A study on radionuclide association with soil components using a sequential extraction procedure

Measurements performed in 1986–1988 demonstrate that most of the radiocesium isotopes (¹³⁷Cs and¹³⁴Cs) deposited after the Chernobyl accident are still located in the upper soil layers (0–2 cm). The vertical migration appears to be slow, and only a small fraction of the radiocesium has been transferred into the biological cycle. Sequential extraction techniques have been utilized in order to investigate the degree of binding or association between deposited radionuclides (¹³⁷Cs,¹³⁴Cs and⁹⁰Sr) and components in soil. The results indicate that a major fraction of the radiocesium is associated strongly with organic and mineral materials in the litter or upper soil layers: less than 10% is easily leachable. The distribution of¹³⁷Cs throughout the fractions was similar to that determined for naturally occurring stable cesium (¹³³Cs), implying that isotopic exchange had been extensive. For⁹⁰Sr, the results show a relatively high leachable fraction. Therefore, present results indicate that radiocesium should be less mobile, and less available for root uptake, than⁹⁰Sr in soil.     

Transfer of137Cs from soil to plants in a wet montane forest in subtropical Taiwan

The distribution of¹³⁷Cs in an undisturbed, multistoried, subtropical wet montane forest ecosystem surrounding Yuanyang Lake (lake surface level ca. 1670m, in northeastern Taiwan), was investigated. The mossy forest here represents a currently-rare perhumid temperate environment in subtropical region. The radioactivity concentration of¹³⁷Cs was determined by γ-spectroscopy with a Ge(Li) detector. Although the soil is extremely acidic (pH 3.3 to 3.6) and the rainfall is high,¹³⁷Cs is evidently retained in the organic layer. The radioactivity concentration of¹³⁷Cs in surface soil ranges from 28 to 71 Bq·kg⁻¹. The concentrations of¹³⁷Cs in the ground moss layer and litter were much lower than that in the soil organic layer, this suggests that¹³⁷Cs detected is not from the newly deposited radioactive fallout. The radioactivity concentration and transfer factor (TF) of¹³⁷Cs varied with plant species. Shrubs and ferns have higher values than a coniferous tree (Taiwan cedar). The TF in this ecosystem is as high as 0.21 to 1.88. The high values of TF is attributed to the abundance of the organic matter in the forest soils. The rapid recycling of¹³⁷Cs through the soil-plant system of this undisturbed multistoried ecosystem suggests the existence of an internal cycling that help the accumulation of¹³⁷Cs in this ecosystem.     

Vertical distributions of global fallout 137Cs and 14C in a Japanese forest soil profile and their implications for the fate and migration processes of Fukushima-derived 137Cs

Vertical distributions of global fallout ¹³⁷Cs and ¹⁴C were investigated in a Japanese forest soil in 2001. Even 38 years after the fallout, ¹³⁷Cs was still observed mostly in the uppermost 5 cm. A preferential accumulation of ¹³⁷Cs was found in a 1-cm-thick transition layer between organic-rich A and underlying B horizons. This unique observation indicated that ¹³⁷Cs migrated through the A horizon at a rate of 0.20 % year⁻¹ and the transition layer acted as a barrier for ¹³⁷Cs migration to deeper layers. The vertical distributions of ¹³⁷Cs and ¹⁴C were significantly correlated, suggesting a coupled downward migration of ¹³⁷Cs and organic matter on a time scale of decades, along the same physical pathways.

     

Plutonium and cesium isotopes in river waters in Japan

Concentrations of cesium isotopes and plutonium in river water samples in Japan, collected during the period from June 1985 to February 1987, have been measured. The total¹³⁷Cs concentrations in the Japanese river waters ranged from 0.063 to 1.89 mBq·l^–1. The portion of particulate¹³⁷Cs to total was observed to be less than 10 to 35%. The total^239,240Pu concentrations ranged from 0.56 to 1.93 Bq·l^–1. Particulate^239,240Pu occupied 13 to 95% of the total. After the Chernobyl fallout, elevated¹³⁷Cs concentrations were observed in the Japanese river waters as well as the detection of¹³⁴Cs, whereas there was no effect on the river plutonium from the Chernobyl fallout. The partition coefficients of¹³⁷Cs and plutonium between suspended particulate and dissolved phases in the Japanese rivers were determined: from 1.0·10⁴ to 3.2·10⁵ and from 4.1·10⁴ to 2.3·10⁶ for¹³⁷Cs and plutonium, respectively. The result suggests that these radionuclides, especially plutonium, are tightly associated with soil particles and/or suspended matter.     

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.     

In-Situ Sample Preparation for Radiochemical Analyses of Surface Water

A new method for radionuclide sample analysis of surface water has been demonstrated at the Savannah River Site, an U.S. Department of Energy manufacturing facility, currently in standby. The method makes use of selective solid phase extraction (SPE) disks being placed in a modified portable aqueous sampler. The analytes currently measured by this in-situ preparation are ⁹⁹Tc, ⁹⁰Sr, ¹³⁷Cs and ^58,60Co. The SPE disks are placed singly or in series in an automatic sampler; water is passed through the SPE disks at the time of collection. The disks are then returned to the laboratory for counting; no additional chemical separation is performed prior to analysis. The modified automatic samplers have been placed at several different locations around the Savannah River Site along side traditional samplers. The traditional samplers were used to collect water that was analyzed for the same analytes using standard laboratory methods. Most of the sample results were less than five times the method detection limit, thus a mean difference statistic was used to compare the data. Within the uncertainties of the methods, there was no statistical difference in the ⁹⁹Tc results, although a slight negative bias was observed for the in-situ ⁹⁰Sr results versus the laboratory method. The in-situ method produces a dissolved (<0.45µm) and particulate ¹³⁷Cs result, whereas the traditional laboratory method measures total activity in the sample. As expected, a negative bias was found between the dissolved in-situ result and the laboratory total ¹³⁷Cs result, and a positive bias between the in-situ total (dissolved plus particulate) and laboratory total ¹³⁷Cs result.     

EB-radiolysis of carbamazepine: in pure-water with different ions and in surface water

A method for the rapid and simultaneous monitoring of particulate and dissolved ¹³⁷Cs concentration in water was developed. This method uses pleated polypropylene nonwoven fabric filter to collect particulate radiocesium, and nonwoven fabric impregnated with Prussian blue (PB) to absorb dissolved radiocesium. The fabric was placed into cylindrical plastic cartridges (SS-cartridge and PB-cartridge). Traditional monitoring methods, such as evaporative concentration, often require time for pre-processing. However, this method described requires much less pre-processing time before the detection. Experiments conducted with simulated river water demonstrated that almost all of the suspended solids weight was collected in the SS-cartridge, and that more than 92 % of dissolved ¹³⁷Cs was absorbed onto the two PB-cartridges by 2.5 L/min flow rate when the range of the pH was 6–8. This device was applied to monitor Abukuma River water at two locations and the results were compared with those obtained using the filtrating and evaporative concentration method. The suspended solids concentration in river water, calculated by weight gain of the SS-cartridge and by sediment weight after filtration with a 0.45-μm membrane filter, agreed well. The radioactivity of the particulate and dissolved ¹³⁷Cs also agreed well in one of the two replications of this method. In addition, the required time for pre-processing was reduced by 60 times that by filtrating and evaporative concentration method. This method can separately collect and concentrate particulate and dissolved radiocesium rapidly and simultaneously in the field.     

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.     

Transfer of 137Cs and stable Cs in soil-grass-milk pathway in Aomori, Japan

The soil-to-grass transfer factors and grass-to-milk transfer coefficients were determined for ¹³⁷Cs and stable Cs in soil, grass and milk samples collected in Aomori Prefecture, Japan. The concentrations of ¹³⁷Cs in the soil and grass samples collected from 25 sampling sites were 13±12 Bq.kg^-1 and 2.0±2.1 Bq.kg^-1 dry wt., respectively. The geometric mean of soil-to-grass transfer factor of ¹³⁷Cs was 0.13 and its 95% confidence interval was 0.017-0.98. The transfer factor of ¹³⁷Cs was higher than that of stable Cs, and they had a positive correlation. The concentration of K in the soil affected both transfer factors. The concentration of ¹³⁷Cs in milk samples collected from 16 sites was 76±43 mBq.kg^-1 fresh wt. and had a good correlation with that of stable Cs. The geometric mean of grass-to-milk transfer coefficient of ¹³⁷Cs was 0.0027, assuming that a cow's total daily intake was 20 kg of dry grass. The transfer coefficient of ¹³⁷Cs was positively correlated with that of stable Cs.     

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.     

Estimation of background radiation levels and associated health risks in mineral rich district Chiniot,Pakistan

The mineral extraction activities may disturb the natural radioactivity, therefore current study aims to generate baseline data of natural radionuclides and anthropogenic ¹³⁷Cs before the start of industrial activities. Gamma spectrometry and gross alpha and beta counting systems were used for activity measurement in environmental samples. In soil, the mean activity of ²³²Th, ²²⁶Ra, ⁴⁰K and ¹³⁷Cs were determined as 79 (66–117), 47 (34–80), 823 (602–1159) and 1.3 (1.1–4.5) Bq kg^?1, respectively. The average annual effective dose rate (128.7 µSv h^?1) in the study area was twice higher than world’s average value. Indoor hazard index was greater than unity at two places; therefore, proper ventilation is proposed during construction.

     

Comparison of radioactive and stable cesium uptake in aquatic macrophytes affected by the Fukushima Dai-ichi Nuclear Power Plant accident

Concentrations of ^134+137Cs and ¹³³Cs in aquatic macrophytes, water, and sediment were measured in samples collected from Fukushima Prefecture, Japan. The concentrations of ¹³⁷Cs in submerged and floating-leaved plants were higher than the values for emergent plants according to their main Cs uptake mode. The geometric mean water-to-plant concentration ratio for ¹³⁷Cs and ¹³³Cs was comparable observed in submerged and floating-leaved plants, while the geometric mean sediment-to-plant concentration ratio for ¹³⁷Cs in emergent plants was higher than that of ¹³³Cs, which suggest that the mobility of Fukushima accident-derived ¹³⁷Cs is not in steady state 4–5 years after the accident.

     

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.     

Chernobyl radioactivity on the Black Sea coast of Turkey

After the Chernobyl reactor accident, Eastern Black Sea coast was one of the heavily contaminated regions of Turkey. Clouds loaded with radioactive isotopes arrived the region on May 1986 and emptied their contents with the heavy rains that are frequently seen in the region. In order to asses the current level of contamination, several different samples, moss, lichen, litter, surface soil and soil cores were collected on August 1994. Samples were brought to the laboratory and their moisture, pH and organic matter contents were determined. Gamma-ray spectra of the samples were collected with a HpGe detector. ¹³⁷Cs was the major isotope observed. Activity of most litter samples were below 1000 Bq/kg, while most of the moss samples had activities below 5000 Bq/kg, there were a few with higher ¹³⁷Cs activities. Surface soil samples generally had activities less than 2000 Bq/kg and depth profiles of cesium activities in the soil cores showed regional variations.     

Temporal and spatial variations of <Superscript>137</Superscript>Cs in the waters off a nuclear fuel reprocessing facility in Rokkasho,Aomori, Japan

Five survey cruises were carried out from 2004 to 2007 to determine ¹³⁷Cs concentrations in the water columns off Rokkasho Village, Aomori Prefecture, Japan, where the spent nuclear fuel reprocessing plant of Japan Nuclear Fuel Ltd has been undergoing test operation since March 2006. Seawater samples were collected with a large volume in situ filtration and concentration system at different depths in the water column. ¹³⁷Cs in particulate form could not be detected in the survey area. Dissolved ¹³⁷Cs showed temporal variation, especially in the surface water. Based on the results, it was concluded that no observable ¹³⁷Cs contamination was present in the investigated area. The distribution of ¹³⁷Cs concentrations was influenced by the mixing between the Tsugaru and Oyashio Currents.     

Anomalously high activities of <Superscript>137</Superscript>Cs in soils and vegetation on and near a diabase outcrop in La Sierra de Lema,Venezuela

As a result of routine soil sampling to determine the ¹³⁷Cs background activities country-wide in Venezuela, it was decided to further investigate El Mirador (Lookout) area at the base of the Sierra de Lema mountain range. In April 2003 (A), soil samples were collected at eight sites on and around the edge of the diabase outcrop to confirm that this area had anomalously high ¹³⁷Cs activities. In July 2003 (B), not only soil samples were collected again, but also black mat, palm tree leaves and trunks, fruit bushes leaves and its fruit and fern leaves. The ¹³⁷Cs content was measured by high resolution gamma-ray spectroscopy by a comparative method with reference materials. The ¹³⁷Cs activity values range from 16.3 to 30.8 Bq·kg-1 in the soil samples collected in July 2003, 20.7–32.1 Bq·kg⁻¹ for the black mat, 26.3–38.4 Bq·kg⁻¹ for the palm leaves, 16.8–31.2 Bq·kg⁻¹ for the palm trunks and 17.6–27.3 Bq·kg⁻¹ for the fruit bush leaves, while, the ¹³⁷Cs activity values for the whole fruit were between 23.4 and 30.7 Bq·kg⁻¹; but, the value of the ¹³⁷Cs activity in the center of the fruit (the edible part) was 51.6 Bq·kg⁻¹, and the value of the ¹³⁷Cs activity for the fern leaves was 51.8 Bq·kg⁻¹. Thus, most of the ¹³⁷Cs activity values determined in the soil, black mat and vegetation samples from El Mirador (Lookout) were considered anomalously high with respect to those found near the equator and in other areas of Venezuela. Only the center of the fruit from the Clusia grandiflora bushes and the fern leaves had high activity ratios, about a factor of three and could be considered as biomonitors that concentrate and retain the ¹³⁷Cs. Finally, these anomalously high ¹³⁷Cs activities have been attributed not only to the rich organic soils, as sinks, but also due to the affect of the cloud forests.     

Depth distribution of239,240Pu and137Cs in soils of South Korea

Depth distribution of^239,240Pu and¹³⁷Cs in the soils of South Korea have been studied. The average accumulated depositions were estimated roughly to be 54.8±32.1 Bq·m^–2 for^239,240Pu, 1.6±1.0 Bq· ·m^–2 for²³⁸Pu and 1982.8±929.1 Bq·m^–2 for¹³⁷Cs. The activity ratios of^239,240Pu/¹³⁷Cs in soils were found to be in the narrow range of 0.0153 to 0.0364 with a mean value of 0.0230±0.006. The concentrations of^239,240Pu and¹³⁷Cs in soils decrease exponentially with increasing the soil depth. A significant correlation was found between the concentration of^239,240Pu and that of¹³⁷Cs. The activity ratios of^239,240Pu/¹³⁷Cs tend to increase slightly with increasing soil depth.     

Vertical Distribution of137 Cs in The Lacustrine Areas and Preliminary Results of 7Be Activity in Snow Samples at Terra Nova Bay (ANTARCTICA)

Abstract

¹³⁷ Cs activity in samples from lacustrine areas around the Italian base in Antarctica is reported as an integration of a previous work. Preliminary data of cosmogenic ⁷ Be activity determined in snowfalls, total atmospheric depositions, soil and air particulate collected during the 1990–91 and 1991–92 Italian expeditions in Antarctica is presented. The results obtained point out the efficiency of snow in the processes of air particulate scavenging and provide useful information for the development of research in Antarctica in the study of air/snow transfer processes by means of natural radionuclides.     

Concentrations of 137Cs and 40K in wild mushrooms collected in a forest on Noto Peninsula,Japan

A variety of wild mushrooms were collected in a forest on the Noto Peninsula, Japan, to determine the concentration of ¹³⁷Cs and ⁴⁰K. The wild mushroom species belong to the orders Agaricales and Aphyllophorales. The concentration of ¹³⁷Cs varied widely (1.4–4,100 Bq/kg dry weight) in mushrooms growing in soil. On the contrary, ¹³⁷Cs concentration levels were relatively low (1.9–20 Bq/kg-dry weight) in mushrooms growing on wood. The concentration of ⁴⁰K varied widely (12–2,400 Bq/kg-dry weight) in contrast with several previous reports that suggest relatively constant ⁴⁰K levels in mushrooms. Unusually low concentrations of ⁴⁰K were observed in a few mushroom species that had very hard fruiting bodies with peculiar shapes. The mean and median of ¹³⁷Cs concentration in the present study were similar to those previously reported for Japanese mushrooms. Among the Agaricales mushrooms, Entolomataceae and Tricholomataceae families growing in soil had the highest concentration of ¹³⁷Cs. Among the Aphyllophorales mushrooms, Gomphaceae and Ramariaceae families growing in soil also had the highest ¹³⁷Cs concentrations. The concentrations of ¹³⁷Cs and stable Cs in mushroom samples were positively correlated. The concentration ratio of ¹³⁷Cs/Cs differed between Agaricales and Aphyllophorales mushrooms. The average ¹³⁷Cs/Cs ratio in mushrooms growing in soil was similar to that calculated for the top soil (<5 cm deep) alone because the mycelia of the mushrooms were mainly distributed near the surface of the soil.     

Temporal reduction of the external gamma dose rate due to 137Cs mobility in sandy beaches

In the present paper the contribution to the external gamma dose rate due to ¹³⁷Cs in soil as a function of time is presented. Sampling sites were selected along the Calabria and Basilicata Regions coastal beaches (southern part of Italy) to assess the external gamma dose rate in air, 1 m above the ground level. A convection-dispersion model, with constant parameters was used to approximate the radiocesium soil vertical migration. The model was calibrated using the initial ¹³⁷Cs activity deposition in this region (Chernobyl fallout) and ¹³⁷Cs activity concentration down the soil profile, measured 10 years later. The dispersion coefficient and the advection velocity values, were respectively: 2.17 cm² y⁻¹ and 0.32 cm y⁻¹. The Radionuclide Software Package (RSP), which uses a Monte Carlo simulation code, was used to determine the primary ¹³⁷Cs gamma dose contribution in air 1 m above the ground surface. The resulting ¹³⁷Cs external dose rate ranged from 0.42 nGy h⁻¹ in 1986, to 0.05 nGy h⁻¹ in 2007.