Soil contamination with radionuclides and potential remediation

Soils contaminated with radionuclides, particularly 137Cs and 90Sr, pose a long-term radiation hazard to human health through exposure via the foodchain and other pathways. Remediation of radionuclide-contaminated soils has become increasingly important. Removal of the contaminated surface soil (often up to 40 cm) or immobilization of radionuclides in soils by applying mineral and chemical amendments are physically difficult and not likely cost-effective in practicality. Reducing plant uptake of radionuclides, especially 137CS and 90Sr by competitive cations contained in chemical fertilizers has the general advantage in large scale, low-level contamination incidents on arable land, and has been widely practiced in central and Western Europe after the Chernobyl accident. Phytoextraction of radionuclides by specific plant species from contaminated sites has rapidly stimulated interest among industrialists as well as academics, and is considered to be a promising bio-remediation method. This paper examines the existing remediation approaches and discusses phytoextraction of radionuclides from contaminated soils in detail.     

Effect of ectomycorrhizae and ammonium on 134Cs and 85Sr uptake into Picea abies seedlings

Microorganisms play an important role in the fixation of radionuclides in forest soils. In particular, fungi have the capacity to absorb and translocate radionuclides. The role of the ectomycorrhizal fungus Hebeloma crustuliniforme in the uptake of radiocaesium (134Cs) and radiostrontium (85Sr) into seedlings of Norway spruce (Picea abies) was investigated in a pouch test system. Inoculated and non-inoculated seedlings; seedlings inoculated during 8 and 15 weeks; seedlings exposed during 2 and 3 weeks to the radioactive solution; and seedlings grown under low and high ammonium conditions prior to the application of the radionuclides were compared. The final 134Cs and 85Sr activity was determined in fine-roots, main-roots, stems and needles. The results showed that ectomycorrhizae reduced the uptake of 134Cs and 85Sr. The degree of ectomycorrhization was of crucial importance and seemed to be governed by the period during which ectomycorrhizae were allowed to develop and by the ammonium concentration in the nutrient solution. The radionuclide uptake increased with increasing exposure time. Both radionuclides were predominantly accumulated in fine-roots. However, needles proved to describe best the result of net root uptake and translocation to the shoot. The uptake-and and translocation-rates of 85Sr were smaller than those of 134Cs. It is assumed that the translocation is coupled with the intensity of water fluxes through the xylem and that 85Sr is more readily adsorbed into mycelium or plant tissue relative to 134Cs. The effect of high ammonium growth conditions was overcome by the effect of ectomycorrhization, except in needles with a very large biomass which behaved as a strong sink and led to a high accumulation of 134Cs.     

Lower variability of radionuclide activities in upland dairy products compared to soils and vegetation: implication for environmental survey

Contamination of the environment by radionuclides is usually estimated using soil and grass sampling. However, radionuclides are often not homogeneously distributed in soils. In the alpine Mercantour region (Western Alps, France) a large heterogeneity in Chernobyl 137Cs deposition has been previously observed. Here we report additional 137Cs results together with new 90Sr and Pu data for soil, grass, milk, and cheese samples. The results show that radioisotopes from nuclear weapons tests fallout are more homogeneously distributed than Chernobyl 137Cs. Further, we observe that the 137Cs and 90Sr contents are less variable in milk samples than in grass or soil samples. This can be attributed to the homogenization effect of cow vagrancy during grazing. Hence milk seems to be a more robust sample than soil or grass to evaluate the extent of contamination on a regional scale. We explore this idea by comparing own unpublished 90Sr results and 90Sr results from the literature to establish the relationship between altitude of grazing and contamination of soil and milk for Western Europe. There is a significant positive correlation between soil contamination and altitude and an even closer correlation between milk 90Sr activity (A) and altitude (h): A = A0 + e(k x h) where A0 is the expected activity of milk sampled at sea level (A0 = 0.064 +/- 0.014 Bq g(-1) Ca) and h is the altitude of grazing, k being a constant (k = 0.95 x 10(-3) +/- 0.11 x 10(-3) m(-1) Bq g(-1) Ca). The fact that there is less scattering in the relationship for the 90Sr(milk)-altitude than for 90Sr(soil)-altitude suggests, again, that milk is a well-suited sample for environmental survey. The relationship between the altitude of grazing and the 90Sr content of milk and cheese can also be used to assess the authenticity of dairy products.     

Impact of an exceptional Saharan dust outbreak in France: PM10 and artificial radionuclides concentrations in air and in dust deposit

The present study focuses on the exceptional Saharan dust event that affected most of France in February 2004. Activity levels of various artificial radionuclides (⁹⁰Sr, ¹³⁷Cs, uranium, thorium and plutonium isotopes, ²⁴¹Am) were examined. Activity or isotopic ratios are discussed in the context of atmospheric nuclear weapons tests, among them French tests performed in Sahara in the 1960s. The daily evolution of ¹³⁷Cs activity levels in the atmosphere was compared to daily PM₁₀ change. A link between airborne ¹³⁷Cs and PM₁₀, is given. It is estimated that this 2-day event deposited as much ¹³⁷Cs as would be deposited on average over a 10-month period. The amount of deposited ¹³⁷Cs and ^239+240Pu represents respectively about 0.1 and 1% of the activity already present in the soil. Such Saharan dust events correspond to an extreme type of “feeder” process of artificial radionuclides in the atmosphere. Therefore, they contribute to the long term background level of artificial radionuclides kept at trace levels in the atmosphere.     

Application of molluscs for radioecological monitoring of the Chernobyl outburst

Accumulation of radionuclides was studied in molluscs from the territories polluted by the Chernobyl outburst. In addition to radiochemical evaluation of (90)Sr, a simple method of beta-radiometry of shells was applied which allowed processing of extensive samples and mapping of contamination of large territories: the Dnieper drainage area and the Kiev administrative region. Pre-Hiroshima and pre-Chernobyl radioactivity was investigated in museum collections. Differences in (90)Sr accumulation in molluscs of different genera were demonstrated for freshwater and terrestrial snails, an especially high accumulation factor was found in Helix. Indices of relative accumulation were calculated treating Lymnaea stagnalis as a standard. All the measurements were recalculated to this standard in order to provide comparisons between sampling sites disregarding collected species and to reduce variance before mapping. Based on shell beta-activity measurements, the average accumulation factor for (90)Sr in Lymnaea compared to its concentration in the river water was about 5000, its transfer factor compared to the soil contamination was about 0.1 m(2) kg(-1), figures for (137)Cs were smaller by an order of magnitude. Inverse dependence between free calcium content in the environment and the transfer factor was demonstrated, as well as a difference in (90)Sr/(137)Cs ratio in molluscs collected on different tracks of Chernobyl pollution. Monitoring the biologically accessible and biologically active fraction of (90)Sr contamination, the shell beta-activity above 15 kBq kg(-1) indicates a dangerous level of contamination for the human population.     

Rice uptake and distributions of radioactive 137Cs, stable 133Cs and K from soil

The distributions of radionuclides in plant components as to radionuclide transfer to animals are important for understanding the dynamics of radionuclides in an agricultural field. Most of the non-edible parts in these components are returned to the soil as organic fertilizer where they may again be utilized in the soil-plant pathway and/or are mixed with feed for livestock. Rice plants were grown in an experimental field and separated at harvest into different components, including polished rice, rice bran, hull, leaves, stem and root, and then the distributions of radioactive 137Cs, stable 133Cs and K in these components were determined. The distribution of 137Cs in polished rice and rice bran was similar to that of 133Cs, while that of K was different. The concentration ratios of 133Cs/K in leaf blade positions increased with aging, which means that the translocation rate of 133Cs in rice plants was slower than that of K. At harvest the distribution of dry weight in polished rice to entire rice plants was 34%, and the distributions of 133Cs in the polished rice and the non-edible parts were 7 and 93%, respectively, whereas those of K in the polished rice and the non-edible parts were 2 and 98%, respectively. Findings suggest that the transfer and distribution of 133Cs, not of K, provide better information on the long-term fate of 137Cs in an agricultural environment.     

Plant uptake of radionuclides in lysimeter experiments

The results of seven years lysimeter experiments to determine the uptake of 60Co, 137Cs and 226Ra into agricultural crops (endive, maize, wheat, mustard, sugarbeet, potato, Faba bean, rye grass) are described. The lysimeter consists of twelve monolithic soil profiles (four soil types and three replicates) and is located in Seibersdorf/Austria, a region with a pannonian climate (pronounced differences between hot and semi-arid summers and humid winter conditions, annual mean of precipitation: 517 mm, mean annual temperature: 9.8 degrees C). Besides soil-to-plant transfer factors (TF), fluxes were calculated taking into account biomass production and growth time. Total median values of TF's (dry matter basis) for the three radionuclides decreased from 226Ra (0.068 kg kg(-1)) to 137Cs (0.043 kg kg(-1)) and 60Co (0.018 kg kg(-1)); flux values exhibited the same ranking. The varying physical and chemical properties of the four experimental soils resulted in statistically significant differences in transfer factors or fluxes between the investigated soils for 137Cs and 226Ra, but not for 60Co. Differences in transfer between plant species and plant parts are distinct, with graminaceous species showing, on average, TF values 5.8 and 15 times lower than dicotyledonous species for 137Cs and 60Co, respectively. This pattern was not found for 226Ra. It can be concluded that 137Cs transfer is heavily influenced by soil characteristics, whilst the plant-specific factors are the main source of TF variability for 60Co. The variability of 226Ra transfer originates both from soil properties and plant species behaviour.     

Possible change in Asian dust source suggested by atmospheric anthropogenic radionuclides during the 2000s

Decades-long monitoring of anthropogenic radionuclides in the atmospheric deposition in Tsukuba, Japan suggests not only the substantial impacts of the Asian dust (Kosa) on the deposition but also the possible change of the Kosa source region, especially during springs of the 2000s. In order to know more about such change, 4 single wet deposition events occurred in the spring of 2007 were scrutinized. The largest anthropogenic radionuclides wet deposition was supplied by the April 2–4 event. It brought several tens % of the monthly depositions (April 2007) of the dust (residue) mass (4.5 g m^?2) and anthropogenic radionulides (⁹⁰Sr: 16, ¹³⁷Cs: 97 and Pu: 3 mBq m^?2). None of the events observed fulfilled both criteria of the specific activities and ⁹⁰Sr/¹³⁷Cs activity ratio to the Tsukuba soil; they did not exhibit local soil dust signature. The Kosa events in fact have extensive impacts on the atmospheric environment over Japan in spring season. Considering the elevated specific activities as well as greater ¹³⁷Cs/⁹⁰Sr activity ratio in the deposited dust, it is hypothesized that the dust source areas in Asian continent would be shifting from the arid zone to the desert-steppe zone suffering from desertification during the 2000s. This type of the Kosa may be called as the ‘new-regime Kosa’. Chemical observation in the far downwind region of the Kosa dust could allow us to know possible shift in the source regions.     

Seasonal variation of radionuclides in Fucus vesiculosus L. from the Oresund, Southern Sweden

The activity concentrations of radionuclides (60Co, 54Mn, 137Cs, 40K) in whole plants of Fucus vesiculosus of different ages, and also in tissues of different ages from the same plants were investigated in the vicinity of the Barseb?ck nuclear power plant in southern Sweden. Activity concentration differed between the tissues of different age of the plants, depending on the radionuclide as well as the time of year. The highest concentrations of 60Co and 54Mn were measured in the older parts of the plants in spring and summer, while the activity concentrations of 137Cs and 40K were highest in receptacles and new vegetative fronds. The discharge of radionuclides from the nuclear power plant was reflected in the measured activity concentration in the algae. For 60Co, the response seemed to be smoothed out when considering the whole plant, while the new vegetative tissue better reflected the discharge during the autumn. Thus, it is important to have knowledge about the autecology of the organism when it is used as an indicator for radionuclides.     

The influence of season and leaf age on concentrations of radiocaesium (137Cs), stable caesium (133Cs) and potassium in Agrostis capillaris

The transfer of radioactive caesium from soils to plants has been well researched. In contrast there is limited knowledge on natural stable 133Cs and its potential role as a predictor for radiocaesium behaviour. In a pot experiment with Agrostis capillaris close correlations were found between plant 137Cs and plant 133Cs concentrations (R2 90-96%). Season and leaf age had significant effects with concentrations increasing 10-30-fold between June and December. Simultaneously the plant concentrations of K, the nutrient analogue of Cs, decreased to around one third. In the soil the exchangeable fractions of K and 137Cs declined. No clear relationships were found between 137+133Cs in the plant and exchangeable K in the soil. However, at the end of the experiment the K content of the above-ground biomass was higher than the exchangeable pool in the soil, suggesting that depletion of soil K could be a key factor in the observed increase of plant 137+133Cs over time.     

Ecological half-life of caesium in roe deer (Capreolus capreolus)

Biological half-lives for various radionuclides have been determined for many animals kept in the laboratory or under controlled conditions. Only occasionally has been it possible to determine the ecological half-lives of radionuclides in wild animals, where the contamination has occurred in their natural habitats. Following the fallout from the Chernobyl accident and its subsequent ingestion by wildlife, no one knew how long it would take the wild animals to eliminate the radionuclides, and in particular radiocaesium, from their bodies. In this study of roe deer (Capreolus capreolus), bucks (males)were shot at weekly/fortnightly intervals from mid-May till the end of July, as part of the annual cull on an area, which included some young forestry (Stone Chest-National Grid Reference NY48090), planted in 1971/72. The ration of 137Cs:134Cs, typical of the Chernobyl fallout, was seldom observed in these animals due to the highly variable concentrations of 137Cs originating from bomb fallout. Therefore, 134Cs was used instead because its presence was almost entirely due to the Chernobyl fallout. After using log10 transformation of the 134Cs concentrations, a significant (p < 0.01) regression was obtained which accounted for 85% of the variation. From the regression, the ecological half-life for 134Cs was found to be 28.3 days.     

Uptake of radionuclides by vegetation at a High Arctic location

Radionuclide levels in vegetation from a High Arctic location were studied and compared to in situ soil concentrations. Levels of the anthropogenic radionuclide 137Cs and the natural radionuclides 40K, 238U, 226Ra and 232Th are discussed and transfer factor (TF) values and aggregated transfer (Tag) values are calculated for vascular plants. Levels of 137Cs in vegetation generally followed the order mosses > lichen > vascular plants. The uptake of 137Cs in vascular plants showed an inverse relationship with the uptake of 40K, with 137Cs TF and Tag values generally higher than 40K TF and Tag values. 40K activity concentrations in all vegetation showed little correlation to associated soil concentrations, while the uptake of 238U, 226Ra and 232Th by vascular and non-vascular plants was generally low.     

Phytoremediation of radiostrontium ((90)Sr) and radiocesium ((137)Cs) using giant milky weed (Calotropis gigantea R.Br.) plants

Potential of plants to remove radionuclides/toxic elements from soils and solutions can be successfully applied for removal of important radionuclides such as strontium-90 (⁹⁰Sr) and cesium-137 (¹³⁷Cs). When uptake of ¹³⁷Cs and ⁹⁰Sr by Calotropis gigantea plants incubated in distilled water spiked with the radionuclides either alone or in combination was studied, it was found to have a high efficiency for the removal of ⁹⁰Sr, with 90% being removed from solutions (5 × 10³ kBq l⁻¹) within 24 h of incubation. However, in case of ¹³⁷Cs, about 44% could be removed from solutions (5 × 10³ kBq l⁻¹) at the end of 168 h of incubation. Accumulation of ⁹⁰Sr and ¹³⁷Cs was higher in roots compared to shoots. The plants could remediate both ⁹⁰Sr and ¹³⁷Cs when they were added together to the solution. When two months old plants were incubated in low level nuclear waste, 99% of activity disappeared at the end of 15 days. The present study suggests that C. gigantea could be used as a potential candidate plant for phytoremediation of ⁹⁰Sr and ¹³⁷Cs.     

A simplified approach to modelling underground migration of radionuclides from contaminated river sediments

Accidental releases of waste water from the first Czechoslovak nuclear power plant, A1, caused contamination of sediments of the Dudváh river, flowing into the Vah river, in Slovakia. Rather high concentrations of ¹³⁷Cs and ⁹⁰Sr (2150Bq dm⁻³ and 215Bq dm⁻³, respectively) were found in bottom sediments of a former channel of the re-engineered river body at a distance of about 250 m from a village, Siladice, with water-supply wells. In order to assess the possibility of contamination of the wells, underground migration of both radionuclides from the contaminated area was simulated using an original layered convection-diffusion model. K_d values determined in laboratory experiments were used. The analysis of the hydrological situation in the area reveals that the critical condition is a dominant horizontal groundwater flow near the water table in the direction from the Váh bank to Siladice, in the periods when the contaminated body lies under the water table. The simulation calculated under conservative conditions showed that the contamination of water-supply wells would not exceed permissible concentration limits.     

Nuclear contamination sources in surface air of Finnish Lapland in 1965–2011 studied by means of 137Cs, 90Sr,and total beta activity

Environmental Science and Pollution Research - Radionuclides 137Cs and 90Sr and total beta activity were determined from air filters collected in Rovaniemi (Finnish Lapland) in 1965–2011....     

Distribution coefficients (Kd) and desorption rates of Cs and Am in Black Sea sediments

The distribution coefficients (K_d) and desorption rates of ¹³⁷Cs and ²⁴¹Am radionuclides in bottom sediments at different locations in the Black Sea were studied under laboratory conditions. The K_d values were found to be 500 for ¹³⁷Cs and 3800 for ²⁴¹Am at the steady state and described exponential curves. Rapid uptake of the radionuclides occurred during the initial period and little accumulation happened after four days. The desorption rates for ¹³⁷Cs in different bottom sediments were best described by a three-component exponential model. The desorption half-times of ¹³⁷Cs ranged from 26 to 50 d at the slow components. However, the desorption rate of ²⁴¹Am described one component for all sediment samples and desorption half-time was found to be 75 d. In general, the results showed that the ²⁴¹Am radionuclide is more effectively transferred to bottom sediment and has longer turnover time than ¹³⁷Cs under Black Sea conditions.     

Role of magnetite and humic acid in radionuclide migration in the environment

Sorption of ¹³⁷Cs, ⁹⁰Sr, ¹⁵⁴Eu and ¹⁴¹Ce by magnetite has been studied at varying pH (4 to 11) in the presence and absence of humic acid. The sorption studies have also been carried out at varying ionic strength (0.01 to 0.2 M NaClO₄) and humic acid concentration (2 to 20 mg/L). Percentage sorption of ¹³⁷Cs and ⁹⁰Sr was found to be pH dependent, with the sorption increasing with increasing pH of the suspension. At any pH, the percentage sorption of ⁹⁰Sr was higher than that of ¹³⁷Cs. The results have been explained in terms of the electrostatic interaction between the positively charged metal ions and the surface charge of the magnetite which becomes increasingly negative with increasing pH. On the other hand, ¹⁵⁴Eu and ¹⁴¹Ce were found to be strongly sorbed by the magnetite at all pH values, with the sorption being independent of pH. The strong sorption of trivalent and tetravalent metal ions suggests the role of complexation reactions during sorption, apart from the electrostatic interactions. However, in the case of ¹⁴¹Ce surface precipitation of Ce(III) formed by reduction of Ce(IV) in the presence of magnetite cannot be ruled out. Presence of humic acid (2 mg/L) was found to have negligible effect on sorption of all metal ions.     

Radionuclides in pinon pine (Pinus edulis) nuts from Los Alamos National Laboratory lands and the dose from consumption

One of the dominant tree species growing within and around the eastern portion of Los Alamos National Laboratory (LANL), Los Alamos, NM, lands is the pinon pine (Pinus edulis). Pinon pine is used for firewood, fence posts, and building materials and is a source of nuts for food--the seeds are consumed by a wide variety of animals and are also gathered by people in the area and eaten raw or roasted. This study investigated the (1) concentration of 3H, 137Cs, 90Sr, totU, 238Pu, 239,240Pu, and 241Am in soils (0- to 12-in. [31 cm] depth underneath the tree), pinon pine shoots (PPS), and pinon pine nuts (PPN) collected from LANL lands and regional background (BG) locations, (2) committed effective dose equivalent (CEDE) from the ingestion of nuts, and (3) soil to PPS to PPN concentration ratios (CRs). Most radionuclides, with the exception of 3H in soils, were not significantly higher (p < 0.10) in soils, PPS, and PPN collected from LANL as compared to BG locations, and concentrations of most radionuclides in PPN fromLANL have decreased over time. The maximum net CEDE (the CEDE plus two sigma minus BG) at the most conservative ingestion rate (10 lb [4.5 kg]) was 0.0018 mrem (0.018 microSv); this is far below the International Commission on Radiological Protection (all pathway) permissible dose limit of 100 mrem (1000 microSv). Soil-to-nut CRs for most radionuclides were within the range of default values in the literature for common fruits and vegetables.     

Radiocaesium activity concentrations in potatoes in Croatia after the Chernobyl accident and dose assessment

Systematic investigations of (137)Cs and (134)Cs activity concentrations in potatoes (Solanum tuberosum) for the post-Chernobyl period (1986-2005) in the Republic of Croatia are summarized. The correlation between (137)Cs activity concentrations in fallout and potatoes, has been found to be very good, the correlation coefficient being r = 0.88 with P(t) < 0.001 for 18 degrees of freedom. As the radiocaesium levels in potatoes decreased exponentially, the mean residence time of (137)Cs in potatoes was estimated by fitting the measured activity concentrations to the exponential curve. The mean residence time was found to be 6.8 +/- 1.1 years, the standard deviation being estimated by the Monte Carlo simulations. The initial observed (134)Cs:(137)Cs activity ratio in potatoes has been found to be quite variable, but slightly lesser than the theoretically predicted value of 0.5, calculated by applying the known inventory of these radionuclides in the Chernobyl reactor to the equation for the differential radioactive decay. This can be explained by presence of the pre-Chernobyl (137)Cs in soil that originated from nuclear fallout. The annual effective doses received by (134)Cs and (137)Cs intake due to consumption of potatoes estimated for an adult member of the Croatian population were found to be very small, as the per caput Dose for the entire 1986-2005 period was calculated to be about 2.9 microSv, (134)Cs accounting approximately for 1/3 of the entire dose. Therefore, after the Chernobyl accident consumption of potatoes was not the critical pathway for human intake of radiocaesium from the environment in Croatia.     

Transport of radionuclides in natural fractures: some aspects of laboratory migration experiments

Results are reported for a series of migration experiments performed in a hydraulically characterized, single, natural fracture in a block of granite with overall dimensions of 1 × 1 × 0.7 m (all approximate), using the conservative, poorly sorbing and strongly sorbing radionuclides ³H₂0, ¹³¹I, ²²Na, ⁸⁵Sr, ¹³⁷Cs, ⁶⁰Co, ^154,155Eu, ²³⁷Np, and ²³⁸Pu. The volumetric flow velocity of the transport solution was 3 ml h⁻¹, giving a residence time in the fracture of approximately 50 h. Elution profiles were obtained for ³H₂0, ¹³¹I, ²²Na, ⁸⁵Sr and ¹³⁷Cs but no evidence of the other radionuclides was observed in the eluent. Results from supporting static sorption measurements on crushed geological materials and granite coupons showed in general higher sorption on alteration minerals than on granite. Sorption was lowest for ²²Na and ⁸⁵Sr.The migration of ¹³¹I, ²²Na, ⁸⁵Sr through the fracture in real time was followed using end-window Geiger-Müller probes located in unused boreholes. Additional information, obtained by alpha and gamma scanning of the fracture surfaces after separating the block along the fracture, confirmed that transport had occurred along the flow path predicted from the hydraulic characterization of the fracture and that, over a 5.5 month period, the bulk of the injected ¹³⁷Cs had migrated only 75 cm along the flow path. The ⁶⁰Co, the rare earths and the actinides had not moved beyond the location of the injection borehole, suggesting that fracture infilling minerals played a major role in retarding radionuclide transport. Additional confirmation of the role of secondary minerals in radionuclide retardation was obtained using selective sequential extraction on the fracture surfaces. These observations support the inclusion of sorption data for fracture infilling minerals in the sorption database developed for the geosphere model for the Canadian Nuclear Fuel Waste Management Program.