Variability in radiocesium activity concentration in growing hardwood shoots in Fukushima, Japan.

The radiocesium contamination caused by the Fukushima Daiichi Nuclear Power Plant accident has made it difficult to use coppice woods as bed logs for mushroom cultivation. Evaluating the variability in the radiocesium activity concentration of logs is necessary in order to predict how many coppice woodlands are available for producing mushroom bed logs. To clarify the variability in radiocesium activity concentrations and to estimate the sample size required to estimate these concentrations with sufficient accuracy, we modeled the log-transformed radiocesium activity concentrations in growing shoots of hardwoods. We designed two models: (1) a model with mean concentrations that varied among stands with a standard deviation that was the same among stands, and (2) a model with varying means and standard deviations. We fit the data pertaining to only Quercus serrata to both models and calculated the widely applicable information criterion values. Consequently, we adopted the simpler model (1). Applying the selected model to data for all species, we examined the relationship between the number of measurement individuals and the predictive distribution of the expected concentration. Based on previous recommendations and measurement costs, we proposed that five individuals would be appropriate for estimating radiocesium activity concentration in a stand.

Factors controlling dissolved 137Cs activities in coastal waters on the eastern and western sides of Honshu, Japan.

The distributions of dissolved 137Cs in river, nearshore, and offshore waters on the east and west coasts of the Japanese island of Honshu were studied in 2018-2021, 7-10 years after the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. On the east side along the north western North Pacific (Fukushima Prefecture), estuarine processes, including desorption from riverine particles and dissolution into pore water from riverine particles that had settled to the seafloor, contributed to the maintenance of high dissolved 137Cs activities in nearshore and offshore waters. A survey and mass-balance calculation in a semi-enclosed estuarine area, the Matsukawa-ura, in the northern part of Fukushima, provided convincing evidence that rivers contributed to the influx of 137Cs to coastal waters. In contrast, the extremely low activities of dissolved and particulate 137Cs in the Tedori River of Ishikawa Prefecture on the western side of Japan along the Japan Sea suggested that inputs of riverine 137Cs made a negligible contribution to the increase of dissolved 137Cs activities in the nearshore and offshore waters. The relatively high dissolved 137Cs activities observed in the offshore waters of the Japan Sea were due to movement of FDNPP-derived 137Cs into the Japan Sea via the Tsushima Warm Current. Mechanisms controlling the distributions of 137Cs activities in coastal waters of the eastern and western sides of Japan therefore differ.

Speciation of cesium in tree tissues and its implication for uptake and translocation of radiocesium in tree bodies.

Since the Chernobyl and Fukushima nuclear power plant accidents, extensive research has focused on the distribution and cycle of radiocesium in forest systems. Nevertheless, direct chemical speciation analyses of Cs by spectroscopic methods are limited by the low abundances of stable Cs as well as radiocesium in trees. In this study, we investigated coordination structures of Cs in 133Cs-doped bark, sapwood, heartwood, needle, and branch samples of trees collected in Fukushima by extended X-ray absorption fine structure (EXAFS) spectroscopy. We examined four representative tree species in Fukushima, Cryptomeria japonica, Pinus densiflora, Quercus serrata, and Eleutherococcus sciadophylloides. EXAFS spectra suggested that Cs was adsorbed as an outer-sphere complex on all parts of the four species, with electrostatic binding to negatively charged functional groups in components of tree tissues. These results were supported by extraction experiments where more than 98.5% of the sorbed Cs was desorbed from all parts of each tree species using 1 M CH3COONH4. Sorption experiments of Cs on cellulose, an important component of plant cell walls, were carried out in ultrapure water, NaCl, and KCl solutions. The Kd values for cellulose and solutions were not high enough to fix Cs, considering the composition of sap in trees. Overall, the results of this study are consistent with previous field observations indicating that radiocesium is translocated in mobile form to metabolically active tree parts.

Relationship between the activity concentration of 137Cs in the growing shoots of Quercus serrata and soil 137Cs, exchangeable cations, and pH in Fukushima, Japan.

Incorporation of radiocesium by plants via root uptake appears to be affected by some of the exchangeable cations in the soil and/or pH of the soil. However, few studies have examined the relationship between 137Cs in trees and soil properties in the area surrounding the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) after the accident in March 2011. To elucidate the relationships between the root uptake of 137Cs by deciduous broadleaved trees and soil properties, we measured the activity concentration of 137Cs in the growing shoots of coppiced konara oak (Quercus serrata) grown after the FDNPP accident and the amounts of total 137Cs; exchangeable (ex-) 137Cs, ex-K, ex-Mg, and ex-Ca; and pH (H2O) in soils collected from 34 forest stands in Fukushima between December 2016 and May 2017. Ex-137Cs showed a positive linear relationship with the activity concentration of 137Cs in the growing konara oak shoots, whereas ln-transformed ex-K, ex-Mg, ex-Ca, and pH (H2O) showed negative linear relationships with ln-transformed 137Cs activity concentrations in the growing shoots. However, only ex-137Cs and ex-K were identified as significant factors determining the activity concentration of 137Cs in konara oak according to multiple regression methods and a model selection using Akaike information criterion; ex-K had a stronger influence on the activity concentration of 137Cs in konara oak than ex-137Cs. In the present study, we demonstrated that soil ex-K negatively and non-linearly alters 137Cs activity concentration in deciduous broadleaved trees. We also noted that the relationship between 137Cs in deciduous broadleaved trees and soil ex-K in forests without K fertilization was similar to the relationships between 137Cs in other plants and ex-K in K-fertilized lands reported in previous studies of the FDNPP accident.

Web-building spider Nephila clavata (Nephilidae: Arachnida) can represent 137Cs contamination of arthropod communities and bioavailable 137Cs in forest soils at Fukushima, Japan.

Large areas of Fukushima's forests were contaminated with radiocesium (137Cs) after the Fukushima Dai-ichi Nuclear Power Plant accident. Most of the contaminated forests have not been decontaminated, and bioavailable 137Cs is likely to circulate within the forest environment's food web. Nephila clavata (Nephilidae: Arachnida) is a top predator in the forest arthropod community, and this web-building spider potentially consumes many arthropod species presented in the grazing and detrital food chains. We tested whether 137Cs in the spider could serve as a proxy for 137Cs contamination of these arthropod communities. We also examined whether N. clavata could serve as a proxy for soil bioavailable 137Cs. Nephila clavata was similarly or more contaminated with 137Cs compared with lower-trophic-level arthropods such as herbivores and other predators at the same trophic level. Thus, the 137Cs activity of N. clavata could represent the extent to which the arthropod community was contaminated with 137Cs. Data from nine 137Cs-contaminated sites in Fukushima showed a significant positive correlation between soil bioavailable 137Cs and N. clavata's 137Cs activity05 but the coefficient of determination was only moderate (R2 = 0.43), suggesting that N. clavata is only a weak proxy of soil bioavailable 137Cs. Our results also showed that the bioavailable fraction of 137Cs in Fukushima was strongly correlated with the total inventory and that the K and Na contents of the soil determined the soil-to-spider transfer factor for 137Cs and the 137Cs activity in N. clavata, respectively. These results improve our understanding of 137Cs transfer from the soil to arthropod species.

Six-year trends in exchangeable radiocesium in Fukushima forest soils.

We investigated the changes in 137Cs exchangeable fraction in the soils of contaminated forest ecosystems until 6 years after the Fukushima radioactive atmospheric deposits. For this investigation, we performed chemical extractions of 137Cs from both organic and mineral soil layer sampled from two forest stands, Japanese cedar (Cryptomeria japonica) and broadleaf deciduous, mainly konara oak (Quercus serrata), which are located 26-27 km inland from the Fukushima Dai-ichi Nuclear Power Plant. The exchangeable 137Cs as a proportion of the total 137Cs inventory was only 10% in the organic layer and 6.1% in the mineral soil layer about 5 months after the accident at the Japanese cedar site. We observed an exponential decrease in the proportion of exchangeable 137Cs in both organic and mineral soil layer samples over the 6-years observation period at both sites. The proportion significantly decreased within 2-4 years after the accident, becoming almost constant (2-4%). These results support the interpretation that contaminated forests have entered a steady-state phase of 137Cs cycling, although we need more integration for an improved vision of the future of Fukushima forests.

Evaluation of radiocesium concentrations in new leaves of wild plants two years after the Fukushima Dai-ichi Nuclear Power Plant accident.

Radiocesium ((137)Cs) transfer to plants immediately after the Fukushima Dai-ichi Nuclear Power Plant accident was investigated by collecting newly emerged leaf and soil samples between May 2011 and November 2012 from 20 sites in the Fukushima prefecture. Radiocesium concentrations in leaf and soil samples were measured to calculate concentration ratios (CR). Woody plants exhibited high CR values because (137)Cs deposited on stems and/or leaves were transferred to newly emerging tissues. The CR values in 2012 declined as compared to that in 2011. Exchangeable (137)Cs rates in soil (extraction rate) samples were measured at five sites. These rates decreased at four sites in 2012 and depended on environmental conditions and soil type. Both CR values and extraction rates decreased in 2012. However, CR values reflected the changes in extraction rates and characteristics of each species. Amaranthaceae, Chenopodiaceae, and Polygonaceae, which had been identified as Cs accumulators, presented no clear (137)Cs accumulation ability. In 2012, the perennial plant Houttuynia cordata and deciduous trees Chengiopanax sciadophylloides and Acer crataegifolium displayed high CR values, indicating that these species are (137)Cs accumulators and may be considered as potential species for phytoremediation.

Inferring the chemical form of 137Cs deposited by the Fukushima Dai-ichi Nuclear Power Plant accident by measuring (137)Cs incorporated into needle leaves and male cones of Japanese cedar trees.

We hypothesized that the water-soluble (ionic) and water-insoluble (stable) radiocesium from the initial fallout of the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident was distributed in various proportions in the surrounding areas and that this distribution was reflected in the trees that suffered deposition from the initial fallout. This study attempted to evaluate local variations in the chemical form of (137)Cs derived from the initial fallout of the FDNPP accident and whether its chemical form affected the radiocesium concentration in the tissues currently growing in trees, even after the initial fallout ceased. For these estimations, the ratio between the (137)Cs concentration in Cryptomeria japonica needle leaves in the tree crown, which existed before the FDNPP accident and subsequently directly exposed to the initial fallout ((137)Cs pre-accident N), and the amount of (137)Cs in the initial fallout itself ((137)Cs fallout) was determined ((137)Cs pre-accident N/(137)Cs fallout) at 66 sites. In addition, the (137)Cs ratios between the male cones produced in 2012 ((137)Cs male cone) and needle leaves that had elongated in the spring of 2011 ((137)Cs 2011N) was determined at 82 sites ((137)Cs male cone/(137) Cs 2011N). Most of the sites with lower (137)Cs pre-accident N /(137)Cs fallout ratios were distributed in eastern Fukushima, relatively close to the Pacific Ocean coastline. Lower (137)Cs pre-accident N/(137)Cs fallout and higher (137)Cs malecone/(137)Cs 2011N were found to be associated with higher proportions of (137)Cs in ionic forms. These observations are consistent with the hypothesis, and likely reflect regional variations in the chemical form of the deposited radiocesium.

Radiocesium accumulation properties of Chengiopanax sciadophylloides.

Through the assessments of radioactive contamination after the Fukushima Dai-ichi Nuclear Power Plant (F1NPP) accident, it has been reported that some sprouts of Chengiopanax sciadophylloides (Franch. et Sav.) at the site contained radiocesium (((134),)(137)Cs) at higher concentrations than the other plants. To assess the phytoremediation properties of C. sciadophylloides for (137)Cs decontamination, we aimed to quantify the (137)Cs accumulation in C. sciadophylloides. We measured the (137)Cs concentrations in various organs of C. sciadophylloides collected from the forest in the town of Kawamata, Fukushima prefecture, together with the concentrations of other elements [potassium (K), rubidium, (133)Cs, calcium, strontium, and manganese] present. In addition, we compared the foliar concentrations of these elements in C. sciadophylloides with those in four different deciduous tree species. The mean of foliar (137)Cs concentration in C. sciadophylloides was 28.1 kBq kg(-1) DW, one order of magnitude higher than that found in the other species. The (137)Cs concentrations were in the order of leaves > bark > wood. The wood of the treetop, leaf scars, and roots contained higher amounts of (137)Cs than that of the trunk. From the distribution of (137)Cs in C. sciadophylloides, we confirmed that (137)Cs tends to accumulate in the young growing parts. The difference in the distribution of (137)Cs and (133)Cs indicated that surface uptake of (137)Cs occurs. A significant correlation between K and (137)Cs concentrations in each organ was found, which suggested that (137)Cs in the plant body is transferred through the same pathway as K. On the other hand, there was no correlation between foliar K and (137)Cs concentrations, implying that the uptake ratio of K to (137)Cs was different for each individual. To determine the factors driving specific (137)Cs accumulation and/or the variability of the ratio between K and (137)Cs, the distribution of (137)Cs and the root in soil, the difference of the expression of transporter, and the existence of mycorrhizal fungi should be considered. However, further research is required.

Relationship between radiocesium contamination and the contents of various elements in the web spider Nephila clavata (Nephilidae: Arachnida).

The accident at the Fukushima Dai-ichi nuclear power plant seriously contaminated a large area in northeast Japan with a large amount of radioactive material. Consequently, various organisms, including arthropods, in the ecosystem have been contaminated with radiocesium ((137)Cs) through the food chain. We previously showed that the web spider Nephila clavata was contaminated with (137)Cs and that the level of contamination, which varied among spider individuals, was independent of the amount of prey consumed. The present study aimed to clarify the mechanisms that could determine the level of (137)Cs contamination in N. clavata. We first demonstrated the patterns of contents of over 30 elements in N. clavata that were collected at two forest sites (PS and ES) in Fukushima and then focused on the relationships between the contents of the alkali metals Li, Na, K, and Rb and the accumulation of (137)Cs in the spiders; Cs is an alkali metal and is expected to act similarly to Li, Na, K, and Rb. We also focused on the content of the non-alkali element, Cu, which is an essential element for oxygen transport in spiders. We found that Na content correlated positively with (137)Cs accumulation at both sites, which suggested that (137)Cs accumulation in N. clavata was related with the dynamics of Na. The K-, Rb-, and Cu-(137)Cs relationships were site specific; the relationships were significant at site PS, but not significant at site ES. Factors causing the site specific relationships and the probable pathway for (137)Cs transfer from soil to plants and then to higher trophic levels are discussed in terms of the transfer processes of the alkali metals.

Radiocesium distribution in sugi (Cryptomeria japonica) in eastern Japan: translocation from needles to pollen.

We assessed the radiocesium contamination of sugi (Cryptomeria japonica) forests in eastern Japan from November 2012 to February 2013, including 80 sites in Fukushima and 35 sites in other regions (Tohoku and Kanto-Koshinetsu), by measuring the (137)Cs concentrations in needles of different ages, male flowers, and pollen. Over a wide geographic area, needles that were present at the time of the Fukushima Dai-ichi Nuclear Power Plant accident contained much higher (137)Cs concentrations than needles that emerged after the accident. This result, together with visual analysis of (137)Cs distribution using autoradiography, indicated that some of the (137)Cs derived from direct fallout remained on the surface of the older needles. Since we also detected (137)Cs in younger needles and male flowers, we concluded that (137)Cs was translocated toward the tips of sugi needles. The (137)Cs concentration in male flowers was higher than and positively correlated with that in the currently growing (2012) needles. Also, a positive relationship was observed between the (137)Cs concentration of male flowers and pollen, and they were found to be nearly identical (137)Cs concentration. These results indicate the occurrence of acropetal translocation of (137)Cs from old needles to young needles, male flowers and pollen. However, the results as related to (137)Cs concentration in the needles of three different ages differed from the results of similar studies conducted more than 4 y after the Chernobyl accident. This suggests that, 2 y after the Fukushima Dai-ichi NPP accident, the distribution of (137)Cs in the sugi forests has not yet reached a steady state.

Radiocesium contamination of the web spider Nephila clavata (Nephilidae: Arachnida) 1.5 years after the Fukushima Dai-ichi Nuclear Power Plant accident.

We measured the concentrations of radiocesium ((134)Cs and (137)Cs) in a large web spider, Nephila clavata L. Koch (Nephilidae: Arachnida), collected at three sites at different distances from the Fukushima Dai-ichi Nuclear Power Plant about 1.5 y after the accident in March 2011. The radiocesium concentrations in spiders were highest in a streamside secondary forest 33 km northwest of the power plant: mean ± a standard deviation of 2.401 ± 1.197 Bq g(-1) dry for (134)Cs and 3.955 ± 1.756 Bq g(-1) dry for (137)Cs. In a hillside secondary forest 37 km northwest of the power plant, the mean concentrations of (134)Cs and (137)Cs were 0.825 ± 0.247 Bq g(-1) dry and 1.470 ± 0.454 Bq g(-1) dry, respectively. In a pine forest 62 km west of the power plant, very low radiocesium concentrations were detected, but in only a few individuals. The concentrations of (134)Cs and (137)Cs in spiders collected at each site tended to be correlated with the air radiation dose rate at each site. Since spiders are key components of food webs in forests, the high concentrations in this species at contaminated sites suggested that the radiocesium from the accident has transferred through food chains and reached to higher trophic level of the food chains.