Bioavailability of sediment-associated and low-molecular-mass species of radionuclides/trace metals to the mussel Mytilus edulis

Sediments can act as a sink for contaminants in effluents from industrial and nuclear installations or when released from dumped waste. However, contaminated sediments may also act as a potential source of radionuclides and trace metals to the water phase due to remobilisation of metals as dissolved species and resuspension of particles. The marine mussel Mytilus edulis is a filter-feeding organism that via the gills is subjected to contaminants in dissolved form and from contaminants associated to suspended particles via the digestive system. In this paper the bioavailability of sediment-associated and seawater diluted Cs, Co, Cd and Zn radioactive tracers to the filtering bivalve M. edulis has been examined. The mussels were exposed to tracers diluted in ultrafiltered (<10 kDa) seawater (Low Molecular Mass form) or to tracers associated with sediment particles from the Stepovogo Fjord at Novaya Zemlya in short-term uptake experiments, followed by 1-month depuration experiments in flow-through tanks. A toxicokinetic model was fitted to the uptake and depuration data, and the obtained parameters were used to simulate the significance of the two uptake pathways at different suspended sediment loads and sediment-seawater distribution coefficients. The results of the model simulations, assuming steady state conditions, suggest that resuspended particles from contaminated sediments can be a highly significant pathway for mussels in the order ¹⁰⁹Cd ≌ ⁶⁵Zn < ¹³⁴Cs < ⁶⁰Co. The significance increases with higher suspended sediment load and with higher K_d. Furthermore, the experimental depuration data suggest that Cs is retained longer and Co, Cd and Zn shorter by the mussels when associated with ingested sediments, than if the metals are taken up from the low molecular mass (LMM) phase.     

Modeling 137Cs migration processes in lake sediments

Lake sediments can be considered as the "diary" of the lake: new layers are continuously deposited on top of the sediments. The migration behavior of radionuclides, particularly of (137)Cs, can be analyzed by modeling the input into and the vertical distribution within the sediment. For this purpose, a model consisting of sedimentation-diffusion equations was developed. Solved with a finite element method, this model can cover the time period from the nuclear weapons testing to the present. It takes into account fixation and redissolution, compaction of sediments, and the influence of competing ions on the retarded diffusion within the sediments. The outcome of the model is compared to water and sediment measurements from Lago Maggiore. The results of an optimization process can produce the sedimentation rate and (137)Cs distribution coefficients which determine the uptake of activity into the sediment and also the retarded diffusion within the sediment.     

A particle-tracking method for simulating the dispersion of non-conservative radionuclides in coastal waters.

A particle-tracking method has been used to simulate the dispersion of non-conservative radionuclides in the sea. Three dimensional turbulent diffusion and the interactions between water, suspended matter and bottom sediments are simulated using a stochastic method. Kinetic transfer coefficients, as in finite difference models, are used to describe the transfers between the liquid and solid phases. Deposition of suspended matter and erosion of sediment are also included in the model. The method has been applied to simulate the dispersion of 137Cs and (239,240)Pu in the English Channel and the results have been compared with those of a finite difference model. The results from both techniques are, in general, in good agreement.     

Levels of 137Cs in muddy sediments on the seabed in the Bay of Cadiz (Spain). Part II. Model of vertical migration of (137)Cs

This second part of the study reports the development of a model to describe the vertical migration of the artificial radioisotope (137)Cs in the sediment column on the seabed of the Bay of Cadiz. The application of the model provides an overall picture of the process of sedimentation in the Inner Bay of Cadiz. The spatial distribution of the rate of sedimentation enables us to study the sources of sediments and the means by which the sediments have been transported. A method has been derived from the rate of sedimentation to perform the dating of the layers of sediment. The model describes the behaviour of (137)Cs in the area under study, taking into account the time of residence in the zones that are the source of accumulation, the origin of the sedimentary material, together with the diffusion of the radionuclide in the sediment of the seabed.     

A process-based model for the partitioning of soluble, suspended particulate and bed sediment fractions of plutonium and caesium in the eastern Irish Sea

A dynamic model of plutonium behaviour in the marine environment has been developed, representing the oxidation state distribution and partitioning of plutonium between the soluble, colloidal, suspended particulate and seabed sediment fractions. With simple re-parameterisation, this model can also be applied to (137)Cs. The model, which is calibrated and validated against field data, has been used to predict concentrations of Pu(alpha) and (137)Cs in both water and seabed sediments from the vicinity of the Sellafield Ltd. reprocessing plant in Cumbria, UK. The model predicts that sediment reworking and transport are the key environmental processes as the Sellafield Pu(alpha) and (137)Cs discharge continues to decline. Inventory calculations generated by the model are consistent with previous estimations. For a hypothetical post-discharge scenario, the concentrations of these radionuclides in both seawater and surface sediments are predicted to decrease sharply, concurrent with a downward vertical migration of the activity retained in sediments.     

137Cs in the Danish Wadden Sea: contrast between tidal flats and salt marshes

The 137Cs activity of salt marsh and tidal flat sediments of the northern part of the European Wadden Sea was studied based on a comprehensive dataset of 210Pb dated cores. The 137Cs inventory of salt marsh sediments shows a major peak corresponding to the Chernobyl accident in 1986, and a minor peak located in the late 1960s interpreted as the combined effect of atmospheric testing of nuclear weapons. Emissions from the nuclear reprocessing plant Sellafield are not reflected as peaks in 137Cs activity, but may contribute to the rising 137Cs activity in the years prior to 1986. The 137Cs activity of tidal flat sediments differs from salt marsh sediment in two respects. First, the activity is much lower and, second, the major peak in the 1980s is located in the beginning instead of in the middle of the decade. The differences in 137Cs inventory between the two environments are interpreted to result from repeated cycles of deposition/resuspension and mixing on tidal flats. A simple model illustrating the consequence of mixings returns an apparent shift of major peaks in 137Cs activities backwards in time corresponding to the mixing depth divided by the deposition rate.     

Inventories of Pu, Cs, and excess Pb in sediments from freshwater and brackish lakes in Rokkasho, Japan, adjacent to a spent nuclear fuel reprocessing plant

We investigated the vertical profiles of ^239+240Pu, ¹³⁷Cs, and excess ²¹⁰Pb (²¹⁰Pb_ex) in sediment core samples obtained from two freshwater lakes and two brackish lakes situated near the first commercial spent nuclear fuel reprocessing plant in Rokkasho, Japan, before the final test of the plant using actual spent nuclear fuel. The inventory of ^239+240Pu in those lakes was larger than that in soil in Rokkasho, which indicated the inflow of ^239+240Pu from the catchment area in addition to direct deposition on the lake surfaces. The ¹³⁷Cs inventory in sediments of the brackish lakes was lower than that in the soil, which showed that part of the ¹³⁷Cs was removed from the sediments by the brackish water or that it was not deposited into the sediments, because of the high solubility of Cs in brackish water. The ¹³⁷Cs inventory in sediments of the freshwater lakes was higher than that of the brackish lakes, and comparable with that in soil except for one core sample out of four. The ^239+240Pu/¹³⁷Cs ratio in freshwater lake sediments was higher than that in soil, and that indicated that part of the ¹³⁷Cs was lost from the sediments. The low inventory of ¹³⁷Cs may be attributable to competition for absorption sites in sediments with ammonium ions formed in the reducing environment which occurs from summer to fall in the sediments. Those data will be used as background data on the artificial radionuclides in the lakes to assess the effect of released radionuclides on their concentrations.     

A modelling study on 137Cs and 239,240Pu behaviour in the Alborán Sea, western Mediterranean

A model for simulating the dispersion processes of 137Cs and 239,240Pu in the Alborán Sea is described. The model consists of two hydrodynamic models: a 2D depth-averaged model and a two-layer model which provide tidal and geostrophic currents, respectively; a sediment transport model which provides suspended particle concentrations and sedimentation rates over the domain; and the radionuclide dispersion model including interactions of dissolved radionuclides with suspended particles and bed sediments. These processes are formulated using kinetic transfer coefficients. The hydrodynamic and sediment models are run and validated in advance, and their results are then used to simulate the dispersion of 137Cs and 239,240Pu, which are introduced from atmospheric fallout. Radionuclide concentrations in the water column and distributions in bed sediments have been compared with measurements in the sea. Both set of data are, in general, in agreement. The model has also been applied to calculate radionuclide fluxes through the Strait of Gibraltar. These computed fluxes have been compared with previous estimations as well.     

Fukushima fallout in Northwest German environmental media

Traces of short- and long-lived fallout isotopes (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were found in environmental samples collected in Northwest Germany (rain water, river sediment, soil, grass and cow milk) from March to May 2011, following the radioactivity releases after the nuclear accident in Fukushima, Japan. The measured concentrations are consistent with reported concentrations in air, amount of rainfall and expected values applying simple radioecological models. The [¹³⁴Cs]/[¹³⁷Cs] ratio reported for air (about 1) allows for discrimination between “recent” and “old” ¹³⁷Cs. Expected ¹³⁶Cs values fell below the detection limits of the instrumentation, despite large sample masses and long counting times.     

137Cs and excess 210Pb deposition patterns in estuarine and marine sediment in the central region of the Great Barrier Reef Lagoon, north-eastern Australia

This paper focuses on the distribution of 137Cs and 210Pb(xs) in 51 estuarine and marine sediment cores collected between the Upstart Bay and Rockingham Bay in the Great Barrier Reef Lagoon, north-eastern Australia. Historical records of 210Pb(xs) and 137Cs atmospheric deposition and present day terrestrial inventories in north-eastern Australia are presented. 210Pb(xs) and 137Cs fluxes measured on suspended sediments in the Burdekin River are considered to be a source of recent inputs of these nuclides to the nearshore region of this part of the Great Barrier Reef. Direct correlations between sediment nuclide inventories, maximum detectable depths, and sediment mass accumulation rates (MARs), calculated using both 137Cs and 210Pb(xs), are explored. In relation to inventories of 210Pb(xs), 60% of atmospheric fallout 137Cs appears to be missing from the sediments. The reasons for these differences in two tracers, primarily of atmospheric origin, are discussed in terms of the geochemical properties of these two nuclides. Evidence is presented to support the hypothesis that the 137Cs distribution in these cores can be a useful independent tracer which provides confirmation of MARs calculated from the decay of 210Pb(xs).     

Land use influence on 137Cs levels in perch (Perca fluviatilis L.) and roach (Rutilus rutilus L.)

The environmental influence on Chernobyl-derived 137Cs levels in perch (Perca fluviatilis L.) and roach (Rutilus rutilus L.) was revealed using partial least-squares regression (PLS). The 53 environmental predictors used describe land use in catchment areas, various catchment area and lake characteristics, lake water chemistry, and fish stock composition. The study showed a profound effect of land use on the 137Cs levels in fish. Radiocaesium deposited on arable land was retained in the soil to a greater extent than was 137Cs deposited on wetlands, which more easily leached out to the lake ecosystems. The 137Cs deposition close to the lakes had a more pronounced effect on 137Cs levels in the fish than did more distant deposition. The radiocaesium bioavailability is mainly governed by lake water cation content, as hardwater lakes had significantly lower 137Cs content in fish. Resuspension of 137Cs contaminated sediments only had a limited influence on the observed levels in fish.     

Preliminary evaluation of (135)Cs/(137)Cs as a forensic tool for identifying source of radioactive contamination

Ratios of the fission products (135)Cs and (137)Cs were determined in soil and sediment samples contaminated from three different sources, to assess the use of (135)Cs/(137)Cs as an indicator of source of radioactive contamination. Soil samples from the Chernobyl exclusion zone were found to have to be heavily depleted in (135)Cs ((135)Cs/(137)Cs approximately 0.45), indicative of a high thermal neutron flux at the source. Sludge samples from a nuclear waste treatment pond were found to have a (135)Cs/(137)Cs ratio of approximately 1, whereas sediment collected downstream from a nuclear reactor was highly variable in both (137)Cs activity and (135)Cs/(137)Cs ratio. Comparison of these preliminary results of variability in radiocaesium isotope ratios with reports of Pu isotope ratios suggests (135)Cs/(137)Cs similarly varies with fuel and reactor conditions, and may be used to corroborate other methods of characterizing radioactive contamination.     

Determining the Chernobyl impact on sediments of a pre-Alpine lake with a very comprehensive set of data

Man-made and natural radionuclides in Lake Wallersee were determined in the pre-Alpine environment at the northern slope of the Alps, which was heavily affected by the Chernobyl fallout in May 1986. The objective of this study was to get knowledge of location and quantity of man-made radionuclide input (especially (137)Cs) generated in the Chernobyl accident to lake sediments. Eleven sediment cores were sampled and activity depth profiles of (137)Cs and (210)Pb were determined with 5mm depth-resolution. The Chernobyl fallout produced an extreme (137)Cs peak in the sediment cores providing an excellent time marker. The chronological interpretation of deeper sediment layers was done by radiochemical analysis of (90)Sr and (239+240)Pu, which were released during atmospheric weapons' tests in the 1950s and 1960s. This allowed a complete chronological analysis of the sediment cores with a very compact set of data.     

Plutonium as a chronomarker in Australian and New Zealand sediments: a comparison with Cs

The construction of high resolution chronologies of sediment profiles corresponding to the last 50-100 years usually entails the measurement of fallout radionuclides ²¹⁰Pb and ¹³⁷Cs. The anthropogenic radionuclide, ¹³⁷Cs, originating from atmospheric nuclear weapons testing can provide an important “first appearance” horizon of known age (1954-1955), providing much-needed validation for the sometimes uncertain interpretations associated with ²¹⁰Pb geochronology. However, while ¹³⁷Cs usually provides a strong signal in sediment in the northern hemisphere, total fallout of ¹³⁷Cs in the southern hemisphere was only 25% that of the north and the low activities of ¹³⁷Cs seen in Australian and New Zealand sediments can make its horizon of first appearance somewhat arguable. Low ¹³⁷Cs fallout also limited the size of the 1963-1964 fallout peak, a peak that is usually seen in northern hemisphere sediment profiles but is often difficult to discern south of the equator.This paper shows examples of the use of nuclear weapons fallout Pu as a chronomarker in sediment cores from Australia (3 sites) and New Zealand (1 site). The Pu profiles of five cores are examined and compared with the corresponding ¹³⁷Cs profiles and ²¹⁰Pb geochronologies. We find that Pu has significant advantages over ¹³⁷Cs, including greater measurement sensitivity using alpha spectrometry and mass spectrometric techniques compared to ¹³⁷Cs measurements by gamma spectrometry. Moreover, Pu provides additional chronomarkers associated with changes in the Pu isotopic composition of fallout during the 1950s and 1960s. In particular, the ²³⁸Pu/^239+240Pu activity ratio shows distinct shifts in the early 1950s and the mid to late 1960s, providing important known-age horizons in southern hemisphere sediments. For estuarine and near-shore sediments Pu sometimes has another significant advantage over ¹³⁷Cs due to its enrichment in bottom sediment relative to ¹³⁷Cs resulting from the more efficient scavenging of dissolved Pu in seawater by sediment particles.     

137Cs budget during the period of 1960s in a small drainage basin on the Loess Plateau of China

A sediment profile with a thickness of 28.12 m in a failed reservoir in a small catchment of the Yuntaishan Gully in the Loess Plateau of China consisted of 44 flood couplets deposited during the period from 1960 to 1970 with total volume of 2.36 x 10(6)m(3). Specific sediment yields for a flood event varied from 300 t km(-2) to 14,400 t km(-2) and annual sediment yields varied from 2500 t km(-2) in 1966 to 40,000 t km(-2) in 1964 with a mean value of 12,700 t km(-2)a(-1) for the period. Average annual (137)Cs concentrations of the sediments increased from 0.92 Bq kg(-1) in 1960 to 4.82 Bq kg(-1) in 1963, then decreased to 1.53 Bq kg(-1) in 1970. The total (137)Cs activity in the reservoir sediments was 9.22 x 10(9) Bq, which accounted for 31.9% of the total (137)Cs fallout precipitation of 2.89 x 10(10) Bq within the catchment during the period. The proportion of the (137)Cs loss from the catchment to the (137)Cs fallout precipitation within the catchment in a year varied between 8.01% and 66.8%, and it was 20.9% for the peak (137)Cs deposition year of 1963 and 52.0% in 1964. By analysis of the (137)Cs budget in the catchment for the (137)Cs peak precipitation period from 1962 to 1964, the (137)Cs surface enrichment coefficient Gamma should be much less than 0.23. And for calculation of soil losses on the cultivated land in the inter-gully area by using the Mass Balance Model II, the value of Gamma should be 0.05-0.1.     

Accumulation of Chernobyl-derived 137Cs in bottom sediments of some Finnish lakes

The amount and vertical distribution of Chernobyl-derived 137Cs in the bottom sediments of some Finnish lakes were studied. Sediment and surface water samples were taken in 2000 and 2003 from 12 stations in nine lakes and the results were compared with those obtained in corresponding surveys carried out in 1969, 1978, 1988 and 1990. Each of the five deposition categories of Chernobyl fallout in Finland were represented. The depth profiles of 137Cs in the sediments showed considerable variety in the lakes studied. The peak values varied between 1.5 and 46 kBq kg(-1) dry wt. The size and shape of the peak did not always correlate with the amount of deposition in the area, but on the other hand, reflected differences in sedimentation processes in different lakes. In some of the lakes the peak still occurred in the uppermost (0-2 cm) sediment layer, but in an extreme case the peak occurred at a depth of 22-23 cm corresponding to a sedimentation rate of 16 mm year(-1) during the 14 years after the Chernobyl accident. The total amounts of 137Cs in sediments varied from 15 to 170 kBq m(-2) at the sampling stations studied. Since 1990, the amounts have continued to increase slightly in two lakes, but started to decrease in the other lakes. In most of the lakes, the total amounts of 137Cs in sediments were about 1.5-2 times higher than in local deposition. In two lakes, the ratio was below 1, but in one case 3.2. Compared with the total amounts of 137Cs at the same stations in the late 1960s and 1970s, the values were now at their highest, at about 60-fold. The most important factors affecting 137Cs values in sediments were the local amount of deposition and the type of the lake and the sediment, but in addition, there were a number of other factors to be considered.     

A simplified 137Cs transport model for estimating erosion rates in undisturbed soil

(137)Cs is an artificial radionuclide with a half-life of 30.12 years which released into the environment as a result of atmospheric testing of thermo-nuclear weapons primarily during the period of 1950s-1970s with the maximum rate of (137)Cs fallout from atmosphere in 1963. (137)Cs fallout is strongly and rapidly adsorbed by fine particles in the surface horizons of the soil, when it falls down on the ground mostly with precipitation. Its subsequent redistribution is associated with movements of the soil or sediment particles. The (137)Cs nuclide tracing technique has been used for assessment of soil losses for both undisturbed and cultivated soils. For undisturbed soils, a simple profile-shape model was developed in 1990 to describe the (137)Cs depth distribution in profile, where the maximum (137)Cs occurs in the surface horizon and it exponentially decreases with depth. The model implied that the total (137)Cs fallout amount deposited on the earth surface in 1963 and the (137)Cs profile shape has not changed with time. The model has been widely used for assessment of soil losses on undisturbed land. However, temporal variations of (137)Cs depth distribution in undisturbed soils after its deposition on the ground due to downward transport processes are not considered in the previous simple profile-shape model. Thus, the soil losses are overestimated by the model. On the base of the erosion assessment model developed by Walling, D.E., He, Q. [1999. Improved models for estimating soil erosion rates from cesium-137 measurements. Journal of Environmental Quality 28, 611-622], we discuss the (137)Cs transport process in the eroded soil profile and make some simplification to the model, develop a method to estimate the soil erosion rate more expediently. To compare the soil erosion rates calculated by the simple profile-shape model and the simple transport model, the soil losses related to different (137)Cs loss proportions of the reference inventory at the Kaixian site of the Three Gorge Region, China are estimated by the two models. The over-estimation of the soil loss by using the previous simple profile-shape model obviously increases with the time period from the sampling year to the year of 1963 and (137)Cs loss proportion of the reference inventory. As to 20-80% of (137)Cs loss proportions of the reference inventory at the Kaixian site in 2004, the annual soil loss depths estimated by the new simplified transport process model are only 57.90-56.24% of the values estimated by the previous model.     

Sedimentation rates and trace metal input history in intertidal sediments from San Simón Bay (Ría de Vigo, NW Spain) derived from 210Pb and 137Cs chronology

(210)Pb and (137)Cs dating methods, accompanied by a high-resolution geochemical study, were applied to intertidal sediments containing both fine and coarse-grained particles and also, anthropogenic Pb in order to establish sedimentation rates and historical trends in heavy metal input. Sedimentation rates were established according to the "Constant Flux:Constant Sedimentation" (CF:CS) (210)Pb dating model, which was preferred rather than the "Constant Rate of Supply-Minimum Variance" (CRS-MV) model. Variations in sediment grain-size were accounted for by application of several normalization procedures. Al was selected for grain-size correction. Corrected sedimentation rates obtained from (210)Pb dating were corroborated through a second independent radionuclide tracer and by comparison of peak trace metal inputs into the environment with peaks in the sediment. The Chernobyl maximum was identified in the normalized (137)Cs activity profile. Sedimentation rates of 6.2+/-1.2 mm y(-1) and 3.1+/-0.5 mm y(-1) for the upper (two muddy layers) and 6.0+/-2.0 mm y(-1) for the lower (sandy) intertidal mud flat deposits of San Simón Bay were determined. According to the established chronology, human-induced environmental changes were detected in total metal concentrations (Cu, Pb, Zn) and in sediment grain-size and composition.     

Migration of Cs in tributaries,lake water and sediment of Lago Maggiore (Italy,Switzerland) – analysis and comparison with Lago di Lugano and other lakes

This paper describes the behaviour of ¹³⁷Cs in Lago Maggiore and other pre-alpine lakes as a consequence of atmospheric nuclear weapons testing fallout and the fallout from the nuclear accident in Chernobyl. It presents data on the ¹³⁷Cs distribution in tributaries, lake water, bottom sediments and reveals the role of ¹³⁷Cs as a marker of the sedimentation processes. The run-off of ¹³⁷Cs from the watershed to the lake is described with a simple compartment model. Measurements of the activity concentration of ¹³⁷Cs in sediments are compared with the output of a model (diffusion–convection type) which describes the input of ¹³⁷Cs into and its vertical distribution within the sediment. Varying sedimentation rates (0.05–0.90 g (cm² y)⁻¹) in Lago Maggiore are compared with data of other authors. Sedimentation rates and total distribution coefficients (of about 10⁵ L kg⁻¹) in Lago Maggiore are discussed and compared with those of Lago di Lugano, Lake Constance, and Lake Vorsee.     

Natural radionuclides and (137)Cs distributions and their relationship with sedimentological processes in Patras Harbour, Greece

Surficial and subsurficial sediment samples derived from gravity cores, selected from the harbour of Patras, Greece, were analyzed for grain size, water content, bulk density, specific gravity, organic carbon content and specific activities of natural radionuclides and (137)Cs. The specific activities of (232)Th, (226)Ra, (40)K and (137)Cs were measured radiometrically. The radionuclides (238)U and (232)Th were also analyzed using the INAA. The differences found between the specific activities of the natural radionuclides measured by the two methods are of no statistical significance. The sediment cores selection was based on a detailed bathymetric and marine seismic survey. Through the study of the detailed bathymetric map and the seismic profiles it was shown that ship traffic is highly influential to the harbour bathymetry. The granulometric and geotechnical properties of the sediments and therefore the specific activities of the natural radionuclides and (137)Cs seem to be controlled by the ship traffic. Relationship between radionuclide activity concentrations and granulometric/geotechnical parameters was defined after the treatment of all the analyses using R-mode factor analysis. The natural radionuclide activities are related to the fine fraction and bulk density of the sediments, while (137)Cs is mainly influenced by the organic carbon content. In addition, (238)U and (226)Ra seem to be in close relation with the heavy minerals fraction in coarse-grained sediments with high specific gravity.