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Benzotriazole-type ultraviolet stabilizers (BUVSs) are emerging contaminants whose exposure to wildlife is of concern. In this study, we investigated the contamination status of BUVSs in green turtles (Chelonia mydas) breeding at Ogasawara Islands, Japan, through chemical analysis of 10 BUVSs and 26 congeners of polychlorinated biphenyls (PCBs) in adipose tissue (n = 21) and blood plasma (n = 9). BUVSs were detected significant levels in adipose tissue (19 of 21 turtles), and UV-327 (not detected - 14.8 ng/g-lipid, detection frequency: 76 %), UV-326 (not detected - 24.1 ng/g-lipid, 29 %), and UV-328 (not detected - 5.8 ng/g-lipid, 24 %) were frequently detected. Turtles exhibiting sporadically high concentrations of BUVSs (>10 ng/g-lipid) did not necessarily correspond to individuals with high total PCB concentrations (1.03-70.2 ng/g-lipid). The sporadic occurrence pattern of BUVSs suggested that these contaminants in sea turtles cannot be explained solely by diet but are likely derived from plastic debris., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Polychlorinated biphenyls (PCBs) are synthetic organic contaminants that are widespread in the environment. There are 209 PCB congeners. Fish oil produced from marine fish is widely used as a health supplement. PCB contamination of fish oil is of concern. We determined the concentrations of all 209 PCB congeners in commercially available fish oil supplements from Japan and estimated PCB intakes for humans consuming the supplements. We determined the concentrations of non-dioxin-like PCBs separately. The total PCB concentrations in 37 fish oil supplements purchased in Japan were 0.024-19 ng/g whole weight, and the non-dioxin-like PCB concentration range was also 0.024-19 ng/g whole weight. The total PCB intakes calculated for a 50 kg human consuming the supplements were 0.039-51 ng/day (0.00078-1.0 ng/(kg body weight per day)) and the non-dioxin-like PCB intake range was also 0.039-51 ng/day (0.00078-1.0 ng/(kg body weight per day)). The total PCB intakes were much lower than the tolerable daily intake of 20 ng/(kg body weight per day) recommended by the WHO. The results indicated that PCBs in the fish oil supplements pose acceptable risks to humans consuming the fish oil supplements daily., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Author(s). Published by Elsevier Inc. All rights reserved.)

Studies have shown that halogenated polycyclic aromatic hydrocarbons (HPAHs), including chlorinated (ClPAHs) and brominated PAHs (BrPAHs), could be hazardous pollutants due to their pervasive occurrence in the environment. However, their accumulation properties and toxic potentials in animal feedstuffs remain unclear. This study investigated 75 congeners of parent PAHs, ClPAHs, and BrPAHs in animal-based feed ingredients and fish and swine feeds in Japan using a GC/Orbitrap MS system. The total parent PAHs ranged from below the method detection limit (

NPPs (Non-phthalate plasticizers) are used as alternative plasticizers to phthalate esters, but there is limited knowledge on environmental residues, and they have not been reported in Japan. A method to analyze NPPs in seawater using solid-phase extraction was developed, and the residual burden of Diisobutyl adipate (DIBA), Acetyl tributyl citrate (ATBC), Di-(2-ethylhexyl) adipate (DEHA), Di-(2-ethylhexyl) sebacate (DEHS) and Trioctyl trimellitate (TOTM) in seawater and sediment from the Osaka Bay was measured. Using an Oasis Max column and acetone as the eluting solvent, the recovery of the target substances in seawater is >68 %. In Osaka Bay, no NPPs were detected in seawater. On the other hand, ATBC and TOTM were detected in the sediment at 36-69 ng/g and 47-131 ng/g, respectively, from about half of the 14 sites, while DEHA and DEHS were detected at 83 ng/g and 181 ng/g, respectively, from only one site., Competing Interests: Declaration of competing interest The authors declare they have no known competing financial interests or personal relationships that could have appeared to influence the research work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Marine debris comprising single-use plastic products (SUPs) is ubiquitous in Asian coastal waters, but there is little information on the types of polymers and the concentrations of plastic additives such waste products contain. In this study, 413 SUPs randomly collected from 4 Asian countries between 2020 and 2021 were analyzed to obtain specific polymer and organic additive profiles. Polyethylene (PE), coupled with external polymers, was prominent in the inside of the SUPs, whereas polypropylene (PP) and polyethylene terephthalate (PET) were prevalent in both the insides and outsides of the SUPs. The use of different polymers in the insides and outsides of PE SUPs implies specific and complicated recycling systems are required to maintain the purity of the products. Phthalate plasticizers including dimethyl phthalate (DMP), diethyl phthalate (DEP), diisobutyl phthalate (DiBP), dibutyl phthalate (DBP), and di(2-ethylhexyl) phthalate (DEHP), and the antioxidant butylated hydroxytoluene (BHT) were prevalent in the SUPs (n = 68). High concentrations of DEHP were detected in PE bags from Myanmar (820,000 ng/g) and Indonesia (420,000 ng/g), which were an order of magnitude greater than the concentrations in PE bags collected in Japan. SUPs containing high concentrations of organic additives may be the primary source of harmful chemicals in the environment, and should be responsible for their ubiquitous distribution in ecosystems., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

We investigated the spatial distribution, mass profiles, and benthic risk assessment of a wide range of methylsiloxanes (MSs), including 7 cyclic MSs (CMSs; D3-D9; the number refers to the number of SiO bonds), 13 linear MSs (LMSs; L3-L15), and 15 modified and other MSs (MMSs) in sediments from the Tokyo Bay catchment basin, Japan. We observed widespread distribution of MSs (ΣCMS, ΣLMS, and ΣMMS) in the sediment samples, with concentrations of 1.0-6180 ng/g dry weight (dw), 1.8-10,100 ng/g dw, and < 0.31-210 ng/g dw, respectively. Our study is the first to measure various MMSs modified with hydrogen, vinyl, or phenyl groups; however, only methyltris(trimethylsiloxy)silane and phenyltris(trimethylsiloxy)silane were detected with high occurrence frequency. Notably, no elevated concentrations of MSs were observed downstream of silicone manufacturers, whereas the sediment was characterized by a specific D4/D5 ratio. With the Si-based mass profiles in extractable organosilicon (EOSi), the measured CMSs, LMSs, and MMSs accounted for 5.4%, 7.8%, and 0.2%, respectively. Unidentified EOSi (unknown fraction) constituted a major proportion of the EOSi in the sediment, with a mean of 87%, suggesting that the organosilicon environmental emissions were more than the measured MSs. In risk assessment of the adverse effects of D4, D5, and D6 in sediment on benthic organisms, the respective distributions indicated no overlap between the 95th percentile field sediment concentration and the 5th percentile chronic sediment no-effect concentration in organic carbon-normalized concentration. Although the hazard quotient compared with the predicted no-effect concentration for D5 and D6 exceeded the threshold level (hazard quotient ≥1), the results of probabilistic risk assessment for the three CMSs were not high enough to indicate a threat to benthic organisms in the study area., Competing Interests: Declaration of competing interest The authors declare no conflict of interest, financial or otherwise., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)

Background: Exposure to several metallic elements has been suggested as a risk factor for gestational diabetes mellitus (GDM), but inconsistent findings have been reported. This study aimed to examine the association between the maternal whole blood concentration of metallic elements (Hg, Pb, Cd, Mn, and Se) and GDM using the dataset of the Japan Environment and Children's Study (JECS), a nationwide birth cohort study, which was designed to examine the adverse effects of pre/post-natal exposure to hazardous environment., Methods: The data of 78,964 pregnant women who were participants of JECS were used. Blood samples were collected from the pregnant women at second/third trimester of gestation. We employed logistic regression analysis, quantile g-computation (QGC) and a distributed lag nonlinear model (DLNM) to examine the association between the blood concentration of metallic elements and the risk of GDM., Results: The prevalence of GDM was 2.1%. In the logistic regression analyses, maternal blood Hg was associated with an increased risk of GDM. In QGC analysis, although metallic elements mixtures were not related to an increased risk of GDM, Hg (52.6%) may be the main contributor. According to the results of DLNM, for maternal exposure to Hg, 4.99 ng/g was identified as its susceptible minimum window for elevated risk of GDM., Conclusions: Our findings highlighted an association between Hg exposure and an increased risk of GDM. Studies of the underlying mechanisms and potential contributing factors, including fish intake, of this association are warranted., (Copyright © 2022 The Authors. Published by Elsevier Inc. All rights reserved.)

A decline in the proportion of male births (secondary sex ratio, SSR) has been seen in several countries including Japan in recent years. Although previous studies have reported that the SSR is affected by exposure to chemical substances such as dioxins and polychlorinated biphenyls, as well as heavy metals such as methylmercury, the effects of lead exposure on the SSR have been little studied. The aim of this study was to determine the association between maternal lead exposure and SSR. In a large-scale nationwide birth cohort study, maternal blood lead level (BLL) was determined using whole blood from the second or third trimester of pregnancy. The association between SSR and maternal BLL was estimated using multivariable logistic models. Binomial distribution was applied to examine the differences in SSR by dividing the participants into five groups based on BLL. The primary outcome was SSR, and the child sex was obtained from the medical record transcripts. Of 104,062 fetal records, 85,171 were examined for analysis. The median maternal BLL was 5.85 ng/g (5th-95th percentile 3.45-10.6 ng/g). The overall proportion of males among participating infants was 0.512. In logistic regression models adjusted for covariates, the analysis revealed an increased odds ratio for SSR with higher blood lead concentrations [Group 2: adjusted OR 1.082, 95% confidence interval 1.037 to 1.129, Group 3: 1.122, 1.074 to 1.171, Group 4: 1.214, 1.163 to 1.268, Group 5: 1.279, 1.224 to 1.336]. Compared to the general birth probability in Japan, the group with low BLL had a lower SSR and the group with high BLL had a higher SSR. Higher maternal lead exposures during pregnancy were associated with increased SSR. Further investigations including assessment of paternal lead exposure are necessary to understand the association between lead exposure and SSR., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021. Published by Elsevier B.V.)

Few studies have investigated the prevalence of polybrominated diphenyl ethers (PBDEs) in deep-sea sharks. In this study, the levels and profiles of PBDEs were determined in liver samples of eight different species of deep-sea sharks collected in Suruga Bay, Japan. Widespread contamination of PBDEs in the deep-sea environment was reconfirmed in this study as these persistent organic pollutants (POPs) were detected in all specimens analyzed. Mean ΣPBDE levels in the deep-sea sharks ranged from 7 to 517 ng/g of lipid weight. The distribution patterns of BDE homologues were similar in all species where tetra-BDEs provided the dominant contribution to total PBDEs (46%). PBDEs levels were similar to, or higher than, those seen in other deep-sea sharks from different regions. The levels of PBDEs were likely to reflect their feeding preferences as higher PBDE levels were seen in species with higher trophic positions., (Copyright © 2022. Published by Elsevier Ltd.)

The widespread occurrence of persistent organic pollutants (POPs) in the environment is a matter of concern. In this study, selected organohalogenated contaminants, including dichlorodiphenyltrichloroethane and its metabolites (DDTs) polychlorinated biphenyls (PCBs), chlordanes (CHLs), hexachlorobenzene (HCB), polybrominated diphenyl ethers (PBDEs), hexabromocyclododecanes (HBCDs), tetrabromobisphenol A (TBBPA), 2,4,6-tribromophenol (TBP), were measured in complete meal sets (24-h duplicate-diet) of Japanese infants to investigate the levels, profiles, and possible sources of contamination. In total, 46 whole-day meals of infants (7-24-months old) were collected during 2017 from Fukuoka, Japan. To the best of our knowledge, this is the first report based on the duplicate-diet method for infants. The median intakes among the POP groups were highest for ΣDDTs (18 ng/day, maximum 251 ng/day), followed by ΣPCBs (17 ng/day, maximum 198 ng/day), ΣCHLs (14 ng/day, maximum 105 ng/day), HCB (11 ng/day, maximum 64 ng/day), TBP (3.5 ng/day, maximum 109 ng/day), ΣHBCDs (1.9 ng/day, maximum 70 ng/day), TBBPA (0.72 ng/day, maximum 34 ng/day), and ΣPBDEs (0.11 ng/day, maximum 4.5 ng/day). Among the PCBs, PCB-138 and PCB-153 were the most abundant congeners (27% and 23%, respectively). p,p'-DDE, the major DDT metabolite, accounted for 96% of total DDTs. Among PBDEs, BDE47 was the only detected congener (present in 4% of the samples). The dietary intake of the targeted compounds was lower than the intake via breast milk, suggesting that the exposure from baby food was limited. In the principal component analysis, chlorinated and brominated compounds were separated on principal component 1, while TBP and α-HBCD were separated on principal component 2, likely suggesting a differing emission time trend or source. PCB-153, PCB-138, trans-chlordane, cis-chlordane, and trans-nonachlor were correlated with seafood consumption (Spearman's ρ = 0.45 to 0.57, p < 0.05), while TBP was correlated with seaweed consumption (Spearman's ρ = 0.46, p < 0.05). Also, four species of commercial edible seaweed in Japan were analyzed to confirm the findings of the duplicate-diet study. The relatively high concentration of TBP (5.5 ± 6.6 ng/g wet weight) was observed in the seaweed samples, indicating that seaweed is a potential exposure source of TBP., (Copyright © 2021 Elsevier Inc. All rights reserved.)

The purpose of this study was to elucidate the potential of using flounders as bioindicators of accumulation and transformation of POPs and to assess the possible environmental risk to the health of the population of the Russian coastal regions. The mean levels of HCH, DDT, and PCBs in the flounders were as follows: in the eastern Sea of Okhotsk, 49 ± 51, 62 ± 89, and 106 ± 83 ng/g lipid weight; in the southern Sea of Okhotsk, 36 ± 37, 15 ± 16, and 97 ± 41 ng/g lipid wt; in the Sea of Japan/East Sea, 62 ± 36, 39 ± 28, and 1616 ± 1177 ng/g lipid wt, respectively. In the Tatar Strait, OCPs were represented mainly by β-HCH with a concentration of 221 ± 182 ng/g lipid wt; the PCB level was 455 ± 317 ng/g lipid wt. Values of ILCR = 2.1·10 -5 due to the consumption of flounder from the Sea of Japan/East Sea at a rate of 29 kg/yr indicate a probability of developing cancer during a lifetime., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

PCBs and PBDEs in microplastics and zooplankton collected in surface water at 27 locations in the Pacific Ocean and around the coast of Japan were investigated. Both PCBs and PBDEs were observed in buoyant microplastics, even in smaller particles of 0.315-1 mm. Concentrations of Σ13 PCBs were 0.04-124 ng/g, and were higher in urban bay areas such as Tokyo Bay. Sporadic moderate to high concentrations of PBDEs were observed in both urban-offshore and rural-offshore locations, consisting mostly of higher-brominated congeners. From the latter, BDE 209 ranged from not detected to 2158 ng/g. The microplastic-to-zooplankton abundance ratio threshold was 0.6 for PCBs and 0.08 for PBDEs, above which exposure would be greater from microplastics than from zooplankton., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

In the latter half of the 1950s, a large amount of methylmercury (MeHg) was discharged directly into Minamata Bay, Japan by a chemical factory, resulting in the contamination of the fish and shellfish. Ultimately, an outbreak of MeHg intoxication, called Minamata disease, occurred. From 1977 to 1988, the Kumamoto Prefectural Government dredged and transferred sediments exceeding 25 μg/g of total mercury (THg, dry basis) into a strictly segregated area of the bay near the wastewater outlet, then this area was landfilled. We conducted analyses of the mercury speciation in preserved Minamata Bay sludge samples (collected from inside of the bay prior to the termination of the remediation project; n=4) and recent Minamata Bay sediments (collected outside the dredging area of the bay; n=5) to evaluate the potential risk of the sludge/sediment leakage from the reclaimed land to the Minamata Bay. Median THg (dry basis) concentrations were 241 μg/g for the preserved sludge, 6.1 μg/g for the recent Minamata Bay sediments, and 0.18 μg/g for a single control sample; median MeHg concentrations (percentage of MeHg in THg) were 108 ng/g (0.031%), 3.7 ng/g (0.12%), and 0.71 ng/g (0.41%), respectively. In all the samples, the MeHg% decreased exponentially with increasing THg concentration. The extractability of THg from each sample into seawater was shown to be much lower than that of MeHg. The extracted MeHg was 0.86% for the preserved sludge, 4.57% for the recent Minamata Bay sediments, and 7.89% for the control. The predominant chemical form of mercury in the preserved sludge containing the highest THg concentration was found to be stable β-mercury sulfide (HgS) based on transmission electron microscopy linked with energy-dispersive X-ray spectroscopy (TEM-EDX) and X-ray absorption fine structure (XAFS) analyses., (Copyright © 2019 Elsevier Inc. All rights reserved.)

In 2014-2019, a total of 31 blubber samples were collected from spotted seals (Phoca largha) in the western Sea of Japan. The samples were analyzed by gas chromatography to determine level of organochlorine pesticides (OCPs). The concentration of hexachlorocyclohexane and its isomers (∑HCH) ranged from 389 to 50,070 ng/g lipid weght; the concentration of dichlorodiphenyltrichloroethane and its metabolites (∑DDT), ranged from 62,720 to 1,110,930 ng/g lipid wt. Transfer of HCH and DDT from mother to pup during pregnancy and lactation was documented. The OCP concentration in blubber of spotted seals from the western Sea of Japan is one to two orders of magnitude higher than in spotted seals inhabiting waters off the Japan coast. Organochlorines detected in the western Sea of Japan likely come from some countries of Southeast Asia still using OCPs in the agriculture sector., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Although persistent organic pollutants (POPs) are currently banned or strictly controlled under the Stockholm Convention on Persistent Organic Pollutants, POPs are still distributed worldwide due to their environmental persistence, atmospheric transport, and bioaccumulation. Herein we investigated the current concentrations of POPs in the sediments from Seto Inland Sea, Japan and sought to clarify the factors currently controlling the POPs concentration of the surface sediments from Seto Inland Sea. The concentrations of hexachlorocyclohexane isomers (HCHs), dichlorodiphenyltrichloroethane and its metabolites (DDTs), and chlordane isomers (CHLs) in sediments from Seto Inland Sea were <0.002-1.20 ng g -1 , 0.01-2.51 ng g -1 , and 0.01-0.48 ng g -1 , respectively. Resuspension increased the concentrations of HCHs, HCB, and DDTs in the surface sediment with the release of historically contaminated pollutants accumulated in a lower layer. We speculate that CHLs in air that were removed by atmospheric deposition affects the concentration of CHLs in surface sediments., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

The environmental contamination by benzotriazole ultraviolet stabilizers (BUVSs) has received consider attention due to their long-term and widespread usage in various consumer and industrial products in accordance with solar UV radiation increase. The present study shows the baseline data of BUVSs in human breast milk from several areas in Japan, the Philippines, and Vietnam. Total concentrations of the 8 BUVSs in breast milk ranged from

Levels and profiles of naturally produced halogenated bipyrroles (Br 4 Cl 2 -DBP and Cl 7 -MBP), methoxylated tetrabromodiphenyl ethers (6-MeO-BDE47), anthropogenic perfluoroalkyl substances (PFASs) and legacy persistent organic pollutants (POPs) were investigated in the livers of 14 cetaceans from the Sea of Japan and the North Pacific Ocean. The concentrations of Br 4 Cl 2 -DBP (4 to 4900 ng/g-wet), Cl 7 -MBP (16 to 3960 ng/g-wet) and 6-MeO-BDE47 (7 to 190 ng/g-wet) were higher in the order of killer whales > toothed whales > baleen whales. Profiles of PFASs were dominated by perfluoroundecanoic and perfluorotridecanoic acids (10 to 540 ng/g-wet), sum of which accounted for 70% of total measured PFASs. Regional difference was observed for Cl 7 -MBP and PFASs, which were higher in the Sea of Japan, whereas Br 4 Cl 2 -DBP was in the North Pacific Ocean. Specific accumulation pattern of these natural contaminants in cetaceans around northern Japan could help compare the exposure profile of PFASs and POPs among other geographic regions., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Organic ultraviolet (UV) filters are used widely in various personal care products and their ubiquitous occurrence in the aquatic environment has been reported in recent years. However, data on their fate and potential impacts in marine sediments is limited. This study reports the occurrence and risk assessment of eleven widely used organic UV filters in marine sediment collected in Hong Kong and Tokyo Bay. Seven of the 11 target UV filters were detected in all sediment samples (median concentrations:

Background: The age-specific impacts of perinatal exposures to polychlorinated biphenyls (PCB), methylmercury (MeHg), and lead on child neurodevelopment remain controversial. Since we have already reported the prenatal effects of these chemicals on neurodevelopment in 3-day-old and 30-month-old children of a birth cohort, the following effects were analyzed in the 42-month-old children in the same cohort., Methods: The Kaufman Assessment Battery for Children (K-ABC), comprised of four scales, was used to assess their intelligence and achievement. The relationships between the chemicals and K-ABC scores were analyzed using multivariate analyses., Results: The median values of chemicals in cord blood of 387 children were 46.5 (5th and 95th percentiles, 16.7-115.7)ng/g-lipid for total PCB, 10.1 (4.3-22.2)ng/g for total mercury (THg), and 1.0 (0.5-1.8) μg/dL for lead. Of the highly chlorinated PCB homologs, 9 CBs was negatively correlated with the sequential and mental processing score of the K-ABC (p<0.05). There were no significant correlations between any K-ABC score and either THg or lead. The negative effect of 9 CBs remained even after adjusting for THg, lead, and other confounders. The K-ABC scores were significantly lower in the boys than in the girls, and the standardized β of 9 CBs for the sequential and mental processing scores in multiple regression analysis was statistically significant in boys., Conclusions: These findings suggest that intellectual ability in the developmental stage may be impaired by prenatal exposures to highly chlorinated PCB homologs, especially in Japanese boys., (Copyright © 2014 Elsevier Inc. All rights reserved.)

The concentrations of PCB congeners in the blubber and liver of mother Steller sea lions (Eumetopias jubatus; SSLs) and their fetuses from the coast of Hokkaido, Japan in 2008, 2010 and 2012 were analyzed by HRGC-HRMS, in order to elucidate PCB congener profiles and maternal-to-fetal transfer of PCBs in SSLs. ΣPCBs in the fetuses were 1400 ± 660 (the mean ± SD) ng/g-fat in the blubber and 570 ± 320 ng/g-fat in the liver, respectively. There was a concern that SSLs had been contaminated by PCBs during the fetal period. The concentrations of the major congeners in the blubber and liver were a correlation between the fetus and mother (blubber: r=0.9934, liver: r=0.9160; P ≦ 0.05). The results indicated that PCBs in the fetuses came from the mothers. #177 and #199 showed no correlations between the fetus and the mother in the blubber and liver. This indicated a selective capture by some natural protector such as the placenta., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Polybrominated diphenyl ethers (PBDEs) were measured in surface sediment samples collected from urban canals or rivers in Lao PDR, Cambodia, Vietnam, India, Indonesia, Thailand, the Philippines, Malaysia and Japan. The total PBDE concentrations in the sediments ranged from 0.83 to 3140 ng/g dry wt. BDE-209 was predominant, ranging from 43% to 97% of total PBDEs, followed by nona-BDEs and some detectable concentrations of BDEs 47, 49, 99, 100, 153, 154 and 183. Sedimentary PBDE levels in Malaysia, Cambodia, the Philippines and Thailand were generally higher than those reported for highly industrialized countries. Spatial distribution of PBDEs indicated that inland sources may impact coastal areas. The presence of BDE congeners which are not contained in technical mixtures and the higher proportions of nona-BDEs relative to BDE-209 in the sediments were identified as indicators of debromination. BDE-209 was possibly debrominated under anaerobic conditions in some of the sediment samples., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Objectives: To assess whether polychlorinated biphenyls (PCBs), methylmercury, lead, or parental child-rearing attitudes was most crucial for maladaptive behavior problems, we examined Japanese 30-month-old children followed up from pregnancy., Methods: The Child Behavior Checklist (CBCL) was used to assess the behavior problems in 306 children. The associations of cord-blood total PCBs (ΣPCB), total mercury (THg), and lead with each CBCL subscale were examined by multivariate analyses., Results: The median values in cord blood of the 306 children were 48.3 (5 and 95 percentiles, 18.6-116.3) ng/g-lipid for ΣPCB, 10.2 (4.1-24.5)ng/g for THg, and 1.0 (0.5-1.7)μg/dl for lead. The internalizing score of the CBCL was significantly correlated with ΣPCB (r=0.113) in the children, though no significant correlation was seen between any CBCL score and either THg or lead. The significant correlation disappeared when conducting multiple regression analysis with possible confounders; at that time, the birth order, home environment, and maternal intelligence quotient were significantly related to the internalizing score. Three CBCL scores and ΣPCB levels were significantly higher in the first-born children than in the second-born or following children, and the partial correlation coefficient with the adjustment for all confounders except birth order was significant between the internalizing score and ΣPCB in the latter children (r=0.175)., Conclusions: Internalizing behavior appears to be affected by prenatal exposure to PCBs at low levels. Under lower-level exposures, however, behavior problems may be more strongly associated with parental child-rearing attitudes involved in birth order, than with such hazardous chemicals., (Copyright © 2012 Elsevier Inc. All rights reserved.)

Twelve species of deep-sea fishes collected in 2005 from the western North Pacific, off-Tohoku, Japan were analyzed for organohalogen compounds. Among the compounds analyzed, concentrations of DDTs and PCBs (up to 23,000 and 12,400 ng/g lipid wt, respectively) were the highest. The present study is the foremost to report the occurrence of brominated flame retardants such as PBDEs and HBCDs in deep-sea organisms from the North Pacific region. Significant positive correlations found between delta(15)N ( per thousand) and PCBs, DDTs and PBDEs suggest the high biomagnification potential of these contaminants in food web. The large variation in delta(13)C (per thousand) values observed between the species indicate multiple sources of carbon in the food web and specific accumulation of hydrophobic organohalogen compounds in benthic dwelling carnivore species like snubnosed eel. The results obtained in this study highlight the usefulness of deep-sea fishes as sentinel species to monitor the deep-sea environment., (Copyright 2009 Elsevier Ltd. All rights reserved.)

Blubber and liver samples were obtained for analysis of wide ranges of contaminants from killer whales (Orcinus orca) which were locked away in drifting sea ice on the coast of Rausu, the Shiretoko Peninsula in Eastern Hokkaido, Japan in February 2005. Among the organohalogen compounds analyzed, DDTs were the predominant contaminants with concentrations ranging from 28 to 220 microg/g on a lipid-weight basis followed by PCBs and other organochlorine pesticides. PBDEs levels were two or three orders of magnitude lower than those of PCBs and DDTs. 2,3,7,8-Tetrachlorodibenzo-p-dioxin toxic equivalents (TEQs) derived by WHO mammal-TEF in killer whales were in the range of 110-440 pgTEQ/g. Mono-ortho coplanar PCBs contributed to 75-98% of total TEQs, indicating coplanar PCBs are significant contaminants for risk assessment in this species. The fact that hepatic residue levels of butyltins (from 13 to 770 ng/g wet weight) were much higher than those of phenyltins may be reflecting extensive use of tributyltin as antifouling paint.

Concentrations of polychlorinated biphenyls (PCBs) in beached resin pellets were examined to reveal variability between individual particles and differences among beaches. Fifty-five resin pellets from a beach in Tokyo were individually analyzed for PCBs, and showed concentrations ranging from <28 to 2,300 ng/g. This indicates that concentrations are highly variable between particles. Among several characters, discoloration (e.g., yellowing) had a positive relationship with PCB concentration: discolored pellets contained more PCBs than others on most of the beaches sampled. Given the color-selective ingestion of food by some organisms, this may be ecotoxicologically important. Measurements of samples from 47 beaches in Japan showed regional differences in PCB concentrations in resin pellets consistent with those in mussels. Sporadic high concentrations of PCBs were also found in pellets from remote islands, suggesting that resin pellets could be the dominant route of exposure to the contaminants at remote sites. The similarity of PCB concentrations between resin pellets and mussels suggests a potential use of resin pellets to monitor pollution in seawater.

Persistent organic pollutants have been linked to various adverse effects on human health. We conducted a retrospective exposure assessment for 11polychlorinated biphenyl (PCB) congeners and 4 polybrominated diphenyl ether (PBDE) congeners. We analyzed paired samples of blood and food duplicate portions collected in the 1980s (1980 survey, N=40) and the mid-1990s (1995 survey, N=40) from females (five participants from each of eight sites per survey) living throughout Japan, from Hokkaido to Okinawa. The study populations in the 1980 and 1995 surveys were different but had lived in the same community. We measured PCBs and PBDEs in serum and PCBs in diet. Total serum PCBs (ng/g lipid) [geometric mean (geometric standard deviation)] were similar in the 1980 [163.0 (1.7)] and the 1995 [142.6 (2.0)] surveys. In contrast, dietary intake (ng/day) between 1980 and 1995 decreased significantly, from 522.8 (2.5) to 165.9 (3.3), respectively, (P<0.05). We classified the participants by birth year-before 1941 (older generation) and equal to or after 1941 (younger generation). Serum PCB levels decreased significantly in the younger generation, from 179.1 (1.8) in the 1980 survey to 115.4 (2.0) in the 1995 survey (P<0.05). However, in the older generation, serum levels (ng/g lipid) did not change: 150.4 (1.6) in the 1980 survey and 180 (1.8) in the 1995 survey. Total PBDE serum levels (ng/g lipid) increased significantly during the 15 years, from 0.5 (3.5) to 1.8 (3.7) (P<0.05). At the Shimane site, PBDE serum levels (ng/g lipid) increased 20-fold, from 1.3 (4.8) to 26.0 (5.0). The serum levels of PCBs decreased in the younger generation but not in the older, although levels in daily intakes decreased significantly. Exposure levels of PBDEs appear to be increasing in an area-specific manner.

Histological examination of gonads as well as chemical analysis of organotin compounds in tissues of the giant abalone, Haliotis madaka, was conducted to evaluate continuing endocrine disruption in abalone populations in Japan. Abalone specimens were collected from two different areas, Tsushima as a reference site and Jogashima as a site representative of declining abalone populations where serious organotin contamination had been observed, each month from January 1998 to March 1999. Scores were given to the development stages of reproductive cells in the ovary and testis. The degree of sexual maturation was evaluated by calculating the mean value of a histogram of these scores for the reproductive cells of each abalone. The temporal variations in degree of sexual maturation showed that female and male abalone from Tsushima matured synchronously, while those from Jogashima did not, which were similar to results of the previous study during September 1995-November 1996. Approximately 19% of the female abalone from Jogashima were masculinized with an ovo-testis, which was also similar to the result of the previous study. The masculinization of female abalone is reported to be induced by tributyltin (TBT) and triphenyltin (TPhT) from antifouling paints. Concentrations of the sum of butyltins (TBT, dibutyltin (DBT) and monobutyltin (MBT): SigmaBTs) and the sum of phenyltins (TPhT, diphenyltin (DPhT) and monophenyltin (MPhT): SigmaPhTs) in the muscle of abalone from Jogashima (n = 73) of 7.8+/-9.0 ng/g wet wt. and 4.5+/-6.8 ng/g wet wt., respectively, were significantly higher than those from Tsushima (n = 87) of 4.7+/-4.9 ng/g wet wt. and 0.8+/-1.7 ng/g wet wt., respectively (p < 0.05 for SigmaBTs; p < 0.001 for SigmaPhTs), although concentrations of TBT and TPhT in the muscle of abalone from Jogashima (n = 73) of 2.2+/-2.5 ng/g wet wt. and 5.8+/-5.1 ng/g wet wt., respectively, were insignificantly and significantly higher than those from Tsushima (n = 87) of 0.4+/-0.6 ng/g wet wt. and 0.5+/-0.9 ng/g wet wt., respectively, (p > 0.05 for TBT; p < 0.001 for TPhT). Thus, endocrine disruption as well as contamination by organotins in the giant abalone from Jogashima is still persisting.

To clarify their mutagenic potential, samples of water from the Mawatari, Asuwa and Kitsune rivers, which flow through the central area of Fukui, Japan, were seasonally collected at six sites using blue rayon from July 1998 to August 2000. Forty-five of 52 (87%) of the water samples exhibited mutagenicity toward Salmonella typhimurium YG1024 and YG1029 with and without S9 mix, and the highest potencies were observed in YG1024 with S9 mix. The samples collected in summer and autumn tended to be more mutagenic than those collected in winter and spring. Fractionation using high-performance liquid chromatography (HPLC) suggests that several compounds are responsible for the mutagenicity of river water samples, and some of the major mutagens seem to be common among the samples. Three 2-phenylbenzotriazole (PBTA)-type mutagens, 2-[2-(acetylamino)-4-[(2-hydroxyethyl)amino]-5-methoxyphenyl]-5-amino-7-bromo-4-chloro-2H-benzotriazole (PBTA-3), 2-[2-(acetylamino)-4-amino-5-methoxyphenyl]-5-amino-7-bromo-4-chloro-2H-benzotriazole (PBTA-4) and 2-[2-(acetylamino)-4-[bis(2-hydroxyethyl)amino]-5-methoxyphenyl]-5-amino-7-bromo-4-chloro-2H-benzotriazole (PBTA-6), were quantified in samples collected between July 1998 and April 1999. At least one of these PBTA-type mutagens was detected in 23/24 (96%) of the samples. The amounts of PBTA-3, -4 and -6 were <0.08-58.7, <0.1-15.0 and <0.07-467.9 ng/g of blue rayon, respectively, and high levels of PBTA congeners were detected in the samples collected from each river in July and November 1998. The contributions of these PBTA congeners to the mutagenicity of water samples were also high in July and November 1998. The highest total contribution was observed for samples from the Asuwa river (67.6%). These findings suggest that these three rivers were continually and heavily contaminated with mutagens, and PBTA congeners were some of the major mutagens in these rivers.

Organochlorine (OCs) and butyltin (BTs) residues were determined in deep-sea organisms collected from the western North Pacific, off-Tohoku, Japan. Among OCs, concentrations of polychlorinated biphenyls (PCBs) and DDTs (DDTs and its metabolites) were the highest in deep-sea organisms (maximum concentrations of 6,700 and 13,000 ng/g lipid wt, respectively). Chlordane compounds (CHLs) were the next most abundant OCs, and hexachlorocyclohexanes (HCHs) and hexachlorobenzene (HCB) were the lowest. BTs were also detected at maximum concentrations of 570 ng/g wet wt. Concentrations of PCBs, CHLs and BTs in deep-sea organisms collected from the western North Pacific, off-Tohoku, were generally lower than those in deep-sea and shallow water organisms from Japanese coastal waters. On the other hand, considerable variations in the concentrations of OCs were found among deep-sea organisms analyzed. Several carnivorous fishes such as snubnosed eel, lanternshark and grenadiers accumulated some OCs such as PCBs, DDTs and CHLs at high concentrations of up to a few microg/g levels. In addition, the residue pattern of OCs and BTs in fishes showed a specific trend according to the sampling depth; higher concentrations of PCBs, DDTs and CHLs and lower concentrations of HCHs, HCB and BTs were found in fishes collected from greater depth (approximately 1,000 m) compared to those from shallower waters. This trend is consistent with the results of our earlier study on mesopelagic myctophid fishes. Results of this study suggest vertical transport of hydrophobic OCs such as PCBs, DDTs and CHLs and its accumulation in benthic deep-sea organisms.

Cereals, especially rice, are a major source of cadmium (Cd) intake for general Japanese populations. In 1998-2000, rice (polished), bread (loaf), noodle and (wheat) flour samples (4113 samples in total) were collected in 63 cities all over Japan, and analyzed for Cd by inductively-coupled plasma mass spectrometry. Another pollutant element of lead (Pb) was determined in parallel. The grand geometric mean for Cd in polished raw (uncooked) rice was 50 ng/g, whereas it was 19 ng/g for flour. The value for Pb was 2-3 ng/g in rice and flour. Calculation for daily Cd intake via rice, taking advantage of the present findings on Cd contents in rice and wheat together with administrative area-specific daily consumptions of rice and wheat showed that Cd via rice is much more than Cd via wheat and that Cd via rice is highest in an area alongside the sea of Japan among the whole country, the observation being in agreement with the results from a previous food duplicate-based field survey.

We previously determined the chemical structures of four 2-phenylbenzotriazole mutagens (PBTA-1, -2, -3 and -4) in blue rayon-adsorbed material from the Nishitakase River in Kyoto prefecture and the Nikko River in Aichi prefecture in Japan. On the basis of a synthesis study, these four PBTA derivatives were deduced to have originated from corresponding dinitrophenylazo dyes by reduction and chlorination. 2-[(2-Bromo-4,6-dinitrophenyl)azo]-5-[bis(2-acetoxyethyl) amino]-4-methoxyacetanilide (Color Index Name, Disperse Blue 79:1; CAS Registry Number, 75497-74-4) is a very common dinitrophenylazo dye used in textile dyeing factories. In the present study, we synthesized 2-[4-[bis(2-acetoxyethyl)amino]-2-(acetylamino)-5-methoxyphenyl]-5-amino-7-bromo-4-chloro-2H-benzotriazole (PBTA-5) from Disperse Blue 79:1 by reduction with sodium hydrosulfite and subsequent chlorination with sodium hypochlorite. On hydrolysis of PBTA-5 with alkali, 2-[2-(acetylamino)-4-[bis(2-hydroxyethyl)amino]-5-methoxyphenyl]-5-amino-7-bromo-4-chloro-2H-benzotriazole (PBTA-6) was obtained. Both PBTA-5 and -6 were potent mutagens, inducing 723,000 revertants and 485,000 revertants per microgram of Salmonella typhimurium YG1024, respectively, in the presence of S9 mix. To clarify whether PBTA-5 and -6 exist in the environment, water samples were collected from five rivers flowing through regions where textile dyeing industries are developed. PBTA-6 was detected at levels of 3-134 ng/g blue rayon in all water samples that were examined. On the other hand, the amount of PBTA-5 in the samples was less than the detection limit.

Based on our previous finding that the concentrations of total mercury in mussel adductor muscle approximated those of methylmercury, we compared concentrations of total mercury in the adductor muscle of the mussel Mytilus galloprovincialis, collected from four sites around Minamata City from 1993 to 1995 and four sites in Kagoshima Bay from 1997 to 1998, to assess the level of localized methylmercury contamination. Though the input of mercury from the chemical plant had stopped by around 1970, concentrations of total mercury in the mussel adductor muscle were higher at two sites (26-121 ng/g, n = 135) near the main fallout of wastewater from the chemical plant in Minamata Bay than at the other sites, i.e. two sites 1-5 km from the former sites in Minamata City (6-28 ng/g, n = 52), and all sites in Kagoshima Bay (2-30 ng/g, n = 287). The localized methylmercury contamination around the chemical plant in Minamata Bay was documented also by our sensitive analysis of mercury concentrations in seawater and sediment samples. The survey of concentrations of total mercury in the mussel adductor muscle seems to be useful for monitoring the methylmercury contamination in coastal areas.

The aim of this study was: (a) to estimate the concentration of total mercury in the renal cortex, liver, cerebellum and hair of 46 persons who died suddenly in the Gdańsk region, northern Poland, between the ages of 17 and 90; and (b) to assess whether a correlation occurs between mercury content in the investigated biological media. The mean concentrations of mercury in the human hair, renal cortex, liver and cerebellum were: 378 +/- 315.4 ng/g; 68.6 +/- 92.3 ng/g; 29.9 +/- 22 ng/g and 5.3 +/- 6.9 ng/g respectively. Positive correlations were found between mercury levels in: cerebellum and liver (r = 0.873), cerebellum and hair (r = 0.853), cerebellum and renal cortex (r = 0.578), hair and liver (r = 0.771), hair and renal cortex (r = 0.478) liver and renal cortex (r = 0.66). The geometric mean levels of mercury in the renal cortex, liver, cerebellum and hair in the residents of the Gdańsk region are 15-19 times lower than in the population of Tokyo and its environs [Suzuki T, Hongo T, Yoshinaga J et al. The hair-organ relationship in mercury concentration in contemporary Japanese. Arch Environ Health 1993;44:361-365].

Samples of red blood cells (RBCs) from 1178 inhabitants, consisting of 546 males and 795 females (over 40 years old), of a coastal town near Minamata City were analyzed for total mercury. The mercury concentrations in the RBCs showed lognormal distributions for both sexes with higher values in males than in females. The geometric mean of the mercury concentrations in the RBCs was 27.5 ng/g (ranging from 8.0 to 69.1 ng/g) for males and 20.4 ng/g (ranging from 7.0 to 63.7 ng/g) for females. The mercury concentrations in the RBCs decreased with advancing age. A significant regression between the geometric mean of the mercury concentrations in the RBCs and age was obtained for both sexes. The mercury concentrations in the RBCs from male inhabitants of the coastland area were significantly higher than those from male inhabitants of the inland area. In terms of occupation, the highest mercury concentrations were observed in the RBCs from fisherman. No significant difference in the present mercury concentrations in the RBCs was observed between the cases with Minamata disease and the controls.

This study showed differences in erythrocyte manganese concentrations in different age groups and in cord blood. All determinations were performed with a flameless atomic absorption spectrophotometer. The mean erythrocyte manganese concentration at one month of age was 435.1 +/- 118.7 ng/g Hb, three to four times higher than in adults. Thereafter, it decreased rapidly and was constant from 4 months to 11 yr of age. However, at 12 to 19 yr of age the concentration in males decreased (108.1 +/- 20.2 ng/g Hb) and was significantly lower than in females (141.7 +/- 25.5 ng/g Hb) (p less than 0.01). This sex difference became even greater in adults aged 20 to 40 yr, when it was 91.5 +/- 22.4 ng/g Hb in males and 141.2 +/- 19.8 ng/g Hb in females (p less than 0.001). The erythrocyte manganese concentration in adults was 31.6 +/- 9.2 ng/ml, somewhat higher than the value previously reported, which may reflect dietary habits in Japan or a racial difference.