Release of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant accident to the marine environment was negligible.

Atmospheric deposition of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has been observed in the terrestrial environment around the FDNPP site; however, their deposition in the marine environment has not been studied. The possible contamination of Pu in the marine environment has attracted great scientific and public concern. To fully understand this possible contamination of Pu isotopes from the FDNPP accident to the marine environment, we collected marine sediment core samples within the 30 km zone around the FDNPP site in the western North Pacific about two years after the accident. Pu isotopes ((239)Pu, (240)Pu, and (241)Pu) and radiocesium isotopes ((134)Cs and (137)Cs) in the samples were determined. The high activities of radiocesium and the (134)Cs/(137)Cs activity ratios with values around 1 (decay corrected to 15 March 2011) suggested that these samples were contaminated by the FDNPP accident-released radionuclides. However, the activities of (239+240)Pu and (241)Pu were low compared with the background level before the FDNPP accident. The Pu atom ratios ((240)Pu/(239)Pu and (241)Pu/(239)Pu) suggested that global fallout and the pacific proving ground (PPG) close-in fallout are the main sources for Pu contamination in the marine sediments. As Pu isotopes are particle-reactive and they can be easily incorporated with the marine sediments, we concluded that the release of Pu isotopes from the FDNPP accident to the marine environment was negligible.

Benthic food web structures as an explanation for prolonged ecological half-life of 137Cs in flatfish species in the Fukushima coastal area.

After the accident at the Fukushima Daiichi Nuclear Power Plant (FDNPP), Japan, in March 2011, 137Cs in demersal fish had, between 2011 and 2015, a prolonged ecological half-life when compared to pelagic fish. Using stable isotope mixing models combined with gut content analysis and 137Cs activity concentrations, this study investigated the hypothesis that an unexplored food web structure could be a contributing factor explaining the ecological half-life of 137Cs in benthic flatfish. Benthic invertebrates and demersal fish species sampled in 2015 still showed 137Cs activity concentrations higher than pre-accident. The mixing models of stable N and C isotopes and gut content analysis identified deposit, suspension and filter feeders to be the main flatfish food items in the benthos. There was a significant correlation between 137Cs activity concentrations in specific flatfish species and benthos, and between 137Cs activity concentrations in benthos and surface sediment. The results of this study partially explained the 137Cs activity concentrations found in the analysed demersal fish, suggesting that the benthos can be a continuous source of 137Cs for the demersal fish during this period of time. Extending monitoring programmes to include invertebrates that are not food species for humans would greatly improve our ability to understand the role of trophic transfer pathways and take appropriate management actions.

Nanomolar phosphate supply and its recycling drive net community production in the subtropical North Pacific.

Seasonal drawdown of dissolved inorganic carbon (DIC) in the subtropical upper ocean makes a significant contribution to net community production (NCP) globally. Although NCP requires macronutrient supply, surface macronutrients are chronically depleted, and their supply has been unable to balance the NCP demand. Here, we report nanomolar increases in surface nitrate plus nitrite (N+N, ~20 nM) and phosphate (PO4, ~15 nM) from summer to winter in the western subtropical North Pacific. Molar ratios of upward fluxes of DIC:N+N:PO4 to the euphotic zone (< 100 m) were in near-stoichiometric balance with microbial C:N:P ratios (107~243:16~35:1). Comparison of these upward influxes with other atmospheric and marine sources demonstrated that total supply is largely driven by the other sources for C and N (93~96%), but not for P (10%), suggesting that nanomolar upward supply of P and its preferential recycling play a vital role in sustaining the NCP.

First isolation and analysis of caesium-bearing microparticles from marine samples in the Pacific coastal area near Fukushima Prefecture.

A part of the radiocaesium from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident was emitted as glassy, water-resistant caesium-bearing microparticles (CsMPs). Here, we isolated and investigated seven CsMPs from marine particulate matter and sediment. From the elemental composition, the 134Cs/137Cs activity ratio, and the 137Cs activity per unit volume results, we inferred that the five CsMPs collected from particulate matter were emitted from Unit 2 of the FDNPP, whereas the two CsMPs collected from marine sediment were possibly emitted from Unit 3, as suggested by (i) the presence of calcium and absence of zinc and (ii) the direction of the atmospheric plume during the radionuclide emission event from Unit 3. The presence of CsMPs can cause overestimation of the solid-water distribution coefficient of Cs in marine sediments and particulate matter and a high apparent radiocaesium concentration factor for marine biota. CsMPs emitted from Unit 2, which were collected from the estuary of a river that flowed through a highly contaminated area, may have been deposited on land and then transported by the river. By contrast, CsMPs emitted from Unit 3 were possibly transported eastward by the wind and deposited directly onto the ocean surface.

Coastal urbanization alters carbon cycling in Tokyo Bay.

The carbon budget of Tokyo Bay, a highly urbanized coastal basin, was estimated using a box model that incorporated inorganic and organic carbon data over an annual cycle (2011-2012). The surface water represented net autotrophic system in which the annual net community production (NCP) was 19 × 1010 gC year-1. The annual loading of dissolved inorganic carbon and total organic carbon (TOC) from freshwater inputs was 11.2 × 1010 and 4.9 × 1010 gC year-1, respectively. The annual TOC sedimentation rate was 3.1 × 1010 gC year-1, similar to the annual air-sea CO2 uptake (5.0 × 1010 gC year-1). Although the NCP and TOC loading from freshwater inputs were respectively 3.0 and 2.7 times lower than those in the 1970s, the TOC sedimentation rate was similar. Therefore, a relatively high carbon efflux from Tokyo Bay likely occurred in the 1970s, including CO2 efflux to the atmosphere and/or export of labile organic carbon to the open ocean. The changes in carbon flow between the 1970s and 2011-2012 resulted from improved water quality due to increased sewage treatment facilities and improved sewage treatment efficiency in the catchment, which decreased the amount of labile organic carbon flowing into the bay.

Automated colorimetric determination of nanomolar urea in seawater by gas-segmented continuous flow analysis using a liquid waveguide capillary cell.

A sensitive automated colorimetric method for the determination of nanomolar concentration of urea in seawater is presented. The colorimetry was based on the diacetyl monoxime method and the automated system was constructed by a gas-segmented continuous flow analyzer equipped with a 100 cm path length of liquid waveguide capillary cell. The most suitable surfactant for the system was hexadecyl-trimethyl-ammonium-bromide as compared to Brij-35, sodium dodecyl sulfate, and Triton X-100. Blank selection using a 3% NaCl solution, filtered subtropical surface seawater, and filtered deep seawaters with and without urease treatment showed that the filtered deep seawater with urease treatment had the lowest absorbance and was appropriate. The sample volume needed for the analysis was 1.8 mL, and the analysis rate was 10 samples h-1. Calibration curves showed good linearity for 0-1000 nM urea-N concentration range (r2 = 0.999). The detection limit was 5 nM urea-N. The coefficient of variation for the analysis of seawater samples collected in the subtropical North Pacific was <5% at 30 and 29 nM urea-N. The proposed analytical system was applicable to vertical observation in the subtropical North Pacific.

Reconstruction of radiocesium levels in sediment off Fukushima: Simulation analysis of bioavailability using parameters derived from observed 137Cs concentrations.

Radiocesium was released to the North Pacific coastal waters by the accident at the Fukushima Dai-ichi Nuclear Power Plant (1FNPP) of the Tokyo Electric Power Company (TEPCO) in March 2011. Since the radiocesium in the sediment off Fukushima was suggested as a possible source for the transfer of this radionuclide through the benthic food chain, we conducted numerical simulations of 137Cs in sediments off the Fukushima coast by using a model which incorporates dynamic transfer processes between seawater and the labile and refractory fractions in sediment particles. This model reproduced the measured temporal changes of 137Cs concentration in seabed surface sediment off Fukusima coasts, by normalizing the radiocsium transfer between seawater and sediment according to the particle diameter sizes. We found that the 137Cs level in sediment decreased by desorption during the first several months after the accident, followed by a reduction in the labile fraction until the end of 2012. The apparent decrease of the total radiocesium level in surface sediment was estimated to occur at rates of approximately 0.2 y-1 within a 20 km distance from the 1FNPP. The comparison of 137Cs level decreases in the demersal fish and the simulated temporal labile fraction in fine sediment demonstrated that the consideration of radiocesium transfer via sediment is important for determining the 137Cs depuration mechanism in some demersal fish.

Changes in radioactive cesium concentrations from 2011 to 2017 in Fukushima coastal sediments and relative contributions of radioactive cesium-bearing microparticles.

Sedimentary cesium-137 concentrations around the Fukushima Daiichi Nuclear Power Plant (FDNPP) were measured from 2011 to 2017 at eight stations. Although high values were observed until 2013, decreasing trends were observed at the surface sediments of seven stations. We isolated 25 radioactive Cs-bearing microparticles (CsMPs; 1.0-5385 Bq per particle). The contribution ratio of CsMPs to each sample ranged from 4.1% to 99.5% (median 58.8%), with the contribution ratio of the CsMPs in the southern part of the FDNPP was low compared to that from the northern part. In the southern part of the FDNPP, small CsMPs that could not be isolated in this study were present in large quantities immediately after the accident, and gradually diffused away and/or were dissolved over time. In contrast, the CsMPs in the northern part of the FDNPP have most likely accumulated over time, as suggested by the silty nature of the sediments there.

Spatial variation in sedimentary radioactive cesium concentrations in Tokyo Bay following the Fukushima Daiichi Nuclear Power Plant accident.

Cesium-137 concentrations in sediment (137Cs) at Tokyo Bay were measured at 26 stations during 2017. Average 137Cs concentrations at the Arakawa river mouth (117 ±â€¯46 Bq kg-1) were approximately six times higher than those of the other stations in the bay (20 ±â€¯16 Bq kg-1). There were radiocesium-bearing microparticles in the bay sediment as well as in suspended matter of Fukushima coastal waters. Radioactivity of radiocesium-bearing microparticles was estimated to be 0.12 Bq. However, the contributions of radiocesium-bearing microparticles to each 137Cs concentration of the bulk sample were low; 3% was the maximum. The 137Cs inventory in sediment at the entire bay was 0.67 TBq, showing that a large amount of 137Cs was supplied to the bay from the river following the Fukushima Daiichi Nuclear Power Plant accident. Approximately 9.2% of the 137Cs which was fallout in the drainage basin has already flowed into the bay from the watershed, which is approximately 3.2 times higher than that of a previous estimate.

Examination of the Catabolic Rates of 13C-Labeled Fatty Acids Bound to the α and ß Positions of Triacylglycerol Using 13CO2 Expired from Mice.

Fatty acids in triacylglycerol (TAG) are catabolized after digestion. However, the catabolic rates of several fatty acids bound to the α (sn-1, 3) or ß (sn-2) position of TAG have not been thoroughly compared. In this study, the catabolic rates of 13C-labeled palmitic acid, oleic acid, linoleic acid, α-linolenic acid, eicosapentaenoic acid (EPA), or docosahexaenoic acid (DHA) bound to the α and ß position of TAG were compared using isotope ratio mass spectrometry. The catabolic rates of the studied fatty acids were evaluated using the ratio of 13C and 12C in carbon dioxide expired from mice. The results indicated that palmitic acid, oleic acid, or α-linolenic acid bound to the ß position was slowly catabolized for a long duration compared to that when bound to the α position. In contrast, EPA bound to the ß position was quickly catabolized, and EPA bound to the α position was slowly catabolized for a long time. For linoleic acid or DHA, no difference in the catabolic rates was detected between the binding positions in TAG. Furthermore, EPA and DHA were less catabolized than the other fatty acids. These results indicate that the catabolic rates of fatty acids are influenced by their binding positions in TAG and that this influence on the catabolic rate differed depending on the fatty acid species.

Mechanisms of radiocesium depuration in Sebastes cheni derived by simulation analysis of measured 137Cs concentrations off southern Fukushima 2014-2016.

The cesium depuration mechanisms were studied in Japanese rockfish Sebastes cheni off Fukushima, in which the radiocesium level remains higher than in other teleost. Samples were collected approximately 5 km south from the nuclear power plant during 2014-2016, and the 137Cs concentrations in fish, stomach content and prey species were measured. The stable cesium content in fish was also analyzed and compared with fish age which was determined by annual ring analysis in otoliths. The 137Cs concentrations in the dominant prey species, mysids and brown shrimp, were several Bq kg-w.w.-1; indicating that transfer via the food chain was substantial compared to that from seawater during the study period. The 137Cs concentrations in S. cheni decreased from 2014 to 2016 due to the metabolic excretion and the rate of decrease in its diet. Biokinetic model analyses confirmed the slower turnover of stable cesium in S. cheni, represented as a biological half-life (Tb1/2) of 140-215 d, and was associated with stable Cs levels in food of 5-7 ng g-w.w.-1. The 137Cs levels in S. cheni were also simulated, which showed that the 137Cs depuration in fish exposed to the initial contaminated plume in 2011 resulted from slower metabolic excretion, while the 137Cs levels in fish born after 2012 could be regarded as equilibrated with the environmental levels of 137Cs. Furthermore, the simulation results suggest that 137Cs depuration in S. cheni population was also caused by the alternation of generation, which can be substantial by the addition of new year class population hatched after 2012 that were not contaminated by the initial contaminated plume from the 2011 accident.

Effect of Calcium Treatment on Catabolic Rates of 13C-Labeled Fatty Acids Bound to the α and ß Positions of Triacylglycerol.

The absorption efficacies and catabolic rates of fatty acids are affected by their binding position on triacylglycerol (TAG). However, the kind of effect calcium treatment has on the catabolism of fatty acids is unclear. In this study, the catabolic rates of 13C-labeled palmitic acid, oleic acid, and linoleic acid bound to sn-1, 3 (α) and sn-2 (ß) position of TAG in the presence of calcium were compared using isotope ratio mass spectrometry. The catabolic rates of 13C-labeled fatty acids were evaluated using the ratio of 13C to 12C in the carbon dioxide expired by mice. The catabolic rate of palmitic acid bound to the α position was significantly lower than that of palmitic acid bound to the ß position of TAG. The rates of 13CO2 formation from palmitic acid at the ß position remained higher for a long time. In contrast, oleic and linoleic acids at the α position were as well catabolized as those at the ß position. These results indicate that in the presence of calcium, the saturated fatty acid bound to the ß position is highly catabolized, whereas that bound to the α position is not well catabolized. Saturated fatty acid at the α position is hydrolyzed by pancreatic lipase to promptly form insoluble complexes with calcium, which are excreted from the body, and thereby reducing the catabolic rate of these fatty acids.

Observation of Dispersion in the Japanese Coastal Area of Released 90Sr, 134Cs, and 137Cs from the Fukushima Daiichi Nuclear Power Plant to the Sea in 2013.

The March 2011 earthquake and tsunami resulted in significant damage to the Fukushima Daiichi Nuclear Power Plant (FDNPP) and the subsequent release of radionuclides into the ocean. Here, we investigated the spatial distribution of strontium-90 (90Sr) and cesium-134/cesium-137 (134, 137Cs) in surface seawater of the coastal region near the FDNPP. In the coastal region, 90Sr activity was high, from 0.89 to 29.13 mBq L-1, with detectable FDNPP site-derived 134Cs. This indicated that release of 90Sr from the power plant was ongoing even in May 2013, as was that of 134Cs and 137Cs. 90Sr activities measured at open ocean sites corresponded to background derived from atmospheric nuclear weapons testing fallout. The FDNPP site-derived 90Sr/137Cs activity ratios in seawater were much higher than those in the direct discharge event in March 2011, in river input, and in seabed sediment; those ratios showed large variability, ranging from 0.16 to 0.64 despite a short sampling period. This FDNPP site-derived 90Sr/137Cs activity ratio suggests that these radionuclides were mainly derived from stagnant water in the reactor and turbine buildings of the FDNPP, while a different source with a low 90Sr/137Cs ratio could contribute to and produce the temporal variability of the 90Sr/137Cs ratio in coastal water. We estimated the release rate of 90Sr from the power plant as 9.6 ± 6.1 GBq day-1 in May 2013 on the basis of the relationship between 90Sr and 137Cs activity (90Sr/137Cs = 0.66 ± 0.05) and 137Cs release rate.

Biogeochemical controls of surface ocean phosphate.

Surface ocean phosphate is commonly below the standard analytical detection limits, leading to an incomplete picture of the global variation and biogeochemical role of phosphate. A global compilation of phosphate measured using high-sensitivity methods revealed several previously unrecognized low-phosphate areas and clear regional differences. Both observational climatologies and Earth system models (ESMs) systematically overestimated surface phosphate. Furthermore, ESMs misrepresented the relationships between phosphate, phytoplankton biomass, and primary productivity. Atmospheric iron input and nitrogen fixation are known important controls on surface phosphate, but model simulations showed that differences in the iron-to-macronutrient ratio in the vertical nutrient supply and surface lateral transport are additional drivers of phosphate concentrations. Our study demonstrates the importance of accurately quantifying nutrients for understanding the regulation of ocean ecosystems and biogeochemistry now and under future climate conditions.

Radioactive cesium concentrations in coastal suspended matter after the Fukushima nuclear accident.

Radioactive cesium concentrations in the suspended matter of the coastal waters around the Fukushima Daiichi Nuclear Power Plant (FDNPP) were investigated between January 2014 and August 2015. The concentrations of radioactive cesium in the suspended matter were two orders higher in magnitude than those determined in the sediment. In addition, we discovered highly radioactive Cs particles in the suspended matter using autoradiography. The geometrical average radioactivity of particles was estimated to be 0.6 Bq at maximum and 0.2 Bq on average. The contribution ratio of highly radioactive Cs particles to each sample ranged from 13 to 54%, and was 36% on average. A major part of the radioactive Cs concentration in the suspended matter around the FDNPP was strongly influenced by the highly radioactive particles. The subsequent resuspension of highly radioactive Cs particles has been suggested as a possible reason for the delay in radioactive Cs depuration from benthic biota.

Seasonal variations and sources of sedimentary organic carbon in Tokyo Bay.

Total organic carbon (TOC), total nitrogen (TN) contents, their stable C and N isotope ratio (δ13C and δ15N), and chlorophyll a ([Chl a]sed) of surface sediments were investigated monthly to identify the seasonal variations and sources of organic matter in Tokyo Bay. The sedimentary TOC (TOCsed) and TN (TNsed) contents, and the sedimentary δ13C and δ15N (δ13Csed and δ15Nsed) values were higher in summer than other seasons. The seasonal variations were controlled by high primary production in the water column and hypoxic water in the bottom water during summer. The fraction of terrestrial and marine derived organic matter was estimated by Bayesian mixing model using stable isotope data and TOC/TN ratio. Surface sediments in Tokyo Bay are dominated by marine derived organic matter, which accounts for about 69±5% of TOCsed.

A significant net sink for CO2 in Tokyo Bay.

Most estuaries and inland waters are significant source for atmospheric CO2 because of input of terrestrial inorganic carbon and mineralization of terrestrially supplied organic carbon. In contrast to most coastal waters, some estuaries with small freshwater discharge are weak source or sometimes sink for CO2. Extensive surveys of pCO2 in Tokyo Bay showed that the overall bay acts as a strong net sink for atmospheric CO2. Although small area was a consistent source for CO2, active photosynthesis driven by nutrient loading from the land overwhelmed the CO2 budget in the bay. Here we show a comprehensive scheme with a border where air-sea CO2 flux was ±0 between nearshore waters emitting CO2 and offshore waters absorbing CO2. The border in Tokyo Bay was extremely shifted toward the land-side. The shift is characteristic of highly urbanized coastal waters with an extensive sewage treatment system in the catchment area. Because highly urbanized coastal areas worldwide are expected to quadruple by 2050, coastal waters such as Tokyo Bay are expected to increase as well. Through extrapolation of Tokyo Bay data, CO2 emission from global estuaries would be expected to decrease roughly from the current 0.074 PgC year-1 to 0.014 PgC year-1 in 2050.

Biokinetics of radiocesium depuration in marine fish inhabiting the vicinity of the Fukushima Dai-ichi Nuclear Power Plant.

Radiocesium (134Cs and 137Cs) released from the Fukushima Dai-ichi Nuclear Power Plant (1FNPP) accident contaminated the fish inhabiting the port of 1FNPP. Radiocesium concentrations in some fishes, especially rockfish, have still remained at elevated levels, while concentrations in olive flounder have decreased in 2015 to the level which is close to the Japanese regulatory limit for seafood products (0.1 kBq kg-wet-1). In this study a dynamic food chain transfer model was applied to reconstruct radiocesium levels in olive flounder residing around the port area. As a result, the observed 137Cs concentrations in olive flounder collected from the port could be explained by the simulated values in the fish, using the seawater level records at the port entrance. The reconstructed maximum 134+137Cs concentration in olive flounder inhabiting the port area was 72 kB kg-wet-1 in July 2011 and the ecological half-life (EHL) was estimated as being 180 days during the period of 2014-2015. Short term simulation which assumed that the coastal water fish swam into the port during 1 month, demonstrated that the radiocesium level in the olive flounder may become equivalent to the depurated level in the fish which were initially contaminated. This result indicated that the increase of radiocesium levels in wandering fish is unlikely to change total radiocesium concentrations in the olive flounder. In this sense, the radiocesium levels in the olive flounder of the port area can be interpreted as being convergent in 2015, regardless of the differences in their contamination histories. On the other hand, the higher 137Cs concentrations in fat greenling, compared to the olive flounder, can be attributed to a history of exposure to the contaminated seawater and food at the inner area of the port, such as the shallow draft quay and seawall area. As a result of the reconstructed initial higher radiocesium concentration, constrained by exposure history at the inner area of the port, the depurated radiocesium concentration in fat greenling is still likely to be greater than the regulatory level in the port area in 2015.

Dietary Starfish Oil Prevents Hepatic Steatosis and Hyperlipidemia in C57BL/6N Mice Fed High-fat Diet.

Starfish oil (SO) is characterized by functional lipids, including n-3 polyunsaturated fatty acid (both in the form of triacylglycerol and in the form of phospholipid), and carotenoids, which may exert beneficial effects on metabolic disorders in obesity-associated diseases. In the present study, the effect of SO on dysregulation of lipid metabolism was examined using C57BL/6N mice treated with high-fat (HF) diet. Mice were fed HF, HF with 2% SO, or HF with 5% SO diet for 8 weeks. Weight gain, blood glucose, serum and hepatic lipid contents, and hepatic fatty acid composition were measured. Fatty acid ß-oxidation activity was monitored by measuring the catabolic rate of 13C-labeled fatty acid, assessed as 13CO2/12CO2 ratio using isotope ratio mass spectrometry (IR-MS). Although there were no differences in body weight or white adipose tissue weight among the test groups, dietary SO reduced blood glucose, and dose-dependently improved hyperlipidemia and decreased hepatic lipid accumulation. Analysis of hepatic fatty acid composition revealed a significant decrease in the ratio of monounsaturated fatty acid to saturated fatty acid, which is attributed to stearoyl-CoA desaturase activity. IR-MS analysis suggested that ß-oxidation activity was enhanced in the mice treated with 5% SO. These results demonstrate that dietary SO improves lipid metabolism measures in HF diet-induced obese mice, suggesting that SO holds promise as an agent for the prevention and treatment of lipid metabolism disorders in the liver.

Comparison of Catabolic Rates of sn-1, sn-2, and sn-3 Fatty Acids in Triacylglycerols Using 13CO2 Breath Test in Mice.

Fatty acids in triacylglycerols (TAGs) are catabolized after digestion. However, the catabolic rates of the fatty acids at the sn-1, sn-2, and sn-3 positions of TAGs have not been compared. To elucidate the differences, we studied the catabolic rates of 13C-labeled palmitic acid, oleic acid, and capric acid at the sn-1, sn-2, or sn-3 position of TAGs using isotope-ratio mass spectrometry. Specifically, we measured the 13C-to-12C ratio in CO2 (Δ13C (‰)) exhaled by mice. For all analyzed fatty acids, we observed significant differences between sn-2 and other binding positions. In contrast, no significant difference was detected between the sn-1 and sn-3 positions. These results indicated that the catabolic rates of fatty acids are strongly influenced by their positions in TAGs.