Publications by authors named "Shinsuke Tanabe"

339 Publications

Nontarget Screening of Organohalogen Compounds in the Liver of Wild Birds from Osaka, Japan: Specific Accumulation of Highly Chlorinated POP Homologues in Raptors.

Environ Sci Technol 2021 Jun 8. Epub 2021 Jun 8.

Center for Marine Environmental Studies (CMES), Ehime University, 2-5 Bunkyo-cho, Matsuyama 790-8577, Japan.

Nontarget screening studies have recently revealed the accumulation of typically unmonitored organohalogen compounds (OHCs) in various marine animals, but information for terrestrial food chains is still lacking. This study investigated the accumulation profiles of known and unknown OHCs in the liver of representative wild bird specimens from Osaka, Japan using nontarget analysis based on two-dimensional gas chromatography-time-of-flight mass spectrometry. A large number of unmonitored OHCs were identified, including anthropogenic contaminants and marine halogenated natural products (HNPs), and their accumulation profiles were considered to be influenced by terrestrial and brackish water-based diets. Anthropogenic OHCs were highly accumulated in terrestrial predator species (peregrine falcon, hawks, and black kite), and some unmonitored highly chlorinated contaminants reached the levels of microgram per gram lipid in the liver, i.e., C-/C-based chlordane related compounds (CHLs) and their epoxides, dichlorodiphenyldichloroethylene (DDE) homologues, and polychlorinated terphenyls (PCTs). In contrast, HNPs were accumulated at higher levels in piscivorous birds (gray heron and common cormorant). Considering the enrichment of the unmonitored C-/C-based CHLs, PCTs, and DDE homologues relative to structurally similar persistent organic pollutants (POPs) in high trophic-level species such as raptors, further studies are needed to elucidate their environmental levels, behavior in terrestrial food chains, and ecotoxicological impacts.
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http://dx.doi.org/10.1021/acs.est.1c00357DOI Listing
June 2021

Polycyclic aromatic hydrocarbons in airborne particulate matter samples from Hanoi, Vietnam: Particle size distribution, aryl hydrocarbon ligand receptor activity, and implication for cancer risk assessment.

Chemosphere 2021 Apr 30;280:130720. Epub 2021 Apr 30.

Centre for Environmental Technology and Sustainable Development (CETASD), University of Science, Vietnam National University, Hanoi, 334 Nguyen Trai, Hanoi, 11400, Viet Nam. Electronic address:

Concentrations and profiles of unsubstituted and methylated polycyclic aromatic hydrocarbons (PAHs and Me-PAHs) were analyzed in airborne particulate matter (PM) samples collected from high-traffic roads in Hanoi urban area. Levels of PAHs and Me-PAHs ranged from 210 to 660 (average 420) ng/m in total PM, and these pollutants were mainly associated with fine particles (PM) rather than coarser ones (PM and PM). Proportions of high-molecular-weight compounds (i.e., 5- and 6-ring) increased with decreasing particle size. Benzo[b+k]fluoranthene, indeno[1,2,3-cd]pyrene, and benzo[ghi]perylene were the most predominant compounds in the PM samples. In all the samples, Me-PAHs were less abundant than unsubstituted PAHs. The PAH-CALUX assays were applied to evaluate aryl hydrocarbon receptor (AhR) ligand activities in crude extracts and different fractions from the PM samples. Benzo[a]pyrene equivalents (BaP-EQs) derived by the PAH-CALUX assays for low polar fractions (mainly PAHs and Me-PAHs) ranged from 300 to 840 ng/m, which were more consistent with theoretical values derived by using PAH-CALUX relative potencies (270-710 ng/m) rather than conventional toxic equivalency factor-based values (22-69 ng/m). Concentrations of PAHs and Me-PAHs highly correlated with bioassay-derived BaP-EQs. AhR-mediated activities of more polar compounds and interaction effects between PAH-related compounds were observed. By using PAH-CALUX BaP-EQs, the ILCR values ranged from 1.0 × 10 to 2.8 × 10 for adults and from 6.4 × 10 to 1.8 × 10 for children. Underestimation of cancer risk can be eliminated by using effect-directed method (e.g., PAH-CALUX) rather than chemical-specific approach.
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http://dx.doi.org/10.1016/j.chemosphere.2021.130720DOI Listing
April 2021

The association between antimicrobials and the antimicrobial-resistant phenotypes and resistance genes of Escherichia coli isolated from hospital wastewaters and adjacent surface waters in Sri Lanka.

Chemosphere 2021 Sep 17;279:130591. Epub 2021 Apr 17.

National Institute of Animal Health, National Agriculture and Food Research Organization, 3-1-5 Kannondai, Tsukuba, 305-0856, Ibaraki, Japan.

The presence of antimicrobials, antimicrobial-resistant bacteria (ARB), and the associated antimicrobial resistance genes (ARGs) in the environment is a global health concern. In this study, the concentrations of 25 antimicrobials, the resistance of Escherichia coli (E. coli) strains in response to the selection pressure imposed by 15 antimicrobials, and enrichment of 20 ARGs in E. coli isolated from hospital wastewaters and surface waters were investigated from 2016 to 2018. In hospital wastewaters, clarithromycin was detected at the highest concentration followed by sulfamethoxazole and sulfapyridine. Approximately 80% of the E. coli isolates were resistant, while 14% of the isolates exhibited intermediate resistance against the tested antimicrobial agents. Approximately 61% of the examined isolates were categorized as multidrug-resistant bacteria. The overall abundance of phenotypes that were resistant toward drugs was in the following order: β-lactams, tetracycline, quinolones, sulfamethoxazole/trimethoprim, aminoglycosides, and chloramphenicol. The data showed that the E. coli isolates frequently harbored bla, bla, tetA, qnrS, and sul2. These results indicated that personal care products were significantly associated with the presence of several resistant phenotypes and resistance genes, implying their role in co-association with multidrug resistance. Statistical analysis also indicated a disparity specific to the site, treatment, and year in the data describing the prevalence of ARB and ARGs and their release into downstream waters. This study provides novel insights into the abundance of antimicrobial, ARB and ARGs in Sri Lanka, and could further offer invaluable information that can be integrated into global antimicrobial resistance databases.
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http://dx.doi.org/10.1016/j.chemosphere.2021.130591DOI Listing
September 2021

Snakes as bimonitors of environmental pollution: A review on organic contaminants.

Sci Total Environ 2021 May 20;770:144672. Epub 2021 Jan 20.

Center for Marine Environmental Studies (CMES), Ehime University, 2-5 Bunkyo-cho, Matsuyama 790-8577, Japan.

Monitoring data on organic pollutants published between the late 1960s and 2020 are reviewed to provide comprehensive and updated insights into their bioaccumulation characteristics, sources, and fate in snakes. Multiple organic pollutant classes including pesticides, polychlorinated biphenyls, chlorinated paraffins, dioxin-related compounds, alkanes, polycyclic aromatic hydrocarbons, flame retardants, plasticizers, etc., were detected in various aquatic and terrestrial snake species with concentrations and patterns varying between species and locations. In general, higher concentrations of organic pollutants were found in snakes collected from contaminated sites (e.g., densely populated, pesticide-treated, and waste processing areas), suggesting that snakes can serve as good biomonitors of environmental pollution caused by organic contaminants. Factors influencing concentrations and patterns of organic pollutants in snakes are discussed, providing an overview of current understanding about their accumulation, transformation, and elimination processes. Potential negative effects associated with organic pollutants in snakes and their predators are also considered. Based on such discussions, research gaps and future perspectives on the utilization of snake biomonitoring studies are addressed, heading towards an effective monitoring and assessment scheme for a variety of legacy and emerging organic pollutants in the environment.
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http://dx.doi.org/10.1016/j.scitotenv.2020.144672DOI Listing
May 2021

Anthropogenic and natural organohalogen compounds in melon-headed whales (Peponocephala electra) stranded along the Japanese coastal waters: Temporal trend analysis using archived samples in the environmental specimen bank (es-BANK).

Chemosphere 2021 Apr 22;269:129401. Epub 2020 Dec 22.

Center for Marine Environmental Studies (CMES), Ehime University, 2-5 Bunkyo-cho, Matsuyama, 790-8577, Japan.

The present study determined recent accumulation levels of polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethane and its metabolites (DDTs), hexachlorocyclohexane isomers (HCHs), chlordane compounds (CHLs), hexachlorobenzene (HCB), polybrominated diphenyl ethers (PBDEs), hexabromocyclododecanes (HBCDDs), polychlorinated diphenyl ethers (PCDEs), methoxylated-PBDEs (MeO-PBDEs) and 2,3,3',4,4',5,5'-heptachloro-1'-methyl-1,2'-bipyrrole (Q1) in the blubber of melon-headed whales (Peponocephala electra) stranded along the Japanese coastal waters in 2015 and examined temporal trends of these organohalogen compound (OHC) levels by analyzing blubber samples of this species archived in the environmental specimen bank which were collected in 1982, 2001, 2002, 2006, 2010 and 2011. The median concentrations in melon-headed whales stranded recently were in the order of DDTs ≈ PCBs > HBCDDs > Q1 > CHLs > MeO-PBDEs > PBDEs > HCB > HCHs > PCDEs, indicating that considerable amounts of HBCDDs, in addition to DDTs and PCBs, have been transported to tropical and subtropical waters of the open ocean and pelagic whale species might be exposed to relatively high levels of these OHCs. Temporal trend analyses of OHC levels in the blubber of melon-headed whales revealed significant decrease for anthropogenic OCs such as DDTs, PCBs, HCB, HCHs and PCDEs, and significant increase for CHLs, PBDEs, HBCDDs, MeO-PBDEs and Q1 since 1982. Besides, the analyses from 2001 to 2015 showed no decreasing trends (unchanged) for some PCB congeners, p,p'-DDE, cis- and trans-nonachlors, Q1, BDE-47, -100 and -154, and significantly increasing trends for α-HBCDD and 6MeO-BDE47, suggesting their chronic exposure for this pelagic whale species.
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http://dx.doi.org/10.1016/j.chemosphere.2020.129401DOI Listing
April 2021

Rapid analysis of 65 pharmaceuticals and 7 personal care products in plasma and whole-body tissue samples of fish using acidic extraction, zirconia-coated silica cleanup, and liquid chromatography-tandem mass spectrometry.

J Chromatogr A 2020 Sep 28;1631:461586. Epub 2020 Sep 28.

Center for Marine Environmental Studies (CMES), Ehime University, 2-5 Bunkyo-cho, Matsuyama, Ehime 790-8577, Japan.

The presence of pharmaceuticals and personal care products (PPCPs) in aquatic systems has raised concern about their potential adverse effects on aquatic organisms. Considering the fact that the physiological/biological effects of PPCPs are triggered when their concentrations in the organism exceeds the respective threshold values, it is important to understand the bioconcentration and toxicokinetics of PPCPs in aquatic organisms. In the present study, we developed a convenient analytical method for the determination of 65 pharmaceuticals and 7 personal care products (log K = 0.14-6.04) in plasma and whole-body tissues of fish. The analytical method consists of ultrasound-assisted extraction in methanol/acetonitrile (1:1, v/v,) acidified with acetic acid-ammonium acetate buffer (pH 4), cleanup on a HybridSPE®-Phospholipid cartridge (zirconia-coated silica cartridge), and quantification with liquid chromatography-tandem mass spectrometry (LC-MS/MS). Acceptable accuracy (internal standard-corrected recovery: 70%-120%) and intra- and inter-day precision (coefficient of variation: <15%) were obtained for both plasma and whole-body tissue samples. In addition, low method detection limits were achieved for both plasma (0.0077 to 0.93 ng mL) and whole-body tissue (0.022 to 4.3 ng g   wet weight), although the developed method is simple and fast - a batch of 24 samples can be prepared within 6 h, excluding the time for measurement with LC-MS/MS. The developed method was successfully applied to the analysis of PPCPs in plasma and whole-body tissue samples of fish collected in a treated wastewater-dominated stream, for a comprehensive evaluation of their bioconcentration properties. The analytical method developed in the present study is sufficiently accurate, sensitive, and rapid, and thus highly useful for the comprehensive evaluation of PPCP residues in fish and would aid in future exposome and risk assessment.
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http://dx.doi.org/10.1016/j.chroma.2020.461586DOI Listing
September 2020

Contamination of habu (Protobothrops flavoviridis) in Okinawa, Japan by persistent organochlorine chemicals.

Environ Sci Pollut Res Int 2021 Jan 22;28(1):1018-1028. Epub 2020 Aug 22.

Center for Marine Environmental Studies (CMES), Ehime University, 2-5 Bunkyo, Matsuyama, Ehime, 790-8577, Japan.

Persistent organochlorine chemicals (OCs), including chlordane compounds (CHLs), DDTs, PCBs, and chlorinated dioxins and related compounds (DRCs), were examined in the adipose tissue and liver from 33 specimens of habu (Protobothrops flavoviridis), a species of venomous pit viper endemic to the Japanese Southwest Islands. The median concentrations of CHLs, DDTs, and PCBs in adipose tissue of 22 habus collected from an urban area were 4400 ng g lipid weight (lw), 610 ng g lw, and 1600 ng g lw, respectively. Their DDT and PCB concentrations were higher in comparison with the specimens from a rural area. Liver of 10 specimens from the urban area were subjected to DRCs analysis, and PCDDs, PCDFs, and DL-PCBs were detected with median values of 1300, 350, and 150,000 pg g lw, respectively. Among PCDD/F congeners, octa-CDD was detected at the highest concentrations in seven liver samples, but considerable concentrations of penta- and hexa-CDD/Fs were found in two samples. Relatively higher concentrations of PCB, DDTs, and PCDD/Fs were found in habus collected within 1 km of the boundary of military facilities, suggesting that OCs from some unknown sources of these OCs inside and/or around some of the facilities accumulated in habus.
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http://dx.doi.org/10.1007/s11356-020-10510-yDOI Listing
January 2021

Mother to Fetus Transfer of Hydroxylated Polychlorinated Biphenyl Congeners (OH-PCBs) in the Japanese Macaque (): Extrapolation of Exposure Scenarios to Humans.

Environ Sci Technol 2020 09 27;54(18):11386-11395. Epub 2020 Aug 27.

Center for Marine Environmental Studies (CMES), Ehime University, Bunkyo-cho 2-5, Matsuyama 790-8577, Japan.

Prenatal hydroxylated polychlorinated biphenyls (OH-PCBs) exposure may disrupt fetal brain development during the critical period of thyroid hormone (TH) action. However, there are limited studies on the OH-PCB transfer to the fetal brain, particularly in primates. In this study, we selected the Japanese macaque () as a model animal for the fetal transfer of OH-PCBs in humans and revealed OH-PCB concentrations and their relationships in maternal and fetal blood, liver, and brain. l-thyroxine (T4)-like OH-PCBs including 4OH-CB187, a major congener in humans, were found in high proportions in the blood, liver, brain, and placenta of pregnant Japanese macaques. OH-PCBs were detected in the fetal brain and liver in the first trimester, indicating their transfer to the brain in the early pregnancy stage. 4OH-CB187 and 4OH-CB202 were the major congeners found in fetal brain, indicating that these T4-like OH-PCBs are transported from maternal blood to the fetal brain via the placenta. These results indicate that further studies are needed on the effects of OH-PCBs on the developing fetal brain.
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http://dx.doi.org/10.1021/acs.est.0c01805DOI Listing
September 2020

Coastal biomonitoring survey on persistent organic pollutants using oysters (Saccostrea mordax) from Okinawa, Japan: Geographical distribution and polystyrene foam as a potential source of hexabromocyclododecanes.

Sci Total Environ 2020 Oct 6;739:140049. Epub 2020 Jun 6.

Center for Marine Environmental Studies (CMES), Ehime University, Bunkyo-cho 2-5, Matsuyama, Ehime 790-8577, Japan. Electronic address:

The present study determined contamination levels of POPs, such as polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethane and its metabolites (DDTs), chlordane compounds (CHLs), polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs), in oysters (Saccostrea mordax) collected throughout the seacoast of Okinawa, Japan and their geographic distribution. PCBs, DDTs, CHLs, PBDEs and HBCDs were detected in almost all the oyster samples analyzed and higher concentrations of PCBs, DDTs and CHLs were found in oysters from southwestern populated areas. On the other hand, HBCDs in oysters showed similar levels throughout Okinawa and the highest concentration in a northern rural site with less human and industrial activities, although oyster concentrations of PBDEs were relatively lower. When POPs in expanded polystyrene (EPS) buoys and polystyrene foam debris floated and drifted on coastal seawater were analyzed, extremely high concentrations of HBCDs were detected in some of these EPS buoys and polystyrene foam debris but other POPs were below the limit of detection in all the samples. To evaluate the specific exposure route of HBCDs for oysters, we further analyzed HBCD diastereomers, and PCB congeners by way of comparison, in seawater and sediment samples collected at an urban site and a rural site and estimated their biota (oyster)-sediment accumulation factors (BSAF) and bioaccumulation factors (BAF). Interestingly, the highest log BAF values were found for α-HBCD despite its lower log Kow than those of γ-HBCD and PCB congeners, although log BSAF values for HBCDs were lower than those for PCBs. Considering that α-HBCD was detected in a few polystyrene foam samples as the predominant diastereomer, oysters inhabiting the coastal region of Okinawa might be frequently exposed to micronized polystyrene foam particles containing HBCDs.
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http://dx.doi.org/10.1016/j.scitotenv.2020.140049DOI Listing
October 2020

Altered hepatic cytochrome P450 expression in cats after chronic exposure to decabromodiphenyl ether (BDE-209).

J Vet Med Sci 2020 Jul 21;82(7):978-982. Epub 2020 May 21.

Faculty of Veterinary Medicine, Hokkaido University, Kita 18, Nishi 9, Kita-ku, Sapporo, Hokkaido 060-0818, Japan.

The knowledge of cytochrome P450 (CYP) expression involved in chemical exposure are necessary in clinical applications for the medication and prediction of adverse effects. The aim of this study was to evaluate the mRNA expression of CYP1-CYP3 families in cats exposed to BDE-209 for one year. All selected CYP isoforms showed no significant difference in mRNA expressions between control and exposure groups, however, CYP3A12 and CYP3A131 revealed tend to be two times higher in the exposure group compared to control group. The present results indicate that the chronic exposure of BDE209 could not alter CYP expression in the liver of cats. This result considered caused by the deficiency of CYP2B subfamily which is major metabolism enzyme of polybrominated diphenyl ethers (PBDEs) in cat.
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http://dx.doi.org/10.1292/jvms.20-0140DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7399315PMC
July 2020

Nontarget and Target Screening of Organohalogen Compounds in Mussels and Sediment from Hiroshima Bay, Japan: Occurrence of Novel Bioaccumulative Substances.

Environ Sci Technol 2020 05 23;54(9):5480-5488. Epub 2020 Mar 23.

Center for Marine Environmental Studies (CMES), Ehime University, 2-5 Bunkyo-cho, Matsuyama, Ehime 790-8577, Japan.

Recent screening surveys have shown the presence of unknown halogenated compounds in the marine environment at comparable levels to persistent organic pollutants (POPs). However, their exposure levels and profiles in marine organisms and bioaccumulative potentials remain unclear. The present study performed nontarget/target screening of organohalogen compounds (OHCs) in mussel and sediment samples collected from Hiroshima Bay, Japan, in 2012 and 2018 by using integrated analyses of two-dimensional gas chromatography-high resolution time-of-flight mass spectrometry (GC×GC-HRToFMS) and magnetic sector GC-HRMS. Nontarget analysis by GC×GC-HRToFMS revealed the detection of approximately 60 OHCs including unknown mixed halogenated compounds (UHC-BrCl) with molecular formulae of CHBrClO, CHBrClO, and CHBrClO in the mussel. Interestingly, UHC-BrCl concentrations in the mussel samples, which were semi-quantified by GC-HRMS, were comparable to or higher than those of POPs at all the locations surveyed, and their geographical distribution patterns differed from those of other OHCs. These results suggest that UHC-BrCl are ubiquitous in coastal waters of Hiroshima Bay and derived from a specific source(s). The biota-sediment accumulation factors (BSAFs) of UHC-BrCl, estimated for a paired sample set of mussel (ng/g lw) and sediment (ng/g TOC), were 1 order of magnitude higher than those for POPs with similar log values, indicating their high bioaccumulative potential.
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http://dx.doi.org/10.1021/acs.est.9b06998DOI Listing
May 2020

Soil and sediment contamination by unsubstituted and methylated polycyclic aromatic hydrocarbons in an informal e-waste recycling area, northern Vietnam: Occurrence, source apportionment, and risk assessment.

Sci Total Environ 2020 Mar 5;709:135852. Epub 2019 Dec 5.

Centre for Environmental Technology and Sustainable Development (CETASD), VNU University of Science, Vietnam National University, Hanoi, 334 Nguyen Trai, Hanoi, Viet Nam. Electronic address:

Improper processing activities of e-waste are potential sources of polycylic aromatic hydrocarbons (PAHs) and their derivatives, however, information about the environmental occurrence and adverse impacts of these toxic substances is still limited for informal e-waste recycling areas in Vietnam and Southeast Asia. In this study, unsubstituted and methylated PAHs were determined in surface soil and river sediment samples collected from a rural village with informal e-waste recycling activities in northern Vietnam. Total levels of PAHs and MePAHs decreased in the order: workshop soil (median 2900; range 870-42,000 ng g) > open burning soil (2400; 840-4200 ng g) > paddy field soil (1200; range 530-6700 ng g) > river sediment samples (750; 370-2500 ng g). About 60% of the soil samples examined in this study were heavily contaminated with PAHs. Fingerprint profiles of PAHs and MePAHs in the soil and sediment samples indicated that these pollutants were mainly released from pyrogenic sources rather than petrogenic sources. The emissions of PAHs and MePAHs in this area were probably attributed to uncontrolled burning of e-waste and agricultural by-products, domestic coal and biomass combustion, and traffic activities. Carcinogenicity and mutagenicity of PAHs in the e-waste workshop soils were significantly higher than those of the field soils; however, the incremental lifetime cancer risk of PAH-contaminated soils in this study ranged from 5.5 × 10 to 4.6 × 10, implying acceptable levels of human health risk. Meanwhile, concentrations of some compounds such as phenanthrene, anthracene, fluoranthene, benz[a]anthracene, and benzo[a]pyrene in several soil samples exceeded the maximum permissible concentrations, indicating the risk of ecotoxicological effects.
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http://dx.doi.org/10.1016/j.scitotenv.2019.135852DOI Listing
March 2020

Effects of PCB exposure on serum thyroid hormone levels in dogs and cats.

Sci Total Environ 2019 Oct 23;688:1172-1183. Epub 2019 Jun 23.

Center for Marine Environmental Studies (CMES), Ehime University, Bunkyo-cho 2-5, Matsuyama, Ehime 790-8577, Japan. Electronic address:

Polychlorinated biphenyls (PCBs) and their hydroxylated metabolites (OH-PCBs) might disrupt thyroid function. However, there is no clear evidence of PCB exposure disrupting thyroid hormone (TH) homeostasis in dogs and cats. The present study conducted in vivo experiments to evaluate the effects of a mixture of 12 PCB congeners (CB18, 28, 70, 77, 99, 101, 118, 138, 153, 180, 187 and 202, each congener 0.5 mg/kg BW, i.p. administration) on serum TH levels in male dogs (Canis lupus familiaris) and male cats (Felis silvestris catus). In PCB-exposed dogs, the time courses of higher-chlorinated PCBs and L-thyroxine (T4)-like OH-PCBs (4-OH-CB107 and 4-OH-CB202) concentrations were unchanged or tended to increase, whereas those of lower-chlorinated PCBs and OH-PCBs tended to decrease after 24 h. In PCB-exposed cats, concentrations of PCBs increased until 6 h and then remained unchanged. The levels of lower-chlorinated OH-PCBs including 4'-OH-CB18 increased until 96 h and then decreased. In PCB-exposed dogs, free T4 concentrations were higher than those in the control group at 48 and 96 h after PCB administration and positively correlated with the levels of T4-like OH-PCBs, suggesting competitive binding of T4 and T4-like OH-PCBs to a TH transporter, transthyretin. Serum levels of total T4 and total 3,3',5-triiodo-L-thyronine (T3) in PCB-exposed dogs were lower than in the control group at 24 and 48 h and negatively correlated with PCB concentrations, implying that PCB exposure enhanced TH excretion by increasing TH uptake and TH conjugation enzyme activities in the dog liver. In contrast, no obvious changes in TH levels were observed in PCB-exposed cats. This could be explained by the lower levels of T4-like OH-PCBs and lower hepatic conjugation enzyme activities in cats compared with dogs. Different effects on serum TH levels in PCB-exposed dogs and cats are likely to be attributable to species-specific PCB and TH metabolism.
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http://dx.doi.org/10.1016/j.scitotenv.2019.06.300DOI Listing
October 2019

Tissue distribution and characterization of feline cytochrome P450 genes related to polychlorinated biphenyl exposure.

Comp Biochem Physiol C Toxicol Pharmacol 2019 Dec 2;226:108613. Epub 2019 Sep 2.

Faculty of Veterinary Medicine, Graduate School of Veterinary Medicine, Hokkaido University, Kita 18, Nishi 9, Kita-ku, Sapporo, Hokkaido 060-0818, Japan. Electronic address:

Cats have been known to be extremely sensitive to chemical exposures. To understand these model species' sensitivity to chemicals and their toxicities, the expression profiles of xenobiotic-metabolizing enzymes should be studied. Unfortunately, the characterization of cytochrome P450 (CYP), the dominant enzyme in phase I metabolism, in cats has not extensively been studied. Polychlorinated biphenyls (PCBs) are known as CYP inducers in animals, but the information regarding the PCB-induced CYP expression in cats is limited. Therefore, in the present study, we aimed to elucidate the mRNA expression of the CYP1-CYP3 families in the cat tissues and to investigate the CYP mRNA expression related to PCB exposure. In cats, the greatest abundance of CYP1-CYP3 (CYP1A2, CYP2A13, CYP2C41, CYP2D6, CYP2E1, CYP2E2, CYP2F2, CYP2F5, CYP2J2, CYP2U1, and CYP3A132) was expressed in the liver, but some extrahepatic isozymes were found in the kidney (CYP1A1), heart (CYP1B1), lung (CYP2B11 and CYP2S1) and small intestine (CYP3A131). In cats, CYP1A1, CYP1A2 and CYP1B1 were significantly upregulated in the liver as well as in several tissues exposed to PCBs, indicating that these CYPs were distinctly induced by PCBs. The strong correlations between 3,3',4,4'-tetrachlorobiphenyl (CB77) and CYP1A1 and CYP1B1 mRNA expressions were noted, demonstrating that CB77 could be a potent CYP1 inducer. In addition, these CYP isoforms could play an essential role in the PCBs biotransformation, particularly 3-4 Cl-PCBs, because a high hydroxylated metabolite level of 3-4 Cl-OH-PCBs was observed in the liver.
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http://dx.doi.org/10.1016/j.cbpc.2019.108613DOI Listing
December 2019

Targeted metabolome analysis of the dog brain exposed to PCBs suggests inhibition of oxidative phosphorylation by hydroxylated PCBs.

Toxicol Appl Pharmacol 2019 08 10;377:114620. Epub 2019 Jun 10.

Center for Marine Environmental Studies (CMES), Ehime University, Bunkyo-cho 2-5, Matsuyama, Ehime 790-8577, Japan.

Canis lupus familiaris (domestic dog) possess a high capacity to metabolize higher-chlorinated polychlorinated biphenyls (PCBs) to thyroid hormone (TH)-like hydroxylated PCB metabolites (OH-PCBs). As a result, the brain could be at high risk of toxicity caused by OH-PCBs. To evaluate the effect of OH-PCBs on dog brain, we analyzed OH-PCB levels in the brain and the metabolome of the frontal cortex following exposure to a mixture of PCBs (CB18, 28, 70, 77, 99, 101, 118, 138, 153, 180, 187, and 202). 4-OH-CB202 and 4-OH-CB107 were major OH-PCBs in the brain of PCB-exposed dogs. These OH-PCBs were associated with metabolites involved in urea cycle, proline-related compounds, and purine, pyrimidine, glutathione, and amino-acid metabolism in dog brain. Moreover, adenosine triphosphate levels in the PCBs exposure group were significantly lower than in the control group. These results suggest that OH-PCB exposure is associated with a disruption in TH homeostasis, generation of reactive oxygen species, and/or disruption of oxidative phosphorylation (OXPHOS) in brain cells. Among them, OXPHOS disturbance could be associated with both disruptions in cellular amino-acid metabolism and urea cycle. Therefore, an OXPHOS activity assay was performed to evaluate the disruption of OXPHOS by OH-PCBs. The results indicated that 4-OH-CB107 inhibits the function of Complexes III, IV, and V of the electron transport chain, suggesting that 4-OH-CB107 inhibit these complexes in OXPHOS. The neurotoxic effects of PCB exposure may be mediated through mitochondrial toxicity of OH-PCBs in the brain.
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http://dx.doi.org/10.1016/j.taap.2019.114620DOI Listing
August 2019

Complex Mixtures of Brominated/Chlorinated Diphenyl Ethers and Dibenzofurans in Soils from the Agbogbloshie e-Waste Site (Ghana): Occurrence, Formation, and Exposure Implications.

Environ Sci Technol 2019 03 1;53(6):3010-3017. Epub 2019 Mar 1.

Center for Marine Environmental Studies (CMES) , Ehime University , 2-5 Bunkyo-cho , Matsuyama 790-8577 , Japan.

The distribution and toxic equivalents (TEQs) of brominated and chlorinated dibenzo- p-dioxins/dibenzofurans (PBDD/Fs and PCDD/Fs) in soils from Agbogbloshie e-waste site (Ghana) were investigated. The composition of brominated/chlorinated dibenzofurans (PXDFs) and diphenyl ethers (PBDEs, PCDEs, and PXDEs) was examined using two-dimensional gas chromatography-time-of-flight mass spectrometry to elucidate possible formation pathways of dioxins from e-waste recycling. The highest concentrations of PCDD/Fs and PBDD/Fs were found, respectively, in the open burning (1.3-380 ng/g dry weight) and dismantling areas (11-1000 ng/g dry weight) and were comparable to the highest reported for informal e-waste sites. PXDFs and PXDEs were detected at up to the range of hundreds of nanograms per gram. The homologue profiles suggest that PXDFs were formed mainly from PBDFs through successive Br-to-Cl exchange. However, monobromo-PCDFs were also derived from de-novo-generated PCDFs in open burning areas. PBDFs contributed similar or higher TEQs (7.9-5400 pg/g dry weight) compared with PCDD/Fs (6.8-5200 pg/g dry weight), whereas PXDFs were also substantial TEQ contributors in open burning areas. The high TEQs of PBDFs in the dismantling area (120-5200 pg/g dry weight) indicate the need to consider brominated dioxins besides chlorinated dioxins in future studies on health implications for e-waste workers and local residents.
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http://dx.doi.org/10.1021/acs.est.8b06929DOI Listing
March 2019

Protecting the environment from psychoactive drugs: Problems for regulators illustrated by the possible effects of tramadol on fish behaviour.

Sci Total Environ 2019 May 6;664:915-926. Epub 2019 Feb 6.

Institute of Environment, Health and Societies, Brunel University London, Uxbridge, Middlesex, UB8 3PH, United Kingdom.

There is concern that psychoactive drugs present in the aquatic environment could affect the behaviour of fish, and other organisms, adversely. There is considerable experimental support for this concern, although the literature is not consistent. To investigate why, fish were exposed to three concentrations of the synthetic opiate tramadol for 23-24 days, and their anxiolytic behaviour in a novel tank diving test was assessed both before and after exposure. The results were difficult to interpret. The positive control drug, the anti-depressant fluoxetine, produced the expected results: exposed fish explored the novel tank more, and swam more slowly while doing so. An initial statistical analysis of the results provided relatively weak support for the conclusion that both the low and high concentrations of tramadol affected fish behaviour, but no evidence that the intermediate concentration did. To gain further insight, UK and Japanese experts in ecotoxicology were asked for their independent opinions on the data for tramadol. These were highly valuable. For example, about half the experts replied that a low concentration of a chemical can cause effects that higher concentrations do not, although a similar number did not believe this was possible. Based both on the inconclusive effects of tramadol on the behaviour of the fish and the very varied opinions of experts on the correct interpretation of those inconclusive data, it is obvious that more research on the behavioural effects of tramadol, and probably all other psychoactive drugs, on aquatic organisms is required before any meaningful risk assessments can be conducted. The relevance of these findings may apply much more widely than just the environmental risk assessment of psychoactive drugs. They suggest that much more rigorous training of research scientists and regulators is probably required if consensus decisions are to be reached that adequately protect the environment from chemicals.
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http://dx.doi.org/10.1016/j.scitotenv.2019.02.090DOI Listing
May 2019

Evaluation of a data-processing method for target and non-target screening using comprehensive two-dimensional gas chromatography coupled with high-resolution time-of-flight mass spectrometry for environmental samples.

Talanta 2019 Mar 17;194:461-468. Epub 2018 Oct 17.

Center for Marine Environmental Studies (CMES), Ehime University, 2-5 Bunkyo-cho, Matsuyama-shi, Ehime 790-8577, Japan.

We evaluated the possibility of semi-automatic target and non-target screening by comprehensive two-dimensional gas chromatography coupled with high-resolution time-of-flight mass spectrometry (GC×GC-HRToFMS) by using estuarine sediment samples. Two-way screening consisting of compound-based (target screening) and data-based (non-target screening) analyses was performed by using two original software programs, including mass-spectral deconvolution software based on non-negative matrix factorization, the NIST Mass Spectral Library, and an in-house accurate mass spectral library with a retention index (RI) for the 1st column. Target screening detected 47 organohalogen compounds, including polychlorinated biphenyls, polybrominated diphenyl ethers and organochlorine pesticides, in the sediment sample. Among about 54,000 peaks detected in the non-target screening, 53.6% showed match factors (MF) of ≥ 700 in an automatic mass spectral library search using the peak-top mass spectra. Both mass error of molecular ions and RI error were calculated automatically for the first-hit compounds in the library search; 0.03% of peaks passed all criteria, namely MF ≥ 700, mass error ≤± 20 ppm, RI error ≤ ± 20, and intensity of molecular ion ≥ 10,000. Two compounds-a phosphorus flame retardant and a brominated phenol-were tentatively identified in the non-target screening process. The advantages of semi-automatic GC×GC-HRToFMS data processing with the two original software programs is its simplicity, high reproducibility, and shortened time for processing a large volume data. The results suggest that an In-source HiRes search-i.e. library matching using accurate mass spectra-is useful and could be applied for non-target screening using high-resolution MS in the future.
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http://dx.doi.org/10.1016/j.talanta.2018.10.050DOI Listing
March 2019

Occurrence of benzotriazole ultraviolet stabilizers (BUVSs) in human breast milk from three Asian countries.

Sci Total Environ 2019 Mar 22;655:1081-1088. Epub 2018 Nov 22.

Center for Health and Environmental Risk Research, National Institute for Environmental Studies. Electronic address:

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
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http://dx.doi.org/10.1016/j.scitotenv.2018.11.298DOI Listing
March 2019

Seasonal variation of atmospheric organochlorine pesticides and polybrominated diphenyl ethers in Parangipettai, Tamil Nadu, India: Implication for atmospheric transport.

Sci Total Environ 2019 Feb 3;649:1653-1660. Epub 2018 Aug 3.

Lancaster Environmental Centre, Lancaster University, LA1 4YQ Lancaster, UK.

Past studies have reported several persistent organic pollutants (POPs) in different environmental matrices from a tropical coastal site, Parangipettai (PI), located along the bank of the Vellar River in Tamil Nadu, south India. Hence to fill the data gap after the strict ban on several POPs, high volume air sampling was conducted in PI to study the variability of atmospheric organochlorine pesticides (OCPs) and polybrominated diphenyl ethers (PBDEs) during summer, pre-monsoon and monsoon seasons. Emission source regions were tracked by using five days back trajectory analysis. Range of air concentrations in pg/m were: dichlorodiphenyltrichloroethane (DDT), 13 - 1976; hexachlorocyclohexane (HCH), 260-1135, hexachlorocyclobenzene (HCB), 52-135, chlordanes, 36-135 and endosulfans, 66-1013. Six PBDE congeners ranged between 25 and 155 pg/m with the highest concentration in summer followed by pre-monsoon and monsoon. Atmospheric DDT and HCH in PI have drastically reduced from the past report thereby showing the strict ban on agricultural use of these compounds. During monsoon, fresh source of o,p'-DDT, trans-chlordane and α-endosulfan was evident. Higher level of endosulphan sulfate in PI seems to be likely affected by the air mass, originating from a neighbouring state Kerela, where endosulfan has been extensively used for cashew plantations. Similarly in summer, the day recorded with the highest level of PBDEs, the sample was concurrently impacted by air parcel comprised of two major clusters, 1 (25%) and 2 (49%) that traversed through the metropolitan cities like Bangalore and Chennai. Dominance of BDE-99 over BDE-47 in PI is in line with the PBDE profile reported from Chennai city during similar time frame. Average concentration of tetra and penta BDE congeners in summer samples were nearly 2-3 folds higher than pre-monsoon or monsoon. Given the fact that strong localised sources for heavier BDE congeners are lacking in PI, regional atmospheric transport from the strong emission source regions in Chennai might have impacted PBDE concentration in PI.
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http://dx.doi.org/10.1016/j.scitotenv.2018.07.414DOI Listing
February 2019

Alterations in urinary metabolomic profiles due to lead exposure from a lead-acid battery recycling site.

Environ Pollut 2018 Nov 26;242(Pt A):98-105. Epub 2018 Jun 26.

Center for Preventive Medical Sciences, Chiba University, Inage-ku Yayoi-cho 1-33, Chiba, 263-8522, Japan; Department of Bioenvironmental Medicine, Graduate School of Medicine, Chiba University, Chuo-ku Inohana 1-8-1, Chiba, 260-8670, Japan.

Lead poisoning is considered a public health threat, particularly in developing countries. Health problems from Pb exposure occur in many parts of the world, especially near Pb mines, Pb smelters, and used lead-acid battery (ULAB) recycling plants. In this study, we analyzed the urine metabolome of residents in a village located near a ULAB recycling facility to investigate the biological effects of Pb exposure (ULAB: n = 44, Reference: n = 51). Lasso linear regression models were moderately predictive of blood Pb levels, as evaluated by a training set (R = 0.813) and against an external test set (R = 0.647). In lasso logistic regression models, areas under receiver operating characteristic curves, as measured by 5-fold cross-validation (AUC = 0.871) and against an external test set (AUC = 0.917), indicated accurate classification of urine samples from the affected village and from a reference site. Ten candidate biomarkers identified at false discovery rates of <0.05 were associated with ATP-binding cassette (ABC) transporters, possibly related to the disruption of small-molecule transport in the kidney; amino acid, porphyrin, and chlorophyll metabolism; and the heme biosynthetic pathway. Collectively, the results suggest that lead Pb is related to the health effects in individuals residing in ULAB site by alteration of these biological pathways.
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http://dx.doi.org/10.1016/j.envpol.2018.06.071DOI Listing
November 2018

Determination of free thyroid hormones in animal serum/plasma using ultrafiltration in combination with ultra-fast liquid chromatography-tandem mass spectrometry.

J Chromatogr A 2018 Mar 31;1539:30-40. Epub 2018 Jan 31.

Center for Marine Environmental Studies (CMES), Ehime University, 2-5, Bunkyo-cho, Matsuyama, Ehime 790-8577, Japan. Electronic address:

Thyroid hormones (THs), which mainly consist of 3, 3', 5-triiodo-l-thyronine (T3) and L-thyroxine (T4), play a critical role in regulating biological processes such as growth and metabolism in various animal species. Thus, accurate measurement of T3 and T4, especially physiologically active free (protein-unbound) forms, in serum/plasma is needed for the evaluation of TH homeostasis. However, such high-precision determination of free THs is lacking for non-human species. The present study aimed to develop a highly sensitive and reliable liquid chromatography-tandem mass spectrometry (LC-MS/MS) method for the determination of six free THs in serum/plasma, which is applicable to not only humans but also non-human species. Two different physical separation steps, ultrafiltration (UF) and equilibrium dialysis (ED), were examined to obtain the free TH fraction. Several experimental conditions were carefully optimized and validated for UF or ED using the commercially available bovine serum. As a result, UF at 1100 × g and 37 °C for 30 min with a 30 kDa ultrafiltration device (Centrifree YM-30, Millipore) yielded excellent precision (CV: <10%). The optimized ED step also yielded high precision (CV: <10%) and the measurement values were approximately equal to those of UF, but at least 16 h were required to reach equilibrium. Thus, UF combined with LC-MS/MS was finally chosen, in terms of the time needed for the measurement. Acceptable accuracy (recovery: 70%-110%) and intra- and inter-day precision (CV: <10% and <12%, respectively) were obtained, when triplicate analyses in three different days were conducted using the bovine serum. The developed analytical method was successfully applied to the determination of free THs in serum/plasma samples of humans, cats, and dogs. Furthermore, comparison with free T4 concentrations measured by a common immunoassay method evidently indicated that the ultrafiltration-LC-MS/MS method developed in this study can increase the specificity and accuracy of TH measurement.
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http://dx.doi.org/10.1016/j.chroma.2018.01.044DOI Listing
March 2018

Exposure assessment of heavy metals in an e-waste processing area in northern Vietnam.

Sci Total Environ 2018 Apr 2;621:1115-1123. Epub 2017 Nov 2.

Center for Material Cycles and Waste Management Research, National Institute for Environmental Studies, Japan.

In developing countries, inappropriate recycling of e-waste has resulted in the environmental release of toxicants, including heavy metals, that may have deleterious health effects. In this study, we estimated daily metal intakes in five households in a Vietnamese village located in an e-waste processing area and assessed the health risk posed by exposure to the metals. Garden soil, floor dust, 24-h duplicate diet, and ambient air samples were collected from five households in northern Vietnam in January 2014. All samples were acid-digested, and contents of Cd, Cu, Mn, Pb, Sb, and Zn were measured by using ICP mass spectrometry and ICP atomic emission spectroscopy. In addition, the soil, dust, and diet samples were subjected to an bioaccessibility extraction test to determine bioaccessible metal concentrations. Hazard quotients were estimated from bioaccessible metal concentrations, provisional tolerable weekly intakes, and reference doses. Garden soil and floor dust were estimated to be mainly contributors to daily Pb intake, as indicated by calculations using bioaccessible metal concentrations and the U.S. Environmental Protection Agency soil plus dust ingestion rate. Diet was suggested to contribute significantly to daily Cd, Cu, Mn, Sb, and Zn intake. Estimated metal exposures via inhalation were negligible, as indicated by calculations using International Atomic Energy Agency reference inhalation rates. The maximum hazard quotients were calculated as 0.2 (Cd), 0.09 (Cu), 0.3 (Mn), 0.6 (Pb), 0.2 (Sb), and 0.5 (Zn), on the basis of bioaccessible metal concentrations. The contributions of Cd, Cu, Mn, Sb, and Zn except Pb to potential noncancer risk for adult residents of the five households in the e-waste processing area may be low.
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http://dx.doi.org/10.1016/j.scitotenv.2017.10.115DOI Listing
April 2018

Uptake and Metabolism of Human Pharmaceuticals by Fish: A Case Study with the Opioid Analgesic Tramadol.

Environ Sci Technol 2017 Nov 19;51(21):12825-12835. Epub 2017 Oct 19.

Institute of Environment, Health and Societies, Brunel University , Uxbridge, Middlesex, London UB8 3PH, United Kingdom.

Recent species-extrapolation approaches to the prediction of the potential effects of pharmaceuticals present in the environment on wild fish are based on the assumption that pharmacokinetics and metabolism in humans and fish are comparable. To test this hypothesis, we exposed fathead minnows to the opiate pro-drug tramadol and examined uptake from the water into the blood and brain and the metabolism of the drug into its main metabolites. We found that plasma concentrations could be predicted reasonably accurately based on the lipophilicity of the drug once the pH of the water was taken into account. The concentrations of the drug and its main metabolites were higher in the brain than in the plasma, and the observed brain and plasma concentration ratios were within the range of values reported in mammalian species. This fish species was able to metabolize the pro-drug tramadol into the highly active metabolite O-desmethyl tramadol and the inactive metabolite N-desmethyl tramadol in a similar manner to that of mammals. However, we found that concentration ratios of O-desmethyl tramadol to tramadol were lower in the fish than values in most humans administered the drug. Our pharmacokinetic data of tramadol in fish help bridge the gap between widely available mammalian pharmacological data and potential effects on aquatic organisms and highlight the importance of understanding drug uptake and metabolism in fish to enable the full implementation of predictive toxicology approaches.
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http://dx.doi.org/10.1021/acs.est.7b03441DOI Listing
November 2017

Occurrence of Natural Mixed Halogenated Dibenzo-p-Dioxins: Specific Distribution and Profiles in Mussels from Seto Inland Sea, Japan.

Environ Sci Technol 2017 Oct 29;51(20):11771-11779. Epub 2017 Sep 29.

Center for Marine Environmental Studies (CMES), Ehime University , 2-5 Bunkyo-cho, Matsuyama, Ehime 790-8577, Japan.

In addition to unintentional formation of polychlorinated (PCDD/Fs), polybrominated (PBDD/Fs), and mixed halogenated (PXDD/Fs) dibenzo-p-dioxins/dibenzofurans during industrial activities, recent studies have shown that several PBDD and PXDD congeners can be produced by marine algal species from the coastal environment. However, multiple exposure status of anthropogenic and naturally derived dioxins in marine organisms remains unclear. The present study examined the occurrence, geographical distribution, and potential sources of PCDD/Fs, PBDD/Fs, and PXDD/Fs using mussels and brown algae collected in 2012 from Seto Inland Sea, Japan. The results showed the widespread occurrence of not only PCDD/Fs but also PBDDs and PXDDs in Seto Inland Sea. The geographical distribution pattern of PBDDs was similar to that of PXDDs, which were obviously different from that of PCDDs and PCDFs, and a significant positive correlation was observed between the levels of their predominant congeners, i.e., 1,3,7-/1,3,8-TrBDDs and DiBMoCDDs. Interestingly, potential precursors of 1,3,7-/1,3,8-TrBDDs and DiBMoCDDs, hydroxylated tetrabrominated diphenyl ethers (6-HO-BDE-47 and 2'-HO-BDE-68) and their mixed halogenated analogue (HO-TrBMoCDE), were also identified in the mussel and brown alga samples collected at the same site, by comprehensive two-dimensional gas chromatography with time-of-flight mass spectrometry (GC × GC-ToFMS) analyses. It is noteworthy that residue levels of 1,3,7-/1,3,8-TrBDDs and DiBMoCDDs in the mussel were 30 times higher than those in the brown alga, suggesting the bioaccumulation of these natural dioxins.
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http://dx.doi.org/10.1021/acs.est.7b03738DOI Listing
October 2017

Anthropogenic and Naturally Produced Brominated Phenols in Pet Blood and Pet Food in Japan.

Environ Sci Technol 2017 Oct 13;51(19):11354-11362. Epub 2017 Sep 13.

Center for Marine Environmental Studies (CMES), Ehime University , Bunkyo-cho 2-5, Matsuyama, Ehime 790-8577, Japan.

Present study determined concentrations and residue patterns of bromophenols (BPhs) in whole blood samples of pet cats and pet dogs collected from veterinary hospitals in Japan. BPhs concentrations were higher in cat blood than in dog blood, with statistically insignificant differences (p = 0.07). Among the congeners, 2,4,6-tribromophenol (TBPh) constituted the majority of BPhs (>90%) detected in both species. Analysis of commercial pet food to estimate exposure routes showed that the most abundant congener in all pet food samples was 2,4,6-TBPh, accounting for >99% of total BPhs. This profile is quite similar to the blood samples of the pets, suggesting that diet might be an important exposure route for BPhs in pets. After incubation in polybrominated diphenyl ether (PBDE) mixtures (BDE-47, BDE-99 and BDE-209), 2,4,5-TBPh was found in dog liver microsomes but not in cat liver microsomes, implying species-specific metabolic capacities for PBDEs. Formation of 2,4,5-TBPh occurred by hydroxylation at the 1' carbon atom of the ether bond of BDE-99 is similar to human study reported previously. Hydroxylated PBDEs were not detected in cats or dogs; therefore, diphenyl ether bond cleavage of PBDEs can also be an important metabolic pathway for BPhs formation in cats and dogs.
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http://dx.doi.org/10.1021/acs.est.7b01009DOI Listing
October 2017

Lead exposure in raptors from Japan and source identification using Pb stable isotope ratios.

Chemosphere 2017 Nov 28;186:367-373. Epub 2017 Jul 28.

Laboratory of Toxicology, Department of Environmental Veterinary Sciences, Graduate School of Veterinary Medicine, Hokkaido University, Kita18, Nishi9, Kita-ku, Sapporo, Hokkaido, 060-0818, Japan. Electronic address:

Lead (Pb) poisoning is widespread among raptors and water birds. In Japan, fragments of Pb ammunition are still found in endangered eagles although more than 10 years have passed since legislation regarding use of Pb ammunition was introduced. This study was performed to investigate Pb exposure in raptors from various locations in Japan. We measured hepatic and renal Pb concentrations and hepatic Pb isotope ratios of Steller's sea eagles (Haliaeetus pelagicus), white-tailed sea eagles (Haliaeetus albicilla), golden eagles (Aquila chrysaetos), and 13 other species (total 177 individuals) that were found dead, as well as blood samples from three eagles found in a weakened state during 1993-2015 from Hokkaido (northern part), Honshu (the main island), and Shikoku (a southern island) of Japan. In the present study in Hokkaido, one quarter of the sea eagles showed a high Pb concentration, suggesting exposure to abnormally high Pb levels and Pb poisoning. Pb isotope ratios indicated that endangered Steller's sea eagle and white-tailed sea eagle were poisoned by Pb ammunition that was used illegally in Hokkaido. In other areas of Japan, both surveillance and regulations were less extensive than in Hokkaido, but Pb poisoning in raptors was also noted. Therefore, Pb poisoning is still a serious problem in raptors in various areas of Japan due to accidental ingestion of materials containing Pb, especially Pb ammunition.
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http://dx.doi.org/10.1016/j.chemosphere.2017.07.143DOI Listing
November 2017

Spatio-temporal trends of polybrominated dibenzo-p-dioxins and dibenzofurans in archived sediments from Tokyo Bay, Japan.

Sci Total Environ 2017 Dec 4;599-600:340-347. Epub 2017 May 4.

Center for Marine Environmental Studies (CMES), Ehime University, Bunkyo-cho 2-5, Matsuyama 790-8577, Japan. Electronic address:

The present study examined the occurrence and potential sources of mono- to octa-brominated dibenzo-p-dioxins/dibenzofurans (Mo-OBDD/Fs) in Tokyo Bay, Japan, using surface sediments and Pb-dated sediment cores (covering the period 1895-2000) collected in 2002. The results showed a clear difference in the spatio-temporal trend between PBDFs and PBDDs. The spatial distribution of PBDF concentrations in the surface sediments showed a decreasing trend from the head to the mouth of the bay, which was similar to that of polybrominated diphenyl ethers (PBDEs) reported previously for the same sediment samples. In the sediment cores, PBDF and PBDE concentrations increased drastically after the 1960s and reached the highest levels in the late 1990s. In addition, a significant positive correlation was observed between the concentrations of their predominant congeners, 1,2,3,4,6,7,8-HpBDF and BDE-209. These results indicate that main contamination sources of PBDFs were technical PBDE formulations, especially DecaBDE. In contrast, total PBDDs in the surface sediments were rather uniform in the whole area of the bay. Furthermore, in the sediment cores, PBDD levels showed marginal fluctuation over the past century, with the predominance of 2,7-/2,8-DiBDDs and 1,3,7-/1,3,8-TrBDDs in all the sediment layers. It is noteworthy that these PBDD congeners were also found in the sediment layers corresponding to the pre-industrial era, supporting their natural formation in the coastal environment.
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http://dx.doi.org/10.1016/j.scitotenv.2017.04.166DOI Listing
December 2017

Uridine Diphosphate-Glucuronosyltransferase (UGT) 2B Subfamily Interspecies Differences in Carnivores.

Toxicol Sci 2017 07;158(1):90-100

Laboratory of Toxicology, Department of Environmental Veterinary Science, Graduate School of Veterinary Medicine, Hokkaido University, N18, W9, Kita-ku, Sapporo 060-0818, Japan.

UDP-glucuronosyltransferases (UGTs) are among the most important xenobiotic metabolizing enzymes that conjugate a wide range of chemicals. Previous studies showed that Felidae and Pinnipedia species have very low UGT activities toward some phenolic compounds because of the UGT1A6 pseudogene and small numbers of UGT1A isozymes. In addition to the UGT1As, UGT2Bs isozymes also conjugate various endogenous (eg, estrogens, androgens, and bile acids) and exogenous compounds (opioids, non-steroidal anti-inflammatory drugs, and environmental pollutants). However UGT2B activity and genetic background are unknown in carnivore species. Therefore, this study was performed to elucidate the species differences of UGT2Bs. Using typical substrates for UGT2Bs, UGT activity was measured in vitro. In addition, UGT2B genetic features are analyzed in silico. Results of UGT activity measurement indicate marked species differences between dogs and other carnivores (cats, Northern fur seals, Steller sea lions, Harbor seals, and Caspian seals). Dogs have very high Vmax/Km toward estradiol (17-glucuronide), estrone, lorazepam, oxazepam, and temazepam. Conversely, cats and pinniped species (especially Caspian seals and Harbor seals) have very low activities toward these substrates. The results of genetic synteny analysis indicate that Felidae and pinniped species have very small numbers of UGT2B isozymes (one or none) compared with dogs, rodents, and humans. Furthermore, Felidae species have the same nonsense mutation in UGT2B, which suggests that Felidae UGT2B31-like is also a pseudogene in addition to UGT1A6. These findings of lower activity of UGT2B suggest that Felidae and some pinniped species have very low UGT activity toward a wide range of chemicals. These results are important for Felidae and Pinnipedia species that are frequently exposed to drugs and environmental pollutants.
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http://dx.doi.org/10.1093/toxsci/kfx072DOI Listing
July 2017

Species- and Tissue-Specific Profiles of Polybrominated Diphenyl Ethers and Their Hydroxylated and Methoxylated Derivatives in Cats and Dogs.

Environ Sci Technol 2017 May 2;51(10):5811-5819. Epub 2017 May 2.

Center for Marine Environmental Studies (CMES), Ehime University , Bunkyo-cho 2-5, Matsuyama, Ehime 790-8577, Japan.

The adverse effects of elevated polybrominated diphenyl ether (PBDE) levels, reported in the blood of domestic dogs and cats, are considered to be of great concern. However, the tissue distribution of PBDEs and their derivatives in these animals is poorly understood. This study determined the concentrations and profiles of PBDEs, hydroxylated PBDEs (OH-PBDEs), methoxylated PBDEs (MeO-PBDEs), and 2,4,6-tribromophenol (2,4,6-tri-BPh) in the blood, livers, bile, and brains of dogs and cats in Japan. Higher tissue concentrations of PBDEs were found in cats, with the dominant congener being BDE209. BDE207 was also predominant in cat tissues, indicating that BDE207 was formed via BDE209 debromination. BDE47 was the dominant congener in dog bile, implying a species-specific excretory capacity of the liver. OH-PBDE and MeO-PBDE concentrations were several orders of magnitude higher in cat tissues, with the dominant congener being 6OH-BDE47, possibly owing to their intake of naturally occurring MeO-PBDEs in food, MeO-PBDE demethylation in the liver, and lack of UDP-glucuronosyltransferase, UGT1A6. Relatively high concentrations of BDE209, BDE207, 6OH-BDE47, 2'MeO-BDE68, and 2,4,6-tri-BPh were found in cat brains, suggesting a passage through the blood-brain barrier. Thus, cats in Japan might be at a high risk from PBDEs and their derivatives, particularly BDE209 and 6OH-BDE47.
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http://dx.doi.org/10.1021/acs.est.7b01262DOI Listing
May 2017