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Particle-size-fractioned transfer of dioxins from sediments to water columns by resuspension process Full text
2009
Kitamura, Kimiyoshi | Sakurai, Takeo | Choi, Jae-Won | Kobayashi, Jun | Imaizumi, Yoshitaka | Suzuki, Noriyuki | Morita, Masatoshi
Particle-size-fractioned transfer of dioxins from sediments to water columns by resuspension process was investigated, using supernatant samples obtained from shaking experiments of sediment-water pairs simulating natural disturbances. The concentrations (dry-matter mass basis) of individual compounds (Cfraction) in two particle size fractions (0.1-1 and 1-10 μm) in the supernatants were generally slightly higher than those in the original sediment (Csed). Cfraction/Csed ratios ranged from 0.45 to 5.9 (median 1.5) without consistent differences among congener groups or consistent correlations against the number of chlorine atoms. The dioxin concentrations in the water column associated with the remaining sediment particles can therefore be estimated by those in the original sediment and by the concentration of suspended sediment particles in the water. The concentration of each compound in the remaining sediment particles (mostly 0.1-10 μm in size) can be roughly estimated by multiplying the concentration in the original sediment by 1.5. Dioxin concentrations (dry-matter mass basis) in sediment particles resuspended in the water column were slightly higher than or comparable to those in the bottom sediment.
Show more [+] Less [-]Cesium-137 and 137Cs/133Cs atom ratios in marine zooplankton off the east coast of Japan during 2012–2020 following the Fukushima Dai-ichi nuclear power plant accident Full text
2022
Ikenoue, Takahito | Yamada, Masatoshi | Ishii, Nobuyoshi | Kudo, Natsumi | Shirotani, Yuhei | Ishida, Yasuo | Kusakabe, Masashi
We measured the concentrations of cesium isotopes (¹³³Cs, ¹³⁴Cs, and ¹³⁷Cs) in zooplankton samples collected in waters off the east coast of Japan from May 2015 to June 2020. By combining these data with those obtained previously from May 2012 to February 2015, we evaluated the long-term impacts of the Fukushima Dai-ichi Nuclear Power Plant accident on marine zooplankton. Relatively high ¹³⁷Cs concentrations in zooplankton, exceeding 10 Bq/kg-dry weight, were sporadically observed until June 2016, regardless of year or station. After May–June 2017, ¹³⁷Cs concentrations decreased to below 1 Bq/kg-dry at most stations, and by May 2020, concentrations were below 0.5 Bq/kg-dry except those off Fukushima Prefecture. Since the accident, the ¹³⁷Cs/¹³³Cs atom ratios of zooplankton samples were higher than those of ambient seawater until 2019, but in May–June 2020 the ratios matched those of seawater except off Fukushima Prefecture. Highly radioactive particles were not detected in zooplankton samples by autoradiography using imaging plates after May–June 2017, although they were before. Therefore, the persistence of elevated ¹³⁷Cs/¹³³Cs ratios in zooplankton relative to seawater for nine years after the accident was probably due to the incorporation of highly radioactive particles (cesium-bearing particles or clay-mineral aggregates with highly adsorbed radiocesium) onto/into zooplankton for several years after the accident. However, since at least May–June 2017, these elevated ratios have likely been caused by small highly radioactive particles (or larger particles disaggregated into small pieces) entering the ocean from land via rivers or directly discharged from the Fukushima Nuclear Power Plant. Microplastics enriched with radiocesium with higher ¹³⁷Cs/¹³³Cs ratios than seawater may have also contributed ¹³⁷Cs to the zooplankton.
Show more [+] Less [-]Quantitative analysis of organophosphate pesticides and dialkylphosphates in duplicate diet samples to identify potential sources of measured urinary dialkylphosphates in Japanese women Full text
2022
Tsuchiyama, Tomoyuki | Ito, Yuki | Oya, Naoko | Nomasa, Karin | Sato, Hirotaka | Minato, Kyoko | Kitamori, Kazuya | Oshima, Shiori | Minematsu, Ayako | Niwa, Kazumasa | Katsuhara, Miki | Fukatsu, Kosuke | Miyazaki, Hitoshi | Ebara, Takeshi | Kamijima, Michihiro
Increased levels of dialkylphosphates (DAP) in maternal urine are associated with a variety of adverse developmental outcomes in children. Although urinary DAP levels are usually considered to be a marker of exposure to organophosphate (OP) pesticides, excretion of DAP may also increase by ingesting preformed DAP. To date, no study has quantitatively assessed the possible contribution of the dietary intake of preformed DAP and OP pesticides to urinary levels of DAP. Therefore, we aimed to estimate the levels of 6 DAPs and 84 OP pesticides in duplicate diet samples and urine samples collected from 73 women living in urban areas of Japan in 2018. DAP and OP pesticides were detected in 94% and 45% of diet samples, while DAP was detected in 100% of urinary samples, respectively. The average daily intake of preformed DAP was significantly higher than that of parent OP pesticides in our participants. Dimethylphosphate and diethylphosphate were predominant in the preformed DAP, and the estimated average daily intake of total amount of DAP was 78.3 nmol. Fruits and vegetables were the major dietary sources of DAP. Dietary intake of DAP was positively associated with urinary DAP levels, suggesting that a considerable amount of urinary DAP was derived from ingesting preformed DAP. Our results show that attributing urinary DAP levels exclusively to OP pesticide exposure would result in a substantial overestimation of the exposure level. Therefore, the urinary levels of DAP may not be suitable for evaluating OP pesticide exposure in the general urban population.
Show more [+] Less [-]Long-term changes in atmospheric nitrogen deposition and stream water nitrate leaching from forested watersheds in western Japan Full text
2021
Chiwa, Masaaki
Japan receives nitrogenous air pollutants via long-range transport from China. However, emissions of nitrogenous air pollutants in China have stabilized or decreased in recent years. This study examined both the long-term trends in atmospheric nitrogen (N) deposition from the 1990s to the 2010s and the response of stream water nitrate (NO₃⁻) leaching from forested areas in western Japan. A long-term (1992–2018) temporal analysis of atmospheric N deposition in Fukuoka (western Japan) was conducted. Atmospheric bulk N deposition was collected at forested sites in a suburban forest (Swₑₛₜ) and a rural forest (Rwₑₛₜ) in western Japan during 2009–2018. Stream water samples were also collected from four locations at sites Swₑₛₜ and Rwₑₛₜ during the same period. Results showed that atmospheric N deposition in Fukuoka started to decrease from the mid-2000s at an annual rate of −2.5% yr⁻¹. The decrease in atmospheric N deposition was attributable mainly to decreased atmospheric ammonium (NH₄⁺) deposition, which caused greater contribution of NO₃⁻ deposition to atmospheric N deposition. Concentrations of NO₃⁻ in the stream water samples from three of the four locations decreased significantly at an annual rate of −3.7 to −0.7% yr⁻¹. However, stream water NO₃⁻ concentrations increased in one watershed where understory vegetation has been deteriorating owing to the increased deer population. This might weaken the recovery of N leaching from forested areas.
Show more [+] Less [-]Evaluation of origin-depended nitrogen input through atmospheric deposition and its effect on primary production in coastal areas of western Kyusyu, Japan Full text
2021
Umezawa, Yu | Toyoshima, Kanae | Saitoh, Yu | Takeda, Shigenobu | Tamura, Kei | Tamaya, Chiaki | Yamaguchi, Akira | Yoshimizu, Chikage | Tayasu, Ichiro | Kawamoto, Kazuaki
Long term monitoring of atmospheric wet and dry depositions and associated nutrients fluxes was conducted on the coast of Japan facing the East China Sea continuously for 1 year and 2 months, with the origin of air mass investigated based on isotope analyses (Sr, Nd, and NO₃). During the same period, intensive observations of ocean conditions and the chemical composition of sinking particles collected using sediment traps were conducted to investigate the effects of atmospheric deposition-derived nutrients on phytoplankton blooms. Dry-deposition-derived nutrient inputs to the surface ocean were larger during autumn to spring than in summer due to the effect of continental air mass occasionally carrying Asian dust (yellow sand). However, these nutrients fluxes were limited (1.1–1.5 mg-N m⁻² day⁻¹ on average) and didn't appear to cause phytoplankton blooms through the year. Although average dissolved inorganic nitrogen (DIN) concentrations in rainwater were lower in oceanic air masses compared to continental air masses, wet-deposition-derived nutrient inputs to the surface ocean on rainy days during the summer (26.0 mg-N m⁻² day⁻¹ on average) were large due to higher precipitation from oceanic air masses. Wet-deposition-derived nutrients significantly increased nutrient concentrations in the surface ocean and seemed to cause phytoplankton blooms in the warm rainy season when nutrients in the surface were depleted due to increased stratification. The increase in phytoplankton biomass was reflected in increased particle sinking into the bottom layer, as well as changing chemical characteristics. The supply of flesh phytoplankton-derived labile organic matter into the bottom layer could be expected to promote rapid bacterial decomposition and contribute to the formation of hypoxic water masses in early summer when the ocean was strongly stratified. Atmospheric deposition-derived nutrients in East Asia will have important impacts on not only the oligotrophic outer ocean but also surrounding coastal areas in the warm rainy season.
Show more [+] Less [-]Nitrogen budgets in Japan from 2000 to 2015: Decreasing trend of nitrogen loss to the environment and the challenge to further reduce nitrogen waste Full text
2021
Hayashi, Kentaro | Shibata, Hideaki | Oita, Azusa | Nishina, Kazuya | Ito, Akihiko | Katagiri, Kiwamu | Shindo, Junko | Winiwarter, Wilfried
The benefits of the artificial fixation of reactive nitrogen (Nr, nitrogen [N] compounds other than dinitrogen), in the form of N fertilizers and materials are huge, while at the same time posing substantial threats to human and ecosystem health by the release of Nr to the environment. To achieve sustainable N use, Nr loss to the environment must be reduced. An N-budget approach at the national level would allow us to fully grasp the whole picture of Nr loss to the environment through the quantification of important N flows in the country. In this study, the N budgets in Japan were estimated from 2000 to 2015 using available statistics, datasets, and literature. The net N inflow to Japanese human sectors in 2010 was 6180 Gg N yr⁻¹ in total. With 420 Gg N yr⁻¹ accumulating in human settlements, 5760 Gg N yr⁻¹ was released from the human sector, of which 1960 Gg N yr⁻¹ was lost to the environment as Nr (64% to air and 36% to waters), and the remainder assumed as dinitrogen. Nr loss decreased in both atmospheric emissions and loss to terrestrial water over time. The distinct reduction in the atmospheric emissions of nitrogen oxides from transportation, at −4.3% yr⁻¹, was attributed to both emission controls and a decrease in energy consumption. Reductions in runoff and leaching from land as well as the discharge of treated water were found, at −1.0% yr⁻¹ for both. The aging of Japan's population coincided with the reductions in the per capita supply and consumption of food and energy. Future challenges for Japan lie in further reducing N waste and adapting its N flows in international trade to adopt more sustainable options considering the reduced demand due to the aging population.
Show more [+] Less [-]Worldwide cadmium accumulation in soybean grains and feasibility of food production on contaminated calcareous soils Full text
2021
Zhang, Sha | Song, Jing | Wu, Longhua | Chen, Zheng
Elevated toxins in soybeans extensively threaten Asian residents and over one billion vegetarians worldwide. An integrated dataset of toxic trace metal(loid)s especially cadmium (Cd) analysis in soybean grain samples (n = 5217) from 12 countries/regions of origin was compiled for risk analysis. Worldwide grain Cd averaged 0.093 mg kg⁻¹, but mean values varied 16-fold between regions, with South China (0.32 mg kg⁻¹) > Argentina (0.15 mg kg⁻¹) = German (0.13 mg kg⁻¹) > Japan (0.11 mg kg⁻¹) > the United States (0.064 mg kg⁻¹) > Central-North China (0.020–0.60 mg kg⁻¹) ≥ Iran (0.042 mg kg⁻¹) = Brazil (0.023 mg kg⁻¹) = South Korea (0.020 mg kg⁻¹). Regression analysis suggested widespread contamination and acidic soil features significantly contributed the elevated food Cd contamination worldwide. Arsenic (As) and lead (Pb) are also of concern because excessive levels were often observed in grains. Given that soil Cd bioavailability is generally low in alkaline pH ranges, the feasibility of producing safe food from contaminated land was investigated by greenhouse experiments with one low-Cd soybean cultivar grown on 20 contaminated calcareous soils. Equilibrium-based approaches i.e., 0.01 M CaCl₂ and in-situ porewater extractions, and diffusion-based diffusive gradients in thin-films technique were used to determine the plant-available fractions of soil metal(loid)s to explain the bioaccumulation variation. The results suggested that soybean grains bioaccumulated mean 0.76 mg Cd kg⁻¹, ranging from 0.16 to 2.1 mg kg⁻¹, whereas As and Pb bioaccumulation was low. Cadmium accumulation was closely correlated with plant-available Cd fractions especially the 0.01 M CaCl₂-extractable Cd, but negatively correlated with soil pH. Even in the alkaline pH range, a slight decrease of soil pH would increase grain Cd significantly. Study region and those arable lands that have similar soil conditions are not recommended for growing soybean unless novel remediation strategies are developed.
Show more [+] Less [-]Estimating monthly concentrations of ambient key air pollutants in Japan during 2010–2015 for a national-scale birth cohort Full text
2021
Araki, Shin | Hasunuma, Hideki | Yamamoto, Kouhei | Shima, Masayuki | Michikawa, Takehiro | Nitta, Hiroshi | Nakayama, Shoji F. | Yamazaki, Shin
Exposure to ambient air pollution is associated with maternal and child health. Some air pollutants exhibit similar behavior in the atmosphere, and some interact with each other; thus, comprehensive assessments of individual air pollutants are required. In this study, we developed national-scale monthly models for six air pollutants (NO, NO₂, SO₂, O₃, PM₂.₅, and suspended particulate matter (SPM)) to obtain accurate estimates of pollutant concentrations at 1 km × 1 km resolution from 2010 through 2015 for application to the Japan Environment and Children's Study (JECS), which is a large-scale birth cohort study. We developed our models in the land use regression framework using random forests in conjunction with kriging. We evaluated the model performance via 5-fold location-based cross-validation. We successfully predicted monthly NO (r² = 0.65), NO₂ (r² = 0.84), O₃ (r² = 0.86), PM₂.₅ (r² = 0.79), and SPM (r² = 0.64) concentrations. For SO₂, a satisfactory model could not be developed (r² = 0.45) because of the low SO₂ concentrations in Japan. The performance of our models is comparable to those reported in previous studies at similar temporal and spatial scales. The model predictions in conjunction with the JECS will reveal the critical windows of prenatal and infancy exposure to ambient air pollutants, thus contributing to the development of environmental policies on air pollution.
Show more [+] Less [-]Untangling radiocesium dynamics of forest-stream ecosystems: A review of Fukushima studies in the decade after the accident Full text
2021
Sakai, Masaru | Tsuji, Hideki | Ishii, Yumiko | Ozaki, Hirokazu | Takechi, Seiichi | Jo, Jaeick | Tamaoki, Masanori | Hayashi, Seiji | Gomi, Takashi
Forest-stream ecosystems are widespread and biodiverse terrestrial landscapes with physical and social connections to downstream human activities. After radiocesium is introduced into these ecosystems, various material flows cause its accumulation or dispersal. We review studies conducted in the decade after the Fukushima nuclear accident to clarify the mechanisms of radiocesium transfer within ecosystems and to downstream areas through biological, hydrological, and geomorphological processes. After its introduction, radiocesium is heavily deposited in the organic soil layer, leading to persistent circulation due to biological activities in soils. Some radiocesium in soils, litter, and organisms is transported to stream ecosystems, forming contamination spots in depositional habitats. While reservoir dams function as effective traps, radiocesium leaching from sediments is a continual phenomenon causing re-contamination downstream. Integration of data regarding radiocesium dynamics and contamination sites, as proposed here, is essential for contamination management in societies depending on nuclear power to address the climate crisis.
Show more [+] Less [-]Phosphorus compounds in the dissolved and particulate phases in urban rivers and a downstream eutrophic lake as analyzed using 31P NMR Full text
2021
Hafuka, Akira | Tsubokawa, Yoichi | Shinohara, Ryuichiro | Kimura, Katsuki
Phosphorus (P) discharges from human activities result in eutrophication of lakes. We investigated whether the forms of phosphorus (P) in rivers with high effluent loads flowing through urban areas of Sapporo, Japan, were transformed when transported downstream into a eutrophic lake, namely Lake Barato. We hypothesized that the inorganic P supplied from the rivers might be transformed to organic forms in the lake. The results showed that soluble reactive phosphorus (SRP) and particulate inorganic phosphorus (PIP) dominated in the river discharge to the lake. Suspended solids in the rivers were rich in iron (Fe) so PIP was associated with Fe. A comparison of the concentrations at the river mouth and 4.5 km downstream showed that the concentrations of SRP and PIP were lower at 4.5 km downstream than at the river mouth, whereas the concentrations of organic P (i.e., dissolved organic phosphorus and particulate organic phosphorus) were similar. The results from solution ³¹P nuclear magnetic resonance spectroscopy of lake water showed that pyrophosphate was only present in the particulate fraction, while orthophosphate diesters (DNA-P) were only present in the dissolved fraction. Riverine samples contained orthophosphate (ortho-P) only, while lake samples contained ortho-P, orthophosphate monoesters, and DNA-P. The results suggest that the P forms, particularly those of dissolved P, shifted from inorganic to organic forms as the water was discharged from the river to the lake.
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