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Microplastic (MP) pollution is a rising environmental concern. This study investigated MP concentrations in Tokyo Bay using neuston net for surface sampling and deep-sea plankton pump for underwater sampling across six stations at multiple depths. Results revealed substantial variation in MP concentrations. Surface large microplastics (LMP, > 350 µm) ranged from 0.21 × 10-3 to 3.34 × 10-3 pieces L-1, averaging 1.26 × 10-3 pieces L-1, while surface small microplastics (SMP, 60 µm to 350 µm) were highest at head of the bay (11.5 ± 3.05 pieces L-1). SMP concentrations varied with depth and position, peaking at center of the bay (5.79 ± 1.63 pieces L-1 at 2 m). Additionally, the total amount of surface LMP was estimated at 10.3 m3 and SMP at 15.0 m3 in the Tokyo Bay. This study provides a comprehensive picture of the spatial and vertical distribution of MP in Tokyo Bay.

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To reduce microplastic (MP) discharge into the aquatic environment, it is necessary to properly identify its sources and amounts. Here, specific MP sources, i.e., personal care products (PCPs), fibers from clothes, and tire-wear particles (TWPs) were focused, and MP generations from these sources in the Tokyo Bay watershed, Japan, were estimated based on statistical data on production and reported emission factors of the MP sources and executing considering uncertainty on the data. Potential annual MP emission into Tokyo Bay was estimated to be 10.2 ± 1.6, 38 ± 22, and 1500-1800 tons for PCPs, fibers, and TWPs, respectively. Emissions into Tokyo Bay by assuming MP density and diameter was estimated. For fiber, the fraction to potential emission was estimated at 1.0-2.8 %. This study contributes to determining potential discharge pathways. This will assist in the application of appropriate measures to reduce MP discharge into water bodies.

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A sediment trap experiment was conducted at a depth of 750 m at the mouth of Tokyo Bay to clarify the quantity and transport process of particles from the bay to the open ocean. The high total mass flux (8.7 ± 4.5 g m-2 d-1) suggests that the particles not only originate in the surface layer right above the trap, but are also focused in Uraga Channel and discharged into the bay mouth. The organic carbon and nitrogen isotope ratios (δ13Corg, δ15N) of the trapped particles were like those of the surface sediment in the bay, that is, a mixture of particles in rivers and suspended particles in the surface layer of the bay. Compared with the results of the experiment conducted in 1995-2002, the average total mass flux was reduced by 70% and organic carbon content was reduced by 50%. The δ13Corg values of trapped particles were also lower than those observed in the previous experiment, indicating a lower contribution from surface-suspended particles with high δ13Corg values in the bay. These results could partly reflect a decrease of the concentration of the suspended particulate carbon in the bay by half over 20 years. Another factor contributing to the decrease of the flux at the bay mouth would be that the intrusion of Kuroshio coastal water into the bay, which pushes particles out to the bay mouth, has not occurred in recent years.

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We examine the historical changes of 236U/238U and 235U/238U in a sediment core collected in Tokyo Bay and elucidate the anthropogenic sources of uranium in the 1960s-2000s. Uranium-236 was detected in samples deposited in the 1960s-2000s, and the 236U/238U ratio of the sediment core shows peak values in the 1970s. The 235U/238U isotopic ratios in samples deposited in the early 1960s are almost identical to that of natural uranium, implying that the 236U might have originated from global fallout. A decrease in 235U/238U was observed in the late 1960s-2000s, suggesting that depleted uranium from nuclear fuel reprocessing increased the 236U/238U ratios in the sediment. The 236U/238U values in sediments from the 1980s-2000s were lower than those in the 1970s but considerably higher than those in the 1960s, suggesting that the main source of depleted uranium still remains around Tokyo Bay. Our results demonstrated that the depleted uranium released in the 1970s should be considered as an important end-member when using uranium isotopic ratios as environmental tracers in closed aquatic environments around industrial cities.

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Previous studies have shown an increase in otolith Mn caused by exposure to hypoxic water masses. The mechanism leading to the increases in otolith Mn is still unclear, but might possibly be due to the larger amount of available Mn left in the water column under hypoxia. Thus, this study aimed to examine the relationship between hypoxia, water Mn and otolith Mn through marbled flounder (Pseudopleuronectes yokohamae, Günther) captured from Tokyo Bay and reared under different water Mn at laboratory. Otoliths from the Bay showed a higher (Mn/Ca)otolith than outside, together with a seasonal trend of high (Mn/Ca)otolith at the start of translucent zones (which form in the summer), supporting the occurrence of summer hypoxia in Tokyo Bay. Nonetheless, juveniles reared under control (Mn 0.50 µmol l-1 ), middle (Mn 6.94 µmol l-1 ) and high (Mn 10.4 µmol l-1 ) treatments of water Mn concentrations showed a disproportional smaller increase in (Mn/Ca)otolith . Comparing the laboratory experiment with the field data, (Mn/Ca)water under hypoxia in Tokyo Bay could reach a low level similar to control treatment, yet (Mn/Ca)otolith of the Bay showed a higher value than the high treatment. These results revealed an elevated (Mn/Ca)otolith towards hypoxia, but also suggested that changes in water Mn might not be directly recorded by otolith Mn.

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We investigated mass loading and the spatial distribution of volatile methylsiloxanes (VMSs) including four cyclic VMSs (D3-D6; cVMSs, the number refers to the number of SiO bonds) and three linear VMSs (L3-L5; lVMSs) in Tokyo Bay, Japan, which is one of the most industrialized, urbanized, and populated areas in the world. Based on the VMS concentrations determined in eight main inflow rivers to the bay, the mass loading of VMSs via inflow rivers and sewage treatment plants located in Tokyo Bay was estimated at 2500 kg/y for total VMSs. Elevated mass loadings of VMSs were found in three of the rivers, inflowing to the inner west of Tokyo Bay. The distribution and deposition characteristics of VMSs were observed depending on the estuarine condition. Estuarine sediments were found to be efficient and effective traps for VMSs and the salting-out effect is one possible mechanism to explain this phenomenon. The overall profiles of D4, D5, and D6 in surface water and sediment were observed across Tokyo Bay; elevated concentrations were identified in the inner west bay with dispersed low concentrations in the outer bay, except for one hotspot of D4 in the sediment, indicating a major emission route of VMSs via inflow rivers. Additionally, the historical pollution profiles of VMSs in Tokyo Bay were reconstructed based on the VMS concentrations determined in a dated sediment core. VMSs were identified throughout the upper 40 cm of the sediment core (representing the mid 1980s); the profiles correspond with the historical use of VMSs in wash-off personal care-products. The noted decreasing trend of D4 might be a reflection of the early 2000s replacement of D4 with D5 in such products. The elevated VMS concentrations in the estuarine sediment raise concerns about the impact on the aquatic environment.

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Zostera marina (eelgrass) is a widespread seagrass species that forms diverse and productive habitats along coast lines throughout much of the northern hemisphere. The present study investigated the microbial consortia of Z. marina growing at Futtsu clam-digging beach, Chiba prefecture, Japan. The following environmental samples were collected: sediment, seawater, plant leaves, and the root-rhizome. Sediment and seawater samples were obtained from three sampling points: inside, outside, and at the marginal point of the eelgrass bed. The microbial composition of each sample was analyzed using 16S ribosomal gene amplicon sequencing. Microbial communities on the dead (withered) leaf surface markedly differed from those in sediment, but were similar to those in seawater. Eelgrass leaves and surrounding seawater were dominated by the bacterial taxa Rhodobacterales (Alphaproteobacteria), whereas Rhodobacterales were a minor group in eelgrass sediment. Additionally, we speculated that the order Sphingomonadales (Alphaproteobacteria) acts as a major degrader during the decomposition process and constantly degrades eelgrass leaves, which then spread into the surrounding seawater. Withered eelgrass leaves did not accumulate on the surface sediment because they were transported out of the eelgrass bed by wind and residual currents unique to the central part of Tokyo Bay.

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Microplastics (MPs) pollution surveys were conducted in Tokyo Bay using neuston nets (May 2019 and January 2020). Although the pollution level in Tokyo Bay was high (3.98 pcs/m3, May), it was lower than reported in other semi-closed bays because of differences in the Enclosed Index. It was found that polyethylene fragments dominated the retrieved MPs; the mode of MPs size was 800 µm. As MPs abundance in rivers had the same seasonality as found in the inner bay, rivers were considered the main source of MPs. The seawater residence time is shorter than the time required for the density of MPs to become greater than that of seawater; therefore, it was considered that MPs are transported out of the bay instead of sinking. MPs were aggregated into a convergence zone by residual currents (the thermohaline front) in May (January). These findings will improve understanding of MPs pollution in other bays.

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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.

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In this work, the distribution of quaternary ammonium compounds (QACs) in two dated sediment cores, collected from the Pearl River Estuary (PRE) and Tokyo Bay (TB), were investigated to understand the historical input of QACs and their diagenetic behavior in urban estuarine environments. The vertical variation profiles of QAC concentrations showed that benzylalkyldimethyl ammonium compounds (BACs) and dialkyldimethyl ammonium compounds (DADMACs) were widely used during 1970s and 1980s both in China and Japan. The declining environmental concentrations of QACs suggested a compositional change of commodities and the effectiveness of emission control strategies. For the individual QAC homologues, BAC homologues decreased significantly over time, while DADMAC compositions remained relatively stable. The differences in concentration and composition profiles of BACs and DADMACs in the sediment cores provided useful information on the patterns of use of QACs in China and Japan, as well as their diagenetic behaviors in the sediments.

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Ecological thresholds of dissolved oxygen (DO) and sedimentary hydrogen sulfide (H2S) for macrozoobenthos were examined during a 30-month monitoring of two stations in a highly eutrophic canal in inner Tokyo Bay, Japan. Bottom DO and H2S concentrations fluctuated seasonally, and were significantly correlated with water and sediment temperatures. Red tide-derived phytodetritus was a major source of sediment organic matters in the canal bottom, and the sediment became highly reduced and sulfidic condition in warmer months (sedimentary H2S; up to 8.5 mM). Dominant opportunistic taxa, including polychaetes and amphipods, were eliminated under low DO and high H2S conditions (i.e., population thresholds), and devastation of community structure occurred at 2.4-3.3 mg l-1 DO and 1.8-2.7 mM H2S (i.e., community thresholds). To maintain ecosystem function in anthropogenically degraded habitats and ensure colonization by macrozoobenthos throughout the year, DO and H2S levels should be maintained below these thresholds.

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Numerous algorithms have been proposed to retrieve chlorophyll-a concentrations in Case 2 waters; however, the retrieval accuracy is far from satisfactory. In this research, seven algorithms are assessed with different band combinations of multispectral and hyperspectral bands using linear (LN), quadratic polynomial (QP) and power (PW) regression approaches, resulting in altogether 43 algorithmic combinations. These algorithms are evaluated by using simulated and measured datasets to understand the strengths and limitations of these algorithms. Two simulated datasets comprising 500,000 reflectance spectra each, both based on wide ranges of inherent optical properties (IOPs), are generated for the calibration and validation stages. Results reveal that the regression approach (i.e., LN, QP, and PW) has more influence on the simulated dataset than on the measured one. The algorithms that incorporated linear regression provide the highest retrieval accuracy for the simulated dataset. Results from simulated datasets reveal that the 3-band (3b) algorithm that incorporate 665-nm and 680-nm bands and band tuning selection approach outperformed other algorithms with root mean square error (RMSE) of 15.87 mg·m-3, 16.25 mg·m-3, and 19.05 mg·m-3, respectively. The spatial distribution of the best performing algorithms, for various combinations of chlorophyll-a (Chla) and non-algal particles (NAP) concentrations, show that the 3b_tuning_QP and 3b_680_QP outperform other algorithms in terms of minimum RMSE frequency of 33.19% and 60.52%, respectively. However, the two algorithms failed to accurately retrieve Chla for many combinations of Chla and NAP, particularly for low Chla and NAP concentrations. In addition, the spatial distribution emphasizes that no single algorithm can provide outstanding accuracy for Chla retrieval and that multi-algorithms should be included to reduce the error. Comparing the results of the measured and simulated datasets reveal that the algorithms that incorporate the 665-nm band outperform other algorithms for measured dataset (RMSE = 36.84 mg·m-3), while algorithms that incorporate the band tuning approach provide the highest retrieval accuracy for the simulated dataset (RMSE = 25.05 mg·m-3).

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To examine the impacts of urbanization and industrialization on the coastal environment, and assess the effectiveness of control measures on the contamination by chlorinated paraffins (CPs) in East Asia, surface and core sediments were sampled from the urbanized coastal zones in China and Japan (i.e., Pearl River Delta (PRD), Hong Kong waters and Tokyo Bay) and analyzed for short-chain (SCCPs) and medium-chain CPs (MCCPs). Much higher concentrations of CPs were found in the industrialized PRD than in adjacent Hong Kong waters. Significant correlation between CP concentration and population density in the coastal district of Hong Kong was observed (r2 = 0.72 for SCCPs and 0.55 for MCCPs, p < 0.05), highlighting the effect of urbanization. By contrast, a relatively lower pollution level of CPs was detected in Tokyo Bay. More long-chain groups within SCCPs in the PRD than in Hong Kong waters and Tokyo Bay implied the effect of industrialization. Comparison of temporal trends between Hong Kong outer harbor with Tokyo Bay shows the striking difference in historical deposition of CPs under different regulatory situations in China and Japan. For the first time, the declining CP concentrations in Tokyo Bay, Japan, attest to the effectiveness of emissions controls.

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Surface waters including river water and effluent from sewage treatment plants (STPs) were collected from Tokyo Bay watershed, Japan, and analyzed for seven cyclic and linear volatile methylsiloxanes (VMSs), i.e., D3, D4, D5, D6, L3, L4, and L5 by an optimized purge and trap extraction method. The total concentrations of seven VMSs (ΣVMS) in river water ranged from <4.9 to 1700ng/L (mean: 220ng/L). The individual mean concentrations of cyclic VMSs in surface waters were; 10ng/L for D3, 13ng/L for D4, 180ng/L for D5, and 18ng/L for D6. The concentrations of ΣVMS determined in STP effluents varied widely from 99 to 2500ng/L and the individual mean concentrations were 21ng/L for D3, 27ng/L for D4, 540ng/L for D5, and 45ng/L for D6. D5, which is widely used in personal-care products, was found to be the most abundant compound in both river water and STP effluent. Linear VMSs were detected at much lower frequency and concentrations than those of cyclic VMSs. The measured concentrations of D4 were below the no-observed effect concentration (NOEC). The annual emission of ΣVMS through STPs into Tokyo Bay watershed was estimated at 2300kg. Our results indicate widespread distribution of VMSs in Tokyo Bay watershed and the influence of domestic wastewater discharges as a source of VMSs in the aquatic environment.

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We investigated factors that might have disturbed the stock recovery of marbled flounder in Tokyo Bay by focusing on the early life stages. Field surveys in Tokyo Bay from 2006 to 2011 revealed that mature adult biomass increased from 2006 to 2008 and decreased thereafter. Meanwhile, larval and juvenile densities were high in 2006 and 2008 but low in other years. Discrepancies in the yearly trends of these parameters suggest that mortality during life stages between spawning and early larval phases might have affected the abundance of the subsequent life stages. Monthly mean water temperature between January and February, in which hatching and pelagic larvae occur in the bay, was lower in 2006 (8.6 °C) and 2008 (9.6 °C) than was observed in other years (10.4-11.4 °C). Significant negative correlation between water temperature and larval density implies that mortality during pre- and post-larval stages would be higher in warmer winter years (>10 °C). To test this hypothesis, we examined the effects of water temperature on mortality and development in egg and larval stages under controlled laboratory conditions. Hatching rate was high in a water temperature range of 9.2-12.7 °C (66.6-82.5%), whereas it decreased in cooler (3.7% at 5.9 °C) or warmer (33.9% at 14.8 °C) conditions. Meanwhile, days from fertilization to hatching, size of larvae at hatching and survival rate of larvae after 18 d from hatching were monotonically and significantly decreased as water temperature was elevated. Combined evidence of the field and laboratory studies suggests that a warmer reproductive season (>10 °C) might induce mortalities of marbled flounder larvae in Tokyo Bay.

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Bioaccumulation and trophic transfer of cyclic volatile methylsiloxanes (cVMS), specifically octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5), and dodecamethylcyclohexasiloxane (D6), were evaluated in the pelagic marine food web of Tokyo Bay, Japan. Polychlorinated biphenyl (PCB) congeners that are "legacy" chemicals known to bioaccumulate in aquatic organisms and biomagnify across aquatic food webs were used as a benchmark chemical (CB-180) to calibrate the sampled food web and as a reference chemical (CB-153) to validate the results. Trophic magnification factors (TMFs) were calculated from slopes of ordinary least-squares (OLS) regression models and slopes of bootstrap regression models, which were used as robust alternatives to the OLS models. Various regression models were developed that incorporated benchmarking to control bias associated with experimental design, food web dynamics, and trophic level structure. There was no evidence from any of the regression models to suggest biomagnification of cVMS in Tokyo Bay. Rather, the regression models indicated that trophic dilution of cVMS, not trophic magnification, occurred across the sampled food web. Comparison of results for Tokyo Bay to results from other studies indicated that bioaccumulation of cVMS was not related to type of food web (pelagic vs demersal), environment (marine vs freshwater), species composition, or location. Rather, results suggested that differences between study areas was likely related to food web dynamics and variable conditions of exposure resulting from non-uniform patterns of organism movement across spatial concentration gradients.

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In this study, we developed an approach for sequential nontarget and target screening for the rapid and efficient analysis of multiple samples as an environmental monitoring using a comprehensive two-dimensional gas chromatograph coupled to a high resolution time-of-flight mass spectrometer (GC × GC-HRTOFMS). A key feature of the approach was the construction of an accurate mass spectral database learned from the sample via nontarget screening. To enhance the detection power in the nontarget screening, a global spectral deconvolution procedure based on non-negative matrix factorization was applied. The approach was applied to the monitoring of rivers in the Tokyo Bay basin. The majority of the compounds detected by the nontarget screening were alkyl chain-based compounds (55%). In the quantitative target screening based on the output from the nontarget screening, particularly high levels of organophosphorus flame retardants (median concentrations of 31, 116 and 141 ng l(-1) for TDCPP, TCIPP and TBEP, respectively) were observed among the target compounds. Flame retardants used for household furniture and building materials were detected in river basins where buildings and arterial traffic were dominated. The developed GC × GC-HRTOFMS approach was efficient and effective for environmental monitoring and provided valuable new information on various aspects of monitoring in the context of environmental management.

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Concentrations of eight bisphenol analogues (BPs) including BPA, BPS, and BPF were determined in surface waters collected from select rivers in Japan, Korea, China, and India. BPA was found at a concentration in the range of several tens to several hundreds of nanograms per liter in most of the rivers surveyed and some of the highest concentrations (54-1950 ng/L) were found in rivers in Chennai, India. Concentrations of BPF were one to two orders of magnitude higher than those of BPA in river and sea waters collected from Japan, Korea and China, which suggested that BPF is a major contaminant in surface waters in several Southeast Asian countries. BPF concentrations as high as 2850 ng/L were found in the Tamagawa River in Japan. The flux of BPs through riverine discharges into Tokyo Bay was calculated to be approximately 5.5 t per year. Based on the flux estimates and the mass of BPF found in water column and sediment in Tokyo Bay, it was found that BPF degrades faster than BPA in the environment. Elevated concentrations of BPF found in surface waters suggest the need for further studies to determine the fate and toxicity of this compound.

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We investigated effects of severe hypoxia (dissolved oxygen <1 ml l(-1)) on recruitment of mantis shrimp Oratosquilla oratoria in Tokyo Bay. Ten-year field surveys were conducted to examine quantitative relationships in annual mean densities of larvae and juveniles, and spatial distribution of juveniles and severe hypoxia. There was no significant correlation between annual mean densities of larvae and juveniles, suggesting that mortality during larval or juvenile stages varies among years, which might have regulated abundance of young-of-the-year juveniles. Juvenile density was low in the severely hypoxic area, implying that hypoxia could affect survivals and spatial distribution of juveniles. Meanwhile, there are yearly fluctuations in juvenile density in normoxic areas of both northern and southern part of the bay. This evidence suggests that abundance of post-settled juveniles might have been determined by not only effects of hypoxia, but also other factors influencing mortality during the early life stages.

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Data processing tools for non-target analysis using comprehensive two-dimensional gas chromatography coupled with high-resolution time-of-flight mass spectrometry (GC×GC-HRTOFMS) were developed and applied to a sediment core in Tokyo Bay, focusing on chlorinated compounds in this study. The processing tools were classified in two different methods: (1) the consecutive use of mass defect filter followed by artificial neutral loss scan (MDF/artificial NLS) as a qualitative non-target screening method and (2) Entire Domain Combined Spectra Extraction and Integration Program (ComSpec) and two-dimensional peak sentinel (T-SEN) as a semi-quantitative target screening method. MDF/artificial NLS as a non-target screening approach revealed that PCBs, followed by octachlorodibenzo dioxin (OCDD), were the main chlorinated compounds present in all sediment layers. Furthermore, unknown peaks thought to be chlorinated compounds were found in increasing numbers, some in increasing amounts. T-SEN and ComSpec as a target screening approach were adapted for automatic semi-quantitative analysis showed that, in decreasing concentration order, PCBs, OCDD, and dichlorodiphenyltrichloroethane and its metabolites (DDEs, DDDs) were the main chlorinated pollutants in the sediments. The complementary use of both techniques allows us to extract significant chlorinated pollutants, including non-targeted compounds. This retrospective analysis by this approach performed well even on matrix-rich sediment samples and provided us an interesting insight of historical trends of pollution in Tokyo Bay.

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