United States Office of EPA 520/1 -8W)15
Environmental Protection Radiation Programs August 1986
Agency Washington, D.C. 20460
Radiation
<&EPA Laboratory - Determined
Concentration Factors And
Elimination Rates Of Some
Anthropogenic Radionuclides
In Marine Vertebrates And
Invertebrates
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EPA 520/1-85-015
Laboratory-Determined Concentration Factors
and Elimination Rates of
Some Anthropogenic Radionuclides in
Marine Vertebrates and Invertebrates
August 1986
Office of Radiation Programs
U.S. Environmental Protection Agency
Washington, DC 20460
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FOREWORD
In response to the mandate of Public Law 92-532, the
Marine Protection, Research and Sanctuaries Act, as amended, the
Environmental Protection Agency (EPA) has developed a program to
promulgate regulations and criteria to control the ocean disposal
of radioactive wastes. An important technical consideration in
an/ environmental assessment of this option is the potential for
biological uptake of radioactivity as it moves through marine
food chains which could lead to man. An understanding of the
range of concentrations and biological elimination rates of key
radionuc1 ides found in marine organisms is fundamental.
This report reviews and summarizes the experimental
literature on radionuc 1. ide concentration factors and biological
turnover rates of selected radionuclides. It also provides a
comparison of laboratory-determined concentration factors with
field-derived values. The isotopes of low-level waste selected
lor inclusion are plutonium, americium, cesium, strontium, and
cobalt. The data are presented by isotope and according to
the various groups of marine organisms for which data are
available. The concentration factor data are summarized in
tables that include comments concerning conditions of the
experiment. Figures are included that compare laboratory and
fie Id-derived concentration factor values for each isotope.
These data are useful for predictive modelling both to
estimate concentrations of specific nuclides which may occur
in fish or invertebrates from any past or future ocean disposal
activities and to predict the resultant dose to man from
ingestion of these seafoods.
The Agency invites all readers of this report to send any
comments or suggestions to Mr. David E. Janes, Director, Analysis
and Support Division, Office of Radiation Programs (ANR-461),
Environmental Protection A.gency, Washington, D.C. 20460.
Sheldon Meyers,Acting Director
Office of Radiation Programs (ANR-458)
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CONTENTS
Abstract xii
Introduction 1
Objective 1
Concentration Factors 1
Measurement of Concentration Factors 2
Application of Concentration Factors .... 4
Patterns of Concentration Factors 5
Elimination Rates 8
Derivation of Elimination Rates 9
Determination of Elimination Rate Constants 11
Plutonium 12
Physicochemical Form 12
Primary Producers 13
Concentration Factors 13
Microalgae 13
Macroalgae 16
Elimination Rates 16
Microalgae 16
Macroalgae 17
Annelida - Polychaeta 17
Concentration Factors 17
Elimination Rates 19
Mollusca 20
Concentration Factors 20
Pelecypoda 20
Gastropoda 20
Cephalopoda 24
Elimination Rates 24
Pelecypoda 24
Gastropoda 26
Cephalopoda 26
Arthropoda - Crustacea 26
Concentration Factors . 26
Elimination Rates 28
m
-------
Chordata - Pisces 28
Concentration Factors 28
Elimination Rates 29
Americium ........ 30
Physicochemical Form 3°
Primary Producers 30
Concentration Factors . 30
Microalgae 30
Macroalgae ^3
Elimination Rates 33
Microalgae 33
Macroalgae 33
Annelida - Polychaeta 34
Concentration Factors 34
Elimination Rates 34
Mollusca 36
Concentration Factors 36
Pelecypoda ....... 36
Gastropoda 36
Cephalopoda 36
Elimination Rates 39
Pelecypoda 39
Gastropoda 39
Cephalopoda 41
Arthropoda - Crustacea 41
Concentration Factors 41
Elimination Rates 43
Chordata - Pisces 43
Concentration Factors 43
Elimination Rates 43
Cesium 43
Physicochemical Form 43
Primary Producers 45
IV
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Concentration Factors 45
Elimination Rates . 50
Annelida - Polychaeta • • 50
Concentration Factors 50
Elimination Rates .... 50
Mollusca 50
Concentration Factors .... 50
Elimination Rates .... 57
Arthropoda - Crustacea 57
Concentration Factors ... 57
Elimination Rates 57
Chordata - Pisces 61
Concentration Factors 61
Elimination Rates 61
Strontium 64
Physicochemical Form 64
Primary Producers 64
Concentration Factors 64
Elimination Rates 64
Annelida 68
Mollusca 68
Concentration Factors 68
Elimination Rates 68
Arthropoda - Crustacea 68
Concentration Factors 68
Elimination Rates 68
Chordata - Pisces 72
Concentration Factors 72
Elimination Rates 72
Cobalt 72
Physicochemical Form . . . < 72
Primary Producers . 74
Concentration Factors 74
Elimination Rates 74
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Annelida - Polychaeta 77
Concentration Factors . 77
Elimination Rates 77
Mollusca ..... ... 77
Concentration Factors ....••• ^7
Elimination Rates 81
Arthropoda - Crustacea 81
Concentration Factors ..... ....••• 81
Elimination Rates ...... 84
Chordata - Pisces 84
Concentration Factors 84
Elimination Rates 84
Application of Concentration Factor and Elimination Rate Data 87
Concentration Factors 87
Elimination Rates 92
Acknowledgments 92
References . 94
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LIST OF TABLES
1. Laboratory-derived concentration factors (CFs) for
plutonium in primary producers 14
2. Laboratory-derived concentration factors (CFs) for
plutonium in Annelida - Polychaeta ... 18
3. Laboratory-derived concentration factors for plutonium
in Mollusca 21
4. Biological half-life (days) of plutonium in Mollusca 25
5. Laboratory-derived concentration factors (CFs) for
plutonium in Arthropoda - Crustacea 27
6. Laboratory-derived concentration factors (CFs) for
americium in primary producers (microalgae) 31
7. Laboratory-derived concentration factors (CFs) for
americium in Annelida Polychaeta 35
8. Laboratory-derived concentration factors (CFs) for
americium in Mollusca 37
9. Biological half-life (days) of americium in Mollusca 40
10. Laboratory-derived concentration factors (CFs) for
americium in Arthropoda - Crustacea 42
11. Biological half-life (days) of americium in whole
Arthropoda - Crustacea 44
12. Laboratory-derived concentration factors (CFs) for
cesium in primary producers 46
VI 1
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13. Biological half-life (days) of cesium in primary
producers (macroalgae) ....
14. Laboratory-derived concentration factors (CFs) for
cesium in Annelida - Polychaeta ......... . ........
15. Laboratory-derived concentration factors for cesium in
Mollusca. ...... ...... . ................ 53
16. Biological half-life (days) of cesium in Mollusca.
58
17. Laboratory-derived concentration factors (CFs) for
cesium in Arthropoda - Crustacea 59
18. Laboratory-derived concentration factors for cesium in
Chordata - Pisces 62
19. Biological half-life (days) of cesium in Chordata -
Pisces 63
20. Laboratory-derived concentration factors (CFs) for
strontium in primary producers 65
21. Laboratory-derived concentration factors (CFs) for
strontium in Mollusca - Pelecypoda 69
22. Laboratory-derived concentration factors (CFs) for
strontium in Arthropoda - Crustacea 71
23. Laboratory-derived concentration factors (CFs) for
strontium in Chordata - Pisces 73
24. Laboratory-derived concentration factors (CFs) for
cobalt in primary producers 75
25. Laboratory-derived concentration factors (CFs) for
cobalt in Mollusca ..... 78
vm
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26. Biological half-life (days) of cobalt in Mollusca -
Pelecypoda 82
27. Laboratory-derived concentration factors (CFs) for
cobalt in Arthropoda - Crustacea 83
28. Laboratory-derived concentration factors (CFs) for
cobalt in Chordata - Pisces 85
29. Biological half-life (days) of cobalt in Chordata -
Pisces 86
30. Values obtained from statistical analyses of CFs, assuming
a normal distribution and a lognormal distribution 91
31. CF values selected for use in models to predict the dose to
man or aquatic organisms from the release of radionuclides
into marine environments 93
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LIST OF FIGURES
1. Hypothetical model of the partitioning of a
radionuclide among compartments in aquatic ecosystems
Processes in uptake, incorporation, and loss of stable
and radioactive nuclides of metals (modified from George
and Viarengo, 1985). Nuclide (N) in seawater and/or in
the cytosol may be associated with ligands (L) of
different molecular size and affinity for the metal.
Within the cytosol, nuclides bound to ligands may be
associated with metallothioneins and lysosomes
3. Concentration factors (CFs) for plutonium in marine biota:
laboratory-derived CFs from this report (•); field-derived CFs
from Noshkin (1985) (•) or Jackson _et _al_. (1983) (o) 15
4. Concentration factors (CFs) for plutonium in muscle
tissue of marine biota: laboratory-derived CFs from this
report (o); field-derived CFs from Noshkin (1985) (•) 23
5. Concentration factors (CFs) for americium in marine
biota: laboratory-derived CFs from this report (•);
field-derived CFs from Noshkin (1985) (•) 32
6. Concentration factors (CFs) for americium in muscle
tissue of marine biota: laboratory-derived CFs from this
report (•); field-derived CFs from Noshkin (1985) (•) 38
7. Concentration factors (CFs) for cesium in marine
biota: laboratory-derived CFs from this report (•);
field-derived CFs from Noshkin (1985) (•);
field-derived data from Jackson e_t^ a_l_. (1983) (o);
stable-element-derived CFs from Polikarpov (1966) (o). . 49
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8. Concentration factors for cesium in muscle tissue of
marine biota: laboratory-derived CFs from this
report (o); field-derived CFs from Jackson et al.
(1983) (o) or Noshkin (1985) (•); stable-element-
derived CFs from Polikarpov (1966) (o) or Pentreath (1977) (A). . . 56
9. Concentration factors (CFs) for strontium in marine
biota: laboratory-derived CFs from this report (•);
field-derived CFs from Jackson _et _aj_. (1983) (o) or
Noshkin (1985) (t); stable-element-derived CFs from
Polikarpov (1966) (o) or Pentreath (1977) (A) 67
10. Whole-body concentration factors (CFs) for strontium in
muscle tissue of marine biota: laboratory-derived CFs
from this report (•); field-derived CFs from Noshkin
(1985) (•); stable-element-derived CFs from Polikarpov
(1966) (o) or Pentreath (1977) (A) 70
11. Concentration factors (CFs) for cobalt in marine
biota: laboratory-derived CFs from this report (•);
field-derived CFs from Jackson _et _a_L (1983) (o) or
Noshkin (1985) (•); stable-element-derived CFs from
Polikarpov (1966) (o), or Shimizu _et _a_L (1970) (A) 76
12. Concentration factors for cobalt in muscle tissue of
marine biota: laboratory-derived CFs from this report
(•); field-derived CFs from Jackson _e_t _al_. (1983) (o);
stable-element-derived CFs from Polikarpov (1966) (o)
or Pentreath (1977) (A) 80
13. Concentration factors for plutonium in muscles of
fish. The arithmetic mean is 77 (sigma = 220), and
the geometric mean is 8.9 (sigma = 8.7) 90
XI
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LABORATORY-DETERMINED CONCENTRATION
FACTORS AND ELIMINATION RATES OF SOME
ANTHROPOGENIC RADIONUCLIDES IN MARINE
VERTEBRATES AND INVERTEBRATES
ABSTRACT
The literature on radionuclide concentration factors and elimination
rates acquired in laboratory experiments is reviewed and discussed, and then
the laboratory-derived concentration factors are compared to those
concentration factors measured directly in organisms collected from marine
environments. The radionuclides considered in this review are those of
Plutonium, americium, cesium, strontium, and cobalt. The groups of organisms
for which data have been acquired are primary producers, annelids, molluscs,
arthropods, and fishes.
I discuss the measurement, application, and patterns of concentration
factors, as well as the derivation and determination of elimination-rate
constants. In addition, I have compiled tables of concentration factors and
elimination rates for those radionuclides and groups of organisms for which
sufficient data are available.
XI 1
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INTRODUCTION
OBJECTIVE
The objective of this study is to provide data that can be used to assess
the potential for bioconcentration of radioactivity in marine food chains that
could lead to man. Specifically, the literature on radionuclide concentration
factors and elimination rates acquired in laboratory experiments is reviewed
and discussed, and then the laboratory-derived concentration factors are
compared to those concentration factors measured directly in organisms
collected from marine environments. Radionuclides designated by the U.S. EPA
Office of Radiation Programs for inclusion in this review are those of
Plutonium, americium, cesium, strontium, and cobalt. Tables of concentration
factors and elimination rates for major groups of organisms were compiled for
those radionuclides for which sufficient data were available.
CONCENTRATION FACTORS
Concentration factors have been used in models to predict the
concentration of radionuclides when releases from ocean waste disposal or
ocean discharges are continuous and steady-state conditions are present. The
concentration factor (CF) is usually defined as the ratio of the concentration
of the radionuclide (R) in the organism or tissue i, (R-), to that in the
water, (Ru). Thus, if the concentration of a radionuclide in the water in
an ecosystem is known, the concentrations in aquatic organisms can be
calculated from their CFs. Some authors have calculated CFs from the
concentration of the radionuclide in the soluble fraction of the water; others
have used total water concentrations. Furthermore, some CFs have been
calculated from radionuclide concentrations in food-chain organisms and in
sediments. The use of CFs based on specific biotic and abiotic components is
appropriate when sufficient data are available that indicate that the component
(or components) is the actual source of the radionuclide to the organism of
concern.
CFs are affected both by the physical and chemical form of the element in
the environment and by the route of entry of the element into the organism.
Many physicochemical forms of radionuclides may exist, and the distribution
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among forms differs with the radionuclide and the characteristics of the
ecosystem (Fig. 1). The routes of entry of radionuclides into an organism are
dependent in part on the organism's feeding behavior and its habitat. Major
routes of entry are from radionuclides in solution or suspension in water and
in food-chain organisms. However, many organisms live in sediments and may
absorb radionuclides from interstitial waters, from the sediment directly, and
from ingestion of sediments. Unfortunately, for many radionuclides we do not
know the relative bioavailability of the different physicochemical forms or
the relative importance of the food, water, and sediment pathways for transfer
of the radionuclides to the organisms.
Measurement of Concentration Factors
Let us consider some of the parameters affecting the measurement of
concentration factors. Variations in concentration of stable and radioactive
nuclides in organisms can be expected because of differences in their sizes,
ages, and reproductive states and because of fluctuations in temperature and
the concentration of constituents in the environment. If, as has been
frequently done, field measurements of stable or radioactive nuclide
concentrations of organisms are made at only one point in time and on only
limited numbers of the population, the CFs obtained may be erroneous. Thus,
to obtain a meaningful measurement of CF, we may need a knowledge of the
environmental history of the organism and the composition (size, age, and sex)
of the population sampled.
In addition to variations in concentration in the organisms, changes in
concentration in the water occur because of seasonal fluctuations both in the
run-off from the land and in the hydrodynamic and meteorologic conditions.
Furthermore, more than values for just the total concentration of the nuclide
in the water may be required. It may be necessary also to have the values for
the concentrations of prominent chemical and physical species because an
organism may possibly accumulate only one specific form. Consequently, for a
CF to be valid, it should be established both that the concentration measured
in the water is that with which the organism has equilibrated and that it is
for the physicochemical form that existed during the period of equilibration.
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Insoluble
orecipitate
Sorption by
particles
Figure 1. Hypothetical model of the partitioning of a radionuclide among
compartments in aquatic ecosystems.
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Application of Concentration Factors
Wide ranges in CF have been determined for some organisms (Jackson et
al., 1983; Noshkin, 1985). Consequently, before these are used in models, the
method of obtaining the values should be examined to determine if they should
be applied to the situation under consideration.
To select the best CF to apply, one must understand something of the
nature of the physiological processes that have resulted in the concentration
difference between the organism and its environment.
The uptake and loss of a radionuclide may follow the uptake and loss of
its stable nuclide or of related stable or radioactive nuclides that have
similar physicochemical properties. Therefore, to be able to predict the
behavior of some radionuclides, it may be necessary to understand the
metabolism of stable and radioactive nuclides of other elements.
The uptake and loss of elements continues throughout the life of the
organism and may vary considerably with fluctuations in metabolic demands.
When the rate of uptake exceeds the rate of loss, a concentration buildup
between the organism and its environment will ensue. This concentration
buildup may be maintained by a process such as binding to subcellular
constituents and cellular metabolites or by processes that require the
expenditure of metabolic energy. Thus, CFs may be altered by factors that
affect metabolic activity.
The accumulation of a specific element may occur because of needs of
growth, reproduction, and skeleton formation, or because the mechanism for
loss is less effective than that for uptake. The material accumulated may be
in distinct chemical, organ, or tissue pools. Thus, its distribution in the
organism may be distinctly heterogeneous, and a large fraction of the material
may be localized in a small mass.
Mechanisms have frequently evolved in organisms for increasing the rate
of uptake of an element when the environmental concentrations are low and
decreasing it when metabolic demands have been met. When an excess of an
element is accumulated, there is a need for its removal. Excesses can be lost
by elimination of the element back across the body surface or gills and
excreting it into the gut or the urine, or can be metabolically inactivated by
temporarily or permanently storing it in a different form in a particular
tissue. Tissues known to be important storage sites for many elements are the
liver (or hepatopancreas) and the kidney. Some aquatic organisms appear to be
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able to regulate the concentration of elements by combining the processes of
absorption, excretion, and storage. The ability of organisms to regulate
element concentrations has been assessed by analyzing tissues from organisms
exposed to different concentrations of the element of interest. Homeostatic
control of element concentrations has been demonstrated for a number of
elements in fishes, but for only a few elements in invertebrates.
Accumulation can be affected also by the modifications that may occur at
the place of uptake because of the specificity of the binding sites.
Furthermore, because these sites may not discriminate between elements that
are chemically and physically similar, inhibition of uptake may occur as a
consequence of competition for binding sites. Absorption of elements from
seawater may occur across the general body surface or through a special area
such as gills or walls of the gut (Fig. 2). Once in the body fluid, they may
remain free or bind to proteins, or they may be accumulated by individual
tissues. This appears to involve sorption at sites on or within the cells.
Absorption may be an active or passive process, and accumulation may be
related to the stabilities of complexes formed between elements and organic
1igands.
Patterns of Concentration Factors
Three idealized CF patterns have been described by Vanderploeg et a_j_.
(1975). The first pattern is that the CF for a radionuclide (R) in organism
or tissue i, CF(R)., is constant, i.e., is unaffected by the concentration
of elements:
CF(R). = constant. (1
This pattern is shown by radionuclides that are not under homeostatic control
and is exemplified by the behavior of plutonium in marine invertebrates and
fishes.
The second pattern is seen in organisms in which the concentration of an
element in an organism or tissue is under homeostatic control or regulated at
a constant concentration despite different concentrations of the element in
water. In this case, the CF of the element (E) is inversely proportional to
its concentration in the water:
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Environment
Membrane
Cytosol
ML,
N
N
+
U
ML,
* „ ,
» »
•
s 9
* . •
.;•.
• . .
« *
« •
* «
' Metallothion
N
+ Aulusui
L _.._.. . Synthesis
, Secon
L3 lysos
($ §
• ... •••.•.•.-.;... ^ ••...•.;•:•. 11
:•••••••/. •••:•• • •: ••/• L3.'.-.-. /.• .-.:- T
N f
Primary
lysosome
NL
Endocytosis
Residual
body
Exocytosis
Figure 2. Processes in uptake, incorporation, and loss of stable and
radioactive nuclides of metals (modified from George and Viarengo, 1985).
Nuclide (N) in seawater and/or in the cytosol may be associated with ligands
(L) of different molecular size and affinity for the metal. Within the
cytosol, nuclides bound to ligands may be associated with metallothioneins and
lysosomes.
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CF(E). = E./E , (2)
i v w ' v
where E^ = concentration of stable element in organism or tissue i, a
constant (ug/g wet weight), and
E = concentration of stable element in water (ug/g).
If it is assumed that the specific activity (i.e., the ratio of radionuclide
concentration to the stable element concentration) in i is equal to that of
the water, the CF for the radionuclide, CF(R)., is also inversely
proportional to the concentration of the stable element:
CF(R)i - E1/Ew . (3)
This pattern is exemplified by radionuclides of some elements in fishes, but
by few elements in invertebrates. The classical example of this pattern is
the behavior of I in mammals in which the concentration of iodine is
under strict control .
The third pattern is that the CF for the radionuclide, CF(R)., is
inversely proportional to the concentration of a nonisotopic carrier element
in water (i.e., chemically similar to but occurring in higher concentrations
than the stable-element analogue). The derivation of this relationship
follows .
The CF for radionuclide R is related to CF(E*)., the CF for the
*
carrier element E , by
* CF(R)
CF(R). = CF(E ). —-fL , (4)
L r ( t j .
which may be written as
CF(R). = CF(E*)i
(R/E )w
* *
where (R/E ). and (R/E ) are ratios of radionuclide concentration to
carrier-element concentration found in the organism or tissue and in the
water, respectively. Assume that the nonisotopic carrier element is
homeostatically controlled in the organism, that is:
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(6)
^
where E- = concentration of nonisotopic carrier element in organism or
tissue i, a constant (yg/g wet weight),
and E = concentration of nonisotopic carrier element in water (yg/g).
* *
Combining equations (5) and (6) and letting q^ = (R/E )i/(R/E )w, the
desired expression is obtained:
CF(R). = -V- • (7)
1 Ew
This pattern is shown by very few radionuclides in marine organisms. The
classical example of this pattern is the behavior of radionuclides of cesium
in fresh-water animals; the nonisotopic carrier element is potassium in this
case.
ELIMINATION RATES
The accumulation of the stable or radioactive nuclide of an element by any
pathway can involve a number of different processes. If the rate-determining
process can be described mathematically, a model can be developed to predict
changes in concentration with time and location. A considerable effort has
been made to develop models to predict the distribution of radionuclides
released into the environment. The types of models developed to predict
concentrations of radionuclides in aquatic organisms include equilibrium and
dynamic models.
The type of model to be used in a given situation depends on the nature
of the release and on the properties of the ecosystem, when releases of
radionuclides are continuous and steady-state conditions are present, an
equilibrium model such as a CF model can be used. In this case, the important
parameter needed for the model is the CF, and the concentration in the animal
is determined by multiplying the concentration in the water by the CF. In the
case of accidental episodic releases, the result is a dynamic situation in
which organisms accumulate the material for a relatively short period and then
lose it with a characteristic rate constant. In this case, the important
parameters needed for the model are CFs and biological elimination-rate
constants.
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The elimination rate of stable and radioactive nuclides in organisms
depends on dynamic processes of exchange with elements in the environment.
Compartments of elements are identified from a mathematical analysis of the
changes in concentration during accumulation or loss. The resolution of
compartments is limited by experimental error, and the compartments that can
be identified are those whose concentrations differ significantly in their
elimination-rate constants. These compartments may be physiological,
structural, or chemical entities, and their metabolic significance may not be
known.
The biological half-life of a radionuclide in an organism depends upon the
organism and the properties of any element to which it may be related. Data
available on biological half-life of radionuclides indicate that, in most
marine organisms, the transfer of radionuclides to and from the water can be
described by one- or two-compartment models. In small organisms with a large
surface-to-volume ratio, the biological half-life of monovalent elements such
as sodium or cesium may be minutes, whereas in large organisms and multivalent
elements, it may be months. The biological half-life is also a function of
the metabolism of the element by the organism. The quantities accumulated by
organisms when the concentrations are increased in the water differ greatly
for those elements that are and those that are not under homeostatic control.
Derivation of Elimination Rates
The rate of change in concentration of a radionuclide (corrected for
radioactive decay to time zero) in an organism at any time may be described by:
dR-(t)/dt = k1 Rw(t) - k2 R.(t) , (8)
where
R (t) = the concentration in the water at time t,
R-(t) = the concentration in the organism or tissue i, at time t,
k-, = the biological accumulation-rate constant,
k~ = the biological loss-rate constant.
At steady-state conditions, Rw(t) = constant and dR.(t)/dt = 0, and
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R (s) k
F= -±— = ^, (9)
where
R-(s) = the concentration in the organism or tissue i, at steady-state
conditions.
If it is assumed that the radionuclide concentration in the water at any
time t is a constant, then equation 8 upon integration becomes:
k,R -k_t
R.(t) = _Lw [1 - e 2 1 . (10)
T K2
Substituting R^(s) = k-|Rw/k2 into equation 10, we have:
-k9t
R^t) = R^s) [1 - e l ] . (11)
In those situations where the concentration in the organism is not at
steady-state conditions and the concentration in the water is known and is
constant, the ratio of the concentration in the animal to that in the water
(CF ) can be substituted for concentrations in the animal to give:
CF*(t) = CF(s) [1 - e 2 ] , (12)
where
CF (t) = the nonsteady-state concentration factor in the organism at
t i me t,
CF(s) = the concentration factor in the organism at steady-state
conditions.
The loss of stable or radioactive (corrected for radioactive decay to time
zero) nuclides may be described by:
-k,t
Ri(t) - R^o) [e M , (13)
where
R.j(o) = the radionuclide concentration in the organism at time zero,
the time of equilibrium or cessation of exposure.
10
-------
From k?, the biological half-life (T 1/2) of a nuclide in an organism may be
determined from the relationship:
T 1/2 = - . (14)
K2
Determination of Elimination Rate Constants
The kinetics of radionuclide metabolism have been assessed both in whole
organisms and in specific body parts. Some of the techniques used to determine
elimination rates are by monitoring:
o the rate of uptake of radionucl ides in organisms exposed
to radionucl ides under controlled laboratory conditions,
o the rate of uptake of radionucl ides in organisms transferred from a
pristine to a radionucl ide-contaminated environment,
o the rate of loss of radionucl ides in organisms exposed to radionucl ides
under controlled laboratory conditions and then transferred to a
pristine environment, and
o the rate of loss of radionucl ides in organisms transferred from a
radionucl ide-contaminated environment to a pristine environment.
The extrapolation of the kinds of data derived from these types of experiments
to specific field conditions must be done with care. For example, it is
extremely difficult to design laboratory experiments that simulate real-world
conditions and provide the kinds of information required to predict the
accumulation and redistribution by marine organisms of radionucl ides released
into ecosystems. Ideally the radionuclide should be presented to the test
organisms in a manner similar to that which would occur in its habitat. In the
environment, the radionuclide may be present in the particulate and soluble
fraction of the water in different physicochemical forms, has been incorporated
into the food chain, and has been deposited in the sediments. Most laboratory
experiments performed do not have all abiotic compartments represented, and the
physicochemical form of the radionuclide to which the organisms are exposed is
not defined. Also, the test organisms should be fed, and the population
densities in the experimental container should be representative of those found
in the natural habitat. For many organisms, insufficient data are available
on their ecology to permit realistic experimental design. Furthermore, most
laboratory experiments are not conducted long enough to permit steady-state
11
-------
conditions of uptake and loss to be achieved in all compartments; this results
in underestimation of CF values. In spite of these limitations, data have been
acquired on elimination rates and accumulation factors that can be used to
evaluate the dynamics of radionuclide transfer in marine food chains.
PLUTONIUM
PHYSICOCHEMICAL FORM
The chemistry of plutonium is complex and is partly governed by the total
concentration in solution. Multiple oxidation states can coexist in solution
and the oxidation-reduction behavior is complicated (see review of Matters _e_t
al., 1980). There are four principal sources of data on the behavior of
plutonium: world-wide fallout; nuclear test sites (Marshall Islands and
Nevada); Thule, Greenland; and nuclear power plant outfalls.
The behavior of plutonium in seawater has been studied in widely
different ecosystems, and the concentrations measured differ by as much as
three orders of magnitude. Because the pH of the ocean is well buffered,
plutonium apparently cannot exist except as Pu(III) or Pu(IV) in solution in
the water column (Matters ert _aj_., 1980). Plutonium has a high affinity for
particulate material. This is described by a distribution coefficient (K,):
K - fs V
d (1 - fs) W '
where
fs = fraction of nuclide on the particulate fraction
1 - fs = fraction of nuclide in the soluble fraction
V = weight of water (g)
W = dry weight of particles (g).
The K^ as defined is dimensionless, and greater sorption of the nuclide to
the particulate fraction results in higher Kds.
The mean K^ recommended for use in models of both the pelagic and
coastal regions of the ocean is 100,000; the range of values recommended for
sensitivity analysis is from 10,000 to 1,000,000 (International Atomic Energy
Agency (IAEA), 1985). The oxidation state of plutonium on particles is
1 ~\
considered to be Pu(IV). Somewhere in the concentration range of 10 to
12
-------
10 _M, plutonium ceases to exhibit the properties of simple ions, and the
possible formation of polymeric species must be considered (Matters et al.,
1980). Consequently, when moderately concentrated solutions are used in
laboratory experiments, the results should not be used to predict the behavior
of plutonium in the environment.
PRIMARY PRODUCERS
Concentration Factors
Microalgae. Studies have shown that plutonium can be strongly
concentrated by primary producers (Jackson et_ _al_. , 1983). However, few
experimental studies of plutonium uptake by marine phytoplankton have been
conducted despite their importance in geochemical cycling and food chain
processes (Table 1 and Fig. 3). Fi sher _ejt _aj_. (1980) used environmentally
realistic atom concentrations to test the plutonium uptake by Thaiassiosira
pseudonana, Thaiassiosira sp., Platymonas sp., and glass particles. Yen
(1981) described the sorption of plutonium by two species of marine
phytopl ankton. More recently, Fisher _et_ _a_l_. (1983a) determined the ability of
six clones of marine phytoplankton to accumulate plutonium.
CFs obtained by Yen (1981) and Fisher et_ a_L (1983a) for phytopl ankton
tested in the laboratory demonstrated about an order of magnitude difference
with species (Table 1). Some values obtained in the field were lower than
those obtained under laboratory conditions (Fig. 3). It is not known whether
the low values were due to differences in species or to the absence of
steady-state conditions. The former is probably the reason because steady-
state conditions are reached relatively rapidly in phytopl ankton (Fisher _e_t
al., 1983a). Also, it would be expected that CF values determined in the
laboratory would be similar to those determined in the field if the organisms
were exposed to the same physicochemical forms of plutonium.
Dissolved organic matter (DOM) was found to affect the accumulation of
007 OQ7
Pu (III-IV) and Pu (V-VI) by the marine diatom Thaiassiosira pseudonana
(Fisher et al ., 1983b). Ethylenediaminetetraacetate at 0.3 unreduced
plutonium uptake, but marine fulvic and humic acids, naturally occurring DOM,
and diatom exudates did not reduce uptake.
13
-------
Table 1. Laboratory-derived concentration factors (CFs) for plutonium in
primary producers.
Organism
Thalassiosira pseudonana
T. pseudonana
Dunaliella tertiolecta
Oscillatoria woronichinii
Ernil iania huxleyi
E. huxleyi
Tetraselmis chuii
Monochrysis lutheri0
M. lutheri0
M. lutheric
M. lutheri
M. lutheri
Phaeodactylum tricornutunf
P. tricornutunf
P. tricornutum0
Ascophyllum nodosum
(brown algae)
A. nodosum
A. nodosum
A. nodosum
A. nodosum
Exposure,
d CFs
1
4
4
4
4
4
4
1
1
1
1
1
1
1
1
15
15
15
15
15
Microalgae
85,000-2,800,000
380,000
150,000
50,000
50,000
330,000
60,000
8100 + 5600
24,300 + 3700
32,800 + 10,700
34,200 + 15,900
44,900 + 12,500
38,100 + 19,800
46,500 + 10,700
72,300 + 26,600
Hacroalgae
797
415
298
578
738
Comments
Varied with
biotic and
abiotic factors
3H clone
Dun clone
OSE N4 clone
MCH No.l clone
BT-6 clone
Tet C2 clone
At 24°C
At 0°C
At 24°C
At 24°C
At 24°C
At 24°C
At 0°C
At 24°C
a Fisher et al. (1980).
b Fisher _et _al_. (1983a).
0 Yen (1981).
d Zlobin and Mokanu (1970).
14
-------
Primary Producers Annelida
Moltusca
Arthropods
Chordata
1,000.000
100,000
% 10,000
c
g
fD
^^
g
o
c
5 1000
100
10
Microbe**
Wh
-
O
~
o
o
o
—
-
ol.
8
•
:
1
•
M.cro.1^,
Wh
„
0
O
o
8
s
CD
ota
I
PolychMt.
Wh
•
«
_
*
Die
i
•
P«l*cvP»d.
Wh
|
0
ol.
.
•
Bodv
•
A
f
_
*
•
9
,
Sh
«
O
o
o
o
o
•
ell
•
Qinropod*
Wh
^
£
•
ol.
0
Body
•
4
S
LH_1
*
Sh
•
1
8
o
•
.
•ii
o
e
•
Ceph.lopod.
Wh
.
ol.
9
CrinUcva
Wh
•
•
GO
ok*
•
Exoskelelon
p.u*.
Wh
e
•
Bo
S
e
I
|
9
&
0.
-
—
-
.Figure 3. Concentration factors (CFs) for plutonium in marine biota: laboratory-derived CFs from this
report (•); field-derived CFs from Noshkin (1985) (•) or Jackson et al_. (1983) (o).
-------
The accumulation of plutonium appears to be a passive process; dead cells
accumulated about the same amount of plutonium as living cells (Fisher et_ _a1_.»
1980). Also, quantities accumulated were higher at low salinities and high
temperatures. Fisher et_ _al_. (1983a) investigated the effect of valence state
on accumulation; the CFs of Pu(III-IV) were similar to those of Pu(V-VI).
However, Pu(V-VI) may be reduced to Pu(III-IV) once it is associated with the
cells. The data available support the hypothesis that plutonium in marine
environments associates with suspended particles that could act as vertical
vectors for this element.
Macroalgae. Limited data are available on laboratory-derived CFs for
plutonium in benthic algae. Zlobin and Mokanu (1970) determined the uptake of
plutonium by the brown algae Ascophyllum nodosum (Table 1). CF values were the
same order of magnitude as those derived for other algae in the field (Fig. 3).
Guary and Fraizier (1977) proposed that the CF for plutonium is related to the
nature of the algal surface. They reported a CF of 1175 for Corallina
officinalis which has a calcified and strongly ramified structure, a CF of 523
for Fucus serratus which has a ramified, noncalcified blade, and a CF of 85 for
Laminaria digitata which has a large, smooth, noncalcified blade. Wong et al.
(1972) showed plutonium was accumulated on the very outermost (mucilage) layer
of the kelp Pelagophycus porra. Spies _et_ _al_. (1981) showed that high
concentrations of plutonium are associated with the coenocytic filaments in
the calcareous algae Halimeda macrophysa. Evidence currently available on
macroalgae indicates that the likely mechanism for accumulation is by
adsorption and that plutonium may be attached to large macromolecules or
micelles, which have slow diffusivities but great affinity for a variety of
surfaces (Beasley and Cross, 1980).
Elimination Rates
Microalgae. For the phytoplankton species examined by Fisher et al.
(1983a), steady-state conditions of uptake and loss of plutonium were reached
within a few days. Cells accumulated plutonium in proportion to the isotope
concentration in the water, and the amount of isotope associated with cells was
a direct function of their number (hence surface area). The data indicate that
isotope accumulation by cells ceased, not because of saturation of their
surfaces, but because they reached steady-state conditions of uptake and loss
16
-------
from the surfaces. Uptake was strongly affected by the nature of particle
surfaces, and cells from rapidly growing cultures took up more plutonium than
did those that were in late log phase of growth or were senescent (Fisher et_
_al_., 1980). Such differences prevailed even in experiments during which little
or no cell division took place. The authors state that most of the differences
in cellular plutonium levels in their experiments can probably be attributed
to differences in surface physiology related to the growth stages of the
cultures used for inocula. Cells accumulated more plutonium from UV-treated
seawater than from untreated or enriched seawater.
Macroalgae. Accumulation of plutonium in the brown algae Macrocystis
pyrifera appeared to be relatively rapid; steady-state conditions of uptake and
loss were reached within a few days (Hodge et. _al_., 1974). Spies _et ^1_. (1981)
measured the rate of loss of plutonium from Halimeda incrassata that had been
transferred from a highly contaminated crater in the Enewetak Atoll to the
lagoon that had a relatively low level of plutonium. The loss of plutonium
was found to be biphasic. Most of the plutonium was in a fast-exchanging
compartment that had a half-life of 1.4 d; the slow-exchanging compartment had
a half-life of about 30 d.
ANNELIDA - POLYCHAETA
Concentration Factors
Accumulation of plutonium by polychaete worms is of interest because they
live in the sediments and belong to a zoological group that occurs in deep
water. These organisms are expected and have been found in oceanic radioactive
waste disposal sites. Also, Noshkin et_ aj_. (1971) found that Nereis sp.
contained the highest plutonium concentrations of all invertebrates that they
analyzed. Fowler e_tal. (1975) showed that Nereis diversicolor readily
237
accumulated Pu (VI to IV) from seawater reaching CFs of about 200 (Table 2).
The concentration of plutonium in the bioassay container was held relatively
constant by changing the water daily and periodically adding some tracer to the
237
water. A marked reduction of Pu (VI) uptake was noted in worms accumulating
the isotope from water that had been used for the first worm experiment. The
237
authors suggest that Pu might have become associated with excreted
metabolites, e.g., mucus, and was thus rendered less available for
bioaccumulation.
17
-------
Table 2. Laboratory-derived concentration factors (CFs) for plutonium in
Annelida - Polychaeta.
Organism
Hermione hystrix3
H. hystrix3
H. hystrix3
Nereis diversicolor
H. hystrix0
Arenicol a marina
A. marina
Nereis diversicolor
N. diversicolor
Exposure,
d
22
22
20
15
27
21
14
25
25
CFs
370 + 10
275 + 11
0.05 + 0.01
200
130
7
0.002
190
0.001
Comments
Pu(III+IV), water
Pu(V+VI), water
Pu(III+IV) and (V+VI),
sediments
Pu(IV), water
Pu(IV), water
Pu(VI), water
Pu(VI), sediment
Pu, water
Pu, sediment
Aston and Fowler (1984).
Fowler et a_L (1975).
Grille et
(1981).
Miramand et _al_. (1982).
Murray and Renfro (1976).
18
-------
239
A comparison was made of the uptake of Pu from sediment and seawater
by Nereis diversicolor (Murray and Renfro, 1976). Plutonium was added to the
water and the sediment in the IV oxidation state; concentrations used in the
c c
experiments were between 10 and 10 times higher than those normally found
OOQ
under field conditions. Concentrations of Pu in the worm increased
throughout the 25-d exposure period, but steady-state conditions were not
reached. The CF from the sediments was calculated to be 0.001, that from the
seawater to be 190. Under the conditions of the experiment, it appears that
N. diversicolor obtained most of its plutonium from the seawater. The authors
compared the sediment CFs to those reported by Noshkin (1972) for a marine worm
from Cape Cod; the value for day 15 was about two orders of magnitude less than
those Noshkin (1972) measured in the environment.
pOO_OOQ
The accumulation of sediment-bound ~ Pu (VI) and of plutonium in
seawater by the polychaete worm Arenicola marina was determined by Miramand
et_ _al_. (1982). Bioavailabil ity from the sediment was low; after 14 days of
accumulation, the CF was only 0.002. Worms exposed to labeled seawater for
20 d had a CF of about 7.
The range of plutonium CFs in Annelida determined in the laboratory was
lower than that determined in the field (Fig. 3). This is not unexpected
because most of the exposure times were less than the biological half-life of
plutonium observed in N. diversicolor (see below) and that might be expected
in other polychaete worms.
Elimination Rates
The loss of plutonium was followed in N. diversicolor that accumulated
237
Pu (VI) for 8 d and then were transferred to nonradioactive water (Fowler
et_ _a_l_., 1975). The half-life computed for between days 4 and 35 of the loss
period was 79 d. Elimination of plutonium was followed also in Hermione
237
hystrix that had accumulated Pu from contaminated seawater (Aston and
Fowler, 1984). The loss from the worms indicated the presence of two (at
least) pools that had substantially different biological half-lives. The
long-lived pool had a half-life of 54 d and the short one of 1.3 d.
19
-------
MOLLUSCA
Concentration Factors
Pelecypoda. Bivalve molluscs have been used as indicator organisms of
both stable and radioactive nuclides because of their particular efficiency in
accumulating material from the water column. Because of this characteristic
and its world-wide distribution, the mussel Mytilus edulis has been used as a
sentinel organism (Goldberg et_ _al_., 1978). However, proper interpretation of
trends in radionuclide concentrations require knowledge of the rates of
elimination of the isotopes as well as their CFs.
Plutonium CFs determined in the laboratory are available for four
different bivalve molluscs (Table 3 and Fig. 4). CFs varied with species and
body part. The highest concentrations of plutonium were found in byssus
threads (Fowler _e_t _al_., 1975). High concentrations of other radionuclides have
also been found in this material, but the mechanism of binding is not known.
Higher CFs were found in the shell than in the body; the shell also contained
the largest fraction of the activity. The high concentrations in the shell may
primarily be the result of uptake by attached periphyton rather than of actual
accumulation into calcified tissues.
Examination of the changes of plutonium concentration in the body with
time indicated that none of these test organisms had reached steady-state
conditions of uptake and loss with the plutonium in the media. This lack of
equilibrium is the probable explanation for the range of the laboratory-
derived CFs being lower than that of CFs derived in the field (Fig. 3).
Gastropoda. CFs for plutonium that were determined under laboratory
conditions are available for only the gastropod Aporrhais pespelicani. Grille
et_ al_. (1981) determined the accumulation, tissue distribution, and loss of
plutonium in animals that were exposed to the isotope in the water for 20 d.
Accumulation did not reach steady-state conditions in all tissues, and the CF
values differed with the tissue and individual animals (Table 3). At the end
of the uptake period, more than 80% of the activity was in the shell; the
remaining activity was distributed about equally between the muscle and the
viscera.
20
-------
Table 3. Laboratory-derived concentration factors for plutonium in Mollusca
Organism
Body Exposure,
part d CFs
Comments
Venerupis decussata0
V. decussatac
V. decussatac
Pelecypoda
Whole 22 74+5
Whole
Whole
22
20
61 + 1
0.006
Mytilus galloprovincial is
(mussel )
M. galloprovincialis
Tapes decussatus (clam)c
T. decussatus0
T. decussatus0
T. decussatus0
Scrobicularia plana
(clam)
S. plana
S. plana
S. plana
S. plana
S. plana
Byssus
Body
Whole
Shell
Muscle
Viscera
Whole
Shell
Body
Whole
Shell
Body
15-25
25
17
17
17
17
14
14
14
42
42
42
1900-4100
27-70
140
250
0-10
10-30
100
0.01
0.005
190
360
40
Pu (III+IV), water,
nonequilibrium
Pu (V+VI), water,
nonequilibrium
Pu(III+IV) and (V+VI),
sediment
Varied with size and
time
Varied with animal
Pu(IV), water
Pu(IV), water
Pu(IV), water
Pu(IV), water
Pu(VI), sediment
Pu(VI), sediment
0.005 Pu(VI), sediment
Pu(VI), water
Pu(VI), water
Pu(VI), water
Aporrhais pespelicani
(snail)
• c
A. pespelicani
,c
A. pespelicani
A. pespelicani
,c
,c
A. pespelicani
.c
Gastropoda
Whole 21
Shell
Body
Shell
Viscera
21
21
21
21
110
140-230
20-130
10-20
20-210
Pu(IV), water
Pu(IV), water
Pu(IV), water
Pu(IV), water
Pu(IV), water
21
-------
Table 3. (Continued)
Organism
Octopus vulgaris6
Body Exposure,
part d CFs
Cephalopoda
Whole 15 65
Comments
Pu(IV), water
(octopus)
0_._ vulgaris
CK_ vulgaris
0_._ vulgaris
0^ vulgaris
f
Whole 15 65
Muscle 15 15
Hepatopancreas 15 50
Branchial heart 15 9300
and appendages
Pu(IV), water
Pu(IV), water
Pu(IV), water
Pu(IV), water
Aston and Fowler (1984).
Fowler _et _a]_. (1975).
Grille et a]_. (1981).
Miramand _et _al_. (1982).
Guary ej; _aj_. (1981).
Guary and Fowler (1982).
22
-------
10,000
1,000
2 TOO
u
re
0
•4-J
CT3
t»
•4-*
c
-------
Cep^ajopod_a_, Data on accumulation of plutonium are available for Octopus
vu1gari_s (Guary et_ a/L > 1981; Guary and Fowler, 1982). It is noteworthy that
this octopus effectively accumulated and distributed plutonium among the
internal tissues (Table 3). Of special interest was that after the two-week
exposure period, 41% of the plutonium was in the branchial hearts and
appendages9 which had a CF of 9300, The branchial hearts have been implicated
also in the uptake of cesium, cobalt, arnericium, and certain heavy metals.
The unique ability of the br an-mial hearts and appendages to concentrate many
elements may be related to their role in circulatory and excretory processes.
The elements appear to be localized in intracellular granules that include
pigtnented material. Similar granules have been found in other molluscs and may
be related to lysosomes (George and Viarengos 1985).
Elimination Rates
P_e_1_ecy_po_da. The elimination of plutonium in mussels has been followed
both under field and laboratory conditions. Mussels that accumulated Pu(IV)
directly from seawater showed a two-component loss when placed in unlabeled
seawater (Table 4). Under the laboratory conditions used by Fowler et_ al .
(1975)5 the biological half-life for the short-lived compartment containing 35%
of the total plutonium was 7 d; that for the long-lived compartment containing
65% of the total plutonium was 776 d. Mussels that had accumulated Pu(IV) from
both food and water showed more rapid elimination, owing to both a shorter
labeling time and presumably a more rapid clearance of labeled material
eliminated as feces. However,, field data of Goldberg et al „ (1978) on
239 240
' Pu indicated a very rapid elimination, measured in weeks or months.
The half-life of plutonium in the clam Venerupis decussata was followed
237
in animals that had accumulated Pu from either contaminated seawater or
sediment (Aston and Fowler, 1984). Loss of activity in those clams that had
accumulated activity from seawater took place as an approximately single
exponential function; the-half-life was 50 d. Loss of activity from those that
had accumulated activity from sediments took place as a single exponential
function also; the half-life was 24 d. No good explanation was given for the
differences in loss rates. Because loss was followed only for 46 d in the
seawater-contaminated clams and for 25 d in those contaminated from sediment,
the presence of longer components could have been missed.
24
-------
Table 4. Biological half-life (days) of plutonium in Mollusca.
Organism
Body
part Pool A Pool B Pool C Comments
Venerupis decussata
(c1 am)
V. decussata
c
Mytilus galloprovincialis
(mussel)
M^_ galloprovincial isc
Tapes decussatus
(clam)
NL_ galloprovincialis6
(mussel)
M_._ galloprovincialis6
M. galloprovincialis6
Pelecypoda
Whole 50(100)
Whole 24(100)
Whole 776(65) 7(35)
Whole 39(100)
Whole 62(65) 7(35)
Pu (III+IV) and
(V+VI), water
Pu (III+IV) and
(V+VI), sediment
Pu (VI), water
Pu (VI), water,
labeled food
Pu(IV), water
Whole 193(30) 10(40) 2(30) Pu(IV), water
Whole 192(30) 13(40) 1(30) Pu(VI), water
Shell 215(30) 4(40) -- Water
Octopus vulgar is
(octopus)
Cephalopoda
Whole 560(46) 2(30)
Pu(III+IV), water
Number in parentheses is the percent of total activity in the pool.
Aston and Fowler (1984).
Fowler _et _a_K (1975).
Grille _et a_U (1981).
Guary and Fowler (1981).
Guary and Fowler (1982).
25
-------
-
Gastropoda., ihe gastropod Aporrhai s pespel i carn_ lost L Pu at rates
comparable to those of the darn T_ape_£ decussata (half-life = 53 to 80 d)
(Grille et_ a]_«9 1981).
237
Cephalopoda., The loss of Pu from whole jjctopus^ vulgar is was slow and
appeared to take place from two compartments (Table 4). After a 70-d loss
period, the majority (>90%) of the plutonium was in the branchial hearts and
appendages (Guary and Fowler, 1982).
ARTHROPODA - CRUSTACEA
Con centr at iorj^F actors
The accumulation of plutonium by Crustacea has been monitored in only a
few animals (Table 5). The earliest research was performed using the lobster
Homaris vulgaris. Ward (1966) followed the direct uptake by lobsters of
plutonium from seawater and established that near equilbrium was reached in
the exoskeleton and gills after 50 d of exposure. However, at 220 d the
muscles gut, and hepatopancreas were still not at steady-state conditions.
Approximately 90% of the total plutonium taken up by the lobster was found in
the exoskeleton, and, as would be expected, the major portion that accumulated
was lost during molting.
The uptake of Pu(IV) and Pu(VI) from food and water was followed in the
shrimp Lysmata j>eti_caudata (Fowler et_ _a_L, 1975). No change in uptake rate
with different valence states was detected. However,, the valence state of
plutonium in the media was not documented during the course of the experiment.
For this shrimp, direct uptake from the seawater was slow, and body burdens
were reduced when molting occurred. Shrimp fed daily rations of labeled
Artemia sp^ for 15 d did not accumulate higher levels of plutonium than those
fed a single ration of labeled Artemia sp. When feeding of nonlabeled food
was resumed, the burden in the soft tissues was reduced rapidly.
Plutonium was incorporated into the hepatopancreas of the edible crab
Cancer pagunis that had been fed contaminated food. Absorption of plutonium
in the hepatopancreas was as high as 5%; < 0.3% was present in the hemolymph
(Fowler and Guary, 1977). Investigations were conducted to determine the
subcellular distribution of plutonium in the hepatopancreas of crabs that were
contaminated jn_ \nvo_ with b9Fe (Guary and Negrel, 1980). When the cytosolic
26
-------
Table 5. Laboratory-derived concentration factors (CFs) for plutonium in
Arthropoda - Crustacea.
Organism
Body Exposure,
part d CFs Comments
Lysmata seticaudata (shrimp)
Corophium volutator (amphipod)
C. volutator
Homaris vulgar is (lobster)1
Whole 25
Whole 14
Whole 12
Muscle 250
5-19 Pu(VI), water
0.1 Pu(VI), sediment
1000 Pu(VI), water,
nonequi1ibrium
3 Water
Fowler _et aj_. (1975).
Miramand _et aj_. (1982).
Ward (1966).
27
-------
o o 7
fraction of the hepatopancreas was incubated in vitro with Pu, approximately
20% of the plutonium was associated with compounds of molecular weight ranging
from 10,000 to 40,000. The investigators proposed that these proteins could
belong to the metallothionein family that has been shown to bind other heavy
metals such as cadmium, copper, zinc, and mercury. About 70% of the plutonium
eluted in the very low molecular weight fraction, which was below the
operational range of the Sephadex 6-200, and the authors suggest that this
plutonium was present as free metal. The distribution of plutonium was
different than that of Fe9 which was bound primarily with a soluble
protein of high molecular weight (M50,000).
Elimination Rates
Limited data are available on the half-life of plutonium in Crustacea.
Fowler ert _al_. (1975) found the loss of plutonium from shrimp was most rapid
when it was ingested with food. The initial rapid loss was due primarily to
clearance of the gut; the slower loss was due to other excretory processes.
When shrimp were exposed to plutonium in water, most was present in the
exoskeleton. Consequently, molting resulted in a rapid change in the body
burden and a change in the kinetics of elimination. Molts may play an
important role in the biogeochemical cycling of plutonium because the CF in
crustacean exoskeleton is high and plutonium in the molt is lost slowly. In
those areas where the bulk of marine animal biomass is composed of small
Crustacea that molt frequently, cast molts may be an important mechanism for
transporting plutonium to sediments as well as to detrital feeders (Fowler e_t
_aJL, 1976).
CHORDATA - PISCES
Concentration Factors
Laboratory-determined CFs for marine fishes are few in number; more field-
determined values are available (Figs. 3 and 4). Data available were obtained
by Pentreath (1978a, 1978b) who studied the uptake of 237Pu (VI) by plaice
(Pleuronectes platessa) and by the thornback ray (Raja clavate). The
assimilation of Pu by plaice was followed in fish exposed to the isotope in
237
water, in fish fed Pu-contaminated Nereis sp., and in fish injected with
28
-------
the radionuclide. Uptake from the water was very slow; after a 63-d uptake,
the CF was <1. Of the plutonium accumulated, most of it was in the digestive
tract. Plutonium was detectable in the livers of six of the seven fish used,
and only traces were measurable in blood cells, plasma, and bone of two fishes,
The thornback ray, a cartilaginous fish, appeared to assimilate more
237
Pu than the plaice. When rays were fed Nereis sp. that had been injected
with the radionuclide, and crab hepatopancreas that had been incubated with
237
Pu, the isotope was found consistently in the liver. In one fish, 0.2% of
the administered dose was found in the liver. Also, in rays that had been
237
injected with Pu, there were high concentrations of the radionuclide in the
spleen as well as the liver.
It is clear that the thornback ray differs from the plaice in the ability
237
to absorb Pu from labeled food. In comparable experiments, the plaice
livers did not contain more than 0.005% of the total plutonium given in a
single labeled meal, whereas the thornback ray livers contained up to 0.23% of
the plutonium administered. Also, the thornback ray had a higher estimated
percentage of the body burden in the skeleton than did plaice.
Elimination Rates
Data on the biological half-life of plutonium are available only for
237
plaice (Pentreath, 1978a). The retention of Pu by plaice fed injected
Nereis sp. and then fed unlabeled Nereis sp. was determined. The half-life
237
measured in 10 fish ranged from 9 to 49 d. When fish were injected with Pu
(IV) intramuscularly, the half-life was considerably longer; values ranged
between 642 and 877 d. Similar results were obtained from fish that had been
injected directly into the body cavity; half-life values ranged from 282 to
1100 d. There was marked redistribution of the isotope within fish after they
were injected with the isotope. The redistribution was independent of the site
of injection and resulted in the highest accumulations occurring in the liver,
kidney, and spleen. Growing fish incorporated a relatively larger fraction of
?37
the Pu body burden into skeletal material than nongrowing fish, and this
was attained at the expense of the isotopic content of the liver. Very little
237
Pu was incorporated into muscle.
29
-------
AMERICIUM
PHYSICOCHEMICAL FORM
The major source of americium to the environment is from nuclear weapon
testing.. It was assumed because the americiurn3 like plutonium,, was present in
high -fired oxide paitk'GS that it. would not dissolve in natural waters.
However, experimental dria f.-osri a wide variety of environments does not bear
out this assumption, end americium has been reported in the soluble fraction
of marine waters from a number of environments (see review of Matters et_ _a_K ,
1980).
Americium is known to form complexes that affect its physicochemical form
and increase the total concentration of the metal in the water. In seawater,
the most likely oxidation state is the III.,
Information on the biogeochemistry of americium in marine environments
indicates that most of the americium that was deposited in the ocean from
atmospheric fallout and nuclear wastes was transferred to the sediments. The
K, recommended for use in models of both the pelagic and coastal region of
the ocean is 250005,000; the range recommended for sensitivity analysis is from
100,000 to 20,000,000 (IAEA, 1985). However, it appears that americium is not
irreversibly retained on sediment particles,, but can be released into
interstitial waters and hence into the water column upon changes in the
concentration of americium in the overlaying waters (Noshkin and Wong, 1980).
PRIMARY PRODUCERS
Coficertrat,ion Fa. c tors
Americium concentration factors in marine plankton at steady-
state conditions were in the same range as those for plutonium (cf. Tables 1
and 6; Figs. 3 and 5). Appreciable differences were determined with species,
but cells accumulated americium in proportion to the radionuclide concentration
in the water (Fisher _et. _a]L , 1983a)<, The uptake by dead cells was compared to
that by live cells for two species. Uptake was identical , indicating that the
uptake process was passive. Uptake was not affected greatly by the presence
or absence of light, changes in salinity^ or the presence of other metals.
30
-------
Table 6. Laboratory-derived concentration factors (CFs) for americium in
primary producers (microalgae).a
Organism
Exposure,
d
CF
Comments
Thalassiosira pseudonana
Dunaliella tertiolecta
Oscillatoria woronichinii
Emiliania huxleyi
E_._ huxleyi
Tetraselmis chuii
Heterocapsa pygmaea
Monaco port particles
Offshore particles
3 to 7
3 to 7
3 to 7
3 to 7
3 to 7
3 to 7
3 to 7
3 to 7
3 to 7
410,000
130,000
7,000
70,000
150,000
50,000
280,000
110,000
640,000
3H clone
Dun clone
OSE N4 clone
MCH No. 1 clone
BT-6 clone
Tet C2 clone
Gymno clone
Natural
assemblages
Natural
assemblages
Fisher et al. (1983a).
31
-------
Primary Producers Annelida
Mollusca
Arthropoda
Chordata
100,000 L-
1 o.ooo U
1,000l-
-
o
o
100 H
10 U
1.0 h
0.1
Microalgae
Field
-
—
-
Lab
*
®
«
!
•
•
»
Polychaeta
Whole
Lab
»
1
*
•
Pelecypoda
Whole
Lab
Body
Lab
•
•
«
Shell
Lab
•
«®
Gastropoda
Body
Lab
«
Shell
Lab
0
Cephalopoda
Whole
Field
0
Lab
»
Crustacea
Whole
Lab
•
f
Q
®
•
•
•
Pisces
Skeleton
Field
-
®
i
-
Figure 5. Concentration factors (CFs) for americium in marine biota:
laboratory-derived CFs from this report (•); field-derived CFs from Noshkin
(1985) (•).
32
-------
However, the uptake of americium was directly proportional to the cell
concentration in the water and was related to the size and surface area of the
plankton. The effect of naturally occurring dissolved organic matter (DOM) on
the uptake of americium by Thalassiosira pseudonana was determined (Fisher _et
al_., 1983b). They concluded that the DOM did not appreciably affect the
O A ~\
bioavailability of the americium. The cellular distribution of Am was
studied in two algal species: the diatom Thalassiosira pseudonana and the naked
green alga Dunaliella tertiolecta (Fisher et_ al_., 1983c). After a 72-h
exposure of the algae to the isotope, 94% of the cellular 241Am was found in
the 745 x g and 2000 x g pellets. These data indicate that most of the 241Am
is associated with cell walls or membranes and does not generally bind to
soluble cellular proteins.
Macroalgae. No data on laboratory-derived CFs of americium in macroalgae
were available.
Elimination Rates
Microalgae. Different species of phytoplankton accumulated americium
rapidly, but the time to approach steady-state conditions differed with the
species; the range was from 2 to 4 d (Fisher ert _al_., 1983a). The loss of
americium was followed in two species, Thaiassiosira pseudonana and Dunaliel!a
tertiolecta (Fisher _ejt _a_L, 1983a). Loss curves were described by a two-
compartment model with a rapid initial loss (being greater in size in short-
term exposed cells) and a subsequent, more gradual loss. These investigators
proposed that this probably reflected the presence of two americium
compartments in the cells, with a greater fraction of cellular americium in
the more rapid compartment. Biological half-lives in the rapid- and
slow-elimination compartments were <1 to 1 d, and 10 to 12 d, respectively.
241
Macroalgae. The loss of Am was monitored from Halimeda incrassata
that had been transferred from a highly contaminated crater in the Enewetak
241
Atoll to the lagoon, which had a relatively low level of Am (Spies et
al., 1981). The loss rate constant for the fast-exchanging compartment was
0.49 (half-life of 1.4 d) and for the slow-exchanging compartment was 0.067
(half-life of 10.3 d). These exchange rates were similar to those obtained
for plutonium and europium.
33
-------
ANNELIDA - POLYCHAETA
Concentration Factors
Concentration factors for americium in the same species of nereidae worms
were generally higher for americium than plutonium (cf. Tables 2 and 7). Only
a few values are available for the uptake of americium from seawater (Fig. 4),
and these differ widely. It is not known whether the differences are due to
species, analytical methods, or the absence of steady-state conditions. One
potential source of variability is the presence of food or sediment in the gut
of the worms. These materials generally have higher affinities for americium
than worm soft tissues; varying amounts of these substances in the gut could
affect the CF value obtained. Another source of variability is the
physicochemical form of the americium in the water. Murray et_ al_. (1978) found
that the CF obtained in freshly prepared water was different from that obtained
in aged water, and that the CF was also affected by the pH of the water and
the partitioning of the americium between the soluble and particulate phases
of the water.
The CF values were considerably lower for uptake from sediment than from
water (Beasley and Fowler, 1976; Vangenechten et _al_., 1983). The values
determined by Beasley and Fowler (1976) from uptake from the sediment showed
an increase with increased exposure time; these were based on the dry weight
of the animal and sediment.
Elimination Rates
The accumulation of americium by worms from seawater occurred rapidly;
steady-state conditions of uptake and loss were reached in a few days (Beasley
and Fowler, 1976; Murray et _a]_., 1978; Grille _et _a]_., 1981; Miramand et _a_L,
1982). Grille et al_. (1981) followed the loss of 241Am from the polychaete
Herrnione hystrix. Analysis of the loss curves indicated the presence of at
least two distinct compartments within the worm. A long-lived compartment was
identified that contained about 60% of the activity, and radioactivity from
this compartment was eliminated with a biological half-life of 66 d (calculated
for the period between the 15th and 50th day). From the smaller short-lived
compartment, radioactivity was eliminated with a half-life of 6 to 7 d.
34
-------
Table 7. Laboratory-derived concentration factors (CFs) for americium in
Annelida - Polychaeta.
Organism
Nereis diversicolora
N. di versicolora
N. diversicolora
N. diversicolor3
Hermione hystrixc
H. hystrixc
H. hystrixc
Arenicola marina
A. marina
Nereis diversicolor
N. diversicolor6
Hermione hystrix
Body
part
Wholeb
Wholeb
Wholeb
Whole
Whole
Body wal
Setae
Whole
Whole
Whole
Whole
Whole
Exposure,
d CFs
5
15
40
225
22
1 22
22
14
21
20
20
40-50
0.0012
0.002
0.0024
0.004
1000
1900-2200
8000-13,000
2000-3000
18
2-4
16-21
0.05-0.12
Comments
Am in
Am in
Am in
Am in
Am in
Am in
Am in
Am in
Am in
Am in
Am in
Am in
sediment
sediment
sediment
sediment
seawater
seawater
seawater
sediment
seawater
aged seawater
fresh seawater
sediment
a Beasley and Fowler (1976).
Calculated from the dry weight of worm and sediment.
c Grille et al. (1981).
d
Miramand et _al_. (1982).
e Murray et _al_. (1978).
f Vangenechten _et _al_. (1983).
35
-------
MOLLUSCA
Concentration Factors
Pelecypoda. Americium CFs are available for three species of bivalve
molluscs (Table 8). The CFs differed with species and body part (Grillo et
_a_L, 1981; Miramand et _al_., 1982; Vangenechten _et _aj_., 1983). Most of the
activity was associated with the shell, and steady-state conditions of uptake
and loss were not reached. In Tapes decussatus., the uptakes of americium and
Plutonium were followed simultaneously in the same animals. At the end of the
3-wk exposure, plutonium was accumulated to a lesser extent than americium.
However, because steady-state conditions were not reached, it can not be
concluded that this same relationship would continue with time. In
Scrobicularia plana, accumulation from seawater and sediments was determined
independently. The CFs calculated from the sediments were lower than those
from the water. However, if the concentration of americium in the interstitial
water of the sediments instead of the concentration of the sediments is used
in the calculation, the CFs are more similar to those obtained with the
americium in the seawater. No field-derived CFs are available for Pelecypoda
(Figs. 5 and 6).
Gastropoda. Data on the accumulation of americium by gastropod molluscs
are available for only Aporrhais pespel icani (Grillo et_ a!., 1981). The CF
values obtained and the kinetics of bioaccumulation were similar to those for
the clam Tapes decussatus. In this organism also, the uptakes of americium
and plutonium were followed simultaneously in the same animals. Similar to
J_. decussatus, the CFs for americium after the 3-wk exposure were higher than
those for plutonium.
Cephalopoda. CFs were determined for the cephalopod Octopus vulgaris
(Table 8). The animals were exposed to americium and plutonium concurrently
for 15 d. Examination of the accumulation curves for both elements showed that
equilibrium had not been reached. Accumulation of plutonium appeared to be
more rapid than that of americium; after 2 weeks the whole-body CFs were 35 for
americium and 65 for plutonium. CFs for both elements were high in the gills,
but the highest CFs were found in the branchial hearts and appendages (7100 for
americium compared to 9300 for plutonium). In the branchial hearts, the
36
-------
Table 8. Laboratory-derived concentration factors (CFs) for americium in
Mollusca.
Organism
Tapes decussatusa
( c 1 am )
T. decussatus3
T. decussatusa
Scrobicularia plana
( c 1 am )
S. plana
S. p!anab
S. p1anab
S. plana
S. plana
S. plana
Venerupis decussatac
( c 1 am )
Aporrhais pespelicania
(snail )
A. pespelicania
Octopus vulgaris
(octopus)
0. vulgaris
a Grille et _al_. (1981).
Body
part
Shell
Body
Muscle
Whole
Shell
Body
Shell
Body
Shell
Body
Whole
Shell
Body
Whole
Muscle
Exposure,
d
Pelecypoda
20
20
20
14
14
14
14
14
32
32
40-50 0
Gastropoda
20
20
Cephalopoda
15
15
CFs
500
330
30
0.009
0.01
0.01
228
137
220
60
.004-0.02
580
330
35
33
Am
Am
Am
Am
Am
Am
Am
Am
Am
Am
Am
Am
Am
Am
Am
Comments
in seawater
in seawater
in seawater
in sediment
in sediment
in sediment
in interstitial water
in interstitial water
in seawater
in seawater
in sediment
in seawater
in seawater
in seawater
in seawater
c Vangenechten et _al_. (1983).
d Guary and Fowler (1982).
37
-------
Mollusca
Arthropoda
Chordata
1000
100
k.
8
0
(13
| 10
ro
Vm
C
CD
U
C
o
0
1
0.1
0.01
Pelecypoda
Lab
—
.
—
—
—
Cephalopoda
Lab
9
Crustacea
Lab
»
Picsas
Field
—
—
—
t>
@*
—
—
Figure 6. Concentration factors (CFs) for americium in muscle tissue of
marine biota: laboratory-derived CFs from this report (•); field-derived CFs
from Noshkin (1985) («).
38
-------
radionuclides are associated with granular pigment deposits or adenochromes
that occur in the cells and may be important in detoxication processes
(Miramand and Guary, 1981).
When contaminated food is ingested, americium is efficiently assimilated
(mean = 33%) into the tissues of the octopus (Guary and Fowler, 1982). These
investigators state that this assimilation coefficient is of the same order of
magnitude as that measured for plutonium in crabs (Fowler and Guary, 1977) but
is 30 times higher than coefficients for plutonium in fish (Pentreath,
1978a, b) and 300 to 3000 times those of transuranic nuclides in mammals.
Guary and Fowler (1982) proposed that the high degree of assimilation of
americium may be linked to the high food-conversion efficiency reported for
CL vulgaris.
Elimination Rates
Pelecypoda. Data on the biokinetics of americium in bivalve molluscs are
available for the clam Tapes decussatus and for the mussel Mytilus
galloprovincialis (Table 9). In the clam, at least two distinct compartments
that were eliminated at substantially different rates were found.
Radioactivity in the short-lived compartment had a half-life of 6 d and in the
long-lived compartment, 80 d.
Biological half-lives of americium were determined in mussels that had
0 A~\
been exposed to Am in the laboratory and then transferred to small cages
anchored in the littoral zone off Monaco (Guary and Fowler, 1981). Loss of
Am was described as the sum of three exponential functions. Two short-
lived compartments were identified. These represented a total of 80% of the
incorporated radionuclide and had half-lives of 2 and 3 wk. The remaining
241
fraction of Am was associated with a long-lived compartment that was lost
very slowly (half-life of 1.3 y). Loss rates of americium differed with body
part, with the most rapid occurring in gill, viscera, and shell. Some
241
indication of translocation of Am fi
muscle during depuration was obtained.
241
indication of translocation of Am from other tissues to the mantle and
Gastropoda. In the gastropod Aporrhais pespe1icani_, americium was lost
at rates comparable to those of the clam J_._ decussatus (Grille et_ a!., 1981).
Two compartments were identified, one that contained about 65% of the
39
-------
Table 9. Biological half-life (days) of americium in Mollusca.1
Organism
Pool A Pool B Pool C Comments
Tapes decussatus (clam)
Pelecypoda
80(55-65) 6(35-45)
Am in seawater
Mytilus galloprovincialis
(mussel)
480(25) 22(40) 11(40) Am in seawater
Aporrhais pespelicani
(snail)
.b
Gastropoda
80(65) 6(30)
Am in seawater
Octopus vulgaris
(octopus)
Cephalopoda
560(46) 2(30)
Am in seawater
Number in parentheses is the percent of total activity in the pool.
Grille £t _aj_. (1981).
Guary and Fowler (1981).
Guary and Fowler (1982).
40
-------
incorporated radionuclide and in which elimination was very slow, and another
that represented about 30% of the radioactivity and in which elimination was
rapid.
Cephalopoda. Data on the loss of americium are available for CL vulgaris
(Guary and Fowler, 1982). Whole body loss occurred with two compartments. The
short-lived compartment, which contained about 30% of the initial activity,
turned over very rapidly; half-life of about 2 d. Radioactivity in the long-
lived compartment had a half-life of 560 d. These investigators proposed that
the short-lived compartment could represent principally the skin, which
eliminated the radionuclide very rapidly, whereas the long-lived compartment
could represent the branchial hearts, which lost the radioactivity very slowly.
ARTHROPODA - CRUSTACEA
Concentration Factors
One of the early studies of the uptake of americium in crustaceans was
performed on brine shrimp and euphausiids by Fowler and Heyrand (1974). A
higher CF was obtained for the brine shrimp Artemia sp. than for the euphausiid
Meganyctiphanes norvegica (Table 10). A short-term experiment was performed
241
with Artemia sp. to determine uptake of Am from a labeled population of
phytoplankton. Uptake from the food appeared to be less efficient than that
from seawater; a CF of 400 was reached with the tracer in the food and of 1700
with the tracer in the seawater. Filtration of the seawater showed that most
241
of the Am was associated with the phytoplankton. When the CF was calculated
241
from the concentration of Am in the seawater in which the phytoplankton were
suspended, a CF similar to that obtained from the water alone was calculated.
The authors concluded that little americium was accumulated from the food.
The accumulation of americium was followed also in the brackish-water
amphipod Gammarus duebeni and the harpacticoid copepod Tisbe holothuriae
(Murray et^ _aj_., 1978). The CF was affected significantly by the
243
physicochemical form of the Am in the water; aging of the water before
the addition of the organisms reduced the CF values obtained. The uptake by
243
G. duebeni of Am from contaminated food was followed for 10 d. Unlike
243
the uptake from the water alone, the uptake of Am steadily increased;
steady-state conditions were not reached in the course of the experiment.
41
-------
Table 10. Laboratory-derived concentration factors (CFs) for americium in
Arthropoda - Crustacea.
Organism
Body Exposure,
part d CFs Comments
Arternia _sp.
(brine shrimp)
Meganyctiphanes norvegicac
(euphausiid)
Crab or Lobster"1
Crab or Lobster
Gammarus duebeni
(amphipod)
Corophium volutator
(amphipod)
C_._ volutator
C. volutator
Gammarus duebeni6
(amphipod)
G_._ duebeni
Tisbe ho1othuriaee
(copepod)
Cirolana borealis
(isopod)
Whole
Whole
48
64
1700 Am in seawater
125 Am in seawater
Muscle 8 5 Am in seawater
Muscle 8 25 Am in seawater
Whole 12 to 16 25-56 Am in aged seawater
Whole 14 0.12 Am in sediment
Whole 14 1200 Am in seawater
Whole 14 2700 Am in interstitial
waters of sediment
Whole 10 300 Am in seawater
Whole 10 40 Am in aged seawater
Whole 7 1070 Am in seawater
Whole 40-50 0.006-0.032 Am in sediment
a Fowler and Heyrand (1974).
Guary (1980), cited from Jackson et jfL (1983).
C Hoppenheit et _al_. (1980).
d Miramand ot_ a_K (1982).
6 Murray et_ a]_. (1978).
Vangenechten et al. (1983).
42
-------
Elimination Rates
Biokinetics of americium in Crustacea have been determined for a number
of species. The early work of Fowler and Heyrand (1974) did not provide a
value of biological half-life, but the authors report that accumulation was
rapid. In the brine shrimp Artemia sp., steady-state conditions were reached
in 48 h; in the euphausiid Meganyctiphanes norvegica, steady-state conditions
241
were reached in 64 h. When a single euphausiid that had accumulated Am
was placed in unlabeled seawater, it lost 40% of its burden during the first
8 d. When the animal molted, it lost almost all of its activity.
Guary (1980) determined the elimination of americium in a number of
decapod crustaceans (Table 11). Elimination was rapid, and only one
compartment was identified.
CHORDATA - PISCES
Concentration Factors
No data on CFs are available for fishes that were exposed to americium in
the laboratory. However, CFs are reported for tissues from fish exposed to
americium under field conditions (see reviews of Jackson _et _aj_., 1983 and
Noshkin, 1985). In muscle tissue, the CF values reported ranged from 0.05 to 5
(Fig. 6), in liver from 74 to 104, and in the skeleton from 25 to 178 (Fig. 5).
Elimination Rates
No data on biological half-life of americium in fishes were found.
CESIUM
PHYSICOCHEMICAL FORM
Cesium, like other alkali metals, exists primarily as free ions and does
not form inorganic complexes. In solution, it behaves like potassium, which
is present in greater abundance than cesium and serves as a nonisotopic carrier
element. The concentration of cesium in surface and deep seawater is 0.3 vig/kg
43
-------
Table 11. Biological half-life (days) of americium in whole Arthropoda
Crustacea.a*b
Organism
Prawn or shrimp
Prawn or shrimp
Prawn or shrimp
Prawn or shrimp
Prawn or shrimp
Prawn or shrimp
Prawn or shrimp
Pool
45(100)
5(100)
8(100)
2(100)
3(100)
5(100)
20(100)
Comments
Am in seawater
Am in seawater
Am in food
Am in food
Am in food
Am in food
Am in food
a Number in parentheses is the percent of total activity in the pool
b Guary (1980), quoted from Jackson et al. (1983).
44
-------
and 0.3 mg/kg, respectively, and that of potassium is 399 mg/kg for both areas
(Quinby-Hunt and Turekian, 1983). Because cesium sorbs to particulate
material, especially clays, it is present in higher concentration in
sedimentary material. The mean and range of distribution coefficients, K,s,
recommended for use in models of pelagic waters are 2,000 and from 500 to
20,000; recommended mean and range Kds for models of coastal waters are 3,000
and from 100 to 20,000, respectively (IAEA, 1985). Because the Kd for cesium
is relatively low, stable and radioactive nuclides of cesium in marine
ecosystems are primarily in the water column as soluble, ionic forms, and they
behave conservatively.
PRIMARY PRODUCERS
Concentration Factors
Concentration factors for cesium in primary producers are generally low
(Table 12). Because of the chemical similarities and relative abundances of
cesium and potassium concentrations in the water, potassium serves as a
nonisotopic carrier for cesium. Comparison of the CFs determined for field and
laboratory populations for radioactive cesium and stable cesium shows that the
ranges overlap except for the field-determined values for microalgae (Fig. 7).
The uptake of cesium by killed cells of Ulva lactuca gave CF values of 1-2
(Gutknecht, 1965). Also, seaweeds that had been exposed to Cs for up to
35 d released more than 90% of their activity when killed and kept for several
hours in the same radioactive medium. This investigator concluded that neither
physical adsorption, adsorption exchange, nor nonexchangeable binding could
137
account for much of the Cs taken up by the seaweeds examined.
The effect of external cesium concentration on cesium uptake was examined
in Gracilaria foliifera, Fucus vesiculosus, Ulva lactuca, and Porphyra
umbilicus (Gutknecht, 1965). A plot of log cesium uptake vs log external
cesium concentration was linear, indicating that uptake was exactly
proportional to external concentration. This investigator stated that these
137
results are consistent with the data indicating that Cs in seaweeds is
mainly ionic and not extensively adsorbed.
Cesium uptake was stimulated by light in all species examined (Gutknecht,
1965). This was first observed by Scott (1954), who suggested a connection
between the mechanisms of cesium accumulation and photosynthesis.
45
-------
Table 12= Laboratory-derived concentration factors (CFs) for cesium in primary
producers.
Organism
Nitzschia closteriumc
„ , a
Amphora sp.
Nitzschia sp.
Chlamydomorias sp,
Chlorella sp,a
Pyramimimonas sp.a
Nannochloris atomusa
Ulva sp. (green alga)
Enteromorphia sp, (green alga)
Fucus serrata (brown alga)
F. serrata
r j- b
F. serrata
Chrondrus crispus (red alga)
C. crispus
Corallina sp. (red alga)
Chrondus crispus (red alga)c
Acetabularia mediterranea
(green alga)
A. mediterranea
A., mediterranea
A. mediterranea
A. peniculus
A. peniculus
Batophora oerstedii
B, oerstedii
Boerges_en;i_a forbesii
Exposure,
d
Microalgae
13
13
13
13
13
13
13
Macroalgae
74
31
31
153
44
74 4
107
74 859
100-200
13
13
14
3-7
17
3
13
19
13
CFs
1.2
1.5
1.7
1.3
2.4
2.6
3.1
3 4
O ,H
4
6
16
4
,10,19
10-15
,13,13,14
10-20
13
1
1-2
<1
-------
Table 12. (Continued).
Organism
B. forbesiid
B. forbesiid
Fucus serratus (brown alga)
Porphyra sp. (red alga)
Ulva lactuca (green alga)
Porphyridium curentum (red alga)a
Ulva lactuca (green alga)6
Codium decorticatum (green alga)e
Fucus vesiculosus (brown alga)6
Dictyota dichotoma (brown alga)6
Porphyra utnbilicalis (red alga)6
Chondrus crispus (red alga)6
o
Gracilaria foliifera (red alga)
Agardhiella tenera (red alga)6
Q
Hypnea musciformis (red alga)
Monostroma sp. (green alga)
Scytosiphon lomentarium (brown alga)
Gracilaria confervoides (red alga)
Ulva ridiga (green algae)"
Cystoseira barbata (brown alga)^
Sargassum natans (brown alga)
S. fluitans
Green alga"1
Green alga1
Green alga1
Brown alga1
Brown alga1
Brown alga1
Red alga1
Red alga1
Red alga1
Red alga1
Exposure,
d
19
3
8
6
8
13
35
35
35
35
35
35
35
35
35
1
1
1
64
64
32
32
26
26
26
26
26
26
26
26
26
26
CFs
%1
<1
2
4-7
24-28
1.3
7
4
30
10
5
30
2.5
6
11
1.2
2
1.6
4-10
30
3.7
10.2
3.4 + 0.2
1.8 + 0.0
1.6 + 0.0
10 +_ 0.6
11.5 +_ 0.6
2.9 + 0.2
3.8 + 0.0
6.3 + 0.4
4.9 ^ 0.2
3.9 +_ 0.2
Comments
Effluent b
Effluent d
Effluent d
Effluent d
Effluent d
47
-------
Table 12. (Continued)
Organism Exposure, CFs Comments
d
Fucus vesiculosus (brown alga)1-1 45 50 Sulfate form
— ^
Cyrtymenia sp. (red alga)'1 11 5 ---
a Boroughs et _al_. (1957).
b Ancellin and Vilquin (1968).
c Avarques et _al_. (1968).
d Bonotto et aj_. (1981).
e Gutknecht (1965).
Hiyama and Shimizu (1964).
9 Polikarpov (1961),
h Polikarpov (1964).
1 Ryndina (1972), cited from Jackson _et _al_. (1983).
J' Scott (1954).
k Ueda et al. (1978).
48
-------
Primary Producers
Annelida
MoHusca
Arthropoda
Chordata
-pa
UD
10,000
1,000
100
10
_o
0.1
0.01
Microalgae
1
Polychaeta
Pelocypoda
Who
0
o
1
TT
0
8
o
00
O
a
A
••
Sho
O
o
?
B<
A
*
I
1
dy
.
t
Gasliopodii
Wh
0
o
l«
•
Bo
.
.
Jy
Sh
O
•ii
Cephalopoda
Ah
O
o
0
0
1.
Cru.c.e..
Wh
£b
99°
o
o
o
'•
Exoih
O
eleton
*
PllCOT
Wh
O
%
&
$
H^1
#'
ro
O
,i.
s
4
a.
A
•
-
Figure 7. Concentration factors (CFs) for cesium in marine biota: laboratory-derived CFs from this
report (•); field-derived CFs from Noshkin (1985) (•), field-derived data from Jackson ejt aj_. (1983) (o);
stable-element-derived CFs from Polikarpov (1966) (o).
-------
Elimination Rates
Information on the metabolism of cesium in primary producers is available
for only a few species of macroalgae (Gutknecht, 1965; Spies et_ jil_., 1981).
Half-lives ranged from 2 to 21 d (Table 13).
ANNELIDA - POLYCHAETA
Concentration Factors
Limited data are available on cesium for polychaete worms (Table 14).
Values reported for different species were < 10 for worms exposed only 11 d
as well as those exposed for 58 d. Rapid achievement of steady-state
conditions is expected because of the small size of most marine annelids.
Experiments were conducted to determine the relative importance of
137
sediment and seawater on the accumulation of Cs by Nereis japonica (Ueda
_e_t _al_. 5 1977). Worms were placed in direct contact with contaminated sediments
and also suspended in the seawater above the sediments. Although those in
137
direct contact with the sediments acquired greater concentrations of Cs,
the amount the worms acquired from the seawater was about 30 times greater than
that from the sediments.
Elimination Rates
137
The loss of Cs from both fed and unfed Nereis japonica was followed
(Ueda et_ _al_., 1977). The loss was relatively rapid and similar for both groups
of worms. The half-life was calculated to be 6 d for unfed worms and 8 d for
fed worms.
Elimination of cesium was followed in Neanthes diversicolor. In the whole
worm, the half-life was 8 d (Ueda et_ aj_., 1976).
MOLLUSCA
Concentration Factors
More data are available on CFs of cesium in Pelecypoda than for other
classes of Mollusca (Table 15). Data on the soft tissues were generally
50
-------
Table 13. Biological half-life (days) of cesium in primary producers
(macroalgae).
Organism Poola Comments
Ulva lactuca (green alga) 5
Codium decorticatum (green alga) 15
Fucus vesiculosus (brown alga) 8
Porphyra umbilicalis (red alga) 3
Chondrus crispus (red alga) 2
Gracilaria foliifera (red alga) 12
Agardhiella tenera (red alga) 21
Halimeda incrassata (calcareous alga)c 3
a
The percent of the total activity in the pool is 100
b Gutknecht (1965).
c Spies (1981).
51
-------
Table 14. Laboratory-derived concentration factors (CFs) for cesium in
Annelida - Polychaeta.
Organism
Arenicola marinaa
A. marina
Nereis diversicola
N. diversicola
N. japonica
N. japonica0
N. japonica0
N. japonica
M • - d
N. japonica
Exposure, d
21
21
58
33
11
11
11
11
14
CFs
2-3
4-5
7.5
6.3
6 + 1
5
0.16
0.2
0.18
Comments
Nonequilibriun
From sediment
From water
From food
and water
From sediment
From sediment
From sediment
Amiard-Triquet (1975)
Bryan (1963).
Ueda et a/L (1977).
Ueda et al. (1978).
52
-------
Table 15. Laboratory-derived concentration factors for cesium in Mollusca,
Organism
Scrobicularia planaa
(clam)
S. plana3
S. plana3
S. plana3
Macoma balthica3
M. balthica3
Chlamys operculata (clam)
C. operculata
Tapes sp. (clam)
-r b
Tapes sp.
Cardium edulis (clam)
C. edulisb
Mytilus edulis (mussel)
M. edulisb
Gyphaea ang.
Gyphaea ang.
Mytilus galloprovincial is
(mussel )
M. edulisd
Chlamys sp. (clam)
Tapes sp. (clam)
d
Tapes sp.
M. edulis
M. edulisf
M. edulis
M. edulisf
M. edulis
M. edulisf
M. edulis
M. edulisf
M. edulis
Body
part Exposure,
Pelecypoda
Body 21
Body 21
Shell 21
Shell 21
Body 21
Shell 21
Flesh 21
Shell 44
Flesh 74
Shell 31
Flesh 100-200
Shell 100-200
Flesh 100-200
Shell 100-200
Flesh 44
Shell 44
Whole 4
Body 100-200
Body 100-200
Body 100-200
Shell 100-200
Whole 26
Foot 22
Body 22
Shell 22
Foot 47
Body 47
Foot 54
Body 54
Adductor muscle 27
d CFs
8.2
8.9
2.6
1
7.1
0.5
8,14
0.7,0
11
0.9
10
0.3
10-11
0.3-5
8
0
4.3-6.4
10
10-15
10
1
3
7.8
8.5
0.09
8.5
10
9.1
10.5
8.4
Comments
From sediment
From sediment
Sulfate form
Sulfate form
Sulfate form
Sulfate form
Sulfate form
Sulfate form
Sulfate form
Sulfate form
Sulfate form
Sulfate form
53
-------
Table Ib. (Continued)
Organism
M. edulis
M. edulisf
M. edulis
M. edulisf
M. edulis
Crassostrea gigas 9
(oyster)
C. gigas9
C. gigas9
C. gigas9
Mya arenaria (clam)
M. arenaria
M. arenaria
Paphia philippinarum
( c 1 am )
P. philippinarum
Mya truncata (clam)J
Mytilus edulis (mussel )J
Ostrea edulis (oyster)J
Pecten maximus (scallop)J
Mytilus galloprovincialis
(mussel )
L-
M. galloprovincialis
M. galloprovincialis
Bivalve
Bivalve
Bivalve
Mercenaria mercenaria171
(clam)
Crassostrea virginicam
Body part
Pelecypoda
Retractor
Adductor
Retractor
Whole
Body
Whole
Body
Shell
Muscle
Whole
Body
Muscle
Body
Muscle
Whole
Whole
Whole
Whole
Shell
Body
Whole
Whole
Body
Shell
Body
Body
Exposure, d
(continued)
muscle 27
muscle 58
muscle 58
58
58
48
48
48
48
200
200
200
5
5
28
28
28
28
64
64
64
32
20
12
CFs Comments
9.8
7.8
8.8
12.9
9.2
7.7
9.4
9.2
6.6
4.6
3.0
10.0
7-9
3.5
2.3
1.7
1.7
0
10
3
10.5
97
0
6 Nonequilibrium
5
(oyster)
54
-------
Table 15. (Continued)
Organism
Body part Exposure, d
CFs
Comments
Gomphina melanaegis
(c 1 am)
G_._ melanaegis1
Ranqia cuneata0
Pelecypoda (continued)
Body 14
Muscle
Whole
14
29
6
2.3 Estuarine
Li ttorina 1 ittorina1-1
(snail)
Octopus vulgar is13
(octopus)
0. vulgaris
Gastropoda
Whole 28
Cephalopoda
Whole 14
Arms and 14
tentacles
6
6.4
a
b
c
d
e
f
g
h
i
j
k
1
m
n
o
P
Amiard-Triquet (1975).
Ancellin and Vilquin (1968).
Argiero et. _al_. (1966).
Avargues _et_ a_L (1968).
Bonotto _et _al_. (1981).
Bryan (1963).
Cranmore and Harrison (1975).
Harrison (1973).
Hiyama and Shimizu (1964).
Morgan (1964).
Polikarpov (1961), cited from Jackson e^t aj_. (1983)
Polikarpov (1964), cited from Jackson _et_ _al_. (1983)
Price (1965), cited from Jackson et _al_. (1983).
Ueda et aj_. (1978).
Wolfe and Coburn (1970).
Suzuki et al. (1978).
55
-------
Mollusca Arthropoda
100.000
10,000
o
5 1 ,000
c
o
2
c
0
o
100
10
1.0
n 1
PELECYPODA
Lab
—
~ '3k-.
ago
Sublu
O
O
0
o
CRUSTACEA
f=,«ld
••
«
Lib
O
oo
'00
CD
Sllblc
O
o
o
Uhordata
F,»ld
O
o
o
0
o
X
<&
PISCES
Lib
,
Tjf
A
a»
«a»
*
O
o
0°0
o
oo
St«b!»
-
-
A
*
A —
A
^
™
—
A
Figure 8. Concentration factors for cesium in muscle tissue of marine biota:
laboratory-derived CFs from this report (o); field-derived CFs from Jackson et_
a_K (1983) (o) or Noshkin (1985) (•); stable element-derived CFs from
Polikarpov (1966) (o) or Pentreath, 1977 (A).
56
-------
similar to those for muscle and indicate little bioconcentration of cesium.
Shell CFs were lower than those for living tissues, as expected. Comparison
of field-derived and laboratory-derived data shows that the highest values
were determined generally in field populations (Fig. 7).
Elimination Rates
Elimination rates of cesium have been determined for the oyster
Crassostrea gigas, the clam Mya arenaria, Gomphina melanaegis, and Anadara
granosa, and the mussel Mytilus edulis (Table 16). Two compartments were
identified in some species. The biological half-life for the short-lived one
was generally a few days while that for the long-lived one was generally a few
months. In the octopus, cesium in the arms and tentacles, which make up 68%
of the body weight, had a half-life of 90 d (Suzuki _et _aj_., 1978).
ARTHROPODA - CRUSTACEA
Concentration Factors
The range of CFs of cesium for Crustacea was similar to that for other
marine organisms (Table 17, Figs. 7 and 8). Again, some of the highest values
were obtained from Crustacea from field populations.
Elimination Rates
The only data available for elimination rates of cesium in Crustacea are
for a euphausiid and a prawn. Fowler et^ al_. (1971) found the half-life of
1 ^7
Cs in whole Euphausia pacifica to be 6 d. This zooplankton had been fed
radioactive Artemia sp. nauplii. Bryan and Ward (1962) followed the loss of
137
cesium in the prawn Palaemon serratus, which had acquired Cs through the
food chain. They found an average retention in three animals of about 70% of
initial body burden after 48 h in nonradioactive water, and a retention of
about 45% in one prawn after 6 d in nonradioactive water.
57
-------
Table 16. Biological half-life (days) of cesium in Mollusca.'
Organism
Body part Pool A
Pool B
Comments
Crassostrea gjgas
(oyster)
Mytilus edulisc
(mussel)
Mya arenaria (clam)(
FL_ arenaria
M^ arenaria
C_o_ virginica6
Anadara granosa
(clam)
A_._ granosa
Clam9
Clam9
Pelecypoda
Whole 90( —)
Whole
Whole
Body
Muscle
Whole
Whole
Whole
Body
Muscle
7.6(49)
3.6(75)
3.6(77)
3.3(65)
250(100)
3.0(70)
620.5(100)
3(100)
13(100)
60(25)
41(23)
33(35)
15.5(30)
Loss in situ
Octopus vulgaris
(octopus)
Cephalopoda
Whole 90(100)
a Number in parentheses is the percent of the activity in the pool
Cranmore and Harrison (1975).
c Dahlgaard (1981).
d Harrison (1973).
e Hess et a/L (1977).
f Patel e^^l_. (1978).
9 Price (1965)s cited from Jackson et al. (1983).
h Suzuki et al. (1978).
58
-------
Table 17. Laboratory-derived concentration factors (CFs) for cesium in
Arthropoda - Crustacea.
Organism
Crangon vulgaris (shrimp)3
Carcinus maenas (crab)3
C. maenas
C. maenas
Portunus puber (crab)
P . puber
P. depurator
P . depurator
Polybius henslowi (crab)
Cancer pagurus (crab)
C. pagurus
Corystes cassivelaunus
(crab)
C. cassivelaunus
Homarus vulgaris (lobster)0
Decapoda-Stomatopoda
Zooplankton
Zoopl ankton
Galathea squamifera
(squat lobster)
G. squamifera6
H. vulgaris
H. vulgaris
H. vuljjaris
Palaemon serratus
P. serratus
P. serratus
P. serratus
P. serratus
P. serratus
Body part
Whole
Whole
Whole
Muscle
Whole
Muscle
Whole
Muscle
Whole
Whole
Muscle
Whole
Muscle
Whole
Muscle
Whole
Whole
Muscle
Exoskeleton
Whole
Muscle
Exoskeleton
Whole
Muscle
Shell
Whole
Muscle
Whole
Exposure
d
12
7
67
67
67
67
67
67
67
67
67
67
67
28
58
11
11
150
150
150
4.2
4.2
4.2
4.2
4.2
4.2
CFs
20
4
8.5 +_ 0.6
17.7
6.6 + 1.48
13.1
6.5 + 0.0
12.0
5.2
6.0 + 1.4
11.3
4.4
11.4
4.7
19.4
12
14
12.6, 13.6
4.0, 4.2
7.6
14.9
1.5
29.2
33.9 + 2.6
10.9 + 4.5
25
25.6 + 1.6
29.5
Comments
Water, unfed
Water, unfed
Water, unfed
Food and Water
Food and Water
Food and Water
59
-------
Table 17. (Continued).
Organism
P. serratus
f
P. serratus
Leander pacificus^
L, pacificus^
L. pacificus^
Shrimp or prawn
Crangon vulgaris (shrimp)0
Pandalus montagui (shrimp)0
Leander serratus (shrimp)
Nephrops norvegicus
(euphausiid)
Body part
Muscle
Shell
Whole
Body
Body
Whole
Whole
Whole
Whole
Whole
Exposure
d
4.2
4.2
11
4
2
150
28
28
8
28
CFs
27.4 + 2.0
6.6 + 1.2
13.3 + 2.6
15
15
12-13
20
18
15.9
7.3
Comments
Food and Water
Food and Water
Cancer pagurus (crab)'
Whole
28
7.2
Bonotto et _al_. (1981).
Bryan (1961).
Morgan (1964).
Bryan (1963), cited from Jackson et _a_L (1983).
Bryan (1965).
Bryan and Ward (1962).
Hiyama and Shimizu (1964).
Lemee et_ _aj_. (1970), cited from Jackson et_ _a]_. (1983).
60
-------
CHORDATA - PISCES
Concentration Factors
Considerable data are available on CFs of cesium for marine fishes
(Table 18). CF values for fishes are similar in range to those of other
aquatic organisms (Figs. 7 and 8). A number of studies have been undertaken
to try to understand the effect of route of entry of the cesium radionuclides
on CFs and to ascertain whether trophic enrichment occurs (higher CFs in
organisms in higher trophic levels than in those in lower trophic levels).
Data are not available that permit conclusions to be made on the effects of
feeding behavior and trophic level on CF values (see review by Pentreath,
1981).
Factors affecting cesium accumulation that have been examined include the
addition of stable cesium and chelating agents, changes in temperature, and
differences in body weight. No effect on CFs of the addition of stable cesium
or of chelating agents was found (Hiyama and Shimizu, 1964). However, the rate
of accumulation of cesium by a number of species was found to decrease with
increased body size and to increase with increased temperature of the water
(Morgan, 1964; Nakahara et al., 1977).
134
A comprehensive study of the accumulation of Cs from seawater by the
plaice and the thornback ray was conducted (Jefferies and Hewett, 1971). For
these species, information is available on organ as well as whole body
134
accumulation. Every organ of the plaice accumulated Cs at a faster rate
than that of the ray.
Elimination Rates
Elimination of cesium in whole fish and fish muscle is relatively slow
(Table 19). In plaice and the thornback ray, kinetics of elimination of cesium
were evaluated from experiments that followed both the accumulation and loss
of the radionuclide; the biological half-lives compared well.
61
-------
Table 18. Laboratory-derived concentration factors for cesium in Chordata -
Pisces.
Organism
Blennius sp. (blenny)
Blennius sp.
Blennius sp.
Micropogon undu1atusc
(Atlantic croaker)
Paralichthys dentatus (flounder)0
Acanthogobius flavimanus (goby)
Pleuronectes platessa (plaice)6
P. platessa
p
Raja clavata (thornback ray)
R. clavata6
Clupea harengus (herring)
Pollachius virens (coalfish)
P. pollachius
Mugil chelo (grey mullet)
Gadus morhua (cod)
Trisopterus luscus (whiting)
Anguilla anguilla (eel )
Scophthalamus maximus (turbot)
S. rhombus
Limanda 1 imanda (dab)
Solea solea (sole)
P. platessa
R. clavata
Body part
Flesh
Whole
Flesh
Muscle
Whole
Muscle
Muscle
Whole
Muscle
Whole
Whole
Whole
Whole
Whole
Whole
Whole
Whole
Whole
Whole
Whole
Whole
Whole
Whole
Exposure
d
100-200
100-200
100-200
29
91
>30
800
800
800
800
28
28
28
28
28
28
28
28
28
28
28
28
28
CFs Comments
36,15
15-35
15-35
4.5 (Nonequilibrium)
9
25
20.2
10.6
2.3
3.4
9.2
4.0
3.5
2.7
2.7
2.1
1.6
2.8
2.6
2.5
2.5
2.1
0.5
Ancellin and Vilquin (1968).
Avargues ert _a_L (1968).
Baptist and Price (1962).
Hiyama and Shimizu (1964).
Jefferies and Hewett (1971).
Morgan (1964).
62
-------
Table 19. Biological half-life (days) of cesium in Chordata - Pisces.
Organism
Paralichthys dentatus
(flounder)
Micropogon undulatus
(Atlantic croaker)
Blennius pholis (blenny)c
Mugil chelo (mullet)0
Pleuronectes platessa (plaice)
P. platessa
Raja clavata (thornback ray)
R. clavata
P. platessa
P. platessa6
R. clavata6
R. clavata6
Evynnis japonica (sea bream)
Helicolenus hilgendorf
(scorpionf ish)
a Number in parentheses is the
b Baptist and Price (1962).
c Fraizier and Vilquin (1971).
d Hewett and Jefferies (1978).
e Jefferies and Hewett (1971).
f Suzuki et al. (1978).
Body part
Whole
Muscle
Whole
Whole
Whole
Muscle
Whole
Muscle
Whole
Muscle
Whole
Muscle
Whole
Whole
Pool Aa
5.3(34)
34.8(35)
20-30(12)
20-30(25)
57.9(100)
139.0(100)
68.8(100)
126.4(100)
64.7(100)
120.3(100)
179.7(100)
189.3(100)
75-95(100)
75-95(100)
Pool Ba Comments
36.9(66)
94.7(61)
203 + 18(88)
154 + 24(75)
Uptake
from water
Uptake
from water
percent in the pool .
63
-------
STRONTIUM
PHYSICOCHEMICAl FORM
Strontium has physicochemical properties similar to calcium and, like
calcium, appears mainly in ionic form in water. In seawater, calcium serves
as a nonisotopic carrier for strontium. The concentration of strontium in
surface seawater is 7.4 mg/kg and that of calcium is 417.6 mg/kg (Quinby-Hunt
and Turekian, 1983). Neither strontium nor calcium is strongly sorted by
particulate material. The mean Kd recommended for use in models of coastal
waters is 1000 and that for the pelagic waters sea is 200; the ranges are 100
to 5000 and 2 to 500, respectively (IAEA, 1985). Because of the low Kd of
strontium in marine ecosystems, most of the strontium is found in the water
column.
PRIMARY PRODUCERS
Concentration Factors
The CF values of strontium reported for microalgae ranged from 4 to 1600
(Table 20). A comparably wide range was found in field populations also
(Fig. 9). Experiments performed to evaluate factors affecting the uptake of
strontium by phytoplankton showed that the uptake of strontium was proportional
to the concentration of strontium in the medium (Corcoran and Kimball, 1963).
Furthermore, concentrations up to ten times the normal concentrations of
strontium did not seem to affect growth or strontium accumulation. For
macroalgae, the upper extent of the range of values reported was lower than
that for microalgae for both field- and laboratory-derived data (Fig. 9).
Elimination Rates
No laboratory-derived data on elimination rates of strontium in primary
producers were found.
64
-------
Table 20. Laboratory-derived concentration factors (CFs) for strontium in
primary producers.
Organism
Nitzschia closteriuma
Phytoplankton
Chlamydomonas minima
Carteria sp.
Carteria sp.
Diva lactuca (green alga)e
Monostroma sp. (green alga)
Sargassum thunbergii (brown alga)
Gracilaria confervoides (red alga)
Fucus serratus (brown alga)9
Ulva rigida (green alga)9
U. lactuca (green alga)9
Dictyota fasciola (brown alga)9
Padina pavonia (brown algae)9
Cystoseira barbata (brown alga)9
Corallina rubens (red alga)9
Ceramium rubrum (red alga)9
Polysiphonia elongata (red alga)9
Phyllophora nervosa (red alga)9
Green alga
Green alga
Brown alga
Brown alga
Brown alga
Red alga
Red algah
Red alga
Red alga
j n h
Red alqa
Exposure
Microalgae
24
24
Macroalgae
10
7
7
f 7
8
8
8
26
26
26
26
26
26
26
26
26
26
, d CFs
17
9
4
561
1600
0.3
6.7
6.5
5.3
40
2
1
18
19
40
4
1
1
8
0.8 + 0.0
1.0 +_ 0.0
42.1 + 2.0
25.3 +_ 3.4
6.4 +_ 0.2
1.4 +_ 0.0
3.8 + 0.2
1.3 +_ 0.0
2.2 +_ 0.4
2.3 + 0.0
Comments
Rapidly growing
Extracted from
dead plants
7 and 70 mg Sr/L
7 and 70 mg Sr/L
7 and 70 mg Sr/L
65
-------
Table 20. (Continued).
Organism Exposure, d CFs
Fucus serratus (brown alga)1 -- 40
F. serratus1 -- 30
F. vesiculosus -- 23
F. vesiculosus -- 35
Ascophyllum nodosum (brown alga)1 -- 22
Laminaria digitata (brown alga) -- 14
Chrondrus crispus (red alga)1 -- 1.7
Gigartina stellata1 -- 2.2
Ulva lactuca (green alga) -- 1.2
Comments
In dark
New growth
a Boroughs et _al_. (1957).
b Martin (1958), cited from Jackson et al. (1983).
c Polikarpov (1964).
d Rice (1956).
e Hampson (1967), cited from Jackson et al. (1983).
Hiyama and Shimizu (1964).
9 Polikarpov (1966).
h Ryndina (1972), cited from Jackson et al. (1983).
1 Spooner (1949).
66
-------
Primary Producers
Arthropoda
Chordata
10.000
1,000
100
10
,
0.
0.0
Mactoalgae
Whole
Field
0
8
o
o
'£3
QD
Lab
*
£
(
£.
s
?
•
Stable
O
O
O
o
99
«
o
0
o
0
Mictoalgae
Whole
Field
O
O
8
o
0
§
0
CD
Lab
*
*
•
»
•
Stable
0
O
Pelecypoda
Whole
Field
O
0
o
&
0
Ljb
»
Shell
Field
s
O
O
Lab
•
Body
Lab
\
Uaitco
Shell
Field
0
poda
Body
Fluid
V
Cephalopoda
Whole
Field
3
Stable
O
Cmitacea
Whole
Field
•JO
O
o
Lab
•
ac
•
e
Stable
O
0
E
Field
r~keiet
Lab
.
3n
Stable
O
Pitcei
Whole
Field
,»
*
%
O
Lab
•
•
Stable
'-•
Skeleton
Field
O
(j
8
.
Lab
8
•
Stable
-
t
A
Figure 9. Concentration factors (CFs) for strontium in marine biota: laboratory-derived CFs from
this report (•); field-derived CFs from Jackson et a]_. (1983) (o) or Noshkin (1985) (•); stable-
element-derived CFs from Polikarpov (1966) (o) or Pentreath (1977) (A).
-------
ANNELIDA
No laboratory-derived data on CFs and elimination rates of strontium in
Annelida were found.
MOLLUSCA
Concentration Factors
Data on CFs of strontium in Mollusca are available only for Pelecypoda
(Table 21, Figs. 9 and 10). Values are considerably lower for soft tissues
than for the shell. Because of the accumulation of radioisotopes of strontium
90
in shells of bivalves, they have been used to monitor Sr contamination in
the aquatic environment (Nelson, 1962).
Elimination Rates
No data on elimination rates of strontium in Mollusca were available.
ARTHROPODA - CRUSTACEA
Concentration Factors
Limited numbers of CFs of strontium are available for Crustacea (Table 22,
Figs. 9 and 10). However, the range of values is similar to that for other
marine organisms. Some of the highest values were obtained from Crustacea from
field populations. CFs of exoskeletons were higher than those of soft tissues,
and accumulation of strontium in the exoskeleton may account for the high CF
values for whole animals.
Elimination Rates
No data on the elimination of strontium in Crustacea were available.
68
-------
Table 21. Laboratory-derived concentration factors (CFs) for strontium in
Mollusca - Pelecypoda.
Organism
Mytilus galloprovincialis3
(mussel )
Crassostrea sp. (oyster)
Mercenaria mercenaria (clam)c
M. mercenaria0
Meretrix meretrix (clam)
Venerupis phil ippinarum (clam)
V. phil ippinarum
V. phi 1 ippinarum
V. phil ippinarum
V . phi 1 ippinarum
Mytilus edulis (mussel)
M. edulis6
M. edulis6
Body part
Whole
Body
Shell
Body
Muscle
Muscle
Body
Shell
Body
Shell
Body
Shell
Whole
Exposure
d
5
20
20
20
20
18
18
64
64
64
CFs Comments
3.6
1
10 Nonequi 1 ibrium
0.9
>0.7
>0.4
0.8 7 mg Sr/L
1.5 7 mg Sr/L
0.5 70 mg Sr/L
1 .6 70 mg Sr/L
0.7
6
6
a Argiero et al. (1966).
b Boroughs _et _a_L (1957).
c Chipman (1959).
Polikarpov (1961).
69
-------
10,000
1,000
100
0
y
CO
c
0
co
C
§ 10
1
0.1
n m
Mollusca
Pelecypoda
Field
-
-
—
-
_
Lab
•
*
Stable
O
O
00
Arthropoda
Crustacea
'Lab
*
Stable
88
0
O
Chordata
Puces
Field
S
Lab
•
e
Stable
-
-
—
—
O
A —
*
A
O
ox*-
Figure 10. Whole-body concentration factors (CFs) for strontium in muscle
tissue of marine biota: laboratory-derived CFs from this report (•)
field-derived CFs from Noshkin (1985) (•); stable-element-derived CFs from
Polikarpov (1966) (o) or Pentreath (1977) (A).
70
-------
Table 22. Laboratory-derived concentration factors (CFs) for strontium in
Arthropoda - Crustacea.
Organism
Body part
Exposure, CFs
d
Comments
Artemia salina (brine shrimp)3
A. salina3
Tigropus californicus3
Leander sp. (shrimp)
Leander sp.
L. squillac
Krilld
Krilld
Krilld
Whole
Whole
Whole
Muscle
Exoskeleton
Whole
Whole
Whole
Whole
1
3.8
9
9
64
4-6
4-6
4-6
0.7
0.2
1
0.2
15
8
8.0 + 0.6
12.1 +; 0.9
29 + 0.9
Nauplii
Nonequilibrium
Site 1
Site 2
Site 3
Boroughs _et _al_. (1958).
Hiyama and Shimizu (1964).
Polikarpov (1966).
Tolkach and Gromov (1976).
71
-------
CHORDATA - PISCES
Concentration Factors
Laboratory-derived CFs of strontium have been obtained for both bony and
cartilagenous fishes (Table 23). Examination of the experimental data on
accumulation of strontium shows that almost all the experiments were too short
in duration for steady-state conditions of uptake and loss to have occurred.
Absence of equilibrium conditions is indicated also because the field-derived
CFs were larger than the laboratory-derived CFs (Figs. 9 and 10).
The effect of differing calcium and strontium concentrations on the
occurrence of the radioisotopes of these elements in tissues as well as the
relative role of the food and water pathway in accumulation of strontium have
been examined. However, the interpretation of the results from studies of both
of these factors is controversial. Because the results of these investigations
have been reviewed recently (Pentreath, 1981), a discussion of the data will
not be included here.
Elimination Rates
The metabolism of strontium in the Atlantic croaker Micropogon undulatus
was investigated by Baptist et_ aj_. (1970). The loss was biphasic and the
half-lives were 1.25 d and 138 d for the short- and long-lived components,
respectively. The short-lived component was 21% and the long-lived was 79% of
the total activity. Analysis of the rates of loss from tissues indicated that
the long-lived component represented loss from bones and scales.
COBALT
PHYSICOCHEMICAL FORM
Cobalt is commonly present in more than one chemical form in seawater.
It can be present in ionic form or associated with dissolved organic material.
Cobalt may also be present in low concentration in the form of cyanocobalamin
(vitamin B 12), which is required by many aquatic organisms but synthesized by
only a few. The concentration of cobalt in surface waters is 7 ng/kg and in
deep waters is 2 ng/kg (Quinby-Hunt and Turekian, 1983). These authors state
72
-------
Table 23. Laboratory-derived concentration factors (CFs) for strontium in
Chordata - Pisces.
Organism
Tilapia mossambicaa
Mugil cephalus (mullet)
Fundulus heteroclitus
(mummichog)
Rudarius ercodes0
R. ercodesc
Pterogobius elapoidesc
P. elapoides0
Acanthogobius flavimanus (goby)c
A. flavimanus0
Trachurus japonicus
T. japonicus0
Pleuronectes platessa (plaice)
P. platessa
Body part
Whole
Whole
Muscle
Muscle
Vertebra
Muscle
Vertebra
Muscle
Vertebra
Muscle
Vertebra
Whole
Flesh
CFs
0.3
5
0.1
0.03
0.5
0.04
1.4
0.04
0.7
0.06
1.5
1.0
0.15
Comments
Euryhal ine
Young
Nonequilibrium
Nonequi 1 ibrium
Nonequil ibrium
Nonequi 1 ibrium
Boroughs _et _a]_. (1956).
b Chipman (1959).
0 Hiyama and Shimizu (1964).
d Templeton (1959), cited from Jackson et al. (1983).
73
-------
that cobalt is maximum in concentration in surface waters and, with depth, is
positively correlated with the labile nutrients and negatively correlated with
dissolved oxygen.
The K, for cobalt is higher than that for cesium and strontium. The mean
K, recommended for use in models of coastal waters is 100,000 and that for
d
pelagic areas is 3,000,000; the ranges are 20,000 to 500,000 and 50,000 to
5,000,000, respectively. Because of its high affinity for particulate
material, cobalt is found primarily in the particulate fraction of the water
column.
PRIMARY PRODUCERS
Concentration Factors
Although the data available on CFs of cobalt determined under field and
laboratory conditions in microalgae are limited, CFs have been determined for
many different macroalgae (Table 24, Fig. 11). The range of CFs for macroalgae
is similar for stable-element- and radionuclide-derived values. These results
indicate that steady-state conditions of uptake and loss of cobalt were
probably reached in the laboratory experiments.
The marine alga Dunaliella bioculata was found to concentrate Co
rapidly, and the CF determined was considerably lower in the presence of
increased concentrations of stable cobalt (Kirchmann et_ ^1_., 1977). The
accumulation of Co by Ulva sp. is reported to be dependent on light; the
CF was 2.5 times higher in algae grown in the light than in the dark. These
results indicate that accumulation of cobalt may be an active rather than a
passive process,
Elimination Rates
Few data are available on the biological half-life of cobalt in primary
producers. The biological half-life of cobalt in Ulva pertusa was determined
to be 10 d (Nakahara et_ al_., 1975). The loss of 60Co from Halimeda incrassata
was found to be fit best by a one-compartment model; the half-life was 9.4 d
(Spies et_al_._, 1981). Mattsson et_ al_. (1980) reported a biological half-life
of 60 ^ 15 d for Fucus vesiculosus that was collected from waters around the
Barseback Nuclear Plant.
74
-------
Table 24. Laboratory-derived concentration factors (CFs) for cobalt in
primary producers.
Organism
Dunaliella bioculata3
Phytoplankton
Porphyra sp. (red alga)3
Acetabularia mediterranea
(green algae)
A. mediterranea
A. mediterranea
Ulva lactuca (green algae)3
U. pertusa0
U. pertusa0
Sargassum thunbergii (brown alga)
A. mediterranea
A. mediterranea
U. pertusa6
Laminaria japonica (brown alga)
Eisenia bicyclis (brown alga)6
Q
Undaria pinnatifida (brown alga)
Hizikia fusiforme (brown alga)6
Sargassum thunbergii (brown alga)
Chondrus ocellatus (red alga)6
Q
Ahnfeltia paradoxa (red alga)
Body part
Exposure
Microalgae
Whole 27
Whole
Macroalgae
Whole 19
Whole 2
Whole 21
Whole 25
Whole 19
Whole 22
Whole 22
c Whole 22
Whole 7
Chloroplasts 7
Whole 20
Whole 20
Whole 20
Whole 20
Whole 20
6 Whole 20
Whole 20
Whole 20
, d CFs Comments
100
326
314
187
410
228
612
380 August
>17 April
420
200-400
18-25
439
138
34
120
127
2574
833
290
Bonotto et _aj_. (1978).
Martin (1958), cited from Jackson _et _a_L (1983).
Hiyama and Khan (1964).
Kirchmann et^ a]_. (1977).
Nakahara et al. (1975).
75
-------
Primary Producers
Mollusca
Arthropoda
Chordata
100.OOO -
10,000
1.000 -
100 -
10 -
0.1
Macioale*
Whole
Field
O
O
-
_
-
Lab
«
t
t
t
;
*
Stable
0
§
O
0
o
0
0
...
Microelgae
Whole
Lab
Pelecypoda
Whole
Lab
*
.,
Stable
A
A
A
00
Shell
Lab
•
•
•0
**
••
•
•
«
Body
Field
•
Lab
i
*
.
Stable
A
A
A
A
Giutropod*
Body
Stable
A
A
Cephalopoda
Whole
Stsble
A
A
A
A
A
Cruitacae
Whole
Fi«ld
«
Lab
»
•
Stable
-,
O
A
0
•i
A
Crustacea
Exoikeleton
Lab
e
Stoble
A
A
PllCtl
Whole
Lab
t
Stable
-
-
—
Li
g
U
-
~
1 -
Figure 11. Concentration factors (CFs) for cobalt in marine biota: laboratory-derived CFs from this report (•);
field-derived CFs from Jackson e_t al_. (1983) (o) or Noshkin (1985) (•); stable-element-derived CFs from
Polikarpov (1966) (o), Shimizu et _a_L (1970) (A).
-------
ANNELIDA - POLYCHAETA
Concentration Factors
CF values of cobalt have been determined for only a few polychaete worms.
For Arenicola marina, CFs of 10 for the coelomic fluid, 1000 for the blood, and
25 for the digestive tract were determined (Triquet, 1973). For whole A.
marina, a CF of 335 was obtained (Amiard-Triquet, 1975). For Neanthes
diversicolor, uptake of cobalt from water, food and water, and sediment was
investigated (Ueda et al., 1977). The CFs obtained from worms exposed to
radioactive cobalt in the water was 6^1, in the food and water was 7, and in
the sediment was 0.045 and 0.055. Young (1982) investigated the accumulation
by Neanthes virens of Co released into seawater from the corrosion of
neutron-activated stainless steel. The average CF from water during months 6
to 13 of the exposure was 343 ± 123 and from sediment was 2.25 ± 0.36.
Elimination Rates
The loss of Co from Nereis japonica was followed for 24 d (Ueda _e_t
al., 1977). There was a rapid loss of Co during the first 2 to 3 d and
then the rate of loss was slower. The half-life obtained for the slower
compartment was 37 d.
MOLLUSCA
Concentration Factors
CF values of cobalt in Mollusca are presented in Table 25 and Figs. 11 and
12. The highest values were obtained in the experiments of longest duration.
Comparison of the field- and laboratory-derived data shows that the range of
values for the body was different (Fig. 10). These data indicate absence of
steady-state conditions for most, if not all, populations exposed under
laboratory conditions.
Investigations have been made of the importance of food and water in the
uptake of cobalt by Mollusca. Nakahara et al. (1976) showed that the
absorption of Co by some Mollusca depended on the species of algae on
which they were fed; the percent absorbed varied from 26 to 47. Amiard (1978)
77
-------
Table 25. Laboratory-derived concentration factors (CFs) for cobalt in
Mollusca.
Organism
Scrobicularia plana (clam)
S. planaa
Macoma balthica (clam)a
M. ba1thicaa
Mytilus edulis (mussel)
Crassostrea gigas (oyster)
C. gigasc
C. gigas0
C. gigasc
Mya arenaria (clam)
• d
M. arenaria
M. arenaria
Phaphia philippinarum (clam)e
P. philippinarum6
P. philippinarum6
P. philippinarum6
Venerupis philippinarum (clam)
V. philippinarum
V. philippinarum
Mytilisepta virgatus^
(mussel )
M. virgatus^
M. virgatus^
M. virgatus^
M. virgatus^
M. virgatus9
Mytilus edulis (mussel )h
M. edulish
Body part
Pelecypoda
Body
Shell
Body
Shell
Whole
Whole
Body
Muscle
Shell
Whole
Body
Muscle
Shell
Viscera
Shell
Viscera
Viscera
Muscle
Shell
Body
Body
Shell
Shell
Muscle
Muscle
Body
Shell
Exposure
d
35
35
35
35
26
48
48
48
48
179
179
179
10
10
10
10
22
22
22
40
40
40
40
40
40
15-35
15-35
CFs
32
76
22
53
30
300
51
41
610
220
82
100
35
10
3
2
9.2
>7
36
1.4
13
0.7
11
0.8
8.5
140
190
Comments
No carrier
No carrier
Carrier added
Carrier added
Trisglycinato
complex of Co
Ionic Co
Trisglycinato
complex of Co
Ionic Co
Trisglycinato
complex of Co
Ionic Co
CoCl2,200 ppm
CoCl0,200 ppm
78
-------
Table 25. (Continued).
Organism
Exposure
Body part d
CFs
Comments
M_._ edulis1
M^ edulis1
_M_._ edul i s
M_._ edul i s
M. edulis1
M. edulis
Macoma inquinata1-1
M. inquinata
Body
Shell
Body
Shell
Body
Shell
Whole
Whole
60
60
60
60
60
60
390
390
135 j^ 40 Nonequilibrium
40 +_ 18 Nonequilibrium
155 _+ 30 Nonequilibrium
75 +_ 30 Nonequilibrium
120 + 20 Nonequilibrium
52 + 15
244 + 95
Nonequi1ibrium
From water
0.48 + 0.1 From sediment
Octopus or squid
Cephalopoda
Muscle
30
15
Amiard-Triquet (1975).
b Bonotto _et aj_. (1981).
c Cranmore and Harrison (1975)
d Harrison (1973).
e Hiyama (1962).
f Hiyama and Khan (1964).
9 Nishiwaki _et a_L (1981).
h Shimizu _e_t _a]_. (1970).
1 van Weers (1973).
J' Young (1982).
k Nakahara et al. (1979a).
79
-------
Mollusca
Arthropoda
Chordata
10,000
1,000
3
u
CO
c
o
CO
c
8
o 10
1
0.1
0.01
Pelecypoda
Field
-
-
-
-
-
-
Lab
•
s
•
Stable
§
O
Crustacea
Lab
•
Stable
O
Pisces
Field
OO
O
I
Lab
*
Stable
-
-
A
A
^-
O
cmo
'j^yu
A*A
0 _
-
-
Figure 12. Concentration factors for cobalt in muscle tissue of marine biota:
laboratory-derived CFs from this report (•); field-derived CFs from Jackson et
aj_. (1983) (o); stable-element-derived CFs from Polikarpov (1966) (o) or
Pentreath (1977) (A).
80
-------
reported that the CFs obtained from short-term exposure to cobalt in the water
were 300 to 400 times greater than those from food. When accumulation had
occurred over a 2-month period, CFs from the water pathway were 7.6 times that
from the food pathway.
The accumulation of ionic cobalt and cobalamin by the abalone Haliotis
discus was compared (Ueda et_ aj_., 1981). They reported that the distribution
of cobalt in the liver was different for the two forms of cobalt.
Elimination Rates
Metabolism of cobalt has been investigated in both clams and oysters
(Table 26). Generally, elimination was several months in duration in the long-
lived compartment. Pentreath (1973a) investigated the uptake of cobalt in
various tissues of Mytilus edulis. When the radionuclide was administered in
the water, half-lives ranged from 4.7 d in the foot to 17.7 d in the adductor
muscle. He concluded from his analysis of stable-element data that
accumulation of radionuclides from water was minor relative to that from the
food.
The accumulation and loss of Co by the octopus Octopus vulgaris was
followed by Nakahara et a1_. (1981). The distribution of the Co in octopuses
that had accumulated the radionuclide from the food differed from that in
octopuses that had accumulated it from the water. The biological half-life of
Co calculated from the long component of the excretion curve of whole body
radioactivity was approximately 200 d for the organisms reared in labeled
seawater and was 300 d for those administered labeled food.
ARTHROPODA - CRUSTACEA
Concentration Factors
CF values of cobalt for crustaceans are presented in Table 27. It is not
known whether the considerable variability shown is due to differences in
species or the absence of equilibrium conditions. Most of the cobalt was
present in the exoskeleton and would be lost from the animal upon molting.
Amiard and Amiard-Triquet (1977) followed the uptake of cobalt from food
and seawater in the crab Carcinus maenas. The CF resulting from cobalt in the
water was 5.8 times that from food.
-------
Table 26. Biological half-life (days) of cobalt in Mollusca - Pelecypoda.
Organism
Scrobicularia plana (clam)
Crassostrea gigas
(oyster)
C. gigasc
r • c
C . gigas
C. gigas
Mya arenaria (clam)
M. arenaria
M. arenaria
Crassostrea virginica6
(oyster)
Body part
Whole
Whole
Body
Muscle
Shell
Whole
Body
Muscle
Whole
Pool Aa
2-4(~)
220( — )
130(-)
300 ( — )
100(-)
120(100)
240(100)
180(100)
35(100)
Pool Ba
30-57( — )
40(-)
7(~)
12(-)
35(-)
—
—
—
__
Number in parentheses is the percent of total activity in the pool.
Amiard-Triquet and Amiard (1976a, b).
Cranmore and Harrison (1975).
Harrison (1973).
Hess et al. (1977).
82
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Table 27. Laboratory-derived concentration factors (CFs) for cobalt in
Arthropoda - Crustacea.
Organism
Crangon vulgaris
(shrimp)
C. vulgaris3
Carcinus maenasa
(crab)
Leander pacificus
(shrimp)
L. pacificus
L. pacificus0
L. pacificus0
L. pacificus0
L. pacificus0
Clibanarius virescens0
(hermit crab)
C. virescens0
d
Crangon crangon
Body part
Whole
Exoskeleton
Whole
Whole
Whole
Muscle
Exoskeleton
Muscle
Exoskeleton
Whole
Whole
Whole
Exposure, d
12
12
7
19
19
15-35
15-35
15-35
15-35
15-35
15-35
30
CFs
37
100
30
20
5
5
18
4
14
520
57
13
Comments
No carrier
Carrier added
No carrier
No carrier
CoCl2, 200 ppm
CoCl2, 200 ppm
CoCl2, 200 ppm
CoCl2, 200 ppm
Water
a Bonotto _et jj_. (1981).
b Hiyama (1962).
0 Shimizu et _al_. (1970).
d van Weers (1975).
83
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Elimlnation Rates
Little information is available on the biological half-life of cobalt in
Crustacea. Amiard-Triquet and Amiard (1976b) found that the rate of loss of
Co from the fast compartment was related to the frequency of feeding. No
data on half-lives were given. When the shrimp Crangon crangon was fed
Co-labeled mussel flesh and then the loss of activity followed, two
components of loss were identified (van Weers, 1975). The short-lived
component had a mean biological half-life of 1.2 d and accounted for about 80%
of the initial activity. The long-lived component had a half-life of about
10 d and represented about 20% of the activity.
CHORDATA - PISCES
Concentration Factors
Data on CFs of cobalt in marine fishes are limited (Table 28). Values are
considerably lower than those of Mollusca and Crustacea. Comparison of field-
derived stable-element and laboratory-derived radionuclide CF values shows that
the range of the stable-element values is more than an order of magnitude
higher than that obtained under laboratory conditions. The accumulation of
cobalt from food and water was compared in the yellowtail (Seriola
quinqueradiata) (Nakahara _ejt _aj_., 1979b; Suzuki _et al., 1979). After the fish
were exposed for a 7-d period, the percentages of Co in tissues were
different for the two pathways, but the significance of the pattern of the
differences was not apparent.
ro
The accumulation of Co by the thornback ray was followed for 84 d
(Pentreath, 1973b). Data on organ CFs show a high value of 2.2 in the gills
and a low value of 0.3 in the muscle. This investigator concluded that intake
from water played only a relatively minor role in the accumulation of cobalt
by the ray.
Elimination Rates
The biological half-life of cobalt has been determined for a number of
species (Table 29). The elimination of cobalt was followed in the Atlantic
croaker Micropogon undulatus after intraperitoneal injections (Baptist et al.,
84
-------
Table 28. Laboratory-derived concentration factors (CFs) for cobalt in
Chordata - Pisces.
Organism
Girella punctata3
G. punctata3
Chasmichthys gulosus
C. gulosus
C. gulosus
Brevootia tyrannusc
Body part
Whole
Whole
Whole
Whole
Whole
Whole
Exposure,
22
22
22
22
22
16
d CFs
>5
>2
4.5
5.2
2.5
7.1
Comments
No carrier
Carrier added
July, small size
Oct., small size
Medium size
Nonequilibrium
(post-larvae menhaden)
Sebastes nivosusc Whole
(rock fish)
Evynnis japonica0 Whole
(sea bream)
E. japonicac Muscle
Seriola quinqueradiatac Whole
(yellowtail)
S. quinqueradiata0 Muscle
Paralichthys o1ivaceusc Whole
(flounder)
P. olivaceusc Muscle
20
62
62
131
131
120
20
4.2 Nonequilibrium
4.8
0.5
1.2
0.3
5.5
1.5
Hiyama (1962).
Hiyama and Khan (1964).
Nakahara et al. (1979b).
85
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Table 29. Biological half-life (days) of cobalt in Chordata - Pisces.
Organism
Body Part Pool Ac
Pool Bc
Comments
Micropogon undulatus
(Atlantic croaker)
Blennius pholisc
(blenny)
Mugil chelo0
(grey mullet)
Evynnis japonica
(sea bream)
r . - d
E. japonica
Seriola quinqueradiata
(yellowtail)
^_._ quinqueradiata
Paralichthys o1ivaceusc
(flounder)
£_._ olivaceus
Pleuronectes platessa6
(plaice)
?_._ platessa6
Raja clavata6
(thornback ray)
R. clavata6
Whole
Whole
Whole
Whole
Muscle
Whole
Muscle
Whole
31(100)
203±18(88)
154±24(75)
Whole 28.9( —;
Muscle 38.5( — ;
23.9(-)
53.3( —)
49.5(--)
63.0(~)
Whole 65(100)
Muscle 120(100)
180(100)
Muscle 189(100)
Intraperitoneal
injection
20-30(12) Loss after uptake
from water
20-30(25) Loss after uptake
from water
Loss after uptake
from water
Loss after uptake
from water
Loss after uptake
from water
Loss after uptake
from water
Loss after uptake
from water
Loss after uptake
from water
Accumulation from
water
Accumulation from
water
Accumulation from
water
Accumulation from
water
Number in parentheses is the percent of total activity in the pool.
b
Baptist et a/L (1970).
C Fraizier and Vilquin (1971).
d Nakahara &t_ _aJL (1979b).
6 Jefferies and Hewett (1971).
86
-------
1970) and only one compartment was identified compared to two compartments for
the other radionuclides that were examined. These investigators state that
more compartments might have been found if loss of the cobalt had been
followed for a longer time. The accumulation by the common goby Acanthogobius
flavimanus of Co that had been incorporated into Nereis japonica was
followed (Kimura and Ichikawa, 1972). A triphasic pattern of loss was found
after a single meal of worms had been consumed. The absorption of
sediment-bound Co was studied after oral administration of encapsulated
sediment (Koyanagi et al_., 1978); loss was found to be biphasic.
APPLICATION OF CONCENTRATION FACTOR AND ELIMINATION RATE DATA
Concentration Factors
CFs for radionuclides in marine organisms are, in general, higher in
primary producers than in marine invertebrates, and fish usually have lower
CFs than invertebrates (see also reviews by Coughtrey and Thome, 1983a, b).
Examination of the distribution of laboratory-derived CF values for a specific
group of organisms shows that the spread of the values may range over several
orders of magnitude (Pentreath, 1977, 1981). For a given species, the CF is
dependent on whether the analysis was made on the whole organism, on the
eviscerated body, on soft tissues only, or on selected organs or tissues.
Comparison of laboratory- and field-derived CFs shows that there is better
agreement between the data sets for some groups than for others. It is
expected that better agreement would occur for organisms or body parts that
have short elimination times than for those that have long ones, and for those
organisms or body parts where surface adsorption reactions predominate rather
than for those where transfer across membranes and uptake by internal tissues
is required.
The distribution of radionuclide concentrations in environmental media
and the distribution of the resulting CFs calculated from them generally are
highly variable and exhibit a skewness. This is readily demonstrated by the
plots of CFs in this report. Such CF values are not well represented by a
normal distribution, but they are well approximated by a lognormal
distribution (i.e., the values of the logarithms of the CFs appear to be
normally distributed). Such lognormal distributions for radionuclide
87
-------
concentration data and CF values have been described previously by others, and
procedures for the statistical treatment of the data have been given (Gilbert,
1979, 1983).
Because CF values exhibit such a wide range of values, it is difficult to
select a single value to use in dose-assessment models. An approach used
frequently in the past has been to select a conservative value; however, this
practice is currently considered to be a poor procedure except in efforts to
protect the public in advance of an actual release of radioactivity. The
current approach used by modelers to predict the movement of radionuclides
through ecological systems is to stress the use of stochastic models, wherein
the actual distribution of data sets is considered and results are specified
in a probabilistic nature. This more realistic approach has several important
advantages. The most important is that model outputs represent a more
realistic assessment of the inherent variability of natural systems, and the
regulator is presented with a probability distribution. From this
distribution, a desired degree of conservatism can be selected or the dose
being calculated can be presented in terms of a probable value and an
appropriate statement of uncertainty.
To apply these concepts, however, it is necessary to specify a
distribution of values for each of the input parameters used in a model and to
propagate uncertainties throughout the model. Therefore, some of the CF data
in this report have been examined to specify the distributions of values. Of
the radionuclides and groups of organisms discussed in this review, I am
considering only the field-derived CFs for plutonium and cesium in fishes and
molluscs because they are the only ones with a reasonable body of data.
The two-parameter lognormal distribution is described mathematically by
f(x) = [l/(a V^f)] exp[-(ln x - y )2/(2a2)J
•/ J J
X > 0, - oo > y^ > co, a^ > 0 ,
2
where u and a , the two parameters of the distribution, are the true mean
J j
and variance, respectively, of the transformed variate y = In x (Gilbert,
1983). The distribution can be described also by the true geometric mean
[exp(uy)] and true geometric standard deviation [exp(a )]. Such distributions
have several useful properties including the following:
88
-------
• The product of m independent lognormal variates is also a lognormal
variate. This is a very useful property in multiplicative food-chain
models.
• The ratio of two lognormal variates (x/y) is also a lognormal variate.
If the several variates are not independent, then in the calculation of the
variance, the correlation between the variates must also be considered
(Gilbert, 1983). The second point above is important in consideration of the
utilization of CF values.
Analyses were performed on the values, cited by Noshkin (1985), of field-
derived CFs for plutonium and cesium in fishes and molluscs. The analyses
included plotting the values on lognormal probability paper to examine the
assumption of lognormality. If a straight line fitted the data reasonably, a
lognormal distribution was assumed; all of the CF values analyzed appeared to
be reasonably well represented by a lognormal distribution. A probability plot
of the CF values for plutonium in fish muscle is shown in Fig. 13. Analyses
were performed also to provide data on the median and on the mean, variance,
and central percentage interval (plus or minus one standard deviation) with the
assumptions that the data were (1) normally distributed and (2) lognormally
distributed. The arithmetic mean was always larger than the median or the
geometric mean (Table 30).
Examination of the data on the central percentage confidence intervals
shows that the values obtained, assuming a normal distribution, are of little
value for analysis of uncertainty because negative numbers are obtained (the
standard deviation is larger than the mean). It is also clear that the true
geometric standard deviations are large. These large true geometric standard
deviations could be attributed to many causes. First, the data are not
homogeneous; they were obtained by a variety of investigators on a variety of
specimens. Second, there may be systematic errors between investigators whose
data are represented in the data base. And finally, the biological and
chemical systems measured may in fact have very large variability.
In general, the following steps are suggested in the selection of
parameters to be used in models.
• Perform a probability plot of the data to determine whether the data
are best represented by a normal or lognormal distribution.
• Determine the mean, standard deviation, and confidence intervals for
the appropriate distribution.
89
-------
1000
0.1 -
0.14
2
I
c
o
'£
e
0.62 0.23 0.67 16 31 50 69 84 93 97.7 99.4
Cumulative probability (%)
Figure 13. Concentration factors for plutonium in muscles of fish. The
arithmetic mean is 77 (sigma = 220), and the geometric mean is 8.9
(sigma = 8.7).
90
-------
Table 30. Values obtained from statistical analyses of CFs, assuming a normal distribution and a lognormal
distribution.
Organism Number
Fish
Muscle 48
Bone 22
Liver 17
Pelecypods
Soft tissues 16
Fish
Muscle 35
Pelecypods
Soft tissues 10
Normal distribution
Median Mean S.D.a Central
65% interval
Plutonium
9.5 68 220 -152 to 288
77 160 180 -20 to 340
64 1400 2400 -1000 to 3800
420 650 870 -220 to 1600
Cesium
47 54 31 23 to 85
41 380 680 -300 to 1100
Lognormal distribution
GMb S.D. Central
68% interval
9.5 7.8 1 .2 to 74
64 5.4 12 to 350
130 14 9.3 to 1800
340 3.0 110 to 1000
45 2.0 22 to 90
74 7.6 10 to 560
Central
95% interval
0.2 to 530
2.4 to 1,700
0.7 to 23,000
40 to 2000
12 to 180
1.4 to 3900
S.D., standard deviation.
GM, geometric mean.
-------
® Critically review the data for systematic or other biases to derive
the most appropriate values for the particular application.
Single values of CFs for plutonium and cesium in fish muscle and soft
tissues of molluscs to be used in models have been selected previously by
others (Table 31). Comparison of those values to the means given in this
report, which were calculated from the data base from Noshkin (1985), shows
that most are within reasonable agreement, considering the variance of the
data. However, the range of values given differ considerably from the
confidence intervals calculated.
Elimination Rates
It is important in determining the elimination of radionuclides that (1)
the initial pulse labeling of the organisms be performed over a length of time
sufficient to label long-lived compartments and (2) the loss be followed long
enough to identify long-lived compartments. If data on long-lived compartments
are not available, then wrong conclusions can be drawn about the retention of
radionucl ides and their potential for transfer to man. For example, recent
seasonal data from Mussel Watch program (Goldberg _et _a_L , 1978) showed that 50%
of the plutonium and americium were eliminated within 3 to 10 weeks. The
predictions that might be made as to when contaminated mussels might be safe
to ingest after a period of depuration would be considerably longer if the
Guary and Fowler (1981) data were used than if the Goldberg _et _a_L (1978) data
were used.
ACKNOWLEDGMENTS
The author thanks Dr. Lynn Anspaugh for his assistance in the writing of
the section on "Application of Concentration Factor and Elimination Rate Data"
and for his critical review of the report.
92
-------
Table 31. CF values for use in models to predict the dose to man or aquatic
organisms from the release of radionuclides into marine environments.
Organism
Fish
Muscle
Mol luscs
Soft tissues
Thompson et
(1972)
3.5
100b
al. IAEA
(1985)
Plutonium
40 (0.5 to 100)a
3000 (500 to 5000 )C
This report
Mean GM
68 9.5
650d 340d
Fish
Muscle
Molluscs
Soft tissues
30
Cesium
100 (10 to 300)
30 (10 to 50)C
54
3801
45
Numbers in parenthesis are ranges.
Invertebrates.
Molluscs except cephalopods.
Pelecypods.
93
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TECHNICAL REPORT DATA
(Please read Instructions on the reverse before completing}
• REPORT NO.
_EPA_520/l-85-015
'. TITLE ANDSUBTITLE
Laboratory-Determined Concentration Factors and
Turnover Rates of Some Anthropogenic Radionuclides in
Marine Vertebrates and Invertebrates
3 RECIPIENT'S ACCESSION NO.
5. REPORT DATE
July 1935
6. PERFORMING ORGANIZATION CODE
I
\UTHOR(S)
B. PERFORMING ORGANIZATION REPORT NO
F. L. Harrison
PERFORM
ORGANIZATION NAME AND ADDRESS
Environmental Sciences Division
Lawrence Livermore National Laboratory
Livermore, California 94550
10. PROGRAM ELEMENT NO.
11. CONTRACT/GRANT NO.
IAG No. AD89-F00070
12. SPONSORING AGENCY NAME AND ADDRESS
Office of Radiation Programs
Environmental Protection Agency
401 M St., S.W.
Washington, D.C. 20460
13. TYPE OF RE PORT AND PERIOD COVERED
Final
14. SPONSORING AGENCY CODE
ANR-461
5 SUPPLEMENTARY NOTES
16. ABSTRACT
Literature is reviewed and summarized with regard to concentration factor
values and biological elimination rates determined in laboratory experiments
for several anthropogenic radionuclides. Comparison is made with concentration
factors measured in situ in the marine environment.
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
b. IDENTIFIERS/OPEN ENDED TERMS C. COSATI Held/Group
8. DISTRIBUTION STATEMENT
Unclassified
19. SECURITY CLASS (
Unclassified
NO. OF PAGES
2O SECURITY CLASS 11'liu
Unclassified
Form 2220-1 (Rev. J-/7) PREVIOUS EDITION 15 O BSC
7U.S. GOVERNMENT PRINTING OFFICE: 1986-621-735/60520
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