Interception of radionuclides by planophile crops: A simple semi-empirical modelling approach in case of nuclear accident fallout.

Shortly after an atmospheric release, the interception of radionuclides by crop canopies represents the main uptake pathway leading to food chain contamination. The food chain models currently used in European emergency decision support systems require a large number of input parameters, which inevitably leads to high model complexity. In this study, we have established a new relationship for wet deposited radionuclides to simplify the current modelling approaches. This relationship is based on the hypothesis that the stage of plant development is the key factor governing the interception of radionuclides by crops having horizontally oriented leaves (planophile crops). The interception fraction (f) and the leaf area index normalized (fLAI) and mass normalized (fB) interception fractions were assessed for spinach (Spinacia oleracea) and radish (Raphanus sativus) at different stages of plant development and for different contamination treatments and plant densities. A database of 191 f values for Cs-137 and Th-229 was built and complemented with existing literature covering various radionuclides and crops with similar canopy structure. The overall f increased with the plant growth, while the reverse was observed for fB. The fLAI significantly decreased by doubling the contaminated rainfall deposited. Fitting a multiple linear regression to predict the f value as a function of the standing biomass (B), and the radionuclide form (anion and cation) led to a better estimation of the interception (R2 = 81%) than the ECOSYS-87 model (R2 = 35%). Hence, the simplified modelling approach here proposed seems to be a suitable risk assessment tool as fewer parameters will minimize the model complexity and facilitate the decision-making procedures in case of emergencies, when countermeasures need to be identified and implemented promptly.

Uranium and cadmium provoke different oxidative stress responses in Lemna minor L.

Common duckweed (Lemna minor L.) is ideally suited to test the impact of metals on freshwater vascular plants. Literature on cadmium (Cd) and uranium (U) oxidative responses in L. minor are sparse or, for U, non-existent. It was hypothesised that both metals impose concentration-dependent oxidative stress and growth retardation on L. minor. Using a standardised 7-day growth inhibition test, the adverse impact of these metals on L. minor growth was confirmed, with EC50 values for Cd and U of 24.1 ± 2.8 and 29.5 ± 1.9 µm, respectively, and EC10 values of 1.5 ± 0.2 and 6.5 ± 0.9 µm, respectively. The metal-induced oxidative stress response was compared through assessing the activity of different antioxidative enzymes [catalase, glutathione reductase, superoxide dismutase (SOD), ascorbate peroxidase (APOD), guaiacol peroxidase (GPOD) and syringaldizyne peroxidase (SPOD)]. Significant changes in almost all antioxidative enzymes indicated their importance in counteracting the U- and Cd-imposed oxidative burden. However, some striking differences were also observed. For activity of APODs and SODs, a biphasic but opposite response at low Cd compared to U concentrations was found. In addition, Cd (0.5-20 µm) strongly enhanced plant GPOD activity, whereas U inhibited it. Finally, in contrast to Cd, U up to 10 µm increased the level of chlorophyll a and b and carotenoids. In conclusion, although U and Cd induce similar growth arrest in L. minor, the U-induced oxidative stress responses, studied here for the first time, differ greatly from those of Cd.

Predicting the environmental risks of radioactive discharges from Belgian nuclear power plants.

An environmental risk assessment (ERA) was performed to evaluate the impact on non-human biota from liquid and atmospheric radioactive discharges by the Belgian Nuclear Power Plants (NPP) of Doel and Tihange. For both sites, characterisation of the source term and wildlife population around the NPPs was provided, whereupon the selection of reference organisms and the general approach taken for the environmental risk assessment was established. A deterministic risk assessment for aquatic and terrestrial ecosystems was performed using the ERICA assessment tool and applying the ERICA screening value of 10 µGy h(-1). The study was performed for the radioactive discharge limits and for the actual releases (maxima and averages over the period 1999-2008 or 2000-2009). It is concluded that the current discharge limits for the Belgian NPPs considered do not result in significant risks to the aquatic and terrestrial environment and that the actual discharges, which are a fraction of the release limits, are unlikely to harm the environment.

Diffusive gradient in thin FILMS (DGT) compared with soil solution and labile uranium fraction for predicting uranium bioavailability to ryegrass.

The usefulness of uranium concentration in soil solution or recovered by selective extraction as unequivocal bioavailability indices for uranium uptake by plants is still unclear. The aim of the present study was to test if the uranium concentration measured by the diffusive gradient in thin films (DGT) technique is a relevant substitute for plant uranium availability in comparison to uranium concentration in the soil solution or uranium recovered by ammonium acetate. Ryegrass (Lolium perenne L. var. Melvina) is grown in greenhouse on a range of uranium spiked soils. The DGT-recovered uranium concentration (C(DGT)) was correlated with uranium concentration in the soil solution or with uranium recovered by ammonium acetate extraction. Plant uptake was better predicted by the summed soil solution concentrations of UO(2)(2+), uranyl carbonate complexes and UO(2)PO(4)(-). The DGT technique did not provide significant advantages over conventional methods to predict uranium uptake by plants.

Evolution of pH, organic matter and (226)radium/calcium partitioning in U-mining debris following revegetation with pine trees.

Natural attenuation processes resulting from the afforestation of some U-waste rock piles have the potential to limit the linkage of radioelements and other trace pollutants, thereby minimizing exposure risks. We determined the evolution of pH and organic matter and compared the (226)Ra and Ca extractability in pyrite-containing mining debris which was revegetated 35 years ago with Scots pine. Oxidation of sulphidic minerals remaining in the substrate appeared to dominate over acidification processes due to vegetation inputs and litter decomposition. The accumulation of organic matter in forest floor had a negligible effect on the (226)Ra upward recycling compared to the migration losses observed mainly from decarbonatation of the surface mining debris. (226)Ra was overall less soluble than Ca in the soil profile but NH(4)Ac-pH 5 had the capacity to extract a (226)Ra fraction of 31.1-41.5%, i.e. at least twice as much as for Ca. In deeper layers, a majority of both Ca and (226)Ra were extractable from the same non-specific adsorption pool, which mainly involved carbonate. In the upper acidified layer, the incorporation of organic matter had no effect on (226)Ra extractability. A further specific adsorption pool for (226)Ra was attributed to the formation of sparingly soluble Fe-Al oxyhydroxides. However, that specific (226)Ra-bearing phase was readily dissolved in NH(4)Ac-pH 5, indicating a relatively reversibility of the precipitation reaction of (226)Ra with amorphous oxide. Trees are effective at reducing hydrological release of many pollutants but in the mining debris studied, four decades of pine growth did not significantly promote (226)Ra remediation in the soil.

Predicting radium availability and uptake from soil properties.

The results of a potted soil experiment to determine the soil and plant factors ruling radium availability and uptake by ryegrass and clover are described. Nine soils with distinct soil characteristics were spiked with 226 Ra. They were thoroughly characterized and the solid liquid partitioning coefficient, Kd, was determined. Kd ranged from 38 l kg(-1) to 446 l kg(-1) (average: 188+/-156 l kg(-1)) and was linearly related to cation exchange capacity (CEC) and organic matter (OM) content. The soil-to-plant transfer factor (TF) was significantly affected by the chemical properties of the soils and ranged from 0.054 kg kg(-1) to 0.719 kg kg(-1) for ryegrass and from 0.034 kg kg(-1) to 1.494 kg kg(-1) for clover. Overall, no significant difference in TF between ryegrass and clover was observed. TF was related to Kd, to CEC, OM (for ryegrass only when excluding one soil) and the calcium concentration in the soil solution (for both plants if excluding one soil). Radium flux were calculated from the radium concentration in the soil solution and the evapotranspiration, to predict total radium uptake derived from shoot radium concentration and biomass yield. It was found that radium uptake could be predicted from the radium flux (R2=0.61 and 0.83 for ryegrass and clover, respectively). Higher predictability (R2=0.70 and 0.91 for ryegrass and clover, respectively) was obtained when relating total radium uptake to a radium flow considering competition effects at the root surface by bivalent cations.

Method of diffusive gradients in thin films (DGT) compared with other soil testing methods to predict uranium phytoavailability.

The measurement of diffusive gradients in thin films (DGT) has been proposed as a surrogate for metal uptake by plants. A small-scale experiment was performed to test the predictive capacity of the DGT method with respect to uranium availability and uptake by ryegrass. Correlation analyses were performed to compare the results obtained with the DGT device with more conventional bioavailability indices - concentration of uranium in pore water or in selective extracts. Six soils with different uranium contamination history and with distinct soil characteristics were used for the availability tests and the uptake experiment. The four uranium bioavailability indices screened were highly correlated, indicating that at least partially comparable uranium pools were assessed. The uranium concentration in the pore water was a better predictor for uranium uptake by ryegrass than amounts of uranium recovered following extraction with 0.11 M CH3COOH or 0.4 M MgCl2, the fractions considered exchangeable according to, respectively, the BCR or NIST standardized sequential extraction methods. The DGT measured concentration, C(DGT), was also highly correlated with plant uptake but the significance level was sensitive to the value of the diffusion coefficient (pH depend or not) used to calculate C(DGT). From the results obtained it could not be concluded that the DGT method would have an additional value in assessing uranium bioavailability.

Can we predict uranium bioavailability based on soil parameters? Part 1: effect of soil parameters on soil solution uranium concentration.

Present study aims to quantify the influence of soil parameters on soil solution uranium concentration for (238)U spiked soils. Eighteen soils collected under pasture were selected such that they covered a wide range for those parameters hypothesised as being potentially important in determining U sorption. Maximum soil solution uranium concentrations were observed at alkaline pH, high inorganic carbon content and low cation exchange capacity, organic matter content, clay content, amorphous Fe and phosphate levels. Except for the significant correlation between the solid-liquid distribution coefficients (K(d), L kg(-1)) and the organic matter content (R(2)=0.70) and amorphous Fe content (R(2)=0.63), there was no single soil parameter significantly explaining the soil solution uranium concentration (which varied 100-fold). Above pH=6, log(K(d)) was linearly related with pH [log(K(d))=-1.18 pH+10.8, R(2)=0.65]. Multiple linear regression analysis did result in improved predictions of the soil solution uranium concentration but the model was complex.

Can we predict uranium bioavailability based on soil parameters? Part 2: soil solution uranium concentration is not a good bioavailability index.

The present study aimed to quantify the influence of soil parameters on uranium uptake by ryegrass. Ryegrass was established on eighteen distinct soils, spiked with (238)U. Uranium soil-to-plant transfer factors (TF) ranged from 0.0003 to 0.0340kgkg(-1). There was no significant relation between the U soil-to-plant transfer (or total U uptake or flux) and the uranium concentration in the soil solution or any other soil factor measured, nor with the U recovered following selective soil extractions. Multiple linear regression analysis resulted in a significant though complex model explaining up to 99% of variation in TF. The influence of uranium speciation on uranium uptake observed was featured: UO(2)(+2), uranyl carbonate complexes and UO(2)PO(4)(-) seem the U species being preferentially taken up by the roots and transferred to the shoots. Improved correlations were obtained when relating the uranium TF with the summed soil solution concentrations of mentioned uranium species.

Oxidative stress reactions induced in beans (Phaseolus vulgaris) following exposure to uranium.

The present study aimed to analyze the biological effects induced by bioaccumulation of uranium in Phaseolus vulgaris. Ten-day-old seedlings were exposed to 0, 0.1, 1, 10, 100 and 1000 microM U in diluted Hoagland solution. Following 1, 2, 4 and 7 days' exposure, plants were monitored for uranium uptake, biometric parameters, capacities of enzymes involved in the anti-oxidative defense mechanisms (GPOD, SPOD, GLUR, SOD, ICDH, G-6P-DH), glutathione (GSH) pool and DNA integrity. Uranium contents were up to 900-fold higher in roots (31-14,916 mg kg(-1) FW following 7 days' exposure to 0.1 and 1000 microM U, respectively) as compared to primary leaves (1-16 mg kg(-1) FW following 7 days' exposure to 0.1 and 1000 microM U, respectively). Uranium exposure did not significantly affect plant growth compared to the control. For all enzymes studied, except SOD, enzyme capacities in roots were slightly stimulated with increasing contaminant concentrations (though not significantly). For roots exposed to 1000 microM U, enzyme capacities were significantly reduced. Enzyme capacities in leaves were not affected by uranium treatment. Total and reduced GSH levels were higher in primary leaves of uranium (

Plant-induced changes in soil chemistry do not explain differences in uranium transfer.

A greenhouse experiment was set up with maize, ryegrass, Indian mustard, wheat and pea to evaluate to what extent differences in uranium (U) transfer factors can be explained by root-mediated changes in selected soil properties. The experiment involved an acid and an alkaline soil contaminated with (238)U. U soil-to-shoot transfer factors (TFs) ranged between 0.0005 and 0.021 on the acid soil and between 0.007 and 0.179 on the alkaline soil. Indian mustard showed the highest U uptake in shoots and maize the lowest. The root TFs, only available for the acid soil, ranged from 0.58 for maize and Indian mustard to 1.38 for ryegrass. The difference in U uptake between the two soils and the five plants was only partially explained by the different initial U concentrations in soil solution or differences in soil properties in the two soils. However, we obtained a significant relation for differences in shoot TFs observed between the two soils when relating shoot TFs with concentration of UO(2)(2+) and uranyl carbonate complexes in soil solution (R(2)=0.88). The physiological mechanisms by which root-to-shoot U transfer is inhibited or promoted seemed at least as important as the plant-induced changes in soil characteristics in determining soil-to-shoot TFs.

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.

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.

Can barium and strontium be used as tracers for radium in soil-plant transfer studies?

Radium is one of the prominent potential contaminants linked with industries extracting or processing material containing naturally occurring radionuclides. In this study we investigate if 133Ba and 85Sr can be used as tracers for predicting 226Ra soil-to-plant transfer. Three soil types were artificially contaminated with these radionuclides and transfer to ryegrass and clover was studied. Barium is considered a better tracer for radium than strontium, given the significant linear correlation found between the Ra and Ba-TF. For strontium, no such correlation was found. The relationship between soil characteristics and transfer factors was investigated. Cation exchange capacity, exchangeable Ca+Mg content and soil pH did not seem to influence Ra, Ba or Sr uptake in any clear way. A significant relation (negative power function) was found between the bivalent (Ca+Mg) concentration in the soil solution and the Ra-TF. A similar dependency was found for the Sr and Ba-TF, although less significant.

Phytoextraction for clean-up of low-level uranium contaminated soil evaluated.

Spills in the nuclear fuel cycle have led to soil contamination with uranium. In case of small contamination just above release levels, low-cost yet sufficiently efficient remedial measures are recommended. This study was executed to test if low-level U contaminated sandy soil from a nuclear fuel processing site could be phytoextracted in order to attain the required release limits. Two soils were tested: a control soil (317 Bq 238U kg(-1)) and the same soil washed with bicarbonate (69 Bq 238U kg(-1)). Ryegrass (Lolium perenne cv. Melvina) and Indian mustard (Brassica juncea cv. Vitasso) were used as test plants. The annual removal of soil activity by the biomass was less than 0.1%. The addition of citric acid (25 mmol kg(-1)) 1 week before the harvest increased U uptake up to 500-fold. With a ryegrass and mustard yield of 15,000 and 10,000 kg ha(-1), respectively, up to 3.5% and 4.6% of the soil activity could be removed annually by the biomass. With a desired activity reduction level of 1.5 and 5 for the bicarbonate-washed and control soil, respectively, it would take 10-50 years to attain the release limit. However, citric acid addition resulted in a decreased dry weight production.

A metabolic derivation of tritium transfer coefficients in animal products.

Tritium is a potentially important environmental contaminant originating from the nuclear industry, and its behaviour in the environment is controlled by that of hydrogen. Animal food products represent a potentially important source of tritium in the human diet and a number of transfer coefficient values for tritium transfer to a limited number of animal products are available. In this paper we present an approach for the derivation of tritium transfer coefficients which is based on the metabolism of hydrogen in animals. The derived transfer coefficients separately account for transfer to and from free (i.e. water) and organically bound tritium. A novel aspect of the approach is that tritium transfer can be predicted for any animal product for which the required metabolic input parameters are available. The predicted transfer coefficients are compared to available independent data. Agreement is good (R2=0.97) with the exception of the transfer coefficient for transfer from tritiated water to organically bound tritium in ruminants. This may be attributable to the particular characteristics of ruminant digestion. We show that tritium transfer coefficients will vary in response to the metabolic status of an animal (e.g. stage of lactation, diet digestibility etc.) and that the use of a single transfer coefficient from diet to animal product is inappropriate. It is possible to derive concentration ratio values from the estimated transfer coefficients which relate the concentration of tritiated water and organically bound tritium in an animal product to their respective concentrations in the animals diet. These concentration ratios are shown to be less subject to metabolic variation and may be more useful radioecological parameters than transfer coefficients. For tritiated water the concentration ratio shows little variation between animal products ranging from 0.59 to 0.82. In the case of organically bound tritium the concentration ratios vary between animal products from 0.15 (goat milk) to 0.67 (eggs).

Influence of levocabastine suspension on ciliary beat frequency and mucociliary clearance.

The effects of levocabastine, a new fast-acting, highly potent H1-antagonist, on nasal ciliary epithelial function were investigated in an in vitro and in vivo study. In the in vitro study, a suspension of levocabastine in Locke-Ringer solution was applied to 10 bioptic specimens of ciliated human adenoid tissue. Each specimen was exposed to the test solution for 60 min. Ciliary beat frequency (CBF) was recorded with a photoelectric recording device at 10-min intervals. There were small, insignificant decreases in CBF, which were minimal compared to that observed with ciliotoxic agents. In the in vivo study, 8 healthy volunteers were given, intranasally, one droplet of the levocabastine suspension. Mucociliary transit time (MTT) was measured by placing a saccharin particle drenched in indigo carmine in the nose just below the top of the concha and measuring the time until appearance of the dye in the pharyngeal cavity. No statistically significant differences were found in the MTT before and after application of the levocabastine suspension. The studies thus indicate that nasally administered levocabastine does not interfere with ciliary beat frequency and mucociliary function.

Radiocaesium metabolism in pregnant ewes and their progeny.

Pregnant ewes have been chronically contaminated during pregnancy and lactation with Cs-134 administered as CsCl in the food. Plateau concentrations in excreta and blood were reached after about 20 d of contamination. At delivery, the contamination levels in lamb's tissue were lower than those in the corresponding organs from an ewe; they increased rapidly as the lambs received milk from their contaminated dam, up to higher levels than in ewes. The transfer coefficient were estimated in various tissues from an ewe slaughtered at delivery (muscles 0.57 d/kg, kidneys 0.50 d/kg, liver 0.33 d/kg, blood 0.02 d/kg) and milk (0.09 d/l). During the decontamination phase, the radioactivity was excreted from the ewe's body according to a two exponential pattern with half-times of about 1.3 and 20 d. The retention in muscles, kidneys and liver from the ewes was characterised by two compartments with longer half-times of 2.3 to 2.9 d and 123 to 174 d respectively. The contamination levels in organs from lambs separated from their dam 3 days after birth and fed uncontaminated artificial milk decreased with a global half-time of about 10 d.

Technetium absorption and turnover in monogastric and polygastric animals.

Technetium (Tc) released into the environment can reach animals in various chemical forms: as pertechnetate (TcO-4) in drinking water or deposited on the surface of vegetables and forage plants, or as Tc bioincorporated into plants and associated with various plant constituents. In addition to being influenced by chemical speciation in the diet, absorption, metabolism, and retention of Tc in animals are modified by the treatment that the alimentary bolus undergoes during its passage through the gastrointestinal tract. This behavior differs markedly between polygastric and monogastric animals. We have, therefore, studied the fate of 99mTc given in the diet either as TcO-4 or bioincorporated into maize in rats (as an example of a monogastric animal) and in sheep (as an example of a polygastric animal). Urine and feces were collected and assayed for Tc activity by gamma spectrometry. Animals were sacrificed at different times after contamination, and the Tc content of tissues was determined. The pattern of absorption, excretion and, to a certain degree, of organ distribution and retention depended on animal species and species of Tc administered. Excretion was by feces and urine, and several metabolic components could be discerned. A component of very short half-time in urine suggests that newly absorbed Tc is more readily excreted than that already bound by tissues. The highest tissue concentrations were found in the thyroid. Retention of Tc was, however, most pronounced in bone and skin. Hair contains considerable amounts of Tc and may serve as a bioindicator of Tc contamination.

Autoxidation of catechol(amine)s.

The autoxidation of nine catecholamines and two catechols as a function of pH was studied. The reaction rate constants of the distinct charged particles, in which catechol(amine)s can appear, are proved to be independent of pH. Autoxidation appears to be a feasible system for the acquisition of data useful for structure (re)activity relationships.