Ecological Research Series
              CONCENTRATION FACTORS  AND
                    TRANSPORT MODELS  FOR
RADIONUCLIDES IN AQUATIC ENVIRONMENTS
                          A Literature  Report
                     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-600/3-76-054
                                             May  1976
   CONCENTRATION FACTORS AND TRANSPORT MODELS FOR
       RADIONUCLIDES IN AQUATIC ENVIRONMENTS
                A LITERATURE REPORT
                        By
                 Robert G. Patzer
Monitoring Systems Research and Development Division
  Environmental Monitoring and Support Laboratory
                Las Vegas, Nevada
  ENVIRONMENTAL MONITORING AND SUPPORT LABORATORY
       OFFICE OF RESEARCH AND DEVELOPMENT
      U.S. ENVIRONMENTAL PROTECTION AGENCY
            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.
     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.
                                    ii

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                             ABSTRACT
     The relative risks to man. from radionuclides released to the environ-
ment depend heavily on their accumulation or concentration by aquatic
organisms.  The organisms which accumulate those radionuclides present
in the environment may be useful as indicators for environmental moni-
toring purposes.  In addition, these organisms may be directly in food
chain pathways to humans.
     Literature is reviewed and summarized in regard to biological concen-
tration of radionuclides in, freshwater and marine environments.  Concen-
tration factors for elements found in organisms are tabulated for plants,
invertebrates, and fish in marine and freshwater environs.  Literature is
also reviewed on models developed to calculate the possible radiation dose
delivered to humans from radionuclides released into aquatic environments.
The model approaches summarized range from simple generalized forms which,
at best, give order of magnitude estimates to detailed models for a specific
area which may be used to guide waste discharge practices.
                                 iii

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                        TABLE OF CONTENTS
                                                                  Page
Disclaimer                                                          ii
Abstract                                                          iii
List of Figures and Tables                                          vi
Acknowledgment                                                    vii
SECTIONS
  I.  Introduction                                                  1
 II.  Summary                                                       2
III.  Conclusions                                                   3
 IV.  Recommendations                                               5
  V.  Objectives and Approach                                       8
 VI.  Results                                                       12
        Concentration Factors                                       12
        Indicator Organisms                                         21
        Environmental Studies                                       24
        Radiation Pathway and Dose Models                           28
        Critical Pathway Approaches                                 31
        Specific Activity Approaches                                43
VII.  References                                                    50
                                 iv

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                    LIST OF FIGURES AND TABLES

 FIGURES                                                       Page

 1.  General Steps in Critical Pathways Evaluation for          33
     Aquatic Environments
 TABLES

 1.  Comparison of Critical Concentration Factors from          13
     Different Sources—Marine Plants

 2.  Comparison of Critical Concentration Factors from          14
     Different Sources—Marine Animals

 3.  Marine Plants—Critical Concentration Factors              15

 4.  Marine Invertebrates—Critical Concentration               15
     Factors

 5.  Marine Fish—Critical Concentration Factors                15

 6.  Freshwater Plants—Critical Concentration Factors          17

 7.  Freshwater Invertebrates—Critical Concentration           19
     Factors

 8.  Freshwater Fish—Critical Concentration Factors            20

 9.  Relative Abundance of Radionuclides in Four Species        24
     of Mollusca from the Same Environment

10.  Ranges of Element Concentration Factors in Marine          25
     Organisms

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                            ACKNOWLEDGMENT
     The technical assistance of Patricia L. Foster in summarizing
information from the literature and in preparing this paper is
greatly appreciated.
                                   vi

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                            SECTION I
                          INTRODUCTION
     The relative risks to man from radionuclides present in water
depend heavily on their accumulation or concentration by organisms
living in that water.  Organisms which accumulate those radionuclides
present in the environment may be useful as indicators for environ-
mental monitoring purposes.  In addition, these organisms may be
directly or indirectly in food chain pathways to humans.  The assess-
ment of the potential human effects resulting from radionuclide
releases to aquatic environments requires an understanding of the
fate of the radionuclides in various environments.  Of particular
interest is the tendency for many organisms to extract and accumu-
late trace materials from their environment.  This tendency is
commonly measured in terms of a concentration factor (CF).  The
CF is defined as the ratio of the concentration of an element in
an organism or its tissues to that found in ambient water.  While
this definition has some deficiencies, it provides a convenient
means to compare the relative accumulation of substances in various
organisms.  Given the CF and other related parameters, mathematical
models can be developed to provide estimates of the radiation dose
to humans from the consumption of foods derived directly or indirect-
ly from aquatic environments contaminated with radionuclides.

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                          SECTION II
                           SUMMARY
     Literature is reviewed and summarized in regard to biological
concentration of radionuclides in freshwater and marine environments.
Concentration factors for elements found in organisms are tabulated
for plants, invertebrates, and fish in marine and freshwater environs.
The range of concentration factors reported from environmental studies
is given, and potential sources for variability in concentration
factor determinations are discussed.  Elements for which no data
were found in the literature are identified.
     The potential for using producer, primary consumer and higher
order consumer organisms as biological indicators of environmental
pollutant levels is discussed.  Some research efforts in this area
have been reported; however, no reliable pattern has emerged upon
which to base a general monitoring program.
     Considerable effort has been expended toward developing methods
to calculate the possible radiation dose delivered to humans from
radionuclides released into aquatic environments.  Most of such
work involves the use of mathematical models in which specific environ-
mental information provides many of the required parameters.  While
many approaches are summarized in this report, most may be classed as
either critical pathway or specific activity methods.  The approaches
summarized range from simple generalized forms which, at best, give
order of magnitude estimates to detailed models for a specific area
which may be used to guide waste discharge practices.

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                              SECTION III
                              CONCLUSIONS
1.  Concentration. Factors
    Variability in the concentration factors reported for similar
organisms from different but similar environments appears to preclude
the use of general concentration factors to assess the current or
previous levels of radionuclides in any particular aquatic environment.
Although many freshwater and marine organisms accumulate or concentrate
radionuclides present in an aquatic environment, the concentration factors
reported in the literature indicate that local conditions strongly affect
concentration factors for organisms.  Even for a given area the concen-
tration factor for a given organism can be expected to vary with changing
local conditions; for example,  season, water temperature, and total
biomass present.
2.  Preliminary Estimates
    The unit-rad contamination factors, discussed under RECOMMENDATIONS,
page 5, are useful in making preliminary assessments of a situation.
Further assessment will require field studies to evaluate the situation
in aquatic environments where problems are anticipated.  Each body of
water has mixing characteristics which are unique in place and time.
Moreover, radionuclides introduced into and diluted within aquatic environ-
ments can remain in solution or suspension, precipitate and settle on the
bottom, or be reconcentrated by plants and animals.  The species and popu-
lation density of plant and animal life present in a body of water are
also unique in place and time.  In addition, the physical, chemical
and biological interactions of a radioisotope are influenced by the
presence or absence of other isotopes not only of that element but also
of other elements.
3.  Models for the Environment
    Monitoring networks for aquatic environments can provide specific
information required in models.  Large numbers of environmental models

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have been developed for use in calculating potential radiation doses to
humans following release of radionuclides to aquatic environments.  The
radiation exposure of humans through environmental pathways has been
studied extensively from almost the inception of the nuclear industry.
Even the simplest of these models requires considerable information
concerning the particular environment and population at risk in order to
complete a risk or radiation dose assessment.  Although simple or complex
models may be written in generalized forms, the input parameters are
specific for the environment of interest.  The number and degree of
complexity of models reported in the literature allow selection of a
model to use for making calculations based upon the amount of information
available on the environment of interest.  The more extensive the data
base, of course, the more reliable can be the information derived from the
models.
4.  Uses for Aquatic Organism Samples
    Aquatic organisms can provide valuable information on radionuclide
cycling in the environment.  Because aquatic organisms concentrate radio-
nuclides released to their environment to a considerable degree, even if
variable, they provide valuable environmental monitoring samples which
(1) indicate whether radioisotopes are concentrating within food chains
leading to man; (2) delineate the geographical areas involved in a potential
problem; (3) provide valuable information on whether additional control
measures are needed; and (4) demonstrate environmental benefits gained
when control measures are applied.

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                           SECTION IV
                         RECOMMENDATIONS
1.  Field Studies
     This program was limited to a general literature review for data
and models related to the behavior of radionuclides in aquatic environ-
ments.  It was not within the program scope to evaluate the accuracy or
reliability of information reported.  The wide range in concentration
factors found in the literature leads to the recommendation that,
initially, field studies be conducted to evaluate the situation in
each aquatic environment where problems are anticipated.  A sufficient
body of information exists to make preliminary evaluations of most
environments; however, data from detailed field studies would supple-
ment this information and, perhaps, provide a basis for recommending
that less detailed studies be required to adequately assess hazards
of radionuclides in other aquatic environments.
2.  Preliminary Evaluations
     It is recommended that the "unit-rad contamination factors"
as published in Lawrence Livermore Laboratory (LLL) reports be used
to make preliminary evaluations of radionuclide releases to aquatic
environments.  These factors are discussed under RESULTS.  Areas
where detailed field studies should be carried out can be selected
on the basis of the preliminary evaluations.  The LLL program is
a continuing effort and revised information is incorporated into
their system as more specific data become available.  The reports
contain a comprehensive listing of aquatic concentration factors and
population dose estimates.  The LLL program approaches environmental
contamination by radionuclides and the resultant radiation dose to
man from the standpoint of element specific activity—the biological-
exchangeable-pool-i-of-elements concept.  Using this approach, the
passage of a radionuclide through the biosphere is presumed to be
governed by the same factors that govern the distribution of the
related stable element isotopes within the biological exchangeable
pool.  It is assumed that the radionuclide is biologically no more

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available than the related stable isotopes within  the  environment.  This
approach should be valid for the types  of radionuclide releases  anticipated
in the nuclear industry—low-level wastes diluted  and  dispersed  in  large
bodies of air and water.
     The product of the LLL program is  a value for each isotope  called
the "unit-rad contamination in water  (F.)11 for both  freshwater and  sea
                                        f\
water.  This factor is defined as the initial concentration  of a radio-
isotope in water which would yield a 30-year integrated dose of  1 rad
to a specific designated tissue of the  standard man.   In most cases F.
                                                                     A
values for infants are also estimated.  The assumptions in the many
steps involved in reaching F  values are basically conservative  in
                            £\
nature, i.e., they are aimed toward obtaining F  values for  the  worst
                                               A
situation that could develop.
3.  Monitoring Network Design
     Although considerable information  is available  for making generalized
estimates of the radiation dose to people from radionuclides released  to
aquatic environments, information relevant to specific areas generally
has not been collated.  For example, seafood distribution and consump-
tion patterns for an area are generally available  through food distribu-
tors and dietary surveys, but have not  been collated for making  potential
radiation dose estimates.  Before such  information is  tabulated,  however,
a decision should be made on its desired accuracy  and  validity.   The
ultimate objective should be to obtain  radiation dose  estimates  with a
given degree of reliability.  In order  to obtain this  objective,  each
data base for model parameters has a defined degree  of reliability.
Such considerations are part of monitoring network design criteria  which
are being developed at the EPA's Environmental Monitoring and Support
Laboratory at Las Vegas.  At present design criteria are being developed
for air monitoring networks.  These efforts should be  extended to encompass
design criteria for gathering information needed to assess the potential
radiation dose to people from radionuclides released to aquatic  environ-
ments.

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4.  Emphasis for Future Investigations
     Some investigations on critical pathways indicate  that the biomass
and sediments may be neglected as  a depot of radioactivity in a fresh-
water aquatic system, although as  a rule of thumb it  can be assumed
that there is a thousandfold average concentration of all radionuclides
in the biomass and that the bottom sediment has an average concentration
a hundredfold greater than the water concentration.   Apparently, the
biomass and sediment have a small  potential for transferring radioisotopes
to people when compared with direct water intake.  This concept, which has
developed from tracer radioisotope studies in freshwater systems, has
important implications in assessing freshwater pollutants of many types.
The concept should be pursued in depth.  Perhaps priority attention
should be directed toward the oceans where the majority of all pollutants,
however released, will ultimately  reside.  Some pollutants in the oceans
will be returned to man through seafoods; however, the seafood yield of
the world's oceans has been decreasing annually for many years.  It
appears that more emphasis should  be placed on studying pollutant
effects in ocean environments.  Biological effects of released
radioisotopes on ocean biota are not expected to be observable
because of the low concentrations  expected.  However, radioisotopes
already in the environment and those to be released in the future can
provide valuable information" on the rates of pollutant transfer from
land sources to the ocean and on pollutant mixing patterns and fate
in the oceans.  Since man depends  on the oceans for most of his
oxygen, and, potentially, a large  portion of his food, he has a
vital stake in understanding and managing the productivity and
well-being of the seas.

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                             SECTION V
                      OBJECTIVES AND APPROACH
     The objectives of this project were to survey  literature  on
aquatic environments and:
     1.  Tabulate concentration factors for radioisotopes
         which may be released to the environment through
         man's activities and yield a significant radiation
         dose to man through aquatic pathways,,
     2.  Identify indicator organism groups with high concen-
         tration factors for potential use in monitoring and
         assessment efforts, and
     3.  Survey environmental models used for calculating the
         potential radiation dose to man through aquatic
         pathways.
     A concentration factor (CF) is defined as the ratio of the
concentration of an element in an organism or its tissues to that
found in ambient water.  In reviewing and evaluating the literature,
it was found that long-lived radioisotopes with CF's of about  10,000
or greater in biota were of primary importance for identifying
indicator organisms and for estimating potential radiation doses to
man.  A CF of 10,000 or more is herein defined as the critical CF,
and data on critical CF's are summarized in the following sections.
The value of 10,000 was selected to concisely summarize data which
are most pertinent to hazards assessment.   Data on CF values less
than 10,000 can be obtained from the referenced literature.  In
addition to isotopes with critical CF's, the CF's for several  elements
of current interest are included in the data summarized—even  though
the CF's are often relatively small.  However, small amounts of some
of these elements are considered to be much more dangerous to  man than
their CF's might appear to indicate.  Furthermore, their potential
biological effects on man warrant concern, vigilance and control.
These elements include plutonium, strontium, cesium, uranium,  and
iodine.  Since CF's for many isotopes were not identified in the

                                 8

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literature, and because the various isotopes of the same element
generally exhibit the same chemical characteristics, the CF for
one isotope is presumed to be applicable for other isotopes of
the same element.
     Indicator organisms may be useful in the following categories:
     1.  Alert.  Indicate that radioisotopes are concentrating
         within food chains which could lead to man.
     2.  Assess.  Evaluate the potential magnitude of intake by
         man and note trends in aquatic organism concentrations
         (increasing, decreasing, or stable).
     3.  Del-ineate.  Show the geographical area involved in the
         potential problem.
     4.  Control.  Decide whether control measures are needed and,
         if they are applied, demonstrate the environmental
         benefits gained.
     Many models have been reported in the literature for calculating
the potential radiation dose to man through aquatic pathways from
radionuclides released to the environment.  Several of these models
are described in this report.
     The approach was to survey literature on aquatic pathways and
to summarize CF's for elements within organisms which live in various
aquatic environments.  This information, together with information on
the radioisotopes released to the environment from nuclear activities,
gives a data base to identify which radioisotopes may be important
in various food chains leading to man, to identify indicator organisms
with potential value in monitoring and assessment efforts, and to
select appropriate models to make calculations of potential radiation
doses to man.  The type of data available on the environment in question
determines which type of model is appropriate.
     In addition to the critical CF criteria, the following guidelines
were formulated to focus the literature review on information relevant
to the objectives:

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1.  Primary attention is given to those radioisotopes which may
    yield a significant radiation dose to man through
    aquatic pathways.
2.  Long-term and low-level releases of radioisotopes to the
    environment are of primary interest.  Therefore, CF's
    for rathet stable release rates and water concentrations
    are applicable.  The nuclear industry guidelines for
    radioisotope discharges are of this nature.  Concentra-
    tion factors and environmental half-times for accidental
    releases (pulse labeling) are extremely dependent on
    local environmental conditions prevalent at the particu-
    lar time of release and are not amenable to generaliza-
    tion.  Therefore, time-dependent variables such as biolo-
    gical half-times and uptake rates are not identified in
    this report.
3.  Certain types of data necessary for hazards assessment are
    beyond the scope of this report.  The CF for a radioisotope
    bears little relationship to the potential hazard to man.
    Extensive data are available in the literature and in
    federal and international radiation standards on the
    relative hazards of radioisotopes based on decay emissions
    and energies, biological and physical half-lives, biological
    deposition sites, etc.  These data are given for soluble
    and insoluble forms of the isotopes and for various routes
    of exposure.  While such data may not be applicable for
    isotopes incorporated in unknown chemical forms in aquatic
    organisms, no attempt is made in this review to identify
    the chemical forms of radioisotopes within biota.  The
    published data on biological and physical parameters for
    isotopes are not rei.terated,
4.  While certain radioisotopes are considered more hazardous
    than others, none were excluded frorr a search for concentra-
    tion factors.  The exclusion from such a search may lead to
    unwelcome uncertainties in the assessment of a situation
                        10

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         involving a mixture of radionuclides.  In addition, it
         is difficult to predict the kinds and amounts of radio-
         nuclides to be released in the future from nuclear
         facilities, medical facilities, and various laboratories.
     This report serves to present reported information on parameters
needed to estimate radiation doses to man from various radionuclides
which may be discharged to a given sector of an aquatic environment.
Many parameters are extremely location-dependent and, therefore, are
part of this literature survey only in that they are identified and
evaluated in the dose computation models which are referenced.  These
parameters include such things as dilution factors, dispersal rates,
mixing depths, biota prevalence, the organisms and their tissues
directly consumed by man, and the indirect contributions from organisms
in food chains.
                                11

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                            SECTION VI
                              RESULTS
 CONCENTRATION  FACTORS
      The term  concentration factor  (CF) has been defined  (Thompson et al. ,
 1972)  as "the  ratio  of  the concentration  of an element  or radionuclide in
 an aquatic organism  or  its tissues  to that in the surrounding water  under
 equilibrium or steady-state conditions."  This definition does  not allow
 for the fact that  aquatic organisms normally  derive  their nutrients  from
 a variety of sources such as  food, water, and suspended or deposited
 sediments.   Polikarpov  et al.  (1966) noted this restriction in  part  by adding
 that "the capacity of an organism to accumulate radioactive substances is
 expressed by the ratio  of its  radioactivity to that  of  the aqueous medium
 or the preceding food link in which the radionuclide was  concentrated."

      This limitation is especially apparent with certain  benthic  organisms
 that live in bottom  sediments  and feed on debris (for example,  some
 mollusca).   Comparison  of the  trace element concentrations found  in  the
 tissues of  these organisms with  the concentrations found  in open  sea-
 water  is not a truly valid means to determine concentration factors.
 Yet, Lowman et al, (1971) describe many benthic organisms which are efficient
 accumulators of trace elements from water and are an important  fraction
 of the total biomass in marine areas of economic importance.

     Fewer  problems  are encountered in determining a CF for phytoplankton
 because there  are  no intervening trophic  levels between water and their
 nutrient source.   Data  on marine plants  (Thompson et al. , 1972) from the
 Lawrence Livermore Laboratory  (LLL, formerly  the Lawrence Radiation
 Laboratory)  do not distinguish between phytoplankton and  benthic  or
 macrophytic algae, nor  between zooplankton and macroinvertebrates.  This
 ambiguity could lead to misinterpretation of  what organisms are of most
 importance  in  a particular situation.  Table  1 is a  comparison  of CF data
from the LLL report to CF values  for benthic algae and phytoplankton
                                 12

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reported by  the  National Academy of Science/National  Research Council
(NAS/NRC, 1971).   In general, data from the latter report  indicate that
CF's for phytoplankton are higher (sometimes by 1 to  2  orders of magnitude)
than those for benthic algae.  Furthermore, the LLL average measured values
tend to be lower than the NAS/NRC phytoplankton data, indicating that
the LLL data are weighted towards benthic and/or macrophytic  algae.   On
the basis of NAS/NRC data for phytoplankton, the CF's for  aluminum,  cerium,
copper, silver,  and zinc appear to be 10,000 or greater—values  higher  than
the CF's listed  in the LLL report (see Table 1).

       TABLE 1.   COMPARISON OF CRITICAL CONCENTRATION FACTORS FROM
                  DIFFERENT SOURCES—MARINE PLANTS (VALUE LISTED  X
                  10  = CF)
Element
Sc
Mn
Fe
Y
Zr
P
Pb
Al
Ce
Cu
Ag
Zn
Pu
Thompson ei, al. (1972)
Marine Plants
Derived ^
100.0
20.0
50.0
10.0
10.0
2.8
1.0
0.6
5.0
1.0
0.2
1.0
0.35
Maximum ,, ,.
Measured
25.0
22.0
0.9
—
1.6-3.5
Average , .
Measured
5.5
0.73
3.0-4.0
5.0-10.0
0.6-0.7
—
0.9-3.0
NAS/NRC (1971)
Benthic
Algae
2.0
2.3
4.8
0.48
2.2
10.0
0.7
15.0
0.67
0.1
0.41
1.3
Phytoplankton
2.0
4.0
4.0-45.0
1.0
60.0
3.0-34.0
40.0
100.0
90.0
30.0
23.0
1.5-20.0
2.6
       Dash  (—)  indicates no data in reference cited.
       (a)r
       (b)
Derived on the basis of stable element concentrations.
Measured in radioisotope studies.
          Average of values from radioisotope studies.

      In Table 2 marine animal data are  listed  in a similar manner from the
 the above LLL and NAS/NRC reports.  Data  from  the former on marine inverte-
 brates (crustaceans and mollusca) can be  compared with values given for
 zooplankton, mollusc muscle and  crustacean muscle in the NAS/NRC report.
 The latter data indicate two additional elements  (ruthenium and aluminum)
with critical CF's which were not shown in the LLL data.
                                    13

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         TABLE 2.  COMPARISON OF CRITICAL  CONCENTRATION FACTORS FROM
                   DIFFERENT SOURCES—MARINE ANIMALS (VALUE LISTED X
                   103 = CF)
Element
P
Fe
Zn
Ge
Cd
Te
Hg
Sc
Mn
Ta
Tl
Po
Ru
Al
Thompson et al. (1972)
Marine Invertebrates
(a)
Derived v '
28.6
20.0
100.00
16.7
250.0
150.0
33.3
10.0
10.0
16.7
15.0
20.0
2.0
0.06
Average
Measured
30.0
—
50.0
—
—
—
—
—
0.4
—
—
3.0
0.1-1.0
_— .
NAS/NRC C197
Zooplankton
13.0
25.0
8.0
	
—
—
—
1.0
1.5
—
—
—
34.0
9.0
Mollusca
6.0
9.6
11.0
	
—
—
	
—
12.0
	
—
—
0.003
12.0
•>
Crustaceans
24.0
2.4
2.0
	
	
	
	
0.3
1.9
	
—
—
0.1
10.0
       Dash (—) indicates no data in reference cited.
       (a)r
       (b)
Derived on the basis of stable element  concentration.
Average of values  from radioisotope studies.
     Critical CF's  for marine organisms from the literature reviewed are
listed in Tables 3,  4, and  5; those for freshwater organisms are listed in
Tables 6, 7, and 8.  Although much data exists in the literature, very little
has come from environmental studies with radionuclides.  The most compre-
hensive list of CF's found  is contained in the LLL report  (Thompson.@t al.3
1972).  These data  resulted from a multi-year effort which is continuing
to update and extend the  data base.  This effort is part of a project which
has the objective of assessing the radiation dose to people from radio-
nuclides released to aquatic environments.  The dose model being developed
will be discussed later.

     Harrison (1967) suggests that there are two classes of analytical
techniques used to  determine CF's, a distinction which was also incorporated
into the LLL report by Thompson et al.  (1972).  These two classes are:
                                     14

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     1.   CF's obtained  from measurements  of stable element concentration
          in the organisms and water and
     2.   CF's obtained  from measurements  of the radionuclide content
          of the organisms and water.
Theoretically, the CF values obtained  by  these two methods should be
identical,  but in practice, both methods  are subject  to  sampling and
analytical  errors.  Jinks and Eisenbud (1972)  describe several sources of
variability in reported values for CF's,:
          TABLE 3.  MARINE PLANTS—CRITICAL CONCENTRATION FACTORS
                     (VALUE LISTED X 103 = CF)
Element
N
Sc
MH,
Fe
Y
Zr
In
La(e)
Hf
Tl
Bi
P
Pb
Pu
Sr
Cs
U
I
Chapman
at al. (1968)
10.0
10.0
10.0
50.0
10.0
10.0
100.0(d)
10.0
10.0
100.0
—
—
	
1.0
0.013
0.02
1.0
4.0
Thompson & t al. (1972)

Derived ^
10.0
100.0
20.0
50.0
10.0
10.0
—
—
—
—
—
	
0.35
0.013
0.02
0.067
4.0
Measured
_ _
—
5.5
0.73
—
—
--
—
—
—
—
	
1.0
0.01
0.05
—
1.0
For Contaminated Environment 1CJ
Minimum
__
—
5.5
	
—
—
—
—
—
—
0.21
	
0.77
0.009
0.01
—
—
Maximum
__
—
25.0
__
—
—
—
—
	
—
22.0
__
3.5
0.2
0.17
—
—
Average
	
—
—
	
._<_
—
—
—
	
—
4.0
5.0-10.0
3.0
0.025-0.04
0.04-0.07
—
1.0
        Dash (—) indicates no data in reference cited.
          Derived on the basis of stable element concentrations.
        (b)
        (c)
        (d)
        (e)
Measured in radioisotope studies.
Measurements made  in environmental studies.
No data available, estimate based on worst possible case.
For lanthanide series.
                                      15

-------
     TABLE  4.  MARINE INVERTEBRATES—CRITICAL CONCENTRATION
                 FACTORS  (VALUE LISTED X  103  = CF)
Element
M
P
Fe
Zn
Ge
Cd
In
Sb
Te
Hg
Bl
Sc
Mn
Ta
Tl
Po
Pu
Sr
Cs
U
I
Chapman
BE al. (1968)
17.0
28.6
20.0
100.0
16.7
250.0
100.0
16.0
—
100.0
—
1.0
5.0
0.1
150.0
0.4
0.286
0.006
0.02
0.33
0.05
Thompson 3 t al. (1972)
Derived 
-------
      TABLE 6.  FRESHWATER PLANTS—CRITICAL  CONCENTRATION FACTORS
                (VALUE LISTED X 103 = CF)
Element
N
P
Sc
Mn
Y
Zr
In
La(d)
Hf
Tl
Sb
Zn
Ru
Ce
Pu
Sr
Cs
U
I
Chapman
et al. (1168)
25.0
100.0
10.0
10.0
10.0
10.0
100.0
10.0
10.0
100.0
—
4.0
2.0
10.0
1.0
0.5
0.2
1.0
0.1
Thompson et al. (1972)

(al
Derived v '
12.5
10.0
10.0
10.0
5.0
1.0
__
5.0
1.0
__
1.5
1.0
0.2
5.0
0.35
0.5
0.08
1.0
0.04
Measured

500.0
—
10.0
—
—
__
—
—
	
—
20.0
2.0
4.0
—
0.5
0.5
0.0005
—
For Contaminated Environment (c)
Minimum

100.0
—
	
—
—
__
—
—
	
—
—
1.8
2.0
—
0.24-0.33
0.07-0.47
0.0004
—
Maximum
„
850.0
—
	
—
—
__
—
—
	
—
—
12.0
10.0
—
0.28-0.69
0.87-1.2
0.0007
	
Average
_.
270.0,
—
—
—
—
	
—
—
	
—
130.0
	
—
—
0.6
—
0.0006

  Dash (—) indicates no data in reference cited.
  (a)r
  (b)
  (c)
  (d)
Derived on the basis of stable element concentrations.
Measured in radioisotope experiments.
Measurements made in environmental studies.
For lanthanide series.
1.  Because of the higher concentration of stable mineral elements
    in  seawater, the radionuclide CF's for most freshwater organisms
    are much higher than those  for similar seawater biota.
2.  Radionuclide accumulation and concentration in various  tissues of
    an  organism may differ considerably.   Data illustrating this
    variability were published  by Harvey  (1967).
3.  Error originates from the practice of  analyzing the stab.le
    elemental content of biota  and then calculating the CF  from general
    literature data on the elemental  concentrations in freshwater or
    seawater.
4.  Physiological factors (same as  those discussed by Harrison,  1967):
    species  differences, age, size, reactions to changes  in temperature,
                                 17

-------
         and chemical characteristics of the environment vary.   The concen-
         tration of an element in tissue may be controlled hoffieostatically.  Such
         control of potassium and calcium concentrations in organisms may
         strongly affect CF's for their chemical congeners, cesium and
         strontium, respectively,  'dftiile such effects are well-known for
         higher animals, they may occur in many simple organisms.  For
         example, the concentration of manganese in Hudson River fish
         remains constant in spite of large variations in the water concen-
         tration of manganese.
     5.  A CF with respect to water may be influenced by the pathway through
         which the nuclide reaches the organism.  Although an organism may
         not directly concentrate an element from water, some element in its
         food chain may have performed the concentrating function.  Further-
         more, the food source for an organism may vary with seasons and be
         affected by many environmental factors.
     6.  Short-term variations in the concentration of stable elements or
         radionuclides in environmental media may result in nonequilibrium
         conditions between organisms and the environment at the time of
         measurement.  The concentrations of elements with long effective
         half-times in the tissue may reflect an earlier high, concentration
         in the environment rather than that existing at the time of capture.

     Additionally, some studies indicate an apparent selectivity by a few
organisms for certain radionuclides over their stable counterparts.  Pre-
sumably, this is related to differences in physio-chemical availability
or to different pathways of uptake.  For example, data from the LLL report
(Thompson et al. , 1972) show that the following elements have experimentally
measured CF values (based on radionuclide concentrations) that are greater
than the derived values (based on stable element concentrations) by 1 or
more orders of magnitude:
                                    18

-------
       Biota
                         Elements  with CF measured  value
                               >10 x derived value
Marine:
      Plants
      Invertebrates
      Fish

Freshwater:
      Plants

      Invertebrates
      Fish
                         Lead, Plutonium
                         Strontium
                         Strontium
                         Phosphorusj  Chromium, Zinc,  Ruthenium,
                         Cesium
                         Sodium,  Chronium
                         Sodium,  Chronium, Strontium, Cesium,
                         Polonium
    TABLE 7.   FRESHWATER INVERTEBRATES—CRITICAL CONCENTRATION
               FACTORS  (VALUE LISTED X 103  = CF)
Element
N
P
Mn
Zn
Ge
In
Sb
Te
Hg
Tl
Po
Pu
Sr
Cs
U
I
Chapman
et al. (1968)
42.5
100.0
40.0
40.0
16.7
100.0
16.0
—
100.0
100.0
0.4
0.29
0.7
1.0
0.3
0.025
Thompson &k al. (1972)

Derived (a)
150.0
100.0
40.0
10.0
—
—
	
100.0
100.0
10.0
20.0
0.1
0.1
0.1
0.1
6.005
Measured
__
20.0
90.0
10.0
—
—
—
—
—
—
—
—
—
—
0.06
—
For Contaminated Environment *•<-)
Crustacean
__
10.0
—
4.0
—
—
—
—
—
—
—
—
—
—
0.06
	
Mollusca
__
20.0
93.0
20.0
—
—
—
—
—
—
—
—
—
—
—
—
Average
__
20.0
90.0
10.0
—
—
—
—
—
—
—
—
—
—
0.06
— —
 Dash (—) indicates no data in reference cited.
  (a)
  (b).
  (c)'
Derived on the basis of stable element concentrations.

Measured in radioisotope experiments.
Measurements made in environmental studies.
                                 19

-------
          TABLE 8.   FRESHWATER FISH—CRITICAL CONCENTRATION FACTORS
                    (VALUE LISTED X 103 =  CF)
Element
N
P
Nb
In
Tl
Np
Ta
Pu
Sr
Cs
U
I
Chapman
et al. (1968)
150.0
100.0
30.0
100.0
100.0
100.0
0.1
0.01
0.04
0.001
0.01
0.001
Thompson et al. (1972)

Derived (a)
150.0
150.0
30.0
	
10.0
—
30.0
0.003
0.005
0.4
0.01
0.015
Measured
__
100.0
—
—
—
—
—
—
0.03
2.0
0.002-
— —
For Contaminated Environment ^c)
Minimum

0.5-30.0
—
—
—
—
—
—
0.003
0.39-1.6
—
— —
Maximum
__
55.0-100.0
—
	
—
—
—
—
0.17
1.1-4.7
—
—
Average

50.0
—
	
—
—
—
—
0.058
2.4-3.9
0.002
	
      Dash (—)  indicates no data in reference cited.
         Derived on the basis of stable element concentrations.
       (b)
       (c)
Measured in radioisotope experiments.
Measurements made in environmental studies.
     In general,  the  elements that are concentrated significantly in aquatic
organisms  (Tables 1 to  8)  were grouped by Lowman et dl.+  (1971)  into at least
one of five categories:
     1.  Structural elements:  Carbon, Nitrogen, Phosphorus,  Silicon,
         Calcium, Strontium.
     2.  Catalyst elements:   Iron, Copper, Zinc, Manganese,  Cobalt, Nickel,
         Chromium, Cadmium,  Silver.
     3.  Elements easily hydrolyzed at seawater pH:   Aluminum,  Gallium,
         Scandium, Yttrium,  Cerium, Plutonium, Titanium, Zirconium.
     4.  Heavy halogens:   Bromine, Iodine.
     5.  Heavy divalent ions:  Barium, Radium, Rubidium.
     Supportive data  on concentration factors for  several elements in various
biota have not been identified.  For seawater these elements are indium,
tellurium, and bismuth.   In freshwater the elements with least known data
are  indium,  thallium, bismuth, tellurium, and germanium for inverte-
brates  and neptunium for fish.
                                    20

-------
INDICATOR ORGANISMS
     Biological indicators are defined  (Rice, 1965) as  those  organisms
which concentrate relatively large  amounts of specific  radionuclides,
thereby making it possible to detect  the presence  of  those  isotopes
in the environment through an analysis  of the organisms.  Additional
qualifying characteristics of "indicators" are  listed by Feldt  (1971).
The organism must:
     1.  be readily  attainable at all times,
     2.  have a sufficient CF for several radionuclides
         of interest,  and
     3.  yield measurement results  in a form which makes
         it possible to assess the  radiation dose  to
         man.
     The concentration of elements  in aquatic ecosystems is highly
variable.   CF's  are  related  to the  chemical  content of  the  water,
and it  is  impossible to draw general  conclusions from elemental
composition of  organisms without simultaneous reference to  data
from their environment. In  spite of  this, however, Polikarpov
(1966)  states  that it is generally  recognized that CF's (taken  in
the equilibrium state) of each separate radionuclide  for closely
related species  of marine plants and  animals (i.e., same genus
or family) do not differ significantly  in different seas and  oceans.
There  appears  to be  less acceptance of  a second generalization  attri-
buted  to Polikarpov:  that CF's  for radionuclides  which are present
in water in microquantities  are  similar for  related marine  and  fresh-
water  organisms.   It has been more  frequently observed  that the fresh-
water  CF for  a particular isotope by  a  particular  type  of organism
is higher  than  that  in a marine  environment  (due to differential
isotopic dilution in these  two basic  systems).
     A  logical, universal biological indicator  of  radioactivity in  any
aquatic system would appear  to be mixed phytoplankton.   Those elements
that are concentrated by at  least  a factor  of  1,000 by  marine phyto-
plankton have been tabulated by  the NAS/NRC  (1971).   Unfortunately,
however, photoplankton do not accumulate nuclides  in  the same propor-

                                 21

-------
tions as, for example, fish.  For mixed phytoplankton to meet  the
third qualifying characteristic previously noted, they would have  to
be a predictable component of a food web eventually leading to man.
Even though phytoplankton may remove large amounts of radionuclides
from water, the amount of radioactivity that may be passed up  the
food web will vary with cell mass, cell numbers, and specific  con-
centrations, as well as with efficiency of utilization by ensuing
trophic levels.  Another complication with using mixed phytoplankton
has been described by Feldt (1971):  "It is especially difficult.  . ."
(in rivers, and presumably estuaries and coastal areas too)  "...
to separate the plankton from detritus."  He concludes that while the
concentration of certain nuclides in plankton would help to prove
the presence of these nuclides, it would not give useful information
on the risks these radionuclides present to man because they are not
found in the same concentrations in edible aquatic products.
     With these arguments in mind, it seems natural to fall back to the
Polikarpov C1966)  terminology — that there are "biological indicators"
(as previously defined) and there are "biological accumulators" (of
which mixed phytoplankton would be an example).  By the guidelines
set forth for this report, the "accumulators" would be useful only
in the dat-ineatirOn of the geographic area involved in a potential
hazard to man.  "Biological indicators" would be required for the
other categories:  alert (indicate that radioisotopes are concentrating
within food chains that may lead to a hazard for man); assess  (give
indication of the potential magnitude of intake by man); or control
(indicate whether or not control measures are effective).
     In reviewing literature on biological indicators and accumulators,
organisms were separated into the broad categories of producers and
consumers.

Producers
      In  general,  the literature reviewed  does not present  sufficient
information for determining which, specific producer  organism
is an accumulator  or an  indicator for a particular radioisotope.   Most
compilations  of CF's have categorized producers very broadly  and lump
                                  22

-------
together phytoplankton, littoral and benthic seaweeds and algae; submerged,
floating, and emergent angiosperms; etc.  The only generally accepted
generalization concerning producers, according to the IAEA  (1971), is that
phytoplankton tend to concentrate activation products to a  greater extent
than fission products.  This reference also notes that while the degree of
concentration of activation products is highest in the primary producers,
intermediate in the herbivores and lowest in the carnivores, the primary
producer's concentration in comparison to fission products  is more subject
to variation and rapid fluctuation in response to changes in the ambient
contamination level.  The concentration responses in the higher trophic
species are more sluggish and less predictable.

Primary Consumers
     Few valid generalizations can be made from the literature about the
indicator value of tropic levels.  For example, filter feeding animals have
been shown to concentrate different radionuclides even while they are living
in the same microenvironment.  (For example, see Table 9.)  Also, the distri-
bution of a radionuclide within a particular organism may vary greatly; e.g.,
even though scallops were found to be excellent accumulators of manganese-54,
most of  the activity was present in the kidney, which is not eaten by man,
and relatively little was present in the muscle.  Bryan et ai.  (1966) reported
that CF's generally decrease from lower to higher trophic levels because of
radioactive decay, mode of uptake, and turnover rates.  A summary of the
ranges reported for element CF's in marine organisms at various trophic levels
is given in Table 10.

Higher-Order Consumers
     In  general, the same limitations that have already been noted apply to
organisms in the higher trophic levels.  Feldt (1971) argues that fish are
excellent indicators in freshwater systems because of their availability,
their measurable  (although not usually maximal) CF's for a  wide variety of
 isotopes, and their applicability to assessment of hazard to man.   For
 the same reasons, he also supports the use of mussels as the indicator
 organism in river estuaries.
                                   23

-------
 TABLE 9.  RELATIVE ABUNDANCE OF RADIONUCLIDES IN FOUR SPECIES
           OF MOLLUSCA FROM THE SAME ENVIRONMENT (a)

Scallops
Oysters
Clams
Mussels
144Ce
4
2
1
1
106^
Ru
3
3
2
2
137r
Cs
2
(b)
(b)
(c)
54Mn
1
(c)
(c)
(c)
65Zn
5
1
(c)
(b)
 (al
 v 'Data from Bryan et al.  (1966).
    Present but not relatively abundant.
 (c)
    Indication of presence

      Studies on the uptake of radionuclides by various  fish in the Columbia
 River (Foster and McCannon,  1962) have  shown that  there is  a wide  variation
 in uptake between individual specimens  of  the same species, thus requiring
 large samples for statistical validity.  Uptake also  changed rapidly with
 the season.   The most pronounced variations were found  with short-lived
 radionuclides that were necessarily acquired via food chains.
      In  summary,  it appears  that few generalizations  can be made concerning
 indicator organisms.   Most studies have identified accumulators with varying
 degrees  of effectiveness, but  still there  appears  to  be no  consistently
 reliable pattern.   Relatively  few studies  have  attempted to describe, much
 less  quantify, entire aquatic  ecosystems.   Yet,  at present  this appears to
be  the only way  to  make intelligible recommendations  concerning the identity
of  accumulator and/or  indicator  organisms.
ENVIRONMENTAL STUDIES
     Those studies which have  actually identified  indicator organisms have
been, at  least initially, comprehensive ecosystem  effects studies.  Since
the overwhelming complexity of environmental effects  seriously hinders
effective control, it is accepted practice  to determine  just which factors
are critical (i.e., those which give rise  to the greatest risk) and to
                                  24

-------
                 TABLE 10,   RANGES OF ELEMENT CONCENTRATION FACTORS IN MARINE  ORGANISMS
                                                                                                                (a)
N>
Ui


Ag
Cd
Ce
Co
Cr
Cs
Fe
I
Mo
Mn
>:i
Pb
Ru
Sr
11
Zn
2r
A.I
t*ns1 le
100 — 1,000
11 — 20
100 — 3,300
15 — 740
100 — 500
16 — 50
1,000 — 5,000
160 — 7,000
10 , — 200
20 — 20,000
50 — 1,000
8,000 — 20,000
100 — 1,200
0.1 — 90
200 — 30,000
80 — 3 , 000
200 — 3,000
Cfte
P,.nl,,™
< 100 — 220
< 350 — 6,000
2,000 — 4,500
75 — 1,000
< 70 — 600
16 — 22
750 — 7,000
< 3 — 17
300 — 7,000
25 — 300,
1,000 — 3x10°
< 200 —
0.9 — 54
600 — 10,000
200 — 1,300
< 1,000 — 20.000
Graze
Pl.nfcr™^)
l 1 f i sh
330. — 20,000
W — 2xlOp
40 — 300
24 — 260
6x10 — 3x10
3 — 15
7x10* — 3xl05
40 — 70
30 — 90
3,000 — 60,010
17 — 90
200 — 60,000
10 — 2,400
1.2 — 10
110 — 20,000
50 —
<8QO — 40,000

vl. fcf W
<45 — 900.
<300 — 10
<70 — 1,300
<55 — 3,900
3,000 — 30,000
<2 — 14
270 — 1,600
17 — 90
200 — 60,000
10 — 2,iOO
1.2 — 10
110 — 20,000
50 —
<800 — iO.OOO
predators
Fi ch
— > 10
5 — 12
28 — 560
3 — 30
6 — 10
400 — 3,000
10 — —
200 —
95 — 105
5 — 10,000
10 — --
4 — i
280 — 20,000
5 — —

£q!
-------
exclude all other factors which make no significant  contribution  to the
risk.  For each instance of environmental  contamination with  radioactive
materials, it is initially necessary to identify  the critical radionuclides
with reference to man.  The physical and metabolic characteristics  of  these
nuclides determine which ecological pathways or routes to man are critical.
Since it is generally recognized that some members of the general population
may be more affected than others, it is often necessary to  further  identify
a critical population (Comar and Lengemann, 1966; IAEA, 1971;  Straub,  1960).
     Typical of this approach are studies  (Foster and Soldat,  1966)  of radio-
nuclides discharged to the environment from the Hanford operations.  The
critical radionuclides and routes of exposure from effluents released into the
                         o o      /: c
Columbia River involve     P and   Zn in local fish  and the produce  from
                 O /    ^ £L    O O C\       1O^
irrigated farms;   Na,   As,    Np and     I in drinking water; and the
                                 24
external exposure of swimmers to   Na in water.  The critical population
was determined to be persons who ate unusually large quantities of fish
caught in the river immediately downstream from the  reactors.  For most
of the population, however, drinking water provided  the only significant
source of waterborne radionuclides.

     Parker (1964) maintains that only large-scale producers/users of  radio-
nuclides need to be considered in determining permissible discharge  limits to
freshwater environments.  The use of river water for the dilution of low-
level radioactive wastes is widely practiced.  In addition to the studies
on the Columbia River, other environmental studies in freshwater  environments
have generally indicated that local fish were the critical indicator organisms.

     A study of the Clinch River by the Oak Ridge National Laboratory  (Cowser
et al*3  1963)  showed that the major pathways of exposure were  (1) consump-
tion of contaminated water and fish; (2) consumption of agricultural produce
irrigated with river water; (3) exposure to contaminated water and bottom
sediments directly; and (4) exposure to the buildup  of radionuclides in
sludge and deposits in water systems which utilize the river water.  The
                                        90             137
critical radionuclides identified were     Sr for bone,    Cs for  total
body,    Ru for the gastrointestinal tract, and    I for the  thyroid.
                                  26

-------
     Environmental studies of marine ecosystems generally have been under-
taken in response to two types of situations:   (1) to determine the effects
of high-level discharges from nuclear detonations, and  (2) to determine the
effects of continuous low-level discharges from nuclear facilities.  The
latter situation is of primary interest, and studies of discharges from
power reactors in England provide information that illustrates the
variability of critical facto'rs for different environments.

     The Irish Sea coastal area adjacent to the Windscale reprocessing plant
is one of the most important areas known with respect to the degree of radio-
active contamination in the marine environment.  The critical radionuclides
released were determined to be    Cs,    Ru,   Zn,   Nb,    Ce and   Sr.
The most critical pathway is for    Ru in the seaweed, porphyra3  which is
used to make laverbread.  A critical group of heavy consumers of this
foodstuff was identified.  For three nuclear power stations sited on
England's open coastline, the exposures from   Zn,   Cs, and    Sb were
the controlling factors in limiting waste discharges.  At Hinkley,
accumulation of these radionuclides in silt and fish flesh established
the permissible discharge levels, whereas at Dungeness and Sizewell
accumulation in fish flesh alone was definitive (Straub, 1964)
     The potential damage to man and his environment is the limiting
criterion on waste releases in most Western countries, whereas Russian
Interpretation requires that releases to the environment meet drinking
water and breathing tolerances.  The doses that cause injury to plants
and animal life are, according to most Western authorities, much higher
than would be permitted for human exposure.  As an example, no effects
were noted following the irradiation of chinook salmon at dose rates of
up to 5.0 rem/day beginning immediately after fertilization of the egg.
The possibility of synergism occurring with the combination of ionizing
radiation and heated effluent temperatures also has been investigated;
while no such synergism has been demonstrated, it has been shown that
some organisms absorb radionuclides up to 50% faster due to increased
metabolic rates in warmer waters (Eisenbud, 1973).
                                  27

-------
RADIATION PATHWAY AND DOSE MODELS
     This section describes ways in which radionuclide releases to aquatic
environments can be translated into estimates of the resulting potential
radiation dose to people.  Present radiation guides for permissible radio-
nuclide concentrations in water are based upon direct consumption of
the contaminated water by people.  Although such direct intake does not
take into account potential radionuclide transfer and subsequent consump-
tion through aquatic food chains, this intake through the diet is recog-
nized, and the basic radiation standards are based on permissible radia-
tion dose rate and accumulated dose from all sources—exclusive of natural
background and medical radiation (ICRP, 1959, 1962, 1966a and b, and 1968;
USAEC, 1970; NAS/NRC, 1972; NCRP, 1971).  The bas.is for and detailed
descriptions of radiation standards are described and discussed extensively
in  the literature and are outside the scope of this report.  However,
a brief discussion of the models used in deriving air and water
standards is helpful.
     The International Commission on Radiological Protection (ICRP, 1959,
1962, 1966a and b, and 1968) has established recommended values for maximum
permissible total body burdens  (q), and for maximum permissible concen-
trations in air and water  (MPC  and MPC , respectively).  Values are
given for about 240 radionuclides.  These values are based on two
metabolic models:  (1) an exponential or compartmental model, and
(2) a power function model.  In the exponential model each body organ
is  assigned a biological half-life, uptake fraction, etc. , and the
radiation dose to different organs can be calculated following a
given radionuclide intake.  Since considerable data indicate that
for some radionuclides the fraction of the body burden excreted
daily varies inversely with time, an alternative power function model
is  used to estimate the radiation dose for certain long-lived radio-
nuclides (e.g., strontium, radium, plutonium and uranium).  The per-
missible body burdens of these bone-seeking radionuclides are based
on the comparison of the energy deposited in bone by the particular
                                               9 0£
radionuclide with that deposited by 0.1 pCi of    Ra and its daughters
The derivations of these models and a listing of model parameters  for
                                  28

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each radionuclide (with literature references) are given in  the ICRP
reports.
     The ICRP recommendations have been basically incorporated into U.S.
radiation standards.  Such regulations start with a permissible radiation
dose, from which permissible concentrations in air and water are calcu-
lated; these are based on the standard physiological  factors for man,
and would be expected to yield the permissible dose following the direct
intake of such air and water.  It must be emphasized  that the basic
criterion for the standards is radiation dose, and that the  air and water
concentration guides are derived values.  The derived guides must take
into account radionuclide exposure and intake from all sources.  One of
the important routes of radionuclide intake by people is through aquatic
foods from environments which have received discharges of radioactive
materials.  As described in previous sections, many environments have
unique characteristics, and generalizations about critical pathways for
radionuclides are tenuous.  As a result, there exists in the literature
a multitude of models for such pathways in specific cases and for
specific conditions.  The general approaches used in  pathway and dose
modeling are herein described, together with a brief  description of
those modeling efforts which appear to be comprehensive and  applicable
to initial planning for radionuclide pathways assessment.
     There are basically three methods of translating recommendations
for the maximum radiation dose into guides for acceptable discharge
rates for the various radionuclides.  The first, which was described
briefly above, involved maximum permissible concentrations in air and
water for individual radionuclides or mixtures.  If dilution, disper-
sion, and decay rates are known, then a discharge rate which meets
these standards can be calculated.  This approach, as mentioned above,
considers only direct intake of contaminated air or water and neglects
environmental pathways which may be more limiting.
     A second approach, called the critical pathway method,  is frequently
used in assessing the potential dose to segments of the population
through environmental pathways.  Through investigation of environmental
                                 29

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transfer mechanisms for radionuclides anticipated to be present, critical
pathways leading to the exposure of people to radiation are identified.
The groups of people most likely to be exposed through critical pathways
are identified; and the group most likely to receive the highest dose,
in relation to a recommended permissible dose, is identified as the
critical group.  The isotope which provides the largest dose through the
critical pathway may be called the critical radionuclide.  The permissible
environmental levels of the critical radionuclides are then calculated and
frequently called Derived Working Limits (DWL).  Although critical pathways,
radionuclides, and population groups can be identified and may be used to
calculate a DWL for each radionuclide, the basic limiting factor is total
radiation dose from all radionuclides in all pathways—including direct
intake  from air  and water.   This approach, then, is a logical extension
of the  air  and water MFC  approach  and intftgrates  exposures  from indirect
environmental pathways.
      The third approach,  based on specific activity, is  somewhat
 different.   The use of specific activity,  or radioactivity content
 per  unit mass of an element in a medium, was first  proposed by the
 NAS/NRC (1962) for establishing permissible levels  of environmental
 radioactivity in regard to radioactive  waste disposal into the
 Pacific coastal waters of the United States.  In this approach it
 is presumed that the radionuclide specific activity in any organism,
 including man, would not  exceed that in its basic environmental
 substrates.  Although a radionuclide may be concentrated many orders
 of magnitude  through physical or biological processes in the environ-
 ment, radioactive nuclides of that element are always diluted by
 stable  isotopes  in the environment and  the specific activity remains
 the  same throughout various environmental media.  Since  the elemental
 composition of man and his various tissues is well  documented in the
 literature  (e.g., as  summarized by the  ICRP, 1959), the  maximum dose
 to man  which  could result from a given  specific activity in the environ-
ment can be calculated.   For the case in which only a portion of the
 environment is contaminated, the calculated dose is modified by man's
 degree  of involvement  with that portion of the environment.
                                   30

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     These three kinds of models are interrelated and require  (NAS/NRC,
1971) a great deal of supplemental information concerning:
     1.  Kinds and quantities of radionuclides present.
     2.  Physical and chemical forms of the radionuclides.
     3.  Initial mechanism of dispersal.
     4.  Physical processes of dilution.
     5.  Availability to biota.*
     6.  Concentration factors and uptake rates.*
     7.  Consumption of marine products.
     8.  External exposure and exposure to other sources.
*Not used in specific activity approach.
      In both the critical pathway  and  specific activity approaches,
 it is  necessary to know,  or to estimate (1)  the kinds and quantities
 of radionuclides present; (2)  the  physical and chemical form of  the
 nuclides;  (3)  the method  of entry  into the environment; (4)  the  extent
 of environmental transport and deposition through physical and chemical
 processes;  and (5)  the  importance  of biological processes in transport
 and concentration phenomena (Pritchard,  1961 and Russell   1964).
 CRITICAL PATHWAY APPROACHES
     Parker (1959)  has  summarized  major and moderate  contributor path-
 ways to total  radiation dose from  radioactive  wastes  discharged  to
 surface waterways.   The major  pathways Parker  evaluates are   drinking
 water, immersion, biological chains, irrigation, waste  treatment
 plants, and external exposure  from proximity to radioisotopes.
     Varying degrees of sophistication have been used in determining
 the allowable  environmental  contamination by the critical pathways
 approach.   A simple method for seafood is described by  Pritchard (1959)
 who used the following  generalizations:
where:
                MPC   = 20 • MPC                                      (1)
                   s x            w
                MPC ,. = maximum permissible  concentration in
                        seafood
                                   31

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               MFC   = maximum permissible concentration in
                       water; as described by the ICKP (1959)
                 20  = factor derived on the basis of a diet in
                       which 50% of the protein requirement is met
                       by aquatic foods, and radionuclides in such
                       foods constitute the only source of ingestion
               MFC , = 4 • MFC                                       (2)
                  sf          w                                      v '
where:            4  = 20% of the 20, above, on the assumption
                       that 20% of the entire maximum permissible
                       radionuclide intake is assigned to seafoods
               MFC   =    sf                                         (3)
                  sw   	
 where:
                MFC   = maximum permissible concentration in
                        seawater derived from assumptions for
                        either equation (2) or (3)
                CF    = concentration factor from water to
                        organism of interest
 This approach is simple and easily understood.  However, the
 arbitrary assignment of the portion of the total radionuclide
 intake to be permitted from seafood is controversial.  In
 addition, reliable information on CF's and dietary habits for
 most areas are not generally available.
      As an example of a rather sophisticated critical pathway model,
 an outline of some general steps is given in Figure 1.  Starting
 with an allowable dose rate to man, a maximum allowable discharge
 rate for radionuclides is calculated.  The calculation may proceed
 along the following lines for the particular case of ingestion of
 a radionuclide in a contaminated seafood (NAS/NRC, 1959; Parker,
 1959).  Starting with the recommended maximum permissible concen-
 tration for water (MFC ) a derived working limit for seafood,
                       w
 (DWL)  , can be calculated (Wolfe and Rice,  1968);
      S IT
                (DHL)3f - (""^2200 F   ^
                                  32

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where:
                  I        = Rate of  ingestion for seafood, g/day/
                             person

                  2200     = Rate of  water  intake, g/day/person

                  F        = Fraction:   an  administrative number to
                             apportion to seafood  some  fraction of
                             the maximum permissible intake from
                             water.
                                                     , can  be obtained directly
A derived working level for seawater, (DWL)
                                                  sw
 from  (DWL)    by dividing  by the  ratio  of the  elemental concentration
            S JL
 in the  seafood to  that in the seawater,  i.e., by the concentration

 factor, CF  (Wolfe and Rice,  1968):

                              (DWL)
                   (DWL)
                                   'sf
                        sw
                                CF
                                                                               (5)
MAN -
Total allowable
dose rate from
all sources
    MAN - Portion of
        total allow-
        able dose allo-
        cated to aquatic
        pathways
    Routes
           Man .From
    Aquatic Environment :
    Aquatic foods, contact
    on beach sands, water
    ingestion, etc.
                                       Physical and chemical form
                                       of radionuclides and manner
                                       of discharge
                                                                Maximum Allowable
                                                                Discharge Rate of
                                                                radionuclides to an
                                                                aquatic environment
Maximum Allowable
Concentration in
Portions of Aquatic
Environment which
constitute routes to
man: water, aquatic
foods, bottom sedi-
ments, etc.



Concentration
Factors from water
to other routes to
man
                                             Maximum Allowable
                                             Concentration in
                                             water
                                                                 Initial Dilution
                                                                Dispersion and Ex-
                                                                change with other
                                                                adjacent environments
                                                                Transfer Rates for
                                                                radionuclides from
                                                                solution or suspen-
                                                                sion to bottom sedi-
                                                                ments * and back
   FIGURE 1.   General steps in  critical pathways  evaluation for aquatic
                environments — Solid  arrows  indicate direction  of radio-
                nuclides,  broken  arrows  that  of calculations
                                        33

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Application of mixing rates, dilution factors, etc., to  (DWL)   allows
an allowable rate of discharge to be calculated (Aten, 1961; Freke,
1967).
     The rate of seafood ingestion, I in equation (4), has been
estimated in various ways.  These fall into two categories of data
on food consumption patterns (Middleton, 1964).  The first is a food
balance sheet or estimate of the per capita supplies of various
human foods available in a country, and the second is a survey of
dietary habits for selected population groups.  For example, in a
typical U.S. diet it has been estimated (Harley, 1969) that marine
food products contribute 0.01% of the radioisotope intake, while
the contribution is 0.5% for a typical Japanese diet (Pritchard,
1961).
     Marey and Saurov (1964) have developed relative indices which
characterize the movement of an isotope from a water media into a
food product.  These indices, called accumulation multiples (AM), are
very similar to the CF's discussed previously.  An AM is calculated by
dividing the activity per kilogram of the food product by the activity
per liter of the water media.  These factors, along with dietary infor-
mation, can be used to establish the amount of a given isotope contri-
buted to people by individual foods in their diet.  For this purpose
contribution coefficients (CC) were expressed:
               cc =   v                                              v
where:
               AM = accumulation multiple for particular
                    food
                P = g/day intake of the food item
                V = g/day intake of water
By summing the CC values for all food products and radioisotopes, a
general CC is obtained which characterizes the ingestion by people of
radioisotopes via aquatic foods in relation to the potential direct
intake via the water media.  This approach differs from the usual,
                              34

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which utilizes CF's for edible  aquatic  organisms,  in that  radio-
nuclides in actual food products  are measured.   The  accumulation
multiple is a form of CF, but only  for  processed food items.   The
contribution coefficient is  a means to  reduce accumulation multiple
data for various foods and radionuclides  to  a form for intercomparison.
     The amount of radioactivity  in processed foods  is of  primary
importance in determining the radiation dose to  people (Harrison,
1972).  Radionuclide losses  may be  significant during processing and
marketing, e.g., from radioactive decay and  the  tissue selected  for
food.  In addition, food transportation to areas remote from  the
harvest area leads to difficulties  in accurate assessment  of  potential
problems.  World interest in the  expanded use of fish protein concen-
trate (FPC) is growing.  About  three kilograms of  whole fish  yields
about 500 grams of FPC, and  the radionuclide (as well as other pollu-
tants) content of the concentrate  may be hazardous  if it is used  as a
major dietary item.  In one  assessment  (Beasley, 1971)  based  on  a
                                              210    210
reasonable 10 gram per day intake of FPC, the    Pb-   Po  accumulation
was found to be hazardous, the  cobalt intake was increased by a  factor
of 2 to 3, and the silver intake  was increased by  about a  factor of
1.3.
     The consideration of radionuclide  ingestion alone is useful in
assessing pathways to man and relative  hazards;  however, the  dose to
man depends on many other factors such  as summarized from  ICRP reports
by Harrison (1972).  These factors  include:
     1.  Quantity of radionuclides  ingested.
     2.  Fraction of ingested quantity  which is  absorbed and
         deposited in tissues,
     3.  Energy absorbed by  tissues.
     4.  Effective half-life of the radionuclide in  tissue.
     Since aquatic environments may become contaminated from  a variety
of sources (e.g., fallout, reactors, reprocessing  plants,  and nuclear
ships), efforts have been made  by Templeton  (1964) to measure the
relative contributions of these various sources  of natural and artificial
                                 35

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radionuclides.  These data can be used for establishing allowable
discharge rates for the various sources.  However, the establish-
ment of source-oriented MFC   values from MFC  _ data would require
                           sw                sf
both estimations of the seafood ingestion rates and distribution
patterns and an arbitrary allocation of some fraction of the MFC
r                                                               sw
that could come from, for example, nuclear ships.
     The NAS/NRC (1959) recognized that the MFC for aquatic environ-
ments was generally interpreted to be the MFC  , and that this was
                                             vv
generally sufficient when food organisms in question derive their
radionuclides directly from water.  Where the  food organisms derive
radionuclides from other sources (such as bottom debris or via food
chains), then the CF's specific for biota of interest should be
used in calculations.  Usually such data are unknown.
     Eventually, it may be possible to incorporate dynamic food
chain models into the derivation of CF's.  A simple food chain
simulation model has been described by Eberhardt and Nakatani (1969) in
which a tracer substance is released at an exponentially declining rate,
and a fraction is transferred to the first compartment,  a producer.
Two hypothetical animals are included in this model, one with a
single internal compartment and the other with two compartments in
parallel.  This type of compartmentalized food-chain model could be
expanded to describe complex ecological webs.  A similar source-
pathway-receptor model is described by Reichle (1970).
     Another possible refinement of CF determinations may occur if
interspecies variability can be predicted.  The uptake and retention
of many substances is proportional to a fractional power of body
weight.  When this relation is extended to interspecies comparisons,
the resulting power coefficient is much lower  than that expected on
the basis of relationships between size and metabolic rate.  It was
proposed by Thomas and Eberhardt (1969) that interspecies comparisons
be based on "similarity ratios" that depend on the proportionality
coefficient in the equation:
                               36

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               y = a Wb                                               (7)
where:
               y = retention  time
               a = proportionality  coefficient
               W = body weight
               b - 0.75
Eberhardt  (1969) has successfully related  the long-component half-
         137
life for    Cs in humans to body weight with a power coefficient of
0.66.
     Further modifications to calculations can be made by either
broadening or narrowing the scope of dietary assumptions.  Rice
(1963) points out that the organisms which concentrate a radionuclide
to the highest degree are not necessarily  the controlling factor
in allowable radioactive waste disposal rates.  Rather, the organisms
which concentrate to the highest degree in relation to the amount
ingested by man are critical.  He has tabulated CF's for the follow-
ing major organism classifications:  algae, mollusca and fish.
Freke (1967) used a similar approach, but included Crustacea as a
major food subdivision.  In other concentration factor listings,
Aten (1958 and 1961) considered only fish  as critical, while
Polikarpov (1966) lumped together "marine  organisms" and "freshwater
organisms".
     In an International symposium report, Hiyama (1960)  adds yet
another suggestion by pointing out that since man eats numerous
kinds and quantities of marine foods a derived working level should
not be based merely on the CF for one food product.  He recommends
the use of a "seawater equivalent for daily human intake" (W,).
Alternatively, when the specific activity approach is used,  he
recommends a "seawater equivalent for the whole body" (W, ),  or for
the critical organ (W,  ).  The following formulas are derived:
               W, = M . I/S liters/day/person                         (8>
where:
               I  = average daily intake of element, g/day/person
                              37

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               M  = fraction of I that originates  from seawater
                    marine organisms
               S  = concentration of that element  in seawater,  g/1
               W, = seawater equivalent for human  intake
     The ICRP (1959) listings for maximum permissible  daily intake of
certain radionuclides (MPDI in pCi/day/person) can be  used to
derive the maximum permissible concentrations for seawater (MFC  ):
                                                               S vv
            MFC   = MPDI/W,  uCi/1                                    (9)
               sw         d
If little is known about I, but the average amount of the element in
the whole body or in the critical organ is known, then the following
seawater equivalents can be derived:
               W  = M . B/S liters                                  (10)
or
where:
              W   = M . B /S liters                                  (11)
               DC        *--
               W,  = seawater equivalent for the human body
                    (liters)
              W,   = seawater equivalent for the critical
                    organ (liters)
               B  = average amount of element in the human
                    body (grams)
               B  = average amount of element in the critical
                    organ (grams)
               S  = concentration of element in seawater
                    (gram/liter)
               M  = fraction of B or Bc that originates from
                    seawater or marine organisms
     The ICRP (1959) listings for the maximum permissible amounts of
radioisotopes in the total body (q, pCi) and in the critical organ
(q , yCi) also can be used to derive a maximum permissible concentra-
tion for seawater (MFC  ):
                      sw
            MFC   = q/W.   yCi/1                                      (12)
               S V7      D
                              38

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Where radioactive contamination extends  to  terrestial  food, any such
MFC   must be reduced proportionally.  If the isotopic dilution ratios
   S«v
are similar in both terrestrial foods and seafoods, then "M" is not
required for the above equations.
     So far, the foregoing discussion illustrates that the scope of
the terms MFC , and MFC   can  range from very generalized figures that,
at best, give order of magnitude estimates, to more specific derived
working limits for particular  areas which may be used  to guide waste
disposal practices.  An additional interpretation (Miller and Inclan-Suarez,
1970) of allowable discharge rates or MFC values has been applied at least
once by a State regulatory agency with review authority for nuclear
power plants.  This interpretation sets  MFC values as  those attained
by the lowest technologically-feasible point-source radioactive waste
discharge.
     It should be noted that MFC values  are intended for limiting human
exposure risks.  Relatively little is known about the  tolerance of
aquatic biota to chronic radioactive contamination.  There appears to
be considerable species differences and  variability, as well as signi-
ficant variability within the  same species in regard to different
developmental stages and food  intake.  Between species it has been
generally observed that for acute radiation doses the  least specialized
forms are also the most resistant.
     There appears to be no generally applicable approach to describe
the transport of radionuclides introduced into surface waters.  Each
stream, river, lake, bay, estuary, and sea has mixing  characteristics
unique in place and time.  Moreover, introduced radionuclides can remain
in solution or suspension, precipitate and settle on the bottom, or be
concentrated by plants and animals (Rice, 1965).  For  those nuclides
that remain in solution, mixing by physical processes  of diffusion,
turbulence, etc., is generally defined (Eisenbud, 1973) by a combina-
tion of theoretical calculations and measurements that are applicable
only to the specific locality.  An example of an investigation in which
many factors were incorporated is the Delaware River/Estuary Study
                               39

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(Parker et dl.3 1961).  Data on convection and diffusion were obtained
from a scale model with tracer dyes.  Calculations based on these data
were modified for radioactive decay.  Since they are somewhat concen-
tration dependent, sorption and sedimentation reactions were expressed
mathematically as exponential decay.
     The marine environment has been subdivided descriptively by
several investigators.  From the viewpoint of characteristic physical
and biological processes which may return radioactive materials to
man, there are three major divisions (Schaefer, 1961; NAS/NRC, 1959):
(1) near shore areas—harbors, estuaries, and coast out 2 miles from
shore; (2) continental shelf area—subdivided into an inner shelf 2
to 12 miles from shore and an outer shelf from 12 miles to the
200 fathoms contour; and (3) open ocean—more than 12 miles from
shore and 200 fathoms deep.  The latter two areas can be subdivided
further into commercial fishing and noncontributory areas.
     Rice (1965) compares estuarine and oceanic habitats.   He points
out that radionuclides released in the open ocean tend to be rapidly
diluted and dispersed, whereas in an estuary there is more chance of
biological and physico-chemical concentration.  Due to the shallow
depth, sediment and the benthic community involved, radioisotope
exchanges are relatively important in estuaries, but not in open
seas.  A third difference is that oceanic food chains are simple in
comparison with those of an estuary.
     Berglin (1960) has proposed a method for determining mixing in
the Woronara Estuary, Australia, which may be useful for studying other
estuarine situations.  Typically, freshwater discharged to the estuary
moves seawards by mass flow with turbulent mixing resulting from tidal
motion.  If the freshwater inflow rate is monitored, the mean dilution
which can be expected within a particular section (e.g., 1/4 mile) can
be determined by measuring the ratio of seawater to freshwater in the
section.  Then, multiplying the maximum acceptable activity levels in
a section by the mean dilution factor gives the allowable mean input
concentrations for the section.  This method would have limited usefulness
                                 40

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in situations where freshwater overrides  the saltwater  or where fresh-
water plumes extend out to sea.
     Pritchard  (1960) reviews several methods of  calculating mixing and
transport in different aquatic habitats.  Included are  formulas to esti-
mate dispersal  in a continental shelf area so that a radionuclide concen-
tration at an input area boundary can be  calculated.  In another model,
the dispersal of activity from a deep-sea bottom  is estimated using
conservative estimates of the vertical diffusion  and by neglecting the
loss to sediment.  The formulas he presents yield estimates of the
amounts of activity which, if released annually in a deep-sea segment,
would produce at the bottom of the ocean  layer harvested by man an
equilibrium concentration which would not exceed  the allowable values
for the isotopes involved.
     One of the least known components of aquatic ecosystems is the
exchange between water and bottom sediments.  The NAS/NRC (1971) has
even suggested  that it may be impossible  to generalize these sorption
and sedimentation reactions.  However, Lerman (1961) has developed a
generalized sediment transport model which defines several mechanisms
for entry of radioisotopes into the sediment.  These are:
     1.  Deposition of suspended particles of inorganic or organic
         origin;
     2.  Diffusion from the overlying water into  the sediment
         interstitial water, followed by  adsorption; and
     3.  Production from parent radionuclides in  sediments or
         release from decomposition of organic matter.
The effects of  these various factors on the concentration of a radio-
nuclide in sediment is summarized in a series of  equations which
relate these factors to the rate of change of the radionuclide concen-
tration in interstitial water.
     A paper by Reynolds  (1963) on the sorption and release of radio-
nuclides from sediments contained theoretical dispersion formulas
based on a simple compartmental stream model.  He developed an equa-
tion for a sediment distribution coefficient which was  derived from a
                              41

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mass-action equilibrium equation with the assumption that the exchanged
ions were at very low concentrations.
     A study of the Clinch River provides some surprising results in
regard to river transport characteristics.  It was found that sloughs
did not have an appreciably greater buildup of radionuclides than the
main river channel.  Parker (1967) stated that "possibly the most
important outcome of the Clinch River Study is the successful applica-
tion of mass-balance techniques to entire river complexes".  This
study showed that the water-borne load of radionuclides was almost the
entire amount discharged to the river.  The sediment load was small
(2 to 5% maximum); the maximum inventory possible in the biomass was
exceedingly small and could be neglected.  These results support earlier
work reported by Polikarpov et al. (.1966) in which it is postulated that
the biomass may be neglected as a significant depot of activity in a
reservoir or lake system.  This is true, they concluded, even though
the average CF's in the biomass and sediments may be 1,000 and 100,
respectively, because the relative biomass is small as compared to
other system components.
     Armstrong and Gloyna (1967) developed a general equation to
describe radionuclide transport in terms of hydraulic dispersion and
convection in detention systems (compartments) which sorb and release.
For non-conservative substances, such as radionuclides, a sink must
be included to account for the uptake of material from solution.  A
generalized form of the equation for a radionuclide is:
               AC = D - V - U                                         (14)
where:
               AC = change in water concentration
                D = dispersion term
                V = convection term
                U = uptake term
They point out that the uptake term is very poorly defined.  It includes such
variables as sorption of radionuclides by suspended solids, sediment and
plants.  They also proposed a general equation for uptake reactions in which
the uptake is a summation of sorption on various substrates.  The rates of
                                42

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sorption and desorption are dependent  on  the  concentration  gradient
between a transfer substrate and  the sorbent.  A linear  transfer
function is used to correlate sediment specific  activity to that  of
water, although they point out  the possibility of  using  an  alternative
nonlinear function.  The study  showed  that suspended solids, sediment,
and plants (ya££isneria/l sorb according to a  nonlinear (Freundlich
isotherm) function.  However, attempts to use this equation in the
reaction term of the one-dimensional (e.g., a river)dispersion equation
forces it into a nonlinear form and makes analytical solution impossi-
ble.  A by-product of the transport equation  (using a linear transfer
function) is the specific activity of  radionuclides in the  biological
system.  It is feasible to use  these results  to  determine the passage
(transfer coefficients) through aquatic food  chains by using the
general equation for uptake reactions.
     Kaye and Ball (1967) proposed the application of systems analysis
techniques to ecosystem models  describing radionuclide transport.  Their
approach uses input and loss relationships which allow calculation of
the radionuclide concentration  in any  environmental compartment.  Two
important kinds of required information are (1)  an accurate compart-
mentalized representation of the  environment  under review;  and (2) the
rate constants which quantify the intercompartmental transfer of nuclides.
This technique was developed into a comprehensive  model  for predicting
transport of radionuclides from an underground nuclear explosion  through
the seawater—fish—man pathway by Bloom  (1971).   It is  apparent  that
further modifications of this technique may allow  the development of
models to deal with chronic releases of radionuclides from  various
sources.
SPECIFIC ACTIVITY APPROACHES
     The specific activity approach is attractively simple  in concept
and is very useful in assessing long-term problems concerning the radio-
isotopes of elements which (1)  are relatively abundant in nature,  (2)
are rapidly dispersed throughout  the environment,  and  (3) are normal
constituents of organisms  (e.g.,  3H, l C, 2P).   The NAS/NRC (1962)
                                43

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in developing recommendations for ocean disposal of radioactive wastes
stated the principle:  ". . .if the specific activities  (that is, the
radioactive proportions of the elements) of the chemical  elements in
the sea in the environment of human food organisms are maintained below
the allowable specific activities for those elements in the human body
or human food, no person can obtain more than an allowable amount of
radioactivity from the sea, regardless of his habits."  For trace
elements and those radioisotopes which are close chemical congeners
of another element, the specific activity approach lacks  consistency.
A method recently developed at LLL (Pratt, 1970; Tamplin et al.t  1968
and 1969; and Thompson et at* , 1972) is baaed on specific activity and
is similar to the NAS/NRC approach except that it relates to tissue dose
rather than to critical organ dose.
     The specific activity approach, as developed by the NAS/NRC
(1962), was for calculation of derived working limits for radioactive
waste disposal into Pacific coastal waters.  The approach is based on
two major assumptions:
     1.  that a radioisotope introduced into the environment readily
         equilibrates with the stable isotope(s) of the same element,
         and
     2.  that the quantity of each stable element in each body organ
         is fixed and does not fluctuate with the intake  of that
         element.
It is known that the conditions of the first assumption are not always
met.  Known exceptions have been tritium, carbon, sulfur, vanadium,
iron, cobalt, copper, and zinc.  These elements may be introduced as
stable organic complexes and, hence, are not diluted by the common
abundant chemical form of the stable elements.  The NAS/NRC (1962)
recommends that for these elements the safety factor for modifying
figures from occupational worker dose to general public dose be
increased from a factor of 10 to 100.
     The maximum permissible specific activity  (MPSA) for any radio-
isotope with a critical organ other than the GI tract is  readily avail-
able from data on standard man (ICRP, 1959).
                             44

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               MPSA = q/mC   jaCi/g                                    (15)
where:
               MPSA - maximum permissible  specific  activity
                      (pCi/g)
                  q = maximum permissible  burden of radio-
                      isotope in critical  organ (pCi)
                  m = mass of the critical organ (g)
                  C = concentration  of stable element in
                      critical organ (g/g)
The MPSA can then be converted to derived working limits for a media.
For example, the values for
calculated  (NAS/NRS, 1962):
For example, the values for seawater (DWL  ) or seafood (DWL  ) are
                                         sw                 sf
              DWL   = K   (MPSA)  yCi/cm  seawater                   (16)
                 C> W    W
              DWLgf = K   (MPSA)  yCi/g seafood                      (17)
where:
                                                2
                 K  = grams of stable element/cm  seawater
                  w
                 K,. = grams of stable element/g seafood
A DWL derived in this fashion is independent of CF's and the consumption
rates for seafoods.
     For those isotopes that are only slightly absorbed by the body
and mainly affect the gastrointestinal tract, the MFC in water is
converted to a MPSA of the stable species in seafood by utilizing the
abundance of that element in seafood organisms which results in the
most restrictive requirement.  Although developed specifically for
pathways from the sea, this approach can be extended to freshwater
and terrestrial environmental pathways (NAS/NRG, 1962, and Bryant, 1970).
     An alternate method has been proposed by the NAS/NRC (1959) for
computing allowable environmental levels of certain radionuclides for
which a known human discrimation factor exists.  For example, the ratio
   90
of   Sr to calcium in the total body should not exceed 0.1 pCi/kg.
Man physiologically discriminates against strontium in a strontium-
calcium mixture by a ratio of 8:1.  If man receives his total protein
                                  90
allowance from fish which contain   Sr, then the MFC for fish is
                              45

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                      90
defined as 0.8 yCi of   Sr/kg calcium.  Further, since the  calcium
concentration of seawater is about 0.4 g/kg seawater, the seawater
MFC is about 0.8 yCi/2,500 kg or about 3 X 10~  pCi/ml of seawater.
The occupational MFC for continuous exposure in drinking water is
10~10 nCi/ml (ICRP, 1959).
     Odum (1963) has extended this idea of using the known  ratio of
a radionuclide to a stable physiological element in a theoretical
"element ratio method".  Basically, he proposes that if the ratios
of the minor elements to carbon are known, then the measurement of
carbon metabolism can be used to predict cycling of the minor elements.
     Bloom (1971) suggests that two screening operations be performed
before detailed calculations are made.  The first uses a simple two-
compartment specific-activity model in which the specific activity of
each radionuclide in man is assumed to be the same as in the environ-
mental sink before dilution.  Then, using ICRP data on radionuclides,
standard man, etc., the infinite-time internal dose is calculated for
(1) the gastrointestinal tract  and (2) all other organs.   For radio-
isotopes found potentially important in this initial screening, he
recommends an eight-compartment transport model which requires source
term data and transfer coefficients for the radionuclides identified
in screening.  Solution of a complex set of equations provides esti-
mates of the radionuclide concentration in each of the eight compart-
ments as well as of the internal radiation dose to man as a function
of time.
     A modified specific activity method for determining safe discharge
rates for radionuclides into aquatic systems is being developed at the
Lawrence Livermore Laboratory (Chapman et at. 3  1968; Harrison, 1972;
Tamplin, 1967,  1968, 1969; Burton, 1968; Ng et al.f 1966, 1968; Thompson
et al*,  1972).   The approach is similar to that of the NAS/NRC (1962),
except it uses  a tissue dose concept rather than a critical organ dose con-
cept.   The method approaches environmental contamination by radionuclides and
the resultant radiation dose to man from the standpoint of  the specific
activities of ingested elements; this is also known as the  biological
                                46

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exchangeable pool of elements concept  (Ng  and Thompson, 1966).  The
passage of a radionuclide through the biosphere is presumed to be governed
by the same factors that govern the distribution of the related stable
element isotopes within the biological exchangeable pool.   It is also
presumed that the radionuclide is biologically no more (or less) avail-
able than the related stable isotopes within the environment.
     The basic product of this effort is a value for each isotope called
                                                 3
the unit-rad contamination in water  (F ) in yCi/m /rad.  Values have
                                      A.
been derived for freshwater and seawater.  This factor is defined as
the initial concentration of a radioisotope in water which would yield
a 30-year  integrated dose of 1 rad to a specific designated tissue
of standard man.  In most cases F  values for infants are also esti-
                                 A
mated, since values for adults are usually less restrictive than for
infants.   The values for F  are derived with several simplifying
                          £1
assumptions, almost the same as those used by the NAS/NRC (1962),
which must be clearly understood in applying the F  factors to environ-
                                                  £\
mental data.  These assumptions yield very conservative values for
F , for the worst situation that could develop, and are designed in
 A.
this manner so that basic information on the environment and popula-
tion at risk can be used to develop modifying factors.  The simplify-
ing assumptions include:
     1.  Man exists on a diet of totally aquatic origin, and
     2.  Initial water concentrations decrease only through radio-
         active decay.  (Dilution of the system by uncontaminated
         water and dilution beyond the area of initial rapid mixing
         are not accounted
     The basic calculation process is, briefly, to start with the ppm
values for stable elements in seawater and freshwater and to calculate
an uptake by man from various routes.  CF's derived from the literature
for items in man's food chain are used to obtain stable isotope intake.
Various data, e.g., terrestrial and aquatic, are evaluated to obtain
the most critical pathways for calculating FA>  The introduction of
radioisotopes into aquatic environments and the subsequent intake by
man are evaluated on the basis of stable element pathways.  The
                               47

-------
radiation dose to man from radioisotopes is calculated using GI uptake
fractions, daily ingestion amounts, energy absorbed in tissue per disin-
tegration, effective half-lives in the environmental media and man's
tissue, distribution in man's tissues, etc.  In a LLL report (Ng ei^ at* t
1968),  all of these input parameters for calculations are listed for
radionuclides with half-lives greater than 12 hours.  The derived values
for F  are also listed, and some methods are given to modify these
     A.
basic values to those more representative of a given situation.  For
example, the calculations are described for obtaining modified F
                                                                A.
values for a population on a mixed aquatic and terrestrial diet.  The
modified values obtained include corrections for both the dietary mix
and the ratio of isotope concentrations in aquatic and terrestrial
foods.
     The estimated maximum radiation dose to a tissue (EDA) from a
particular isotope is obtained by dividing the aquatic environment
concentration by F  as follows:
                  A.
where:
               EDA = ECA/FA rad
                          A

               EDA = 30-year integrated dose to a specific  tissue
                     of standard man  (or infant when designated
                     value of FA is used) from an aquatic diet
                     and for a specific isotope
               EGA = contamination level of the aquatic environ-
                     ment in nCi/m3
                                                            3
                F. = unit-rad contamination factor in uCi/m /rad
The total dose to a specific tissue is the sum of the doses from
individual radionuclides.
     Pratt (1970) has used much of the above information in deriving unit-
dose-rate water concentration values.  These are water concentration values
for isotopes  which could yield an equilibrium dose rate of  1 rad per year
to an adult  through aquatic foods.  Values are also derived for infants.
Since these  concentrations can be scaled to appropriate maximum allowable
dose rates,  the maximum allowable concentrations in an aquatic environ-
ment can be  calculated.  The maximum  allowable rates of release can
                               48

-------
then be calculated using appropriate dilution  and  dispersion  factors.
The maximum allowable dose to people through aquatic  foods still must
be designated in this approach if firm regulatory  guides are  to be
promulgated.  In general, regulatory bodies have avoided fragmenting
the total allowable dose into portions related to  specific exposure
routes.  The basic criteria is dose from all sources, and the fractional
contribution from a specific route varies with each particular situation.
     In general, the specific activity approach gives less stringent
standards for radioactive waste disposal in seawater  than are derived
through critical pathways models.  The latter  tend to be more restric-
tive, apparently because conservative values are generally used for
unknown concentration factors.  The specific activity approach has the
following limitations (Wolfe and Rice,  1968):
     1.  It is not valid when considering radiation dose to the
         gastrointestinal (GI) tract.
     2.  As the maximum permissible body burden for radioactivity is
         approached in humans, the total activity in the GI tract
         becomes significant, regardless of what the specific
         activity may be.
     3.  Radionuclides introduced into the environment may be more
         (or less) readily available for bioaccumulators than the
         corresponding stable elements.
     In the final transition of adapting allowable dose rates into
maximum permissible concentrations for radionuclides in air, food,
and water, and subsequently into directives for operating practice,
there is practical value in an easily understood index of hazard.
Such an index has been proposed by Rohwer and  Struxness (1972) and is
termed a "cumulative exposure index".  This is a numerical guide
indicating relative significance (dose estimate/dose  limit) of measured
environmental radioactivity on the basis of the total dose to man from
all radionuclides and exposure modes of importance.
                                 49

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71.  "Standards for Protection Against Radiation," USAEC, Title 10-
     Atomic Energy, Part 20, September, 1970.

72.  Wolfe, D. A. and Rice, T. R., "Safe Levels of Radioactivity in
     Aquatic Environments," Scientia. 103 (9-10):469-487, 1968.
                               56

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                                   TECHNICAL REPORT DATA
                            (flease read Instructions on the reverse before completing)
  REPORT NO.
   EPA-600/3-76-054
2.
                              3. RECIPIENT'S ACCESSION-NO.
4. TITLE AND SUBTITLE
  CONCENTRATION FACTORS AND TRANSPORT MODELS FOR
  RADIONUCLIDES IN AQUATIC  ENVIRONMENTS   A
  Literature Report	
                              5. REPORT DATE
                               May  1976
                              6. PERFORMING ORGANIZATION CODE
 '. AUTHOR(S)
  R.  G.  Patzer
                             8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
   Environmental Monitoring  and Support Laboratory
   Office of Research and  Development
   P.  0.  Box 15027
   Las Vegas, NV  89114
                              10. PROGRAM ELEMENT NO.

                                1FA083	.
                              11. CONTRACT/GRANT NO.
                                n/a
12. SPONSORING AGENCY NAME AND ADDRESS

   Same as above
                              13. TYPE OF REPORT AND PERIOD COVERED
                              Final - FY75
                                                           14. SPONSORING AGENCY CODE
                                                           EPA-ORD,  Office of Health  and'
                                                           Ecological Effects
15. SUPPLEMENTARY NOTES
 16. ABSTRACT
   The relative risks to man from radionuclides released  to the environment depend
   heavily on their accumulation or concentration by aquatic organisms.  The
   organisms which accumulate those radionuclides present in the environment may
   be useful as indicators  for environmental monitoring purposes.   In addition,
   these organisms may be directly in food chain pathways to humans.

   Literature is reviewed and summarized in regard to biological concentration of
   radionuclides in freshwater and marine environments.   Concentration factors for
   elements found in organisms are tabulated for plants,  invertebrates, and fish
   in marine and freshwater environs.  Literature is also reveiwed on models
   developed to calculate the possible radiation dose delivered to humans from
   radionuclides released into aquatic environments.  The model approaches
   summarized range from simple generalized forms which,  at best,  give order
   of magnitude estimates to detailed models for a specific area which may be
   used to guide waste discharge practices.
17.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
                                              b.lDENTIFIERS/OPEN ENDED TERMS
                                              COS AT I Field/Gioup
   Concentration
   Isotopes*
   Mathematical Models*
   Radiation Monitors
   Radiation Protection
                  Biological concentration
                  Concentration  factors*
                  Transport models*
  06R
  07E
  08H
  18H
18. DISTRIBUTION STATEMENT
  RELEASE TO PUBLIC
                 19. SECURITY CLASS (ThisReport)
                  UNCLASSIFIED
21. NO. OF PAGES

   64
                                              20. SECURITY CLASS (Thispage)
                                               UNCLASSIFIED
                                                                         22. PRICE
EPA Form 2220-1 (9-73)
                                                                      &GPO 691-217-1 976

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