Contamination of terrestrial ecosystem components with <Superscript>90</Superscript>Sr, <Superscript>137</Superscript>Cs,and <Superscript>226</Superscript>Ra caused by the deterioration of the multibarrier protection of radioactive waste storages

The spatial-temporal features of the radioactive contamination of terrestrial ecosystem components caused by the deterioration of the multibarrier protection of regional radioactive waste storages of the State Research Center of the Russian Federation-Leipunskii Institute of Physics and Power Engineering at the input of radionuclides into the soil and ground water were studied. The composition of the radioactive contamination was determined, and the hydrological and geochemical processes resulting in the formation of large radioactive sources were described. The natural features of the radioactive waste storage areas favoring the entry of ⁹⁰Sr, ¹³⁷Cs, and ²²⁶Ra into the soils and their inclusion in the biological turnover were characterized. The directions of the horizontal migration of ⁹⁰Sr, ¹³⁷Cs, and ²²⁶Ra and the sites of their accumulation within the superaquatic and aquatic landscapes of a near-terrace depression were studied; the factors of the ⁹⁰Sr accumulation in plants and cockles were calculated. The results of the studies expand the theoretical concepts of the mechanisms, processes, and factors controlling the behavior of radionuclides at the deterioration of the multibarrier protection of radioactive waste storages. The presented experimental data can be used for solving practical problems related to environmental protection in the areas of industrial nuclear complexes.     

Radioactive Contamination of Alluvial Soils in the Taiga Landscapes of Yakutia with <Superscript>137</Superscript>Cs, <Superscript>226</Superscript>Ra,and <Superscript>238</Superscript>U

The concentrations and distribution of ¹³⁷Cs in alluvial soils (Fluvisols) of the upper and middle reaches of the Markha River in the northwest of Yakutia and ²²⁶Ra and ²³⁸U in alluvial soils within the El’kon uranium ore deposit in the south of Yakutia have been studied. It is shown that the migration of radiocesium in the permafrost-affected soils of Yakutia owing to alluviation processes extends to more than 600 km from the source of the radioactive contamination. The migration of ¹³⁷Cs with water flows is accompanied by its deposition in the buried horizons of alluvial soils during extremely high floods caused by ice jams. In the technogenic landscapes of southern Yakutia, active water migration of ²³⁸U and ²²⁶Ra from radioactive dump rocks. The leaching of ²³⁸U with surface waters from the rocks is more intense than the leaching of ²²⁶Ra. The vertical distribution patterns of ²³⁸U and ²²⁶Ra in the profiles of alluvial soils are complex. Uranium tends to accumulate in the surface humus horizon and in the buried soil horizons, whereas radium does not display any definite regularities of its distribution in the soil profiles. At present, the migration of ²³⁸U and ²²⁶Ra with river water and their accumulation in the alluvial soils extend to about 30 km from the source.     

Agroecological optimums concerning saturation with calcium of soils contaminated by <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr

A close negative correlation between the biological availability of ⁹⁰Sr and ¹³⁷Cs for agricultural crops and the content of exchangeable calcium in soils has been revealed in a field experiment performed for soddy-podzolic loamy sandy soil. The efficiency of soil saturation with exchangeable calcium regarding ⁹⁰Sr discrimination is much higher in soils with a low supply of plants with this nutrient. For the bulk of the studied crops, the minimal biological availability of ⁹⁰Sr is registered at 1200–1400 mg/kg (6.0–7.0 mg-equiv./100 g) of the exchangeable calcium content in the soil and that of ¹³⁷Cs is registered at 1000–1100 mg/kg (5.0–5.5 mg-equiv./100 g). The crop productivity varies significantly depending on the exchangeable calcium content in the soil.     

Dynamics of Chernobyl <Superscript>137</Superscript>Cs contamination fields at long distances

Structural changes in the ¹³⁷Cs contamination fields in natural and agroecosystems of the northern forest steppe (the remote zone of the Chernobyl accident) were studied. It was shown that the lateral and vertical distribution of ¹³⁷Cs in soils of different biogeocenoses depends on the features of functioning biogeocenoses and the spatial variation of the initial fallout. The effect of biogeocenosis on the spatial variation of the contaminant distribution increases with time. At present, the variation of primary distribution in soils of agrocenoses is changing. The soils of forest biogeocenoses have retained the features of primary distribution, particularly in the upper 0-to 5-cm sublitter layer. The ¹³⁷Cs penetration depth is greatest in the soils of layland and functioning agrocenosis and least in the soils of forest biogeocenoses.     

The role of mineralization of the organic matter of soddy-podzolic and peat bog soils in the accumulation of <Superscript>137</Superscript>Cs by plants

The role of mineralization of soil organic matter (SOM) in the mobilization of ¹³⁷Cs was estimated on the basis of data on the biokinetic fractionation of the organic matter of soddy-podzolic sandy-loam and peat bog soils and on the coefficients of the soil-to-plant transfer of radiocesium under field conditions. The peat bog soils were richer than the soddy-podzolic soils in the total organic carbon (by 7.9–23.8 times), the potentially mineralizable carbon (by 2.4–6.5 times), and the carbon of the microbial biomass (by 2.9–4.6 times). The agricultural use of the soddy-podzolic and peat bog soils led to a decrease in the SOM mineralization capacity by 1.1–1.8 and 1.4–2.0 times, respectively. Simultaneously, the portions of the easily, moderately, and difficultly mineralizable fraction of the SOM active pool changed. The coefficients of the ¹³⁷Cs transfer from the peat bog soils to plants were 3.3–17.6 times higher than those for the soddy-podzolic soils. The content of ¹³⁷Cs in plants grown on the peat bog soils was 2–65 times higher than that in the mobile (salt-extractable) soil pool by the beginning of the growing season. Strong positive linear correlations were found between the coefficients of the soil-to-plant transfer of ¹³⁷Cs and the total content of the SOM, the content of the microbial biomass, the content of the potentially mineralizable carbon, and the intensity of its mineralization. It was concluded that the decisive factors controlling the intensity of the ¹³⁷Cs transfer from mineral and organic soils into plants are the SOM content and its mineralization potential. The mineralization of the SOM is accompanied by the release of both ¹³⁷Cs and mineral nitrogen; the latter facilitates the transfer of radiocesium into plants.     

Role of plants in the spatial differentiation of <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr statuses on the aggregate level

The increased concentration of an element in plant biomass compared to the soil mass is an essential condition for the differentiated spatial distribution and status of the element on the aggregate level. Two forms of this differentiation have been revealed for ¹³⁷Cs and ⁹⁰Sr. Transfer of ¹³⁷Cs from plant roots and concentration on the surface of soil aggregates have been established experimentally. Indirect data also point to the potential localization of ¹³⁷Cs on the surface of intraaggregate pores. The effect of radionuclide concentrating on the outer and inner surfaces of aggregates is due to the rapid and strong fixation of cesium microamounts by mineral soil components. ¹³⁷Cs from the surface of aggregates is more available for the repeated uptake by plant roots than from the intraped mass. The distortion of this spatial differentiation mainly occurs during the reaggregation of soil mass, which in turn decreases the availability of the radionuclide to plants. For ⁹⁰Sr, its elevated concentration in the form of organic residues has been revealed in the inter- and intraaggregate pore space. However, due to the high diffusion rate, ⁹⁰Sr is relatively rapidly (during several months under pot experimental conditions) redistributed throughout the entire volume of soil aggregates and its major part gradually passes into the phase of humic compounds, to which the radionuclide is bound by exchange sorption. The high level of the next root uptake (higher than for ¹³⁷Cs by one to two orders of magnitude) favors the permanent renewal of loci with increased ⁹⁰Sr concentrations in the inter- and intraaggregate pore space in the form of plant residues.     

Vertical distribution of <Superscript>137</Superscript>Cs in alluvial soils of the Lokna River floodplain (Tula oblast) long after the Chernobyl accident and its simulation

Profiles of vertical ¹³⁷Cs distribution in alluvial meadow soils on the low and medium levels of the Lokna River floodplain (central part of the Plavsk radioactive spot in Tula oblast) 28 years after the Chernobyl fallout have been studied. A significant increase in the ¹³⁷Cs pool is revealed on the low floodplain areas compared to the soils of interfluves due to the accumulation of alluvium, which hampers the reduction of the total radionuclide pool in alluvial soils because of radioactive decay. The rate of alluvium accumulation in the soil on the medium floodplain level is lower by three times on average. An imitation prognostic model has been developed, which considers the flooding and climatic conditions in the region under study. Numerical experiments have quantitatively confirmed the deciding role of low-mobile forms in the migration of maximum ¹³⁷Cs content along the soil profile in the absence of manifested erosion–accumulation processes.     

The effect of tree roots on the redistribution of <Superscript>137</Superscript>Cs in the soils of pine and birch forests of the radioactive contamination zone

Accumulation and distribution of ¹³⁷Cs by the root systems of forests in the radioactive contamination zone of Bryansk oblast have been discussed. It has been found that the phytomass and distribution of roots of pine and birch trees along the soil profile in the studied BGCs differ considerably. The specific activity of ¹³⁷Cs in the roots changes depending on their diameter: the lowest specific activity is observed in small fractions of the roots, and the highest one in large fractions. It has been shown that the contribution of roots in the total reserves of ¹³⁷Cs in the soil layer of 0–50 cm of various biogeocenoses is different: the largest contribution is characteristic for birch forests (1.66%) with variation of this parameter in separate soil layers from 1.12 to 3.53%, while the contribution for pine forests is lower (0.97%) with the variation from 0.82 to 7.5%. The contribution of roots to the overall contamination of soils in the studied plant communities increases with depth.     

Some indices of biological cycle of <Superscript>137</Superscript>Cs and <Superscript>39</Superscript>K in forest ecosystems of Bryansk woodland in the remote period after chernobyl fallouts

The features of the biological cycle of ¹³⁷Cs and ³⁹K in the remote period after Chernobyl fallouts are considered on the example of forest ecosystems of Bryansk woodland. It is demonstrated that the maximum amount of ¹³⁷Cs in the total phytomass is concentrated in wood, the minimum amount of ¹³⁷Cs, in the external bark layers; for the annual production, in assimilating organs and the external bark layers, respectively. The distribution of ³⁹K in the total phytomass and the annual production is almost identical to that of ¹³⁷Cs. The arrival of ¹³⁷Cs to the soil with litter in pine and birch forests has recently been equal approximately to 50% of the capacity of the biological cycle. It mostly arrives with the assimilating organs (needles and leaves). In pine forests the return of ³⁹K into the soil with litter is closest to that observed for ¹³⁷Cs.     

Distribution of <Superscript>137</Superscript>Cs in the particle-size fractions and in the profiles of alluvial soils on floodplains of the Iput and its tributary Buldynka Rivers (Bryansk oblast)

Pits of sandy alluvial soils were studied in different parts of the floodplains of the Iput River and its tributary the Buldynka River near the settlement of Starye Bobovichi (Bryansk oblast). The ¹³⁷Cs content in the soil horizons varied from 0.01 to 31.2 Bq/g reaching the maximum in the initially polluted layers buried at depths of 6 to 40 cm. Radiocesium was found in all the particle-size fractions with its predominate concentration in the finest fractions. The specific ¹³⁷Cs activity in the fractions of <1, 1–5, 5–10, and >10 μm comprised 44.1 ± 11.5; 33.3 ± 7.6, 20.9 ± 4.9, and 2.4 ± 0.6 Bq/g of soil. However, the contribution of the coarse (>10 μm) fractions to the total radiocesium pool in the soils (19–60%, or 34 ± 2% on the average) was comparable with that of the clay fraction (16–71%, or 38 ± 3% on the average), because of the predominance of the sand-size fractions in the soils. The highest coefficient of variation with respect to the relative contribution of particular fractions to the total soil pool of ¹³⁷Cs was characteristic of the fraction of 5–10 μm; in the other fractions, it varied from 31 to 41%. The portion of ¹³⁷Cs bound with the finest fractions increased in the deeper layers. The total ¹³⁷Cs activity in the polluted horizons of the soils was mainly determined by its concentration in the clay fraction (Spearman’s coefficient of rank correlation (r) for the moderately polluted horizons comprised 0.926 at n = 14). It was experimentally proved that clay particles, upon the destruction of organic films on their surface, could readsorb the released radiocesium for a second time.     

The 137Cs technique applied to steep Mediterranean slopes (Part I): the effects of lithology,slope morphology and land use

Concentrations in the soil of anthropogenic and natural radionuclides have been investigated in order to assess the applicability of the ¹³⁷Cs technique in an area of typical Mediterranean steep slopes. This technique can be used to estimate net soil redistribution rates but its potential in areas with shallow and stony soils on hard rock lithology have not been evaluated so far. In this research, the validity of using this technique in stony shallow soils at very steep slopes is discussed together with the relations between radionuclide concentrations and other soil properties, lithology, slope morphology and land use in a Mediterranean environment. Both natural Potassium-40 (⁴⁰K), Uranium-238 (²³⁸U), Thorium-232 (²³²Th) and anthropogenic Caesium-137 (¹³⁷Cs) radionuclides have been determined in samples taken along slope transects on uncultivated serpentinite soils and cultivated gneiss soils. In addition to the radionuclide concentrations, parameters such as slope position, slope angle, aspect, soil depth, surface stone cover, moss, litter, vegetation cover, soil crust, stone content and bulk density have been quantified.All the natural radionuclides ⁴⁰K, ²³⁸U, ²³²Th show significantly higher concentrations in the gneiss than in the serpentinite soils, opposed to the ¹³⁷Cs concentration, which is found significantly higher in the serpentinite soils probably because of the difference in clay mineralogy. The exponential decreasing depth distribution of ¹³⁷Cs and its homogeneous spatial distribution emphasise the applicability of the ¹³⁷Cs technique in this ecosystem.Lithology determines the concentration of natural and anthropogenic radionuclides. Land use determines the relations between ¹³⁷Cs concentration/inventory and some soil characteristics. Higher ¹³⁷Cs concentration and inventory are associated with higher percentages of vegetation cover, higher percentage of stones in the soil and higher values of soil bulk density in cultivated gneiss soils. Slope morphology and land use influence the soil redistribution at slope scale. The gneiss slopes show a zonation of four to five areas of differential erosion/accumulation processes corresponding with more regular slopes and soil redistribution due to water erosion and to tillage translocation and erosion. The serpentinites, as an example of a more unstable slope type, show more erosion areas with less accumulation downslope and soil redistribution due to water erosion.     

Distribution of 137Cs and 60Co in plough layer of farmland: Evidenced from a lysimeter experiment using undisturbed soil columns

Radionuclide fallout during nuclear accidents on the land may impair the atmosphere, contaminate farmland soils and crops, and can even reach the groundwater. Previous research focused on the field distribution of deposited radionuclides in farmland soils, but details of the amounts of radionuclides in the plough layer and the changes in their proportional distribution in the soil profile with time are still inadequate. In this study, a lysimeter experiment was conducted to determine the vertical migration of 137Cs and 60Co in brown and aeolian sandy soils, collected from the farmlands adjoining Shidaowan Nuclear Power Plant(NPP) in eastern China, and to identify the factors influencing their migration depths in soil. At the end of the experiment(800 d), >96% of added 137Cs and 60Co were retained in the top 0–20 cm soil layer of both soils;very little 137Cs or 60Co initially migrated to 20–30 cm, but their amounts at this depth increased with time. The migration depth of 137Cs was greater in the aeolian sandy soil than in the brown soil during 0–577 d, but at the end of the experiment, 137Cs migrated to the same depth(25 cm) in both soils. Three phases on the vertical migration rate(v) of 60Co in the aeolian sandy soil can be identified: an initial rapid movement(0–355 d, v = 219 ± 17 mm year-1), followed by a steady movement(355–577 d, v = 150 ± 24 mm year-1) and a very slow movement(577–800 d, v = 107 ± 7 mm year-1). In contrast, its migration rate in the brown soil(v = 133 ± 17 mm year-1) was steady throughout the 800-d experimental period. The migration of both 137Cs and 60Co in the two soils appears to be regulated by soil clay and silt fractions that provide most of the soil surface area, soil organic carbon(SOC), and soil pH, which were manifested by the solid-liquid distribution coefficient of 137Cs and 60Co. The results of this study suggest that most 137Cs and 60Co remained within the top layer(0–20 cm depth) of farmland soils following a simulated NPP accident, and little reached the subsurface(20–30 cm depth). Fixation of radionuclides onto clay minerals may limit their migration in soil, but some could be laterally distributed by soil erosion and taken up by crops, and migrate into groundwater in a high water table level area after several decades.Remediation measures, therefore, should focus on reducing their impact on the farmland soils, crops, and water.     

Studying the kinetics of <Superscript>137</Superscript>Cs selective sorption by the dynamic method with the measurement of radioactivity in the sorbent solid phase

The dynamic method was proposed for studying the kinetics of ¹³⁷Cs selective sorption by the measurement of the ¹³⁷Cs activity directly in the sorbent solid phase. A thin layer of the sorbent in a disposable syringe membrane filter (MF) was eluted with a ¹³⁷Cs solution containing K⁺ and Ca²⁺ ions with a gradual decrease in the solution flow rate from 6 to 0.2 cm³/min. The activity of the sorbed ¹³⁷Cs was determined periodically by placing the same MF in the detector well of a Wizard 1480 gamma counter. It was shown that the masses of the sorbent and water in the MF had no effect on the efficiency of the ¹³⁷Cs measurement. A linear relationship between the RIP(K) value and the square root of the time for the period between 4 and 30 days was revealed using this method. The relative increase in the RIP(K) with time changed by 6 times (from 0.034 to 0.208 days^−0.5) for the soils and by 20 times (from 0.008 to 0.153 days^−0.5) for the mineral sorbents. The RIP(K) values measured for the interaction of soddy-podzolic soils with ¹³⁷Cs during 24 hours using the standard limited volume method were lower than the values determined by the proposed dynamic method for the interaction period of 30 days by 50–100%.     

Einfluß des Jahresniederschlags und der Bodenart auf die 137Cs-Tiefenverteilung in Böden Südchiles

The influence of mean annual rainfall and soil texture on the ¹³⁷Cs vertical distribution in soils from southern Chile The influence of mean annual rainfall and soil texture on the vertical distribution of ¹³⁷Cs from global fallout was studied in undisturbed volcanic ash soils from southern Chile. The areal concentration and translocation depth increase with the mean annual precipitation. In spite of the high rainfall at the sampled area (970 - 2500 mm a^?1), the highest ¹³⁷Cs contamination was found in the upper 10 cm layer. The vertical migration is reduced by the high adsorption capacity of these volcanic ash soils, but on the other side increased in soils with high large-pore volumen. The translocation depth reaches only up to 26 cm in the clay soils, 35 cm in the silty soils and 70 cm in the sandy soil.     

Migration and Chemical Availability of 137Cs and 90Sr in SwedishLong-Term Experimental Pastures

Migration and chemical availability of ¹³⁷Cs and⁹⁰Sr in the long-term was studied on a36-yr-old deposition experiment on pastureconsisting of a sandy soil and a clay soil,contaminated in 1961 with radionuclides in aqueoussolution. Comparisons were made with a study of thesame soils in 1967. Soil samples to 55 cm depth wereanalysed for ¹³⁷Cs and ⁹⁰Sr to establish thevertical distribution. Chemical availability wasstudied using sequential extractions with H₂O,NH₄Ac, NH₂OH·HCl, H₂O₂ andHNO₃. Both ¹³⁷Cs and ⁹⁰Sr were found atall depths in both soil types. Cs-137 waspredominantly retained within the upper 10 cm (70%)in both soils. For ⁹⁰Sr, the soils differedsignificantly, retention within the upper 10 cm was27% in sandy soil and 47% in clay soil. Migrationsince 1967 was faster in the sandy soil for bothnuclides. More than 95% of ¹³⁷Cs was bound inthe acid-digestible and residual fractions in bothsoils. The residual fraction was larger in clay soil.⁹⁰Sr was highly available in both soils. Noresidual fraction was found, and the easilyexchangeable fraction was 63–75%.     

The migration of fallout 134Cs, 137Cs and 106Ru from Chernobyl and of 137Cs from weapons testing in a forest soil

To estimate the accumulation and vertical migration of radiocesium and radioruthenium, the activity concentrations of Chernobyl-derived ¹³⁴Cs, ¹³⁷Cs and ¹⁰⁶Ru as well as of ¹³⁷Cs from the global fallout of weapons testing observed in the upper horizons of a forest soil (Hapludult, spruce stand) were evaluated with a compartment model. The resulting residence half-times were used to estimate the mean rates of transport of these radionuclides. For Chernobyl-derived ¹³⁴Cs and ¹³⁷Cs within the time period of 200–600 days after the beginning of the fallout the rates were between 4 cm/yr (Of1-horizon) and 2 cm/yr (Oh-horizon), and for ¹⁰⁶Ru between 4 cm/yr (Of1-horizon) and 7 cm/yr (Oh-horizon). These rates, though considerably slower than observed in the same soil during the initial infiltration of these radionuclides with a rain shower, are (depending on the soil horizon) still higher by a factor of 3–6, when compared to the rates of transport of ¹³⁷Cs from the global fallout of weapons testing in the same soil. Because global fallout ¹³⁷Cs is in the soil since about 20 years, these results suggest that the fixation of radiocesium in the forest soil is a rather slow process.     

The exchangeable fraction of selectively sorbed <Superscript>137</Superscript>Cs in soils and natural sorbents as a function of the K<Superscript>+</Superscript> and NH<Stack><Subscript>4</Subscript><Superscript>+</Superscript></Stack> concentrations

The exchangeable portion of the selectively sorbed ¹³⁷Cs extractable by a 1 M ammonium acetate solution (α _Ex ) for soils, illite, bentonite, and tripolite was found to increase with the increasing concentration of the competitive cation M⁺ (K⁺ or NH₄⁺) and can be approximated by a logarithmic relationship. For clinoptilolite, the values of α _Ex did not depend on the concentration of M⁺. The expression 1 − α _Ex (C _M=n )/α _Ex (C _M = 16) as a function of the M⁺ concentration (where α _Ex (C _M=n ) is the α _Ex value at the competitive cation concentration equal to 16 mmol/dm³) was proposed to compare the dependence of α _Ex on the concentration of K⁺ or NH₄⁺in different sorbents. For soils and illite, these dependences almost coincided, which indicated that the selective sorption of ¹³⁷Cs in soils is determined by the presence of illite-group minerals.     

<Superscript>137</Superscript>Cs in natural ecosystem components within the 30-km impact zone of the Smolensk nuclear power plant

The accumulation and redistribution of ¹³⁷Cs in natural ecosystems within the 30-km impact zone of the Smolensk nuclear power plant (SNPP) are analyzed. It is shown that the radioactive pollution of this territory is mainly due to the Chernobyl-derived radioactive fallout. However, the radioactive decay of ¹³⁷Cs from the Chernobyl disaster is partly compensated for by the ¹³⁷Cs technologic emission from the SNPP. The highest rate of the vertical migration of ¹³⁷Cs is typical of the bog phytocenoses and deciduous forests. The components of biota may be ranked by their capacity for ¹³⁷Cs accumulation as follows: higher fungi > mosses > herbs and shrubs > trees. The organisms and their parts that may serve as bioindicators of the modern radioactive contamination of the territory have been identified. These are the assimilative organs and bark of the trees, various fern species among herbs, sphagnum mosses and Pleurozium schreberi (among mosses), and Typolius felleus among higher fungi.