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In this study, the effect of temperature, water quality, and the impact of an intense typhoon event on change in 137Cs concentration in the water of agricultural and forested rivers near the Fukushima Daiichi nuclear power plant (Japan) was evaluated using monthly stationary observations obtained under baseflow conditions 2.8–10.6 years after the nuclear accident in 2011. The dissolved 137Cs concentration fluctuated seasonally with water temperature in all rivers, and the increase in dissolved 137Cs concentration for unit increase in temperature was higher in forested rivers than in agricultural rivers. The relationship between water temperature and the apparent distribution coefficient of 137Cs well followed the van 't Hoff equation in the two agricultural rivers, where the enthalpy of reaction was estimated as −15.6 and −19.6 kJ mol−1. The van 't Hoff equation was not well followed for a forested river, where the suspended solids mainly comprised organic matter, suggesting that the dominant process determining dissolved 137Cs concentrations in forested rivers is not only water temperature effect on ion exchange, but rather the input of 137Cs and K+ (competing with 137Cs for exchange sites on mineral particles) into the water phase via litter leaching. Suspended solids concentrations in agricultural rivers correlated negatively with 137Cs concentrations in suspended solids, suggesting an increased proportion of coarse particles or the input of soils with low 137Cs concentration from decontaminated agricultural land. At some sites, 137Cs concentrations in dissolved form and in suspended solids were reduced sharply in association with the passage of Typhoon Hagibis in October 2019, suggesting that Typhoon Hagibis caused large-scale surface erosion that removed the source of 137Cs. [Display omitted] • Trend of 137Cs concentration in river water was analyzed based on 8 years monitoring. • Seasonal change in dissolved 137Cs concentration was mostly affected by temperature. • Typhoon Hagibis caused reduction in particulate/dissolved 137Cs in some rivers. • 137Cs concentration in forested river was poorly regressed by the van't Hoff equation. • The 137Cs reaction enthalpy in two agricultural rivers was −15.6 and −19.6 kJ mol−1. [ABSTRACT FROM AUTHOR]

Abstract This study investigated the transport of 137Cs within a forest ecosystem by examining temporal changes in the inventory and determining the major pathways of transfer following significant atmospheric deposition. A forested area of eastern Japan was monitored for four years immediately after the Fukushima nuclear power plant accident in March 2011 that released a large amount of radionuclides. The long physical half-life of 137Cs means that contamination can persist for decades, so it is vital to understand the mechanisms underlying the 137Cs dynamics in ecosystems. We sampled litterfall, throughfall, and soil, mainly from a cedar stand, over a four-year period, and analyzed the 137Cs concentrations of each sample to determine the transfer rate and total inventory. After validating our methodology through a comparison with results from an earlier study, we determined the temporal changes in the 137Cs distribution and in the major transfer pathway. Results showed that most 137Cs intercepted by canopies was transferred rapidly over the first nine months, and that the major pathway was not litterfall but throughfall. The ecological half-life of the 137Cs stocked in the canopy was calculated for both the early and later stages of contamination. Although the former is consistent with previous results, the latter ecological half-life is somewhat longer, probably because of dependence on the meteorological and tree physiological conditions at the site. This study presents valuable new data on the post-Fukushima 137Cs contamination, enhancing our understanding of the associated dynamics in forest ecosystems. Graphical abstract Unlabelled Image Highlights • The Fukushima accident provided an opportunity to understand the fate of radionuclides • An area in Japan was monitored for 137Cs transfer from canopies to the forest floor • Throughfall transferred much more 137Cs than litterfall, regardless of tree species. • At a cedar stand, most 137Cs was transferred within nine months of the accident. • General trends obtained by comparisons with previous studies are also discussed. [ABSTRACT FROM AUTHOR]

Cryptomeria japonica trees in the area surrounding Fukushima, Japan, intercepted 137 Cs present in atmospheric deposits soon after the Fukushima nuclear accident in March 2011. To study the uptake and translocation of 137 Cs in C. japonica leaves, we analyzed activity concentrations of 137 Cs and the concentration ratios of 137 Cs to 133 Cs ( 137 Cs/ 133 Cs) in old and new leaves of C. japonica collected from a forest on Mount Tsukuba between 9 and 15 months after the accident. Both isotopes were also analyzed in throughfall, bulk precipitation and soil extracts. Water of atmospheric and soil origin were used as proxies for deciphering the absorption from leaf surfaces and root systems, respectively. Results indicate that 20–40% of foliar 137 Cs existed inside the leaf, while 60–80% adhered to the leaf surface. The 137 Cs/ 133 Cs ratios inside leaves that had sprouted before the accident were considerably higher than that of the soil extract and lower than that of throughfall and bulk precipitation. Additionally, more than 80% of 137 Cs in throughfall and bulk precipitation was present in the dissolved form, which is available for foliar uptake, indicating that a portion of the 137 Cs inside old leaves was presumably absorbed from the leaf surface. New leaves that sprouted after the accident had similar 137 Cs/ 133 Cs ratios to that of the old leaves, suggesting that internal 137 Cs was translocated from old to new leaves. For 17 species of woody plants other than C. japonica , new leaves that sprouted after the accident also contained 137 Cs, and their 137 Cs/ 133 Cs ratios were equal to or higher than that of the soil extract. These results suggested that foliar uptake and further translocation of 137 Cs is an important vector of contamination in various tree species during or just after radioactive fallout. [ABSTRACT FROM AUTHOR]

Abstract: Soil cores and rainwater were sampled under canopies of Cryptomeria japonica in four montane areas along an atmospheric depositional gradient in Kanto, Japan. Soil cores (30cm in depth) were divided into 2-cm or 4-cm segments for analysis. Vertical distributions of elemental enrichment ratios in soils were calculated as follows: (X/Al)i/(X/Al)BG (where the numerator and denominator are concentration ratios of element-X and Al in the i- and bottom segments of soil cores, respectively). The upper 14-cm soil layer showed higher levels of Cu, Zn, As, Sb, and Pb than the lower (14–30cm) soil layer. In the four areas, the average enrichment ratios in the upper 6-cm soil layer were as follows: Pb (4.93)≥Sb (4.06)≥As (3.04)>Zn (1.71)≥Cu (1.56). Exogenous elements (kg/ha) accumulated in the upper 14-cm soil layer were as follows: Zn (26.0)>Pb (12.4)>Cu (4.48)≥As (3.43)≥Sb (0.49). These rank orders were consistent with those of elements in anthropogenic aerosols and polluted (roadside) air, respectively, indicating that air pollutants probably caused enrichment of these elements in the soil surface layer. Approximately half of the total concentrations of As, Sb, and Pb in the upper 14-cm soil layer were derived from exogenous (anthropogenic) sources. Sb showed the highest enrichment factor in anthropogenic aerosols, and shows similar deposition behavior to NO3 −, which is a typical acidic air pollutant. There was a strong correlation between Sb and NO3 − concentrations in rainfall (e.g., in the throughfall under C. japonica: [NO3 −]=21.1 [dissolved Sb], r =0.938, p <0.0001, n =182). Using this correlation, total (cumulative) inputs of NO3 − were estimated from the accumulated amounts of exogenous Sb in soils, i.e., 16.7t/ha at Mt. Kinsyo (most polluted), 8.6t/ha at Mt. Tsukuba (moderately polluted), and 5.8t/ha at the Taga mountain system (least polluted). There are no visible ecological effects of these accumulated elements in the Kanto region at present. However, the concentrations of some elements are within a harmful range, according to the Ecological Soil Screening Levels determined by the U.S. Environmental Protection Agency. [Copyright &y& Elsevier]

Abstract: Surface soil samples, which had no significant As contamination, were examined for As(V) reduction, As(III) oxidation and As mobilization capability. All five soil samples tested exhibited microbial As(V)-reducing activities both in aerobic and anaerobic conditions. Under aerobic conditions when As(V) reduction had almost ceased, oxidation of As(III) to As(V) occurred, whereas only As(V) reduction was observed under anaerobic conditions. In cultures incubated with As(III), As(III) was oxidized by indigenous soil microbes only under aerobic conditions. These results indicate that microbial redox transformations of As are ubiquitous in the natural environment regardless of background As levels. Mobilization through microbially mediated As(V) and Fe(III) reduction occurred both in the presence and absence of oxygen. Significant variation in dissolved As occurred depending on the Fe contents of soils, and re-immobilization of As arose in the presence of oxygen, presumably as a consequence of dissolved As(III) and Fe(II) oxidation. There was no apparent correlation between dissolved Fe(II) and As, suggesting that reductive dissolution of Fe(III) minerals does not necessarily determine the extent of As release from soils. [Copyright &y& Elsevier]

Dry deposition fluxes (F L) of NO3 − and SO4 2− to leaf surfaces were measured for Japanese red pine (Pinus densiflora), Japanese cedar (Cryptomeria japonica), Japanese cypress (Chamaecyparis obtusa), and Japanese white oak (Quercus myrsinaefolia), together with atmospheric concentrations (C L) of NO x (NO+NO2), T-NO3 (gaseous HNO3 +particulate NO3 −) and SO x (gaseous SO2 +particulate SO4 2−) around the leaves in a suburban area of Japan, using a modified leaf-washing technique. F L of NO3 − and SO4 2− decreased as follows: pine>>cedar>cypress≥oak and pine>>cedar>oak≥cypress, respectively. F L of NO3 − for all tree species fluctuated synchronously with C L of T-NO3. F L of SO4 2− fluctuated with C L of SO x , but the dominant pollutant deposited (SO2 or SO4 2−) appeared to differ for different tree species. Dry deposition conductance (K L) of T-NO3 and SO x was derived as an F L/C L ratio. Seasonal variations of K L likely reflect the gas/particle ratios of T-NO3 and SO x , which were affected by meteorological conditions such as temperature. Dry deposition velocities (V d) of T-NO3 and SO x were obtained as the mathematical product of annual mean K L and the total leaf surface areas in the forests. The comparison of V d among tree species indicated that the loads of acidic air pollutants were higher to coniferous forests than broad-leaved forest because of the higher K L and/or larger leaf surface areas. [Copyright &y& Elsevier]

Japanese cedar (Cryptomeria japonica) is the main timber species in Japan. The prediction of the temporal changes in the 137Cs concentration in the stemwood of Japanese cedar after the Fukushima nuclear accident is essential for optimizing forest management in contaminated areas. However, it is difficult to estimate the respective contributions of root and foliar uptake to 137Cs accumulation in stemwood from simple field measurements, especially in trees that contain the residue of initially-deposited 137Cs. In this study, we devised a method for estimating the rate of 137Cs root uptake into stemwood using the 133Cs content in stemwood and the 137Cs/133Cs ratio in the exchangeable fraction of soil. As a trial, the method was applied to a cedar stand in Fukushima Prefecture, using available monitoring data from prior studies over 5 years from August 2011 to August 2016. The mean annual rate of 137Cs root uptake into stemwood over this period was estimated as 53 ± 20 Bq m−2 yr−1. We note that our method likely provided a maximum estimate, because it is based on the assumptions that 133Cs in wood is exclusively supplied by root uptake, and that Cs isotopes are taken up by roots in the top 5 cm of mineral soil. Moreover, the mean annual increase of the 137Cs inventory in stemwood during the study period was measured as 108 Bq m−2 yr−1, although this value was associated with considerable uncertainty (95% confidence interval from −109 to 324 Bq m−2 yr−1). As a result, the maximum estimated rate of 137Cs root uptake into stemwood accounted for around half of the measured rate of 137Cs accumulation in stemwood. Our results show that the Cs isotopic approach has potential to distinguish the main pathway of stemwood contamination (i.e., root vs. foliar uptake) following radioactive fallout. Unlabelled Image • A method was devised for estimating the rate of 137Cs root uptake into stemwood. • We tested the method at a cedar stand in Fukushima using data from 2011 to 2016. • Maximum estimate accounted for the half of the total 137Cs accumulation in stemwood. • This isotopic approach can contribute to revealing the origin of 137Cs in stemwood. [ABSTRACT FROM AUTHOR]

Microbially mediated arsenate (As(V)) and Fe(III) reduction play important roles in arsenic (As) cycling in nature. Extracellular electron shuttles can impact microbial Fe(III) reduction, yet little is known about their effects on microbial As mobilization in soils. In this study, microcosm experiments consisting of an As-contaminated soil and microbial communities obtained from several pristine soils were conducted, and the effects of electron shuttles on As mobilization were determined. Anthraquinone-2,6-disulfonate (AQDS) and riboflavin (RF) were chosen as common exogenous and biogenic electron shuttles, respectively, and both compounds significantly enhanced reductive dissolution of As and Fe. Accumulation of Fe(II)-bearing minerals was also observed, which may lead to re-immobilization of As after prolonged incubation. Interestingly, Firmicutes -related bacteria became predominant in all microcosms, but their compositions at the lower taxonomic level were different in each microcosm. Putative respiratory As(V) reductase gene ( arrA ) analysis revealed that bacteria closely related to a Clostridia group, especially those including the genera Desulfitobacterium and Desulfosporosinus , might play significant roles in As mobilization. These results indicate that the natural soil microbial community can use electron shuttles for enhanced mobilization of As; the use of this type of system is potentially advantageous for bioremediation of As-contaminated soils. [ABSTRACT FROM AUTHOR]

The temperature and oxygen environment play important roles in the desorption of 137Cs from freshwater lake sediment to lake water. In this study, 12 quarterly surveys were performed to measure the dissolved 137Cs concentration in surface and bottom lake water, the vertical distribution of water temperature, and the dissolved oxygen (DO) concentration at the upstream, midstream, and downstream sites of the Yokokawa Dam Lake in Fukushima Prefecture, Japan. Higher concentrations of dissolved 137Cs were detected in the bottom water than in the surface water, especially in the summer and midstream lake regions at depths of 8–21 m owing to higher temperatures, which activated the bacterial decomposition of organic matter, and anaerobization, which enhanced the NH 4 + in the pore water and 137Cs desorption from mineral particles. To compare the effects of anaerobization and increasing temperature on 137Cs desorption from sediment particles, intact sediment core samples were collected from the lake midstream and incubated for 1–14 days in a chamber under three controlled temperature and oxygen environment conditions: aerobic +10 °C; anaerobic +10 °C; and anaerobic +20 °C. The vertical distribution of 137Cs in the sediment pore water showed a similar profile as NH 4 + and K+, and both the increased temperature and reduced DO concentration enhanced the 137Cs desorption. A comparison of the standard partial regression coefficients of temperature and DO concentration in the multiple regression equation for the 137Cs concentration in pore water shows that the reduction of DO from saturation to zero at the water–sediment interface accelerated the desorption of 137Cs more strongly than did the temperature rise from 10 to 20 °C. The experimental results show a nearly inverse proportional relationship between NH 4 + and the distribution coefficients of 137Cs after thermodynamic correction, except in the surface layer. These findings indicate that the 137Cs concentration in pore water can be explained by the temperature-dependent chemical distribution between the solid–aqueous phase and its equilibrium with NH 4 +. [Display omitted] • Dissolved 137Cs in the midstream area of bottom lakewater is high in summer. • Reduced dissolved oxygen promotes Cs desorption more than temperature rise. • 137Cs desorption in sediment appears to be determined by NH 4 + dynamics. [ABSTRACT FROM AUTHOR]

Abstract: Speciation of Al, including inorganic monomeric Al (Ali, the sum of aquo, hydroxy and inorganically complexed forms), organic monomeric Al (Alo, the organically complexed form), and colloidal mineral Al (Alc, the fine particulate form that passes through a 0.4-μm pore size membrane filter), was investigated in stream waters (pH 6–8) of 4 watersheds in Japan. Total dissolved Al (Alt, the sum of Alc, Ali and Alo) ranged from 0.03 to 3.31μM, and Alc was a minor component (<22% of Alt) in most of the streams. Ali was dominant (71% of Alt) in stream waters with low concentrations of Alt (<0.25μM), while the Alo fraction (37%) was almost as large as the Ali fraction (39%) in the highest class (Alt >1μM). In spite of the variation in the range of reactive Al (Alr, the sum of Ali and Alo) in the 4 watersheds (Miomote, 0.03–3.27μM; Tsukuba, 0.06–0.71μM; Dorokawa, 0.05–0.71μM; Tama, 0.03–0.38μM), the entire data set for Alr could be expressed as a function of the ratio of dissolved organic C (DOC) and Ca: [Al r (μM)]= 0.13 [DOC/Ca (mol/mol)]+0.11 (r =0.86, P <0.001). Alr increased in proportion to the DOC/Ca ratio in Japanese stream waters. Although acidic deposition in Japan has already resulted in elevated concentrations of in stream waters, a high level of Ca (instead of Al) is serving as a major counterion for . However, an additional loading of acidic deposition may result in shortage of Ca and mobilization of Al as a counterion for , and continuous observation of the speciation of Al in Japanese stream waters may reveal future change in the conditions for mobilization of Al from “low Ca and high DOC” to “low Ca and high ”. [Copyright &y& Elsevier]