Laboratory experiments to predict changes in radiocaesium root uptake after flooding events

Changes in soil solution composition after a flooding event were hypothesised to be one of the key factors in explaining changes in radiocaesium incorporation in the food chain in the areas affected by the Chernobyl accident. A laboratory methodology was set up to monitor changes in the soil solution composition after a sequence of flooding cycles. Experiments were performed using column and batch approaches on test soils with contrasting initial soil solution composition (high and low initial concentrations of K+). Results from column experiments indicated a potential increase in NH(4)(+) concentrations, a parameter which could lead to an increase in the radiocaesium root uptake. Batch results in the soil with high initial K+ concentration showed that after a number of flooding cycles, especially for high ratios of flooding solution/mass of soil, K+ concentration decreased sometimes below a threshold value (around 0.5-1 mmol l(-1)), a fact that could lead to an increase in radiocaesium transfer. For the soils with a low initial K+ concentration, the flooding solution increased K+ and NH(4)(+) values in the soil solution. The comparison of test soils with soils from Ukraine areas affected by flooding showed that the final stage in soil solution composition was similar in both cases, regardless of the initial composition of the soil solution. Moreover, the comparison with unflooded soils from the same area showed that potential changes in other soil parameters, such as (137)Cs activity concentration, clay content, and radiocaesium interception potential, RIP (a parameter that estimates the radiocaesium specific sorption capacity of a soil), should also be monitored for additional effects due to the flooding event. Therefore, the changes in the root uptake would depend on the resulting situation from changes in RIP, K+ and NH(4)(+) values in the soil solution.     

Radiocaesium soil-to-wood transfer in commercial willow short rotation coppice on contaminated farm land

The feasibility of willow short rotation coppice (SRC) for energy production as a revaluation tool for severely radiocaesium-contaminated land was studied. The effects of crop age, clone and soil type on the radiocaesium levels in the wood were assessed following sampling in 14 existing willow SRC fields, planted on radiocaesium-contaminated land in Sweden following Chernobyl deposition. There was only one plot where willow stands of different maturity (R6S2 and R5S4: R, root age and S, shoot age) and clone (Rapp and L78183 both of age category R5S4) were sampled and no significant differences were found. The soils differed among others in clay fraction (3-34%), radiocaesium interception potential (515-6884 meq kg(-1)), soil solution K (0.09-0.95 mM), exchangeable K (0.58-5.77 meq kg(-1)) and cation exchange capacity (31-250 meq kg(-1)). The soil-to-wood transfer factor (TF) of radiocaesium differed significantly between soil types. The TF recorded was generally small (0.00086-0.016 kg kg(-1)), except for willows established on sandy soil (0.19-0.46 kg kg(-1)). Apart from the weak yet significant exponential correlation between the Cs-TF and the solid/liquid distribution coefficient (R2 = 0.54) or the radiocaesium interception potential, RIP (R2 = 0.66), no single significant correlations between soil characteristics and TF were found. The wood-soil solution 137Cs concentration factor (CF) was significantly related to the potassium concentration in the soil solution. A different relation was, however, found between the sandy Tr?dje soils (CF = 1078.8 x m(K)(-1.83), R2 = 0.99) and the other soils (CF = 35.75 x m(K)(-0.61), R2 =0.61). Differences in the ageing rate of radiocaesium in the soil (hypothesised fraction of bioavailable caesium subjected to fast ageing for Tr?dje soils only 1% compared to other soils), exchangeable soil K (0.8-1.8 meq kg(-1) for Tr?dje soils and 1.5-5.8 meq kg(-1) for the other soils) and the ammonium concentration in the soil solution (0.09-0.31 mM NH4+ for the Tr?dje soils compared to 0.003-0.11 mM NH4+ for the other soils) are put forward as potential factors explaining the higher CF and TF observed for the Tr?dje soils. Though from the dataset available it was not possible to unequivocally predict the Cs-soil-to-wood-transfer, the generally low TFs observed point to the particular suitability for establishment of SRC on radiocaesium-contaminated land.     

Predicting the transfer of radiocaesium from organic soils to plants using soil characteristics

A model predicting plant uptake of radiocaesium based on soil characteristics is described. Three soil parameters required to determine radiocaesium bioavailability in soils are estimated in the model: the labile caesium distribution coefficient (kd1), K+ concentration in the soil solution [mK] and the soil solution-->plant radiocaesium concentration factor (CF, Bq kg-1 plant/Bq dm-3). These were determined as functions of soil clay content, exchangeable K+ status, pH, NH4+ concentration and organic matter content. The effect of time on radiocaesium fixation was described using a previously published double exponential equation, modified for the effect of soil organic matter as a non-fixing adsorbent. The model was parameterised using radiocaesium uptake data from two pot trials conducted separately using ryegrass (Lolium perenne) on mineral soils and bent grass (Agrostis capillaris) on organic soils. This resulted in a significant fit to the observed transfer factor (TF, Bq kg-1 plant/Bq kg-1 whole soil) (P < 0.001, n = 58) and soil solution K+ concentration (mK, mol dm-3) (P < 0.001, n = 58). Without further parameterisation the model was tested against independent radiocaesium uptake data for barley (n = 71) using a database of published and unpublished information covering contamination time periods of 1.2-10 years (transfer factors ranged from 0.001 to 0.1). The model accounted for 52% (n = 71, P < 0.001) of the observed variation in log transfer factor.     

Effect of K and bentonite additions on Cs-transfer to ryegrass

Bentonite amendments are generally ineffective in reducing the soil-to-plant radiocaesium transfer but have previously been shown that bentonites in the K-form having been subjected to wetting-drying cycles had pronounced radiocaesium binding capacities. We have investigated the effect of wetting-drying (WD) on Radiocaesium Interception Potential (RIP) development in three K-bentonites and K-bentonite soil mixtures, using a variety of procedures: homogenisation of the bentonites with K through dialysis (K(B)), or partial transformation of the bentonite to the K-form in the presence of a solution of K2CO3 (K(L)) or in presence of solid K2CO3 (K(S)). Of the three strategies tested, addition of K2CO3 (solid) at a dose of 2 meq g(-1) clay and adding the K-bentonite mixtures to the soil resulted in the highest RIP increase after 20 WD cycles. The procedure giving the highest RIP yield is the most practical for further applications and was used in a pot experiment under greenhouse condition. When expressing the RIP increase of the soil-bentonite mixtures per unit bentonite added (RIP yield), 28- to 110-fold RIP increases were observed up to a value of approximately 60,000 meq kg(-1) (6 times higher than the RIP for illite). The beneficial effect following K-bentonite application was shown to be dependent both on a sorption enhancement effect (direct RIP effect) and fixation effects (indirect RIP effect). Greenhouse testing proved that the RIP effects observed in greenhouse could be predicted by making use of the sorption data from the laboratory tests. Optimum soil-amendment would be obtained with bentonites with high initial sorption RIP and a high sorption RIP increase when subjected to WD in the presence of potassium. Hypothised Transfer Factor (TF)-reductions of at least 10-fold could result when mixing approximately 1% bentonite, like Otay bentonite (RIP yield 99,000 meq kg(-1) after WD in presence of K if only fine particle size of <1mm considered) with the contaminated ploughing layer.     

Radiocaesium soil-to-plant transfer in tropical environments

In this work, soil-to-plant transfer factors of radiocaesium are predicted based on soil properties such as pH, organic matter content, exchangeable K+ and clay content valid for the tropical environments in Bangladesh, China and Japan, and using a previously published model. Due to insufficient data of soil properties in the selected regions, the average values of pH, organic matter content, exchangeable K+ and clay content were taken as the input model parameters within the ranges given for Asia. Nevertheless, a complete set of soil properties of Japanese soils was used to compare the measured and calculated TF values of radiocaesium for radish. The calculated TF values for radiocaesium are comparable with the measured values especially for leafy parts of a plant. However, calculated values for rice, an important crop in Asia are found to overestimate the measured values due to an overestimate of calculated CECs in soils in the selected regions. The empirical parameters used in the model need to be re-evaluated for the specific part of a plant and/or for a variety of different plants. Alternatively, a general conversion factor for each part of a plant and/or for a variety of different plants for a specific region is suggested for tropical environments.     

Radiocaesium fallout behaviour in volcanic soils in Iceland

The retention of 137Cs in various types of Andosols in Iceland was investigated. Soils were sampled at 29 sites with varying precipitation and environmental conditions. Samples were obtained from 0 to 5, 5 to 10, and 10 to 15 cm depths. The amount of radiocaesium present was quite variable, ranging between 300 and 4800 Bq m(-2) and correlated closely to total annual precipitation (r2=0.71). The majority of 137Cs, 82.7% on average, was retained in the uppermost 5 cm of the soil. The greatest penetration of 137Cs was observed for organic Histosols (76.3% in top 5 cm). The Icelandic Vitrisols (barren, poorly developed Andosols) are coarse grained with only 2-5% clay content and contain little organic matter (<1%). Yet these soils retained 74% of 137Cs in the top 5 cm. The results indicate that radiocaesium fallout is strongly retained by colloidal materials characteristic of Andosols, such as allophane and ferrihydrite. Most soils in Iceland are subject to severe and prolonged freezing and waterlogging; despite this, 137Cs is retained in the upper soil horizons and vertical migration is negligible in Icelandic Andosols. However, erosion and aeolian activity can markedly influence the amount and vertical distribution of radiocaesium in Icelandic 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.     

Effect of external potassium (K) supply on the uptake of 137Cs by spring wheat (Triticum aestivum cv. Tonic): a large-scale hydroponic study.

A large-scale hydroponic experiment was carried out in a non-controlled greenhouse. Spring wheat plants were grown to maturity at four levels of external K concentration (2, 4, 20 and 40 mgl(-1)) and one concentration of radiocaesium (8 Bqml(-1)). Concentrations of K and radiocaesium in the growth solution were closely monitored, and replenishments were made upon depletion. K effectively competed with radiocaesium in terms of root uptake. Activity concentrations of radiocaesium in plants differed significantly between the four K treatments; the activity concentration at the lowest external K concentration being 100 times higher than that at the highest K level. The relationship between radiocaesium uptake and external K level could be described by a negative power function; this showed that when the K level reached around 12 mgl(-1), further increases in the external K level resulted only in slight changes in its inhibitory effect. As a result of this inhibitory effect of potassium supply, concentrations of radiocaesium in plant tissues, grains in particular, were greatly reduced at high external K concentration. Mechanisms involved in Cs-K interaction in root uptake are also discussed.     

A simple method for the estimation of the bioavailability of radiocaesium from herbage contaminated by adherent soil

Adherent soil may contribute a large proportion of the radiocaesium content of sampled vegetation. Consequently, inadvertent ingestion of adherent soil can contribute significantly to the radiocaesium intake of grazing animals, and needs to be accounted for within radiological assessments. However, accurate estimation of the degree of soil adhesion on vegetation is acknowledged to be difficult. To determine the relative contributions of vegetation and soil to the radiocaesium contamination of milk and tissues, soil-specific estimation of radiocaesium bioavailability values would be required. Here we suggest that a previously developed in-vitro bioavailability assay (involving a 2 h extraction with 0.1 M stable CsCl) can be used to estimate the true absorption coefficient of radiocaesium associated with sampled vegetation directly. Using this technique, seasonal trends in bioavailability are demonstrated to vary in accordance with estimations of the degree of soil adherent to vegetation collected from an upland pasture. The use of this technique would negate the need for detailed measurements of the amount of soil adhering to sampled vegetation and soil-specific radiocaesium bioavailability assessments.     

Seasonal variation of the radiocaesium transfer soil-to-Swiss chard (Beta vulgaris var. cicla L.) in allophanic soils from the Lake Region, Chile

The transfer factor (TF) of radiocaesium from soil-to-Swiss chard (Beta vulgaris var. cicla L.) was studied in two different characteristic allophanic soils (umbric andosol and dystric fluvisol) of the Lake Region, an important agricultural region situated in central-south Chile. To investigate especially the time dependence and the effect of K-fertilisation on the TF, field experiments were conducted. Plots of 7.6 m2 were labelled with 100 kBq 134Cs m(-2) at Santa Rosa Experiment Station close to the city of Valdivia characterised by a temperate climate and high precipitation rates. The variation in time of the radiocaesium TF soil-to-Swiss chard was observed during two consecutive years after soil contamination by sequential harvests and radiocaesium analyses of the plants. The TFs showed no significant ageing effect, but a pronounced seasonal decrease with effective half-lives of about 140 and 160 days for the umbric andosol without and with K-fertilisation, respectively, and of 50 and 60 days for the dystric fluvisol without and with K-fertilisation, respectively. The effect of K-fertilisation on the absolute values of the TF was determined by the ratio between the median TF values obtained for corresponding dates without and with use of K-fertiliser. A ratio of TF(without K)/TF(with K) = 1.8 for the umbric andosol and TF(without K)/TF(with K) = 2.9 for the dystric fluvisol was obtained, indicating a reduction of the TF by applying 90 kg K ha(-1). The maximal values of the TF to chard predicted by the equation characterising the seasonal decrease of the TF at the beginning of the harvest periods are 0.19 for the umbric andosol and 0.11 for the dystric fluvisol, both values for soil treated with common K-fertilisation.     

An overview of the effect of organic matter on soil-radiocaesium interaction: implications in root uptake

This paper aims to give an overview of the effect of organic matter on soil-radiocaesium interaction and its implications on soil-to-plant transfer. Studies carried out after the Chernobyl accident have shown that high 137CS soil-to-plant transfer persists in organic soils over years. In most of these soils, the specific sites in clays control radiocaesium adsorption, organic compounds having an indirect effect. Only in organic soils with more than 95% of organic matter content and negligible clay content does adsorption occur mostly on non-specific sites. After a contamination event, two main factors account for the high transfer: the low solid-liquid distribution coefficient, which is due to the low clay content and high NH4+ concentration in the soil solution, and the low K+ availability, which enhances root uptake. The estimation of the reversibly adsorbed fraction, by means of desorption protocols, agrees with the former conclusions, since it cannot be correlated with the organic matter content and shows the lack of specificity of the adsorption in the organic phase. Moreover, the time-dependent pattern of the exchangeable fraction is related to soil-plant transfer dynamics.     

Modelling the role of humic acid in radiocaesium distribution in a British upland peat soil

The significance of exchange sites on organic matter in the retention of radiocaesium in highly organic soils remains unclear. To quantify this retention, we measured the binding of 134Cs to a humic acid isolated from a British upland peat soil, under a range of chemical conditions. We interpreted our results using Humic Ion Binding Model V, a model of humic substance chemistry which simulates ion exchange by non-specific accumulation of cations adjacent to the humic molecules. Model V could simulate the humic acid-solution partitioning of Cs under all the solution conditions used. The model was used to estimate the contribution of organic matter to Cs sorption by the whole soil composite. An estimate of Cs sorption by illite frayed edge sites was also made. These simulations show that organic matter may play only a minor role in binding Cs. even in highly organic soils.     

Experimental values for 241Am and 239+240Pu Kd's in French agricultural soils

Experiments resulted in determination of K(d) values for (241)Am and (239+240)Pu in 6 soils whose characteristics are representative of agricultural soils found around French nuclear power plant sites. These experiments were conducted in stirred batch reactors and the sorption isotherms were plotted. For americium, the experimental K(d) values varied from 60 to 4000 Lkg(-1) (d.w.) and correlated well with soil pH, K(d) increased with increasing pH. As regards plutonium, the experimental K(d) values varied between 300 and 9600 Lkg(-1) and decreased with increasing total sand content. The estimation of the total residence time determined by using a particular and experimentally refined value for K(d)-with a model similar to those currently used for impact assessments-illustrates the importance of establishing values that are better suited to specific soils than generic values. Lastly, depending on the type of evaluation envisioned, it might be important to look for a specific value of K(d)-and even modelling-more suited to the specificity of the scenario studied, by performing more complex, or even in situ, experiments.     

Radioactive contamination of tropical rainforest soils in Southern Costa Rica

Radionuclide content in soils from four locations in a tropical rainforest near Golfito in Southern Costa Rica was investigated. For comparison, two nearby locations in open grassland were also studied. From each site 5 soil cores down to a depth of 15 cm were taken. The median contamination with 137Cs was 584 Bq m-2 (reference date 1 January 1996) and the coefficient of variation (CV) was 50%. This contamination can be attributed to global fallout from atmospheric nuclear weapon tests between 1945 and 1980. The mean contamination is slightly lower than the value expected for the latitude (8 degrees 42': 700 Bq m-2), which may be explained by migration of radiocaesium to subsoil below 15 cm or by uptake into the living biomass. Out of the total variability of 50%, around 20% can be attributed to the sampling and measuring process uncertainties, thus leaving a 45% contribution of spatial variability. A significant difference between forest and meadow sites could be detected: the meadow sites showed lower radiocaesium soil inventories (median: 291 Bq m-2) than the forest sites (643 Bq m-2). This may be explained by the agricultural activities carried out on meadow sites which lead to an increased redistribution of caesium in the soil profile and therefore a larger fraction of the total 137Cs lying below 15 cm. Another reason for higher contamination levels under forest can be attributed to the high interception potential of dense tree canopies for dry deposition. Extrapolating the 137Cs concentration below the sampling horizon, i.e. accounting for the cut-off of the profiles by the sampling technique, results in an estimated mean of 710 Bq m-2 for the forest sites, which is very close to the expected figure. The mainly mineral part of the forest soil profiles was analysed for the 137Cs transport parameters, apparent convection velocity (v = 0.14 +/- 0.09 cm a-1) and apparent diffusion constant (D = 0.79 +/- 0.49 cm2 a-1). The maximum concentration can be found at 5.3 +/- 2.9 cm depth, the half-value depth being 7.4 +/- 1.3 cm. The mean 40K activity concentration was 175 Bq kg-1 dry matter (CV = 69%) and 226Ra and 228Ra concentrations of 9.90 Bq kg-1 (CV = 23%) and 7.93 Bq kg-1 (CV = 20%) have been found, respectively.     

Distribution of pre- and post-Chernobyl radiocaesium with particle size fractions of soils

The association of radiocaesium with particle size fractions separated by sieving and settling from soils sampled eight years after the Chernobyl accident has been determined. The three size fractions were: <2 microm, 2-63 microm and >63 microm. 137Cs in the soil samples was associated essentially with the finer size fractions, which generally showed specific activities 3-5 times higher than the bulk samples. Activity ratios of 134Cs/137Cs in the clay-sized fractions appear to be lower with respect to the corresponding values in bulk soil samples. This result indicates that some differences still exists in the particle size distribution between 137Cs originating from nuclear weapons, which has been in the soil for decades after fallout, and 137Cs coming from the Chernobyl accident, eight years after the deposition event. This behaviour could be related to "ageing" processes of radiocaesium in soils.     

Evaluating and reducing a model of radiocaesium soil-plant uptake

An existing model of radiocaesium transfer to grasses was extended to include wheat and barley and parameterised using data from a wide range of soils and contact times. The model structure was revised and evaluated using a subset of the available data which was not used for model parameterisation. The resulting model was then used as a basis for systematic model reduction to test the utility of the model components. This analysis suggested that the use of 4 model variables (relating to radiocaesium adsorption on organic matter and the pH sensitivity of soil solution potassium concentration) and 1 model input (pH) are not required. The results of this analysis were used to develop a reduced model which was further evaluated in terms of comparisons to observations. The reduced model had an improved empirical performance and fewer adjustable parameters and soil characteristic inputs.     

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.     

The influence of a coal-fired power plant operation on radionuclide concentrations in soil

Fifty-two soil samples in the vicinity of a coal-fired power plant (CFPP) in Figueira (Brazil) were analyzed. The radionuclide concentration for the uranium and thorium series in soils ranged from <9 to 282 Bq kg(-1). The range of 40K concentration in soils varied from <59 to 412 Bq kg(-1). The CFPP (10 MWe) has been operating for 35 years and caused a small increment in natural radionuclide concentration in the surroundings. This technologically enhanced natural radioactivity (TENR) was mainly due to the uranium series (234Th, 226Ra and 210Pb) and was observable within the first kilometer from the power plant. The CFPP influence was only observed in the 0-25 cm soil horizon. The soil properties prevent the radionuclides of the 238U-series from reaching deeper soil profiles. The same behavior was observed for 40K as well. No influence was observed for 232Th, which was found in low concentrations in the coal.     

Modelling 137Cs uptake in plants from undisturbed soil monoliths

A model predicting 137Cs uptake in plants was applied on data from artificially contaminated lysimeters. The lysimeter data involve three different crops (beans, ryegrass and lettuce) grown on five different soils between 3 and 5 years after contamination and where soil solution composition was monitored. The mechanistic model predicts plant uptake of 137Cs from soil solution composition. Predicted K concentrations in the rhizosphere were up to 50-fold below that in the bulk soil solution whereas corresponding 137Cs concentration gradients were always less pronounced. Predictions of crop 137Cs content based on rhizosphere soil solution compositions were generally closer to observations than those based on bulk soil solution composition. The model explained 17% (beans) to 91% (lettuce) of the variation in 137Cs activity concentrations in the plants. The model failed to predict the 137Cs activity concentration in ryegrass where uptake of the 5-year-old 137Cs from 3 soils was about 40-fold larger than predicted. The model generally underpredicted crop 137Cs concentrations at soil solution K concentration below about 1.0 mM. It is concluded that 137Cs uptake can be predicted from the soil solution composition at adequate K nutrition but that significant uncertainties remain when soil solution K is below 1 mM.