Radionuclides in the Ecosystem of Lake Tygish in the Zone of the Eastern Ural Radioactive Trace

The radioecological situation in Lake Tygish is described. The lake is situated on the central axis of the Eastern Ural Radioactive Trace (EURT), which was formed after the nuclear accident in the Southern Urals in 1957. The distributions of ⁹⁰Sr and ¹³⁷Cs among the main components of the water body and the results of the measurement of tritium concentration in the water are presented. Mathematical models are described that have made it possible to estimate changes in the concentrations of radionuclides and their amounts accumulated in the water and bottom sediments of the lake during the long period after the accident and to predict the development of the radioecological situation in the lake until 2057. Based on the mathematical models, more accurate data on the initial ecological situation in the lake in the year of the accident have been obtained.     

Effect of liming on the behaviour of (90)Sr and (137)Cs in a lake ecosystem

Liming of lakes is considered one possible remedial action to reduce the accumulation of radionuclides into fish in the case of a radiological accident. These responses were tested in field conditions in a small acidified lake that was divided into two parts: one limed with CaCO₃ and the other half left as an unlimed control. The transfer of ⁹⁰Sr from water into fish decreased on average by 50% during the first year after liming. However, at the same time the ⁹⁰Sr concentration in water increased, reaching a maximum within 6 months after liming. Approximately 50% more ⁹⁰Sr was detected in water in the limed part of the lake than on control side during the first year. ⁹⁰Sr was most probably released from the sediment as the Ca concentration and pH of the water increased. As a result of these two processes, which counterbalanced each other (increased release of ⁹⁰Sr into water from sediment and decreased transfer of ⁹⁰Sr from water into fish), the ⁹⁰Sr concentration in fish did not notably differ between the limed and control sides of the lake. Liming may only be suitable as a remedial action if carried out immediately after a radiological accident, before significant amounts of radionuclides have been deposited in lake sediments. In the case of ¹³⁷Cs, the effect of liming was less pronounced. ¹³⁷Cs activity concentration in water increased in the first year by 20% and uptake by fish decreased by 20%.     

Radioecological investigation of the Techa-Iset' river system

Data on the current radioecological situation in the Techa-Iset' river system, which was contaminated by radioactive wastes from the Mayak Production Association in the 1940s and 1950s, are discussed. Mathematical models are presented that describe the decrease in the contamination of water, bottom sediments, hydrobionts, and floodplain soils with an increase in the distance from the discharge site. The amounts of⁹⁰Sr,⁹⁹Tc,¹³⁷Cs, and transuranium elements in the main components of the ecosystem are estimated.     

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.     

Model simulations of the fate of 14C added to a Canadian shield lake

Carbon-14 was added to the epilimnion of a small Canadian Shield lake to investigate primary production and carbon dynamics. The nature of the spike and subsequent monitoring allowed the investigation of both short-term and longer-term processes relevant to evaluating impacts of accidental and routine releases and of solid waste disposal. Data from this experiment were used in the BIOMOVS II program as a validation test for modelling the fate of the ¹⁴C added to the lake. Four models were used: (1) a simple probabilistic mass balance model of a lake; (2) a relatively complex deterministic model; (3) a complex deterministic model; and (4) a more complex probabilistic model. Endpoints were ¹⁴C concentrations in water, sediment and lake whitefish over a thirteen year period. Each model produced reasonable predictions when compared to the range of the observed data and when uncertainty in model predictions is taken into consideration. The simple lake model did not account for internal recycling of ¹⁴C and, in this respect, its predictions were not as realistic as those of the more complex models for concentrations in water. However, the simple model predictions for the ¹⁴C inventory remaining in lake sediment were closest to the observed values. Overall, the more complex probabilistic model was the most accurate in simulating ¹⁴C concentrations in water and in whitefish but it overestimated ¹⁴C retention in the lake sediments, as did the other complex models. Choice of parameter values for transfer rate to sediment and gaseous evasion are important in influencing model predictions. Although predicted concentrations of ¹⁴C in fish of dynamic models were more accurate than those using equilibrium bioconcentration factors typically used in assessments, large variability in observed ¹⁴C concentrations in whitefish emphasizes the need for a better understanding of the important processes that influence these contaminant concentrations.     

Chemical speciation of metals in sediment elutriates

Surface sediments from two localities in Lake Ontario (Hamilton Harbour and Portsmouth Harbour in Kingston, Ontario) were elutriated with lake water. The distribution of chemical species of metals (Fe, Cu, Ni, Pb, Mn, Cd, and Zn) and nutrients (N and P) was investigated in the elutriates and in the lake water by using the computer program geochem and separation by Chelex 100 resin. The concentration of Mn in the water increased from 10^?6.44M to 10^?5.09M during the elutriation of Lake Ontario sediments. The concentrations of other investigated metals were smaller and different in each of the elutriates. Both methods, the calculations by geochem and the separation by Chelex 100, showed that only Mn was present in the four elutriates as a free ion. However, the chemical speciation of other metals by these two methods was only partially similar. All four sediments released significant quantities of NH₃ which was associated in the elutriates mainly with H. The pH of the lake water decreased from 8.4 to 7.5 during the elutriation.     

On seasonal variations of radiocesium speciation in the surface sediments of Lake Juodis, Lithuania

Data on radiocesium speciation measured seasonally in black silt surface sediments in the shallow terrace and in the deepest southern part of Lake Juodis (Lithuania) in 2004-2005 are presented. It is shown that seasonal variations of radiocesium exchangeable fractions in the sediments in the shallow terrace are mainly related to its redistribution due to the vital cycle of green algae covering bottom surfaces - processes of their growth and decomposition. A seasonal course of those fractions in surface sediments of the deepest bottom areas of the lake follows a distinct pattern and is annually recycling. It is maximum in winter and declines due to stagnant bottom water zone disruption in summer. It is shown that surface sediments in the deepest bottom areas of the lake are not a radiocesium source during the formation of the anaerobic zone in bottom water in winter, and act in that case as its acceptor. The radiocesium remobilization to the bottom water is seasonal and site-specific. It is suggested to be due to three main processes: its diffusion from deeper and more active sediments, its redistribution during decomposition of organics freshly accumulated in surface sediments and a radiocesium flux induced by the mechanism of the seasonal anaerobic zone formation in near-bottom water.     

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.     

Distribution and hydrodynamic model of the Keumdong oil spill in Kwangyang Bay, Korea

Oil concentrations in the seawater, seabed sediments, and shoreline sediments were measured from the samples collected 165 days after the Keumdong oil spill accident, which had occurred in Kwangyang Bay of the South Sea, Korea in September 1993. Distribution patterns of the concentrations in the seabed and shoreline sediments have allowed us to hindcast the transport and fate of the spilled oil. Overall, the patterns agree better with the southward (seaward) surface water circulation than with the northward (landward) bottom water circulation over the region. Rapid, initial dispersal of the spilled oil to the south and its subsequent grounding onto the intertidal seabed sediments, as well as onto the shorelines, appear to have made ineffective the subsurface oil transport by the bottom current.     

Cs,Pu and Am in bottom sediments and surface water of Lake Päijänne,Finland

The concentrations and vertical distribution of ^239,240Pu, ²⁴¹Am and ¹³⁷Cs in the bottom sediments and water samples of Lake Päijänne were investigated. This lake is important, since the Päijänne area received a significant deposition from the Chernobyl fallout. Furthermore Lake Päijänne is the raw water source for the Helsinki metropolitan area. In addition no previous data on the distribution of plutonium and americium in the sediment profiles of Lake Päijänne exist. Only data covering the surface layer (0–1 cm) of the sediments are previously available. In the sediments the average total activities were 45 ± 15 Bq/m² and 20 ± 7 Bq/m² for ^239,240Pu and ²⁴¹Am, respectively. The average ²⁴¹Am/^239,240Pu ratio was 0.45 ± 0.14. The ²⁴¹Am/^239,240Pu ratio is lowest in the surface layer of the sediments and increases as a function of depth. The ²³⁸Pu/^239,240Pu ratio of the sediment samples varied between 0.012 ± 0.025 and 0.162 ± 0.079, decreasing as a function of depth. The average activity in water was 4.9 ± 0.9 mBq/m³ and 4.1 ± 0.2 mBq/m³ for ^239,240Pu and ²⁴¹Am, respectively. The ²⁴¹Am/^239,240Pu ratio of water samples was 0.82 ± 0.17. ^239,240Pu originating from the Chernobyl fallout calculated from the average total activities covers approximately 1.95 ± 0.01% of the total ^239,240Pu activity in the bottom sediments. The average total ¹³⁷Cs activity of sediment profiles was 100 ± 15 kBq/m² and 19.3 ± 1.4 Bq/m³ in water samples.     

Sediment problems and lake restoration in Wisconsin

Twelve dredging projects are underway or will soon begin in Wisconsin. These include both natural and man-made lakes, with lake size and sediment removal up to 205 ha and 1,720,250 m³, respectively. Solids content of the sediments ranges from 70%–80% to 1%–5%. The projects were designed using a mixture of on-site data collection, predictive models, and professional judgement. Sediment disposal has limited project implementation, with arsenic being a special problem. Theoretically, sediment concentrations below 4 μg/g could still produce unacceptable contamination of groundwater at the disposal site. One project is being held up, pending completion of laboratory testing. Organic sediments from Lilly Lake were deposited in an active gravel pit and within diked areas on agricultural land. Passage through a spray irrigation system proved impractical. Rapid infiltration of water into the bottom and sides of the settling basins was short-lived due to the self-sealing characteristics of these sediments. Studies are now underway to determine the effect of lake sediment application to upland soils on corn production.     

Association of organic matter, iron and inorganic phosphorus in lake waters

Gel permeation chromatography was used to fractionate ³²PO₄³⁻ labelled components by molecular size in filtered, destabilized lake foam, concentrated lake water, and lake sediment extracts. Evidence is presented for the abiotic formation of organic matter iron inorganic P complexes in lake foam, water and sediments. ³²PO₄^staggered was found to excahnge with low molecular weight, dissolved P fraction, probably an organic matter -Fe- inorganic P complex, but not with a high molecular weight, non-inorganic dissolved reactive P pool, hypothesized to be similar to the dimer. Our experiments suggest that inorganic P binding by high molecular weight organic matter may play a significant role in the P cycle. If the bound P is unavailable to algae and bacteria, the complexes could explain Rigler's (1968) hypothesis that the molybdenum blue technique may overestimate the free orthophosphate concentration by 10–100 times.     

Disequilibrium between uranium and its progeny in the Lake Issyk-Kul system (Kyrgyzstan) under a combined effect of natural and manmade processes

The Kadji-Sai abandoned field of U-bearing brown coal on the southern coast of Lake Issyk-Kul (Kyrgyzstan) poses a threat of radioactive pollution to the world's fifth deepest and second largest pristine highland lake. The valleys of ephemeral streams in the lake catchment are filled with coarse-grained sand and clay, with a background U--Ra activity of 35--55 Bqkg(-1). High activity areas vs. this background come from three sources: (1) scarce outcrops of uraniferous brown coal and mining wastes containing fragments of this coal with (238)U/(226)Ra ratios of 0.8 due to uranium losses through weathering; (2) manmade anomalies caused by a radioactive waste dump, where U was extracted from the ash of coal burnt at a coal-fired power plant. As a result, the (238)U/(226)Ra ratios become 0.15--0.25; (3) six catch pools terraced below the mine, where U activity decreases downslope, and (238)U/(226)Ra ratios reach 150--200. Uranium lost in the extraction process may have been retained on the terraces. The distribution pattern of radionuclides in the bottom sediments of the lake is controlled by water depth and offshore distance. The upper section of homogeneous limy--argillic deposits in the lake center remains undisturbed by currents, as indicated by regular sub-exponential distribution of atmospheric (137)Cs and (210)Pb(atm). Sedimentation rate in the lake center for the past century, found from (210)Pb, was 0.32 mmyr(-1). (238)U/(226)Ra in deep-water sediments was about 3. The activity of uranium adsorbed by sediments from the lake water was estimated by subtraction of the Ra-equilibrium component from the total U activity. Thus, the flux of dissolved U to the bottom sediments was as 2.07 x 10(-7)gcm(-2)yr(-1). The upper section of near-shore deposits was disturbed by currents, with (137)Cs and (210)Pb(atm) more or less uniformly distributed in this layer. Peaks of (226)Ra and (210)Pb occur at different depths from 5 to 20 cm below the sediment surface, with (238)U/(226)Ra ratios 0.28--0.44. The presence of mullite in these sediments indicated that radioactive ash penetrated into the lake in the past. At present, (226)Ra in the ash is buried under a non-radioactive cap.     

Ra–Po–Pb isotope systematics in waters of Sambhar Salt Lake,Rajasthan (India): geochemical characterization and particulate reactivity

The Sambhar Salt Lake hydrological system, including river waters, groundwaters, evaporating pans and sub-surface brines, has been analyzed for the salt content (TDS) and naturally occurring radionuclides (²¹⁰Po, ²¹⁰Pb and ^226,228Ra). The abundance of these radionuclides and their activity ratios show a wide variation in different hydrological regimes, which helps to geochemically characterize the lake system. A significantly lower Ra to total dissolved solids (TDS) ratio in the brines (by two to three orders of magnitude), when compared to the groundwaters and river waters, suggests removal of dissolved Ra by co-precipitation with Ca–Mg minerals at an early stage of the brine evolution. The concentration of Ra in evaporating lake/pan waters saturates at a value of about 35 Bq L⁻¹ over the salinity range of 100–370 g L⁻¹; attributable to its equilibration with the clay minerals. The two distinct regimes, saline lake system (lake water, evaporating pans and sub-surface brines) and groundwaters have been identified based on their differences in the distribution of ^226,228Ra isotopes. This observation points to the conclusion that the groundwaters and the lake brines are not intimately coupled in terms of their origin and evolution. The abundances of ²¹⁰Po and ²¹⁰Pb along with their activity ratios (²¹⁰Po/²¹⁰Pb) are markedly different among the surface lake waters/evaporating pans, sub-surface lake brines and groundwaters. These differences are explained in terms of different geochemical behaviour of these nuclides in presence of algae and organic matter present in these water regimes.     

Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005

A radioactivity survey was launched in 1991 to determine the background levels of ^239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ^239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ^239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ^239+240Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ^239+240Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.     

Fuel particles in the Chernobyl cooling pond: current state and prediction for remediation options

During the coming years, a management and remediation strategy for the Chernobyl cooling pond (CP) will be implemented. Remediation options include a controlled reduction in surface water level of the cooling pond and stabilisation of exposed sediments. In terrestrial soils, fuel particles deposited during the Chernobyl accident have now almost completely disintegrated. However, in the CP sediments the majority of ⁹⁰Sr activity is still in the form of fuel particles. Due to the low dissolved oxygen concentration and high pH, dissolution of fuel particles in the CP sediments is significantly slower than in soils. After the planned cessation of water pumping from the Pripyat River to the Pond, significant areas of sediments will be drained and exposed to the air. This will significantly enhance the dissolution rate and, correspondingly, the mobility and bioavailability of radionuclides will increase with time. The rate of acidification of exposed bottom sediments was predicted on the basis of acidification of similar soils after liming. Using empirical equations relating the fuel particle dissolution rate to soil and sediment pH allowed prediction of fuel particle dissolution and ⁹⁰Sr mobilisation for different remediation scenarios. It is shown that in exposed sediments, fuel particles will be almost completely dissolved in 15–25 years, while in parts of the cooling pond which remain flooded, fuel particle dissolution will take about a century.     

Application of the ERICA Assessment Tool to freshwater biota in Finland

In recent years there has been growing international interest in the assessment of doses and risks from ionising contaminants to biota. In this study the ERICA Tool, developed within the EC 6th Framework Programme, was applied to estimate incremental dose rates to biota in freshwater ecosystems in Finland mainly resulting from exposure to the Chernobyl-derived radionuclides ¹³⁷Cs, ¹³⁴Cs and ⁹⁰Sr. Data sets consisting of measured activity concentrations in fish, aquatic plants, lake water and sediment for three selected lakes located in a region with high ¹³⁷Cs deposition were applied in the assessment. The dose rates to most species studied were clearly below the screening level of 10 μGy h⁻¹, indicating no significant impact of the Chernobyl fallout on these species. However, the possibility of higher dose rates to certain species living on or in the bottom sediment cannot be excluded based on this assessment.     

On the radiocesium carbonate barrier in organics-rich sediments of Lake Juodis, Lithuania

Radiocesium vertical profiles in organics-rich sediments of running shallow eutrophic Lake Juodis (Lithuania) were studied in relation to seasonal variations of vertical profiles (in water column and sediments) of standard variables (pH, redox potential, temperature, oxygen concentrations, conductivity). It is shown that the sedimentation rate, radiocesium mobility and its vertical profiles in sediments are controlled by the vital cycle (processes of the growth, accumulation and decomposition) of green algae covering the main bottom areas of the lake. It is also shown that calcite deposits are formed in the shallow bottom areas that are oxygenated throughout the year because of the photosynthetic activity of the green algae covering the sediment. Formation of the calcite coatings on freshly accumulated organics is remarkable for causing elevated densities of sediment solids in the upper part of the respective vertical profiles. These calcite deposits behave as a barrier for radiocesium backward flux to the bottom water making the respective bottom areas a radionuclide sink. Together with the jelly-structured sediments lying below these deposits, the calcite preserves the shape of the primary radiocesium vertical profiles formed due to free-ion diffusion after the deposition event. It was determined that bottom areas anaerobic in winter are the main radiocesium source in the water column and cause characteristic radiocesium redistribution in surface sediments.     

Upward movement of plutonium to surface sediments during an 11-year field study

An 11-year lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The ²⁴⁰Pu/²³⁹Pu and ²⁴²Pu/²³⁹Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments.     

Characterization of plutonium in deep-sea sediments of the Sulu and South China Seas

Anthropogenic Pu isotopes are important geochemical tracers for sediment studies. Their distributions and sources in the water columns as well as the sediments of the North Pacific have been intensively studied; however, information about Pu in the Southeast Asian seas is limited. To study the isotopic composition of Pu, and thus to identify its sources, we collected sediment core samples in the South China Sea and the Sulu Sea during the KH-96-5 Cruise of the R/V Hakuho Maru. We analysed the activities of ^239+240Pu and the atom ratios of ²⁴⁰Pu/²³⁹Pu using isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The ²⁴⁰Pu/²³⁹Pu atom ratios in the sediments of both areas (inventory weighted mean: 0.251 for the South China Sea and 0.280 for the Sulu Sea) were higher than the global fallout value (0.178 ± 0.019), suggesting the existence of Pu from the Pacific Proving Grounds in the North Pacific. Low inventories of ^239+240Pu in sediments were observed in the South China Sea (3.75 Bq/m²) and the Sulu Sea (1.38 Bq/m²). Most of the Pu input is still present in the water column. Scavenging and benthic mixing processes were considered to be the main processes controlling the distribution of Pu in the deep-sea sediments of both study areas.