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.     

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.     

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.     

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.     

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.     

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.     

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.     

The influence of temperature and hydration on the sorption properties of bentonite

The effects of exposure to synthetic groundwater at elevated temperature gradients on the sorption properties of bentonite were investigated using the Mock-Up-Cz experiment. This experiment simulated the vertical placement of a container of radioactive waste according to the Swedish KBS-3 system for a period of more than 3 years. The mineralogical composition, as well as its chemical and physico-chemical properties, including the uptake of (99)TcO(4)(-) and (134)Cs(+), was used to evaluate the chemical changes caused by the long-term exposure of bentonite buffer to thermal and hydration gradients. It was found that the bentonite material was predominantly stable. No more than 2% of the montmorillonite was transformed due to thermal and moisture gradients. It was concluded that the new-formed mineral phases have no significant influence on the ion exchange and sorption properties of bulk bentonite samples.     

Comparative study of 137Cs partitioning between solid and liquid phases in Lakes Constance, Lugano and Vorsee.

The methodology for estimating radiocaesium distribution between solid and liquid phases in lakes is applied for three prealpine lakes: Lake Constance (Germany), Lake Lugano (Switzerland) and Lake Vorsee (Germany). It is based on use of the exchangeable distribution coefficient and application of the exchangeable radiocaesium interception potential (RIPex). The methodology was tested against experimental data. Good agreement was found between estimated and measured 137Cs concentrations in Lake Constance and Lake Lugano, whereas for Lake Vorsee a discrepancy was found. Bottom sediments in Lake Vorsee are composed mainly of organic material and probably cannot be described in terms of the specific sorption characteristics attributed to illitic clay minerals.     

Influence of fertilizing on the Cs soil–plant transfer in a spruce forest of Southern Germany

Fertilization with 2.5 t/ha limestone: (83% CaCO₃, 8% MgO, 6% K₂O, 3% P₂O₅) reduces the ¹³⁷Cs transfer from spruce forest soil into plants like fern (Dryopteris carthusiana) and blackberry (Rubus fruticosus) by a factor of 2–5 during at least 11 years as measured by the aggregated transfer factor T_ag. In 1997 and 2006 these results were confirmed by additional measurements of the ¹³⁷Cs transfer factor TF, related to the root zone (O_h horizon), which were explained by the selective sorption of ¹³⁷Cs in the root zone by measurements of the Radiocaesium Interception Potential (RIP) in fertilized (RIP > 179 meq/kg) and non-fertilized soils (RIP < 74 meq/kg).     

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.     

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.     

Distribution coefficients of tin in Japanese agricultural soils and the factors affecting tin sorption behavior

Sorption behavior of tin (Sn) in Japanese agricultural soils was studied. Soil-soil solution distribution coefficient (K(d)) of Sn (K(d)-Sn) for 142 soil samples ranged between 128 and 1,590,000 L kg(-1) with the geometric mean of 12 400 L kg(-1). The K(d)-Sn values for Andosol tended to be higher than those of the other soil groups. Among the relationships between K(d)-Sn values and soil properties, a high correlation was observed for soil active-Al (Al-(hydr)oxide and Al-humus complex) amount and K(d)-Sn. The pH effect on Sn sorption was also investigated. The results suggested that the low pH condition enhanced the Sn sorption in soils. The soil-sorbed Sn fractions in each type of soil material were also evaluated with selective extraction methods. The results showed that most of the soil-sorbed Sn was as organic matter bound or Al/Fe-(hydr)oxide-bound forms.     

Fibre crops as alternative land use for radioactively contaminated arable land

The transfer of radiocaesium, one of the most important and widespread contaminants following a nuclear accident, to the fibre crops hemp (Cannabis sativa L.) and flax (Linum usitatissimum L.) as well as the distribution of radiocaesium during crop conversion were studied for sandy soil under greenhouse and lysimeters conditions. Soil parameters did not unequivoqually explain the transfer factors (TF) observed. TFs to flax stems ranged from 1.34 to 2.80x10(-3) m2 kg(-1). TFs to seeds are about a factor of 4 lower. During the retting process for separating the fibres from the straw, more than 95% of the activity was removed with the retting water. For hemp, the TF to the stem was about 0.6x10(-3) m2 kg(-1). For hemp, straw and fibres were mechanically separated and TF to straw was about 0.5x10(-3) m2 kg(-1) and to fibres 1.0x10(-3) m2 kg(-1). Generally, the TFs to the useable plant parts both for hemp and flax, are low enough to allow for the production of clean end-products (fibre, seed oil, biofuel) even on heavily contaminated land. Given the considerable decontamination during retting, contamination levels in flax fibres would only exceed the exemption limits for fibre use after production in extreme contamination scenarios (>12,300kBq m(-2)). Since hemp fibres are mechanically separated, use of hemp fibres is more restricted (contamination <740kBq m(-2)). Use of stems as biofuel is restricted to areas with contamination levels of <250 and 1050kBq m(-2) for flax and hemp, respectively. Use of seeds for edible oil production and flour is possible almost without restriction for flax but due to the high TFs to seed observed for hemp (up to 3x10(-3) m2 kg(-1)) consumption of hemp seed products should be considered with care.     

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.     

Sorption of metals onto natural organic matter as a function of complexation and adsorbent-adsorbate contact mode

The effect of complexing anion and adsorbate-adsorbent contact mode (static equilibrium or dynamic non-equilibrium) on binding and partition of Cu(2+), Cd(2+) and Zn(2+) onto organic matter (exemplified in a low-moor peat) was studied. The study comprised comparative batch and column flow-through sorption experiments on monometallic solutions of Me-Cl and Me-SO(4) salts, at pH 4.0, and sequential fractionation of sorbed metals with respect to binding strength. Both the presence of an anion having complexing properties (Cl(-)) as well as a contact mode was found to quantitatively and qualitatively affect the sorption capacity and binding strength of organic matter (peat) for metal ions. Complexing effect of Cl(-) on metal ions resulted mostly in reduction of metal ability to form strongly bound metal-organic compounds, in accordance with the order of stability constant of complex ions log K: Cd>Zn>Cu. Flow-through (dynamic) contact mode, which is the most appropriate to simulate environmental conditions, appeared to strongly attenuate the complexing effect of chloride ions on Cd and Zn sorption, and significantly enhance sorption capacity also in the absence of complexing ions. For Cd, it was mainly due to the enrichment in the strongly bound "insoluble organic" fraction, while for Zn the quantitative increase of sorption capacity did not alter significantly its partitioning. Neither a quantitative nor qualitative effect of contact mode on Cu binding was observed. Complex and diverse effects of different environmental parameters on metal sorption capacity and binding strength onto organic matter, which strongly influence metal mobility, leads to the conclusion that the correct simulation of these parameters for ecotoxicological testing is crucial for the reliable predicting of metal bioavailability under actual terrestrial environmental conditions.     

Transfer factors of (134)Cs to crops from Typic Haplustept under tropical region as influenced by potassium application

Under greenhouse condition a pot culture investigation was carried out using Inceptisol soil (Typic Haplustept) contaminating with (134)Cs @ 1muCikg(-1) soil to study the transfer factor to Mustard, Gram, Spinach and Wheat crops as influenced by potassium application (0, 27.3, 54.6 and 81.9mgKkg(-1) soil). Potassium application in general improved the biomass, grain yield and also the potassium concentration in all the crops. Irrespective of the crops, (134)Cs transfer factor to straw and grain was highest in control treatment (no K addition) and found to decrease significantly with increase in K application levels. The (134)Cs uptake was highest in Spinach followed by Mustard, Gram and Wheat crops. The weighted transfer factor values (straw plus grain) to Spinach, Mustard, and Gram were observed to be 5.54, 4.38 and 2.20 times higher as compared to Wheat crop.     

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.     

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.