An in situ method for remediating 137Cs-contaminated wetlands using naturally occurring minerals

Cesium's enhanced bioavailability in contaminated wetlands onthe U.S. Department of Energy's Savannah River Site (SRS) is thoughtto be due to the low clay fraction of SRS soils, and that the clay mineralogyis dominated by kaolinites. Remediation of the wetlands is problematic becausecurrent technologies are destructive to the sensitive ecosystems. We tested11 clay minerals (two micas, a vermiculite, six illites, a kaolinite, anda smectite) for their propensity to sorb and retain ¹³⁷Cs. Twominerals were subsequently chosen as candidates for in situ remediation amendmentmaterials because they had ¹³⁷Cs distribution coefficients (K d) well in excess of 10,000 ml . g –1 , and desorbed less than 20% ofthe Cs when mixed in a 0.1M NH 4 Cl solution. Incremental additions of thecandidate minerals to ¹³⁷Cs-contaminated sediments appreciablyintercepted and retained desorbed ¹³⁷Cs in the presence of highlevels of NH₄ . Implications for using the minerals as a nondestructive,in situ remediation technique are discussed.     

Plutonium isotopes and 137Cs in Dolon settlement near the Semipalatinsk Nuclear Test Site: About 50 years after the first nuclear weapon testing

Recent controversies concerning the radiation doses for populations living in the village of Dolon due to the nuclear explosions carried out at the Semipalatinsk Nuclear Test Site (SNTS) have encouraged us to evaluate in more detail the levels and distributions of residual long-lived radionuclides¹³⁷Cs and Pu isotopes (²³⁸Pu,^239,240Pu) in soils within the village. Soil core samples up to a depth of about 30 cm and/or 100 cm were collected at 25 sites and subjected to analysis of ¹³⁷Cs and Pu isotopes. The inventories of ¹³⁷Cs and ^239,240Pu were found to be in the wide range of 790-10,310 and 530-14,320 Bq/m², respectively. Sequential leaching of Pu from the soil showed that more than ca. 80% of the ^239,240Pu was not leached by hot digestion with conc. HNO³ + H₂O₂, indicating the presence of Pu associated with fused silicates. Further, the presence of hot-particles from the Pu contaminants by a-track radiography technique using CR-39 polycarbonate was confirmed in the soil, even at present, after about 50 years from the first nuclear weapon testing. This revised version was published online in July 2006 with corrections to the Cover Date.     

Variability in 137Cs inventories and potential climatic and lithological controls in the central Ebro valley, Spain

The extent of soil erosion in some Spanish semiarid regions has caused great concern regarding the sustainability of soil resources. Accelerated soil erosion, particularly in some Mediterranean areas, is likely to be one of the main environmental problems associated with climate change. Fallout ¹³⁷Cs has been shown to provide a reliable basis for assessing soil erosion rates in different environments around the world. However, existing information concerning the spatial variation of ¹³⁷Cs inventories at reference sites has identified a need for further investigation of the factors affecting their spatial variability in semiarid environments, where stony and skeletal soils are predominant. Reference sites at three locations in the central Ebro valley were selected to investigate the ¹³⁷Cs content of several grain size fractions. Each site included both natural vegetated conditions and cultivated land and the three sites were characterized by different values of mean annual rainfall. The results obtained demonstrate the influence of lithology, land use and climate on the spatial variability of ¹³⁷Cs inventories that increase from 1190, to 1500 and 1710 Bq·m^?2 with increasing annual rainfall values from 300 to 500 mm at the study sites. The soils on marls at the Valareña site had the highest proportion of ¹³⁷Cs in the coarse fractions of cultivated soils (12%) in comparison with soils developed on limestones at Loma Negra (5%), whereas no ¹³⁷Cs content was found in the coarse fractions of soils on glacis-terrace materials at Peñaflor. The ¹³⁷Cs reference inventories are higher in soils on marls and sands at cultivated locations at Valareña and Peñaflor, but have similar values in soils at cultivated and uncultivated locations on limestones at Loma Negra. Therefore, in absence of level undisturbed soils with natural vegetation cover, cultivated flat soils on hard rocks could provide reliable reference inventories.     

The effect of sorption properties of soil minerals on the vertical migration rate of cesium in soil

The vertical distribution of¹³⁷Cs is shown for two types of soil: silly loamy “supposed” soil and silly lessive one, slightly eroded, occuring in the vicinity of Lublin (Eastern Poland). Based on the distribution data the vertical migration rates of¹³⁷Cs are calculated for both soils. These rates are found to be 0.045 and 0.3 cm/year respectively. The percent contribution of¹³⁷Cs originating from the damaged reactor in Chernobyl is also calculated. The kinetics of cesium adsorption and its adsorption isotherms on minerals separated from the tested soils are also studied. The sorption of Cs on soil minerals markedly affects the migration rate of¹³⁷Cs in soil. The experimental results indicate that, among the extracted mineral fractions, the largest adsorption takes place on marls from the silly loamy soil. This work is supplemented by results of a physicochemical analysis of the studied soils.     

Influence of major cations of sea water on the desorption of137Cs from marine sediments

Desorption studies of¹³⁷Cs from marine sediments by artificial sea water and artificial sea water devoid of individual major cations such as Na, K, Ca, Mg and Sr indicated that only Na and K were effective in the desorption of¹³⁷Cs. Studies with various ionic strengths ranginf from 0.01 to 1.6M KCl and NaCl solutions showed that KCl desorbs constantly about 45%¹³⁷Cs at and above an ionic strength of 0.1. In case of NaCl, the percent desorption increases linearly with ionic strength. The difference in desorption by K and Na is attributed to the contraction of the clay mineral layers by K ion and expansion of the layers by Na ion.     

Leaching behavior of137Cs in cement

To assess the safety of disposal of a radioactive waste-cement composite, the leaching of¹³⁷Cs from a waste composite into a surrounding fluid has been studied. Leaching tests were carried out in accordance with a method recommended by IAEA.¹ The leachability was measured as a function of bentonite clay to cement ratio. The fraction of¹³⁷-Cs leached from a specimen of Portland cement is 0.03–0.13 at a leaching time of 400 d. Results presented in this paper are examples of data obtained in a 10 y mortar and concrete testing project, which will influence the design of the engineered trench system for a future Yugoslav radioactive waste storage center.^2,3     

Mobility of 137Cs Related to Speciation Studies in Contaminated Soils of the Chernobyl Area

Chernobyl derived ¹³⁷Cs present in upper soil layers can still remain available to cation exchange and hence to downward migration. More than its physico-chemical deposit forms (fuel particles and/or condensed aerosols), radiocesium mobility is influenced by soil properties. Although all the soils studied contain illitic clay minerals, different ¹³⁷Cs fixation levels were observed due to: (1) the reactivity state of sorption sites with a low radiocesium content in soil, and (2) the presence, or absence, of organic matter complexes inhibiting cation sorption on clays.     

Movement of Phosphamidon in Soil Columns

Abstract

Adsorption and movement of phosphamidon, a systemic non-ionic insecticide, was studied using two different types of Indian soil, clay loam and silt loam, of alluvial origin. Equilibrium adsorption coefficient, K, values determined by batch slurry technique were in the order: clay loam>silt loam. The distribution coefficient, K_d , for both soils in batch adsorption as well as in columns was also calculated. The phosphamidon movement measured in soil columns during water infiltration was in the order: silt loam > clay loam. This order was anticipated from the K and K_d values. A larger amount of water was needed for leaching the phosphamidon to 60 inches in clay loam than in silt loam soil.     

Removal of226Ra(II) from uranium mining and processing effluents

The activity of¹³⁷Cs was determined in mosses and their surrounding soils in three Venezuelan cloud forests. The concentration of¹³⁷Cs in both the mosses and their respective soils were correlated with elevation (m.a.s.l.). This relationship was the result of the cloud forest effect, no direct deposition by condensation below the base of the clouds and increasing deposition of¹³⁷Cs with the density of the clouds. The ratio of the activity of¹³⁷Cs in the mosses to their surrounding soils was in general the same for sites near the top of the mountains, but the ratio at the Altos de pipe location was 3.5 times higher than that of the La Sierra mountain. This was explained by the difference in the water content of the surface and the top soil layer. It was concluded that the¹³⁷Cs measured in the mosses was from the soil effect rather than new deposition of¹³⁷Cs in the last three years.     

Study on the Horizontal Transport of Some Radionuclides in the Wieprz River Valley

A horizontal transport of radionuclides was studied by the analysis of the radioactivity of the surface soil samples from valleys of Wieprz river and its bottom sediments. Natural gamma-isotopes (⁴⁰K, ²³⁸U and ²³²Th series) antropogenic (¹³⁴Cs and ¹³⁷Cs) and alpha-isotopes ²³⁸Pu and ^239,240Pu were measured. The different kind of bed rock and terrain configuration, influenced the radionuclide transportation from the soil to river bottom sediments. Radioactivity of the sediment samples is definitely lower than the soils. Very strong adsorption of isotopes in soil hinders their horizontal migration. Calculated ²³⁸Pu/^239,240Pu ratio is characteristic for global fallout and about 90% of the ¹³⁷Cs comes from Chernobyl.     

Development of a method for nuclide leaching from glass fiber in HEPA filter

For the disposal of the high efficiency particulate air (HEPA) glass filter to environment, the glass fiber should be leached to lower its radioactive concentration. To derive the optimum method for removal of Co and Cs from HEPA glass fiber, four methods were applied in this study. Results of electrochemical leaching of glass fiber by 4.0 M HNO₃–0.1 M Ce(IV) solution showed that the removal efficiency of ¹³⁴Cs, ¹³⁷Cs, and ⁶⁰Cs from glass fiber after 5 h was 96.4, 93.6, and 93.8%, respectively. Results by 5 wt% NaOH solution showed that the removal efficiency of ¹³⁴Cs, ¹³⁷Cs, and ⁶⁰Cs after 30 h was 81.7, 82.1, and 10.0%, respectively. Results by repeat 2.0 M HNO₃ solution showed that the removal efficiencies of ¹³⁴Cs, ¹³⁷Cs, and ⁶⁰Cs after 2 h of three repetitions were 96.2, 99.4, and 99.1%, respectively. Finally, results by repeat 4.0 M HNO₃ solution showed that the removal efficiencies of ¹³⁴Cs, ¹³⁷Cs, and ⁶⁰Cs after 4 h of three repetitions were 100, 99.9, and 99.9%, respectively, and their radioactivities were below 0.1 Bq/g. Therefore, the chemical leaching method by 4.0 M HNO₃ solution was considered as an optimum one for removal of cesium and cobalt from HEPA glass fiber for self disposal. Also the removal efficiencies of ⁶⁰Co, ¹³⁴Cs, and ¹³⁷Cs from the waste-solution after its precipitation-filtration treatment for reuse of 4.0 M HNO₃ waste-solution were 88.0, 95.0, and 99.8%.     

Determination and spatial distribution of <Superscript>137</Superscript>Cs in soils,mosses and lichens near Kavanayen,Venezuela

The activity of ¹³⁷Cs was determined in soils, mosses, lichens and other vegetation along the Caruay River and near the town of Kavanayen. The range of values for the soils was from <1.2 Bq·kg⁻¹ of ¹³⁷Cs (our detection limit) to 14.1 Bq·kg⁻¹. The range of ¹³⁷Cs activities in the mosses ranged from 9.9 to 17.9 Bq·kg⁻¹ with a mean value of 13.4±4 Bq·kg⁻¹; all the moss samples were found along the river. While the ¹³⁷Cs activities in the lichens ranged from 9.1 to 29.8 Bq·kg⁻¹; the two values along the river were about three factors higher than the one near Kavanayen. It was concluded that the ¹³⁷Cs activities in the soils, mosses and lichens are much higher along the river in respect to the nearby town of Kavanayen.     

Sources of 137Cs fluvial export from a forest catchment evaluated by stable carbon and nitrogen isotopic characterization of organic matter

Fluvial export of particulate and dissolved ¹³⁷Cs was investigated to reveal its sources and transfer mechanisms in a broadleaved forest catchment using a continuous collection system. The finest size fraction (<75 µm), consisting of decomposed litter and surface mineral soil, was the dominant fraction in the particulate ¹³⁷Cs load, although the contribution of coarser size fractions increased during high water discharge in 2014. The dissolved ¹³⁷Cs originated from the decomposition of ¹³⁷Cs-contaminated litter. Temporal changes in ¹³⁷Cs distribution in the litter–mineral soil system indicated that the dissolved ¹³⁷Cs load will be moderated in several years, while particulate ¹³⁷Cs load has the potential to continue for a long time.

     

Relationships among <Superscript>137</Superscript>Cs, <Superscript>133</Superscript>Cs,and K in plant uptake observed in Japanese agricultural fields

Plant uptake of radiocesium (¹³⁷Cs) was investigated in consideration of the relationships with naturally existing ¹³³Cs and potassium (K). We first determined plant-unavailable fraction of ¹³⁷Cs in soil by batch sorption and sequential extraction methods with a radiotracer. Then, using the data obtained from the batch sorption and extraction methods, we clarified the relationships of plant-available and plant-unavailable fractions between ¹³⁷Cs, ¹³³Cs, and K in soil. Additionally, ¹³⁷Cs concentrations in crop were estimated using ¹³⁷Cs in soil and several factors, i.e. fixation ratio of ¹³⁷Cs in soil, cation exchange capacity, and K concentration in crop. The results implied that the fixation ratio of ¹³⁷Cs in soil was a very important key to understanding ¹³⁷Cs plant uptake.     

Investigation of the leaching behavior of components of the magnesium potassium phosphate matrix after high salt radioactive waste immobilization

The samples of the magnesium potassium phosphate (MPP) matrix have been synthesized during solidification of the simulator of acid intermediate level waste. The main phase of the obtained samples corresponds to MgK_1?x(NH₄)_xPO₄ × 6H₂O. The behavior of the matrix components during leaching with bidistilled water according to the semi-dynamic test GOST R 52126-2003 has been studied. The high hydrolytic stability of the MPP matrix to leaching of ¹³⁷Cs, ⁹⁰Sr, ²³⁹Pu and ²⁴¹Am exceeding the stability of the cement matrix has been shown. It has been found that the components leaching process is controlled by various mechanisms due to the formation of the salts with different solubility.     

Soil-to-plant transfer factors of fallout <Superscript>137</Superscript>Cs and native <Superscript>133</Superscript>Cs in various crops collected in Japan

In order to compare the soil-to-plant transfer factors (TFs) of fallout ¹³⁷Cs and those of native stable ¹³³Cs, concentrations of these isotopes were determined in various crops and the associated soils collected throughout Japan. The results showed that TF-¹³⁷Cs was 11 times higher than TF-native ¹³³Cs for brown rice, while those values were almost the same for leafy vegetables. Possibly, fallout ¹³⁷Cs would be more mobile and more easily adsorbed by plants than native ¹³³Cs in the soil because a part of the ¹³³Cs is in a soil structure where it is hard to replace with ¹³⁷Cs. However, ¹³⁷Cs and native ¹³³Cs have reached an approximately isotopic equilibrium in the bioavailable fraction in the soils, therefore, the TF-native ¹³³Cs can be used for long-term transfer of ¹³⁷Cs in the environment.     

Depth profiles of long lived radionuclides in Chernobyl soils sampled around 10 years after the accident

Depth profiles of the long-lived radionuclides, ¹³⁷Cs, ⁹⁰Sr, Pu isotopes and ²⁴¹Am were examined in undisturbed sandy, peaty and Podsol soils in the Chernobyl 30 km exclusion zone sampled around 10 years after the accident. Two Podsol soils, which have different radioactive deposition characteristics, have also been examined. Activity ratios of ^239,240Pu/¹³⁷Cs, ⁹⁰Sr/¹³⁷Cs, and ²⁴¹Am/¹³⁷Cs in the 0-1 cm layer of the two Podsol soils differed very much. Speciation of the radionuclides by sequential selective extraction was examined in the soils. Depth profiles of the soils have been analyzed according to the speciation results and soil characteristics.     

Fractionation of 137Cs and 60Co in soils by sequential extractions

Comparison of six sequential extraction schemes either widely used or specifically developed for speciation of ¹³⁷Cs and ⁶⁰Co in two types of soil (Chromic Luvisol and Eutric Fluvisol) is presented. The results from the comparison show that extractable radiocesium in Chromic Luvisol (14%) is about three times lower than in Eutric Fluvisol (39%). For Chromic Luvisol the total extractable radiocobalt varies from 42 to 78% while the variation for Eutric Fluvisol is not so substantial (55–83%). The results show that BCR and NIST schemes developed for heavy metals are not efficient for radiocesium fractionation, but give very good results in the case of radiocobalt. The efficiency of a scheme is dependant not only on the type of radionuclide but on the type of soil as well. The best reagent for evaluation of bioavailable cesium is NH₄NO₃ or other NH⁺ ₄-salt. Practically most of the radiocobalt is in extractable form in both soils (about 83%) and major part of radiocesium (more than 60% depending on the soil type) is strongly bound in the soils and not extractable.     

The Effect of Carbonate Soil on Transport and Dose Estimates for Long-Lived Radionuclides at a U.S. Pacific Test Site

The United States conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are cesium-137, strontium-90, plutonium-239+240 and americium-241. Cesium-137 in the coral soils is more available for uptake by plants than ¹³⁷Cs associated with continental soils of North America or Europe. Soil-to-plant ¹³⁷Cs median concentration ratios (CR) (kBq·kg^-1 dry weight plant/kBq·kg^-1 dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, ⁹⁰Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of ¹³⁷Cs and ⁹⁰Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for ^239+240Pu and ²⁴¹Am are very similar to those observed in continental soils. Values range from 10^-6 to 10^-4 for both ^239+240Pu and ²⁴¹Am. No significant difference is observed between the two in coral soil. The uptake of ¹³⁷Cs by plants is enhanced because of the absence of mineral binding sites and the low concentration of potassium in the coral soil. Cesium-137 is bound to the organic fraction of the soil, whereas ⁹⁰Sr, ^239+240Pu and ²⁴¹Am are primarily bound to soil particles. Assessment of plant uptake for ¹³⁷Cs and ⁹⁰Sr into locally grown food crops was a major contributing factor in: (1) reliably predicting the radiological dose for returning residents and (2) developing a strategy to limit the availability and uptake of ¹³⁷Cs into locally grown food crops.     

Examination of the modified monostandard method in neutron activation analysis

The reproducibility, the small scale as well as the large scale variability of¹³⁷Cs extracted sequentially from the soil by using a modified Tessier procedure was investigated at several grassland sites in Bavaria/Germany and in the Chemobyl area. Because undisturbed grassland soils are never homogeneous with respect to their soil properties, all sequential extractions at the German sites were carried out at each plot separately for different soil layers (e.g., 0–2, 2–5, 5–10, 10–15, 15–20 and 20–30 cm). The results show that the coefficients of variation (CV) for the reproducibility of the extraction procedure for¹³⁷Cs was (with some exceptions) around 10–20% for all fractions. For the small scale variability of¹³⁷Cs (samples within an area of 10×10m²) the values for theCV were (again with a few exceptions) in the same range. Compared to that, the large scale variability of extractable¹³⁷Cs (random soil samples within an area of 100×200 km²) was higher for all fractions, even though only moderately. The implications of these results with respect to a sampling design are discussed.