-------
TABLE 6. FRESHWATER PLANTSCRITICAL CONCENTRATION FACTORS
(VALUE LISTED X 103 = CF)
Element
N
P
Sc
Mn
Y
Zr
In
La(d)
Hf
Tl
Sb
Zn
Ru
Ce
Pu
Sr
Cs
U
I
Chapman
et al. (1168)
25.0
100.0
10.0
10.0
10.0
10.0
100.0
10.0
10.0
100.0
4.0
2.0
10.0
1.0
0.5
0.2
1.0
0.1
Thompson et al. (1972)
(al
Derived v '
12.5
10.0
10.0
10.0
5.0
1.0
__
5.0
1.0
__
1.5
1.0
0.2
5.0
0.35
0.5
0.08
1.0
0.04
Measured
500.0
10.0
__
20.0
2.0
4.0
0.5
0.5
0.0005
For Contaminated Environment (c)
Minimum
100.0
__
1.8
2.0
0.24-0.33
0.07-0.47
0.0004
Maximum
850.0
__
12.0
10.0
0.28-0.69
0.87-1.2
0.0007
Average
_.
270.0,
130.0
0.6
0.0006
Dash () indicates no data in reference cited.
(a)r
(b)
(c)
(d)
Derived on the basis of stable element concentrations.
Measured in radioisotope experiments.
Measurements made in environmental studies.
For lanthanide series.
1. Because of the higher concentration of stable mineral elements
in seawater, the radionuclide CF's for most freshwater organisms
are much higher than those for similar seawater biota.
2. Radionuclide accumulation and concentration in various tissues of
an organism may differ considerably. Data illustrating this
variability were published by Harvey (1967).
3. Error originates from the practice of analyzing the stab.le
elemental content of biota and then calculating the CF from general
literature data on the elemental concentrations in freshwater or
seawater.
4. Physiological factors (same as those discussed by Harrison, 1967):
species differences, age, size, reactions to changes in temperature,
17
-------
and chemical characteristics of the environment vary. The concen-
tration of an element in tissue may be controlled hoffieostatically. Such
control of potassium and calcium concentrations in organisms may
strongly affect CF's for their chemical congeners, cesium and
strontium, respectively, 'dftiile such effects are well-known for
higher animals, they may occur in many simple organisms. For
example, the concentration of manganese in Hudson River fish
remains constant in spite of large variations in the water concen-
tration of manganese.
5. A CF with respect to water may be influenced by the pathway through
which the nuclide reaches the organism. Although an organism may
not directly concentrate an element from water, some element in its
food chain may have performed the concentrating function. Further-
more, the food source for an organism may vary with seasons and be
affected by many environmental factors.
6. Short-term variations in the concentration of stable elements or
radionuclides in environmental media may result in nonequilibrium
conditions between organisms and the environment at the time of
measurement. The concentrations of elements with long effective
half-times in the tissue may reflect an earlier high, concentration
in the environment rather than that existing at the time of capture.
Additionally, some studies indicate an apparent selectivity by a few
organisms for certain radionuclides over their stable counterparts. Pre-
sumably, this is related to differences in physio-chemical availability
or to different pathways of uptake. For example, data from the LLL report
(Thompson et al. , 1972) show that the following elements have experimentally
measured CF values (based on radionuclide concentrations) that are greater
than the derived values (based on stable element concentrations) by 1 or
more orders of magnitude:
18
-------
Biota
Elements with CF measured value
>10 x derived value
Marine:
Plants
Invertebrates
Fish
Freshwater:
Plants
Invertebrates
Fish
Lead, Plutonium
Strontium
Strontium
Phosphorusj Chromium, Zinc, Ruthenium,
Cesium
Sodium, Chronium
Sodium, Chronium, Strontium, Cesium,
Polonium
TABLE 7. FRESHWATER INVERTEBRATESCRITICAL CONCENTRATION
FACTORS (VALUE LISTED X 103 = CF)
Element
N
P
Mn
Zn
Ge
In
Sb
Te
Hg
Tl
Po
Pu
Sr
Cs
U
I
Chapman
et al. (1968)
42.5
100.0
40.0
40.0
16.7
100.0
16.0
100.0
100.0
0.4
0.29
0.7
1.0
0.3
0.025
Thompson &k al. (1972)
Derived (a)
150.0
100.0
40.0
10.0
100.0
100.0
10.0
20.0
0.1
0.1
0.1
0.1
6.005
Measured
__
20.0
90.0
10.0
0.06
For Contaminated Environment *<-)
Crustacean
__
10.0
4.0
0.06
Mollusca
__
20.0
93.0
20.0
Average
__
20.0
90.0
10.0
0.06
Dash () indicates no data in reference cited.
(a)
(b).
(c)'
Derived on the basis of stable element concentrations.
Measured in radioisotope experiments.
Measurements made in environmental studies.
19
-------
TABLE 8. FRESHWATER FISHCRITICAL CONCENTRATION FACTORS
(VALUE LISTED X 103 = CF)
Element
N
P
Nb
In
Tl
Np
Ta
Pu
Sr
Cs
U
I
Chapman
et al. (1968)
150.0
100.0
30.0
100.0
100.0
100.0
0.1
0.01
0.04
0.001
0.01
0.001
Thompson et al. (1972)
Derived (a)
150.0
150.0
30.0
10.0
30.0
0.003
0.005
0.4
0.01
0.015
Measured
__
100.0
0.03
2.0
0.002-
For Contaminated Environment ^c)
Minimum
0.5-30.0
0.003
0.39-1.6
Maximum
__
55.0-100.0
0.17
1.1-4.7
Average
50.0
0.058
2.4-3.9
0.002
Dash () indicates no data in reference cited.
Derived on the basis of stable element concentrations.
(b)
(c)
Measured in radioisotope experiments.
Measurements made in environmental studies.
In general, the elements that are concentrated significantly in aquatic
organisms (Tables 1 to 8) were grouped by Lowman et dl.+ (1971) into at least
one of five categories:
1. Structural elements: Carbon, Nitrogen, Phosphorus, Silicon,
Calcium, Strontium.
2. Catalyst elements: Iron, Copper, Zinc, Manganese, Cobalt, Nickel,
Chromium, Cadmium, Silver.
3. Elements easily hydrolyzed at seawater pH: Aluminum, Gallium,
Scandium, Yttrium, Cerium, Plutonium, Titanium, Zirconium.
4. Heavy halogens: Bromine, Iodine.
5. Heavy divalent ions: Barium, Radium, Rubidium.
Supportive data on concentration factors for several elements in various
biota have not been identified. For seawater these elements are indium,
tellurium, and bismuth. In freshwater the elements with least known data
are indium, thallium, bismuth, tellurium, and germanium for inverte-
brates and neptunium for fish.
20
-------
INDICATOR ORGANISMS
Biological indicators are defined (Rice, 1965) as those organisms
which concentrate relatively large amounts of specific radionuclides,
thereby making it possible to detect the presence of those isotopes
in the environment through an analysis of the organisms. Additional
qualifying characteristics of "indicators" are listed by Feldt (1971).
The organism must:
1. be readily attainable at all times,
2. have a sufficient CF for several radionuclides
of interest, and
3. yield measurement results in a form which makes
it possible to assess the radiation dose to
man.
The concentration of elements in aquatic ecosystems is highly
variable. CF's are related to the chemical content of the water,
and it is impossible to draw general conclusions from elemental
composition of organisms without simultaneous reference to data
from their environment. In spite of this, however, Polikarpov
(1966) states that it is generally recognized that CF's (taken in
the equilibrium state) of each separate radionuclide for closely
related species of marine plants and animals (i.e., same genus
or family) do not differ significantly in different seas and oceans.
There appears to be less acceptance of a second generalization attri-
buted to Polikarpov: that CF's for radionuclides which are present
in water in microquantities are similar for related marine and fresh-
water organisms. It has been more frequently observed that the fresh-
water CF for a particular isotope by a particular type of organism
is higher than that in a marine environment (due to differential
isotopic dilution in these two basic systems).
A logical, universal biological indicator of radioactivity in any
aquatic system would appear to be mixed phytoplankton. Those elements
that are concentrated by at least a factor of 1,000 by marine phyto-
plankton have been tabulated by the NAS/NRC (1971). Unfortunately,
however, photoplankton do not accumulate nuclides in the same propor-
21
-------
tions as, for example, fish. For mixed phytoplankton to meet the
third qualifying characteristic previously noted, they would have to
be a predictable component of a food web eventually leading to man.
Even though phytoplankton may remove large amounts of radionuclides
from water, the amount of radioactivity that may be passed up the
food web will vary with cell mass, cell numbers, and specific con-
centrations, as well as with efficiency of utilization by ensuing
trophic levels. Another complication with using mixed phytoplankton
has been described by Feldt (1971): "It is especially difficult. . ."
(in rivers, and presumably estuaries and coastal areas too) "...
to separate the plankton from detritus." He concludes that while the
concentration of certain nuclides in plankton would help to prove
the presence of these nuclides, it would not give useful information
on the risks these radionuclides present to man because they are not
found in the same concentrations in edible aquatic products.
With these arguments in mind, it seems natural to fall back to the
Polikarpov C1966) terminology that there are "biological indicators"
(as previously defined) and there are "biological accumulators" (of
which mixed phytoplankton would be an example). By the guidelines
set forth for this report, the "accumulators" would be useful only
in the dat-ineatirOn of the geographic area involved in a potential
hazard to man. "Biological indicators" would be required for the
other categories: alert (indicate that radioisotopes are concentrating
within food chains that may lead to a hazard for man); assess (give
indication of the potential magnitude of intake by man); or control
(indicate whether or not control measures are effective).
In reviewing literature on biological indicators and accumulators,
organisms were separated into the broad categories of producers and
consumers.
Producers
In general, the literature reviewed does not present sufficient
information for determining which, specific producer organism
is an accumulator or an indicator for a particular radioisotope. Most
compilations of CF's have categorized producers very broadly and lump
22
-------
together phytoplankton, littoral and benthic seaweeds and algae; submerged,
floating, and emergent angiosperms; etc. The only generally accepted
generalization concerning producers, according to the IAEA (1971), is that
phytoplankton tend to concentrate activation products to a greater extent
than fission products. This reference also notes that while the degree of
concentration of activation products is highest in the primary producers,
intermediate in the herbivores and lowest in the carnivores, the primary
producer's concentration in comparison to fission products is more subject
to variation and rapid fluctuation in response to changes in the ambient
contamination level. The concentration responses in the higher trophic
species are more sluggish and less predictable.
Primary Consumers
Few valid generalizations can be made from the literature about the
indicator value of tropic levels. For example, filter feeding animals have
been shown to concentrate different radionuclides even while they are living
in the same microenvironment. (For example, see Table 9.) Also, the distri-
bution of a radionuclide within a particular organism may vary greatly; e.g.,
even though scallops were found to be excellent accumulators of manganese-54,
most of the activity was present in the kidney, which is not eaten by man,
and relatively little was present in the muscle. Bryan et ai. (1966) reported
that CF's generally decrease from lower to higher trophic levels because of
radioactive decay, mode of uptake, and turnover rates. A summary of the
ranges reported for element CF's in marine organisms at various trophic levels
is given in Table 10.
Higher-Order Consumers
In general, the same limitations that have already been noted apply to
organisms in the higher trophic levels. Feldt (1971) argues that fish are
excellent indicators in freshwater systems because of their availability,
their measurable (although not usually maximal) CF's for a wide variety of
isotopes, and their applicability to assessment of hazard to man. For
the same reasons, he also supports the use of mussels as the indicator
organism in river estuaries.
23
-------
TABLE 9. RELATIVE ABUNDANCE OF RADIONUCLIDES IN FOUR SPECIES
OF MOLLUSCA FROM THE SAME ENVIRONMENT (a)
Scallops
Oysters
Clams
Mussels
144Ce
4
2
1
1
106^
Ru
3
3
2
2
137r
Cs
2
(b)
(b)
(c)
54Mn
1
(c)
(c)
(c)
65Zn
5
1
(c)
(b)
(al
v 'Data from Bryan et al. (1966).
Present but not relatively abundant.
(c)
Indication of presence
Studies on the uptake of radionuclides by various fish in the Columbia
River (Foster and McCannon, 1962) have shown that there is a wide variation
in uptake between individual specimens of the same species, thus requiring
large samples for statistical validity. Uptake also changed rapidly with
the season. The most pronounced variations were found with short-lived
radionuclides that were necessarily acquired via food chains.
In summary, it appears that few generalizations can be made concerning
indicator organisms. Most studies have identified accumulators with varying
degrees of effectiveness, but still there appears to be no consistently
reliable pattern. Relatively few studies have attempted to describe, much
less quantify, entire aquatic ecosystems. Yet, at present this appears to
be the only way to make intelligible recommendations concerning the identity
of accumulator and/or indicator organisms.
ENVIRONMENTAL STUDIES
Those studies which have actually identified indicator organisms have
been, at least initially, comprehensive ecosystem effects studies. Since
the overwhelming complexity of environmental effects seriously hinders
effective control, it is accepted practice to determine just which factors
are critical (i.e., those which give rise to the greatest risk) and to
24
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TABLE 10, RANGES OF ELEMENT CONCENTRATION FACTORS IN MARINE ORGANISMS
(a)
N>
Ui
Ag
Cd
Ce
Co
Cr
Cs
Fe
I
Mo
Mn
>:i
Pb
Ru
Sr
11
Zn
2r
A.I
t*ns1 le
100 1,000
11 20
100 3,300
15 740
100 500
16 50
1,000 5,000
160 7,000
10 , 200
20 20,000
50 1,000
8,000 20,000
100 1,200
0.1 90
200 30,000
80 3 , 000
200 3,000
Cfte
P,.nl,,
< 100 220
< 350 6,000
2,000 4,500
75 1,000
< 70 600
16 22
750 7,000
< 3 17
300 7,000
25 300,
1,000 3x10°
< 200
0.9 54
600 10,000
200 1,300
< 1,000 20.000
Graze
Pl.nfcr^)
l 1 f i sh
330. 20,000
W 2xlOp
40 300
24 260
6x10 3x10
3 15
7x10* 3xl05
40 70
30 90
3,000 60,010
17 90
200 60,000
10 2,400
1.2 10
110 20,000
50
<8QO 40,000
vl. fcf W
<45 900.
<300 10
<70 1,300
<55 3,900
3,000 30,000
<2 14
270 1,600
17 90
200 60,000
10 2,iOO
1.2 10
110 20,000
50
<800 iO.OOO
predators
Fi ch
> 10
5 12
28 560
3 30
6 10
400 3,000
10
200
95 105
5 10,000
10 --
4 i
280 20,000
5
£q!
-------
exclude all other factors which make no significant contribution to the
risk. For each instance of environmental contamination with radioactive
materials, it is initially necessary to identify the critical radionuclides
with reference to man. The physical and metabolic characteristics of these
nuclides determine which ecological pathways or routes to man are critical.
Since it is generally recognized that some members of the general population
may be more affected than others, it is often necessary to further identify
a critical population (Comar and Lengemann, 1966; IAEA, 1971; Straub, 1960).
Typical of this approach are studies (Foster and Soldat, 1966) of radio-
nuclides discharged to the environment from the Hanford operations. The
critical radionuclides and routes of exposure from effluents released into the
o o /: c
Columbia River involve P and Zn in local fish and the produce from
O / ^ £L O O C\ 1O^
irrigated farms; Na, As, Np and I in drinking water; and the
24
external exposure of swimmers to Na in water. The critical population
was determined to be persons who ate unusually large quantities of fish
caught in the river immediately downstream from the reactors. For most
of the population, however, drinking water provided the only significant
source of waterborne radionuclides.
Parker (1964) maintains that only large-scale producers/users of radio-
nuclides need to be considered in determining permissible discharge limits to
freshwater environments. The use of river water for the dilution of low-
level radioactive wastes is widely practiced. In addition to the studies
on the Columbia River, other environmental studies in freshwater environments
have generally indicated that local fish were the critical indicator organisms.
A study of the Clinch River by the Oak Ridge National Laboratory (Cowser
et al*3 1963) showed that the major pathways of exposure were (1) consump-
tion of contaminated water and fish; (2) consumption of agricultural produce
irrigated with river water; (3) exposure to contaminated water and bottom
sediments directly; and (4) exposure to the buildup of radionuclides in
sludge and deposits in water systems which utilize the river water. The
90 137
critical radionuclides identified were Sr for bone, Cs for total
body, Ru for the gastrointestinal tract, and I for the thyroid.
26
-------
Environmental studies of marine ecosystems generally have been under-
taken in response to two types of situations: (1) to determine the effects
of high-level discharges from nuclear detonations, and (2) to determine the
effects of continuous low-level discharges from nuclear facilities. The
latter situation is of primary interest, and studies of discharges from
power reactors in England provide information that illustrates the
variability of critical facto'rs for different environments.
The Irish Sea coastal area adjacent to the Windscale reprocessing plant
is one of the most important areas known with respect to the degree of radio-
active contamination in the marine environment. The critical radionuclides
released were determined to be Cs, Ru, Zn, Nb, Ce and Sr.
The most critical pathway is for Ru in the seaweed, porphyra3 which is
used to make laverbread. A critical group of heavy consumers of this
foodstuff was identified. For three nuclear power stations sited on
England's open coastline, the exposures from Zn, Cs, and Sb were
the controlling factors in limiting waste discharges. At Hinkley,
accumulation of these radionuclides in silt and fish flesh established
the permissible discharge levels, whereas at Dungeness and Sizewell
accumulation in fish flesh alone was definitive (Straub, 1964)
The potential damage to man and his environment is the limiting
criterion on waste releases in most Western countries, whereas Russian
Interpretation requires that releases to the environment meet drinking
water and breathing tolerances. The doses that cause injury to plants
and animal life are, according to most Western authorities, much higher
than would be permitted for human exposure. As an example, no effects
were noted following the irradiation of chinook salmon at dose rates of
up to 5.0 rem/day beginning immediately after fertilization of the egg.
The possibility of synergism occurring with the combination of ionizing
radiation and heated effluent temperatures also has been investigated;
while no such synergism has been demonstrated, it has been shown that
some organisms absorb radionuclides up to 50% faster due to increased
metabolic rates in warmer waters (Eisenbud, 1973).
27
-------
RADIATION PATHWAY AND DOSE MODELS
This section describes ways in which radionuclide releases to aquatic
environments can be translated into estimates of the resulting potential
radiation dose to people. Present radiation guides for permissible radio-
nuclide concentrations in water are based upon direct consumption of
the contaminated water by people. Although such direct intake does not
take into account potential radionuclide transfer and subsequent consump-
tion through aquatic food chains, this intake through the diet is recog-
nized, and the basic radiation standards are based on permissible radia-
tion dose rate and accumulated dose from all sourcesexclusive of natural
background and medical radiation (ICRP, 1959, 1962, 1966a and b, and 1968;
USAEC, 1970; NAS/NRC, 1972; NCRP, 1971). The bas.is for and detailed
descriptions of radiation standards are described and discussed extensively
in the literature and are outside the scope of this report. However,
a brief discussion of the models used in deriving air and water
standards is helpful.
The International Commission on Radiological Protection (ICRP, 1959,
1962, 1966a and b, and 1968) has established recommended values for maximum
permissible total body burdens (q), and for maximum permissible concen-
trations in air and water (MPC and MPC , respectively). Values are
given for about 240 radionuclides. These values are based on two
metabolic models: (1) an exponential or compartmental model, and
(2) a power function model. In the exponential model each body organ
is assigned a biological half-life, uptake fraction, etc. , and the
radiation dose to different organs can be calculated following a
given radionuclide intake. Since considerable data indicate that
for some radionuclides the fraction of the body burden excreted
daily varies inversely with time, an alternative power function model
is used to estimate the radiation dose for certain long-lived radio-
nuclides (e.g., strontium, radium, plutonium and uranium). The per-
missible body burdens of these bone-seeking radionuclides are based
on the comparison of the energy deposited in bone by the particular
9 0£
radionuclide with that deposited by 0.1 pCi of Ra and its daughters
The derivations of these models and a listing of model parameters for
28
-------
each radionuclide (with literature references) are given in the ICRP
reports.
The ICRP recommendations have been basically incorporated into U.S.
radiation standards. Such regulations start with a permissible radiation
dose, from which permissible concentrations in air and water are calcu-
lated; these are based on the standard physiological factors for man,
and would be expected to yield the permissible dose following the direct
intake of such air and water. It must be emphasized that the basic
criterion for the standards is radiation dose, and that the air and water
concentration guides are derived values. The derived guides must take
into account radionuclide exposure and intake from all sources. One of
the important routes of radionuclide intake by people is through aquatic
foods from environments which have received discharges of radioactive
materials. As described in previous sections, many environments have
unique characteristics, and generalizations about critical pathways for
radionuclides are tenuous. As a result, there exists in the literature
a multitude of models for such pathways in specific cases and for
specific conditions. The general approaches used in pathway and dose
modeling are herein described, together with a brief description of
those modeling efforts which appear to be comprehensive and applicable
to initial planning for radionuclide pathways assessment.
There are basically three methods of translating recommendations
for the maximum radiation dose into guides for acceptable discharge
rates for the various radionuclides. The first, which was described
briefly above, involved maximum permissible concentrations in air and
water for individual radionuclides or mixtures. If dilution, disper-
sion, and decay rates are known, then a discharge rate which meets
these standards can be calculated. This approach, as mentioned above,
considers only direct intake of contaminated air or water and neglects
environmental pathways which may be more limiting.
A second approach, called the critical pathway method, is frequently
used in assessing the potential dose to segments of the population
through environmental pathways. Through investigation of environmental
29
-------
transfer mechanisms for radionuclides anticipated to be present, critical
pathways leading to the exposure of people to radiation are identified.
The groups of people most likely to be exposed through critical pathways
are identified; and the group most likely to receive the highest dose,
in relation to a recommended permissible dose, is identified as the
critical group. The isotope which provides the largest dose through the
critical pathway may be called the critical radionuclide. The permissible
environmental levels of the critical radionuclides are then calculated and
frequently called Derived Working Limits (DWL). Although critical pathways,
radionuclides, and population groups can be identified and may be used to
calculate a DWL for each radionuclide, the basic limiting factor is total
radiation dose from all radionuclides in all pathwaysincluding direct
intake from air and water. This approach, then, is a logical extension
of the air and water MFC approach and intftgrates exposures from indirect
environmental pathways.
The third approach, based on specific activity, is somewhat
different. The use of specific activity, or radioactivity content
per unit mass of an element in a medium, was first proposed by the
NAS/NRC (1962) for establishing permissible levels of environmental
radioactivity in regard to radioactive waste disposal into the
Pacific coastal waters of the United States. In this approach it
is presumed that the radionuclide specific activity in any organism,
including man, would not exceed that in its basic environmental
substrates. Although a radionuclide may be concentrated many orders
of magnitude through physical or biological processes in the environ-
ment, radioactive nuclides of that element are always diluted by
stable isotopes in the environment and the specific activity remains
the same throughout various environmental media. Since the elemental
composition of man and his various tissues is well documented in the
literature (e.g., as summarized by the ICRP, 1959), the maximum dose
to man which could result from a given specific activity in the environ-
ment can be calculated. For the case in which only a portion of the
environment is contaminated, the calculated dose is modified by man's
degree of involvement with that portion of the environment.
30
-------
These three kinds of models are interrelated and require (NAS/NRC,
1971) a great deal of supplemental information concerning:
1. Kinds and quantities of radionuclides present.
2. Physical and chemical forms of the radionuclides.
3. Initial mechanism of dispersal.
4. Physical processes of dilution.
5. Availability to biota.*
6. Concentration factors and uptake rates.*
7. Consumption of marine products.
8. External exposure and exposure to other sources.
*Not used in specific activity approach.
In both the critical pathway and specific activity approaches,
it is necessary to know, or to estimate (1) the kinds and quantities
of radionuclides present; (2) the physical and chemical form of the
nuclides; (3) the method of entry into the environment; (4) the extent
of environmental transport and deposition through physical and chemical
processes; and (5) the importance of biological processes in transport
and concentration phenomena (Pritchard, 1961 and Russell 1964).
CRITICAL PATHWAY APPROACHES
Parker (1959) has summarized major and moderate contributor path-
ways to total radiation dose from radioactive wastes discharged to
surface waterways. The major pathways Parker evaluates are drinking
water, immersion, biological chains, irrigation, waste treatment
plants, and external exposure from proximity to radioisotopes.
Varying degrees of sophistication have been used in determining
the allowable environmental contamination by the critical pathways
approach. A simple method for seafood is described by Pritchard (1959)
who used the following generalizations:
where:
MPC = 20 MPC (1)
s x w
MPC ,. = maximum permissible concentration in
seafood
31
-------
MFC = maximum permissible concentration in
water; as described by the ICKP (1959)
20 = factor derived on the basis of a diet in
which 50% of the protein requirement is met
by aquatic foods, and radionuclides in such
foods constitute the only source of ingestion
MFC , = 4 MFC (2)
sf w v '
where: 4 = 20% of the 20, above, on the assumption
that 20% of the entire maximum permissible
radionuclide intake is assigned to seafoods
MFC = sf (3)
sw
where:
MFC = maximum permissible concentration in
seawater derived from assumptions for
either equation (2) or (3)
CF = concentration factor from water to
organism of interest
This approach is simple and easily understood. However, the
arbitrary assignment of the portion of the total radionuclide
intake to be permitted from seafood is controversial. In
addition, reliable information on CF's and dietary habits for
most areas are not generally available.
As an example of a rather sophisticated critical pathway model,
an outline of some general steps is given in Figure 1. Starting
with an allowable dose rate to man, a maximum allowable discharge
rate for radionuclides is calculated. The calculation may proceed
along the following lines for the particular case of ingestion of
a radionuclide in a contaminated seafood (NAS/NRC, 1959; Parker,
1959). Starting with the recommended maximum permissible concen-
tration for water (MFC ) a derived working limit for seafood,
w
(DWL) , can be calculated (Wolfe and Rice, 1968);
S IT
(DHL)3f - (""^2200 F ^
32
-------
where:
I = Rate of ingestion for seafood, g/day/
person
2200 = Rate of water intake, g/day/person
F = Fraction: an administrative number to
apportion to seafood some fraction of
the maximum permissible intake from
water.
, can be obtained directly
A derived working level for seawater, (DWL)
sw
from (DWL) by dividing by the ratio of the elemental concentration
S JL
in the seafood to that in the seawater, i.e., by the concentration
factor, CF (Wolfe and Rice, 1968):
(DWL)
(DWL)
'sf
sw
CF
(5)
MAN -
Total allowable
dose rate from
all sources
MAN - Portion of
total allow-
able dose allo-
cated to aquatic
pathways
Routes
Man .From
Aquatic Environment :
Aquatic foods, contact
on beach sands, water
ingestion, etc.
Physical and chemical form
of radionuclides and manner
of discharge
Maximum Allowable
Discharge Rate of
radionuclides to an
aquatic environment
Maximum Allowable
Concentration in
Portions of Aquatic
Environment which
constitute routes to
man: water, aquatic
foods, bottom sedi-
ments, etc.
Concentration
Factors from water
to other routes to
man
Maximum Allowable
Concentration in
water
Initial Dilution
Dispersion and Ex-
change with other
adjacent environments
Transfer Rates for
radionuclides from
solution or suspen-
sion to bottom sedi-
ments * and back
FIGURE 1. General steps in critical pathways evaluation for aquatic
environments Solid arrows indicate direction of radio-
nuclides, broken arrows that of calculations
33
-------
Application of mixing rates, dilution factors, etc., to (DWL) allows
an allowable rate of discharge to be calculated (Aten, 1961; Freke,
1967).
The rate of seafood ingestion, I in equation (4), has been
estimated in various ways. These fall into two categories of data
on food consumption patterns (Middleton, 1964). The first is a food
balance sheet or estimate of the per capita supplies of various
human foods available in a country, and the second is a survey of
dietary habits for selected population groups. For example, in a
typical U.S. diet it has been estimated (Harley, 1969) that marine
food products contribute 0.01% of the radioisotope intake, while
the contribution is 0.5% for a typical Japanese diet (Pritchard,
1961).
Marey and Saurov (1964) have developed relative indices which
characterize the movement of an isotope from a water media into a
food product. These indices, called accumulation multiples (AM), are
very similar to the CF's discussed previously. An AM is calculated by
dividing the activity per kilogram of the food product by the activity
per liter of the water media. These factors, along with dietary infor-
mation, can be used to establish the amount of a given isotope contri-
buted to people by individual foods in their diet. For this purpose
contribution coefficients (CC) were expressed:
cc = v v
where:
AM = accumulation multiple for particular
food
P = g/day intake of the food item
V = g/day intake of water
By summing the CC values for all food products and radioisotopes, a
general CC is obtained which characterizes the ingestion by people of
radioisotopes via aquatic foods in relation to the potential direct
intake via the water media. This approach differs from the usual,
34
-------
which utilizes CF's for edible aquatic organisms, in that radio-
nuclides in actual food products are measured. The accumulation
multiple is a form of CF, but only for processed food items. The
contribution coefficient is a means to reduce accumulation multiple
data for various foods and radionuclides to a form for intercomparison.
The amount of radioactivity in processed foods is of primary
importance in determining the radiation dose to people (Harrison,
1972). Radionuclide losses may be significant during processing and
marketing, e.g., from radioactive decay and the tissue selected for
food. In addition, food transportation to areas remote from the
harvest area leads to difficulties in accurate assessment of potential
problems. World interest in the expanded use of fish protein concen-
trate (FPC) is growing. About three kilograms of whole fish yields
about 500 grams of FPC, and the radionuclide (as well as other pollu-
tants) content of the concentrate may be hazardous if it is used as a
major dietary item. In one assessment (Beasley, 1971) based on a
210 210
reasonable 10 gram per day intake of FPC, the Pb- Po accumulation
was found to be hazardous, the cobalt intake was increased by a factor
of 2 to 3, and the silver intake was increased by about a factor of
1.3.
The consideration of radionuclide ingestion alone is useful in
assessing pathways to man and relative hazards; however, the dose to
man depends on many other factors such as summarized from ICRP reports
by Harrison (1972). These factors include:
1. Quantity of radionuclides ingested.
2. Fraction of ingested quantity which is absorbed and
deposited in tissues,
3. Energy absorbed by tissues.
4. Effective half-life of the radionuclide in tissue.
Since aquatic environments may become contaminated from a variety
of sources (e.g., fallout, reactors, reprocessing plants, and nuclear
ships), efforts have been made by Templeton (1964) to measure the
relative contributions of these various sources of natural and artificial
35
-------
radionuclides. These data can be used for establishing allowable
discharge rates for the various sources. However, the establish-
ment of source-oriented MFC values from MFC _ data would require
sw sf
both estimations of the seafood ingestion rates and distribution
patterns and an arbitrary allocation of some fraction of the MFC
r sw
that could come from, for example, nuclear ships.
The NAS/NRC (1959) recognized that the MFC for aquatic environ-
ments was generally interpreted to be the MFC , and that this was
vv
generally sufficient when food organisms in question derive their
radionuclides directly from water. Where the food organisms derive
radionuclides from other sources (such as bottom debris or via food
chains), then the CF's specific for biota of interest should be
used in calculations. Usually such data are unknown.
Eventually, it may be possible to incorporate dynamic food
chain models into the derivation of CF's. A simple food chain
simulation model has been described by Eberhardt and Nakatani (1969) in
which a tracer substance is released at an exponentially declining rate,
and a fraction is transferred to the first compartment, a producer.
Two hypothetical animals are included in this model, one with a
single internal compartment and the other with two compartments in
parallel. This type of compartmentalized food-chain model could be
expanded to describe complex ecological webs. A similar source-
pathway-receptor model is described by Reichle (1970).
Another possible refinement of CF determinations may occur if
interspecies variability can be predicted. The uptake and retention
of many substances is proportional to a fractional power of body
weight. When this relation is extended to interspecies comparisons,
the resulting power coefficient is much lower than that expected on
the basis of relationships between size and metabolic rate. It was
proposed by Thomas and Eberhardt (1969) that interspecies comparisons
be based on "similarity ratios" that depend on the proportionality
coefficient in the equation:
36
-------
y = a Wb (7)
where:
y = retention time
a = proportionality coefficient
W = body weight
b - 0.75
Eberhardt (1969) has successfully related the long-component half-
137
life for Cs in humans to body weight with a power coefficient of
0.66.
Further modifications to calculations can be made by either
broadening or narrowing the scope of dietary assumptions. Rice
(1963) points out that the organisms which concentrate a radionuclide
to the highest degree are not necessarily the controlling factor
in allowable radioactive waste disposal rates. Rather, the organisms
which concentrate to the highest degree in relation to the amount
ingested by man are critical. He has tabulated CF's for the follow-
ing major organism classifications: algae, mollusca and fish.
Freke (1967) used a similar approach, but included Crustacea as a
major food subdivision. In other concentration factor listings,
Aten (1958 and 1961) considered only fish as critical, while
Polikarpov (1966) lumped together "marine organisms" and "freshwater
organisms".
In an International symposium report, Hiyama (1960) adds yet
another suggestion by pointing out that since man eats numerous
kinds and quantities of marine foods a derived working level should
not be based merely on the CF for one food product. He recommends
the use of a "seawater equivalent for daily human intake" (W,).
Alternatively, when the specific activity approach is used, he
recommends a "seawater equivalent for the whole body" (W, ), or for
the critical organ (W, ). The following formulas are derived:
W, = M . I/S liters/day/person (8>
where:
I = average daily intake of element, g/day/person
37
-------
M = fraction of I that originates from seawater
marine organisms
S = concentration of that element in seawater, g/1
W, = seawater equivalent for human intake
The ICRP (1959) listings for maximum permissible daily intake of
certain radionuclides (MPDI in pCi/day/person) can be used to
derive the maximum permissible concentrations for seawater (MFC ):
S vv
MFC = MPDI/W, uCi/1 (9)
sw d
If little is known about I, but the average amount of the element in
the whole body or in the critical organ is known, then the following
seawater equivalents can be derived:
W = M . B/S liters (10)
or
where:
W = M . B /S liters (11)
DC *--
W, = seawater equivalent for the human body
(liters)
W, = seawater equivalent for the critical
organ (liters)
B = average amount of element in the human
body (grams)
B = average amount of element in the critical
organ (grams)
S = concentration of element in seawater
(gram/liter)
M = fraction of B or Bc that originates from
seawater or marine organisms
The ICRP (1959) listings for the maximum permissible amounts of
radioisotopes in the total body (q, pCi) and in the critical organ
(q , yCi) also can be used to derive a maximum permissible concentra-
tion for seawater (MFC ):
sw
MFC = q/W. yCi/1 (12)
S V7 D
38
-------
Where radioactive contamination extends to terrestial food, any such
MFC must be reduced proportionally. If the isotopic dilution ratios
S«v
are similar in both terrestrial foods and seafoods, then "M" is not
required for the above equations.
So far, the foregoing discussion illustrates that the scope of
the terms MFC , and MFC can range from very generalized figures that,
at best, give order of magnitude estimates, to more specific derived
working limits for particular areas which may be used to guide waste
disposal practices. An additional interpretation (Miller and Inclan-Suarez,
1970) of allowable discharge rates or MFC values has been applied at least
once by a State regulatory agency with review authority for nuclear
power plants. This interpretation sets MFC values as those attained
by the lowest technologically-feasible point-source radioactive waste
discharge.
It should be noted that MFC values are intended for limiting human
exposure risks. Relatively little is known about the tolerance of
aquatic biota to chronic radioactive contamination. There appears to
be considerable species differences and variability, as well as signi-
ficant variability within the same species in regard to different
developmental stages and food intake. Between species it has been
generally observed that for acute radiation doses the least specialized
forms are also the most resistant.
There appears to be no generally applicable approach to describe
the transport of radionuclides introduced into surface waters. Each
stream, river, lake, bay, estuary, and sea has mixing characteristics
unique in place and time. Moreover, introduced radionuclides can remain
in solution or suspension, precipitate and settle on the bottom, or be
concentrated by plants and animals (Rice, 1965). For those nuclides
that remain in solution, mixing by physical processes of diffusion,
turbulence, etc., is generally defined (Eisenbud, 1973) by a combina-
tion of theoretical calculations and measurements that are applicable
only to the specific locality. An example of an investigation in which
many factors were incorporated is the Delaware River/Estuary Study
39
-------
(Parker et dl.3 1961). Data on convection and diffusion were obtained
from a scale model with tracer dyes. Calculations based on these data
were modified for radioactive decay. Since they are somewhat concen-
tration dependent, sorption and sedimentation reactions were expressed
mathematically as exponential decay.
The marine environment has been subdivided descriptively by
several investigators. From the viewpoint of characteristic physical
and biological processes which may return radioactive materials to
man, there are three major divisions (Schaefer, 1961; NAS/NRC, 1959):
(1) near shore areasharbors, estuaries, and coast out 2 miles from
shore; (2) continental shelf areasubdivided into an inner shelf 2
to 12 miles from shore and an outer shelf from 12 miles to the
200 fathoms contour; and (3) open oceanmore than 12 miles from
shore and 200 fathoms deep. The latter two areas can be subdivided
further into commercial fishing and noncontributory areas.
Rice (1965) compares estuarine and oceanic habitats. He points
out that radionuclides released in the open ocean tend to be rapidly
diluted and dispersed, whereas in an estuary there is more chance of
biological and physico-chemical concentration. Due to the shallow
depth, sediment and the benthic community involved, radioisotope
exchanges are relatively important in estuaries, but not in open
seas. A third difference is that oceanic food chains are simple in
comparison with those of an estuary.
Berglin (1960) has proposed a method for determining mixing in
the Woronara Estuary, Australia, which may be useful for studying other
estuarine situations. Typically, freshwater discharged to the estuary
moves seawards by mass flow with turbulent mixing resulting from tidal
motion. If the freshwater inflow rate is monitored, the mean dilution
which can be expected within a particular section (e.g., 1/4 mile) can
be determined by measuring the ratio of seawater to freshwater in the
section. Then, multiplying the maximum acceptable activity levels in
a section by the mean dilution factor gives the allowable mean input
concentrations for the section. This method would have limited usefulness
40
-------
in situations where freshwater overrides the saltwater or where fresh-
water plumes extend out to sea.
Pritchard (1960) reviews several methods of calculating mixing and
transport in different aquatic habitats. Included are formulas to esti-
mate dispersal in a continental shelf area so that a radionuclide concen-
tration at an input area boundary can be calculated. In another model,
the dispersal of activity from a deep-sea bottom is estimated using
conservative estimates of the vertical diffusion and by neglecting the
loss to sediment. The formulas he presents yield estimates of the
amounts of activity which, if released annually in a deep-sea segment,
would produce at the bottom of the ocean layer harvested by man an
equilibrium concentration which would not exceed the allowable values
for the isotopes involved.
One of the least known components of aquatic ecosystems is the
exchange between water and bottom sediments. The NAS/NRC (1971) has
even suggested that it may be impossible to generalize these sorption
and sedimentation reactions. However, Lerman (1961) has developed a
generalized sediment transport model which defines several mechanisms
for entry of radioisotopes into the sediment. These are:
1. Deposition of suspended particles of inorganic or organic
origin;
2. Diffusion from the overlying water into the sediment
interstitial water, followed by adsorption; and
3. Production from parent radionuclides in sediments or
release from decomposition of organic matter.
The effects of these various factors on the concentration of a radio-
nuclide in sediment is summarized in a series of equations which
relate these factors to the rate of change of the radionuclide concen-
tration in interstitial water.
A paper by Reynolds (1963) on the sorption and release of radio-
nuclides from sediments contained theoretical dispersion formulas
based on a simple compartmental stream model. He developed an equa-
tion for a sediment distribution coefficient which was derived from a
41
-------
mass-action equilibrium equation with the assumption that the exchanged
ions were at very low concentrations.
A study of the Clinch River provides some surprising results in
regard to river transport characteristics. It was found that sloughs
did not have an appreciably greater buildup of radionuclides than the
main river channel. Parker (1967) stated that "possibly the most
important outcome of the Clinch River Study is the successful applica-
tion of mass-balance techniques to entire river complexes". This
study showed that the water-borne load of radionuclides was almost the
entire amount discharged to the river. The sediment load was small
(2 to 5% maximum); the maximum inventory possible in the biomass was
exceedingly small and could be neglected. These results support earlier
work reported by Polikarpov et al. (.1966) in which it is postulated that
the biomass may be neglected as a significant depot of activity in a
reservoir or lake system. This is true, they concluded, even though
the average CF's in the biomass and sediments may be 1,000 and 100,
respectively, because the relative biomass is small as compared to
other system components.
Armstrong and Gloyna (1967) developed a general equation to
describe radionuclide transport in terms of hydraulic dispersion and
convection in detention systems (compartments) which sorb and release.
For non-conservative substances, such as radionuclides, a sink must
be included to account for the uptake of material from solution. A
generalized form of the equation for a radionuclide is:
AC = D - V - U (14)
where:
AC = change in water concentration
D = dispersion term
V = convection term
U = uptake term
They point out that the uptake term is very poorly defined. It includes such
variables as sorption of radionuclides by suspended solids, sediment and
plants. They also proposed a general equation for uptake reactions in which
the uptake is a summation of sorption on various substrates. The rates of
42
-------
sorption and desorption are dependent on the concentration gradient
between a transfer substrate and the sorbent. A linear transfer
function is used to correlate sediment specific activity to that of
water, although they point out the possibility of using an alternative
nonlinear function. The study showed that suspended solids, sediment,
and plants (ya££isneria/l sorb according to a nonlinear (Freundlich
isotherm) function. However, attempts to use this equation in the
reaction term of the one-dimensional (e.g., a river)dispersion equation
forces it into a nonlinear form and makes analytical solution impossi-
ble. A by-product of the transport equation (using a linear transfer
function) is the specific activity of radionuclides in the biological
system. It is feasible to use these results to determine the passage
(transfer coefficients) through aquatic food chains by using the
general equation for uptake reactions.
Kaye and Ball (1967) proposed the application of systems analysis
techniques to ecosystem models describing radionuclide transport. Their
approach uses input and loss relationships which allow calculation of
the radionuclide concentration in any environmental compartment. Two
important kinds of required information are (1) an accurate compart-
mentalized representation of the environment under review; and (2) the
rate constants which quantify the intercompartmental transfer of nuclides.
This technique was developed into a comprehensive model for predicting
transport of radionuclides from an underground nuclear explosion through
the seawaterfishman pathway by Bloom (1971). It is apparent that
further modifications of this technique may allow the development of
models to deal with chronic releases of radionuclides from various
sources.
SPECIFIC ACTIVITY APPROACHES
The specific activity approach is attractively simple in concept
and is very useful in assessing long-term problems concerning the radio-
isotopes of elements which (1) are relatively abundant in nature, (2)
are rapidly dispersed throughout the environment, and (3) are normal
constituents of organisms (e.g., 3H, l C, 2P). The NAS/NRC (1962)
43
-------
in developing recommendations for ocean disposal of radioactive wastes
stated the principle: ". . .if the specific activities (that is, the
radioactive proportions of the elements) of the chemical elements in
the sea in the environment of human food organisms are maintained below
the allowable specific activities for those elements in the human body
or human food, no person can obtain more than an allowable amount of
radioactivity from the sea, regardless of his habits." For trace
elements and those radioisotopes which are close chemical congeners
of another element, the specific activity approach lacks consistency.
A method recently developed at LLL (Pratt, 1970; Tamplin et al.t 1968
and 1969; and Thompson et at* , 1972) is baaed on specific activity and
is similar to the NAS/NRC approach except that it relates to tissue dose
rather than to critical organ dose.
The specific activity approach, as developed by the NAS/NRC
(1962), was for calculation of derived working limits for radioactive
waste disposal into Pacific coastal waters. The approach is based on
two major assumptions:
1. that a radioisotope introduced into the environment readily
equilibrates with the stable isotope(s) of the same element,
and
2. that the quantity of each stable element in each body organ
is fixed and does not fluctuate with the intake of that
element.
It is known that the conditions of the first assumption are not always
met. Known exceptions have been tritium, carbon, sulfur, vanadium,
iron, cobalt, copper, and zinc. These elements may be introduced as
stable organic complexes and, hence, are not diluted by the common
abundant chemical form of the stable elements. The NAS/NRC (1962)
recommends that for these elements the safety factor for modifying
figures from occupational worker dose to general public dose be
increased from a factor of 10 to 100.
The maximum permissible specific activity (MPSA) for any radio-
isotope with a critical organ other than the GI tract is readily avail-
able from data on standard man (ICRP, 1959).
44
-------
MPSA = q/mC jaCi/g (15)
where:
MPSA - maximum permissible specific activity
(pCi/g)
q = maximum permissible burden of radio-
isotope in critical organ (pCi)
m = mass of the critical organ (g)
C = concentration of stable element in
critical organ (g/g)
The MPSA can then be converted to derived working limits for a media.
For example, the values for
calculated (NAS/NRS, 1962):
For example, the values for seawater (DWL ) or seafood (DWL ) are
sw sf
DWL = K (MPSA) yCi/cm seawater (16)
C> W W
DWLgf = K (MPSA) yCi/g seafood (17)
where:
2
K = grams of stable element/cm seawater
w
K,. = grams of stable element/g seafood
A DWL derived in this fashion is independent of CF's and the consumption
rates for seafoods.
For those isotopes that are only slightly absorbed by the body
and mainly affect the gastrointestinal tract, the MFC in water is
converted to a MPSA of the stable species in seafood by utilizing the
abundance of that element in seafood organisms which results in the
most restrictive requirement. Although developed specifically for
pathways from the sea, this approach can be extended to freshwater
and terrestrial environmental pathways (NAS/NRG, 1962, and Bryant, 1970).
An alternate method has been proposed by the NAS/NRC (1959) for
computing allowable environmental levels of certain radionuclides for
which a known human discrimation factor exists. For example, the ratio
90
of Sr to calcium in the total body should not exceed 0.1 pCi/kg.
Man physiologically discriminates against strontium in a strontium-
calcium mixture by a ratio of 8:1. If man receives his total protein
90
allowance from fish which contain Sr, then the MFC for fish is
45
-------
90
defined as 0.8 yCi of Sr/kg calcium. Further, since the calcium
concentration of seawater is about 0.4 g/kg seawater, the seawater
MFC is about 0.8 yCi/2,500 kg or about 3 X 10~ pCi/ml of seawater.
The occupational MFC for continuous exposure in drinking water is
10~10 nCi/ml (ICRP, 1959).
Odum (1963) has extended this idea of using the known ratio of
a radionuclide to a stable physiological element in a theoretical
"element ratio method". Basically, he proposes that if the ratios
of the minor elements to carbon are known, then the measurement of
carbon metabolism can be used to predict cycling of the minor elements.
Bloom (1971) suggests that two screening operations be performed
before detailed calculations are made. The first uses a simple two-
compartment specific-activity model in which the specific activity of
each radionuclide in man is assumed to be the same as in the environ-
mental sink before dilution. Then, using ICRP data on radionuclides,
standard man, etc., the infinite-time internal dose is calculated for
(1) the gastrointestinal tract and (2) all other organs. For radio-
isotopes found potentially important in this initial screening, he
recommends an eight-compartment transport model which requires source
term data and transfer coefficients for the radionuclides identified
in screening. Solution of a complex set of equations provides esti-
mates of the radionuclide concentration in each of the eight compart-
ments as well as of the internal radiation dose to man as a function
of time.
A modified specific activity method for determining safe discharge
rates for radionuclides into aquatic systems is being developed at the
Lawrence Livermore Laboratory (Chapman et at. 3 1968; Harrison, 1972;
Tamplin, 1967, 1968, 1969; Burton, 1968; Ng et al.f 1966, 1968; Thompson
et al*, 1972). The approach is similar to that of the NAS/NRC (1962),
except it uses a tissue dose concept rather than a critical organ dose con-
cept. The method approaches environmental contamination by radionuclides and
the resultant radiation dose to man from the standpoint of the specific
activities of ingested elements; this is also known as the biological
46
-------
exchangeable pool of elements concept (Ng and Thompson, 1966). The
passage of a radionuclide through the biosphere is presumed to be governed
by the same factors that govern the distribution of the related stable
element isotopes within the biological exchangeable pool. It is also
presumed that the radionuclide is biologically no more (or less) avail-
able than the related stable isotopes within the environment.
The basic product of this effort is a value for each isotope called
3
the unit-rad contamination in water (F ) in yCi/m /rad. Values have
A.
been derived for freshwater and seawater. This factor is defined as
the initial concentration of a radioisotope in water which would yield
a 30-year integrated dose of 1 rad to a specific designated tissue
of standard man. In most cases F values for infants are also esti-
A
mated, since values for adults are usually less restrictive than for
infants. The values for F are derived with several simplifying
£1
assumptions, almost the same as those used by the NAS/NRC (1962),
which must be clearly understood in applying the F factors to environ-
£\
mental data. These assumptions yield very conservative values for
F , for the worst situation that could develop, and are designed in
A.
this manner so that basic information on the environment and popula-
tion at risk can be used to develop modifying factors. The simplify-
ing assumptions include:
1. Man exists on a diet of totally aquatic origin, and
2. Initial water concentrations decrease only through radio-
active decay. (Dilution of the system by uncontaminated
water and dilution beyond the area of initial rapid mixing
are not accounted
The basic calculation process is, briefly, to start with the ppm
values for stable elements in seawater and freshwater and to calculate
an uptake by man from various routes. CF's derived from the literature
for items in man's food chain are used to obtain stable isotope intake.
Various data, e.g., terrestrial and aquatic, are evaluated to obtain
the most critical pathways for calculating FA> The introduction of
radioisotopes into aquatic environments and the subsequent intake by
man are evaluated on the basis of stable element pathways. The
47
-------
radiation dose to man from radioisotopes is calculated using GI uptake
fractions, daily ingestion amounts, energy absorbed in tissue per disin-
tegration, effective half-lives in the environmental media and man's
tissue, distribution in man's tissues, etc. In a LLL report (Ng ei^ at* t
1968), all of these input parameters for calculations are listed for
radionuclides with half-lives greater than 12 hours. The derived values
for F are also listed, and some methods are given to modify these
A.
basic values to those more representative of a given situation. For
example, the calculations are described for obtaining modified F
A.
values for a population on a mixed aquatic and terrestrial diet. The
modified values obtained include corrections for both the dietary mix
and the ratio of isotope concentrations in aquatic and terrestrial
foods.
The estimated maximum radiation dose to a tissue (EDA) from a
particular isotope is obtained by dividing the aquatic environment
concentration by F as follows:
A.
where:
EDA = ECA/FA rad
A
EDA = 30-year integrated dose to a specific tissue
of standard man (or infant when designated
value of FA is used) from an aquatic diet
and for a specific isotope
EGA = contamination level of the aquatic environ-
ment in nCi/m3
3
F. = unit-rad contamination factor in uCi/m /rad
The total dose to a specific tissue is the sum of the doses from
individual radionuclides.
Pratt (1970) has used much of the above information in deriving unit-
dose-rate water concentration values. These are water concentration values
for isotopes which could yield an equilibrium dose rate of 1 rad per year
to an adult through aquatic foods. Values are also derived for infants.
Since these concentrations can be scaled to appropriate maximum allowable
dose rates, the maximum allowable concentrations in an aquatic environ-
ment can be calculated. The maximum allowable rates of release can
48
-------
then be calculated using appropriate dilution and dispersion factors.
The maximum allowable dose to people through aquatic foods still must
be designated in this approach if firm regulatory guides are to be
promulgated. In general, regulatory bodies have avoided fragmenting
the total allowable dose into portions related to specific exposure
routes. The basic criteria is dose from all sources, and the fractional
contribution from a specific route varies with each particular situation.
In general, the specific activity approach gives less stringent
standards for radioactive waste disposal in seawater than are derived
through critical pathways models. The latter tend to be more restric-
tive, apparently because conservative values are generally used for
unknown concentration factors. The specific activity approach has the
following limitations (Wolfe and Rice, 1968):
1. It is not valid when considering radiation dose to the
gastrointestinal (GI) tract.
2. As the maximum permissible body burden for radioactivity is
approached in humans, the total activity in the GI tract
becomes significant, regardless of what the specific
activity may be.
3. Radionuclides introduced into the environment may be more
(or less) readily available for bioaccumulators than the
corresponding stable elements.
In the final transition of adapting allowable dose rates into
maximum permissible concentrations for radionuclides in air, food,
and water, and subsequently into directives for operating practice,
there is practical value in an easily understood index of hazard.
Such an index has been proposed by Rohwer and Struxness (1972) and is
termed a "cumulative exposure index". This is a numerical guide
indicating relative significance (dose estimate/dose limit) of measured
environmental radioactivity on the basis of the total dose to man from
all radionuclides and exposure modes of importance.
49
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TECHNICAL REPORT DATA
(flease read Instructions on the reverse before completing)
REPORT NO.
EPA-600/3-76-054
2.
3. RECIPIENT'S ACCESSION-NO.
4. TITLE AND SUBTITLE
CONCENTRATION FACTORS AND TRANSPORT MODELS FOR
RADIONUCLIDES IN AQUATIC ENVIRONMENTS A
Literature Report
5. REPORT DATE
May 1976
6. PERFORMING ORGANIZATION CODE
'. AUTHOR(S)
R. G. Patzer
8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
Environmental Monitoring and Support Laboratory
Office of Research and Development
P. 0. Box 15027
Las Vegas, NV 89114
10. PROGRAM ELEMENT NO.
1FA083 .
11. CONTRACT/GRANT NO.
n/a
12. SPONSORING AGENCY NAME AND ADDRESS
Same as above
13. TYPE OF REPORT AND PERIOD COVERED
Final - FY75
14. SPONSORING AGENCY CODE
EPA-ORD, Office of Health and'
Ecological Effects
15. SUPPLEMENTARY NOTES
16. ABSTRACT
The relative risks to man from radionuclides released to the environment depend
heavily on their accumulation or concentration by aquatic organisms. The
organisms which accumulate those radionuclides present in the environment may
be useful as indicators for environmental monitoring purposes. In addition,
these organisms may be directly in food chain pathways to humans.
Literature is reviewed and summarized in regard to biological concentration of
radionuclides in freshwater and marine environments. Concentration factors for
elements found in organisms are tabulated for plants, invertebrates, and fish
in marine and freshwater environs. Literature is also reveiwed on models
developed to calculate the possible radiation dose delivered to humans from
radionuclides released into aquatic environments. The model approaches
summarized range from simple generalized forms which, at best, give order
of magnitude estimates to detailed models for a specific area which may be
used to guide waste discharge practices.
17.
KEY WORDS AND DOCUMENT ANALYSIS
DESCRIPTORS
b.lDENTIFIERS/OPEN ENDED TERMS
COS AT I Field/Gioup
Concentration
Isotopes*
Mathematical Models*
Radiation Monitors
Radiation Protection
Biological concentration
Concentration factors*
Transport models*
06R
07E
08H
18H
18. DISTRIBUTION STATEMENT
RELEASE TO PUBLIC
19. SECURITY CLASS (ThisReport)
UNCLASSIFIED
21. NO. OF PAGES
64
20. SECURITY CLASS (Thispage)
UNCLASSIFIED
22. PRICE
EPA Form 2220-1 (9-73)
&GPO 691-217-1 976
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