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.     

Distributions of radionuclide sorption coefficients (Kd) in sub-surface sediments and the implications for transport calculations

The effect of the spatial variability of K_d on calculations of contaminant travel time in the vadose zone was determined. Depth discrete measurements of K_d were made for a suite of radionuclides (¹⁰⁹Cd, ⁵⁷Co, ⁶⁰Co, ⁸⁵Sr, ¹³⁷Cs, and ⁸⁸Y) utilizing a sediment core from the E-Area at the Savannah River Site. The K_d’s were ordered as ⁸⁵Sr²⁺ < ¹³⁷Cs⁺ < ¹⁰⁹Cd²⁺ < ⁵⁷Co²⁺ = ⁶⁰Co²⁺ << ⁸⁸Y³⁺ and the values generally fell below or near the lowest quartile of values reported in the literature. Correlations were generally weak between soil properties and K_d values. Most importantly, all of the K_d distributions could be reasonably approximated as log-normal. Deterministic and stochastic calculations of contaminant travel time to the water table were made. The deterministic calculations were based on each of three conceptual models of the vadose zone: complete stratification (17 strata, each with a different K_d), two strata (two sections of the vadose zone, each characterized by a single, average K_d), and unstratified (a single zone with an average K_d). Stochastic calculations were based on log-normal fits to the K_d data. The two strata model generally yielded travel times 2× greater than those in the completely stratified model. The unstratified model yielded travel times that were between 3 and 5 times greater than the completely stratified model. The stochastic mean travel times were comparable to those of the two strata model.     

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%.     

Probabilistic distribution coefficients (Kds) in freshwater for radioisotopes of Ag,Am, Ba,Be, Ce,Co, Cs,I, Mn,Pu, Ra,Ru, Sb,Sr and Th – implications for uncertainty analysis of models simulating the transport of radionuclides in rivers

The objective of this study was to provide operational probability density functions (PDFs) for distribution coefficients (K_ds) in freshwater, representing the partition of radionuclides between the particulate and the dissolved phases respectively. Accordingly, the K_d variability should be considered in uncertainty analysis of transport and risk assessment models. The construction of PDFs for 8 elements (Ag, Am, Co, Cs, I, Mn, Pu and Sr) was established according to the procedure already tested in Durrieu et al. [2006. A weighted bootstrap method for the determination of probability density functions of freshwater distribution coefficients (K_ds) of Co, Cs, Sr and I radioisotopes. Chemosphere 65 (8), 1308–1320]: (i) construction of a comprehensive database where K_ds values obtained under various environments and parametric conditions were collected; (ii) scoring procedure to account for the ‘quality’ of each datapoint (according to several criteria such as the presentation of data (e.g. raw data vs mean with or without replicates), contact time, pH, solid-to-liquid ratio, expert judgement) in the construction of the PDF; (iii) weighted bootstrapping procedure to build the PDFs, in order to give more importance to the most relevant datapoints. Two types of PDFs were constructed: (i) non-conditional, usable when no knowledge about the site of concern is available; (ii) conditional PDFs corresponding to a limited range of parameters such as pH or contact time; conditional PDFs can thus be used when some parametric information is known on the site under study. For 7 other radionuclides (Ba, Be, Ce, Ra, Ru, Sb and Th), a simplified procedure was adopted because of the scarcity of data: only non-conditional PDFs were built, without incorporating a scoring procedure.     

Inventory and vertical migration of 90Sr fallout and 137Cs/90Sr ratio in Spanish mainland soils

In this paper the inventory of ⁹⁰Sr in 34 points distributed along the Spanish peninsular territory is presented. Obtained values range between 173 Bq/m² and 2047 Bq/m². From these data set and those ¹³⁷Cs data obtained in a previous work the ¹³⁷Cs/⁹⁰Sr activity ratio has been established, laying this value between 0.9 and 3.6. Also the migration depth of both radionuclides has been analysed obtaining for ¹³⁷Cs an average value 57% lower than that obtained for ⁹⁰Sr.Additionally, this paper presents the results obtained in 11 sampling points in which the activity vertical profile has been measured. These profiles have been analysed to state the behaviour of strontium in soils and after, by using a convective-diffusive model, the parameters of the model which governs the vertical migration of ⁹⁰Sr in the soil, v (apparent convection velocity) and D (apparent diffusion coefficient) have been evaluated. Mean values obtained are 0.20 cm/year and 3.67 cm²/year, respectively.     

Variability of the sorption of Cs, Zn, Sr, Co, Cd, Ce, Ru, Tc and I at trace concentrations by a forest soil along a transect

The variability of the sorption properties (characterized by the distribution coefficient K_d) of a forest soil for Cs, Zn, Sr, Co, Cd, Ce, Ru, Tc, and I were determined along a transect of 150 m in regular intervals of 3 m. Radioactive tracers were used to ensure trace concentrations of these elements. For comparison, for each soil sample the loss on ignition, as a measure of the soil organic matter content, and the pH were also determined. On average, the K_d values increase in the sequence Tc < I < Ru ≈ Co ≈ Zn ≈ Sr < Cd < Ce < Cs; the spatial variability in the sequence I < Zn ≈ Sr ≈ Co ≈ Cd ≈ Ru ≈ Tc < Cs, and I ≈ Ce < Tc. Correlation analysis revealed that, when moving along the transect, the K_d values for some elements changed in a similar, and for others in a dissimilar pattern. In a few cases a correlation between the pH or the loss on ignition and the K_d values was also present. The spatial structure of the data was examined by semivariograms. For the elements Co, Cd, Zn, and Sr, the K_d values showed an almost periodic behaviour along the transect, which is probably due to periodic changes of some soil properties in a forest with regularly spaced trees.     

New best estimates for radionuclide solid–liquid distribution coefficients in soils. Part 3: miscellany of radionuclides (Cd,Co, Ni,Zn, I,Se, Sb,Pu, Am,and others)

New best estimates for the solid–liquid distribution coefficient (K_d) for a set of radionuclides are proposed, based on a selective data search and subsequent calculation of geometric means. The K_d best estimates are calculated for soils grouped according to the texture and organic matter content. For a limited number of radionuclides this is extended to consider soil cofactors affecting soil–radionuclide interaction, such as pH, organic matter content, and radionuclide chemical speciation. Correlations between main soil properties and radionuclide K_d are examined to complete the information derived from the best estimates with a rough prediction of K_d based on soil parameters. Although there are still gaps for many radionuclides, new data from recent studies improve the calculation of K_d best estimates for a number of radionuclides, such as selenium, antimony, and iodine.     

New best estimates for radionuclide solid–liquid distribution coefficients in soils. Part 2. Naturally occurring radionuclides

Predicting the transfer of radionuclides in the environment for normal release, accidental, disposal or remediation scenarios in order to assess exposure requires the availability of an important number of generic parameter values. One of the key parameters in environmental assessment is the solid liquid distribution coefficient, K_d, which is used to predict radionuclide–soil interaction and subsequent radionuclide transport in the soil column. This article presents a review of K_d values for uranium, radium, lead, polonium and thorium based on an extensive literature survey, including recent publications. The K_d estimates were presented per soil groups defined by their texture and organic matter content (Sand, Loam, Clay and Organic), although the texture class seemed not to significantly affect K_d. Where relevant, other K_d classification systems are proposed and correlations with soil parameters are highlighted. The K_d values obtained in this compilation are compared with earlier review data.     

Assessment of surface area normalisation for interpreting distribution coefficients (Kd) for uranium sorption

Adsorption of radionuclides on soils and sediments is commonly quantified by distribution coefficients (K_d values). This paper examines the relationship between K_d values for uranium(VI) adsorption and the specific surface area (SSA) of geologic materials. We then investigate the potential applicability of normalising uranium (U) K_d measurements using the SSA, to produce ‘K_a values’ as a generic expression of the affinity of U for the surface. The data for U provide a reasonably coherent set of K_a values on various solid phases, both with and without ligands. The K_a representation provides a way of harmonising datasets obtained for materials having different specific surface areas, and accounting for the effects of ligands in different systems. In addition, this representation may assist in developing U sorption models for complex materials. However, a significant limitation of the K_a concept is that sorption of radionuclides at trace levels can be dominated by interactions with specific surface sites, whose abundances are not reflected by the SSA. Therefore, calculated K_a values should be interpreted cautiously.     

Laboratory studies of the diffusive transport of Cs and Co through potential waste repository soils

Tests using reconstituted samples have been performed to assess the diffusive transport of ¹³⁷Cs and ⁶⁰Co through natural regolith materials from a region in South Australia being considered for a radioactive waste repository. A double diffusion cell apparatus made of polycarbonate resin was developed to estimate the effective diffusion (D_e) and sorption coefficients (K_d) that allowed large withdrawals from the source and collector cells and has enabled tests with low concentrations of radioactivity. An alternative to porous stainless steel filter plates has also been used to reduce uncertainty in test interpretation. Analysis of the transient data used a staged method of the Laplace transform to take into consideration the volume of the samples withdrawn from the apparatus during testing. At test completion samples were cut into slices and analysed for radionuclide concentration. Data obtained from the sliced samples confirmed that both numerical and experimental data produced acceptable mass balance. The D_e values obtained in this study were of the order of 10⁻⁶ cm² s⁻¹ for both species, higher than previously published data. The K_d values from the diffusion and batch sorption tests were in reasonable agreement for ¹³⁷Cs, but an order of magnitude different for ⁶⁰Co. The sorption of the latter radionuclide was strongly pH dependent, and this dependency during diffusion tests would benefit from further investigation.     

Proposal for new best estimates for the soil solid–liquid distribution coefficient and soil-to-plant transfer of nickel

The objective of this study was to compile data, based on an extensive literature survey, for the soil solid–liquid distribution coefficient (K_d) and soil-to-plant transfer factor (TF) for nickel. The K_d best estimates were calculated for soils grouped according to texture and organic matter content (sand, loam, clay and organic) and soil cofactors affecting soil–nickel interaction, such as pH, organic matter, and clay content. Variability in K_d was better explained by pH than by soil texture.     

Accumulation of 90Sr in the bone tissue of northern mole voles in the head portion of the East Ural Radioactive Trace

The accumulation of ⁹⁰Sr in the bone tissue of northern mole voles (Ellobius talpinus Pallas, 1770) living under chronic exposure to ⁹⁰Sr in the center of the Eastern Ural Radioactive Trace (EURT) with a ⁹⁰Sr contamination density of 37 MBq/m² or 1000 Ci/km² has been evaluated. Northern mole voles live under-ground and are characterized by family organization of populations and an extremely weak tendency toward dispersal. While there are no sex- or age-related differences in ⁹⁰Sr accumulation, sevenfold interindividual differences have been found. Hereditary (familial) determination of the variability of ⁹⁰Sr accumulation has been demonstrated. The probable causes of the difference in the familial component from the results of laboratory experiments on inbred mice are considered. The age-related inversion of ⁹⁰Sr accumulation previously found in other mammalian species in the EURT area has been confirmed. A possible mechanism of its formation is suggested.     

Transfer of Sr into fish in Finnish lakes

The long-term behavior of ⁹⁰Sr was investigated from 1987 to 1997 in fifteen lakes in southern and central Finland following the 1986 Chernobyl accident. Both water and fish samples (perch, pike, vendace) were analyzed. ⁹⁰Sr stays long in the freshwater ecosystem; the observed half-lives during the study period were generally around 10 years in water and even longer in fish. One lake exhibited very different behavior for ⁹⁰Sr, with elevated levels in fish and water and very short observed half-life in fish, less than 2 years. Concentration factors of ⁹⁰Sr in fish (Bqkg⁻¹ f.w. in fish/Bqkg⁻¹ in water) among the studied lakes significantly correlated with both the Ca concentration and electrical conductivity of the water. More ⁹⁰Sr was transferred into fish in lakes with a low electrical conductivity and a low Ca concentration. Among other water parameters evaluated were pH, color, total nitrogen, and phosphorus.     

A review and test of predictive models for the bioaccumulation of radiostrontium in fish

Empirical relations between the ⁹⁰Sr concentration factor (CF) and the calcium concentration in freshwater aquatic systems have previously been determined in studies based on data obtained prior to the Chernobyl accident. The purpose of the present research is to review and compare these models, and to test them against a database of post-Chernobyl measurements from rivers and lakes in Ukraine, Russia, Belarus and Finland. It was found that two independently developed models, based on pre-Chernobyl empirical data, are in close agreement with each other, and with empirical data. Testing of both models against new data obtained after the Chernobyl accident confirms the models’ predictive ability. An investigation of the influence of fish size on ⁹⁰Sr accumulation showed no significant relationship, though the data set was somewhat limited.     

Assessing the fate of radioactive nickel in cultivated soil cores

Parameters regarding fate of ⁶³Ni in the soil–plant system (soil: solution distribution coefficient, K_d and soil plant concentration ratio, CR) are mostly determined in controlled pot experiments or from simple models involving a limited set of soil parameters. However, as migration of pollutants in soil is strongly linked to the water migration, variation of soil structure in the field and seasonal variation of evapotranspiration will affect these two parameters. The aim of this work was to explore to what extent the downward transfer of ⁶³Ni and its uptake by plants from surface-contaminated undisturbed soil cores under cultivation can be explained by isotopic dilution of this radionuclide in the pool of stable Ni of soils. Undisturbed soil cores (50 cm × 50 cm) were sampled from a brown rendzina (Rendzic Leptosol), a colluvial brown soil (Fluvic Cambisol) and an acidic brown soil (Dystric Cambisol) using PVC lysimeter tubes (three lysimeters sampled per soil type). Each core was equipped with a leachate collector. Cores were placed in a greenhouse and maize (DEA, Pioneer^®) was sown. After 44 days, an irrigation was simulated at the core surfaces to supply 10 000 Bq ⁶³NiCl₂. Maize was harvested 135 days after ⁶³Ni input and radioactivity determined in both vegetal and water samples. Effective uptake of ⁶³Ni by maize was calculated for leaves and kernels. Water drainage and leaching of ⁶³Ni were monitored over the course of the experiment. Values of K_d in surface soil samples were calculated from measured parameters of isotopic exchange kinetics. Results confirmed that ⁶³Ni was strongly retained at the soil surface. Prediction of the ⁶³Ni downward transfer could not be reliably assessed using the K_d values, since the soil structure, which controls local water fluxes, also affected both water and Ni transport. In terms of ⁶³Ni plant uptake, the effective uptake in undisturbed soil cores is controlled by isotope dilution as previously shown at the pot experiment scale.     

The Role of Floodplain Soils as a Barrier to Radionuclide Migration: An Example of the Techa–Iset' River System

The contents of ⁹⁰Sr and ¹³⁷Cs and the pattern of their redistribution in the soil and plant cover of floodplain ecosystems have been assessed. It is shown that the radionuclide distribution across the floodplain and along the river flow is determined by the formation of a barrier to their migration near the river channel, at which less mobile ¹³⁷Cs accumulates. The soil and plant cover of the central floodplain are enriched with ⁹⁰Sr. Differences in radionuclide migration in floodplain soils and their input into plants are determined by the relationship between the processes of their immobilization and migration with soil water.     

Sources and pathways of Sr in the North Atlantic–Arctic region: present day and global warming

The spatial and temporal distributions of the anthropogenic radionuclides ¹³⁷Cs and ⁹⁰Sr, originating from nuclear bomb testing, the Sellafield reprocessing plant in the Irish Sea (UK), and from the Ob and Yenisey river discharges to the Arctic Ocean, have been simulated using the global version of the Miami Isopycnic Coordinate Ocean Model (MICOM). The physical model is forced with daily atmospheric re-analysis fields for the period of 1948–1999. Comparison of the temporal evolution of the observed and the simulated concentrations of ⁹⁰Sr has been performed in the Kara Sea. The relative contributions of the different sources on the temporal and spatial distributions of the surface ⁹⁰Sr are quantified over the simulated period. It follows that the Ob river discharge dominated the surface ⁹⁰Sr over most of the Arctic Ocean and along the eastern and western coasts of Greenland before 1960. During the period of 1980–1990, the atmospheric fallout and the Ob river discharge were equally important for the ⁹⁰Sr distribution in the Arctic Ocean. Furthermore, an attempt has been made to explore the possible dispersion of accidental released ⁹⁰Sr from the Ob and Yenisey rivers under a global warming scenario (2 × CO₂). The difference between the present-day and the global warming scenario runs indicates that more of the released ⁹⁰Sr from the Ob and Yenisey rivers is confined to the Arctic Ocean in the global warming run, particularly in the near coastal, non-European part of the Arctic Ocean.     

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.     

Antlers of Cervus elaphus as biomonitors of ⁹⁰Sr in the environment

Adequate radioprotection of the environment requires the identification of biomonitors sensitive to the variation of its radionuclide content. Due to the chemical similarities between calcium and strontium, calcified tissues of mammals are considered to be good ⁹⁰Sr biomonitors. This work considered Cervus elaphus antlers which, being shed annually, can give information about the importance of radiostrontium contamination in an ecosystem in the time period required for the growth of the antler. The samples were collected at various points of W and SW Spain. The mean value of their ⁹⁰Sr content was (70 ± 43 (S.D.)) Bq/kg d.w., range (16-218) Bq/kg d.w., and the radionuclide was evenly distributed in the different parts of the antler. There was a good correlation between the antlers’ ⁹⁰Sr content and the ⁹⁰Sr deposited in the soil. The antlers’ content of ²²⁶Ra (from the natural uranium series) and the contents of some stable elements (Ca, Mg, Sr, and K) were also determined. The values for these stable elements were practically constant in the analyzed samples, and the concentrations measured decreased in the following order:Ca » Mg > K > Sr » ⁹⁰Sr > ²²⁶Ra     

Dependence of dose loads on bone surfaces of murine rodents on the level of 90Sr accumulation in the skeleton

The relationship between ⁹⁰Sr accumulation in the skeleton after single injection and the resulting dose load on bone surfaces was studied in laboratory mice. Radiation doses were measured by a thermoluminescent method. A positive correlation was revealed between the surface dose rate on the skull and mandible and ⁹⁰Sr specific radioactivity in these bones. The possibility to calculate ⁹⁰Sr incorporation into the bone tissue from dosimetric data was evaluated as an analytical approach allowing preservation of the bone material for subsequent studies. Conversion coefficients relating surface doses to ⁹⁰Sr specific radioactivity in bones were calculated. However, their values have to be specifically defined for cases of chronic ⁹⁰Sr input and with regard to bone anatomy and species-specific and ecological features of test animals.