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the model was tested against independent radiocaesium uptake data for barley (n = 71) using a database of published and unpublished information covering contamination time periods of 1.2-10 years (transfer factors ranged from 0.001 to 0.1).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.     

Does soil adhesion matter when predicting radiocaesium transfer to animals?

A sward will often have significant amounts of soil adhered to the vegetation surfaces which will be ingested by grazing animals. If the soil is contaminated by radioactive fallout then it can serve as a dietary source of radionuclides, in addition to any root uptake by the plants. This study is an attempt to quantitatively assess the importance of soil adhesion as a source of radiocaesium to sheep using the RUINS model which simulates radiocaesium transfer in grazing systems.The method of simulating the contamination of vegetation surfaces used by the RUINS model is described, and the importance of the availability of radiocaesium associated with adhered soil relative to plant incorporated radiocaesium discussed. Two sets of simulations are presented: one in which the soil is treated as a medium providing a uniform availability of radiocaesium, and the second in which account is taken of the partitioning of radiocaesium in the soil between ‘fixed’ and ‘labile’ phases.The results demonstrate that, because of the reduced absorption in the gut of radiocaesium associated with soil, animals grazing pastures with significant amounts of radiocaesium associated with adhered soil will not be as contaminated as radiocaesium activity concentrations measured in bulk vegetation samples would suggest. Therefore, the extent of soil adhesion needs to be considered if predictions of radiocaesium contamination of animal products are to be made on the basis of measured activities of sampled vegetation. However, soil adhesion is unlikely to be a significant dietary source of available radiocaesium, unless the soil concerned exhibits an unusually high bioavailability of radiocaesium. Moreover the simulation results indicate that differences in availability between soil types observed experimentally are consistent with the partitioning between fixed and labile soil compartments made by the RUINS model.     

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.     

Predictions of in situ solid/liquid distribution of radiocaesium in soils

Previous work has demonstrated that plant uptake of radiocaesium (RCs) is related to the activity concentration of RCs in soil solution, which is linked to the soil/soil solution distribution coefficient, K(D). The solid-liquid distribution of RCs is generally studied in soil suspensions in the laboratory and there are few reported measurements for in situ soil solutions. From a data set of 53 different soils (contaminated with either 134CsCl or 137CsCl) used in pot trials to investigate grass uptake of RCs, we analysed the variation of in situ K(D) with measured soil properties. The soils differed widely in % clay (0.5-58%), organic matter content (1.9-96%) and pH (2.4-7.0, CaCl2). The K(D) varied between 29 and 375,000 L kg-' (median 1460 L kg(-1)). Stepwise multiple regression analysis showed a significant correlation between the log K(D) and pH (p < 0.001), log %clay (p < 0.01) and log exchangeable K (p < 0.001) (overall R2 = 0.70). The in situ K(D) values were further compared to K(D)S predicted using an existing model, which assumes that RCs sorption occurs on specific sites and regular ion-exchange sites on the soil solid phase. Sorption of RCs on specific sites was quantified from the radiocaesium interception potential (RIP) measured for each soil and the soil solution concentrations of K+ and NH4+. The in situ log K(D) correlated well with the predicted K(D) (R2 = 0.85 before plant growth, R2 = 0.83 after plant growth). However, the observations were fivefold to eightfold higher than the predictions, particularly for the mineral soils. We attribute the under-prediction to the long contact times (minimum 4 weeks) between the RCs tracers and our experimental soils relative to the short (24 h) contact times used in RIP measurements. We conclude that our data confirmed the model but that ageing of RCs in soil is a factor that needs to be considered to better predict in situ KD values.     

Will the application of Ammonium-Ferric-Hexacyano-Ferrate enhance the vertical migration of radiocaesium?

The consideration of a possible enhanced vertical migration of radiocaesium with the application of ammonium-ferric-hexacyano-ferrate (AFCF) as countermeasure, due to the colloidal nature of AFCF, made us set up a series of migration experiments. For the study two soil types were considered, which were either left unplanted or cultivated with ryegrass. Two AFCF concentrations, 1 and 10 g m^-2, and an untreated control were applied. A simple diffusion–convection model was fitted to the data.The application of AFCF did not enhance the downward migration of radiocaesium in the profile. Moreover, for an unplanted sandy soil the application of AFCF significantly retarded the migration: 10 g AFCF m^-2 decreased the convection term, V, from 0·78 to 0·42 cm a^-1 and the diffusion component, D, from 0·21 to 0·09 cm² a^-1. For all other experimental conditions (unplanted loamy soil, ryegrass cultivated sandy and loamy soil), the application of AFCF did not have any effect on radiocaesium migration. Since AFCF does not promote the vertical migration of radiocaesium, enhanced groundwater contamination is improbable.     

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.     

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.     

Surface ground contamination and soil vertical distribution of 137Cs around two underground nuclear explosion sites in the Asian Arctic, Russia

Vertical distributions of 137Cs have been determined in vegetation-soil cores obtained from 30 different locations around two underground nuclear explosion sites--"Crystal" (event year - 1974) and "Kraton-3" (event year - 1978) in the Republic of Sakha (Yakutia), Russia. In 2001-2002, background levels of 137Cs surface contamination densities on control forest plots varied from 0.73 to 0.97 kBq m(-2) with an average of 0.84+/-0.10 kBq m(-2) and a median of 0.82 kBq m(-2). 137Cs ground contamination densities at the "Crystal" site ranged from 1.3 to 64 kBq m(-2); the activity gradually decreased with distance from the borehole. For "Kraton-3", residual surface contamination density of radiocaesium varied drastically from 1.7 to 6900 kBq m(-2); maximal 137Cs depositions were found at a "decontaminated" plot. At all forest plots, radiocaesium activity decreased throughout the whole vertical soil profile. Vertical distributions of 137Cs in soil for the majority of the plots sampled (n=18) can be described using a simple exponential function. Despite the fact that more than 20 years have passed since the main fallout events, more than 80% of the total deposited activity was found in the first 5 cm of the vegetation-soil cores from most of the forested landscapes. The low annual temperatures, clay-rich soil type with neutral pH, and presence of thick lichen-moss carpet are the factors which may hinder 137Cs transport down the soil profile.     

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.     

Uptake and elimination of radiocaesium in fish and the "size effect."

A number of hypotheses have previously been developed concerning the rates of uptake and elimination of radiocaesium (137Cs) in fish. These include the influence of potassium and other water chemical parameters on both uptake and elimination, and the effect of fish size on accumulation. In order to test these hypotheses, we have assembled a data set comprising more than 1,000 measurements of radiocaesium (137Cs) in predatory fish (perch, pike and brown trout) in nine European lakes during the years after Chernobyl. These data have been analysed using simple models for uptake and excretion of 137Cs in fish, showing that: 1. Fish-water concentration factors (CF) were inversely proportional to potassium [K+] concentration of the different lakes, in agreement with previous studies. 2. The uptake rate of 137Cs in fish was negatively correlated with lake [K+], but excretion rate was independent of [K+]. 3. Lower than expected CF values were found in one lake, Iso Valkj?rvi, Finland. This is attributed to inhibition of the K+ (and therefore 137Cs) high affinity transport system in aquatic plants and fish by low pH and/or low Ca2+. 4. The inclusion of fish weight as a parameter in our dynamic model significantly improves the ability of the model to fit the observed measurements of 137Cs. 5. The model developed from the above hypotheses was able to fit the data from nine different lakes to within approximately a factor of 3 of the observed values.     

Long-term investigations of radiocaesium activity concentrations in carp in North Croatia after the Chernobyl accident

Long-term investigations of radiocaesium activity concentrations in carp in the Republic of Croatia are presented. The radiocaesium levels in carp decreased exponentially and the effective ecological half-life of (137)Cs was estimated to be about 1 year during 1987-2002 and 5 years during 1993-2005. The observed (134)Cs:(137)Cs activity ratio in carp was found to be similar to the ratio observed in other environmental samples. The concentration factor for carp (wet weight) was estimated to be 128+/-74 Lkg(-1), which is in reasonable agreement with model prediction based on K(+) concentrations in water. Estimated annual effective dose received by adult members of the Croatian population due to consumption of carp contaminated with (134)Cs and (137)Cs are small: per capita dose from this source during 1987-2005 was estimated to be 0.5+/-0.2 microSv. Due to minor freshwater fish consumption in Croatia and low radiocaesium activity concentrations in carp, it can be concluded that carp consumption was not a critical pathway for the transfer of radiocaesium from fallout to humans after the Chernobyl accident.     

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.     

Radionuclide migration in forest ecosystems--results of a model validation study

The primary objective of the IAEA's BIOMASS Forest Working Group (FWG) was to bring together experimental radioecologists and modellers to facilitate the exchange of information which could be used to improve our ability to understand and forecast radionuclide transfers within forests. This paper describes a blind model validation exercise which was conducted by the FWG to test nine models which members of the group had developed in response to the need to predict the fate of radiocaesium in forests in Europe after the Chernobyl accident. The outcomes and conclusions of this exercise are summarised. It was concluded that, as a group, the models are capable of providing an envelope of predictions which can be expected to enclose experimental data for radiocaesium contamination in forests over the time scale tested. However, the models are subject to varying degrees of conceptual uncertainty which gives rise to a very high degree of divergence between individual model predictions, particularly when forecasting edible mushroom contamination. Furthermore, the forecasting capability of the models over future decades currently remains untested.     

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.     

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.     

Can 239 + 240Pu replace 137Cs as an erosion tracer in agricultural landscapes contaminated with Chernobyl fallout?

Erosion studies often use 137Cs from the global fallout (main period: 1953-1964) as a tracer in the soil. In many European countries, where 137Cs was deposited in considerable amounts also by the Chernobyl fallout in 1986, the global fallout fraction (GF-Cs) has to be separated from the Chernobyl fraction by means of the isotope 134Cs. In a few years, this will no longer be possible due to the short half-life of 134Cs (2 yr). Because GF-Cs in the soil can then no longer be determined, the potential of using 239 + 240Pu as a tracer is evaluated. This radionuclide originates in most European countries essentially only from the global fallout. The activities and spatial distributions of Pu and GF-Cs were compared in the soil of a steep field (inclination about 20%, area ca. 3 ha, main soil type Dystric Eutrochrept), sampled at 48 nodes of a 25 x 25 m2 grid. The reference values were determined at 12 points adjacent to the field. Their validity was assured by an inventory study of radiocaesium in a 70 ha area surrounding the field sampling 275 nodes of a 50 x 50 m2 grid. In the field studied, the activity concentrations of GF-Cs and Pu in the Ap horizon were not correlated (Spearman correlation coefficient R = 0.20, p > 0.05), and the activity balance of Pu differed from that of GF-Cs. Whereas no net loss of GF-Cs from the field was observed as compared to the reference site, Pu was more mobile with an average loss of ca. 11% per unit area. In addition, the spatial pattern of GF-Cs and Pu in the field differed significantly. The reason may be that due to their different associations with soil constituents, Pu and Cs represent different fractions of the soil, exhibiting different properties with respect to erosion/deposition processes. This indicates that both radionuclides or one of them may not be appropriate to quantity past erosion. When tracer losses are used to calibrate or verify erosion prediction models, systematic deviations may not only stem from model shortcomings but also from tracer technique.     

Examination of the effect of particle size on the radionuclide content of soils

Information on the distribution of radiocaesium as a function of soil particle size is fundamental for its use as tracer in soil transport. Since the processes involved in soil erosion are known to remove and transport finer particles with larger efficiency, the aim of this work was to obtain data on the particle size versus radionuclide content distribution regarding the reference site of a soil erosion study. The analysis done was based on more than 5kg of source material and the changes happened to the radionuclide content of the different size fractions between the individual separation steps have been carefully monitored. About 10% of the total amount of (137)Cs present was found to be trapped in the serrations of larger stone-fragments while another 10% is transportable only during heavier storm-events. Within the remaining 80%, physical weathering products and clay particles have a (137)Cs-activity concentration, transportability and mass ratio of about 1:10, 1:2 and 1:1, respectively.     

Assessment of state-of-the-art models for predicting the remobilisation of radionuclides following the flooding of heavily contaminated areas: the case of Pripyat River floodplain

The performances of models are assessed to predict the wash-off of radionuclides from contaminated flooded areas. This process should be accounted for in the proper management of the aftermath of a nuclear accident. The contamination of the Pripyat River water following the inundation of a floodplain heavily contaminated by (90)Sr and (137)Cs of Chernobyl origin is used as the basis for modelling. The available experimental evidence demonstrated that remobilisation of radiostrontium is an important process implying a significant secondary radioactive load of water flowing over the contaminated floodplain. On the contrary, there is no empirical evidence of a similar behaviour for radiocaesium. In general, state-of-the-art models properly predicted the remobilisation of strontium, whereas they significantly overestimated radiocaesium concentrations in water. The necessary model improvements for a more accurate prediction of radiocaesium contamination levels include a reassessment of the values of the model parameters controlling the remobilisation process.     

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.