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Neptunium-237 and 239 Pu are important radionuclides in the safety assessment related to geological disposal of radioactive waste because of the possibility of long-term exposure to humans. Mobilities of these radionuclides in the environment are of particular importance for their radiation dose evaluation; therefore, in this study, we have made the assessment of the soil-soil solution distribution coefficient (K d , L/kg) using global fallout 237 Np and 239 Pu in Japanese upland soils. The K d values were determined by extracting these radionuclides from 24 soil samples using a laboratory batch method. The desorption K d values of 237 Np ranged from 3.3 × 10 2 to 1.0 × 10 4  L/kg, and their geometric mean (GM) and arithmetic mean (AM) were 1.7 × 10 3  L/kg and 2.6 × 10 3  L/kg, respectively. The desorption K d values of 239 Pu were found to vary from 9.4 × 10 3 to 7.1 × 10 4  L/kg, and their GM and AM were 3.3 × 10 4  L/kg and 4.0 × 10 4  L/kg, respectively. In Japanese upland soils, the K d value of 239 Pu was one order of magnitude higher than that of 237 Np., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

In this work, we report a rapid and highly sensitive analytical method for the determination of tellurium in soil and plant samples using sector field inductively coupled plasma mass spectrometry (SF-ICP-MS). Soil and plant samples were digested using Aqua regia. After appropriate dilution, Te in soil and plant samples was directly analyzed without any separation and preconcentration. This simple sample preparation approach avoided to a maximum extent any contamination and loss of Te prior to the analysis. The developed analytical method was validated by the analysis of soil/sediment and plant reference materials. Satisfactory detection limits of 0.17 ng g(-1) for soil and 0.02 ng g(-1) for plant samples were achieved, which meant that the developed method was applicable to studying the soil-to-plant transfer factor of Te. Our work represents for the first time that data on the soil-to-plant transfer factor of Te were obtained for Japanese samples which can be used for the estimation of internal radiation dose of radioactive tellurium due to the Fukushima Daiichi Nuclear Power Plant accident., (Copyright © 2013 Elsevier B.V. All rights reserved.)

Sorption kinetics of iodide (I(-)), which is one of the major inorganic chemical forms of iodine in soil environments, were studied under four sets of experimental conditions characterised by temperature or biological activity. We compared partitioning ratios in solid, liquid and gas phases in soils as well as soil-soil solution distribution coefficients (K(d)s) at two different temperatures 4 and 23 °C, for 63 paddy soil samples collected throughout Japan. Interestingly, (125)I emission from soil was observed; the partitioning ratios in gas phase ranged from 0 to 27 % at 4 °C and from 0 to 42 % at 23 °C. In addition, the authors found that K(d) values at 23 °C had good correlation with pH though there was no correlation between K(d) values at 4 °C and pH because of the difference in biological activity.

New best estimates for the solid-liquid distribution coefficient (K(d)) for a set of radionuclides are proposed, based on a selective data search and subsequent calculation of geometric means. The K(d) best estimates are calculated for soils grouped according to the texture and organic matter content. For a limited number of radionuclides this is extended to consider soil cofactors affecting soil-radionuclide interaction, such as pH, organic matter content, and radionuclide chemical speciation. Correlations between main soil properties and radionuclide K(d) are examined to complete the information derived from the best estimates with a rough prediction of K(d) based on soil parameters. Although there are still gaps for many radionuclides, new data from recent studies improve the calculation of K(d) best estimates for a number of radionuclides, such as selenium, antimony, and iodine.

Radium-226 ((226)Ra) should be assessed to determine the safety of geological disposal of high-level radioactive and transuranic wastes. Among the environmental transfer parameters that have been used in mathematical models for the environmental safety assessment, soil-to-plant transfer factor (F(v)) is of importance; it is defined as the plant/soil concentration ratio. Reported F(v) data for (226)Ra are still limited due to the low concentration of (226)Ra in plants in the natural environment. In this study, we collected F(v) of (226)Ra (F(v)-Ra) for crops and then applied a statistical approach to estimate F(v)-Ra instead of directly measuring the radionuclide. We found high correlations between (226)Ra and U concentrations in soils (because (226)Ra is a progeny in the (238)U series), and between (226)Ra and Ba concentrations in plants (because they are chemically similar in plant uptake). Using U in soil and Ba in plant values, we could estimate F(v)-Ra with good accuracy; the difference between estimated and measured F(v)-Ra values was a factor of 1.2 on average for crops. The method could estimate F(v)-Ra for the soil-to-plant systems where (226)Ra and Ba concentrations in soil are within the normal range, e.g. 8-100 Bq kg(-1)-dry for (226)Ra and 84-960 mg kg(-1)-dry for Ba.

We propose a new approach for estimation of soil-soil solution distribution coefficient (K(d)) of radiostrontium using some selected soil properties. We used 142 Japanese agricultural soil samples (35 Andosol, 25 Cambisol, 77 Fluvisol, and 5 others) for which Sr-K(d) values had been determined by a batch sorption test and listed in our database. Spearman's rank correlation test was carried out to investigate correlations between Sr-K(d) values and soil properties. Electrical conductivity and water soluble Ca had good correlations with Sr-K(d) values for all soil groups. Then, we found a high correlation between the ratio of exchangeable Ca to Ca concentration in water soluble fraction and Sr-K(d) values with correlation coefficient R=0.72. This pointed us toward a relatively easy way to estimate Sr-K(d) values.

Rhenium (Re) mobility in agricultural soils was studied in order to obtain information relevant to (99)Tc mobility in soil-to-plant systems. Since water soluble Tc and Re are highly bioavailable, extraction of Re with water was carried out in addition to a total Re determination in the soils. The geometric means of total Re for paddy field, upland field and other soils were 0.34, 0.23, and 0.28 ng g(-1), respectively, while those of water soluble Re (<0.45 microm membrane filterable) were 0.053, 0.015 and 0.008 ng g(-1), respectively. There were no differences for total Re among soil uses; however, the water soluble Re/total Re ratio was significantly higher in paddy field soils (16%) than in other soil uses (6% for upland fields and 3% for other uses). Rhenium mobility and plant availability were higher in paddy fields than in other agricultural fields, and similar phenomena would be expected for (99)Tc.

The mobility of antimony (Sb) in Japanese agricultural soils was studied by radiotracer experiments using 124Sb tracer. The soil-solution distribution coefficients (Kd) of Sb were measured for 110 soil samples. These Kds ranged from 1 to 2065 L kg(-1); the geometric mean was 62 L kg(-1) excluding one extremely high value, 2065 L kg(-1). Experimental measurement of Kd showed a decrease with both increasing pH and increasing phosphate concentration. The latter suggested that one aspect of the Sb sorption phenomena in Japanese soil was influenced by specific adsorption of anions such as phosphate. However, other aspects could not be explained by this specific adsorption mechanism, because only 20-40% of soil-sorbed Sb could be extracted by phosphate solution.

Desorption levels of soil-sorbed selenium (Se) were studied by adding phosphate to 22 typical Japanese agricultural soils. Soil-soil solution distribution coefficients of Se (Kd-Se) were measured using a batch process as an index of Se sorption level, adding 75Se as a tracer. After the Kd measurement, extraction of soil-sorbed 75Se with a 0.1 M or 1 M Na2HPO4 solution followed to determine the amount of 75Se desorbed by the phosphate. When the 0.1 M Na2HPO4 solution was used, 18-70% of soil-sorbed Se was extracted (average: 47%). However, when the 1 M Na2HPO4 solution was used, 27-83% of soil-sorbed Se was extracted (average: 57%). The observed 75Se desorption percentage indicated the maximum Se removability by phosphate addition. The desorption percentage of Se with 1 M Na2HPO4 correlated with Kd-Se values, suggesting that the soil sample with higher Kd-Se contained more reactive components for phosphate-sorption than the soil sample with lower Kd-Se. To evaluate the effect of phosphate concentration on the Se sorption, the Kd-Se was measured for two typical soils under different levels of phosphate (0.1-10 mM PO4). The Kd values were decreased by phosphate addition for both soils. The Kd decrease was observed even for just 1 mM PO4. The phosphate addition with 1 mM PO4 is the same level as in P fertilizer applied to paddy fields in Japan. Therefore, it was suggested that Se desorption should occur in Japanese soils due to the phosphate input.

In order to evaluate the selenium (Se) sorption level in Japanese soils, soil/soil solution distribution coefficients (K(d)s) were obtained for 58 agricultural soil samples (seven soil classification groups) using 75Se as a tracer. Although several chemical forms of Se are present in agricultural fields, selenite was used, because it is the major inorganic Se form in acid soils such as found in Japan. The Kd values obtained covered a wide range, from 12 to 1060l/kg, and their arithmetic mean was 315l/kg. Among the soil groups, Andosols had higher Kd values. The Kd values for all samples were highly correlated with soil active-aluminum (Al) and active-iron (Fe) contents. Thus, active-Al and active-Fe were considered to be the major adsorbents of Se. Then, a new sequential extraction procedure was applied to 12 soil samples in order to quantify the effect of soil components on Se adsorption. The sequential extraction results showed that 80-100% of the adsorbed Se was recovered as Al-bound Se and Fe-bound Se. The amount of Al-bound Se was the highest in the soils that showed high Kd values, though the relative contribution of Fe-bound Se tended to increase with decreasing Kd values. The high values of Kd seemed to be caused mainly by the adsorption of Se onto active-Al in Japanese soils.

The behavior of an element in the environment depends on its physicochemical form. Basic data for the behavior of technetium in an agricultural environment were obtained by determining the physicochemical forms of Tc in 28 surface water samples from paddy and upland fields. Most of the (95m)Tc was present as TcO(4)(-) in the samples. The relative amount of this chemical form was 72% on average. A significant amount of insoluble Tc (particles more than 0.2 microm in size), however, was found in some samples. The maximum amount of the insoluble Tc was 91%. Other forms were found in insignificant amounts. The amount of insoluble Tc was relatively high in paddy soil samples. Paddy soils, gley soils and gray lowland soils were particularly effective in the insolubilization of Tc. Among the soil characteristics studied, cation exchange capacity, anion exchange capacity, and active aluminum showed significant correlations with the relative amount of insoluble Tc. When microorganisms were eliminated from the surface water samples before the addition of (95m)TcO(4)(-), little insoluble Tc was found, suggesting that microorganisms cause the physicochemical transformation. These results showed that the physicochemical form of Tc changes from TcO(4)(-) to insoluble forms in surface water covering paddy fields. The insoluble forms would restrict the mobility of Tc in paddy fields.

To evaluate the impact of the 1999 criticality accident in Tokai-mura on the U isotope composition in soils, U isotopes (235U and 238U) were determined with inductively coupled plasma-mass spectrometry (ICP-MS) for soil core samples collected on the JCO grounds after the accident. The 235U/238U ratios were higher than the natural ratio in most samples. The highest ratio observed was 0.0262. Although vertical profiles of the 235U/238U ratio differed among the soil cores, the ratios tended to be high at the surface and decreased with depth. The U concentration also changed with depth. The percentages of 235U in the excess U, estimated from the positive correlation between U concentration and the 235U/238U ratio in soil samples, were less than 4% by mass (mostly 1-3%) and were much lower than the enrichment of the U used in the uranium conversion building at the time of the criticality accident (18.8%). These findings indicate that enriched U had been released before the criticality accident during the U processing at JCO in connection with the reconversion of light water reactor fuel. Since the range of the U concentrations found was comparable to the range of uncontaminated Japanese surface soils, the amount of U added to the soil was judged negligible from a radiation protection viewpoint.