A 10-year study of the 137Cs distribution in soil and a comparison of Cs soil inventory with precipitation-determined deposition

During a 10-year period, 1988-1998, surface soil samples have been collected at Blentarp in southern Sweden and analysed for 137Cs from the Chernobyl accident and from the nuclear weapons tests. The distance between the sampling plots on the different sampling occasions has been no more than 3 m. The results show that the depth distribution of 137Cs is very similar for each of the sampling occasions, indicating that the caesium migration at this site is very small. The total activity measured in the soil cores is in agreement with the calculated activity of 137Cs deposited at the site after nuclear weapons tests and the Chernobyl accident, based on air activity concentration and the amount of precipitation. The calculated deposition of 137Cs originating from the bomb tests amounts to 1.41 kBq m-2 for the period 1962-1986, which is in agreement with the activity of nuclear weapons fallout measured in the soil samples (1.60 kBq m-2 as a mean value of the first four years of sampling). The calculated activity of 137Cs of Chernobyl origin was 0.79 kBq m-2, which agrees well with the value of 0.79 kBq m-2 measured in the soil samples in 1988.     

Contamination of Austrian soil with caesium-137

Austria ranks among the countries that have been most strongly affected by the Chernobyl fallout. The mean contamination with 137Cs is 21.0 kBq/m2, of which 18.7 kBq/m2 is due to the Chernobyl accident, whereas global fallout contributes 2.3 kBq/m2. Maximum values of total 137Cs contamination are nearly 200 kBq/m2. Total deposition of Chernobyl 137Cs on Austrian territory is 1.6 PBq or a fraction of around 2% of the 137Cs released from the reactor. 2115 measurements were used to draw the Austrian "caesium map". The geographical pattern of fallout distribution shows regional differences of contamination as high as 1:100.     

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.     

Post-depositional redistribution and gradual accumulation of 137Cs in a riparian wetland ecosystem in Sweden

After the Chernobyl accident, high activity concentrations of (137)Cs (>1 MBq m(-2)) were detected in a riparian swamp in the central-eastern part of Sweden. The objective of this study was to clarify the redistribution processes behind the accumulation of (137)Cs in the wetland. A mass balance budget of (137)Cs was calculated based on soil and sediment samples and reports in the literature. Results showed that accumulation occurred over several years. Of all the (137)Cs activity discharged between 1986 and 2002 from the upstream lake, 29% was estimated to be retained in the wetland. In 2003, measurements showed that 17 kBq m(-2) sedimented on the stream banks of the wetland. Continuing overbank sedimentation by spring flooding prolongs the time that the wetland will contain high activity concentrations of (137)Cs. Consequently, organisms living in wetlands serving as sinks for (137)Cs may become exposed over long time periods to high activity concentrations.     

Discharge of 137Cs and 90Sr by Finnish rivers to the Baltic Sea in 1986-1996

The total amounts of 137Cs and 90Sr transported from Finland by rivers into the Gulf of Finland, Gulf of Bothnia and Archipelago Sea since 1986 were estimated. The estimates were based on long-term monitoring of 137Cs and 90Sr in river and other surface waters and on the statistics of water discharges from Finnish rivers to the above sub-areas of the Baltic Sea. The total amounts of 137Cs and 90Sr removed from Finland into the Baltic Sea during 1986-1996 were estimated to be 65 and 10 TBq, respectively. The results show that, although the deposition of 137Cs was much higher than that of 90Sr after the Chernobyl accident, the amount of 137Cs removed from Finland is only six times as high as that of 90Sr. This emphasizes the importance of 90Sr while considering radiation doses from surface waters and 137Cs while estimating doses via pathways from catchment soil, lake sediments and biota after a fallout situation.     

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.     

137Cs and 90Sr transfer to milk in Austrian alpine agriculture

The alpine regions of Austria were among the most contaminated territories outside of the former USSR after the Chernobyl accident. In the investigated province of Salzburg the median (137)Cs surface deposition was 31.4 kBq m(-2) with maximum values exceeding 90 kBq m(-2) (May 1986). To quantify the transfer of (137)Cs and (90)Sr from vegetation to milk in these seminatural conditions nine seasonally grazed alps were identified and vegetation and milk sampled during summer 2002 and summer 2003. Mean+/-SD milk transfer coefficients (fm) for (137)Cs and (90)Sr were 0.0071+/-0.0009 d l(-1), and 0.0011+/-0.0004 d l(-1), respectively; which for (137)Cs is markedly higher than those fm values found in intensive agricultural systems. Transfer kinetics for (137)Cs into cow milk were approximated using a 2-compartment model with a short and a long-term component. Fitting the model to empirical data results in reliable estimates of the time constant of the short-term component, biological half-life 1.06+/-0.28 d, whereas the estimates of the long-term component are subject to high uncertainties.     

Radionuclide tracing of water masses and processes in the water column and sediment in the Algerian Basin

Caesium-137 and (239,240)PU were analysed in the water column along the Algerian coast. The (137)Cs activity concentration in surface water increased from the west to the east from 1.6 to 3.3 mBq L(-1), documenting a presence of Modified Atlantic Water (MAW) in the region. Higher concentrations observed in deep waters may be due to an intrusion of Levantine Intermediate Water (LIW), which has been carrying higher levels of (137)Cs from Chernobyl accident. The (239,240)Pu sub-surface concentration peaked at about 250 m water depth as a result of biogeochemical processes in the water column. The observed (239,240)Pu/(137)Cs activity ratio at the surface (0.003) was significantly lower than that in global fallout (0.04). This decrease exceeds that expected from radioactive decay of (137)Cs, and confirms that Pu due to its adsorption on sinking particles is more effectively removed from surface layers than is (137)Cs. An increase of the (239,240)Pu/(137)Cs activity ratio with depth suggests that (239,240)Pu, similarly as (137)Cs, should be also transported by advection to maintain the observed ratios in deep waters. An intrusion of LIW may enhance therefore both the (137)Cs and (239,240)Pu concentrations in deep waters. The average (238)Pu/(239+240)Pu activity ratio in seawater was 0.03+/-0.02, confirming a global fallout origin of Pu in the Algerian Basin. Caesium-137 and (239,240)Pu inventories in the water column were estimated to be from 2.7+/-0.5 kBq m(-2) to 3.8+/-0.7 kBq m(-2), and from 13.8+/-2.6 Bq m(-2) to 41+/-7B qm(-2), respectively. The (137)Cs massic activities in surface sediment were almost constant, the average activity was 9.0+/-0.8 Bq kg(-1). Sedimentation rates obtained using the (210)Pb method were from 0.1 to 0.7 cm y(-1), and resulting penetration depths of (137)Cs in the sediment cores were from 15 to over 40 cm. The (137)Cs peaks found in the sediment cores were associated with the Chernobyl accident (1986) and global fallout (1964). The (137)Cs inventories in the sediment were increasing from the west (180 Bq m(-2)) to the east (350 Bq m(-2)).     

Lake fish as the main contributor of internal dose to lakeshore residents in the Chernobyl contaminated area

Two field expeditions in 1996 studied 137Cs intake patterns and its content in the bodies of adult residents from the village Kozhany in the Bryansk region, Russia, located on the shore of a drainless peat lake in an area subjected to significant radioactive contamination after the 1986 Chernobyl accident. The 137Cs contents in lake water and fish were two orders of magnitude greater than in local rivers and flow-through lakes, 10 years after Chernobyl radioactive contamination, and remain stable. The 137Cs content in lake fish and a mixture of forest mushrooms was between approximately 10-20 kBq/kg, which exceeded the temporary Russian permissible levels for these products by a factor of 20-40. Consumption of lake fish gave the main contribution to internal doses (40-50%) for Kozhany village inhabitants Simple countermeasures, such as Prussian blue doses for dairy cows and pre-boiling mushrooms and fish before cooking, halved the 137Cs internal dose to inhabitants, even 10 years after the radioactive fallout.     

137Cs in freshwater fish in Finland since 1986--a statistical analysis with multivariate linear regression models

The accident at the Chernobyl nuclear power plant in 1986 significantly elevated the 137Cs levels of fish in Finnish lakes. About 6200 fish samples from 390 lakes comprising 20 species have been analysed for 137Cs since 1986. The sizes of the lakes varied from a few hectares to about 1000 km2. Activity concentrations of 137Cs in fish still varied widely in 2003, from 16 to 6400 Bq/kg fresh weight. This paper presents the results of statistical analyses with multivariate linear regression models carried out on the empirical data collected since 1986. The statistical analysis resulted in separate models for two time periods describing temporal changes of 137Cs in fish. The explanatory variables were fish species with various feeding habits, the size class of the lake, municipal division, drainage area, time since the deposition and deposition level of the municipality. The calculated values for 137Cs in fish did not differ statistically significantly from the observed values in the validation data. The explanatory variables explained 58% (the first time period) and 72% (the second time period) of the total variability of 137Cs in fish.     

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.     

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.     

Modelling the long-term dynamics of radiocaesium in closed lakes

During the years after the Chernobyl accident the radioceasium activity concentration in most contaminated aquatic ecosystems decreased markedly. Lakes with no permanent inflows and outflows (closed lakes), however, still present a radioecological problem which is expected to continue for some time. In this paper, a mechanistic model for the long-term prediction of radiocaesium behaviour in closed lakes is developed. The model of Prokhorov (Radiokhimiya (Radiochemistry) 11 (1969) 317) was modified to describe the effects of bottom sediment bioturbation, surface runoff from the catchment and suspended solids formation and sedimentation. The model input parameters are the effective diffusion coefficient in bottom sediments, depth of the completely mixed layer, the distribution coefficient in the sediment-water system, the runoff coefficient, sedimentation rate, and deposition density. Values of all these parameters can be independently estimated or measured in a short-term experiment. Given negligible runoff and sedimentation, the dynamics of radiocaesium in lake water is described by a simple equation with only one unknown parameter. This allows us to make long-term predictions on the basis of a series of measurements carried out during the relatively short period. The model was tested against 137Cs activity concentrations measured between 1993 and 1999 in Svyatoe lake in the Bryansk region of Russia. Calculated and measured activity concentrations are in good agreement.     

Long-term studies on transfer of 137Cs from soil to vegetation and to grazing lambs in a mountain area in northern Sweden

Studies were made during 1990-1997 on the transfer of 137Cs from soil to vegetation (herbage) and to grazing lambs on a mountain farm with an uncultivated grazing area of about 10 km2. The farm is situated in an area in Northern Sweden which was contaminated by the Chernobyl fallout in 1986. The mean concentration of 137Cs in the soil to a depth of 10 cm for eight sampling sites observed in the 8-year period was 14.51 kBq/m2, while in the cut herbage the average concentration was 859 Bq/kg d.w. and in lamb meat 682 Bq/kg w.w. A slow vertical migration of 137Cs in the 0-10 cm soil layer was indicated. Although the 137Cs concentration in herbage gradually decreased, the concentration in lamb meat varied from year to year. Soil ingestion by the lambs as a pathway for activity transfer was shown to be negligible, while ingestion of fungi with high concentrations of 137Cs was demonstrated to occur, as large numbers of fungi spores were counted in samples of the lambs' faeces. Fungi ingestion might therefore partly explain the varying mean yearly 137Cs concentrations in lamb muscle. The mean transfer parameters were as follows: for "soil to herbage" 61.3 Bq/kg d.w. herbage per kBq/m2 soil, for "herbage to lamb meat" 0.81 Bq/kg w.w. meat per Bq/kg d.w. herbage, and for "soil to lamb meat" 47.1 Bq/kg w.w. meat per kBq/m2 soil. A trend of decreasing values of the transfer parameter for "soil to herbage" indicated that 137Cs was becoming less available for root-uptake with time. The effective ecological half-life of 137Cs in soil, herbage and lamb meat was calculated to be 19, 7 and 16 years, respectively. It can be concluded that natural areas are vulnerable to 137Cs contamination, resulting in high concentrations in plants, fungi and lamb meat for a long time.     

长江中下游湖泊沉积速率的测定及环境意义——以洪湖、巢湖、太湖为例

对长江中下游洪湖、巢湖和太湖沉积物采用210Pb和137Cs相结合的方法测定沉积速率。洪湖钻孔中210Pbex随深度的增加没有呈现指数衰减分布,因此获得的平均沉积速率并不可靠;而根据137Cs蓄积峰计算得出洪湖钻孔在1963~1986年沉积速率最大,这可能是因为当时大规模开垦导致湖区周围水土流失,大量的侵蚀物质被带入湖中,从而导致沉积速率上升。对巢湖钻孔用210Pb法和137Cs得到的沉积速率具有可比性,研究发现20世纪70年代以来随着深度的减少,巢湖钻孔中沉积通量在增加,说明巢湖流域内水土流失逐步加重,可能与土地开发、植被破坏等人为活动有关。对太湖钻孔利用137Cs 1963年对应的蓄积峰进行校正,采用210Pb计年的CRS模式获得不同时段的沉积速率发现在80年代末尾沉积物堆积通量最高,达到0.6 g·cm-2·a-1。两种计年方法的结合有助于认识沉积速率的变化情况。     

Geographical mapping and associated fractal analysis of the long-lived Chernobyl fallout radionuclides in Greece

Immediately after the Chernobyl accident, a soil sampling programme was undertaken in order to detect and quantitatively analyse the long-lived radionuclides in the Chernobyl fallout. Soil samples (1242 in number) of 1 cm thick surface soil were collected in Greece during the period from May-November 1986. The samples were counted and analysed using Ge detector set-ups. The 137Cs fallout data have already been analysed, mapped and published. In an attempt to improve this analysis and also to extent it to other fallout radionuclides, an in-house unix-based data base/geographical information system (DBGIS) was developed. Multifractal analyses of the deposition patterns have also been performed. In the present work, an analysis of the results of the deposition of 137Cs, 134Cs, 144Ce, 141Ce, 125Sb, 110mAg, 106Ru, 103Ru, 95Zr and 54Mn are presented together with relevant fractal analysis and three characteristic contour maps. The maximum detected values of the above-mentioned radionuclides were 149.5 +/- 0.1, 76.1 +/- 0.1, 32.9 +/- 0.2, 46 +/- 2, 4.56 +/- 0.02, 7.98 +/- 0.02, 79.1 +/- 0.4, 337 +/- 2, 20.1 +/- 0.2 and 3.02 +/- 0.02 kBq m-2, respectively. Furthermore, a statistical technique to compare contour maps was introduced and applied to explain the differences which appeared in the maps of the above-mentioned radionuclides.     

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.     

Short- and long-term patterns of ¹³⁷Cs in fish and other aquatic organisms of small forest lakes in southern Finland since the Chernobyl accident

We summarize the patterns of ¹³⁷Cs activity concentrations and transfer into fish and other biota in four small forest lakes in southern Finland during a twenty-year period following the Chernobyl accident in April 1986. The results from summer 1986 showed fastest accumulation of ¹³⁷Cs into planktivorous fishes, i.e. along the shortest food chains. Since 1987, the highest annual mean values of ¹³⁷Cs have been recorded in fish occupying the highest trophic levels, for perch (Perca fluviatilis) 13,600 Bq/kg (ww) and for pike (Esox lucius) 20,700 Bq/kg (ww). At the same time, activity concentrations of ¹³⁷Cs in crustacean zooplankton and Asellus aquaticus have ranged between 1000 and 19,500 Bq/kg (dw). In 2006, 5-28% of the 1987 ¹³⁷Cs activity concentration levels were still present in perch and pike. Since 1989 their ¹³⁷Cs activity concentrations in oligohumic seepage lakes have remained significantly higher than in polyhumic drainage lakes due to the increased transfer of ¹³⁷Cs into fish in the seepage lakes with lower electrolyte concentrations, longer water retention times and lower sedimentation rate.     

Deposition and distribution of Chernobyl fallout fission products and actinides in a Russian soil profile

In this article the distribution of fission products and actinides in a soil profile from Novo Bobovicky in Russia, which was contaminated due to the Chernobyl nuclear power plant accident, is described. The ground deposition of long-lived fission products determined by gamma-spectrometry was (recalculated to 26 April 1986) 1600 kBq (137)Cs/m(2), 900 kBq (134)Cs/m(2) and 60 kBq (125)Sb/m(2). Of these radionuclides (137)Cs shows the dominating activity at the present time. After 6.5 years 90% of the Cs and Sb activity was contained in the upper 4 cm. A (239,240)Pu ground deposition of 77.4+/-8.0 Bq/m(2) was determined by alpha-spectrometry. The (238)Pu/(239,240)Pu activity ratio of 0.30+/-0.03 and (241)Pu/(239,240)Pu activity ratio of 115+/-14 (in 1986) measured in the soil profile, indicates that the analysed Pu originates mainly from the Chernobyl accident. The average (234)U/(238)U activity ratio of 1.06+/-0.29 indicates that the uranium in this soil is dominated by naturally occurring uranium.The alpha- and beta-autoradiography revealed that the activity is mainly present in particulate form. It could further be observed that the spots containing alpha- or beta-activity originated from different particles. A comparison of alpha-autoradiography with the bulk Pu and Am activity showed that 92% of the alpha-activity was present as clearly detectable alpha-spots.The beta-active particles, located by beta-autoradiography were correlated with gamma-spectrometric measurements and contained only (137)Cs. These hot spots ranged from 0.02 to 0.15 Bq.It could be concluded that the vertical transport of (137)Cs and fuel fragments occurs mainly by movement of particles through the soil. It could also be concluded that the fuel fragments found, in this soil were depleted in respect to Cs, Sb and Eu.Comparison of the analysed (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu ratios with the ratios calculated with ORIGEN-S code gave an estimate of the average burn-up of the fuel particles to be in the range of 11-12 GWd/tU.The results presented in this article are valid for this single soil profile and should not be generalised unless validated in a more rigorous study of a larger number of soil profiles.     

Hot particles of the Yenisei River flood plain, Russia.

Some high-activity hot particles (HP) were found in the flood plain of the Yenisei River, near the Krasnoyarsk Mining-and-Chemical Combine (MCC), and their radionuclide compositions were determined. The ratios of plutonium and caesium isotopes in the particles are indicative of their reactor origin. The 137Cs activity of the particles amounts to 29,200 kBq/particle, which is higher than the corresponding activities of the fuel particles that formed as a result of the accident at the Chernobyl NPP. All the particles have been divided into two major groups according to the 137Cs/34Cs ratio: in the first group, the 137Cs/134Cs ratio is more than or equal to 3000, and in the second the 137Cs/134Cs ratio is less than or equal to 1000. The particles of the first and the second groups were preliminarily estimated to be formed 30 and 20 years ago, which suggests that there must have been at least two accidents at the MCC reactors, with part of the fuel released into the Yenisei River.