Uptake and elimination of radiocaesium in fish and the "size effect."

A number of hypotheses have previously been developed concerning the rates of uptake and elimination of radiocaesium (137Cs) in fish. These include the influence of potassium and other water chemical parameters on both uptake and elimination, and the effect of fish size on accumulation. In order to test these hypotheses, we have assembled a data set comprising more than 1,000 measurements of radiocaesium (137Cs) in predatory fish (perch, pike and brown trout) in nine European lakes during the years after Chernobyl. These data have been analysed using simple models for uptake and excretion of 137Cs in fish, showing that: 1. Fish-water concentration factors (CF) were inversely proportional to potassium [K+] concentration of the different lakes, in agreement with previous studies. 2. The uptake rate of 137Cs in fish was negatively correlated with lake [K+], but excretion rate was independent of [K+]. 3. Lower than expected CF values were found in one lake, Iso Valkj?rvi, Finland. This is attributed to inhibition of the K+ (and therefore 137Cs) high affinity transport system in aquatic plants and fish by low pH and/or low Ca2+. 4. The inclusion of fish weight as a parameter in our dynamic model significantly improves the ability of the model to fit the observed measurements of 137Cs. 5. The model developed from the above hypotheses was able to fit the data from nine different lakes to within approximately a factor of 3 of the observed values.     

Trace metal bioaccumulation: models, metabolic availability and toxicity

Aquatic invertebrates take up and accumulate trace metals whether essential or non-essential, all of which have the potential to cause toxic effects. Subsequent tissue and body concentrations of accumulated trace metals show enormous variability across metals and invertebrate taxa. Accumulated metal concentrations are interpreted in terms of different trace metal accumulation patterns, dividing accumulated metals into two components - metabolically available metal and stored detoxified metal. Examples of different accumulation patterns are described from crustaceans but have a general applicability to all aquatic invertebrates. Toxicity does not depend on total accumulated metal concentration but is related to a threshold concentration of internal metabolically available metal. Toxicity ensues when the rate of metal uptake from all sources exceeds the combined rates of detoxification and excretion (if present) of the metal concerned. The biodynamic model of trace metal bioaccumulation allows the prediction and explanation of widely differing accumulated trace metal concentrations in organisms, combining geochemical analyses of environmental metal concentrations with the measurement of key physiological parameters for a species from the site under consideration. The combination of the biodynamic model as a unified explanation of metal bioaccumulation with an understanding of the relationship between accumulation and toxicity sets the stage for a realistic understanding of the significance of trace metal concentrations in aquatic invertebrates.     

Dynamic model for the assessment of radiological exposure to marine biota

A generic approach has been developed to simulate dynamically the uptake and turnover of radionuclides by marine biota. The approach incorporates a three-compartment biokinetic model based on first order linear kinetics, with interchange rates between the organism and its surrounding environment. Model rate constants are deduced as a function of known parameters: biological half-lives of elimination, concentration factors and a sample point of the retention curve, allowing for the representation of multi-component release. The new methodology has been tested and validated in respect of non-dynamic assessment models developed for regulatory purposes. The approach has also been successfully tested against research dynamic models developed to represent the uptake of technetium and radioiodine by lobsters and winkles. Assessments conducted on two realistic test scenarios demonstrated the importance of simulating time-dependency for ecosystems in which environmental levels of radionuclides are not in equilibrium.     

Measurement of transuranic elements,chiefly 237Np (by neutron activation analysis), in the physical and biological compartments of the French shore of the English channel

The behaviour of transuranic elements in the marine environment has been studied via both in situ sampling and laboratory tracer experiments. In particular, the radionuclide ²³⁷Np was investigated and techniques for its quantitative determination are described. In the field investigations, a preliminary separation of Np from samples was performed prior to neutron activation analysis, with subsequent γ-ray spectrometry of ²³⁸Np. In the laboratory studies, ²³⁷Np was determined by a radiochemical method followed by α-spectrometry. The results obtained from the in situ study in the English Channel (sea water, seaweed, molluscs) and from laboratory-uptake experiments (water and mussels) are described. Levels of Pu, Am and Np are compared and the characteristics of neptunium transfer to molluscs are discussed.     

Predicting the transfer of radiocaesium from organic soils to plants using soil characteristics

A model predicting plant uptake of radiocaesium based on soil characteristics is described. Three soil parameters required to determine radiocaesium bioavailability in soils are estimated in the model: the labile caesium distribution coefficient (kd1), K+ concentration in the soil solution [mK] and the soil solution-->plant radiocaesium concentration factor (CF, Bq kg-1 plant/Bq dm-3). These were determined as functions of soil clay content, exchangeable K+ status, pH, NH4+ concentration and organic matter content. The effect of time on radiocaesium fixation was described using a previously published double exponential equation, modified for the effect of soil organic matter as a non-fixing adsorbent. The model was parameterised using radiocaesium uptake data from two pot trials conducted separately using ryegrass (Lolium perenne) on mineral soils and bent grass (Agrostis capillaris) on organic soils. This resulted in a significant fit to the observed transfer factor (TF, Bq kg-1 plant/Bq kg-1 whole soil) (P < 0.001, n = 58) and soil solution K+ concentration (mK, mol dm-3) (P < 0.001, n = 58). Without further parameterisation the model was tested against independent radiocaesium uptake data for barley (n = 71) using a database of published and unpublished information covering contamination time periods of 1.2-10 years (transfer factors ranged from 0.001 to 0.1). The model accounted for 52% (n = 71, P < 0.001) of the observed variation in log transfer factor.     

Particle and solution phase depth distributions of transuranics and 55Fe in the North Pacific

In situ large volume filtration and chemisorption techniques were used to collect samples from the North Pacific for radiochemical analyses of fallout transuranics and ⁵⁵Fe in filterable and filtered phases. The data cover several locations for surface collections and a detailed depth profile north of Hawaii at 30°N. The observed partition of these nuclides between suspended particulate and filtered phases is directly linked to the rates at which they are moved downward through the water column in association with sinking particles. Particulate phases in open ocean surface waters contain higher Pu (12–35%) than subsurface particulates (which average about 6%). ²⁴¹Am was found to exhibit much stronger particle association—typically close to 50% in both surface and subsurface waters—in accord with its known greater particle reactivity. In the high Pu deep water layer, particle associated Pu dropped to close to 1% of total Pu concentration. Together with a correlated increase in the proportion of oxidized Pu in this layer close to the sediment-water interface, this is taken as clear evidence of remobilization Pu from particles at, or near to, the interface. ⁵⁵Fe distributions on filtered particulates indicate a much deeper depth distribution relative to the transuranics. This may reflect both a higher particle association reactivity in respect to scavenging and a longer exposure history to scavenging (especially relative to ²⁴¹Am—produced by in situ decay).     

A kinetic-allometric approach to predicting tissue radionuclide concentrations for biota

Allometry, or the biology of scaling, is the study of size and its consequences. It has become a useful tool for comparative physiology. There are several allometric equations that relate body size to many parameters, including ingestion rate, lifespan, inhalation rate, home range and more. While these equations were originally derived from empirical observations, there is a growing body of evidence that these relationships have their origins in the dynamics of energy transport mechanisms. As part of an ongoing effort by the Department of Energy in developing generic methods for evaluating radiation dose to biota, we have examined the utility of applying allometric techniques to predicting radionuclide tissue concentration across a large range of terrestrial and riparian species of animals. This particular study examined 23 radionuclides. Initial investigations suggest that the allometric approach can provide a useful tool to derive limiting values of uptake and elimination factors for animals.     

The plant/soil concentration ratio for calcium,radium, lead,and polonium: Evidence for non-linearity with reference to substrate concentration

Evidence exists from both the literature and our own observations that plant nuclide uptake for a variety of plants and elements is a non-linear function of substrate concentration. The uptake response to increasing substrate concentration is usually in the form of a single or multi-phasic saturation curve. For some plant types and elements the uptake response may also take the form in which a threshold of soil activity is necessary before uptake is measurable. We present a generic uptake response curve and the resulting concentration ratio function determined by computer simulation. Data describing the uptake response of plants to ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po as well as for calcium and stable lead are discussed. Functions are also presented for these elements to describe the uptake response and the concentration ratio and their mathematical forms are compared to the generic model.     

Health concerns of consuming cockles (Cerastoderma edule L.) from a low contaminated coastal system

Commercial and recreational harvesting of shellfish within the coastal systems is usually very extensive. Since these ecosystems are frequently subjected to contamination, namely from agricultural, urban and industrial activities, and shellfish generally display a high capacity to bioaccumulate metals, populations may be at risk in terms of toxic metal exposure as a consequence of the harvesting and ingestion of near shore coastal marine organisms. Shellfish is regularly tested for concentrations of metals and other contaminants by legal authorities for commercial purposes, but although health officials use total metal as standards of food safety, only a part of the metal accumulated in shellfish is available to be assimilated and to cause toxic effect. In order to elucidate these issues an investigation on cockles inhabiting the Aveiro estuary was conducted. Element levels in sediments and wild Cerastoderma edule from sampling areas with different levels of contamination were measured; total element burden of cockles was related to accessible fraction for assimilation (TAM); element concentrations in wild C. edule were compared to EFSA (European Food Safe Authorities), USFDA (United States Food and Drug Administration) and FSANZ (Food Standards Australia and New Zealand) maximum levels (MLs); and the amount of cockle flesh needed to be consumed to exceed provisional tolerable weekly intake (PTWI) was determined. The present work showed that although sediment metal and metalloid contamination in Aveiro estuary is low the concentration of elements in C. edule does not reflect the contamination of the sediment. Aluminium (Al) and mercury (Hg) were the less and nickel (Ni), lead (Pb), zinc (Zn) and cadmium (Cd) were the most bioaccumulated metals by cockles. Comparison of MLs from international organisations with the concentration of elements in C. edule showed that arsenic (As) and Pb exceeded standard levels. The ingestion of less than 1 kg for As and 1.5 kg for Pb of cockles would result in exceeding the PTWI threshold (0.015 and 0.025 mg kg?1 week?1 respectively) in any of the areas considered in the study. Cd and Al also appear to be limiting elements for human consumption. Indeed, consumption of more than 3.1 kg and 2.1 kg of whole cockle soft part from one of the study areas during a single week would lead to exceedance of the recommended PTWI value for Cd (0.007 mg kg?1 week?1) and Al (7 mg kg?1 week?1) respectively. The health concerns to humans from cockle consumption from Aveiro estuary are discussed.     

Transfer of radionuclides in aquatic ecosystems--default concentration ratios for aquatic biota in the Erica Tool

The process of assessing risk to the environment following a given release of radioactivity requires the quantification of activity concentrations in environmental media and reference organisms. The methodology adopted by the ERICA Integrated Approach involves the application of concentration ratios (CR values) and distribution coefficients (K(d) values) for aquatic systems. Within this paper the methodologies applied to derive default transfer parameters, collated within the ERICA Tool databases, are described to provide transparency and traceability in the documentation process. Detailed information is provided for the CR values used for marine and freshwater systems. Of the total 372 CR values derived for the marine ecosystem, 195 were identified by literature review. For the freshwater system, the number of values based on review was less, but still constituted 129 from a total of 372 values. In both types of aquatic systems, 70-80% of the data gaps have been filled by employing "preferable" approaches such as those based on substituting values from taxonomically similar organisms or biogeochemically similar elements.     

Probabilistic biokinetic modelling of radiocaesium uptake in Arctic seal species: verification of modelled data with empirical observations

The necessity to provide information about radionuclide concentrations in Arctic marine species has been heightened in recent years due to a number of accidents in Arctic regions involving nuclear vessels and the presence of a large number of potential radioactive contamination sources. The provision for such information is largely dependent on the use of radionuclide uptake and transfer models. The uptake of radionuclides in Arctic seal species in this study has been modelled using a probabilistic biokinetic approach. In this paper, model results are compared with empirical data from relevant samples taken within the Arctic region. Results indicate that the model performs well when estimating concentrations of (137)Cs in two seal species for both median values and reproduction of the distribution of data values, but not as well for a third seal species. Likely factors affecting the results are the probability density functions used for the input parameters.     

Accumulation of 210Po in Baltic invertebrates

This paper presents the results of an investigation of the ²¹⁰Po contents of Baltic marine invertebrates. The ²¹⁰Po concentrations fall within the range 11·3–78·9 Bq kg⁻¹ (dry wt), the higher values relating to polychaeta, priapulida and malacostraca and the lower levels to bivalvia. It is demonstrated that ¹⁰Po is non-uniformly distributed within the isopod Mesidotea entomon and the bivalve Mya arenaria. The ²¹⁰Po contents of the internal organs decreasing in the order-hepatopancreas > alimentary tract > gill > muscle. Moreover, the results indicate the dominant role of the digestive organs of these invertebrates in controlling absorption and elimination of ²¹⁰Po.     

Effects of Soil Hydrothermal Conditions on the Complexes of Soil Invertebrates in Coniferous and Deciduous Forest Cultures

The effects of hydrothermal conditions on the complexes of soil invertebrates in 20-year-old cultures of Siberian stone pine, larch, Scotch pine, spruce, birch, and aspen are considered. The role of soil temperature and moisture content in determining the density of pedobionts and their vertical distribution is revealed. Seasonal fluctuations of hydrothermal parameters are shown to affect the vertical migrations of soil invertebrates and the dynamics of trophic structure of their complexes under forest cultures during the growing season.     

Uptake, retention and organ/tissue distribution of 137Cs by Japanese catfish (Silurus asotus Linnaeus)

The work describes the uptake, retention/biological elimination and organ/tissue distribution of 137Cs by freshwater Japanese catfish (Silurus asotus Linnaeus) under laboratory conditions. The fish were divided into three groups based on their size and age and reared in 137Cs-spiked water. The concentration of 137Cs in the whole body of the live fish was measured at regular intervals up to 60 days. A significant accumulation of 137Cs was found, but a steady state condition was not achieved by the end of the experiment. The bioaccumulation factors at steady state and the required time to reach steady state were estimated to be 1.55 and 255 days, 1.76 and 180 days and 1.99 and 160 days for large, medium and small size fish, respectively. To determine the effective half-life of 137Cs, the fish were transferred and reared in the non-contaminated host water. The concentration of the remaining 137Cs in the whole body of the live fish was measured up to 66 days. The average effective half-life of 137Cs in the fish species was found to be approximately 142 days for fish of all sizes. The distribution of 137Cs in different organs/tissues of the fish was determined. Accumulation of 137Cs in muscle/flesh of the fish was found to be approximately 75% of whole body accumulation. The uptake rate and the retention capability of juvenile fish were found to be higher and therefore, these were more susceptible to 137Cs than adult and old fish, and could be an important source of 137Cs in the human food chain.     

Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland)

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.     

Accumulation and release of 241Am by a macrophyte of the Yenisei River (Elodea canadensis)

The source of radioactive contamination of the Yenisei River floodplain, including contamination with transuranic elements, is the Mining-and-Chemical Combine of the Russian Ministry of Atomic Energy, which has for many years been producing weapons-grade plutonium. Transuranic elements have been detected not only in the soil and sediment of the river but also in the biomass of aquatic plants. This work is an investigation of accumulation and release of 241Am by a submerged macrophyte of the Yenisei River (Elodea canadensis) in laboratory experiments. In 2000-2003, laboratory experiments were carried out with biomass of E. canadensis Mich. and filtered river water. The samples were collected from the Yenisei River upstream of the discharge of the Combine's radioactive effluent. The experiments showed that 241Am is accumulated by Elodea biomass: the activity concentration of 241Am can reach 3280+/-240 Bq/g, with the concentration factor for 241Am 16 600+/-2200l/kg. Results of chemical fractionation have proved that in the course of 241Am accumulation by Elodea biomass, 241Am tightly bound to biomass increases from 11% to 27% of the total 241Am in the biomass. Release of 241Am from the decaying Elodea biomass has been evaluated experimentally. By the end of the experiment (lasting up to 127 days), the Elodea plants had lost up to 65% of their initial 241Am activity and the rate of 241Am release into the water environment reached 23 Bq/day.     

210Po in the marine environment with emphasis on its behaviour within the biosphere

The distribution and behaviour of the natural-series alpha-emitter polonium-210 in the marine environment has been under study for many years primarily due to its enhanced bioaccumulation, its strong affinity for binding with certain internal tissues, and its importance as a contributor to the natural radiation dose received by marine biota as well as humans consuming seafoods. Results from studies spanning nearly 5 decades show that ²¹⁰Po concentrations in organisms vary widely among the different phylogenic groups as well as between the different tissues of a given species. Such variation results in ²¹⁰Po concentration factors ranging from approximately 10³ to over 10⁶ depending upon the organism or tissue considered. ²¹⁰Po/²¹⁰Pb ratios in marine species are generally greater than unity and tend to increase up the food chain indicating that ²¹⁰Po is preferentially taken up by organisms compared to its progenitor ²¹⁰Pb. The effective transfer of ²¹⁰Po up the food chain is primarily due to the high degree of assimilation of the radionuclide from ingested food and its subsequent strong retention in the organisms. In some cases this mechanism may lead to an apparent biomagnification of ²¹⁰Po at the higher trophic level. Various pelagic species release ²¹⁰Po and ²¹⁰Pb packaged in organic biodetrital particles that sink and remove these radionuclides from the upper water column, a biogeochemical process which, coupled with scavenging rates of this radionuclide pair, is being examined as a possible proxy for estimating downward organic carbon fluxes in the sea. Data related to preferential bioaccumulation in various organisms, their tissues, resultant radiation doses to these species, and the processes by which ²¹⁰Po is transferred and recycled through the food web are discussed. In addition, the main gaps in our present knowledge and proposed areas for future studies on the biogeochemical behaviour of ²¹⁰Po and its use as a tracer of oceanographic processes are highlighted in this review.     

Bioaccumulation of 137Cs and 57Co by five marine phytoplankton species.

Under controlled laboratory conditions, we have examined the bioaccumulation of 137Cs and 57Co in three prymnesiophytes, the coccolithophorid Emiliania huxleyi and the noncalcareous species Isochrysis galbana and Phaeocystis globosa, and two diatoms Skeletonema costatum and Thalassiosira pseudonana. We measured the uptake in growing and non-growing cells and determined concentration factors on both volume and dry weight bases. For uptake of 57Co in non-growing cells, volume concentration factors (VCF) at equilibrium ranged from 0.2 x 10(3) for E. huxleyi to 4 x 10(3) for T. pseuedonana. For uptake of 137Cs in non-growing cells, the VCFs were low for all species and the uptake pattern seemed unsystematic. The results suggest that, in contrast to Co, the cycling and bioaccumulation of Cs in marine animals are unlikely to be affected by Cs accumulation in primary producers.     

Uptake and depuration of 131I by the edible periwinkle Littorina littorea: uptake from seawater

Uptake and depuration experiments for the edible periwinkle Littorina littorea have been performed using 131I-labelled seawater. Throughout the experimental phase the winkles were fed on unlabelled Chondrus crispus. 131I concentrations in winkles during uptake followed linear first-order kinetics with an uptake half-time of 11 days, whereas for depuration a triphasic sequence with biological half-lives of 4, 23 and 56 days was determined. In general, iodine turnover in winkles via labelled seawater appears to be slower than observed for other molluscs (2-3 days). Most of the activity prior to and after depuration is found to be in the shell, with indications that shell and soft parts accumulate and depurate 131I at a similar rate. The operculum displays the highest specific activity of all fractions with a concentration factor of 750 l kg(-1). Concentration factors for whole winkle, shell, soft parts and digestive gland are in the order of 40-60 l kg(-1), higher than the IAEA recommended CF value for iodine in molluscs of 10 l kg(-1). The 131I CF in winkles is closer to that of the conservative radionuclides 99Tc and 137Cs than the CF of the particle reactive radionuclides (239,240)Pu and 241Am.