Modeling of Cs migration in soils using an 80-year soil archive: role of fertilizers and agricultural amendments

An 80-year soil archive, the 42-plot experimental design at the INRA in Versailles (France), is used here to study long-term contamination by ¹³⁷Cs atmospheric deposition and the fate of this radioisotope when associated with various agricultural practices: fallow land, KCl, NH₄(NO₃), superphosphate fertilizers, horse manure and lime amendments. The pertinence of a simple box model, where radiocaesium is supposed to move downward by convectional mechanisms, is checked using samples from control plots which had been neither amended, nor cultivated since 1928. This simple model presents the advantage of depending on only two parameters: α, a proportional factor allowing the historical atmospheric ¹³⁷Cs fluxes to be reconstructed locally, and k, an annual loss coefficient from the plow horizon. Another pseudo-unknown is however necessary to run the model: the shape of historical ¹³⁷Cs deposition, but this function can be easily computed by merging several curves previously established by other surveys. A loss of ∼1.5% per year from the plow horizon, combined with appropriate fluxes, provides good concordance between simulated and measured values. In the 0–25 cm horizon, the residence half time is found to be ∼18 yr (including both migration and radioactive decay). Migration rate constants are also calculated for some plots receiving continuous long-term agricultural treatments. Comparison with the control plots reveals significant influence of amendments on ¹³⁷Cs mobility in these soils developed from a unique genoform.     

Sources and distributions of Cs, Pu, Pu radionuclides in the north-western Barents Sea

Sediment deposits are the ultimate sink for anthropogenic radionuclides entering the marine environment. The major sources of anthropogenic radionuclides to the Barents Sea are fallout from nuclear weapons tests, long range transport from other seas, and river and non-point freshwater supplies. In this study we investigated activity concentrations, ratios, and inventories of the anthropogenic radionuclides, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu in dated sediment cores collected along a north-south transect in the northwestern Barents Sea. The data were used to evaluate the influence of different sources on the derived spatial and temporal patterns of anthropogenic radionuclides in seafloor sediment deposits. Activity concentrations of ¹³⁷Cs ranged from <0.1 Bq/kg to 10.5 Bq/kg while ^239,240Pu ranged from <0.01 Bq/kg to 2.74 Bq/kg and ²³⁸Pu activity concentrations ranged from <0.01 Bq/kg to 0.22 Bq/kg. Total inventories of ¹³⁷Cs ranged from 29.5 ± 1.5 Bq/m² to 152.7 ± 5.6 Bq/m² and for ^239,240Pu inventories (6 sediment layers only) ranged from 9.5 ± 0.3 Bq/m² to 29.7 ± 0.4 Bq/m². Source contributions varied among stations and between the investigated radionuclides. The ²³⁸Pu/^239,240Pu ratios up to 0.18 indicate discharges from nuclear fuel reprocessing plants as a main contributor of plutonium. Based on ²³⁸Pu/^239,240Pu ratio, it was calculated that up to 19-27% of plutonium is supplied from sources other than atmospheric global fallout. Taking into account Atlantic current flow trajectories and that both activity concentrations and inventories of plutonium negatively correlate with latitude, Sellafield is a major source for the Barents Sea. Concentrations and inventories of ¹³⁷Cs correlate positively with latitude and negatively with distance from the Svalbard archipelago. The ¹³⁷Cs concentrations are highest in an area of intensive melting of sea ice formed along the Siberian coast. Thus, sea ice and supplies from Svalbard may be important source of ¹³⁷Cs to the Barents Sea seafloor.     

Plant uptake of radiocaesium from artificially contaminated soil monoliths covering major European soil types

Uptake of ¹³⁷Cs was measured in different agricultural plant species (beans, lettuce, barley and ryegrass) grown in 5 undisturbed soil monoliths covering major European soil types. The first cultivation was made three years after soil contamination and plants were grown during 3 successive years. The plant–soil ¹³⁷Cs transfer factors varied maximally 12-fold among soils and 35-fold among species when grown on the same soil. Single correlations between transfer factors and soil properties were found, but they varied widely with plant type and can hardly be used as a predictive tool because of the few soils used. The variation of ¹³⁷Cs concentrations in plants among soils was related to differences in soil solution ¹³⁷Cs and K concentrations, consistent with previous observations in hydroponics and pot trials. Absolute values of transfer factors could not be predicted based on a model validated for pot trials. The ¹³⁷Cs activity concentration in soil solution decreased significantly (11- to 250-fold) for most soils in the 1997–1999 period and is partly explained by decreasing K in soil solution. Transfer factors of lettuce showed both increasing and decreasing trends between 2 consecutive years depending on soil type. The trends could be explained by the variation in ¹³⁷Cs and K concentrations in soil solution. It is concluded that differences in ¹³⁷Cs transfer factors among soils and trends in transfer factors as a function of time can be explained from soil solution composition, as shown previously for pot trials, although absolute values of transfer factors could not be predicted.     

Diet monitoring for assessment of human exposure to environmental pollutants

Daily intake of lead, cadmium, aluminium, radiocaesium, DDT and metabolites, and lindane in the whole-day food rations collected in hospital canteens in Kraków, ?ód?, Olsztyn and Poznań in winters of 1993-1994, 1995 and 1996 were determined. The diets contained almost 40 microg of cadmium, corresponding to 70% of PTWI, and compared to the levels recognised as safe (ADI or PTWI) small amounts of the other contaminants. The highest content of Pb, Cd, Al and lindane was determined in the diets collected in Kraków, that of radiocaesium in ?ód?, and DDT level was the highest in Poznań. The whole-day food rations from Olsztyn, situated in a region called "green lungs of Poland", were not statistically less contaminated than the diets from the other towns. The Pb and radiocaesium levels decreased significantly with time.     

Seasonality of Cs in roe deer from Austria and Germany

Empirical data on the ¹³⁷Cs activity concentration in meat of roe deer (Capreolus capreolus) roaming in 3 spruce forest areas and one peat bog area are presented and compared. They cover time series of nearly 20 years after a spike contamination in 1986 originating from Chernobyl. A model is presented which considers three soil compartments to describe the change of the availability of ¹³⁷Cs with time.     

A Dynamic model of Cs accumulation by fish of different age classes

A dynamic model of radionuclide accumulation in fish is developed. In the model, the fish population is represented by a set of discrete age classes. Each age class is characterized by a specific growth rate, diet and activity of metabolic processes. The model describes all known types of size effect in the contamination of fish with radiocaesium. The detailed dynamics of ¹³⁷Cs accumulation by fish are demonstrated using the results of the model's application to ichtiofauna in a water body which has a high level of contamination with radiocaesium — namely, the cooling pond of the Chernobyl NPP.     

Spatial assessment of the economic feasibility of short rotation coppice on radioactively contaminated land in Belarus, Ukraine, and Russia. II. Monte Carlo analysis

A Monte Carlo analysis of two sequential GIS-embedded submodels, which evaluate the economic feasibility of short rotation coppice (SRC) production and energy conversion in areas contaminated by Chernobyl-derived (137)Cs, was performed to allow for variability of environmental conditions that was not contained in the spatial model inputs. The results from this analysis were compared to the results from the deterministic model presented in part I of this paper. It was concluded that, although the variability in the model results due to within-gridcell variability of the model inputs was considerable, the prediction of the areas where SRC and energy conversion is potentially profitable was robust. If the additional variability in the model input that is not contained in the input maps is also taken into account, the SRC production and energy conversion appears to be potentially profitable at more locations for both the small scale and large scale production scenarios than the model predicted using the deterministic model.     

Migration of Cs and Sr in undisturbed soil profiles under controlled and close-to-real conditions

Migration of ¹³⁷Cs and ⁹⁰Sr in undisturbed soil was studied in large lysimeters three and four years after contamination, as part of a larger European project studying radionuclide soil–plant interactions. The lysimeters were installed in greenhouses with climate control and contaminated with radionuclides in an aerosol mixture, simulating fallout from a nuclear accident. The soil types studied were loam, silt loam, sandy loam and loamy sand. The soils were sampled to 30–40 cm depth in 1997 and 1998. The total deposition of ¹³⁷Cs ranged from 24 to 45 MBq/m², and of ⁹⁰Sr from 23 to 52 MBq/m². It was shown that migration of ¹³⁷Cs was fastest in sandy loam, and of ⁹⁰Sr fastest in sandy loam and loam. The slowest migration of both nuclides was found in loamy sand. Retention within the upper 5 cm was 60% for both ¹³⁷Cs and ⁹⁰Sr in sandy loam, while in loamy sand it was 97 and 96%, respectively. In 1998, migration rates, calculated as radionuclide weighted median depth (migration centre) divided by time since deposition were 1.1 cm/year for both ¹³⁷Cs and ⁹⁰Sr in sandy loam, 0.8 and 1.0 cm/year, respectively, in loam, 0.6 and 0.8 cm/year in silt loam, and 0.4 and 0.6 cm/year for ¹³⁷Cs and ⁹⁰Sr, respectively, in loamy sand. A distinction is made between short-term migration, caused by events soon after deposition and less affected by soil type, and long-term migration, more affected by e.g. soil texture. Three to four years after deposition, effects of short-term migration is still dominant in the studied soils.     

New best estimates for radionuclide solid–liquid distribution coefficients in soils,Part 1: radiostrontium and radiocaesium

Best estimates for the solid-liquid distribution coefficients (K_d) of radiostrontium and radiocaesium for various soil types, were derived from geometric means (GM) calculated from grouping soils by texture and organic matter content, and also using soil cofactors governing soil–radionuclide interaction. The K_d (Sr) GM for Sand, Loam, Clay and Organic groups were similar, although the value for the Sand group was significantly lower. The Sr cofactor approach, based on the ratios of cation exchange capacity (CEC) to Ca and Mg concentrations in the soil solution, leads to K_d (Sr) GM with a lower variability, from which best estimates could be proposed. The K_d (Cs) GM for Sand and Organic groups differed, although similar values were obtained for Loam and Clay groups. Grouping the K_d (Cs) according to the Radiocaesium Interception Potential (RIP) and the RIP divided by the K concentration in the soil solution also allows to suggest K_d (Cs) best estimates with a lower variability.     

The influence of hot particle contamination on Sr and Cs transfers to milk and on time-integrated ingestion doses

Most models for transfers of radionuclides through the food chain typically assume that the radioactivity is initially deposited in chemically available forms. It is known, however, that releases of radionuclides in the form of hot particles may significantly influence their environmental transfers and uptake to the food chain. This study presents models for time changes in ⁹⁰Sr and ¹³⁷Cs in milk which incorporate hot particle contamination using observed rates of hot particle dissolution following the Chernobyl accident. A general equation is presented for the influence of hot particles on overall ingestion doses. As expected from previous work, fallout of hot particles significantly influences time changes in radionuclide activity concentrations in foodstuffs. It is also shown that incorporation of radionuclides in hot particles influences time-integrated ingestion doses. For a situation in which a large proportion (90–100%) of fallout is in slowly dissolving hot particles, time-integrated ingestion doses from ⁹⁰Sr and ¹³⁷Cs are reduced by a factor of approximately two compared to the case where all radioactivity is deposited in bioavailable forms. However, the influence of rapidly dissolving hot particles on time-integrated ingestion doses is relatively minor. Remaining significant uncertainties in dose estimates are discussed.