Spatial variations in radiocesium deposition and litter-soil distribution in a mountainous forest catchment affected by the Fukushima nuclear accident.

The Fukushima Dai-ichi Nuclear Power Plant accident caused serious 137Cs contamination in mountainous forest areas. To understand the spatial variation in soil 137Cs inventory in complex mountainous topography and the influencing factors, a whole-area investigation of 137Cs deposition in a broad-leaved forest catchment of a mountain stream was conducted using grid sampling. Across the catchment, organic and surface mineral soil layers were collected at 42 locations in 2013 and 6 locations in 2015. Cesium-137 deposition on the forest floor exhibited high spatial heterogeneity and altitude-dependent distribution over the catchment. The 137Cs retention ratio in the organic layer, determined as the inventory in the organic layer divided by the soil (organic and mineral soil layers) inventory, ranged from 6% to 82% in 2013, and the coefficient of variation was 0.6. The 137Cs retention ratios had positive correlations with the material inventory in the organic layer and the elevation. The 137Cs retention ratios in the organic layer were less than 20% in 2015, even at the locations where the retention ratio was higher than 55% in 2013. Although there was spatial variation in the migration speed, 137Cs migration from the organic layer to mineral soil was almost completed within 4 y of the deposition, suggesting a decrease in 137Cs circulation within the forest ecosystem. This study also examined a relationship between the 137Cs inventory and the air dose rate to assess the potential of using the air dose rate to estimate soil 137Cs inventory. Soil 137Cs inventories and air dose rates were highly positively correlated, indicating that measurement of air dose rate can provide an easier and quicker alternative to measurement of soil 137Cs inventory in forest ecosystems.

Rapid analytical method of 90Sr in urine sample: Rapid separation of Sr by phosphate co-precipitation and extraction chromatography, followed by determination by triple quadrupole inductively coupled plasma mass spectrometry (ICP-MS/MS).

A rapid analytical method for determining 90Sr in urine samples (1-2 L) was developed to assess the internal exposure of workers in a radiological emergency. Strontium in a urine sample was rapidly separated by phosphate co-precipitation, followed by extraction chromatography, and the 90Sr activity was determined by triple quadrupole inductively coupled plasma mass spectrometry (ICP-MS/MS). Measurement in the MS/MS mode with an O2 reaction gas flow rate 1 mL min-1 showed no tailing of 88Sr at m/z = 90 up to 50 mg L-1 Sr. The interferences of Ge, Se and Zr at m/z = 90 were successfully removed by phosphate co-precipitation, followed by extraction chromatography with a tandem column of Pre-filter, TRU and Sr resin. This analytical method was validated by the results of the analyses of synthetic urine samples (1.2-1.6 L) containing a known amount of 90Sr along with 1 mg of each of Ge, Se, Sr and Zr. The turnaround time for Sr purification from the urine sample and the 90Sr measurement by ICP-MS/MS was about 10 h. The detection limit of 90Sr was approximately 1 Bq per urine sample, which was lower than 15 Bq per urine after a day of intake giving 5 mSv of unplanned exposure of worker limited by Nuclear Regulation Authority of Japan.

Post-deposition early-phase migration and retention behavior of radiocesium in a litter-mineral soil system in a Japanese deciduous forest affected by the Fukushima nuclear accident.

The fate of radiocesium (137Cs) derived from the Fukushima nuclear accident and associated radiation risks are largely dependent on its migration and retention behavior in the litter-soil system of Japanese forest ecosystems. However, this behavior has not been well quantified. We established field lysimeters in a Japanese deciduous broad-leaved forest soon after the Fukushima nuclear accident to continuously monitor the downward transfer of 137Cs at three depths: the litter-mineral soil boundary and depths of 5 cm and 10 cm in the mineral soil. Observations were conducted at two sites within the forest from May 2011 to May 2015. Results revealed similar temporal and depth-wise variations in 137Cs downward fluxes for both sites. The 137Cs downward fluxes generally decreased year by year at all depths, indicating that 137Cs was rapidly leached from the forest-floor litter layer and was then immobilized in the upper (0-5 cm) mineral soil layer through its interaction with clay minerals. The 137Cs fluxes also showed seasonal variation, which was in accordance with variations in the throughfall and soil temperature at the sites. There was no detectable 137Cs flux at a depth of 10 cm in the mineral soil in the third and fourth years after the accident. The decreased inventory of mobile (or bioavailable) 137Cs observed during early stages after deposition indicates that the litter-soil system in the Japanese deciduous forest provides only a temporary source for 137Cs recycling in plants.

Catchment-scale distribution of radiocesium air dose rate in a mountainous deciduous forest and its relation to topography.

A large number of air dose rate measurements were collected by walking through a mountainous area with a small gamma-ray survey system, KURAMA-II. The data were used to map the air dose rate of a mountainous deciduous forest that received radiocesium from the Fukushima Dai-ichi Nuclear Power Plant accident. Measurements were conducted in a small stream catchment (0.6 km(2) in area) in August and September 2013, and the relationship between air dose rates and the mountainous topography was examined. Air dose rates increased with elevation, indicating that more radiocesium was deposited on ridges, and suggesting that it had remained there for 2.5 y with no significant downslope migration by soil erosion or water drainage. Orientation in relation to the dominant winds when the radioactive plume flowed to the catchment also strongly affected the air dose rates. Based on our continuous measurements using the KURAMA-II, we describe the variation in air dose rates in a mountainous forest area and suggest that it is important to consider topography when determining sampling points and resolution to assess the spatial variability of dose rates and contaminant deposition.

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 ((137)Cs) contamination of forest ecosystems located in mountainous and hilly regions with steep terrain. To understand topographic effects on the redistribution and accumulation of (137)Cs on forest floor, we investigated the distribution of Fukushima-derived (137)Cs 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 (137)Cs were accumulated in large amounts at the bottom of the hillslope. At the bottom, a significant fraction (65%) of the (137)Cs 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 (137)Cs in May 2011 (two months after the accident) and (137)Cs 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 (137)Cs redistribution on a forested hillslope is strongly controlled by biologically mediated processes and continues to supply (137)Cs to the bottom via litterfall at a reduced rate.

Non-HPLC rapid separation of metallofullerenes and empty cages with TiCl4 Lewis acid.

Rapid and efficient separation/purification of pure metallofullerenes M(x)@C(n) (M = metal; x = 1, 2; n > 70) and carbide metallofullerenes of the type M(y)C(2)@C(n-2) (y = 2, 3, 4; n - 2 > 68) has been reported. The present method utilizes rapid and almost perfect preferential formation of TiCl(4) (generally known as a Lewis acid)-metallofullerene complexes, which easily decompose to provide pure metallofullerene powders by a simple water treatment. The present method enables one to separate the metallofullerenes up to >99% purity within 10 min without using any type of high-performance liquid chromatography (HPLC). It is found that the oxidation potentials of the metallofullerenes are crucial factors for efficient purification. The current separation/purification technique may open a brand-new era for inducing further applications and commercialization of endohedral metallofullerenes.