A model testing study for the transfer of radioactivity to fruit

This paper compares predictions of the foodchain model SPADE with experimental data for the transfer of (134)Cs and (85)Sr to strawberry plants following acute foliar and soil contamination. The transfer pathways considered in this exercise included direct deposition to fruit, leaf-to-fruit, soil-to-leaf and soil-to-fruit transfers. Following foliar contamination, the difference between predicted and measured radionuclide activity values varied between a factor of 0.5-10 for fruit and 4.5-7 for leaf. Following soil contamination, the difference between predicted and measured values varied between a factor of 3-74 for fruit and 32-44 for leaf. In all cases the difference between measured and predicted values was smaller for (85)Sr than (134)Cs. Measured and predicted activities were higher for leaf than fruit. Both measured and predicted (134)Cs concentrations in fruit and leaf are higher when deposition occurs at ripening than at anthesis. These results confirm the need for more data on fruit, even for Cs and Sr, to support models in predicting the transfer of radionuclides to fruit crops. Ongoing research projects funded by the UK Food Standards Agency aim to provide some data on radionuclide transfer to herbaceous, shrub and tree fruits, which will help improve radiological assessment models in order to provide better protection for consumers.     

Foliar uptake of 134Cs and 85Sr in strawberry as function by leaf age

In this paper a study of the foliar uptake and translocation of 134Cs and 85Sr in a herbaceous fruit plant is presented. In particular, absorption, translocation and loss of these radionuclides in strawberry plants have been studied in relation to the age of contaminated leaves. Strawberry plants were contaminated by distributing droplets of an aqueous solution containing 134CsCl and 85SrCl2 on the surface of two leaves per plant. One half of the plants was contaminated through two young leaves, a second half through two old leaves. Sets of plants were collected 1 day, 7 days and 15 days after contamination. One half of them was rinsed with double distilled water before gamma analysis. Rinsing contaminated leaves removes on average 55% of the applied 134Cs and 45% of 85Sr. The activity removed decreases during the 15 days of the experimental study, both for 134Cs and for 85Sr, suggesting an increase in foliar absorption during this period. The activity removed does not differ between old and young leaves. "External loss" is lower for young than old contaminated leaves. "Internal loss" through translocation occurs mainly for 134Cs. Translocation coefficients from contaminated leaves to fruits are two orders of magnitude higher for 134Cs (4.0%), than for 85Sr (0.05%). Leaf to fruit translocation coefficients for 134Cs are higher from young leaves (5.8%), than from old leaves (2.3%).     

Post-deposition transport of radionuclides in fruit

This paper considers two main pathways for contamination of fruit by radionuclides: (i) absorption after deposition directly to exposed fruit surfaces, and (ii) absorption after deposition to other exposed plant surfaces followed by translocation to fruit. The aim is to collect the available information on fruit from temperate regions, identify the factors affecting post deposition processes in fruit plant systems, identify gaps in knowledge and give recommendations for future work. The majority of information available on above-ground absorption and further translocation to fruit concerns 134Cs and 85Sr in soluble form in apple, strawberry and grapevine. In general, 85Sr is absorbed and translocated to a lesser extent than is 134Cs. The rate of absorption and translocation depends on the physiological stage and age of the plant, and varies between different plant species and varieties.     

Evaluation of a model for leaf to fruit transfer of radionuclides in processing tomato plants using an independent set of data

Because of their varied possibilities of consumption, tomatoes are an important component of the human diet. This paper presents results of the evaluation of a dynamic model (Ventomod) for the short-term behaviour of radionuclides deposited on tomato plants following a direct contamination event. To check its forecasting capability in assessing the risk of radionuclide contamination of the human diet, it has been tested with an independent dataset on the leaf to fruit transfer of 134Cs in a typical Hungarian tomato variety, "Dwarf of Kecskemet". Data obtained from this pot experiment were used to evaluate model behaviour. Model constants were varied according to the differences between the Hungarian dataset and the one used to calibrate it. Results show that the model output well reproduces the observed activity of fruits for various levels of contamination and at different contamination dates. The main part of this report summarises the experimental protocol, compares the experimental results with model predictions generated by Ventomod and makes recommendations for both updating model parameters and undertaking further experimental work.     

Foliar and root uptake of Cs, Sr and Zn in processing tomato plants (Lycopersicon esculentum Mill.)

The results of an experimental study on the behaviour of ¹³⁴Cs, ⁸⁵Sr and ⁶⁵Zn in processing tomato plants grown in peat substrate are presented. Plants were contaminated by wet deposition of ¹³⁴Cs, ⁸⁵Sr and ⁶⁵Zn, either by sprinkling the above ground part at two phenological stages or by administering ¹³⁴Cs, ⁸⁵Sr and ⁶⁵Zn to the soil. The plants contaminated at the second phenological stage intercepted 38.3% less than those contaminated at the first stage, although leaf area increased by more than double. Transfer coefficients from peat soil to ripe fruit for ¹³⁴Cs are significantly higher than those for ⁸⁵Sr and ⁶⁵Zn. Leaf to fruit transfer coefficients for ¹³⁴Cs are one order of magnitude higher than for ⁶⁵Zn and two orders higher than for ⁸⁵Sr. Only when deposition affects fruits, as at the second phenological stage, are transfer coefficients to fruits similar for the three radionuclides.     

Plant uptake of 134Cs in relation to soil properties and time

134Cs uptake by sunflower and soybean plants grown on seven different soils and its relation to soil properties were studied in a greenhouse pot experiment. Soil in each pot was contaminated by dripping the 134Cs in layers, and sunflower and soybean plants were grown for three and two successive periods, respectively. 134Cs plant uptake was expressed as the transfer factor (TF) (Bq kg(-1) plant/Bq kg(-1) soil) and as the daily plant uptake (flux) (Bq pot(-1) day(-1)) taking into account biomass production and growth time. For the studied soils and for both plants, no consistent trend of TFs with time was observed. The use of fluxes, in general, provided less variable results than TFs and stronger functional relationships. A negative power functional relationship between exchangeable potassium plus ammonium cations expressed as a percentage of cation exchange capacity of each soil and 134Cs fluxes was found for the sunflower plants. A similar but weaker relationship was observed for soybean plants. The significant correlation between sunflower and soybean TFs and fluxes, as well as the almost identical highest/lowest 134Cs flux ratios, in the studied soils, indicated a similar effect of soil characteristics on 134Cs uptake by both plants. In all the studied soils, sunflower 134Cs TFs and fluxes were significantly higher than the respective soybean values, while no significant difference was observed in potassium content and daily potassium plant uptake (flux) of the two plants.     

Cs uptake by four plant species and Cs-K relations in the soil-plant system as affected by Ca(OH)2 application to an acid soil

Three rates of Ca(OH)₂ were applied to an acid soil and the ¹³⁴Cs uptake by radish, cucumber, soybean and sunflower plants was studied. The ¹³⁴Cs concentration in all plant species was reduced from 1.6-fold in the sunflower seeds to 6-fold in the soybean vegetative parts at the higher Ca(OH)₂ rate. Potassium (K) concentration in plants was also reduced, but less effectively. The significantly decreased ¹³⁴Cs-K soil to plant distribution factors (D.F.) clearly suggest a stronger effect of soil liming on ¹³⁴Cs than on K plant uptake. This observation was discussed in terms of ionic interactions in the soil matrix and within the plants. The results also indicated that the increased Ca²⁺ concentration in the exchange phase and in the soil solution along with the improved root activity, due to the soil liming, enhanced the immobilization of ¹³⁴Cs in the soil matrix and consequently lowered the ¹³⁴Cs availability for plant uptake.     

Ventomod: a dynamic model for leaf to fruit transfer of radionuclides in processing tomato plants (Lycopersicon esculentum Mill.) following a direct contamination event

This paper presents results on the calibration and validation of a model (Ventomod) for leaf to fruit transfer of (134)Cs, (85)Sr and (65)Zn in processing tomato plants after leaf contamination. Several models (e.g. FARMLAND) that deal specifically with the transfer of radionuclides to fruits are adaptations of models that were developed for agricultural crops such as leafy green vegetables. "Ventomod" represents a dynamic evaluation model exclusively built for the short-term behaviour of radionuclide depositions. It forecasts the level of radionuclide contamination in ripe processing tomato fruits following an accidental radionuclide release into the atmosphere. A validation of the developed model by data sets from an independent experiment showed that the model successfully reproduced the observed radionuclide distribution and dynamics in tomato fruits. The level of uncertainty was within the normal range of similar assessment models. For a more general use of this model further testing with independent data sets from experiments obtained under different environmental conditions and data from other horticulturally important plant species would be desirable.     

Assessment of the genotoxicity of 137Cs radiation using Vicia-micronucleus, Tradescantia-micronucleus and Tradescantia-stamen-hair mutation bioassays

Since the middle of the 20th century, ionizing radiations from radioactive isotopes including 137Cs have been investigated to determine their genotoxic impact on living organisms. The present study was designed to compare the effectiveness of three plant bioassays to assess DNA damage induced by low doses of 137Cs: Vicia-micronucleus test (Vicia-MCN), Tradescantia-micronucleus test (Trad-MCN) and Tradescantia-stamen-hair mutation test (Trad-SH) were used. Vicia faba (broad bean) and Tradescantia clone 4430 (spiderwort) were exposed to 137Cs according to different scenarios: external and internal (contamination) irradiations. Experiments were conducted with various levels of radioactivity in solution or in soil, using solid or liquid 137Cs sources. The three bioassays showed different sensitivities to the treatments. Trad-MCN appeared to be the most sensitive test (significative response from 1.5 kBq/200 ml after 30 h of contamination). Moreover, at comparable doses, internal irradiations led to larger effects for the three bioassays. These bioassays are effective tests for assessing the genotoxic effects of radioactive 137Cs pollution.     

Erosion of atmospherically deposited radionuclides as affected by soil disaggregation mechanisms

The interactions of soil disaggregation with radionuclide erosion were studied under controlled conditions in the laboratory on samples from a loamy silty-sandy soil. The fate of 134Cs and 85Sr was monitored on soil aggregates and on small plots, with time resolution ranging from minutes to hours after contamination. Analytical experiments reproducing disaggregation mechanisms on aggregates showed that disaggregation controls both erosion and sorption. Compared to differential swelling, air explosion mobilized the most by producing finer particles and increasing five-fold sorption. For all the mechanisms studied, a significant part of the contamination was still unsorbed on the aggregates after an hour. Global experiments on contaminated sloping plots submitted to artificial rainfalls showed radionuclide erosion fluctuations and their origin. Wet radionuclide deposition increased short-term erosion by 50% compared to dry deposition. A developed soil crust when contaminated decreased radionuclide erosion by a factor 2 compared to other initial soil states. These erosion fluctuations were more significant for 134Cs than 85Sr, known to have better affinity to soil matrix. These findings confirm the role of disaggregation on radionuclide erosion. Our data support a conceptual model of radionuclide erosion at the small plot scale in two steps: (1) radionuclide non-equilibrium sorption on mobile particles, resulting from simultaneous sorption and disaggregation during wet deposition and (2) later radionuclide transport by runoff with suspended matter.     

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.     

Vertical migration of 134Cs bearing soil particles in arid soils: implications for plutonium redistribution

Vertical migration of plutonium in soils at the Waste Isolation Pilot Plant (WIPP) and the Rocky Flats Environmental Technology Site (RFETS) was evaluated based on observed 134Cs migration in soil column experiments. After applying 134Cs-labeled soil particles to the surfaces of large, undisturbed soil cores collected from each site, resulting soil columns were subjected to experimental cycles of irrigation plus drying (treatment columns) or to cycles of irrigation only (control columns). Mean losses of 134Cs inventory from soil surfaces were 3.1 +/- 0.6% cycle(-1) and 0.7 +/- 0.6% cycle(-1) respectively for RFETS treatment and control columns. WIPP columns had mean respective losses of 1.3 +/- 1.2% cycle(-1) and 0.5 +/- 0.2% cycle(-1). Bulk transport of labeled soil particles through soil cracks was an important process in RFETS soils, accounting for 64-86% of total 134Cs migration. Colloidal transport processes governed migration in WIPP soils.     

Distribution of 137Cs in soil along Ta-han River Valley in Tau-Yuan County in Taiwan

Environmental 137Cs contamination was suspected from accidents at spent fuel storage pits of a research reactor site in the Ta-han River valley in Taiwan. In order to further characterize this contamination, soil samples were collected and measured by a gamma-spectroscopy system in 1999. It was found that 137Cs contamination is distributed up to 4 km from the reactor in an area covered mostly by rice and plant fields. 137Cs concentration in the topsoil ranged up to about 1000 Bq kg-1, as compared with soil beyond the contaminated area, which does not exceed 15 Bq kg-1. Spatial distribution of 137Cs was characterized by strong non-uniformity, which complicated our understanding of the distribution pathway of the radionuclides. The highest concentrations of 137Cs, up to more than 1000 Bq kg-1, were found within a few rice fields. The relative location of these rice fields and the water supplies from local streams suggested that the 137Cs was distributed along water pathways in the valley.     

Current contamination by 137Cs and 90Sr of the inhabited part of the Techa river basin in the Urals

Previous discharges of radioactivity from the Mayak Production Association plant in the Urals have resulted in considerable radionuclide contamination of the Techa River, and consequent high radiation doses during the late 1940s and 1950s to residents of villages along the Techa river. The most contaminated villages close to the site were evacuated in the period 1954-1962. The objective of this recent study was to conduct a preliminary assessment of the current radioactive contamination of soil, vegetation and foodstuffs in the two remaining villages closest to the Mayak site, Muslyumovo and Brodokalmak. The highest contamination levels in soil were found in the floodplain at 5.5 MBq m(-2) for 137Cs and 1.0 MBq m(-2) for 90Sr. Radionuclide contamination in soil of the villages was much lower, but exceeded that expected from global fallout. Data from 1207 measurements of 137Cs in milk and 1180 for 90Sr in milk for the period 1992-1999 were collated. There was no change with time in the 90Sr or 137Cs activity concentration in milk over the measured period. There were significantly higher 137Cs activity concentrations in milk sampled during the housed winter period in Muslyumovo compared with the grazing summer period, but compared to that for Brodokalmak or for either settlement for 90Sr. The highest measured activity concentrations in food products of 137Cs and 90Sr were found in river fish, waterfowl, poultry and milk. The measured activity concentrations of 137Cs and 90Sr in some animal products were higher than that expected from soil and vegetation from fields and pasture in the villages (not including the floodplain) confirming that the highly contaminated floodplains are contributing to contamination of some animal products.     

Fixation of Cs to marine sediments estimated by a stochastic modelling approach

Dumping of nuclear waste in the Kara Sea represents a potential source of radioactive contamination to the Arctic Seas in the future. The mobility of 137Cs ions leached from the waste will depend on the interactions with sediment particles. Whether sediments will act as a continuous permanent sink for released 137Cs, or contaminated sediments will serve as a diffuse source of 137Cs in the future, depends on the interaction kinetics and binding mechanisms involved. The main purpose of this paper is to study the performance of different stochastic models using kinetic information to estimate the time needed for Cs ions to become irreversibly fixed within the sediments. The kinetic information was obtained from 134Cs tracer sorption and desorption (sequential extractions) experiments, conducted over time, using sediments from the Stepovogo Fjord waste dumping site, on the east coast of Novaya Zemlya. Results show that 134Cs ions interact rapidly with the surfaces of the Stepovogo sediment, with an estimated distribution coefficient Kd(eq) of 300 ml/g (or 13m2/g), and the 134Cs ions are increasingly irreversibly fixed to the sediment over time. For the first time, stochastic theory has been utilised for sediment-seawater systems to estimate the mean residence times (MRTs) of Cs ions in operationally defined sediment phases described by compartment models. In the present work, two different stochastic models (i) a Markov process model (MP) being analogous to deterministic compartment models, and (ii) a semi-Markov process model (SMP) which should be physically more relevant for inhomogeneous systems, have been compared. As similar results were obtained using the two models, the less complicated MP model was utilised to predict the time needed for an average Cs ion to become irreversibly fixed in the Stepovogo sediments. According the model, approximately 1100 days of contact time between Cs ions and sediments is needed before 50% of the 134Cs ion becomes fixed in the irreversible sediment phase. while about 12.5 years are needed before 99.7% of the Cs ions are fixed. Thus, according to the model estimates the contact time between 137Cs ions leached from dumped waste and the Stepovogo Fjord sediment should be about 3 years before the sediment will act as an efficient permanent sink. Until then a significant fraction of 137Cs should be considered mobile. The stochastic modelling approach provides useful tools when assessing sediment-seawater interactions over time, and should be easily applicable to all sediment-seawater systems including a sink term.     

MUD: a Model to investigate the migration of 137Cs in the Urban environment and Drainage and sewage treatment systems

A model is presented for the migration of 137Cs in the urban environment, including the drainage systems and the sewage treatment plants, with flexibility to be adapted to different configurations common in urban areas. The dynamics of 137Cs is simulated both under natural evolution and in case of forced decontamination, which can have a direct impact on the radioactivity going to sewers. The model assesses the activity concentrated in sewage sludge and that discharged with the treated or untreated effluent to the receiving watercourse. Tests made for two post-Chernobyl contamination scenarios in Sweden show differences between model predictions and observed results within the range of the experimental uncertainties. An uncertainty and sensitivity analysis of the main model parameters indicates that some parameters may have a significant influence on the results of the model. Moreover, the model uncertainty is driven by a few parameters; therefore, additional research could be necessary into these parameters, aiming at simplifying the model without losing its predictive power.     

Equilibrium of radiocesium with stable cesium within the biological cycle of contaminated forest ecosystems

Concentrations of (137)Cs and stable Cs were determined in plant, mushroom, lichen and soil samples collected at two forest sites with different contamination levels in Belarus in 1998. The concentration of (137)Cs in soil was the highest in near-surface organic layers (Of and Oh horizons) and decreased with depth in the mineral layers, whereas the concentrations of stable Cs were almost constant in the soil profile. The levels of (137)Cs and stable Cs in biological samples varied depending both on the species and the plant part sampled. Even though different species and parts of the same species were included, the concentration ratios of (137)Cs to stable Cs were fairly constant for samples collected at the same forest site, and were in the same order of magnitude as the (137)Cs to stable Cs ratios for the organic soil layers. This finding suggests that (137)Cs, mainly deposited on the forest ecosystems from the Chernobyl accident in 1986, was well mixed with stable Cs within the biological cycle in the forest ecosystems by 1998. The transfer factor for each biological sample of (137)Cs was almost the same as that of stable Cs, if they were calculated based on the concentrations in the Of + Oh layer. This suggests that the stable-Cs-based transfer factor could be used as equilibrium transfer factor of (137)Cs for different types of biological samples in the forest.     

Monitoring of radionuclides contamination of soils in Shatsk National Natural Park (Volyn region, Ukraine) during 1994-2001

The results of studies of radionuclide contamination of the soils in the western part of the territory of Shatsk National Natural Park (ShNNP), Volyn region, Ukraine, performed during 1994-2001 are presented. Based on the experimental results, the three-dimensional plot of the 137Cs density contamination for the soils at the territory under investigation has been constructed. The monitoring during 1994-2001 of the 137Cs vertical distributions in the different kinds of soils from the Park and the forecasting of the distribution changes of the depth down to 50 cm for the sod loamy sandy gleyed loamy sand soil of the Park up to 2086 have been performed.     

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.     

Radioactivity concentrations of 40K, 134Cs, 137Cs, 90Sr, 241Am, 238Pu and 239+240Pu radionuclides in Jordanian soil samples

In November 2000, surface and core soil samples were collected from different regions of Jordan. The samples were analyzed by direct gamma spectrometry and combined radiochemical separation procedure to quantify (40)K, (134)Cs, (137)Cs, (90)Sr, (241)Am, (238)Pu and (239+240)Pu radioactivity. Concentrations (Bq.kg(-1) dry weight) have been observed to vary in the range 1.5-2.6 for (134)Cs, 2.8-11.4 for (90)Sr, and 0.13-0.48 for (241)Am, 0.016-0.062 for (238)Pu, 0.28-1.01 for (239+240)Pu and 155-543 for (40)K. The typical concentration of (137)Cs found in topsoils (0-2 cm) ranged in 7.5-576 Bq.kg(-1), dry weight. These values were greater than those observed in samples taken at greater depths (up to 32 cm). Activity ratios of (134)Cs/(137)Cs, (90)Sr/(137)Cs, (239+240)Pu/(137)Cs, (238)Pu/(137)Cs, (241)Am/(137)Cs, (239+240)Pu/(238)Pu and (241)Am /(238)Pu have mean values of 0.0049 (R=1), 0.29 (R=0.76), 0.41 (R=0.90), 0.39 (R=0.85), 0.41 (R=0.88), 7.72 (R=0.97) and 16.66 (R=0.98), respectively. The underlying concentrations were correlated and relatively higher than those reported in neighboring countries. One moss sample, as a biomonitor indicator, was measured and evaluated along with the soil samples. Its data showed higher concentrations of all measured radionuclides due to accumulations over years. The depth distribution of the fission product (137)Cs and the total deposition (Bq.m(-2)) were also studied in selected samples. Estimations of the annual effective dose equivalent due to (137)Cs-soil contamination showed values up to more than 200 microSv.