Mariko Atarashi-Andoh

Factors affecting vertical distribution of Fukushima accident-derived radiocesium in soil under different land-use conditions

The Fukushima Dai-ichi nuclear power plant accident in Japan, triggered by a big earthquake and the resulting tsunami on 11 March 2011, caused a substantial release of radiocesium ((137)Cs and (134)Cs) and a subsequent contamination of soils in a range of terrestrial ecosystems. Identifying factors and processes affecting radiocesium retention in these soils is essential to predict how the deposited radiocesium will migrate through the soil profile and to other biological components. We investigated vertical distributions of radiocesium and physicochemical properties in soils (to 20 cm depth) at 15 locations under different land-use types (croplands, grasslands, and forests) within a 2 km × 2 km mesh area in Fukushima city. The total (137)Cs inventory deposited onto and into soil was similar (58.4±9.6 kBq m(-2)) between the three different land-use types. However, aboveground litter layer at the forest sites and herbaceous vegetation at the non-forested sites contributed differently to the total (137)Cs inventory. At the forest sites, 50-91% of the total inventory was observed in the litter layer. The aboveground vegetation contribution was in contrast smaller (<35%) at the other sites. Another remarkable difference was found in vertical distribution of (137)Cs in mineral soil layers; (137)Cs penetrated deeper in the forest soil profiles than in the non-forested soil profiles. We quantified (137)Cs retention at surface soil layers, and showed that higher (137)Cs retention can be explained in part by larger amounts of silt- and clay-sized particles in the layers. More importantly, the (137)Cs retention highly and negatively correlated with soil organic carbon content divided by clay content across all land-use types. The results suggest that organic matter inhibits strong adsorption of (137)Cs on clay minerals in surface soil layers, and as a result affects the vertical distribution and thus the mobility of (137)Cs in soil, particularly in the forest ecosystems.

Comparison of the vertical distributions of Fukushima nuclear accident radiocesium in soil before and after the first rainy season, with physicochemical and mineralogical interpretations

Effect of intense rainfall on the distribution of Fukushima-accident-derived (137)Cs in soil was examined. Inventories and vertical distributions of (137)Cs in soils were determined at 15 locations (including croplands, grasslands, and forests) in Fukushima city in the post-rainy season, approximately 4.5months after the accident, and were compared with those in the pre-rainy season determined in our former study. The (137)Cs inventory levels scarcely changed between points in time spanning the first rainy season after the accident. Moreover, the majority of (137)Cs remained stored in the aboveground vegetation and in the upper 5cm of soil layer at undisturbed locations in the post-rainy season. A more quantitative analysis with the characterization of the vertical profile of (137)Cs using the relaxation length confirmed that the vertical profile was almost unchanged at most locations. Accordingly, it is concluded that rainfall during the rainy season had a limited effect on (137)Cs distribution in the soil, indicating the very low mobility. Chemical extraction of (137)Cs from selected soil samples indicated that (137)Cs in the soil was barely water soluble, and even the fraction extracted with 1M ammonium acetate was only approximately 10%. This further supports the low mobility of (137)Cs in our soils. Soil mineralogical analyses, which included the identification of clay minerals, suggested that smectite and mica could lower the exchangeable fraction of (137)Cs. However, no direct relationship was obtained between mineral composition and (137)Cs retention in the upper soil layer. In contrast, positive correlations were observed between (137)Cs extractability and soil properties such as pH, organic matter content, finer-sized particle content, and cation-exchange capacity. These results suggest that the mineralogical effect on the firm fixation of (137)Cs on soil constituents may be masked by the non-specific adsorption offered by the physicochemical properties of the soils.

Retention of potentially mobile radiocesium in forest surface soils affected by the Fukushima nuclear accident

The fate of 137Cs derived from the Fukushima nuclear accident fallout and associated radiological hazards are largely dependent on its mobility in the surface soils of forest ecosystems. Thus, we quantified microbial and adsorptive retentions of 137Cs in forest surface (0–3 cm) soils. The K2SO4 extraction process liberated 2.1%–12.8% of the total 137Cs from the soils. Two soils with a higher content of clay- and silt-sized particles, organic carbon content, and cation exchange capacity showed higher 137Cs extractability. Microbial biomass was observed in all of the soils. However, the 137Cs extractability did not increase after destruction of the microbial biomass by chloroform fumigation, providing no evidence for microbial retention of the Fukushima-fallout 137Cs. The results indicate that uptake of 137Cs by soil microorganisms is less important for retention of potentially mobile 137Cs in the forest surface soils compared to ion-exchange adsorption on non-specific sites provided by abiotic components.

Topographic heterogeneity effect on the accumulation of Fukushima-derived radiocesium on forest floor driven by biologically mediated processes

The accident at the Fukushima Daiichi nuclear power plant caused serious radiocesium (137Cs) contamination of forest ecosystems located in mountainous and hilly regions with steep terrain. To understand topographic effects on the redistribution and accumulation of 137Cs on forest floor, we investigated the distribution of Fukushima-derived 137Cs in forest-floor litter layers on a steep hillslope in a Japanese deciduous forest in August 2013 (29 months after the accident). Both leaf-litter materials and litter-associated 137Cs were accumulated in large amounts at the bottom of the hillslope. At the bottom, a significant fraction (65%) of the 137Cs inventory was observed to be associated with newly shed and less degraded leaf-litter materials, with estimated mean ages of 0.5–1.5 years, added via litterfall after the accident. Newly emerged leaves were contaminated with Fukushima-derived 137Cs in May 2011 (two months after the accident) and 137Cs concentration in them decreased with time. However, the concentrations were still two orders of magnitude higher than the pre-accident level in 2013 and 2014. These observations are the first to show that 137Cs redistribution on a forested hillslope is strongly controlled by biologically mediated processes and continues to supply 137Cs to the bottom via litterfall at a reduced rate.

An overview of organically bound tritium experiments in plants following a short atmospheric HTO exposure.

The need for a less conservative, but reliable risk assessment of accidental tritium releases is emphasized in the present debate on the nuclear energy future. The development of a standard conceptual model for accidental tritium releases must be based on the process level analysis and the appropriate experimental database. Tritium transfer from atmosphere to plants and the subsequent conversion into organically bound tritium (OBT) strongly depends on the plant characteristics, seasons, and meteorological conditions, which have a large variability. The present study presents an overview of the relevant experimental data for the short term exposure, including the unpublished information, also. Plenty of experimental data is provided for wheat, rice, and soybean and some for potato, bean, cherry tomato, radish, cabbage, and tangerine as well. Tritiated water (HTO) uptake by plants during the daytime and nighttime has an important role in further OBT synthesis. OBT formation in crops depends on the development stage, length, and condition of exposure. OBT translocation to the edible plant parts differs between the crops analyzed. OBT formation during the nighttime is comparable with that during the daytime. The present study is a preliminary step for the development of a robust model of crop contamination after an HTO accidental release.

Conversion Rate of HTO to OBT in Plants

ABSTRACT The conversion rate of tritiated water (HTO) in plants’ leaves to organically bound tritium (OBT) in their edible parts in the open air was obtained for several vegetables (komatsuna, radish and cherry tomato) during a chronic tritiated hydrogen (HT) release experiment at Chalk River in 1994. During the experiment, HT gas was continuously released to the atmosphere at the cultivated site for 12 days, and HTO and OBT concentrations in cultivated plants were measured. For plants’ leaves, the conversion rate of HTO to OBT was about 0.2 (% hr−1), but it varied with their growth stage. A chamber experiment was also carried out in laboratory for comparison. The chamber experiment results showed that the conversion rate under artificial lights was half that in the field experiment.

Forest type effects on the retention of radiocesium in organic layers of forest ecosystems affected by the Fukushima nuclear accident

The Fukushima Daiichi nuclear power plant disaster caused serious radiocesium (137Cs) contamination of forest ecosystems over a wide area. Forest-floor organic layers play a key role in controlling the overall bioavailability of 137Cs in forest ecosystems; however, there is still an insufficient understanding of how forest types influence the retention capability of 137Cs in organic layers in Japanese forest ecosystems. Here we conducted plot-scale investigations on the retention of 137Cs in organic layers at two contrasting forest sites in Fukushima. In a deciduous broad-leaved forest, approximately 80% of the deposited 137Cs migrated to mineral soil located below the organic layers within two years after the accident, with an ecological half-life of approximately one year. Conversely, in an evergreen coniferous forest, more than half of the deposited 137Cs remained in the organic layers, with an ecological half-life of 2.1 years. The observed retention behavior can be well explained by the tree phenology and accumulation of 137Cs associated with litter materials with different degrees of degradation in the organic layers. Spatial and temporal patterns of gamma-ray dose rates depended on the retention capability. Our results demonstrate that enhanced radiation risks last longer in evergreen coniferous forests than in deciduous broad-leaved forests.

Formation and retention of organically bound deuterium in rice in deuterium water release experiment.

As a substitute of tritium, deuterated water (D2O) vapor release experiments were performed in a greenhouse to estimate the different formation and subsequent retention of organically bound deuterium in rice plants between daytime and nighttime exposure. Potted rice plants were exposed to D2O vapor in the greenhouse for 8 h, under day or night conditions. Deuterium concentrations in free water and organic matter in rice leaves and ears were investigated until harvest time. The formation of organically bound deuterium in the daytime was higher than during the nighttime by the factors of 2.4 for the ear and 2.9 for the leaf. The decrease of the organically bound deuterium concentration in the ear after the nighttime exposure was faster than that after the daytime exposure. Data analysis was carried out using a compartment model in which different generating processes of organic matter were considered. The calculated organically bound deuterium retention in rice agreed with the measured value.

A passive collection system for whole size fractions in river suspended solids

In order to solve difficulties in collection of river suspended solids (SS) such as frequent observations during stochastic rainfall events, a simple passive collection system of SS has been developed. It is composed of sequentially connected two large-scale filter vessels. A portion of river water flows down into the filter vessels utilizing a natural drop of streambed. The system enable us to carry out long-term, unmanned SS collection. It is also compatible with dissolved component collection. Its performance was validated in a forested catchment by applying to radiocesium and stable carbon transport.

Seasonal and snowmelt-driven changes in the water-extractable organic carbon dynamics in a cool-temperate Japanese forest soil, estimated using the bomb-14C tracer

Water-extractable organic carbon (WEOC) in soil consists of a mobile and bioavailable portion of the dissolved organic carbon (DOC) pool. WEOC plays an important role in dynamics of soil organic carbon (SOC) and transport of radionuclides in forest soils. Although considerable research has been conducted on the importance of recent litter versus older soil organic matter as WEOC sources in forest soil, a more thorough evaluation of the temporal pattern of WEOC is necessary. We investigated the seasonal variation in WEOC in a Japanese cool-temperate beech forest soil by using the carbon isotopic composition ((14)C and (13)C) of WEOC as a tracer for the carbon sources. Our observations demonstrated that fresh leaf litter DOC significantly contributed to WEOC in May (35-52%) when the spring snowmelt occurred because of the high water flux and low temperature. In the rainy season, increases in the concentration of WEOC and the proportion of hydrophobic compounds were caused by high microbial activity under wetter conditions. From summer to autumn, the WEOC in the mineral soil horizons was also dominated by microbial release from SOC (>90%). These results indicate that the origin and dynamics of WEOC are strongly controlled by seasonal events such as the spring snowmelt and the rainy seasons intense rainfall.