aerosol parameters.
The dogs exposed to the cloud passage at the time of detonation showed
generally higher burdens than the animals exposed to resuspended plutonium,
even though the former were not at the range of maximum airborne concentra-
tions at ground level. There was no appreciable increase in lung burden
with time and very little difference in burden in animals placed at several
different surface contamination areas. This may have been difficult to
ascertain as radiochemical analysis at that time lacked sensitivity for very
low levels .
Results reported from Operation Roller Coaster have not all been
declassified at this time but what is available is included in papers by
Wilson and Terry16'17 and Stewart223 et al. The initial lung concentrations
for dogs, sheep and burros were very similar despite wide differences in lung
size, etc. There was, however, a marked difference in clearance pattern among
the three species. The lung clearance for the dog closely resembles that
found in laboratory studies with inhaled
A review of the comparative metabolism of radionuclides in mammals was
published by Stara22"* et al. in 1971. They note that the rate of absorption
through the gastrointestinal tract was low when 239Pu was given to rats.
Katz and Weeks225 reported absorption was 0.001-0.004%. Plutonium-239 (N03K
orally administered to rats was found to be absorbed between 0.002 and 0.003%,
with a maximum of 0.009%. Carritt226 et al., demonstrated in 1947, that the
amount absorbed is related to the dose; with a lower dose, the absorption was
0.30%, whereas with a dose approximately tenfold higher, the absorption was
decreased to 0.01%. Absorption of 239Pu (N03)i, given orally to swine was
reported as 0.002% by Weeks227 et al. in 1956. Inhaled 239Pu02 in dogs was
absorbed in a range from 0.1 to 16.9% with a mean value of 3.7% as calculated
by Morrow228 et al. in 1967.
In 1972 Kashima229 et al. conducted studies to clarify the relation between
the physicochemical form of plutonium and its distribution in all organs and
tissues after subcutaneous injection in mice. The forms used were monomeric
plutonium with pH adjusted to 1, 4.5, 7.2, and 13.0 immediately before injec-
tion; and polymeric plutonium solution with its pH adjusted to 9.0. After
subcutaneous injection of the monomeric form,-239Pu remained mostly at the
injected site for the 56 days studied. Concentration of plutonium in bone
increased with time, the level of plutonium in liver, especially around the
central vein, was relatively high in the initial 3 days, but was lower at 21
or 56 days. The distribution pattern was only slightly affected by changing
pH or time prior to injection after preparation. With polymeric plutonium,
however, relatively low plutonium concentrations were observed only in the'
bone and liver.
32
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Ballou et al, in 1972 found that about 0,08% of an oral dose of 239Pu
citrate was retained in dogs after 3 days, distributed mainly between skeleton
(50%) and liver (25%). After intravenous administration the liver retained
32 to 45%3
-------
at generally comparable, decreasing rates. Polymeric plutonium was as much as
10 to 30 times more concentrated in predominantly red (erythropoietic) marrow
than in fatty marrow. Monomeric plutonium was 1.3 to 2,8 times more concen-
trated in the red marrow. Mice injected with the same plutonium solution as
the rabbits showed, in comparison, a higher percent of the injected monomeric
Plutonium in the femurs and a lower percent in the liver; they showed a higher
uptake of polymeric plutonium in the marrow and a higher uptake of both forms
in the spleen and lungs than did the rabbits.
\ 9 3 Q
In 1974 Zapol'skaya235 et al. intravenously injected male rats with Pu
chloride salt solution and determined the biological half-life in various
tissues, organs and albumin proteins. The results indicated that the exchange
of plutonium is determined by the exchange of the albumins with which they
form bonds.
Durbin236 et al. constructed a kinetic model to describe the transport
and deposition of intravenously injected Pu(IV) citrate in the rat.
The implications of the solution of the model led to the following working
hypothesis: (a) Unbound plutonium reacts with protein, presumably transferrin,
in extracellular fluid compartments as well as in plasma. The Pu-transferrin
complex is the most likely form in which orally administered plutonium is
carried once it reaches the plasma. (b) Little, if any, protein bound plutonium
is excreted or deposited in the liver. Formation of the Pu-transferrin complex
is probably not necessary preliminary to liver deposition of diffusible pluto-
nium. (c) Both unbound plutonium and bound plutonium are sources of plutonium
deposited in bone. The surface of the reticulocyte (where iron is released
from the Fe-transferrin complex) is considered the most likely site of dissoci-
ation of the Pu-transferrin complex.
j-.
A good review of the metabolism of monomeric and polymeric plutonium in
small animals and the radiotoxic implications for man was prepared in 1971
by Lindenbaum2 3 7.
Matsuoka 38 et al. compared autoradiograms obtained from animals admini-
stered monomeric or polymeric plutonium. Results were compared with those
obtained from animals administered metabolically stable reference particles
of known particle size. It was found that the behavior of plutonium soon after
injection is largely influenced by its particulate character rather than by
its chemical nature. Results following inhalation of a plutonium nitrate
aerosol showed no obvious translocation to the liver, despite the water solubil-
bility of the nitrate form. The initial uniform distribution of inhaled pluto-
nium changed to a nonuniform distribution after 3 months.
Baxter and Sullivan239 studied the gastrointestinal absorption and reten-
tion of plutonium chelates administered to rats. They found the intestinal
absorption of plutonium nitrate is increased about 700-fold when chelated with
DTPA. Within 2 days, virtually all of the absorbed plutonium-DTPA complex is
excreted in urine. Thus, plutonium retention in the liver and skeleton is
quite low, but more than twice as high as when DTPA is not present. Citrate
is less effective than DTPA in increasing absorption, but more effective in
increasing retention.
34
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In 1972 Mays^and Dougherty2"*° reported results of beagle studies, The
initial distribution of plutonium was uniform throughout beagle liver follow-
ing intravenous; injection of monomeric plutonium in citrate solution. Most
of the initial burden appeared in the hepatic cells.
Subsequently, much of the activity shifted into the liver reticulo-
endothelial cells lining the sinusoids; the rate of translocation was great-
est at the higher dose levels, presumably due to release of the nuclide from
cells killed by the irradiation. At very high doses, the skeletal burden may
actually increase due to the amount released from the liver. At long times
after injection the nuclide distribution is very nonuniform within the liver,
being highest in the portal region and lowest in regenerative nodules that
grow after the time of injection. In the lower-level 239Pu beagles, the net
liver burden remains roughly constant at about 30% of the injected activity
for about the first 1,000 days after injection. The loss of liver 239Pu during
this period is at least, in part, compensated by the influx of 239Pu released
from the skeleton. After 1,000 days, the liver burden at the lower levels
decreases with a half-time of about 8 years.
Placental transfer of 239Pu in rats and mice has been reported to be
inversely related to the size of dose given to the dam, (Finkel21*1 in 1947,
Wilkinson and Hoecker21*2 in 1953) with maximum transfer of 3 to 8% of the
dose, when the dose was given about 1 week after conception. Detectable
amounts of Pu were found in milk of mice, rats and cats after administer-
O it 0
ing plutonium to the lactating dam. A more recent study by Ovcharenko in
1971 showed that when pregnant rats were administered Pu-citrate intravenously
on the day of birth and then allowed to give birth and nurse their young, the
lactation did not significantly reduce the content of plutonium in the organs
of the lactating mothers. Sacrifice of the mother rats after 1 and 10 days
indicated 84.4% and 96.4% of the administered activity was retained in the
body. The content of 239Pu in the entire litter of baby rats fed by treated
mothers from 1 to 10 days of age was 4.24 to 7.36% of the amount introduced.
After 20 to 30 days 1.44 to 2.32% remained in the bodies of the baby rats.
In 1972 Sikov and Mahlum21*11 reviewed the deposition and retention of pluto-
nium in immature, developing animals. The absorption of 239Pu from the gastro-
intestinal tract of juvenile rats and dogs relative to absorption in adults was
shown graphically. As would be expected, the graph shows enhanced uptake of
plutonium from the gut of the neonatal rat and dog is about 100-fold greater than
in the adult of these species, with a gradual decrease to adult values to about
the time of weaning.
Ballou21*5 reported in 1958 that age appears to have a direct effect on
absorption in rats. He noted 0.25% absorption of 239Pu nitrate at 1 day of
age, decreasing to 0.10% at 7 to 13 days of age, 0.02% at weaning and 0.003%
in adult animals.
Finkel21*6 in 1947 indicated that the absorption of plutonium bound to
protein, as in milk, may be as much as 20-fold greater than in the uncombined
form. This might increase the hazard to juveniles whose diet is primarily
milk. On the other hand, McClellan2"7 et al. in 1962 reported there are
discrimination processes, which result in the concentration of plutonium in
35
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breast milk being substantially lower than that in the diet or the plamsa of
the mother.
Sikov and Mahlum21"* indicated that there is a possibility that there is
greater hazard to the gastrointestinal tract from ingestion of insoluble
Plutonium in the infant than in the adult. It has been shown that the gastro-
intestinal passage time of particles in juvenile rats does not differ from
that in adults, although the average rate of passage is substantially reduced
and there is evidence of prolonged retention in the stomach and ileum. This
results in an increase in the average time that the plutonium is in contact
with any given segment of the tract, and a corresponding increase in the
radiation dose in the young, which is further increased because of the smaller
organ diameters.
Sikov and Mahlum2"*1* also found that at 1 day after injection into
adult rats, a much greater fraction of polymeric than of monomeric plutonium
was localized in the liver. In the femur, the initial deposition of mono-
meric plutonium was much higher than that of polymeric. In the newborn
there was an equal fraction of the administered dose of monomer and polymer
in the femur at 1 day after injection and the concentration of the two forms
in the liver were more similar than in the adult. With the passage of time,
the monomer was removed from the liver of both age groups and the polymer was
retained. This retention was more marked in the adults than in newborns,
while the initial redistribution of plutonium from liver to bone was more
marked in the juvenile rat than in the adult. As a result, at 30 days and
again at 90 days, the patterns of partition of the two forms of plutonium
were not markedly dissimilar in either the animals injected at birth or as
adults. Buldakov 21f 8 et al. in 1970 found similar patterns in studies on
lambs.
The interpretation of data on immature animals is complicated by the
fact that the size of individual organs or organ systems relative to that of
the total body changes during development. Sikov and Mahlum21*1* summarized
the changes in the size of various organs with age. They also found that
although the adult and newborn rat had a similar fraction of administered
polymer in the liver at 1-day after ingestion, the corresponding concentra-
tion in the liver of the newborn was 20-fold that in the adult. In the adult,
the concentration of polymeric plutonium in the liver decreased by about half
in the first 90 days after injection; in the newborn, the dilution produced
by growth resulted in an 80-fold decrease in concentration. At both ages
there was a net increase in the fraction of the dose in the femur. This
resulted in a slight increase in concentration in the adult, while there
was a 20-fold decrease in the newborn. It is therefore evident that age
at the time of injection influences the total radiation dose as well as
the temporal distribution of the dose.
Incorporation of 239Pu into the hair of rabbits was reported by
2^9
Jaworowski et al. in 1971. They found that when doses of 0.1, 1.0 and
10.0 yCi of Pu chloride, dissolved in 0.5% phenol, pH 5.5, were injected
subcutaneously into red-haired New Zealand rabbits, the mean incorporation
of 239Pu in the anagenetic hair of the first fleece (grown 22 days after dosing)
ranged from 1.22 X 10" to 2.73 X 10"3% of the dose per gram of hair. There
appeared to be an inverse relationship of percent incorporation to dose
amounts. Twice as much was incorporated at the 0.1 yCi per animal, as
36
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at 1.0 and 10.0 yCi per animal. In the growth of the second fleece, the
rate of incorporation was 10 times lower at 10,0 yCi than at the lower
doses. At the dose levels studied, the amount in hair was similar to that
in muscle but much lower than bone or liver.
A recent report of the biological effects of plutonium in experimental
animals was presented by Bair in 1975.
BIOLOGICAL BEHAVIOR OF INHALED PLUTONIUM IN ANIMALS
Airborne plutonium particles are similar to most other particles when
they are inhaled in that deposition in the respiratory tract is primarily
dependent upon the physical properties of the particles and the respiratory
characteristics of the individual inhaling the particles. After deposition
in the respiratory tract, plutonium may be retained in the lung for a long
time, be translocated to other tissues in the body, accumulated in the lymph
nodes associated with the respiratory tract or excreted in urine and feces.
The actual deposition 'of inhaled plutonium depends largely upon the physical
and chemical characteristics of the inhaled material (Bair251 and Lafuma252).
Bair251 reviewed the literature in 1974 and presented figures and tables
showing lung clearance and translocation values of several investigators. He
notes that within the first week after exposure, a fraction of the deposited
plutonium is cleared from the respiratory tract and excreted. In the case of
PuOz inhaled by beagle dogs, all plutonium cleared from the respiratory
tract is excreted in feces except for a small fraction that may be solubilized,
absorbed into the circulating blood, and either cleared by the kidneys or
deposited (by the blood) in another tissue. The magnitude of the fraction
cleared within the first week depends upon the fraction of readily soluble
material present and also upon the distribution of the deposited plutonium
within the respiratory tract. Plutonium particles deposited on the ciliated
epithelium of the upper respiratory tract are trapped in mucus, propelled to
the esophagus and swallowed. Plutonium deposited in the lower regions of
the lung, in the alveoli, is not available for clearance and may be incorpor-
ated into the cellular structure of the lung and retained for a long time.
The clearance of plutonium deposited in the lower lung is generally assumed
to be exponential over a reasonably long period of time.
Bair251 gives retention half-times of several plutonium compounds. The
retention half-times for organic complexes of plutonium, plutonium nitrate
and fluoride range from less than 100 days to about 300 days in rats and dogs.
The retention half-times for Pu02 are substanially longer, ranging from 200
to 500 days in rats, and from 300 to 1000 days in dogs. The wide range of
values observed in dogs is largely due to extensive experimentation with a
variety of plutonium oxides with different particle size characteristics.
Studies with 238Pu02 in dogs indicate a much shorter lung retention time than
is observed for 239Pu02. This appears to be due to instability of 238Pu02
particles, possibly caused by radiolysis in tissue fluids.
In 1970 Bair253 presented figures showing the relationship of particle
size and isotope on retention of plutonium in lung as well as for oxides
prepared under different conditions. Oxide prepared by calcining the oxalate
37
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at 1000° C was retained with a half-time of 650 to 950 days compared with 300
to 400 days for the oxalate calcined at 350° C. Oxides prepared from metal
powder at temperatures of 123° C to 450° C were retained in lung longer than
the low-fired oxalate. Small particle size high-fired oxide was retained with
a half-time of 400 to 500 days, compared with half-times up to 900 days for
the larger particle size high-fired oxide. Retention of the small particle
size 238Pu02 was less than for the comparable 239Pu02.
Plutonium may be removed from lung via bronchial and tracheal mucociliary
processes and excreted but this accounts for only part of the plutonium cleared
from the respiratory tract. Another fraction is accumulated by the lymphatics
and deposited in lymph nodes. Data from an 11-year study with beagle dogs were
presented by Park25" et al. in 1972. After 5 years both lung and thoracic lymph
nodes each contained 30% of the plutonium initially deposited in the lower
respiratory tract. After 11 years the lung burden had decreased to about 9%
and the thoracic lymph nodes had increased to 40%. Translocation of plutonium
from lung resulted in levels in liver of about 10% of the alveolar-deposited
plutonium, in bone of about 5% and in the abdominal lymph nodes of about 7%.
The relative distribution among body tissues of plutonium translocated
from lung is essentially the same for all plutonium compounds. In beagle
dogs, within several months after inhalation of plutonium nitrate, the fraction
remaining in lung decreased to 40% or less of the amount deposited in the
lower respiratory tract according to Ballou et al. in 1972.
Translocation from the lung resulted in bone accumulating about 30% and
liver about 10% of the alveolar-deposited plutonium. A small percentage was
found in spleen, lymph nodes, and the soft tissues and the remainder was
excreted in urine and feces.
Data presented by Park255 et al. in 1973 showed that 238Pu02 may be
cleared from lung more rapidly than 239Pu02- It has also been found that
translocation of 239Pu from lung to other tissues in the body may be greater
than for 238Pu.
Distributions of plutonium in tissues of beagle dogs 5 years after inhala-
tion of 238Pu02 and 239Pu02 are also compared by Park25 et al. Both oxides
were calcined at 350° C. The particle size of 238Pu02 was 0.1 pm (CMD) and of
239Pu02 was 0.1 to 0.5 ym (CMD). The ultrafilterability was 1 to 2% for the
238Pu02 and <1% for the 239Pu02. After 5 years, only 10% of the body burden
of the 238Pu was in lung compared with 46% for 39Pu. Accumulation in thoracic
lymph nodes was 3 times greater for 239Pu than for 238Pu, however, the bone
burden of 238Pu was 12 times that of 239Pu. This illustrates that the behavior
of 38Pu02 in the body may differ significantly from that of 239PU02.
In 1972 Craig256 et al. exposed beagle dogs to 239Pu02 aerosols as part
of a low-level effects study of the oxides of both 238Pu and 239Pu. The alveo-
lar deposition of 239Pu02 aerosols was measured as a function of the aerodynamic
particle size distribution of the aerosol and the tidal volume of the dog during
exposure.
Matsuoka257 et al. studied the distribution of plutonium nitrate aerosol
by rats. Rats sacrificed immediately after exposure showed deposition in the
-------
tracheo-bronchial and pulmonary region. One day after exposure, plutonium
was mainly in the lung with very small amounts in the intestine. One month
after inhalation, the plutonium deposited in the lungs still remained, with
very small amounts translocated to the trabecular bone of the vertebra and
to the ileum. Isolated lung specimens showed no deposition in the tracheo-
bronchial region and very little deposition in the pulmonary region.
In 1972 Suzuki258 et al. also exposed rats to submicron aerosols of
plutonium nitrate and determined the retention and excretion. Excretion of
plutonium was mainly observed in the feces on the first day following inhala-
tion and the daily fecal excretion decreased to 1/40 to 1/100 of the total
intake of plutonium on the third day and thereafter. The urinary excretion
was less than 1/10 of that of the feces.
Ballou259 et al. studied the deposition of inhaled 239Pu citrate in dogs
and found that 239Pu reached a peak concentration in blood after 6 hours, then
decreased with clearance kinetics similar to intravenous administration. One
day after exposure the lung, skeleton, liver, blood and intestines retained
most of the inhaled 239Pu. After 100 days 36% of the initial deposit was
retained; 33% in the lung, 44% in the skeleton and 17% in the liver. Although
the concentration in specific lymph nodes (hepatic, splenic, and tracheo-
bronchial) was among the highest of any tissues analyzed, the total amount
deposited in a selection of 12 lymph nodes (~10 g tissue) was always less
than 0.6% of the body burden.
Wandall260 reviewed the mechanisms involved in the lung clearance of
inhaled 238Pu02 and 239Pu02 aerosols in dogs and rats and the subsequent
translocation of the solubilized fraction throughout the body.
Dionne and Sanders261 found that 239Pu02 particles inhaled by rats were
deposited in alveoli and rapidly phagocytized and concentrated within pulmonary
macrophages. A hybrid computer alveolar model was developed in order to demon-
strate the distribution of alpha energy in the alveoli and the modifying
influence of pulmonary macrophages on the alveolar alpha-energy from phagocy-
tized particles.
BONE DEPOSITION
Atherton262 et al. administered 239Pu(IV) intravenously to beagles in:
(1) the Pu-transferrin complex, (2) the 0.08 M citrate buffer and (3)as a
suspension of near colloid size particles at pH ~6. The skeletal retention
of plutonium, when injected in a monomeric form, is 50% of the injected dose.
The retention of polymeric plutonium in the skeleton was less than 1/20 that
seen in monomeric or transferrin complexed plutonium at comparable times.
The uniformity of skeletal distribution of polymeric plutonium from bone to
bone is markedly less than that seen with the two monomeric forms. Reduced
skeletal retention in animals injected with polymeric plutonium indicates a
different skeletal retention mechanism in animals injected with polymeric
plutonium. The authors postulated that skeletal retention of the polymer is
not associated with bone per se but likely increases with the amount of red
marrow a bone contains.
39
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Stover263 et al. reported the retentions of plutonium in the humerus and
third lumbar vertebra, of dogs injected with 0.016, 0,048, and 0.095 yCi/kg
239Pu. The dogs survived from 1600 to 5200 days after injection, The data
show that the rate of decrease of retention is greater during the first 2
years than at later times. There appear to be two phases in the time depend-
ence of skeletal retention. Two things are happening during the first years
after injection. Both the rates of the remodeling processes which remove
plutonium from the bone surfaces and the fraction of skeletal plutonium that
remains on the surfaces are decreasing. Both of these factors contribute to
a decreasing loss of plutonium from the skeleton. The remaining plutonium
which has been buried during the remodeling of the bone is much less access-
ible and is lost from the skeleton only at a very slow rate, if at all.
Another 1972 report by Stover 26l( et al. compared the skeletal and hepatic
dose rates from intravenously injected dogs. Young adult dogs were administer-
ed 0.0059 yCi 239Pu(IV)/kg in 0.08 M citrate buffer, pH 3.5. The dogs were
sacrificed at 1648 and 2546 days. The cumulative rad doses to the skeleton
and liver were compared and the results show that the average dose to the liver
exceeds that to the skeleton, except at the 2.8 UCi/kg dose level, after 1300
days.
1 J. Q
In 1972 Jee found that the effectiveness of the various routes of
administration in delivering plutonium to bone, in decreasing order is:
intravenous>intraperitoneal>subcutaneousIntramuscular>inhalation>oral>direct
application upon skin. Reticuloendothelial cells in the marrow compete with
bone for polymeric plutonium and thus decreases the plutonium available for
bone surfaces. The uptake in young and adult bones differed by a factor of
two. The fate of the plutonium surface deposits is modified by bone growth,
modeling and remodeling in growing animals and remodeling in adults. These
age-related processes remove the plutonium from bone surfaces and/or bury
the surface deposits with new bone.
A very complete summary of the metabolism of plutonium after administration
in different forms and by different routes up to 1972, is given in tabular form
in the International Commission on Radiological Protection (ICRP) Publication 19265.
BIOLOGICAL EFFECTS OF PLUTONIUM IN ANIMALS
In animal experimentation, the acute forms of toxicity are manifested
by an irradiation syndrome comparable to that produced by a total irradiation
with x-rays- Forms of a chronic nature can produce broncho-alveolar tumors
in the lung, bone cancers, and bone fractures in the skeleton, and, with less
frequency, liver tumors. Saenz and Ramos1 present lethal and tumor-causing
doses of plutonium in dogs, rabbits and mice.
It has been shown that the distribution of plutonium and the radiation
dose among the tissues in the body will vary depending upon the physical and
chemical characteristics of the plutonium inhaled. The biological effects
that occur will depend upon the radiation exposure and the relative radia-
tion sensitivity of each tissue into which plutonium is transported and
deposited. These are primarily blood, bone, liver, lung and lymphatic system.
4Q
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Blood
Plutonium is cleared from the circulating blood within a few hours after
absorption. Therefore, the effects seen in blood cells are probably due to
irradiation of hematopoietic tissue in which plutonium is deposited or to
irradiation of blood circulating through plutonium-containing tissues.
In 1972 Dougherty266 reported blood cell alterations in dogs receiving
a single intravenous injection of a wide range of dose of 239Pu (0.016 to
2.8 yCi/kg). Dogs receiving the four highest dose levels showed changes that
were dose-dependent and were most marked in granular leukocytes which were
maximally depressed at 2 to 3 weeks post injection. A sustained lymphopenia
occurred at the two highest dose levels. A transient early thrombocytopenia
and anemia were also found in higher level dogs. A moderate anemia reappeared
as the animals became terminal.
In 1972 Nabors267 noted that beagles bearing 239Pu burdens show the most
marked alterations in serum alkaline phosphatase and serum glutamic oxaloacetic
transaminase and serum glutamic pyruvic transaminas.e. Animals with low dose
levels appear to have a much longer latent period prior to the appearance, of
altered serum biochemistry than do animals with higher dose levels.
Bone
The most sensitive effect of plutonium deposited in bone is radiation-
induced osteogenic sarcoma. Because plutonium deposits on bone surfaces,
a large fraction of the alpha energy is absorbed in sensitive cells. Although
osteogenic sarcoma has been reported in rats that accumulate doses of less
than 10 rads, statistically significant increases in tumor incidence have not
occurred at doses less than 30 to 50 rads (Bair250). The available data suggest
that the dose-effect curve for dogs is different from that for rodents. Mays
and Lloyd258 conclude that the incidence of plutonium-induced osteogenic sarcoma
is 0.38%/rad for beagle dogs, 0.10%/rad for mice and 0.06%/rad for rats.
n q n
No bone sarcomas have been reported in dogs following PuOa inhalation
but they are the important late biological effects in dogs which have survived
intravenous injection of plutonium citrate for more than 3 or 4 years (Mays
et al.).
Osteogenic sarcoma has been observed in mice, rats, rabbits, and dogs
after intravenous injection of several 239Pu compounds including organic
complexes and plutonium nitrates.
Osteogenic sarcoma has also been observed in rats after inhalation of
238Pu02, but has not been reported in any animal species after inhalation of
239Pu02.
In 1973 Moskalev and Strelt'sova270 found that optimun osteosarcomogenic
doses to rat skeleton were in the range of 0.7 to 1.8 krads for 239Pu. The
osteosarcoma incidence was identical for both male and female rats but signifi-
cantly age dependent for each sex.
41
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Pesternikov and Bukhtoyarova27* discussed the quantitative assessment of
osteosarcoma growth rate in rats following a single intraperitoneal administra-
tion of 2.5 mCi/kg of 239Pu citrate. Osteosarcomas are shown not to predomi-
nantly originate at the sites of the highest isotope concentration. Of some
tumors, primary multiple growth was characteristic. Possible extrapolation for
determining the osteosarcomas development time was noted.
James272 reported a study in which 6 to 8 week-old rats were given a
single injection of 4.5 yCi/kg soluble Pu(N03K, a dose level expected to give
an approximate 80% yield of osteosarcomas. Localized dose rates were measured
at fixed reference distances between 5 to 20 ym from bone surfaces by counting
gamma-flux entering small cylindrical targets located in a thin nuclear emul-
sion in contact with a bone section. Dose rates 1 day after the injection
ranged from 22 to 57, 12 to 37, and 7 to 26 rads/day at distances of 5, 12.5,
and 20 ym, respectively, from a number of different endosteal surfaces. These
local dose rates changed with time by factors of the order of 2, in either
direction, depending on the prevailing conditions of remodeling. A cumulative
alpha dose of about 2000 rads (delivered to primitive cells at trabecular
surfaces over a period of 36 weeks) may be associated with a 10% probability
of developing a tumor in an individual femoral epiphysis. Taylor 73 et al.
studied the general syndrome induced by 239Pu(IV) injected intravenously in
beagle dogs. The most critical factors were the induction of bone cancer,
hematopoietic changes and liver lesions. Some of the less serious end points
were pathological fractures, dental changes and atrophy of the turbinates.
These latter conditions produced functional impairment in only part of the
dogs and principally at the higher dose levels.
Taylor and Mays271* gave young adult St. Bernard dogs a single intravenous
injection of Pu, because of their high spontaneous incidence of bone cancer.
The appearance time of radiation induced osteosarcomas in this giant breed
was approximately one-half of that observed in beagles when both were injected
with 0.3 yCi 239Pu/kg of body weight.
In 1972 Moskalev275 reviewed the results of studies by Soviet scientists
on problems of the biological action of 239Pu. Main attention was given to the
analysis of late effects (tumor and nontumor effects) developing in the body
as a result of injury by 239Pu, dose-effect curves for bone and luiig tumors,
estimation of minimum carcinogenic dose levels, and determination of doses
not affecting the natural life span.
Liver
Liver accumulates levels of plutonium similar to bone. However, liver
tumors have not been a common finding in experimental animal studies. Bile
duct tumors have been observed to occur in beagle dogs at doses as low as
60 rads. However, not only was the incidence very low, but bile duct tumors
also occurred in control dogs (Taylor276 et al.).
Kashima277 et al. demonstrated in 1973 that liver function at 21 days
post exposure was markedly reduced in rats injected with 239Pu at birth or
at 7 days of age. The differing effects produced by monomeric and polymeric
plutonium were explained by differences in radiation dose to the liver.
42
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Lung
Inhalation of relatively soluble plutonium compounds, such as organic
complexes, plutonium nitrate and plutonium oxide, has resulted in primary
pulmonary neoplasia in rodents, rabbits and dogs (Bair25i).
Pulmonary neoplasia has also been observed in beagle dogs, baboons
(Metivier278 et al.) and rodents after inhalation of 239PuO . Tumors were
observed in animals that had lung doses less than 10 rads. Statistically
significant increases in pulmonary neoplasia occurred at doses of about
30 rads and above. In several experiments, increased incidences of lung
tumors occurred at doses between 10 and 100 rads. In an 11-year study of
239Pu02 in beagle dogs, nearly all animals which had depositions of between
about 3 nCi and 50 nCi per gram of lung had lung tumors. Dogs which had a
deposit of more than 50 nCi per gram of lung died early due to radiation
pneumonitis and fibrosis (Park251* et al.). The mean dose to the lungs of
the dogs that developed neoplasia ranged from 1200 to 4000 rads. As in the
case of osteogenic sarcoma, the dose-effect curve for pulmonary neoplasia
in dogs appears to differ from the rodent dose-effect curve.
Howard279 described the results of a long-term study to evaluate the
pathologic effects in the lungs of beagle dogs following 239PuO particle
inhalation by 40 dogs exposed to 239Pu02 particles having a CMD of 0.1 to
0.5 ym; 22 died with primary lung neoplasia 38 to 110 months post exposure;
8 died of pulmonary fibrosis; 5 were sacrificed for radionuclide distribution
measurements; and 5 were still alive over 9 years post exposure. Initial
alveolar deposition ranged from 0.5 to 3.5 yCi and accumulated radiation
dose was 2500 to 12,000 rads. Most lung tumors were found to be bronchial-
alveolar carcinomas of peripheral origin, with two peripheral squamous cell
carcinomas and three epidermoid carcinomas. Also in this group of dogs
there were three thoracic sarcomas and two with malignant lymphomas-
Sanders and Park280 and Sanders281'282 reported on the carcinogenicity
of inhaled 238Pu and 239Pu in soluble and insoluble forms by rats and dogs.
It was concluded that exposure of rats to even small amounts of 238Pu resulted
in significant incidence of tumors in lungs. The type of metaplasia and neo-
plasia in rats and dogs indicates the epithelial, either alveolar or bronchi-
olar, origin of most of the observed tumors.
Anderson283 et al. reported on lung_irradiation of Syrian (golden) ham-
sters with static plutonium microspheres. Exposure was accomplished by inject-
ing 10 ym microspheres into the jugular vein. The microspheres were trapped in
the capillary bed of the lung. Activity range was 0.01 to 59 pCi/sphere. Of
1,142 hamsters exposed to 5,700,000 microspheres, only two lung tumors were
observed. Although the experiment was not complete at the time of the report
the authors felt that the volume of tissue irradiated was an important factor
and that locally concentrated alpha irradiation is less damaging in the hamster
lung than the. same amount of energy delivered over larger volumes.
Lymph
Plutonium accumulates in lymph nodes following deposition of plutonium in
the respiratory tract. Months or years after the contaminating event, lymph
43
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nodes may attain concentrations of plutonium many times the average concentra-
tions remaining at the site of deposition and consequently the accumulated
radiation dose to lymph nodes may be greater than to any other tissue.
Although dogs have been studied for 11 years after inhaling a variety
of plutonium compounds, primary neoplasia of lymphatic tissue has not been a
common observation (Bair 53). Metastases of tumors from lung to lymph nodes
have occurred, but none has been the primary cause of death. It can be
concluded from the many rodent and dog life-span experiments with 38Pu and
239Pu, in which many lymph nodes have been exposed to doses ranging from near
background to thousands of rads delivered at a wide range of dose rates, that
the lymph nodes are not especially susceptible to the carcinogenic action of
alpha radiation from plutonium.
Dagle284 reported on lymph node clearance of 239Pu02 administered as
insoluble particles from subcutaneous implants in adult beagles to simulate
accidental contamination of hand wounds. The popliteal lymph nodes were
monitored following implantation ranging from 9.2 to 39.4 uCi 239Pu02 into
the hind paw. Groups of dogs were sacrificed 4, 8, 16, and 32 weeks later
and it was found that the popliteal lymph node contained from 1 to 10% of
of the implant dose. Histopathologic changes in the popliteal lymph nodes
with plutonium particles were characterized primarily by reticular cell hyper-
plasia, increased numbers of macrophages, necrosis and fibroplasia. Eventu-
ally, the plutonium particles became sequestered by scar tissue that often
replaced the entire architecture of the lymph node. There was slight clearance
of plutonium from the popliteal lymph nodes of dogs monitored for 32 weeks.
Other Effects
f\ Q |-
Stover et al. found correlation between dose level and life-shortening
in beagle dogs. Sikov and Mahlum21*1* found that 12 yCi/fcg of 239Pu, which is
well below the acute lethal range for the adult rat, produces extensive
prenatal death within 3 to 5 days when administered to the pregnant rat at
9 days>of gestation. There was evidence that-these deaths-occur by alterations
of the nutritive function of the fetal membranes. In contrast, no prenatal
mortality is produced at doses beyond the lethal level for the mother,
150 nCi/kg, if administered at 15 or 19 days of gestation. In 1972 Ovcharenko286
found similar results when studying the effects of plutonium on reproductive
ability of rats. He found that the character and depth of radiation-induced
changes depended upon the amount of activity injected and the time elapsed
since injection.
In the course of investigating the postulated development of the offspring
of experimental animals, a number of peculiarities were observed: decrease in
viability, delayed physical development, variations in weight, disturbance of
blood formation, change in radiosensitivity and depression of sex function.
/
Sanders287'288 and Sanders and Jackson289 studied the synergistic effects
of plutonium and asbestos administered to rats. It was found that coadmini-
stration by inhalation of 239Pu02 with asbestos resulted in less excretion of
239Pu than was the case with 239Pu02 only. Focal granulomatous lesions were
common around bronchiolar areas of the lung in animals receiving asbestos.
Plutonium oxide particles tended to concentrate in these asbestos-induced
44
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lesions forming hot spots of alpha activity. When the same combination was
intra-abdominally injected into rats, asbestos acted in an additive manner with
Pu02 in inducing mesotheliomas, the two agents combined having an effect
equal to the sum of their effects when administered separately. A similar
additive response was found when benzpyrene and 239Pu02 were injected with
resulting formation of abdominal sarcomas.
COUNTEKMEASURES FOR PLUTONIUM IN ANIMALS
239 A number of chelating agents have been used in experiments to remove
Pu by increasing the excretion rate. Smith290, as reported in 1958,
testing 10 of the amino-acetic acid-type chelators administered intraperi-
toneally in a dose of 1.5 mM/kg in an equivalent amount of calcium gluconate
1 hour after intravenous injection of 239Pu to rats. The most effective agent,
diethylene-triamino-pentaacetic acid (DTPA), decreased deposition of plutonium
in the liver and bone by about 99%; the next most effective, diamino-diethylether-
tetraacetic acid (DDETA), reduced deposition by about 95%. Even when DTPA
calcium gluconate plus 25,000 IU of Vitamin A was administered 39 days after a
dose of 39Pu, it reduced retention in bone by 25% and in liver by 80%.
Zirconium citrate and certain phosphate compounds, especially hexameta-
phosphate (HMP) reduced retained 239Pu by 50 to 70% if administered immediately
after a dose of 239Pu according to Wagner and Temple201 and Rosenthal292.
However, all of the above mentioned treatments have certain drawbacks: DTPA
O O O
and its analogs increased Pu concentration in the kidney, while zirconium
and phosphates increased concentration in the liver. Desferriox-amine (DFOA)
appears to be as effective or nearly as effective as DTPA if given within a
few hours after 239Pu exposure; it did not show significant 239Pu renal concen-
n n o
tration according to Taylor
Nenot294 et al. found that the therapeutic effectiveness of DTPA on bone
deposits of plutonium can be appreciable. DTPA treatment begun 3 weeks follow-
ing intramuscular injection of 239Pu decreased bone burdens by a factor of one-
half to one-third in 3 months.
Pretreatment of rats with tetracycline was found to decrease retention
of 239Pu in bone to about 60% of control values according to Taylor295 et al.
Tetracycline increased the initial rate of clearance of 239Pu from plasma.
Treatment with tetracycline was found to have no effect on the distribution
of intramuscularly-injected 239Pu, even when treatment was started immediately
after contamination.
Morin231 et al. studied the effect of treatment by DTPA following intra-
muscular and inhaled 238Pu nitrate by rats. Treatment was initiated 24 hours
after exposure and repeated twice a week. Protection of or removal from bone
by DTPA was clearly demonstrated at the 30th day when the respective bone
burdens of control and treated animals were in a ratio of 8:1, a decrease from
45 to 17% of bone activity. Postponing treatment until the 21st day showed
the importance of early treatment.
Sanders296 and Sanders and Meier297 studied the influence of fasting on
the efficiency of DTPA in enhancing the excretion of intraperitoneally injected
238Pu in female rats. Complete fasting for 10 days had no significant effect
45
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on the cumulative excretion of injected 238Pu. In animals given DTPA within
the first hour after 238Pu there was a 2.2-fold increased excretion, and a
1.4-fold increased excretion when DTPA was administered 14 days after 238Pu,
irrespective of fasting. They concluded that distribution of 238Pu bound to
liquids in extracellular fluids and bone was not significantly altered by
fasting so as to influence the chelation of 238Pu or 239Pu by DTPA.
Studies of the translocation of plutonium from wound sites and effects
of treatments were reported by Bestline298 et al., Lebel and Watters299,
Watters and Lebel300, Watters and Johnson301, and Gomez302 et al. The investi-
gators found that the effect of DTPA treatment was greater for Pu(N03),t than
for Pu02 implants. A time study of the buildup of plutonium in the lymph
node draining the wound site disclosed that the lymphatic system provides
rapid translocation from the wound. Rapid surgical excision, to be highly
effective, should be performed as soon as possible. If accumulation of
plutonium is detected in lymph nodes, lymphadenectomy should be considered.
Rosenthal303 et al. , Rosenthal301* et al. and Baxter305 et al. studied
the effectiveness of DTPA and glucan, a polysaccharide derived from yeast
cell walls, as agents for plutonium decorporation. DTPA therapy removed over
96% of intravenously injected monomeric 239Pu from beagle dogs. Removal from
spleen, lungs, kidneys, testes, muscle and lymph nodes ranged between 50 to
90%. The total skeletal content was also reduced by 50%. Adjunct therapy
with glucan did not result in significant additional removal of plutonium.
Use of the same treatment following polymeric 239Pu injection of mice showed
that at 47 days after administration, the net removal was 8.5% of the injected
dose by glucan, above 11.5% by twice weekly DTPA treatments and 19.5% by
combined therapy.
In 1972 Ballou and Hess306 found that about 50% of the plutonium excreted
into the perfused intestine of the rat during the first hour after plutonium
injection arrived by way of the bile. After DTPA treatment, the proportion
excreted in bile was increased to 75% and the bile plutonium concentration
increased 15 to 20-fold.
Rahman307 et al. in 1973, successfully encapsulated EDTA and DTPA within
lipid spherules (liposomes). Encapsulated EDTA given intravenously to mice
was retained longer in tissues than nonencapsulated EDTA. Encapsulated DTPA,
given to mice 3 days after 239Pu injection, removed an additional fraction of
plutonium in the liver, presumably intracellular, not available to nonencapsu-
lated DTPA. It also increased urinary excretion of plutonium.
Inhaled insoluble plutonium is not effectively mobilized by a wide variety
of expectorants, mucolytes agents, bronchodilators, surface-active agents,
phagocytic stimulating procedures, chelating and other physiologically active
materials (Smith308). Recent experiments have shown that pulmonary lavage
with physiological saline may remove 50% or more of Pu02 from the lung of rats
[(Sanders309); dog and rat (McDonald310); monkeys (Kunzle-Lutz311 et al. ,
Nolibe312); and baboons (Kunzle-Lutz313 et al,)],
DEPOSITION OF PLUTONIUM IN MAN
Plutonium has found its way to man, in readily measurable quantities, only
through occupational exposure, where the route is usually direct—by ingestion,
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inhalation, or by way of a Plutonium-contaminated wound (Bair and Thompson31").
In 1959 Langham315 found that alpha radiation from plutonium on the skin
surface does not penetrate to the sensitive basal layer of the epithelium.
Absorption of plutonium through the skin occurs only to a very slight degree,
and probably only when the skin is damaged. Lister316 studied fecal and
urinary plutonium excretion from two subjects who sustained high levels of
contamination on the uncut skin of the hand from accidental contact with
acid plutonium solutions. In one case, where the contaminant was mixed
plutonium isotopes in aqua regia and nitric acid, the measurements covered
150 days. In the other case, contamination with a solution of plutonium in
dilute hydrochloric acid containing EDTA and a detergent was followed for
110 days. The excretion patterns showed marked differences from those found
by Langham315, particularly in the high and variable amount of plutonium
excreted in feces relative to urine.
Laylee317 also studied excretion of plutonium following a lacerated wound
contaminated with 100 nyCi of Pu02. No translocation values were given.
In October 1970, a 59-year-old employee of Dow Chemical Company died
from complications following open heart surgery. This employee had an
estimated systemic burden of 0.22 yCi of plutonium or 541% of the maximum
permissible system burden, at the time of his death. The employee had been
involved in several contamination incidents and had two contaminated puncture
wounds prior to November 1965. He had excreted measurable amounts of pluto-
nium in his urine since 1960 and had an estimated 21% of the maximum permis-
sible systemic burden. In July 1965, he received another puncture wound
which left 18.5 yg of plutonium. A surgical incision removed 5.9 yg in
1967, a second incision removed all but about 0.3 yg. Autopsy and tissue
analysis showed plutonium concentration>skeleton>liver>lung>ttacheobronchial
lymph nodes>spleen>kidneys. The total extrapolated system burden from
autopsy samples was 0.07 yCi or about 177% of the maximum permissible amount
(Lagerquist318 et al.).
In 1973, Popplewell3l9 reviewed the chemistry of plutonium incorporated
in the body. Subjects covered are transport within the body in relation to
use of chelates, especially Ca-DTPA; studies of transferrin complexes in
body fluids; intracellular uptake in liver and deposits in bone.
Keely and Wenstrand32° calculated the urine to fecal ratios for two
workers following inhalation of soluble plutonium nitrate. Twenty days post
exposure the residual body burden was primarily in the skeleton. After 80
days and 250 days post-exposure <10 nCi was in the skeleton and <2 nCi total
plutonium in liver or lung as determined by in vivo counts. Urinary excre-
tion was erratic after 20 days post exposure but indicated a 1.8-day half-
life during the initial time of translocation.
Lagerquist321 et al. studied 19 cases where tissues were obtained from
autopsy and analyzed for plutonium. Twelve of the cases had no known record
of plutonium exposure. All of these had some detectable plutonium in their
organs but generally an amount that is representative of less than 1% of the
Maximum Permissible Systemic Burden (MPSB), In the seven others, the distribu-
tion varied from case to case, depending on the mode of entry, the chemical form
and the length of time since exposure. A typical distribution was not found, but
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on the average, the lung and tracheo-bronchial lymph nodes had the highest con
centration of material followed by the liver, the bones, and other tissues.
Przyborowski322 and Vaane323 et al. studied the deposition of plutonium
particles in the human respiratory tract after inhalation. A combined experi-
mental mathematical procedure was used,
Mclnroy321* et al. studied autopsy samples from 70 former employees of
Los Alamos Scientific Laboratory who had exposures ranging from 4 to 30 years.
Exposure in most cases was to inhaled Pu02 aerosols. Thirty-three of the
measured cases had plutonium deposition in th tracheobronchial lymph nodes.
No abnormalities of the lymph nodes were found.
Richmond325 presented a summary of information on human experience with
plutonium. Groups studied ranged from exposed GI's in 1944 to 1945 weapons
development, to occupationally exposed workers at Los Alamos and Rocky Flats,
to inhalation intake and burden in man of fallout 239Pu in New York. Data
are presented in tabular and graphical forms with tissue distribution included.
The retention half-time for Pu02 inhalation in humans was reported as
250 to 300 days. The relatively low values for human beings, compared with
dogs, suggest either that man clears plutonium particles from his lungs more
rapidly than dogs or that the materials inhaled in human accident cases were
more soluble than plutonium dioxide (Bair326).
Durbin reviewed old data and applied more recent knowledge derived
from animal experiments. Much of the older information was derived from intra-
venous administration of tracer amounts of 239Pu citrate to men suffering incur-
able diseases in 1945 and 1946. A few days after injection, human soft tissues
(other than blood and liver) contained as much as 20% of the plutonium dose.
Five to 15 months after injection the average liver plutonium content was 31%
of the dose for three cases with presumably normal liver function. Four to
457 days after injection, mean total skeletal plutonium was 49% for the seven
cases judged to have most nearly normal liver and skeletons.
Plutonium is transported in blood combined with transferrin, the iron trans-
port protein, and is stored in the liver in association with stored iron. After
being bound to transferrin, plutonium partially traces the behavior of the carrier
protein. The early phases of plutonium transport which are apparently associated
with extracellular fluid mixing, were prolonged in individuals with impaired cir-
culation.
Maximum urinary plutonium excretion occurred before the bulk of plutonium
was protein-bound. Minimum urinary excretion coincided with the time of maximum
Pu-transferrin binding. These observations were taken to mean that some pluto-
nium is filtered by the kidney in the form of a low-molecular weight chelate.
Urinary plutonium excretion was reduced by one-half in those persons who were
anemic, presumably because of their more efficient Pu-transferrin binding.
Fecal excretion of plutonium apparently represents secretion in bile and
other digestive juices. Fecal excretion was reduced by one-half or more in
those persons whose gastrointestinal tracts were judged not to be normally
stimulated.
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Average soft tissue release half-time was estimated to be.not less than
480 days and bone surface turnover for the whole adult human skeleton was
estimated to be about 5% per year. For an individual on a diet adequate in
iron and with normal iron stores, the model predicts that bone and liver will
contain equal amounts of plutonium 15 years after exposure.
EFFECTS OF PLUTONIUM IN HUMANS
328
Hemplemann et al., reporting a 27-year study of Los Alamos workers,
found that to date, none of the medical findings in the group can be attri-
buted definitely to internally deposited plutonium. The bronchial cells of
several of the subjects showed moderate to marked metaplastic change, but the
significance of these changes is not clear. Diseases and physical changes
characteristic of a male population entering its sixth decade were observed.
Because of the small body burdens, on the order of the maximum permissible
level, in these men so heavily exposed to plutonium compounds, it was concluded
that the body has protective mechanisms that are effective in discriminating
against these materials following some types of occupational exposures. This
is presumably explained by the insolubility of many of its compounds. Pluto-
nium is more toxic than radium if deposited in certain body tissues, especially
bone; however, from the practical point of view, plutonium seems to be less
hazardous to handle.
3 O Q
In 1974 Tamplin and Cochran reported two cases of cancer presumably
caused by plutonium contaminated puncture wounds of the hand. At this time
these were the only reported cases of cancers in people working with plutonium.
COUNTERMEASURES FOR HUMANS EXPOSED TO PLUTONIUM CONTAMINATION
The most successful treatment of inhaled plutonium particles appears
to be pulmonary lavage, followed by chelation therapy (Nolibe330, Smith331,
McClellan332 et al.). Lavage appears to remove about half the inhaled parti-
culates. Chelation by means of administration of DTPA either by aerosol or
intramuscular injection has been successful in removing soluble translocated
plutonium (Nenot et al. and Schofield and Lynn334).
Treatments of contaminated wounds include immediate use of a venous
tourniquet; flushing and decontaminating the wound site; excising tissue;
and administering chelating agents (intravenously, orally, and by aerosol
inhalation) (Jolly335 et al., Hesp and Ledgerwood336 and Larson337 et al.).
PRESENT ANALYTICAL METHODS
A thorough evaluation of present analytical methods for the transuranic
elements including plutonium in environmental samples has been prepared by
Bernhardt338 and is in press at this time.
It has been noted by numerous authors that analytical results are only
as good as the methods by which the samples are collected. Among the environ-
mental samples posing the greatest sampling problems are air and soil. In
1972 Hull3 reported tentative methods for the sampling and analysis of
radioactive substances in air as formulated by the Radioactive Substances
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Subcommittee of the Intersociety Committee on Methods for Air Sampling and
Analysis.
In 1973 Eberhardt and Gilbert3"*0 discussed the problems associated with
sampling of soils for environmental levels of plutonium. The general statisti-
cal considerations of sampling, problems associated with compositing samples
and consistent use of random sampling as a basic technique were examined.
The literature contains many methods for determination of plutonium in
biological and environmental samples. Most of these methods are variations
of basic procedures which utilize the precipitation, ion exchange and complex
forming properties of plutonium followed by electroplating and counting.
GENERAL METHODS
In 1971 Wong341 reported on the radiochemical determination of plutonium
in seawater sediments, and marine organisms. Seawater samples of 50 to 60
liters were collected at various depths; 50 to 100 g of dried shallow water
sediments or a larger aliquot from core samples was used. The author provides
a table of average 239Pu concentrations in marine organisms to allow selection
of proper sample size for optimal sample counting rate; the activity should be
about 0.5 to 5 dpm. An iron(II) hydroxide coprecipitation method was used for
the concentration of plutonium in seawater. A nitric-hydrochloric acid leach-
ing method was adapted for the treatment of sediments and ashed organisms.
The sensitivity for this method is 0.004 dpm per 100 liters of seawater (using
50-liter sample), 0.02 dpm per kg of sediments (100-g sample) and 0.002 dpm per
kg of marine organisms (1-kg sample). Factors influencing the uncovering,
contamination and blank activity were discussed.
Darrall3"*2 et al. described a method for the simultaneous determination
of 21|1Pu and plutonium alpha activity in effluent samples from nuclear
installations. The plutonium was isolated by coprecipitation on barium sulfate
followed by extraction into di-(2-ethylhexyl)-phosphoric acid, which was incor-
porated in a liquid scintillator for counting in a liquid scintillation spectro-
meter. Interferences from alpha- and beta-emitting radionuclides were studied
together with interferences from nonradioactive elements. The lower limit of
detection is in the region of 1 pCi. This is a modification of the method
described by Sill31*3 and by Sill and Williams3"1* in 1969 who reported that
plutonium will coprecipitate on barium sulfate provided it was in the tervalent
or quadrivalent state and the coprecipitation was carried out in the presence
of potassium ions. By coprecipitation after selective oxidation the elements
can be separated. The barium sulfate precipitate may be alpha counted directly
or the plutonium can be electrodeposited for alpha spectrometry. Talvitie3"*5'31*6
described methods for radiochemical determination of plutonium in environmental
and biological samples by ion exchange and an electrodeposition method for
alpha spectrometric determination. Sample preparation procedures were given
for urine, animal tissue, bone, saline and nonsaline water, siliceous and
limestone soil, and glass fiber air filters. Samples were prepared as azeo-
tropic 6M hydrochloric acid solutions of Pu(IV), stabilized with hydrogen
peroxide, and absorbed on anionic resin from 9M hydrochloric acid solution.
Coadsorbed iron was removed from the resin with 7.2M nitric acid. Plutonium
was selectively eluted with 1.2M hydrochloric acid - 0.6% hydrogen peroxide
and electrodeposited from 1M ammonium sulfate at pH 2 for alpha spectrometric
determination. Minimum detectable activity for 1000-min counts was 0.02 pCi
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239Pu. Puphal and Olson31*7 describe a method for electrodepositing various
'alpha-emitting nuclides singly or in combination onto a stainless steel cathode
from a mixed ammonium oxalate-ammonium chloride electrolyte. The nuclides were
deposited as hydroxides to better than 98% in 50 minutes. Interferences are
also discussed.
Gillette3lt8 et al. investigated the determination of plutonium in soil.
The method involves a complete dissolution of the soil by a fusion technique
followed by chemical separation of the plutonium by barium sulfate, extraction,
electrodeposition, and alpha pulse height analysis.
Hampson and Tennant31*9 reported the simultaneous determination of acti-
nide nuclides in environmental materials contaminated by controlled discharges
of liquid wastes. Multielement actinide analysis is achieved by extracting
the whole group, or part of it, in the tri-n-octylphosphine oxide-n-heptone-
nitric acid-sodium nitrate system, stripping into ammonium carbonate solution
and electrodeposition, followed by solid-state alpha spectrometry. Up to 2 kg
of edible seaweed or 10 kg of fish flesh can be handled, with detection limits
(in terms of activity to double background) of 2 X 10 6 and 4 X 10 7 pCi/g,
respectively, for a 1-week counting time. Sensitivities for precision with
4 percent standard deviation are 4 X 10 "* and 8 X 10 5 pCi/g, respectively,
which corresponds to levels associated with fallout.
Piltingsrud and Stencel350 report a direct method for evaluating 239Pu
content in large soil samples (up to 1 kg) by means of a phoswich detector.
Sample 239Pu + 21tlAm specific activity must be >20 pCi/g. When high levels
of other gamma emitters, a ratio >1000:1, are present causing analysis
interference, specific radiochemical analysis of the sample is indicated.
In 1973 Thomas351 presented a method for measuring 238Pu and 239Pu in
air samples. The membrane filter was prepared by fusion and the plutonium
was retained on an ion exchange column and eluted with HC1 containing HI.
After electroplating, the plutonium isotopes were alpha counted.
Novoselova352 et al. described the optimum conditions of concentration,
separation and measurement of 239Pu after the latter had been added to ashed
bone tissue. Bone tissue was ignited in a muffle furnace at 600° C, and the
inorganic residue was dissolved in HN03. The plutonium was extracted with
TBP, reextracted with aqueous hydroxylamine HC1, and precipitated from solu-
tion into bismuth phosphate. The latter was washed, mixed with a phosphor,
and the plutonium was determined in a scintillation counter.
Ershova353 et al. described a method for determination of 239Pu based
on liquid-liquid extraction by monoisoactyl methyl phosphonate and mixed
isoamyl phosphate at a phase volume ratio of at least 100. This method is
used for the estimation of the 239Pu content in lung tissue, bone tissue,
surface waters, and other environmental objects.
Ghysels351* reported the extraction of plutonium was effected with liquid
ion exchangers (e.g., tertiary amines such as triisooctylamine). The pluto-
nium was put back into organic solution by extraction with DEHPA. After mixing
with a liquid scintillator, the counting yield was determined (close to 100%).
This method was intended for determination of plutonium in biological substances.
It was applied to the analysis of radioactive dusts of different origin.
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Schieferdecker355 presented a method for separation of plutonium in pCi
amounts from biological material by extraction with bis (2-ethyl-hexyl) phosphate
(DEHPA). It was possible to identify individual transuranic elements after joint
carrier-free preparation by electrodeposition and subsequent alpha spectrometry.
Amounts below 0.2 pCi can be determined.
In 1973 Budnitz356 provided an overview of the techniques for measuring
plutonium in various media. The emphasis was on measurements for surveillance
and protection in environmental and occupational situations. Overviews were
first provided for the characteristics of, sources of, and typical levels of
plutonium concentrations. The various measurement techniques were discussed.
AUTORADIOGRAPHY
Fission track autoradiography has been used by several investigators to
study the distribution of plutonium in bone and other biological samples
(Hamilton357, Becker358 et al., Jee359'360 et al. and Schlenker and Oltman361).
The autoradiographs are produced by placing thin bone sections in contact with
plastic films which register fission fragment tracks. The bone and film are
inserted into a nuclear reactor where neutrons induce fissioning of plutonium.
Some plastics show not only the fission tracks but an image of the bone
itself. The image shows no detail but does reveal where the boundaries between
the bone and marrow spaces lie so that positioning of the fission tracks rela-
tive to the boundaries may be easily determined. Lexan is the plastic which
has been most widely used to produce images of irradiated materials (Schlenker
and Oltman361).
Q C O
Lindenbaum and Russell found good agreement between liver burdens
determined autoradiographically or radiochemically. Using livers from mice
injected intravenously wiht polymeric 239Pu, at dose levels ranging from
6.6 to 93 yCi/kg, the quantitative technique for assay of plutonium deposited
in animal tissue was tested for linearity in the relationship between photo-
graphic exposure time and number of alpha tracks formed.
INSTRUMENTAL ANALYSIS
In 1973 Winkle and Hoetzi363 reported a sensitivity of 0.04 to 0.01 pCi/m3
for long-lived alpha-emitters in air. The sensitivity was obtained by alpha
spectrometry of electrostatically-precipitated aerosols in a large Frisch grid
ionization chamber after decay of the natural activity for 2 to 4 hours and
100 minutes counting. This sensitivity corresponds to about 0.1 to 0.01 of
the maximum permissible concentrations (168/h/wk) for 239Pu.
Liquid scintillation counting of plutonium in biological samples is the
subject of a report by Joshima and Matsuoka36\ The liquid scintillation
method without ashing was established for plutonium in animal tissues by use
of a commercially available tissue solubilizer. Samples up to 250 mg wet
weight could be handled with this procedure. The samples were then counted
in a liquid scintillation spectrometer set for the optimal gain setting for
plutonium.
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Matsuoka and Joshima365 developed a method for determining particle size
of plutonium in solution by a diffusion chamber. The diffusion chamber was
prepared from a plastic ringe (20 mm x 5 mm), both sides of which were
covered with millipore membrane of adequate pore size of Visking membrane.
The diffusion chamber containing 0.1 ml of test solution was placed in a plastic
container with 5 ml to 10 ml saline solution and incubated 1 hour with shaking
in a 37° C water bath. The "diffusibility" of plutonium particles from the
diffusion chamber was estimated from the sample measurement of extra fluid at
the final point by liquid scintillation counting and for external counting at
17 keV L-x-ray of the diffusion chamber before and after the incubation. The
particle size of "monomeric" and polymeric plutonium was estimated by this
method. This technique may be useful in future studies of the effect of
chelating agents on plutonium in vitro.
BIOASSAY FOR PLUTONIUM
A review of current methods for bioassay of plutonium is given by Low-
Beer366. Collection and initial handling of samples is included.
The history of the plutonium bioassay program at Los Alamos Scientific
Laboratory from 1944 to 1972 was reviewed by Campbell367 et al. Methods of
urine sample collection, radiochemical separation, and counting are described.
A number of investigators have published methods for determination of
plutonium in urine samples. In Japan, Kara et al. used a method of ion
exchange, and counted with a 27T gas flow counter. When plutonium is ingested
or inhaled, fecal samples are collected for 3 to 5 days after intake. In France,
Ventadour et al. have a rapid method using a large surface area xenon-methane
proportional counter having low background noise.
In India, Iyer and Kamath370 have developed a rapid determination of
uranium, thorium, plutonium, and americium sequentially in a single urine sample.
The actinides are precipitated with BiPOij and the hydrolysis method used for
separation.
In Russia, Mikhailova371 et al. developed a method in which Pu(IV) as the
cupferronate is separated from macro impurities by chloroform extraction from
a nitric acid medium using zirconium carrier or no carrier. About 3 percent
of the 239Pu remains in the aqueous phase. After removal of the chloroform from
the organic phase, the 239Pu is precipitated with ammonia, using a lanthanum
carrier and is counted after further processing. The plutonium can also be
electro-precipitated. Golutvina372 et al., in determining 239Pu in the presence
of enriched uranium, used a method based on boiling urine with nitric acid and
hydrogen peroxide, concentration of isotopes by precipitation and subsequent
extraction with precipitates of bismuth phosphate (239Pu) and lantan fluoride
(enriched uranium). The precipitates are mixed with a fluorescent compound
and counted in a layer of hard scintillator. The efficacy of registration
of alpha-particles comprises 90 to 95%.
In Germany, Schieferdecker373 detected plutonium in urine and feces based
on DEHPA extraction, and subsequent counting by alpha spectrometry. Activity
amounts of 0.1 pCi can be determined.
53
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In England, Popplewell and Stradling374 developed a 2 to 3 hour deter-
mination for plutonium in urine. The procedure utilizes the fact that plutonium
binds to transferrin in solutions of pH >6. This serum protein, M.W. 88,000,
was filtered from aqueous solutions with appropriate membranes. Another rapid
method was developed by Bates375 et al. for determination of plutonium in urine
within 4 hours of receipt, excluding counting time. The method consists of
evaporating a 250-ml sample to dryness with nitric acid, baking at 550° C to
remove organic matter, dissolution of the residue and removal of interfering
condensed phosphates by boiling with a catalyst. The plutonium was isolated
by an anion-exchange column and finally counting the plutonium on a tray in a
low background counter.
In Italy, Camera376 et al. described a method for the determination of
alpha activity in urine by means of extraction, in a beaker, of radionuclides
in a solution of triactylphosphine oxide (TOPO) on a base of Mitene 350/80
(polyethylene). Testa377 et al. reported using wet mineralization, plutonium
coprecipitation, a passage in an anion-exchange resin column, an electroplating
procedure and alpha counting on an automatic solid state detector. They report-
ed recovery of 78 ± 22%, with a sensitivity limit of 0.04 pCi/1 or urine,
Campbell and Mclnroy378 discussed the various aspects of handling human
autopsy tissues and methods used for the determination of plutonium. It was
pointed out that 5 mrem/y has been proposed as the maximum permissible level of
plutonium for the general human population, which is equal to approximately
three 1 ym particles of plutonium deposited per person per year and the analytical
chemist is confronted with what appears to be an almost insurmountable task to
detect this level of plutonium in man. The interlaboratory calibration of count-
ing methods, using standards of 239Pu, 238Pu, and 236Pu plated on stainless steel
or samples of ashed beef bones, liver and lung spiked with 239Pu, was discussed.
Methods used for the chemical preparation of the ashed tissue samples for radio-
metric analysis were included.
Once analyzed the process of determining body content from urine data is
just begun. Evaluation of excretion data by computer programs, models, and
equations was reported by many investigators (Henle and Bramson379, Heid380'381
et al., Osanov382'383 et al., Snyder38", Nelson385 and Beach386).
IN VIVO MEASUREMENT OF PLUTONIUM
The detection and measurement of plutonium in wounds was the subject of
an article by Sharma and Somasundaram387 in 1971. A thin Nal(Tl) scintillation
detector was optimized for the detection of soft x-rays for use as a 239Pu wound
monitor. The resolution obtained for 17-keV x-rays was between 60 and 65%. Data
on monitor sensitivity, background, minimum detectable 239Pu activity and varia-
tion of the count rate in the plutonium channel with depth of plutonium source
in a simulated human wound were presented.
Ohlenschlaeger and Fromhein388 reported on the operational and technical
features of a measuring system for the determination of radionuclides, particu-
larly 239Pu, in contaminated wounds. Special consideration was given to the
integration of different detectors and devices into a mobile and portable measur-
ing unit with central control. Experimental results gave proof of the system
performance.
54
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As in vivo determination of plutonium is only as good as the standardi-
zation of the systems used for its detection; a number of authors have reported
on calibration of these systems.
An IAEA plutonium interlaboratory calibration experiment was described
by Button in 1973. Calibration factors for the in vivo measurement of 238Pu
and Pu in human lungs as a function of body size were obtained using inhaled
Cr and Pd particles as simulants. Optimum subject-detector geometry for
the in vivo measurement of low-energy photon emitters in human lungs was deter-
mined. A mathematical model for americium and plutonium distribution in human
lungs was developed. The performance of scintillation detectors inside a
shielded whole-body counting room was evaluated.
390
Tomlinson et al. reported in 1973 on chest wall tissue measurements for
lung counting applications. Because the half-layer for 17-keV x-rays in tissue
is only 6 to 7 mm, the effective thickness of tissue overlying the lungs was
determined by ultrasonic measurements over the second, third and fourth rib.
In 1973, Swinth and Dean391 discussed an intercalibration program consist-
ing of tabulation of photon intensities for actinides, an intercomparison of
counting systems using a standard consisting of either a source or a phantom,
and counting of a subject or subjects who had been accidentally exposed to
plutonium.
Tomlinson392 et al. reviewed the basic, whole body counting program for
the Mound Laboratory since December 1969, The phoswich detection system is
described. Detection limits were given as a function of the subject's tissue
thickness between the lungs and detectors. For a typical subject with an
effective tissue thickness of 2.3 cm over the lungs, the system has a detection
limit of 4 nCi.
Detection systems with various modifications of Nal(Tl) crystals and propor-
tional counters have been reported by many investigators. The problems of
detecting low-energy photons from plutonium deposited in the human body were
discussed by these investigators and detectors modified to attempt to obtain
direct plutonium measurement for assessing body burdens (Yaniv393, Newton391*
et al., Ishihara395 et al.,.Tomitani and Tanaka396, Sharma397 et al., Dolgirev39i
et al., Clemente399, Boulay*00, Morsy1*01, Loessner"02, and Newton1*03 et al.).
Swinth lf°" et al., Swinth and Ewins405, Swinthlf06, and Moldofsky"0 7 discuss
in vivo plutonium measurements in tracheobronchial lymph nodes by means of intra-
esophogeal probes designed to minimize attenuation of the x-rays associated with
plutonium.
MONITORING INSTRUMENTATION
As the primary hazard of plutonium to humans is inhalation of respirable
aerosols and particulates, improvements and modifications in air filters and
monitoring instrumentation have been continually under investigation.
Davis1*08, Angel and Anderson1*09, and Ettinger"10 et al. discussed the use
of high-efficiency particulate air (HEPA) filters for plutonium particle and
aerosol entrapment.
53
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Plutonium monitoring instruments for laboratory use were reported by
Binard1*11, Hardy1*12 et al., Nichols"13, Singh and Chugh1*", and Kikkawa1*15
et al.
The instrument described by Nichols413 was found to eliminate greater
than 90% of the 2,250 dpm alpha natural background activity collected in
order to detect 48 RCGS of soluble 239Pu within 1-1/2 hours. The instrument
utilized two ZnS scintillation detectors. It was believed that by using
discriminators, lower concentrations of 239Pu could be detected.
Singh and Chugh1*11* reported using an alpha spectrometer technique using
a silicon surface barrier detector. The system is capable of indicating
alarm at a level of 8 MPC hours in the presence of natural activity.
Portable plutonium detectors for use in the field were discussed by
Burton and Anastasi1*16 who used a probe with a CaF(Eu) scintillator with a
pulse height analytical capability to detect fissile material in the presence
of background. The absolute sensitivity is ~24 counts/min/yg/m2 of 239Pu
on a uniformly contaminated surface with no overburden.
Cohen and Gundersen1*17 discussed field experience with the mobile AEC
measurement van.
The necessity of surveying large areas of land has required the develop-
ment of instruments for aerial surveys. Stuart**18 reported on such a system,
set to sense the 60-keV x-ray from 21tlAm, a decay product of 21tlPu. The
detector was mounted inside an Air Force helicopter and flown over known
concentrations at the Nevada Test Site.
Boyns and Anderson1*19 discussed an airborne spectrometer designed to
search for ruptured plutonium capsules in event of an accident involving a
space mission utilizing 238Pu thermoelectric generators. A spectrometer
capable of_detecting 2 8Pu in air below the maximum permissible concentra-
tion of 10 yCi/cm3 without interference from naturally occurring airborne
alpha emitters was mounted in an Airborne Radiological Monitoring System
(ARMS). Information was included on the aircraft positioning system, air
sampling, and the procedures to be followed when actually using the spectrome-
eter.
56
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Plutonium in Urine. Separation from Baked Urine Residues Using Ion
Exchange," BNWL-Report-L, 21 p., 1971.
376. Camera, V., Barassi, G., and Legras, J. J., "Rapid and Simple Method for
Determination of Total Alpha' Radioactivity in Urine," EUR-4675, 14 p.,
1971.
377. Testa, C., Masi, G., and Marchionne', U., "Plutonium Bio-Assay Laboratory
at the Casaccia Nuclear Centre," EUR-4612, pp. 421-435, 1971.
378. Campbell, E. and Mclnroy, J. F., "Plutonium and Environmental Metals in
Man," LA-5445-C, 10 p., November, 1973.
379. Henle, R. C. and Bramson, P. E., "Evaluation of Internally Deposited
21|1Am From Bioassay Data," AT (45-l)-1830, pp. 731-741, 1972.
380. Heid, K. R. , Jeck, J. J., and Anderson, B. V., "Interpretation of Data on
Internal Plutonium Contamination," EUR-4612, pp. 437-468, 1971.
381. Heid, K. , "Evaluations of Intake and Deposition Based on Bioassay Data,"
BNWL-SA-4724, 36 p., 1973.
382. Osanov, D. P., Tessin, M. Y., and Filatov, V. V., "Determination of the
Plutonium Content in the Human Organism by the Rate of Its Elimination,"
Med. Radiol. 14:4, pp. 44-51, April, 1971.
383. Osanov, D. P., Filatov, V., and Tessin, M., "Determination of 239Pu in a
81
-------
Living Human Organism From the Rate of Its Elimination," CONF-720503,
pp. 491-496, 1973.
384. Snyder, W. S., "Method of Interpreting Excretion Data Which Allows
for Statistical Fluctuation of the Data," CONF-711104, pp. 485-494,
November, 1971.
385. Nelson, I. C., "Simplified Method for Evaluating the Healy Plutonium
Excretion Equation," Health Phys. ^2:2, pp. 191-193, February, 1972.
386. Beach, S. A., "SEBEACH, A Digital Computer Program for the Estimation
of Body Content of Plutonium from Urine Data," Health Phys. 24, pp. 9-
16, January, 1973.
387. Sharma, R. C. and Somasundaram, C., "Detection and Measurement of 239Pu
in Wounds," BARC-559, 23 p., 1971.
388. Ohlenschlaeger, L. and Fromhein, 0., "Structure and Function of a
Medical Measuring System for Wounds," Strahlentherapie (STRAA) 146:4,
pp. 422-432, October, 1973 (in German).
389. Button, J., "IAEA Plutonium Interlaboratory Calibration Experiment,"
COO-3382-13, pp. 6-7, 1973.
390. Tomlinson, F. K., Brown, R., Anderson, H., and Robinson, B., "Chestwall
Tissue Measurements for Lung Counting Applications," MLM-2047 (OP)
6 p., 1973.
391. Swinth, K. L. and Dean, P. N., "Intercalibration for Low-Energy Photon
Measurements," Health Phys. ^5:6, pp. 599-603, December, 1973.
392. Tomlinson, F. K., Brown, R., Anderson, H., and Robinson, B., "Applica-
tion of Phoswich Detectors for Lung Counting Plutonium-238," MLM-2048
(OP), 6 p., 1973.
393. Yaniv, S. S., "Plutonium and Americium Measurement in Humans by X-
and Gamma-Ray Spectral Analysis," WASH-1241, 94 p., April, 1973.
394. Newton, D. J., Rundo, J. , and Taylor, B, T., "Progress in Instrumentation
and Calibration Techniques for the Assessment of Lung Burdens of 239Pu,"
EUR-4612, pp. 469-482, 1971.
395. Ishihara, T., Nahara, N., linama, T.?Tonaka, E., and Yashiro, S., "Tl
Crystal of Large Area," NIRS-Pu-7, pp. 31-34, 1972.
396. Tomitani, T. and Tanaka, E., "Large Area Proportional Counter for
Assessment of Plutonium Lung Burden," NIRS-Pu-7, pp. 34-37, 1972.
397. Sharma, R." C., Nilsson, I., and Lindren, L., "Twin Large Area Propor-
tional Flow Counter for the Assay of Plutonium in Human Lungs," AE-463,
49 p., December, 1972.
398. Dolgirev, E. I., Kaidanovsky, G., and Shamar, V., "In Vivo Counting of
82
-------
Transuranium Isotopes in the Human Body - 239Pu and 2lflAm," CONF-
720503, pp. 497-502, May, 1972.
399. Clemente, G. F. , "In Vivo Measurements of 239Pu in Man," CONF-720503
pp. 503-507, May, 1972.
400. Boulay, P., "Direct Measurement of Pulmonary Plutonium Contamination,"
Advances in Physical and Biological Radiation Detectors, Vienna, IAEA,
pp. 287-297, 1971.
401. Morsy, S. M., "Direct Methods for the Assessment of 239Pu and 235U
Body Burdens," CONF-711104, pp. 115-127, 1972.
402. Loessner, V., "Assessment of Low Energy Photon Emitters in Man:
Technical Aspects of Detection," CONF-720503, pp. 459-463, May, 1972.
403. Newton, D. J., Fry, F. A., Taylor, B, T., and Eagle, M. C., "Factors
Affecting the Assessment of 239Pu jn Vivo by External Counting Methods,"
CONF-711104, pp. 83-96, November, 1971.
404. Swinth, K. L., Park, J. F. , and Moldofsky, P. J., "Counting Plutonium
in the Tracheo-Bronchial Lymph Nodes," Health Phys. 22, pp. 899-904,
June, 1972.
405. Swinth, K. L. and Ewins, J. H. , "Biomedical Probe Using a Fiber Optic
Coupled Scintillator," BNWL-SA-4761, 17 p., 1973.
406. Swinth, K. L. , "Radiation Instrumentation: In Vivo Plutonium Measure-
ments," BNWL-1751 (Pt. 2), pp. 89-92, April, 1973.
407. Moldofsky, P. J., "Avalanche Detector Arrays for In Vivo Measurement
of Plutonium and Other Low-Activity, Low-Energy Emitters," CONF-711111,
pp. 55-63, 1971.
408. Davis, W., Jr., "High Efficiency Particulate Air Filters: State of the
Art Summary Pertaining to Plutonia Aerosols," ORNL-TM-4463, 10 p.,
April, 1974.
409. Angel, K. C. and Anderson, H. F., "Different Type Glove Box Filters Used
for 238Pu Work," CONF-690103-P2, pp. 981-993, 1972.
410. Ettinger, H., Elder, J., and Gonzales, M., "Performance of Multiple
HEPA Filters Against Plutonium Aerosols Progress Report, July 1 -
December 31, 1972," LA-5170, 27 p., January, 1973.
411 Binard L., "Air Monitoring in Plutonium Laboratories," Safety Measure-
ments in Nuclear Research. Freium, G., Ed., Mol, Belgium, Centre d'Elude
de 1'Energie Nuclaire, pp. B.7.1-B.7.3, 1972.
412. Hardy, R. W., Knowlen, R. B. , Sandifer, C. W., and Plake, W. C.,
"Personnel Plutonium Monitor," U.S. Patent 3,670,164, June 13, 1972,
Filed August 18, 1970.
413. Nichols, C. E. , "Plutonium Sensitive Alpha Air Monitor," Health Physics
83
-------
Operational Monitoring, _2, Willis, C. A., Ed., New York, Gordon
and Breach, Science Pub., Inc., pp. 1117-1125, 1972.
414. Singh, A. N. and Chugh, P. K., "Air Monitor for Continuous Measurement
of Airborne 239Pu," CONF-701138, pp. 585-593, November, 1970.
415. Kikkawa, M., Yashikawa, K., and Sumita, H., "Study on Routine Operation
for Plutonium Air Monitor," NIRS-Pu-7, pp. 73-74, 1972.
416. Burton, B. S. and Anastasi, M. N., "Portable Plutonium Detector,"
Anal. Instrum. 10, pp. A7-A16, 1972.
417. Cohen, I. and Gundersen, G., "Field Experience With the AEC Measure-
ment Van," CONF-710617-3, 23 p., 1971.
418. Stuart, T. P., "Use of Aerial Surveys for Determining Plutonium Concen-
tration," EGG-1183-1517, 10 p., April, 1971.
419. Boyns, P. K. and Anderson, C. N., "Airborne Alpha Spectrometer: Systems
and Procedures in Support of the Apollo Program," ARMS-69.6.11, 20 p.,
November, 1969.
84
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AUTHOR INDEX
Author/Reference
A
Aarkrog, A./127
Adams, W. H./119.166
Alvarez-Raines, C./217
Ames, L. L./190
Anderson, H. F./283
Angel, K. C./409
Anspaugh, L. R./184
Argonne National Laboratory/
50
Atherton, D. R./262
Atomic Energy Commission,
WASH/35,36,39,48
Au, F. H. F./197
B
Bair, W. J./132,250,251,
253,314,326
Ballou, J. E./230,245,253,
259,306
Bates, T. H./375
Baxter, D./232,239,305
Beach, S. A./386
Becker, R. C./43,358
Belliayer, Y. A./134
Bernhardt, D./338
Bestline, R. W./298
Biles, M. B./28
Binard, L./411
Bliss, W./196
Boyns, P. K./419
Brown, C. L./44
Bruenger, F. W./136
Bowen, V. T./169
Boss, M. R./99
Boocock, G./141
Boulay, P./400
Budnitz, R. J./356
Buldakov, L. A./248
Burton, B. S./416
Bustad, L. K./224
Button, J./389
85
Author/Reference
C
Camera, V. G./376
Campbell, E. E./367,378
Carfagno, D. G./74,96,97,98
Carritt, J./226
Cellini, R. F./69
Cherdyntsev, V. V./5,6
Chipperfield, A. R./144
Christenson, C. W./92
Clarke, R. H./105
Clemente, G. F./399
Cline, J. F./207
Cochran, T. H./153
Cohen, I./417
Conway, T. W./63
Cowan, M./15
Craig, D. K./256
Cummings, S. L./205
Curtis, M. L./121
D
Dagle, R. E./284
Darrall, K. G./342
Daub, W. 0./49
Davis, W., Jr./408
DeBortoli, M./8
Dionne, P. J./261
Dix, G. P^/65,123
Dolgirev, E./398
Dougherty, J. H./266
Drobinski, J. G./9
Dunaway, P. B./24
Durbin, P. W./236,327
E
Eberhardt, L. L./185,340
Eisenbud, M./12.21
Emelity, L. A./33
Engstroem, S./54
Erleksova, E. V./150
-------
Ershov, E. B./219,220
Ershova, Z. V./353
Ettinger, H./410
Feenez, R. E./143
Finkel, M. P./241.246
Finkle, R. D./221
Fish, B. R./101
Folsom, T. R./173
Francis, C./200
Howard, E. B./279
Hudson, J./118
Hull, A. P./339
Hunt, D. C./29
Hunzinger, W./72
Hvinden, T./25
ICRP Publication/265
Ishihara, T./395
Iyer, R. S./370
General Electric Company/52
Ghysels, J. P./354
Gilbert, R. 0./186
Gillette, J. H./348
Gofman, J. W./60
Golutvina, M. M./372
Gomez, L. S./302
Gromov, V. V./171,172
Jacobson, L./203
James, A. C./272
Jaworowski, Z./249
Jee, W. S. S./149,264,359,360
Johnson, L. J./19
Jolly, L. J./335
Joshima, H./364
H
Haas, F. X./68
Hajek, B. F./89
Hakonson, T. E./18,20
Hale, V. Q./211
Hamilton, D./47
Hamilton, E. I./357
Hamilton, J. G./222
Hampson, B. L./349
Hanson, W. C./26
Kara, T. S./368
Hardy, E. P./22,23,30,192,106
Hardy, R. W./412
Hayden, J. A./117
Healy, J. W./195
Held, K. R.7380,381
Heine, W. F./57
Hemplemann, L. H./328
Henle, R. C./379
Herring, G. M./148
Hesp, R./336
Hickman, W.~ W./34
Hilborn, J. W./61
Hodge, V. F./165
Hoffman, D. C./4
K
Kapshukov, I. I./113
Kashima, M./229,277
Katz, J./225
Keely, R. B./320
Kikkawa, M./415
Klepper, B./216
Kneip, T. J./167
Kotrappa, P./62
Krey, P. W./85
Krivolutskii, D. S./198
Kubose, D. A./114,128
Kunzle-Lutz, M./311,313
Lai, M. G./125
Lafuma, J./252
Lagerquist, C. R./318.321
Langham, W. H./124,178,179,315
Lapp, R. E./55
Larson, H. V./337
Laylee, A. M./317
Leavitt, V. D./187
Lebel, J. Z./299'
86
-------
Levine, C. A./3
Lindenbaum, A./154,237,362
Lingren, W. E./115
Lister, B. A. J./316
Lloyd,. M. H./116
Loessner, V./402
Los Alamos Scientific Laboratory/
37,90
Low-Beer, A./366
Me
McClellan, R. 0./247.332
McCurdy, D. E./32
McDonald, K. E./310
Mclnroy, J. F./324
Nichols, C. E./413
Nishita, H. E./201
Nolibe, D./312,330
Norwood, W. D./7
Noshkin, V. E./158,159
Novoselova, G. P./352
0
Ohlenschlaeger, L./388
Olafson, J. H./218
Oltman, B. G./58
Osanov, D. P=/382, 383
Ouchi, S./168
Ovcharenko, E. P./243,286
M
Marshall, J./170
Massey, P./146
Matheson, W. E./73
Matsuoka, M./238,257,365
Mays, C. W./240,268,269
Menzel, R. G./156
Metivier, H./278
Michels, D./93
Mikhailova, 0. A./371
Miner, F. J./81.82
Mishima, J. M. /31,42,59,102
103
Miyake, Y./161
Moldofsky, P. J./407
Morsy, S. M./401
Morin, M./231,296
Mork, H. M./181
Morrow, P. E./228
Moskalev, Y./270,275
Muntz, J. A./138
N
Nabors, C. J./267
National Environmental Research
Center-Las Vegas/194
Nelson, I. C./385
Nenot, J. C./294,333
Neubold, P./208,209
Nevissi, A./129
Newton, D. J./394,403
Palmer, R. F./133
Park, J. F./254.255
Patin, S. A./163
Patterson, J. H./91
Paxton, H. C./27
Penn, A. W./66
.Pesternikov, V. M./271
Pigford, T. H./46
Pillar, K. C./160
Piltingsrud, H./350
Platt, R. B./77
Poet, S. E./80,86
Polzer, W. L./lll
Popplewell, D. S./145,319,374
Price, K. R./182,214
Przyborowski, S./322
Puphal, K. W./347
R
Raabe, 0". G./120
Rahman, Y./307
Rasmussen, N. C./56
Rediske, J. H./204
Reichle, D. E./78
Reynolds Electrical and
Engineering Company/193
Rhodes, D. W./87,88
Richmond, C. R./325
Romney, E. M./76,155,180
210,212,213
Rosenthal, M. W./234,292,304
87
-------
Routson, R. C./189
Saenz, M. D. L./l
Sakanoue, M./188
Sanders, C. L./280,281,282
287,288,289,296,297,309
Sayre, W. W./157
Schieferdecker, H.7355,373
Schlenker, R. A./361
Schmid, L. C./53
Schofield, G./334
Schwendlman, L. C./104
Seaborg, G. T./ll
Sedlet, J./83
Sehmel, G. A./94,95
Selders, A. A./202
Slkov, M. R./244
Sharma, R. C./387,397
Sill, C. W./343,344
Silver, G. L./112.122
Silver, W. J./191
Singh, A. N./414
Smith, D. D./215
Smith, V. A./331
Smith, V. H.7290,308
Snyder, W. S./384
Stara, J. P./224
Stannard, J. N./13
Stevens, W./137
Stewart, K./223
Stover, B. J./135,147,263
264,285
Stuart, T. P./418
Suzuki, M./258
Swanson, J. L./84
Swinth, K. L./391,404,405
406
Tomlinson, F. K./390,392
Toyoshima, E./71
Travis, J. R.779,108
Turner, G. A./139.142
U
Ulrich, W. C./40
U.S. Environmental Protection
Agency775
V
Vaane, J. P./323
Vaughn, J./151
Ventadour, J./369
Volchok, H. L.710,100
W
Wagner, R. W./291
Wahgren, M. A./130
Wallace, A./199
Wandell, J./260
Warner, E. E./70
Watters, R. L.7300,301
Weast, R. C./2
Webb, G./110
Weeks, M. H./227
Weiner, R./64
Williams, D. C./67
Wilkinson, P. N./242
Wilson, D. 0./206
Wilson, R. H.714,16,17
Winkle, R./363
Wischow, R. P./41
Wong, K. M./162,164,174,177,341
Wymer, R. G./51
Talvitie, N. A./345,346
Tamplin, A. R./329
Tamura, T./183
Taube, M./126
Taylor, D. M./131,140,293,295
Taylor, G. N.7152,233,273,274
276
Testa, C./377
Thomas, C. W. 7107,109,351
Thomas, J. T./45
Todd, D. K./38
Tomitani, T./396
88
Yaniv, S. S./393
Zapol'skaya, N. A./235
Zlobin, V./175,176
GPO 690— SOI/Z51
-------
TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing)
1. REPORT NO.
EPA-600/3-76-043
3. RECIPIENT'S ACCESSION-NO.
4. TITLE AND SUBTITLE
AVAILABILITY, UPTAKE AND TRANSLOCATION OF PLUTONIUM
WITHIN BIOLOGICAL SYSTEMS: A Review of the Significant
Literature
5. REPORT DATE
April 1976
6. PERFORMING ORGANIZATION CODE
'. AUTHOR(S)
Anita A. Mullen and Robert E. Mosley
8. PERFORMING ORGANIZATION REPORT NO
9. PERFORMING ORG ANIZATION NAME AND ADDRESS
Environmental Monitoring and Support Laboratory-LV
U.S. Environmental Protection Agency
P. 0. Box 15027
Las Vegas, NV 89114
10. PROGRAM ELEMENT NO.
1FA083
11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
Same as above
n/a
13. TYPE OF REPORT AND PERIOD COVERED
Final FY75
14. SPONSORING AGENCY CODE
EPA-ORD
Office of Health and Ecologi-
15. SUPPLEMENTARY NOTES
16. ABSTRACT
This report is a selective review of the literature on the availability of
plutonium in the environment and its cycling throughout representative biological
systems ranging from large biomes covering hundreds of miles to the molecular
transformations within individual cells. No attempt was made to develop a
comprehensive bibliography. Rather, references were selected for inclusion
as representative documentation for the vast spectrum of material that is
available on the subject.
Important general references are listed separately. Thereafter the literature
is described in essay form on a subject basis. References cited by number in
the text are listed in complete bibliographic form at the end of the report
together with an author index. The majority of the material reviewed is limited
to relatively recent publications.
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
b.lDENTIFIERS/OPEN ENDED TERMS
c. COSATI Field/Group
Chemical Analysis
Ecology
PhysicoChemical Properties
Plutonium Isotopes
Radiation Effects
Radiation Hazards
biological accumulation
environmental
contaminants
06F
06R
06T
07D
18B
3. DISTRIBUTION STATEMENT
RELEASE TO PUBLIC
19. SECURITY CLASS (ThisReport)
TTWTr.ASSTFTBT)
,GES
96
20. SECURITY CLASS (Thispage)
UNCLASSIFIED
22. PRICE
EPA Form 2220-1 (9-73)
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