Variation of 137Cs activity concentration in flood and pore water in paddy fields and its transfer to rice.

Caesium-137 (137Cs) is a major anthropogenic radionuclide released into the environment as a result of the TEPCO Fukushima Daiichi Nuclear Reactor Station accident (occurring on March 11, 2011). Rice, being a staple food in Asian countries, including Japan, and is predominantly cultivated in paddy fields. Consequently, 137Cs present in rice is absorbed from both soil and irrigation water, making it the most important crop for estimating internal radiation doses. In this study, over the 2018-2022 cultivation periods, flood water and pore water samples were collected biweekly from paddy fields. These samples were analyzed to measure the 137Cs activity concentration, as well as the potassium (K+) and ammonium (NH4+) concentrations. Under anaerobic conditions, the 137Cs + activity concentration in pore water increased markedly to reach a value 20-fold higher than that in flood water, correlating with NH4+ concentration. However, despite the release of 137Cs + caused by increased NH4+ concentrations in pore water due to reduction processes, the 137Cs+/K+ ratio did not increase, which was attributed to the simultaneous release of K+. The competition between 137Cs+ and K+ uptake by plants indicates that rice uptake of 137Cs is not necessarily enhanced during the waterlogging period.

Chemical implication of the partition coefficient of 137Cs between the suspended and dissolved phases in natural water.

After the Fukushima Daiichi nuclear power plant accident, the terrestrial environment became severely contaminated with radiocesium. Consequently, the river and lake water in the Fukushima area exhibited high radiocesium levels, which declined subsequently. The partition coefficient of 137Cs between the suspended sediment (SS) and dissolved phases, Kd, was introduced to better understand the dynamic behavior of 137Cs in different systems. However, the Kd values in river water, ranging from 2 × 104 to 7 × 106 L kg-1, showed large spatiotemporal variability. Therefore, the factors controlling the 137Cs partition coefficient in natural water systems should be identified. Herein, we introduce a chemical model to explain the variability in 137Cs Kd in natural water systems. The chemical model includes the complexation of Cs+ with mineral and organic binding sites in SS, metal exchange reactions, and the presence of colloidal species. The application of the chemical model to natural water systems revealed that Cs+ is strongly associated with binding sites in SS, and a major chemical interaction between 137Cs and the binding sites in SS is the isotope exchange reaction between stable Cs and 137Cs, rather than metal exchange reactions with other metal ions such as potassium ions. To explain the effect of the SS concentration on Kd, the presence of colloidal 137Cs passing through a filter is significant as the dominant dissolved species of 137Cs in river water. These results suggest that a better understanding of stable Cs dissolved in natural water is important for discerning the geochemical and ecological behaviors of 137Cs in natural water.

Transfer of 137Cs and 90Sr from soil-to-potato: Interpretation of the association from global fallout in Aomori to accidental release in Fukushima and Chornobyl.

Ceasium-137 and 90Sr are major artificial radionuclides that have been released into the environment. Soil-to-plant transfer of radionuclides is an important route to food contamination. The radionuclide activity concentrations in crops must be quantitatively predicted for estimating the internal radiation doses from food ingestion. In this study, soil and potato samples were collected from three study sites contaminated with different sources of 137Cs and 90Sr: Aomori Prefecture (global fallout) and two accidental release areas (Fukushima Prefecture and the Chornobyl exclusion zone). The 137Cs activity concentrations in the soil and potato samples widely ranged from 1.0 to 250,000 and from 0.048 to 200,000 Bq kg-1 dry weight, respectively. The soil-to-potato transfer factor of 137Cs also ranged widely (0.0015-1.1) and decreased with increasing concentration of exchangeable K. Meanwhile, the activity concentrations of 90Sr in the soil and potato samples were 0.50-64,000 and 0.027-18,000 Bq kg-1 dry weight respectively, and the soil-to-potato transfer factor of 90Sr was 0.023-0.74, decreasing with increasing concentration of exchangeable Ca. The specific activity ratios of 137Cs/Cs and 90Sr/Sr in the exchangeable fraction were similar to those in potatoes, with a factor of 3 in the ±95 % confidence intervals over six orders of magnitude and a factor of 2 in the ±95 % confidence intervals over five orders of magnitude, respectively. According to the data, the accuracy of predicting the activity concentrations of 137Cs and 90Sr in potatoes can be improved by applying the specific activity ratios of 137Cs/Cs and 90Sr/Sr in the exchangeable fraction. This approach accounts for variable factors such as the effects of K and Ca fertilization and soil characteristics. It also emphasizes the benefit of determining the stable Cs and Sr concentrations in potatoes and other crops prior to possible future contamination.

Rapid survey of de novo mutations in naturally growing tree species following the March 2011 disaster in Fukushima: The effect of low-dose-rate radiation.

The impact of low-dose-rate radiation on genetics is largely unknown, particularly in natural environments. The Fukushima Dai-ich Nuclear Power Plant disaster resulted in the creation of contaminated natural lands. In this study, de novo mutations (DNMs) in germ line cells were surveyed from double-digest RADseq fragments in Japanese cedar and flowering cherry trees exposed to ambient dose rates ranging from 0.08 to 6.86 µGy h-1. These two species are among the most widely cultivated Japanese gymnosperm and angiosperm trees for forestry and horticultural purpose, respectively. For Japanese flowering cherry, open crossings were performed to produce seedlings, and only two candidate DNMs were detected from uncontaminated area. For Japanese cedar, the haploid megagametophytes were used as next generation samples. The use of megagametophytes from open crossing for next generation mutation screening had many advantages such as reducing exposure to radiation in contaminated areas because artificial crossings are not needed and the ease of data analysis owing to the haploid nature of megagametophytes. A direct comparison of the nucleotide sequences of parents and megagametophytes revealed an average of 1.4 candidate DNMs per megagametophyte sample (range: 0-40) after filtering procedures were optimized based on the validation of DNMs via Sanger sequencing. There was no relationship between the observed mutations and the ambient dose rate in the growing area or the concentration of 137Cs in cedar branches. The present results also suggest that mutation rates differ among lineages and that the growing environment has a relatively large influence on these mutation rates. These results suggested there was no significant increase in the mutation rate of the germplasm of Japanese cedar and flowering cherry trees growing in the contaminated areas.

SOIL-SOIL SOLUTION DISTRIBUTION COEFFICIENT OF RADIOIODINE IN SURFACE SOILS AROUND SPENT NUCLEAR FUEL REPROCESSING PLANT IN ROKKASHO, JAPAN.

The soil-soil solution distribution coefficient (Kd) of radioiodine in soil samples with various total carbon (TC) contents was measured in a batch sorption experiment using 125I tracer spiked as I-. The log values of Kd-125I and TC concentration in low-TC soils (< 10g kg-1) were positively correlated, whereas those of Kd-125I in TC rich soils (> 10 g kg-1) and dissolved organic carbon (DOC) in liquid phase were negatively correlated. The proportion of 125I in the < 3 kDa fraction in the liquid phase is negatively correlated with the log of DOC, implying that 125I is primarily combined with high-molecular-weight organic matter in soil solutions rich in DOC. The results suggest that Kd-125I in soil with high soil organic material (SOM) content is governed by DOC via the combination of 125I and DOC. In contrast, Kd-125I in soils with a low SOM content was governed by SOM because the anion exchange capacity of SOM was vital for the sorption of 125I-.

Estimation of rooting depth of 137Cs uptake by plants.

Understanding the soil-to-plant transfer process of 137Cs is essential for predicting the contamination levels of plants in contaminated areas. The rooting depth is considered one of the key factors explaining the difference in the activity concentration of 137Cs in different plant species. In this study, the distributions of 137Cs and 133Cs in soils and plants were investigated, and the plants' rooting depth of 137Cs uptake was estimated using the 137Cs/133Cs ratios in exchangeable fractions of soils and biological samples. The results showed that different plant species accumulate different levels of 137Cs and 133Cs. The 137Cs/133Cs ratios were fairly constant in plants of the same species. The average 137Cs/133Cs ratios in bamboo grasses and ferns were 0.015 ± 0.009 (n = 5) and 0.13 ± 0.04 Bq ng-1 (n = 10) in Yamakiya, respectively. The percentage of 137Cs in the exchangeable fraction of the uppermost soil layer was lower than that in the deeper soil layers. The activity concentrations of 137Cs in the soil profiles decreased sharply with depth, whereas the depth distributions of 133Cs were uniform. Therefore, the 137Cs/133Cs ratios were driven mainly by the 137Cs activity concentrations in soil. The plants' rooting depths of 137Cs uptake were estimated on the basis of the relationships between the averaged 137Cs/133Cs ratio in the soil layer and the 137Cs/133Cs ratio in the plant. The results indicate that the deeper-rooted species such as bamboo grasses have a lower accumulation of 137Cs than the superficial-rooting species such as ferns. The soil-to-plant transfer factors would be determined using rooting depth by calculating the averaged activity concentration of 137Cs within the estimated rooting depth.

Accumulation of 137Cs in aggregated organomineral assemblage in pasture soils 8 years after the accident at the Fukushima Daiichi nuclear power plant.

Despite the presence of minerals that allow Cs fixation in soils, 137Cs remains available to crops for several years after its deposition, particularly in pasture soils. Larger amounts of organic matter derived from herbage residues are accumulated in pasture soils than in tilled farmland soils. As the above-ground part of herbage crops initially received airborne 137Cs during the accident at Fukushima Daiich nuclear power plant (FDNPP), the organic matter originated from the contaminated herbage should play an important role in the fate of 137Cs in soils. To evaluate the role of organic matter on 137Cs distribution between potentially mobile and immobile fractions, we compared the distribution of 137Cs and stable 133Cs, which are differently associated with organic matter, by sequential extraction and density fractionation. Soil samples were collected 8 years after the accident from Andosols in pasture fields located about 160 km southwest of FDNPP. More than 90% of 137Cs was not extracted even after oxidative digestion of organic matter, suggesting that most 137Cs was strongly associated with soil minerals. Density fractionation results showed that the 137Cs/133Cs ratio was highest in the density fraction of 1.6-1.8 g cm-3, in which organic matter -including fragmented and decomposed plant detritus -was associated with minerals. Mineral-free organic matter, mostly composed of fresh plant detritus (<1.6 g cm-3), had a higher 137Cs/133Cs ratio than that of crops harvested in the same year of soil sampling. Thus, the transfer of 137Cs from soil to plants decreased with cultivation cycles. Our results demonstrate that plant-available 137Cs in pasture soil decreased with aging time, not only through increased 137Cs fixation in mineral-dominated fractions but also through its physical sequestration in aggregates.

Radiation dose rate to Japanese cedar and plants collected from Okuma, Fukushima Prefecture.

After the 2011 Fukushima Dai-ichi Nuclear Power Station (FDNPS) accident, wild populations of animals and plants living in the evacuation zone received additional ionizing radiation of both internal and external radiation doses. Morphological abnormalities of pine and fir trees near the FDNPS were reported. In order to evaluate dose-effect relationships, it is necessary to quantify the radiation doses to trees and plants. In this study, the internal and external dose rates to Japanese cedar and plants collected at three sites in Okuma, approximately 4 km southwest of FDNPS were estimated applying the ERICA Assessment Tool. The activity concentrations of 134Cs and 137Cs in soils, cedar trunks, and plants were determined. The total dose rates to cedar ranged from 2.2 ± 1.2 to 6.1 ± 2.2 µGy h-1. These rates were within the derived consideration reference levels (DCRLs) reported by ICRP 108 as 4-40 µGy h-1 for pine trees. The highest estimate for plants was 7.1 ± 2.7 µGy h-1, much smaller than the DCRLs reported for grasses and herbs (40-400 µGy h-1). On average, the internal radiation dose rates to cedars at the two sites accounted for 5% and 29% of the external dose rates, respectively, while the value in another site was only 0.4% for cedar. This was attributed to differences in the crown area between the three sites. The trunk diameter of cedars shows a positive correlation with the ratio of internal to external radiation dose rates. It indicates that the total dose rate to cedars is easily estimated with the soil radiocaesium inventory and trunk diameter. The internal radiation dose rate to the plant varied depending on the plant species. This variation was considerably large in plants due to the presence of two species, including Solidago altissima and Artemisia indica var. maximowiczii.

Differentiating Fukushima and Nagasaki plutonium from global fallout using 241Pu/239Pu atom ratios: Pu vs. Cs uptake and dose to biota.

Plutonium (Pu) has been released in Japan by two very different types of nuclear events - the 2011 Fukushima accident and the 1945 detonation of a Pu-core weapon at Nagasaki. Here we report on the use of Accelerator Mass Spectrometry (AMS) methods to distinguish the FDNPP-accident and Nagasaki-detonation Pu from worldwide fallout in soils and biota. The FDNPP-Pu was distinct in local environmental samples through the use of highly sensitive 241Pu/239Pu atom ratios. In contrast, other typically-used Pu measures (240Pu/239Pu atom ratios, activity concentrations) did not distinguish the FDNPP Pu from background in most 2016 environmental samples. Results indicate the accident contributed new Pu of ~0.4%-2% in the 0-5 cm soils, ~0.3%-3% in earthworms, and ~1%-10% in wild boar near the FDNPP. The uptake of Pu in the boar appears to be relatively uninfluenced by the glassy particle forms of fallout near the FDNPP, whereas the 134,137Cs uptake appears to be highly influenced. Near Nagasaki, the lasting legacy of Pu is greater with high percentages of Pu sourced from the 1945 detonation (~93% soils, ~88% earthworm, ~96% boar). The Pu at Nagasaki contrasts with that from the FDNPP in having proportionately higher 239Pu and was distinguished by both 240Pu/239Pu and 241Pu/239Pu atom ratios. However, compared with the contamination near the Chernobyl accident site, the Pu amounts at all study sites in Japan are orders of magnitude lower. The dose rates from Pu to organisms in the FDNPP and Nagasaki areas, as well as to human consumers of wild boar meat, have been only slightly elevated above background. Our data demonstrate the greater sensitivity of 241Pu/239Pu atom ratios in tracing Pu from nuclear releases and suggest that the Nagasaki-detonation Pu will be distinguishable in the environment for much longer than the FDNPP-accident Pu.

Relationship between radiocaesium in muscle and physicochemical fractions of radiocaesium in the stomach of wild boar.

After the accident at the TEPCO Fukushima Daiichi Nuclear Power Plant in 2011, it became important to study radiation dynamics, assess internal radiation exposure and specify factors affecting radionuclide variation in wildlife. Therefore, it is necessary to investigate which physicochemical fractions of radiocaesium (137Cs) are absorbed from ingested material in species with high activity concentrations of 137Cs, such as wild boar. This study analysed the physicochemical fractions of 137Cs in the stomach contents of wild boar to evaluate the transfer from ingested food to muscle. The 137Cs activity concentration in muscle showed a significantly positive relationship with the 137Cs activity concentration in the exchangeable fraction, and the sum of the 137Cs activity concentrations in the exchangeable and bound to organic matter fractions. Seasonal variations were also found in the 137Cs activity concentration in the exchangeable fraction, and the sum of the 137Cs activity concentrations in the exchangeable and bound to organic matter fractions. These findings suggest that the proportions of the physicochemical fractions of 137Cs in the exchangeable and bound to organic matter fractions in the stomach contents are important factors affecting the increases and seasonal dynamics of the activity concentrations of 137Cs in wild boar muscle.

Effects of organic amendments on the natural attenuation of radiocesium transferability in grassland soils with high potassium fertility.

Organic amendments affect the behavior of radiocesium in soil-plant systems in a complex way; they can inhibit radiocesium fixation by clay minerals by blocking selective sorption sites, whereas K supplied to the soil solution by amendments can reduce Cs uptake by plant roots. Here, we investigated the influence of inorganic and organic amendments on the transferability of radiocesium from soil to grass seedling in a humus-rich Andosol with high exchangeable K content. Soil samples were spiked with a137Cs tracer, treated with N, N-P-K, compost (cattle manure using rice straw), or no amendment (control soil), and subjected to repeated two-week wetting and air-drying treatments for one year in an artificial climate chamber. Small-scale cultivations of orchard grass were performed four times during the experimental period to assess temporal changes of availability of 137Cs in the soils. The 137Cs transfer factor (TF), defined as the 137Cs concentration in the plant divided by that in the soil, decreased with time in the control soil. The soil treated with compost showed higher TFs than the control soil in each cultivation and a slower attenuation of 137Cs transferability. By comparing the extractability of 137Cs, NH4+, and K+ with the observed TFs, we show that K released from the compost was not effective in reducing root uptake of 137Cs, but enhanced 137Cs desorption from the soil under K-rich conditions. This result suggests that organic amendment is ineffective in reducing root uptake of radiocesium under high exchangeable K concentrations, and may instead enhance the long-term availability of radiocesium in soils.

Dynamics of Strontium and geochemically correlated elements in soil during washing remediation with eco-complaint chelators.

In the study, the dynamics of Sr2+ and geochemically correlated elements (Ca2+, Ba2+, and Y3+) in soil with chelators in the mix (soil to chelator ratio, 1:10; matrix, H2O) were assessed to understand chemical-induced washing remediation of radiogenic waste solids. Specifically, EDTA (2,2',2″,2‴-(ethane-1,2-diyldinitrilo)tetraacetic acid), EDDS (2-[2-(1,2-dicarboxyethylamino)ethylamino]butanedioic acid), GLDA (2-[bis(carboxymethyl)amino]pentanedioic acid), and HIDS (2-(1,2-dicarboxyethylamino)-3-hydroxy-butanedioic acid) are chelators that are used as extractants. The effect of solution pH on chelator-induced extractions of the target elements (t-Es: Sr2+, Ca2+, Ba2+, or Y3+) from soil and stability constants of the t-Es complexes with chelators were used to explain the trends and magnitudes in interactions. Pre- and post-extractive solid-phase speciation was used to define the extent of the competence of each chelator in persuading dissolution of t-Es in the soil. The effects of ultrasonic energy, admixtures of biodegradable chelators, and excess chelators in solution (1:20) were also analyzed on the extractive removal of t-Es from soil. The results indicate that the Sr2+ removal with biodegradable chelators significantly exceeded (approximately 70%) when compared to that of environmentally-persistent EDTA at lower solution pHs and a higher soil to chelator ratio (GLDA > HIDS > EDDS ≈ EDTA). However, the extraction of the geochemically related element was significantly lower.

Vertical distribution of 129I and radiocesium in forest soil collected near the Fukushima Daiichi Nuclear Power Plant boundary.

Three soil core samples were collected from a forest located about 1.1 km south of the Fukushima Daiichi Nuclear Power Plant (FDNPP) boundary in 2017, and the vertical profiles of 129I from the FDNPP accident were determined by the combination of TMAH (tetramethyl ammonium hydroxide) extraction and ICP-MS/MS analysis. The humus layer above the soil layer was heavily contaminated with 134Cs (1983-5985 Bq g-1) and 137Cs (1947-5902 Bq g-1) (decay-corrected to March 11, 2011). The 129I activity concentrations decreased sharply with the soil depth, from 1894 to 34.1, from 9384 to 78.9, and from 2536 to 51.3 mBq kg-1, for the three sites. Downward migration of 129I was slightly faster than the one of 134Cs. In addition, the cumulative 129I inventories were observed to be 43.4 ±â€¯1.0, 71.7 ±â€¯1.8, and 56.5 ±â€¯1.8 Bq m-2, respectively. Subsequently, the cumulative 131I inventories were estimated to be 1.76 ±â€¯0.06, 2.90 ±â€¯0.11, and 2.28 ±â€¯0.10 GBq m-2 (decay-corrected to March 11, 2011), respectively. Finally, the total atmospheric deposition of 129I on the land of Japan due to the FDNPP accident was estimated to be around 1.09-1.71 kg (7.11-11.2 GBq).

Phytoavailability of 137Cs and stable Cs in soils from different parent materials in Fukushima, Japan.

Weathered micaceous minerals (micas) are able to release potassium ion (K+) and fix caesium-137 (137Cs), both of which reduce soil-to-plant transfer of 137Cs. Among micas, trioctahedral micas such as biotite is expected to have a stronger ability to supply nonexchangeable K+ and a higher amount of Cs fixation sites than dioctahedral micas such as illite. Although biotite is predominant in granitic soils (G soils), illite is mainly dominant in sedimentary rock soils (S soils). Therefore, we hypothesized that G soils have a lower 137Cs transfer risk than S soils because of this difference in mineralogy. The objective of the present study was to determine the transfer factor (TF) of 137Cs and stable Cs (SCs) and to elucidate the determinant factors of TFs for G and S soils in Fukushima, Japan. Pot experiments were carried out with rice (Oryza sativa L. cv. Hokuriku 193) in G and S soils to determine the TF of 137Cs (TF-137Cs) and stable Cs (TF-SCs) under K-deficient conditions. TF-137Cs and TF-SCs were highly correlated, and both were significantly lower for G soils than for S soils. Higher TF values were shown for soils with lower amounts of exchangeable and nonexchangeable K or with higher percentages of exchangeable 137Cs (ex137Cs). The percentage of ex137Cs was negatively correlated with the amount of Cs fixation sites, represented by the radiocaesium interception potential. Thus, we concluded that smaller TF values for G soils were caused by a stronger ability to supply nonexchangeable K+ and a higher amount of Cs fixation sites. These findings will contribute to the establishment of soil screening techniques based on 137Cs transfer risk in Fukushima prefecture.

The transfer of fallout plutonium from paddy soil to rice: A field study in Japan.

Reported transfer factor (TF) values of Pu from paddy soil to rice are rather scarce, despite the radiotoxicity of Pu and the irreplaceable role of rice in Asian peoples' diets. Here, we conducted a field study to investigate the transfer of global fallout Pu from paddy soil to rice grain (hulled rice) in Japan. The 240Pu/239Pu atomic ratios in two rice grain samples out of 16 samples were determined and the ratios corresponded well with the global fallout value. The soil-to-rice TFPu in 12 Japanese prefectures ranged from 4.5 × 10-6 to 1.2 × 10-4 with a geometric mean of 3.3 × 10-5. The TFs of rice obtained in this study were compatible to the TFs for the broad heading "cereals" compiled in the IAEA Technical Report Series No. 472. Weak correlations were found between the TF and the investigated soil characteristics such as soil pH and loss on ignition. Regarding the TFs for cerium (Ce) and thorium (Th) which are commonly considered as Pu analogues, we observed no significant correlations between the log(TFPu) and log(TFCe) or log(TFPu) and log(TFTh). On the other hand, interestingly, a significantly positive correlation (r = 0.795, p < 0.001) was observed between log(TFPu) and log(TFU). In view of the observed similarity of TF values for U and Pu from soil to rice, we thought that using the easy-to-measure TFU to estimate TFPu from soil to rice might be suggested although the mechanism was unclear.

Changes in the Soil to Brown Rice Concentration Ratio of Radiocaesium before and after the Fukushima Daiichi Nuclear Power Plant Accident in 2011.

Radiocaesium (RCs) mobility in soil is initially relatively high when the nuclide first comes into contact with soil, after which the mobile fraction decreases with time due to RCs fixation to soil particles (aging effect). Consequently, the RCs activity concentration in plants grown in soil was expected to decrease with time after the Fukushima Daiichi nuclear power plant accident in 2011. In this study, we collated data on concentration ratios (CR) of RCs between brown rice grain and paddy soil and compared CR values reported for periods before and after the accident. For this purpose, soil and rice data were collected after the accident specifically from paddy fields that did not have additional potassium fertilizer added (for remediation purposes). The geometric mean rice/soil CR of RCs for all types of soil was 1.2 × 10-2 in 2011 ( n = 62) and by 2013 the value had declined to 3.5 × 10-3 ( n = 32), which was similar to that for 1995-2007 of 3.4 × 10-3 ( n = 120). The comparison suggests that the mean soil-to-rice grain concentration ratio had returned to that prevailing before the accident after less than three years. It was also confirmed that CR values for rice sampled from paddy fields were lower than those obtained from pot experiments.

Source analysis of radiocesium in river waters using road dust tracers.

Following the Fukushima Dai-ichi Nuclear Power Station accident, regional road dust, heavily contaminated with radiocesium, now represents a potential source of radiocesium pollution in river water. To promote effective countermeasures for reducing the risk from radiocesium pollution, it is important to understand its sources. This study evaluated the utility of metals, including Al, Fe, and Zn as road dust tracers, and applied them to analyze sources of 137Cs in rivers around Fukushima during wet weather. Concentrations of Zn in road dust were higher than agricultural and forest soils, whereas concentrations of Fe and Al were the opposite. Concentrations of Zn were weakly but significantly correlated with benzothiazole, a molecular marker of tires, indicating Zn represents an effective tracer of road dust. Al, Fe, and Zn were frequently detected in suspended solids in river water during wet weather. Distribution coefficients of these metals and 137Cs exceeded 104, suggesting sorptive behavior in water. Although concentrations of Al, Fe, Zn, and 137Cs were higher in fine fractions of road dust and soils than in coarse fractions, use of ratios of 137Cs to Al, Fe, or Zn showed smaller differences among size fractions. The results demonstrate that combinations of these metals and 137Cs are useful for analyzing sources of radiocesium in water. These ratios in river water during wet weather were found to be comparable with or lower than during dry weather and were closer to soils than road dust, suggesting a limited contribution from road dust to radiocesium pollution in river water.

The 137Cs activity concentration of suspended and dissolved fractions in irrigation waters collected from the 80 km zone around TEPCO's Fukushima Daiichi Nuclear Power Station.

Fifty-four samples of irrigation water were collected in 2014 from agricultural ponds, rivers, and dams within the 80 km zone around TEPCO's Fukushima Daiichi Nuclear Power Station (FDNPS). The samples were filtered with a 0.45 µm pore-size membrane filter to produce suspended and dissolved fractions. The 137Cs activity concentration of the suspended fraction varied from 1.5 to 300 Bq g-1 dry weight and was significantly higher than that in the soil around each sampling site. The range of 137Cs activity concentrations in the dissolved fraction varied over three orders of magnitude at 0.0075-6.7 Bq l-1, which was a larger range than that of the suspended fraction; the higher values for samples were from within the 20 km zone. In the dissolved fraction 87 ± 9% of the 137Cs (n = 37) was in a monovalent cationic form (Cs+) and therefore potentially mobile. The distribution coefficient (Kd) ranged from 4100 to 2,100,000; the geometric mean value (110,000) was higher than that reported by the IAEA (2010). The geometric mean Kd of samples collected from the 20 km zone was 61,000 (n = 27), which was significantly lower than that collected from 20 to 80 km zone (200,000, n = 27). The Kd-value was negative correlated with the concentration of stable 133Cs and the electric conductivity in the dissolved fraction. This shows relatively higher mobility of radiocaesium in irrigation waters may occur when there are higher contents of cations present.

Soil-soil solution distribution coefficient of soil organic matter is a key factor for that of radioiodide in surface and subsurface soils.

We investigated the vertical distribution of the soil-soil-solution distribution coefficients (Kd) of 125I, 137Cs, and 85Sr in organic-rich surface soil and organic-poor subsurface soil of a pasture and an urban forest near a spent-nuclear-fuel reprocessing plant in Rokkasho, Japan. Kd of 137Cs was highly correlated with water-extractable K+. Kd of 85Sr was highly correlated with water-extractable Ca2+ and SOC. Kd of 125I- was low in organic-rich surface soil, high slightly below the surface, and lowest in the deepest soil. This kinked distribution pattern differed from the gradual decrease of the other radionuclides. The thickness of the high-125I-Kd middle layer (i.e., with high radioiodide retention ability) differed between sites. Kd of 125I- was significantly correlated with Kd of soil organic carbon. Our results also showed that the layer thickness is controlled by the ratio of Kd-OC between surface and subsurface soils. This finding suggests that the addition of SOC might prevent further radioiodide migration down the soil profile. As far as we know, this is the first report to show a strong correlation of a soil characteristic with Kd of 125I-. Further study is needed to clarify how radioiodide is retained and migrates in soil.

Concentration of radiocaesium in rice and irrigation water, and soil management practices in Oguni, Date, Fukushima.

The concentration of radiocaesium ((134) Cs and (137) Cs) in brown rice collected from Oguni, Date, Fukushima in 2011 was over 500 Bq kg(-1) , which was the provisional regulation value in 2011, and rice cultivation was prohibited in 2012. Rice culture was resumed following the application of K fertilizer as a countermeasure in 2013. The concentration of (137) Cs in soils and irrigation water in 2013 was in the range of 1200 to 4000 Bq kg(-1) (n = 31) and 0.078 to 1.1 Bq L(-1) (n = 7), respectively. The concentration of (137) Cs in the dissolved fraction in irrigation water filtered with 0.45 µm pore-size membrane filter was a relatively constant at 0.019 to 0.038 Bq L(-1) (n = 7). The concentration of (137) Cs in brown rice cultivated in the paddy fields after implementing the countermeasure was 1.1 to 24 Bq kg(-1) dry weight (n = 29), which was lower than the Standard Limits (100 Bq kg(-1) ). However, the concentration of Cs in rice cultivated under a similar agricultural management as in 2011 and prior to the Tokyo Electric Power Company Holdings' (TEPCO) Fukushima accident was over the Standard Limits. Integr Environ Assess Manag 2016;12:659-661. © 2016 SETAC.