TAKAHASHI, Shin

Researcher Information

Degree

• Ph.D.（Ehime University）

URL

http://keisoku.deca.jp/

J-Global ID

• 200901040861693074

Profile

• Dr. Shin Takahashi is currently Professor of Ehime University, Center of Advanced Technology for the Environment, Faculty of Agriculture. He was a former researcher of Research Center for Material Cycles and Waste Management, National Institute for Environmental Studies (NIES). Ph.D. in Environmental Chemistry. Current special fields are environmental chemistry and ecotoxicology on persistent toxic substances including POPs, dioxin-related compounds, organometallics and endocrine-disrupting chemicals. Major research interests are related to elucidate global contamination and fate of persistent toxic substances and to assess their potential risk and emission behavior during material cycling processes. He is a member of the advisory committee for the waste management policy of the Ministry of Environment, Japan, and a member of the editorial board of the Japan Society of Environmental Chemistry.

Research Interests

• 深海生態系   海洋汚染   アジア-太平洋地域   途上国   e-waste   電子・電気機器廃棄物   資源循環   廃棄物処理   内分泌撹乱   毒性影響   リスク評価   環境動態   生物濃縮   有機スズ化合物   臭素系難燃剤   DDT   PCB   ダイオキシン類   有機ハロゲン化合物   微量元素   有機金属   重金属   残留性有機汚染物質   Deep-Sea Ecosystem   Marine Pollution   Asia-Pacific Region   Developing Countries   E-waste   Waste Electrical and Electronic Equipment   Material Recycle   Waste Treatment   Endocrine Disruption   Toxic Impact   Risk Assessment   Environmental Behavior   Bioconcentration   Organotin Compounds   Brominated Flame Retardants   DDT   PCB   Dioxin-Related Compounds   Organohalogen Compounds   Trace elements   Organometallic Compounds   Heavy metals   Persistent Organic Pollutants   

Research Areas

• Environmental science/Agricultural science / Environmental effects of chemicals

Academic & Professional Experience

• 2018/01 - Today  Ehime UniversityGraduate School of AgricultureProfessor
• 2016/04 - 2017/12  Ehime UniversityGraduate School of AgricultureAssociate Professor
• 2012/12 - 2016/03  Ehime UniversityFaculty of AgricultureAssociate Professor
• 2005/04 - 2012/11  Ehime UniversityCenter for Marine Environmental StudiesAssociate Professor
• 2002/09 - 2005/03  National Institute for Environmental StudiesCenter for Material Cycles and Waster Management ResearchResearcher
• 2000/04 - 2002/09  Ehime UniversityCenter for Marine Environmental StudiesJSPS PD fellow

Education

•        - 2000  Ehime University  連合農学研究科  生物環境保全学
•        - 2000  Ehime University  Graduate School, Division of Agricltural Sciences  Life Environmental Conservation
•        - 1997  Ehime University  農学研究科  生物生存環境学
•        - 1997  Ehime University  Graduate School, Division of Agriculture  Eco-Environmental Science
•        - 1995  Hirosaki University  理学部  地球科学科
•        - 1995  Hirosaki University  Faculty of Science  Geoscience

Association Memberships

• Japan Society on Water Environment   American Chemical Society   廃棄物資源循環学会   日本内分泌撹乱化学物質学会   日本環境毒性学会   日本環境化学会   (社）環境科学会   SETAC Asia-Pacific   

Published Papers

• Antibiotics in surface water of East and Southeast Asian countries: A focused review on contamination status, pollution sources, potential risks, and future perspectives.

  Hoang Quoc Anh, Thi Phuong Quynh Le, Nhu Da Le, Xi Xi Lu, Thi Thuy Duong, Josette Garnier, Emma Rochelle-Newall, Shurong Zhang, Neung-Hwan Oh, Chantha Oeurng, Chaiwat Ekkawatpanit, Tien Dat Nguyen, Quang Trung Nguyen, Tran Dung Nguyen, Trong Nghia Nguyen, Thi Lieu Tran, Tatsuya Kunisue, Rumi Tanoue, Shin Takahashi, Tu Binh Minh, Huu Tuyen Le, Thi Ngoc Mai Pham, Thi Anh Huong Nguyen

  The Science of the total environment 764 142865 - 142865 2021/04 [Peer-reviewed]
   Scientific journal 

  This review provides focused insights into the contamination status, sources, and ecological risks associated with multiple classes of antibiotics in surface water from the East and Southeast Asia based on publications over the period 2007 to 2020. Antibiotics are ubiquitous in surface water of these countries with concentrations ranging from <1 ng/L to hundreds μg/L and median values from 10 to 100 ng/L. Wider ranges and higher maximum concentrations of certain antibiotics were found in surface water of the East Asian countries like China and South Korea than in the Southeast Asian nations. Environmental behavior and fate of antibiotics in surface water is discussed. The reviewed occurrence of antibiotics in their sources suggests that effluent from wastewater treatment plants, wastewater from aquaculture and livestock production activities, and untreated urban sewage are principal sources of antibiotics in surface water. Ecological risks associated with antibiotic residues were estimated for aquatic organisms and the prevalence of antibiotic resistance genes and antibiotic-resistant bacteria were reviewed. Such findings underline the need for synergistic efforts from scientists, engineers, policy makers, government managers, entrepreneurs, and communities to manage and reduce the burden of antibiotics and antibiotic resistance in water bodies of East and Southeast Asian countries.
• Inhalation bioaccessibility and health risk assessment of flame retardants in indoor dust from Vietnamese e-waste-dismantling workshops.

  Tatiya Wannomai, Hidenori Matsukami, Natsuyo Uchida, Fumitake Takahashi, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Tatsuya Kunisue, Go Suzuki

  The Science of the total environment 760 143862 - 143862 2021/03 Scientific journal 

  Although bioaccessibility testing is applied worldwide for appropriate chemical risk assessment, few studies have focused on the bioaccessibility of flame retardants (FRs), especially inhalation exposure. This study assessed inhalation exposure to FRs in indoor dust by workers at e-waste-dismantling workshops in northern Vietnam, by using modified simulated epithelial lung fluid (SELF) and artificial lysosomal fluid (ALF). The average mass concentrations of FRs were 130,000 ng/g for workplace dust (n = 3), 140,000 ng/g for floor dust (n = 3), and 74,000 ng/g for settled dust (n = 2), whereas the average bioaccessible concentrations of FRs were 1900, 1400, and 270 ng/g in the SELF condition and 2600, 770, and 490 ng/g in the ALF condition, respectively. Results clearly indicate that the bioaccessible concentrations of FRs are markedly lower than their mass concentrations. Tris(2-chloroethyl) phosphate (TCEP, ~19%), tris(2-chloroisopropyl) phosphate (TCIPP, ~35%), and tris(1,3-dichloroisopropyl) phosphate (TDCIPP, ~22%) showed comparably high bioaccessibility in both SELF and ALF conditions. In contrast, the bioaccessibility of tetrabromobisphenol A (TBBPA, ~20%) was high in the SELF condition, but not in the ALF condition. With regard to the test compounds' physicochemical properties, the inhalation bioaccessibility of FRs in both conditions increased as molecular weight or octanol-water partition coefficient decreased, and it decreased as water solubility decreased. Health risk assessment clearly indicated that the hazard quotient of FRs via inhalation exposure for workers in the e-waste-dismantling workshops was less than 1, suggesting that the inhalation exposure to FRs during indoor dismantling of e-waste at this site was negligible based on the current methodology of non-cancer health risk assessment used in this study.
• Contamination levels and temporal trends of legacy and current-use brominated flame retardants in a dated sediment core from Beppu Bay, southwestern Japan.

  Anh Quoc Hoang, Daichi Aono, Isao Watanabe, Michinobu Kuwae, Tatsuya Kunisue, Shin Takahashi

  Chemosphere 266 129180 - 129180 2021/03 Scientific journal 

  Contamination levels and temporal trends of polybrominated diphenyl ethers (PBDEs) and some alternative brominated flame retardants (BFRs) were examined in a dated sediment core from the deepest part of the Beppu Bay, southwestern Japan. PBDEs were found in the upper layers of 0-15 cm depth at concentrations ranging from 5200 to 32,600 pg g-1 with the peak estimated at 1995. Decabromodiphenyl ether (BDE-209) was the most abundant congener, accounting for 96% in average of total PBDEs. The vertical profile of BDE-209 observed in our sediment core generally agreed with the historical pattern of domestic demand of commercial deca-BDE mixtures in Japan, and perfectly matched with maximum stock of these products (i.e., 42,000 tons in 1995). Among alternative BFRs, only decabromodiphenyl ethane (DBDPE), a replacement of deca-BDE, was found at significant levels with concentrations of 69-850 pg g-1 in sediment layers dated between 1991 and 2011. Ratios of DBDPE to BDE-209 gradually increased during this period, implying opposite trends of these two compounds and the role of DBDPE as a deca-BDE's alternative. The occurrence of deca-BDE components in sediments may pose medium risk to benthic aquatic life, while the ecological risk of other PBDE homologs and DBDPE was negligible.
• Polybrominated diphenyl ethers in indoor and outdoor dust from Southeast Asia: An updated review on contamination status, human exposure, and future perspectives.

  Anh Quoc Hoang, Tri Manh Tran, Minh Binh Tu, Shin Takahashi

  Environmental pollution 272 116012 - 116012 2021/03 [Peer-reviewed]
   Scientific journal 

  Contamination status, potential emission sources, environmental fate, and human exposure risk of polybrominated diphenyl ethers (PBDEs) are reviewed for indoor and outdoor dust from Southeast Asian countries, under an international comparison point of view. PBDEs have been widely detected in house, workplace, car, and road dust samples collected from Indonesia, Philippines, Singapore, Thailand, and Vietnam. The highest PBDE levels up to hundreds of μg/g were found in settled dust from some e-waste processing areas in Thailand and Vietnam. Concentrations of PBDEs in house, car, and road dust from this region were generally lower than those reported in China and Western developed countries. BDE-209 was the most predominant congener in almost all analyzed samples, reflecting the widespread application of materials and products treated with commercial deca-BDE mixtures in this region. The market demand and application rate of commercial PBDE mixtures in Southeast Asia were lower than those documented for other regions in the world. As a result, PBDE contamination levels in the environments (e.g., indoor and outdoor dust) and associated risks in these countries were not significantly high. However, more attention should be paid to informal processing activities and management strategies for modern wastes such as e-waste, plastics, and end-of-life vehicles. There exist several knowledge gaps about spatiotemporal trends, potential sources, risk assessment, inventory, management, and legislation regarding PBDEs in dust from this region, which should be filled by additional comprehensive, detailed studies with relevant inter-country/regional monitoring schemes.
• Extractable organochlorine (EOCl) and extractable organobromine (EOBr) in GPC-fractionated extracts from high-trophic-level mammals: Species-specific profiles and contributions of legacy organohalogen contaminants.

  Kota Mukai, Takashi Fujimori, Hoang Quoc Anh, Satoshi Fukutani, Tatsuya Kunisue, Kei Nomiyama, Shin Takahashi

  The Science of the total environment 756 143843 - 143843 2021/02 Scientific journal 

  Previous studies have suggested that unidentified compounds constitute a large proportion of extractable organochlorine (EOCl) and extractable organobromine (EOBr) in the crude extracts without fractionation; however, the proportion of unidentified EOX (X = chlorine, bromine) associated with high-/low-molecular-weight compounds is still unknown. In this study, we applied gel permeation chromatography to fractionate extracts from archived liver samples of high-trophic marine and terrestrial mammals (striped dolphins, cats, and raccoon dogs), for which concentrations of legacy organohalogen contaminants (polychlorinated biphenyls, organochlorine pesticides, and polybrominated diphenyl ethers [PBDEs]) had been previously reported. EOX in high- (>1000 g/mol) and low- (≤1000 g/mol) molecular-weight fractions (EOX-H and EOX-L) were determined by neutron activation analysis. Comparison of EOCl and EOBr enabled the characterization among species. Despite small differences in the concentrations and molecular-weight profiles of EOCl among species, the contribution of chlorine in identified compounds to EOCl-L varied from 1.5% (cats) to 79% (striped dolphins). Considerable species-specific variations were observed in the concentrations of EOBr: striped dolphins exhibited significantly greater concentrations of both EOBr-H and EOBr-L than cats and/or raccoon dogs. Moreover, the contribution of bromine in PBDEs to EOBr-L was >50% in two cats, while it was <6% in other specimens. This is the first report on EOBr mass balance in cetaceans and on EOX mass balance in terrestrial mammals living close to humans. These results suggest the need for analysis of unidentified chlorinated compounds in terrestrial mammals and unidentified brominated compounds in marine mammals.
• Unintentionally produced polychlorinated biphenyls in pigments: An updated review on their formation, emission sources, contamination status, and toxic effects.

  Hoang Quoc Anh, Isao Watanabe, Tu Binh Minh, Shin Takahashi

  The Science of the total environment 755 (Pt 1) 142504 - 142504 2021/02 [Peer-reviewed]
   Scientific journal 

  The formation, emission, environmental occurrence, and potential adverse effects of unintentionally produced polychlorinated biphenyls (PCBs) in pigments are reviewed, providing a comprehensive and up-to-date picture on these pollutants. PCBs are typically formed during manufacturing of organic pigments that involve chlorinated intermediates and reaction solvents, rather than those of inorganic pigments. Concentrations and profiles of PCBs vary greatly among pigment types and producers, with total PCB levels ranging from lower than detection limits to several hundred ppm; major components can be low-chlorinated (e.g., CB-11) or high-chlorinated congeners (e.g., CB-209). Pigment-derived PCBs can be released into the environment through different steps including pigment production, application, and disposal. They can contaminate atmospheric, terrestrial, and aquatic ecosystems, and then affect organisms living there. This situation garners scientific and public attention to nonlegacy emissions of PCBs and suggests the need for appropriate monitoring, management, and abatement strategies regarding these pollutants.
• Snakes as bimonitors of environmental pollution: A review on organic contaminants.

  Anh Quoc Hoang, Minh Binh Tu, Shin Takahashi, Tatsuya Kunisue, Shinsuke Tanabe

  The Science of the total environment 770 144672 - 144672 2021/01 Scientific journal 

  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.
• Use of comprehensive target analysis for determination of contaminants of emerging concern in a sediment core collected from Beppu Bay, Japan.

  Kou Nishimuta, Daisuke Ueno, Shin Takahashi, Michinobu Kuwae, Kiwao Kadokami, Takashi Miyawaki, Hidenori Matsukami, Hidetoshi Kuramochi, Taiki Higuchi, Yuki Koga, Hideaki Matsumoto, Noriko Ryuda, Hideki Miyamoto, Tomokazu Haraguchi, Shin-Ichi Sakai

  Environmental pollution (Barking, Essex : 1987) 115587 - 115587 2020/11 Scientific journal 

  In recent years, concern about the release of anthropogenic organic micropollutants referred to as contaminants of emerging concern (CECs) has been growing. The objective of this study was to find potential CECs by means of an analytical screening method referred to as comprehensive target analysis with an automated identification and quantification system (CTA-AIQS), which uses gas and liquid chromatography combined with mass spectrometry (GC-MS and LC-QTOF-MS). We used CTA-AIQS to analyze samples from a sediment core collected in Beppu Bay, Japan. With this method, we detected 80 compounds in the samples and CTA-AIQA could work to useful tool to find CECs in environmental media. Among the detected chemicals, three PAHs (anthracene, chrysene, and fluoranthene) and tris(isopropylphenyl)phosphate (TIPPP) isomers were found to increase in concentration with decreasing sediment depth. We quantified TIPPP isomers in the samples by means of targeted analysis using LC-MS/MS for confirmation. The concentration profiles, combined with previous reports indicating persistent, bioaccumulative, and toxic properties, suggest that these chemicals can be categorized as potential CECs in marine environments.
• Characterization of mono- to deca-chlorinated biphenyls in a well-preserved sediment core from Beppu Bay, Southwestern Japan: Historical profiles, emission sources, and inventory

  Shin Takahashi, Hoang Quoc Anh, Isao Watanabe, Daichi Aono, Michinobu Kuwae, Tatsuya Kunisue

  Science of The Total Environment 743 140767 - 140767 0048-9697 2020/11 [Peer-reviewed]
   Scientific journal
• Polychlorinated biphenyls in settled dusts from an end-of-life vehicle processing area and normal house dusts in northern Vietnam: Occurrence, potential sources, and risk assessment

  Hoang Quoc Anh, Isao Watanabe, Tu Binh Minh, Nguyen Minh Tue, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi

  Science of The Total Environment 728 138823 - 138823 0048-9697 2020/08 [Peer-reviewed]
   Scientific journal
• Bioaccessibility and exposure assessment of flame retardants via dust ingestion for workers in e-waste processing workshops in northern Vietnam

  Tatiya Wannomai, Hidenori Matsukami, Natsuyo Uchida, Fumitake Takahashi, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Tatsuya Kunisue, Go Suzuki

  Chemosphere 251 126632 - 126632 2020/07 [Peer-reviewed]
   Scientific journal 

  Flame retardants (FRs) from electronic waste (e-waste) are a widespread environmental concern. In our study, in vitro physiologically based extraction tests (PBETs) for FRs were conducted in three different areas where dust remained after processing of e-waste to identify the bioaccessible FRs and quantify their bioaccessibilities of gastrointestinal tract for human as well as to assess the exposure via ingestion of workers in e-waste processing workshops. All 36 FRs were measured and detected in indoor dusts. Among the FRs, the mean concentrations of polybrominated diphenyl ethers (PBDEs) in the floor dust and settled dust were highest, 65,000 ng/g, and 31,000 ng/g, respectively. In contrast, phosphorus containing flame retardants (PFRs) presented the highest mean concentration in the workplace dust samples, 64,000 ng/g. However, the highest bioaccessible concentrations in workplace dust, floor dust, and settled dust were observed for PFRs: 5900, 1600, and 680 ng/g, respectively. This study revealed that the higher bioaccessibility of PFRs versus other compounds was related to the negative correlation between FR concentrations and log KOW (hydrophobicity) values. The fact that hazard indices calculated using measured bioaccessibilities were less than 1 suggested that the non-cancer risk to human health by the FRs exposure via dust ingestion might be low.
• Nontarget and Target Screening of Organohalogen Compounds in Mussels and Sediment from Hiroshima Bay, Japan: Occurrence of Novel Bioaccumulative Substances.

  Akitoshi Goto, Nguyen Minh Tue, Tomohiko Isobe, Shin Takahashi, Shinsuke Tanabe, Tatsuya Kunisue

  Environmental science & technology 54 (9) 5480 - 5488 2020/05 [Peer-reviewed]
   

  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-Br3-5Cl) with molecular formulae of C9H6Br3ClO, C9H5Br4ClO, and C9H4Br5ClO in the mussel. Interestingly, UHC-Br3-5Cl 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-Br3-5Cl are ubiquitous in coastal waters of Hiroshima Bay and derived from a specific source(s). The biota-sediment accumulation factors (BSAFs) of UHC-Br3-5Cl, 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 Kow values, indicating their high bioaccumulative potential.
• Polyurethane foam-based passive air sampling for simultaneous determination of POP- and PAH-related compounds: A case study in informal waste processing and urban areas, northern Vietnam.

  Hoang Quoc Anh, Isao Watanabe, Nguyen Minh Tue, Le Huu Tuyen, Pham Hung Viet, Ngo Kim Chi, Tu Binh Minh, Shin Takahashi

  Chemosphere 247 125991 - 125991 2020/05 [Peer-reviewed]
   

  Polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), hexabromobiphenyl (BB-153), novel brominated flame retardants (NBFRs), and unsubstituted/methylated polycyclic aromatic hydrocarbons (PAHs/Me-PAHs) were simultaneously monitored in the air samples collected from Vietnamese urban and vehicular waste processing areas by using polyurethane foam-based passive air sampling (PUF-PAS) method. Concentrations (pg m-3) of organic pollutants decreased in the order: PAHs (median 29,000; range 5100-100,000) > Me-PAHs (6000; 1000-33,000) > PCBs (480; 170-1100) > PBDEs (11; 5.3-86) > NBFRs (0.20; n. d. - 51) > BB-153 (n.d.). The difference in total PCB and PBDE concentrations between the urban and waste processing air samples was not statistically significant. Meanwhile, levels of PAHs, Me-PAHs, benzo [a]pyrene equivalents (BaP-EQs), and toxic equivalents of dioxin-like PCBs (WHO-TEQs) were much higher in the waste processing sites. This is the first report on the abundance of mono- and di-CBs (notably CB-11) in the air from a developing country, suggesting their roles as emerging and ubiquitous air pollutants. Our results have indicated potential sources of specific organic pollutants such as dioxin-like PCBs, PAHs, and Me-PAHs from improper treatment of end-of-life vehicles and other vehicle related materials (e.g., waste oils and rubber tires), as well as current emission of PCBs and PBDEs in the urban area in Vietnam. Further atmospheric monitoring studies should be conducted in this developing country that cover both legacy and emerging contaminants with a focus on areas affected by rapid urbanization and informal waste processing activities.
• 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.

  Nguyen Thi Quynh Hoa, Hoang Quoc Anh, Nguyen Minh Tue, Nguyen Thanh Trung, Le Nhu Da, Tran Van Quy, Nguyen Thi Anh Huong, Go Suzuki, Shin Takahashi, Shinsuke Tanabe, Pham Chau Thuy, Pham Thi Dau, Pham Hung Viet, Le Huu Tuyen

  The Science of the total environment 709 135852 - 135852 0048-9697 2020/03 [Peer-reviewed]
   

  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-1) > open burning soil (2400; 840-4200 ng g-1) > paddy field soil (1200; range 530-6700 ng g-1) > river sediment samples (750; 370-2500 ng g-1). 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 × 10-9 to 4.6 × 10-6, 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.
• Characterization of Unsubstituted and Methylated Polycyclic Aromatic Hydrocarbons and Screening of Potential Organic Compounds in Solid Waste and Environmental Samples by Gas Chromatography–Mass Spectrometry

  HOANG Anh Quoc, LE Tuyen Huu, TU Minh Binh, TAKAHASHI Shin

  Journal of Environmental Chemistry 一般社団法人 日本環境化学会 30 (0) 82 - 93 0917-2408 2020 

  Concentrations of 19 polycyclic aromatic hydrocarbons (PAHs) and 15 methylated derivatives (Me-PAHs) were determined in different solid waste and environmental samples collected from Japan and Vietnam. Total levels of PAHs and Me-PAHs were the highest in vehicular soot samples (12,000-800,000 ng/g), followed by settled dusts (940-1,700 ng/g), and ash samples (100-270 ng/g). Fingerprint profiles of PAHs and Me-PAHs were characterized for the examined samples: the ash samples were dominated by low-molecular-weight compounds (2-3 rings) while the dust and soot samples exhibited significant proportions of high-molecular-weight PAHs (≧ 4 rings). Our results provide basic information about the occurrence of PAHs in vehicular exhausts (especially gasoline-powered vehicles) and their impacts on environmental contamination levels in a typical developing country as Vietnam. The samples were also screened for potential major organic substances by using GC-MS scan mode, revealing several specific pollutants in each sample type. Based on the analytical results, preliminary discussions about source apportionment and human health risk assessment of organic pollutants were addressed with a focus on PAHs and Me-PAHs. More comprehensive investigations of multiple organic contaminant classes in a wide variety of source-related samples and environmental compartments are needed.

• Road dust contamination by polycyclic aromatic hydrocarbons and their methylated derivatives in northern Vietnam: Concentrations, profiles, emission sources, and risk assessment.

  Anh HQ, Minh TB, Tran TM, Takahashi S

  Environmental pollution (Barking, Essex : 1987) 254 (Pt B) 113073  0269-7491 2019/08 [Peer-reviewed]
  
• Polycyclic aromatic hydrocarbons and their methylated derivatives in settled dusts from end-of-life vehicle processing, urban, and rural areas, northern Vietnam: Occurrence, source apportionment, and risk assessment.

  Anh HQ, Tue NM, Tuyen LH, Minh TB, Viet PH, Takahashi S

  The Science of the total environment 672 468 - 478 0048-9697 2019/07 [Peer-reviewed]
  
• Screening analysis of organic micro-pollutants in road dusts from some areas in northern Vietnam: A preliminary investigation on contamination status, potential sources, human exposure, and ecological risk.

  Anh HQ, Tran TM, Thu Thuy NT, Minh TB, Takahashi S

  Chemosphere 224 428 - 436 0045-6535 2019/06 [Peer-reviewed]
  
• Quantitative Speciation of Insoluble Chlorine in Environmental Solid Samples

  Mukai K, Fujimori T, Shiota K, Takaoka M, Funakawa S, Takeda A, Takahashi S

  ACS Omega 4 (4) 6126 - 6137 2019/04 [Peer-reviewed]
  
• Occurrence of benzotriazole ultraviolet stabilizers (BUVSs) in human breast milk from three Asian countries

  Joon-Woo Kim, Kwang-Hyeon Chang, Maricar Prudente, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe, Tatsuya Kunisue, Tomohiko Isobe

  Science of The Total Environment 655 1081 - 1088 0048-9697 2019/03 [Peer-reviewed]
   Scientific journal
• Soil Pollution by Chlorobenzenes and Polychlorinated Biphenyls from an Electronic Waste Recycling Area in Northern Vietnam

  Nishimura C, Suzuki G, Matsukami H, Agusa T, Takaoka M, Takahashi S, Tue NM, Viet PH, Tanabe S, Takigami H, Fujimori T

  International Journal of Environment and Pollution 63 (4) 283 - 297 2019/02 [Peer-reviewed]
  
• Seasonal variation of atmospheric organochlorine pesticides and polybrominated diphenyl ethers in Parangipettai, Tamil Nadu, India: Implication for atmospheric transport.

  Chakraborty P, Zhang G, Li J, Sampathkumar P, Balasubramanian T, Kathiresan K, Takahashi S, Subramanian A, Tanabe S, Jones KC

  The Science of the total environment 649 1653 - 1660 0048-9697 2019/02 [Peer-reviewed]
  
• 残留性有機汚染物質(POPs)対策の方向性 アーカイブ試料を活用したPOPs汚染の時系列評価と今後の課題

  国末達也, 高橋真

  廃棄物資源循環学会誌 29 (6) 423 - 432 1883-5864 2018/11
• Alterations in urinary metabolomic profiles due to lead exposure from a lead-acid battery recycling site.

  Eguchi A, Nomiyama K, Sakurai K, Kim Trang PT, Viet PH, Takahashi S, Iwata H, Tanabe S, Todaka E, Mori C

  Environmental pollution (Barking, Essex : 1987) 242 (Pt A) 98 - 105 0269-7491 2018/11 [Peer-reviewed]
  
• A preliminary investigation of 942 organic micro-pollutants in the atmosphere in waste processing and urban areas, northern Vietnam: Levels, potential sources, and risk assessment.

  Anh HQ, Tomioka K, Tue NM, Tuyen LH, Chi NK, Minh TB, Viet PH, Takahashi S

  Ecotoxicology and environmental safety 167 354 - 364 0147-6513 2018/10 [Peer-reviewed]
  
• Characterization of 209 polychlorinated biphenyls in street dust from northern Vietnam: Contamination status, potential sources, and risk assessment.

  Anh HQ, Watanabe I, Tomioka K, Minh TB, Takahashi S

  The Science of the total environment 652 345 - 355 0048-9697 2018/10 [Peer-reviewed]
  
• Comprehensive analysis of 942 organic micro-pollutants in settled dusts from northern Vietnam: pollution status and implications for human exposure

  Hoang Quoc Anh, Keidai Tomioka, Nguyen Minh Tue, Go Suzuki, Tu Binh Minh, Pham Hung Viet, Shin Takahashi

  Journal of Material Cycles and Waste Management 21 (1) 1 - 10 1611-8227 2018/05 [Peer-reviewed]
   Scientific journal 

  Contamination status of 942 organic micro-pollutants was examined for settled dust samples collected from an informal end-of-life vehicle (ELV) recycling site and an urban area in northern Vietnam. One hundred and ninety-five contaminants including 73 domestic chemicals, 79 industrial chemicals and 43 pesticides were detected at least once in our samples. Total concentrations (median and range) of organic pollutants in dusts from ELV site and Hanoi urban area were 20,000 (5600–93,000) and 21,000 (12,000–26,000) ng g−1, respectively. Pyrethroid insecticides, polycyclic aromatic hydrocarbons (PAHs) and plasticizers were the major contributors to the overall contamination levels. Concentrations of some specific chemical classes such as petroleum alkanes, PAHs, heat storage and transfer agents, and compounds leached from tires in dusts from the recycling area were significantly higher than those from the urban area, suggesting their emission during ELV dismantling and stockpiling processes. Human exposures to selected organic pollutants were also estimated by calculating daily intake doses to evaluate their hazard quotients (HQs). Although almost HQs were markedly lower than the critical value of 1, potential health risk caused by multiple organic contaminants via dust ingestion and other exposure pathways should be considered in future studies.
• Exposure assessment of heavy metals in an e-waste processing area in northern Vietnam.

  Tomoko Oguri, Go Suzuki, Hidenori Matsukami, Natsuyo Uchida, Nguyen Minh Tue, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe, Hidetaka Takigami

  The Science of the total environment 621 1115 - 1123 0048-9697 2018/04 [Peer-reviewed]
   

  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.
• PBDEs and novel brominated flame retardants in road dust from northern Vietnam: Levels, congener profiles, emission sources and implications for human exposure

  Hoang Quoc Anh, Keidai Tomioka, Nguyen Minh Tue, Tran Manh Tri, Tu Binh Minh, Shin Takahashi

  Chemosphere 197 389 - 398 1879-1298 2018/04 [Peer-reviewed]
   Scientific journal 

  Polybrominated diphenyl ethers (PBDEs) and selected novel brominated flame retardants (NBFRs) were examined in road dust samples collected from three representative areas in northern Vietnam, including seven inner districts of Hanoi metropolitan area, an industrial park in Thai Nguyen province and a rural commune in Bac Giang province. This study aims to provide basic information on the contamination status, potential sources and human exposure to PBDEs and NBFRs associated with road dust in northern Vietnam. PBDEs were detected in all the samples at a range of 0.91–56 ng g−1 with a median value of 16 ng g−1. PBDE concentrations in road dusts from urban sites were significantly higher than those from industrial zone and rural area, suggesting their environmental load related to urbanization in northern Vietnam. BDE-209, major component of deca-BDE technical mixtures, dominated the congener patterns in all samples, accounting for 60.8–91.9% of total PBDE levels. Decabromodiphenyl ethane, an alternative of deca-BDE, was observed in a detection frequency of 100% in urban and industrial areas and at levels comparable to those of BDE-209. Other NBFRs such as pentabromoethylbenzene, hexabromobiphenyl and 1,2-bis-(2,4,6-tribromophenoxy)ethane, were found at trace levels. Daily intake doses of PBDEs via road dust ingestion from 2.3 × 10−5 to 0.11 ng kg-bw−1 d−1 were estimated for residents in study areas, indicating a negligible risk with hazard indexes of 10−9 to 10−5 for selected congeners such as BDE-47, 99, 153 and 209.
• Hazardous metals emissions from e-waste-processing sites in a village in northern Vietnam

  Natsuyo Uchida, Hidenori Matsukami, Masayuki Someya, Nguyen Minh Tue, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe, Go Suzuki

  Emerging Contaminants 4 (1) 11 - 21 2405-6650 2018/01 

  © 2018 KeAi Communications Co., Ltd Inappropriate e-waste-processing operation is a serious issue in developing countries since the early 2000's. Field research was conducted to clarify its influences and diffuse toxic substances in the environment at e-waste-processing sites in a village in northern Vietnam from 2012 to 2014. We investigated surface soil samples collected from e-waste-processing sites, open burning sites, and rice paddy sites. Sediment samples and water samples were also collected from a river that runs through the village. The hazardous metal concentration in soil and river sediment samples indicated that 7 elements (Ca, Cu, Mo, Ni, Pb, Sn, and Zn) had high concentrations as a result of e-waste-processing. Most notably, Pb and Cu had high concentrations in soil samples (Pb: 26–2200 mg/kg, Cu: 22–3000 mg/kg). The results of a multivariate analysis indicated that these 7 elements were closely correlated with e-waste-processing. Concentrations of hazardous metals showed an upward trend where e-waste-processing occurred during the 3-year study period, although it was not significant statistically at present. Open burning activity had a great influence on Cu accumulation, and maximum Cu concentrations increased from 340 mg/kg in 2012–3000 mg/kg in 2014 in soil samples from open-burning sites. There were large differences in the dominant hazardous metal depending on the type of e-waste-processing workshop because hazardous metal composition was influenced by the types of e-waste and the processing procedures. It is necessary to avoid e-waste processing in open-air environment to control emissions of hazardous substances. Especially, open burning should be prohibited.
• Spatio-temporal trends of polybrominated dibenzo-p-dioxins and dibenzofurans in archived sediments from Tokyo Bay, Japan

  Akitoshi Goto, Nguyen Minh Tue, Masayuki Someya, Tomohiko Isobe, Shin Takahashi, Shinsuke Tanabe, Tatsuya Kunisue

  SCIENCE OF THE TOTAL ENVIRONMENT 599 340 - 347 0048-9697 2017/12 [Peer-reviewed]
   Scientific journal 

  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-210-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 (C) 2017 Elsevier B.V. All rights reserved.
• PCBs, PBDEs and dioxin-related compounds in floor dust from an informal end-of-life vehicle recycling site in northern Vietnam: contamination levels and implications for human exposure

  Shin Takahashi, Nguyen Minh Tue, Chika Takayanagi, Le Huu Tuyen, Go Suzuki, Hidenori Matsukami, Pham Hung Viet, Tatsuya Kunisue, Shinsuke Tanabe

  JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 19 (4) 1333 - 1341 1438-4957 2017/10 Scientific journal 

  Floor dusts from Vietnamese end-of-life vehicle (ELV)-processing households were investigated to elucidate the contamination levels and exposure risk of polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and dioxin-related compounds (DRCs). The concentrations were in order of PBDEs (260-11,000, median 280 ng/g overall) > PCBs (19-2200, median 140 ng/g) > dioxin-like PCBs (8.8-450, median 22 ng/g) >> polybrominated dibenzo-p-dioxin/dibenzofurans (PBDD/Fs, 2000-28,000, median 8500 pg/g) > polychlorinated dibenzo-p-dioxin/dibenzofurans (PCDD/Fs, 440-4100, median 1800 pg/g) > MoBPCDD/Fs (1.9-1200, median 250 pg/g). Concentrations of PCBs and DRCs were higher than those reported for Vietnamese urban houses, indicating ELV processing as a significant source of these contaminants. Higher concentrations of PCBs relative to PBDEs suggest the abundance of old electrical capacitors/transformers in ELVs. The PBDD/F and PCDD/F profiles were indicative of DecaBDE-containing materials and combustion sources, respectively. PBDFs, PCDFs and DL-PCBs were the most important dioxin-like toxic equivalent (TEQ) contributors. The estimated PCB and TEQ intake doses from dust ingestion approached or exceeded the reference doses for children living in some ELV-processing households, indicating potential health risk. More comprehensive risk assessment of the exposure to PCBs and DRCs is required for residents of informal ELV recycling sites.
• Soil contamination by halogenated polycyclic aromatic hydrocarbons from open burning of e-waste in Agbogbloshie (Accra, Ghana)

  Nguyen Minh Tue, Akitoshi Goto, Shin Takahashi, Takaaki Itai, Kwadwo Ansong Asante, Kei Nomiyama, Shinsuke Tanabe, Tatsuya Kunisue

  JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 19 (4) 1324 - 1332 1438-4957 2017/10 Scientific journal 

  Detailed composition of chlorinated and brominated polycyclic aromatic hydrocarbons (Cl-PAHs and Br-PAHs) generated during informal recycling of e-waste and their toxic relevance are still poorly understood. This study investigated the occurrence of Cl-PAHs and Br-PAHs in surface soil samples from the Agbogbloshie e-waste recycling site (Accra, Ghana) using quantitative gas chromatography-mass spectrometry (GC-MS) and comprehensive two-dimensional GC-time-of-flight mass spectrometry (GC x GC-ToFMS) profiling. The results of GC-MS analysis showed elevated concentrations in open e-waste burning areas (160-220 and 19-46 ng/g dry weight for Cl- and Br-PAHs, respectively) with substantial contribution from unidentified compounds (respectively, more than 36 and 70%, based on the total areas of potential peaks). Cl- and Br-PAHs from e-waste burning had a distinctive composition dominated by ring-ring compounds. Several homologue groups not monitored with GC-MS were found using GC x GC-ToFMS: PAHs with up to 5 Cl or 3Br, mixed halogenated PAHs and chlorinated methylPAHs. The dioxin-like toxic equivalents of the identified Cl-/Br-PAHs in soils, estimated from their in vitro AhR agonist potencies relative to 2,3,7,8-tetrachlorodibenzo-p-dioxin, were much lower than the range reported for chlorinated and brominated dioxins. However, the toxicity of the unidentified halogenated PAHs remained unclear.
• Occurrence of Natural Mixed Halogenated Dibenzo-p-Dioxins: Specific Distribution and Profiles in Mussels from Seto Inland Sea, Japan

  Akitoshi Goto, Nguyen Minh Tue, Masayuki Someya, Tomohiko Isobe, Shin Takahashi, Shinsuke Tanabe, Tatsuya Kunisue

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 51 (20) 11771 - 11779 0013-936X 2017/10 [Peer-reviewed]
   Scientific journal 

  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 X GCToFMS) 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.
• Waste prevention for sustainable resource and waste management

  Shin-ichi Sakai, Junya Yano, Yasuhiro Hirai, Misuzu Asari, Ritsuki Yanagawa, Takeshi Matsuda, Hideto Yoshida, Tetsuji Yamada, Natsuko Kajiwara, Go Suzuki, Tatsuya Kunisue, Shin Takahashi, Keijiro Tomoda, Joachim Wuttke, Paul Maehlitz, Vera Susanne Rotter, Mario Grosso, Thomas Fruergaard Astrup, Julian Cleary, Gil-Jong Oh, Lili Liu, Jinhui Li, Hwong-wen Ma, Ngo Kim Chi, Stephen Moore

  JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 19 (4) 1295 - 1313 1438-4957 2017/10 [Peer-reviewed]
   

  Although the 2Rs (reduce and reuse) are considered high-priority approaches, there has not been enough quantitative research on effective 2R management. The purpose of this paper is to provide information obtained through the International Workshop in Kyoto, Japan, on 11-13 November 2015, which included invited experts and researchers in several countries who were in charge of 3R policies, and an additional review of 245 previous studies. It was found that, regarding policy development, the decoupling between environmental pressures and economy growth was recognized as an essential step towards a sustainable society. 3R and resource management policies, including waste prevention, will play a crucial role. Approaches using material/substance flow analyses have become sophisticated enough to describe the fate of resources and/or hazardous substances based on human activity and the environment, including the final sink. Life-cycle assessment has also been developed to evaluate waste prevention activities. Regarding target products for waste prevention, food loss is one of the waste fractions with the highest priority because its countermeasures have significant upstream and downstream effects. Persistent organic pollutants and hazardous compounds should also be taken into account in the situation where recycling activities are globally widespread for the promotion of a material-cycling society.
• Levels of TBT and other selected organotin compounds in duplicate diet samples

  Ana C. A. Sousa, Sonia D. Coelho, M. Ramiro Pastorinho, Luis Taborda-Barata, Antonio J. A. Nogueira, Tomohiko Isobe, Tatsuya Kunisue, Shin Takahashi, Shinsuke Tanabe

  SCIENCE OF THE TOTAL ENVIRONMENT 574 19 - 23 0048-9697 2017/01 [Peer-reviewed]
   Scientific journal 

  Organotin compounds (OTs) are ubiquitous contaminants with a broad range of applications ranging from biocides and pesticides to catalysts for the production of polyurethane foams and silicones. The deleterious effects of some OTs (particularly tributyltin - TBT) upon wildlife and experimental animals are well documented and include endocrine disruption, immunotoxicity, neurotoxicity, genotoxicity and metabolic dysfunction in which obesity is included. However, virtually no data on the current human exposure levels is available. In order to bridge this gap, we quantified for the first time the levels of OTs in duplicate diet samples from members of the University of Aveiro in Portugal. OTs were detected in 32% of the 28 diet samples analyzed, at relatively low levels. TBT and monobutyltin were detected only in two samples and dibutyltin was detectable in three samples. Dioctyltin was quantified in four samples and monooctyltin in three samples. Phenyltins were below the detection limit in all the diet samples analyzed. Overall, for the vast majority of the samples (89%), the estimated daily intakes (EDI) of organotins through food were much lower than the established tolerable daily intakes (TDI). Hence, for the majority of the participants the risk associated with food ingestion is low. (C) 2016 Elsevier B.V. All rights reserved.
• Global Contamination and Emerging Issues regarding PCBs

  高橋 真, 田辺 信介

  廃棄物資源循環学会誌 = Material cycles and waste management research 廃棄物資源循環学会 28 (2) 99 - 111 1883-5864 2017
• Concentrations of polybrominated diphenyl ethers and alternative flame retardants in surface soils and river sediments from an electronic waste-processing area in northern Vietnam, 2012-2014

  Hidenori Matsukami, Go Suzuki, Masayuki Someya, Natsuyo Uchida, Nguyen Minh Tue, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe, Hidetaka Takigami

  CHEMOSPHERE 167 291 - 299 0045-6535 2017/01 [Peer-reviewed]
   Scientific journal 

  We investigated the concentrations of polybrominated diphenyl ethers (PBDEs) and alternative flame retardants (FRs) in environmental samples collected, in January 2012, 2013, and 2014 from an electronic waste-processing area in northern Vietnam. During the study period, PBDE and alternative FR concentrations in soils around the electronic waste-processing workshops ranged from 37 to 9200 ng g(-1) dry weight (dw) and from 35 to 24,000 ng g(-1) dw; the concentrations in soils around the open-burning sites ranged from 1.6 to 62 ng g(-1) dw and from <4 to 1900 ng g(-1) dw; and the concentrations in river sediments around the workshops ranged from 100 to 3800 ng g(-1) dw and from 23 to 6800 ng g(-1) dw, respectively. Over the course of study period, we observed significant decreases in concentrations of PBDEs and significant increases in concentrations of alternative FRs, particularly Dechlorane Plus isomers and oligomeric organophosphorus FRs (o-PFRs) in both soils and sediments around the workshops. We also report information on concentrations and environmental emissions of o-PFRs and their low molecular-weight impurities in the same soils and sediments. The detection of o-PFR impurities around the workshops and the open-burning sites highlights an enhanced breakdown of o-PFRs probably due to weathering during open storage and high temperature attained during the burning of electronic wastes. (C) 2016 Elsevier Ltd. All rights reserved.
• Lead contamination in surface soil on roads from used lead-acid battery recycling in Dong Mai, Northern Vietnam

  Takashi Fujimori, Akifumi Eguchi, Tetsuro Agusa, Nguyen Minh Tue, Go Suzuki, Shin Takahashi, Pham Hung Viet, Shinsuke Tanabe, Hidetaka Takigami

  JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 18 (4) 599 - 607 1438-4957 2016/09 Scientific journal 

  Used lead-acid battery (ULAB) recycling has caused numerous health and environmental issues in developing countries. Surface soil pollution from ULAB recycling activities has been linked with elevated levels of lead in human blood. We measured surface soil lead in and surrounding the ULAB recycling village of Hung Yen in northern Vietnam in 2011, 2013, and 2014. The data were analyzed statistically and discussed with respect to distance from the contamination source, year of measurement, contamination pathway, and countermeasures against the contamination. Transportation routes from the smelter or collection site displayed the greatest concentration of surface soil lead (median 6400-10,000 mg/kg). Surface soil lead decreased significantly with distance along the road from the ULAB recycling site, although such a decrease was not observed for rice fields, agricultural roads, or garden soil. Re-suspension and adherence by traffic were identified as key pollution pathways. Distance from the source, covering of the surface of roads, construction of walls, and position relative to the source were shown to be the most effective factors in the reduction of surface soil lead pollution. Application of a combination of these measures should result in improvement in the health of residents.
• Halogenated polycyclic aromatic hydrocarbons in soil and river sediment from e-waste recycling sites in Vietnam.

  Wang, Q, Miyake, Y, Amagai, T, Matsukami, H, Tue, N. M, Takahashi, S, Tanabe, S, Viet, P. H, Takigami, H

  Journal of Water and Environment Technology 14 (3) 166 - 176 2016/06 [Peer-reviewed]
  
• Dechlorane Plus and Dechlorane (Mirex) in Surface Sediment of the Northern Shikoku Island, Japan

  KAWANO Masahide, NISHIYAMA Tatsuya, MATSUDA Muneaki, MORITA Masatoshi, TAKAHASHI Shin

  Journal of Environmental Chemistry 一般社団法人 日本環境化学会 26 (2) 67 - 76 0917-2408 2016/06 

  Dechlorane Plus (DP), a chlorinated flame retardant, was determined in the sediment samples collected in twentynine sampling sites in the northern Shikoku Island along the coast of the Seto Inland Sea, from 2012 to 2013. Dechlorane(Mirex) and PCBs were also measured in this study comparing with the concentrations of DP in the same samples. Concentrations of DP detected in the sediment samples were significantly higher than those of Mirex. On the other hand, statistically slight difference was found between the concentrations of DP and PCBs, indicating significant environmental load and residue of DP in coastal sediments of this region. Principal component analysis based on the analytical results indicated that the chemical manufacture facility, E-waste recycling facility and the waste dumping site would be potential contamination sources of DP. To our knowledge, this is the first paper on DP accumulation in coastal sediments, which showed PCB residues at comparable concentrations, in the northern Shikoku Island.
• Comprehensive evaluation of dioxins and dioxin-like compounds in surface soils and river sediments from e-waste-processing sites in a village in northern Vietnam: Heading towards the environmentally sound management of e-waste

  Go Suzuki, Masayuki Someya, Hidenori Matsukami, Nguyen Minh Tue, Natsuyo Uchida, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe, Abraham Brouwer, Hidetaka Takigami

  Emerging Contaminants 2 (2) 98 - 108 2405-6642 2016/06 Scientific journal 

  The management of electronic waste (e-waste), which can be a source of both useful materials and toxic substances, depending on the processing method, is important for promoting material cycling. In this study, we used the dioxin-responsive chemical-activated luciferase gene expression (DR-CALUX) assay combined with gas chromatography–high-resolution mass spectrometry to evaluate the levels of dioxin-like compounds in surface soils and river sediments collected in and around an e-waste-processing village in northern Vietnam. The WHO-TEQs (Toxic equivalents) of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), coplanar polychlorinated biphenyls (Co-PCBs), and polybrominated dibenzo-p-dioxins and dibenzofurans (PBDD/Fs) in soils collected in January 2012 ranged from 0.29 to 310 pg/g (median 2.9 pg/g, n = 32), and the WHO-TEQs in sediments ranged from 0.96 to 58 pg/g (median 4.4 pg/g, n = 8). Dioxin-like activities (CALUX-TEQs [2,3,7,8-TCDD equivalent]) in soils collected in January 2012, 2013, and 2014 ranged from < 30 to 4300 pg/g (median < 30 pg/g, n = 96), and the activities in sediments ranged from < 30 to 4000 pg/g (median 33 pg/g, n = 24). Dioxin-like compounds accumulated in samples collected around e-waste-processing areas such as open-burning sites and e-waste-processing workshops, and the compounds may be transported from their sources to surrounding areas over the course of several years. Some of the CALUX-TEQs, but not WHO-TEQs, values were higher than the maximum acceptable WHO-TEQs promulgated by various authorities, indicating that all dioxin-like compounds should be evaluated in samples collected from e-waste-processing areas. Our findings suggest that open burning and open storage of e-waste should be prohibited and that wastewater treatment should be implemented at each workshop to reduce contamination by dioxin-like compounds from e-waste.
• Analysis of monomeric and oligomeric organophosphorus flame retardants in fish muscle tissues using liquid chromatography–electrospray ionization tandem mass spectrometry: Application to Nile tilapia (Oreochromis niloticus) from an e-waste processing area in northern Vietnam

  Hidenori Matsukami, Go Suzuki, Nguyen Minh Tue, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe, Hidetaka Takigami

  Emerging Contaminants 2 (2) 89 - 97 2405-6642 2016/06 Scientific journal 

  Using electrospray ionization tandem mass spectrometry combined with liquid chromatography (LC), a novel analytical method was developed to quantify eight monomeric organophosphorus flame retardants (m-PFRs) and three oligomeric organophosphorus flame retardants (o-PFRs) in fish muscle samples. The optimization and validation experiments indicate that the developed method can determine accurately the concentrations of analytes in fish muscle samples. The recoveries of analytes in fish muscle samples were in the range of 74–105%. The coefficients of variation of the concentrations of analytes in fish muscle samples were 0.6–8.9%. The concentrations of analytes in procedural blanks were below the limit of quantification (LOQ) values. Furthermore, the developed method was applied to the analysis of m-PFRs and o-PFRs in the muscle samples of tilapias collected from an electronic waste (e-waste) processing area in northern Vietnam. The concentrations of m-PFRs such as tris(2-chloroethyl) phosphate (TCEP), tris(2-chloroisopropyl) phosphate (TCIPP), and triphenyl phosphate (TPHP) were dominant among the investigated m-PFRs. The respective concentrations of TCEP, TCIPP, and TPHP were up to 160, 300, and 230 ng g−1 lipid weight, respectively, whereas those of o-PFRs were up to 10 ng g−1 lipid weight. The results of this study indicate lower accumulation potential of o-PFRs compared with m-PFRs for the first time.
• Occurrence of emerging flame retardants from e-waste recycling activities in the northern part of Vietnam

  Masayuki Someya, Go Suzuki, Alin C. Ionas, Nguyen Minh Tue, Fuchao Xu, Hidenori Matsukami, Adrian Covaci, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe, Hidetaka Takigami

  Emerging Contaminants 2 (2) 58 - 65 2405-6642 2016/06 Scientific journal 

  This study investigated the contamination status of 21 emerging flame retardants (FRs) in soils (n = 32) and river sediments (n = 8) from an e-waste recycling (EWR) site in the northern part of Vietnam. Among analyzed FRs, higher levels of decabromodiphenyl ethane (DBDPE) (ND–4200 ng/g dw), 1,2-bis-(2,4,6-tribromophenoxy)ethane (BTBPE) (ND–350 ng/g dw) and Dechlorane Plus isomers (DPs) (ND–65 ng/g dw) were found in soils near EWR workshops and open burning places. The highest concentrations of DBDPE (20 ng/g dw), BTBPE (5.7 ng/g dw) and DPs (6.7 ng/g dw) were also detected in sediments collected from the middle of the EWR site. The levels decreased concomitantly with increasing distance from the EWR site. These results indicate that these FRs were released to the surrounding environment from improper recycling activities, such as manual dismantling of devices and open burning of e-wastes. Moreover, the estimated daily intakes of those FRs via soil ingestion were approximately ten times higher for children than adults. To our knowledge, this is a first comprehensive study on characterization of soil and sediment contamination by a series of emerging FRs at an EWR site in Vietnam.
• The potential of oceanic transport and onshore leaching of additive-derived lead by marine macro-plastic debris

  Etsuko Nakashima, Atsuhiko Isobe, Shin'ichiro Kako, Takaaki Itai, Shin Takahashi, Xinyu Guo

  MARINE POLLUTION BULLETIN 107 (1) 333 - 339 0025-326X 2016/06 Scientific journal 

  The long-distance transport potential of toxic lead (Pb) by plastic marine debris was examined by pure water leaching experiments using plastic fishery floats containing high level of additive-Pb such as 5100 74.3 mg kg(-1). The leaching of Pb ended after sequential 480-h leaching experiments, and the total leaching amount is equivalent to approximately 0.1% of total Pb in a float. But it recovered when the float was scratched using sandpaper. We propose that a "low-Pb layer," in which Pb concentration is negligibly small, be generated on the float surface by the initial leaching process. Thickness of the layer is estimated at 2.5 +/- 1.2 mu m, much shallower than flaws on floats scratched by sandpaper and floats littering beaches. The result suggests that the low-Pb layer is broken by physical abrasion when floats are washed ashore, and that Pb inside the floats can thereafter leach into beaches. (C) 2016 Elsevier Ltd. All rights reserved.
• Evaluation of female aphally in imposex-affected populations of Nucella lapillus at the southernmost distributional limit of the species in Europe

  Paula Sanchez-Marin, Isabel B. Oliveira, Ana C. A. Sousa, Shin Takahashi, Shinsuke Tanabe, Susana Galante-Oliveira

  JOURNAL OF MOLLUSCAN STUDIES 82 144 - 153 0260-1230 2016/02 Scientific journal 

  Male and female aphally in Nucella lapillus has been reported in some populations from the northeastern Atlantic coast, namely in localized areas in southeastern England, northwestern France and northwestern Spain. This occurrence has been associated with Dumpton syndrome (DS), a genetic anomaly that causes under-development of the male genital tract and confers resistance to the masculinizing effects of tributyltin (TBT), i.e. to the development of imposex (superimposition of male sexual characters on neogastropod females). In an effort to elucidate the potential occurrence of DS among Portuguese populations of N. lapillus, data obtained from imposex levels monitoring campaigns performed from 2000 to 2006, during which female aphally was frequently observed, were compiled and analysed. Several characteristics associated with a demasculinizing syndrome were observed in two sampling sites near the port of Lisbon: high frequency of female aphally, undersized penises in males and lower incidence of TBT-induced imposex together with the simultaneous presence of females with contrasting vas deferens sequence values (0 and 4) at the same site. Despite the similarities with DS, the relatively lower levels of TBT pollution recorded in Portugal in comparison with other European coastal areas, and the fact that male aphally was only occasionally found, are reasons to suggest that other nongenetic causes are potentially involved in the development of female aphally in this geographical area. Nevertheless, a lower sensitivity to TBT of Portuguese N. lapillus populations that present a high frequency of aphally is apparent and this hypothetical resistance is discussed.
• Interplay of metals and bromine with dioxin-related compounds concentrated in e-waste open burning soil from Agbogbloshie in Accra, Ghana

  Takashi Fujimori, Takaaki Itai, Akitoshi Goto, Kwadwo A. Asante, Masanari Otsuka, Shin Takahashi, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 209 155 - 163 0269-7491 2016/02 Scientific journal 

  Open burning of electronic waste (e-waste) releases various metals and organohalogen compounds in the environment. Here we investigated the interplay of metals (Cu, Pb, Zn, Fe, Co, and Sr) and bromine (Br) in the formation of dioxin-related compounds (DRCs), including polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) and dioxin-like polychlorinated biphenyls (DL-PCBs), as well as non-regulated DRCs such as polybrominated dibenzo-p-dioxins/furans (PBDD/Fs) and their monobrominated PCDD/Fs in soils sampled from open burning e-waste sites at Agbogbloshie in Accra, Ghana. The predominant DRCs were PBDFs, PCDFs, PCDD5, and DL-PCBs. Statistical analyzes, X-ray absorption spectroscopy, and the PCDF/PCDD ratio suggested possible formation paths of PCDD/Fs and DL-PCBs by catalytic behaviors of copper chlorides (CuCI, CuCl2, and Cu-2(OH)(3)Cl) and thermal breakdown of polyvinyl chloride. Predominant formation of brominated furans may be derived from electron transfer from intermediates of PBDE to copper, Cu(II) -> Cu(I). Lead chloride also contributed to generate DRCs and may become highly bioaccessible through the open burning of e-waste. The main zinc species (ZnCl2 and ZnS) suggested a possible relationship to generate DRCs and specific zinc source such as tire burning. Cu, Pb, Zn, and Br contained in various e-wastes, wires/cables, plastics, and tires strongly influenced generation of many DRCs. (C) 2015 Elsevier Ltd. All rights reserved.
• Release of chlorinated, brominated and mixed halogenated dioxin-related compounds to soils from open burning of e-waste in Agbogbloshie (Accra, Ghana)

  Nguyen Minh Tue, Akitoshi Goto, Shin Takahashi, Takaaki Itai, Kwadwo Ansong Asante, Tatsuya Kunisue, Shinsuke Tanabe

  JOURNAL OF HAZARDOUS MATERIALS 302 151 - 157 0304-3894 2016/01 Scientific journal 

  Although complex mixtures of dioxin-related compounds (DRCs) can be released from informal e-waste recycling, DRC contamination in African e-waste recycling sites has not been investigated. This study examined the concentrations of DRCs including chlorinated, brominated, mixed halogenated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs, PBDD/Fs, PXDD/Fs) and dioxin-like polychlorinated biphenyls (DLPCBs) in surface soil samples from the Agbogbloshie e-waste recycling site in Ghana. PCDD/F and PBDD/F concentrations in open burning areas (18-520 and 83-3800 ng/g dry, respectively) were among the highest reported in soils from informal e-waste sites. The concentrations of PCDFs and PBDFs were higher than those of the respective dibenzo-p-dioxins, suggesting combustion and PBDE-containing plastics as principal sources. PXDFs were found as more abundant than PCDFs, and higher brominated analogues occurred at higher concentrations. The median total WHO toxic equivalent (TEOJ concentration in open burning soils was 7 times higher than the U.S. action level (1000 pg/g), with TEQ contributors in the order of PBDFs >> PCDD/Fs > PXDFs. DRC emission to soils over the e-waste site as of 2010 was estimated, from surface soil lightness based on the correlations between concentrations and lightness, at 200 mg (95% confidence interval 93-540 mg) WHO-TEQ over three years. People living in Agbogbloshie are potentially exposed to high levels of not only chlorinated but also brominated DRCs, and human health implications need to be assessed in future studies. (C) 2015 Elsevier B.V. All rights reserved.
• Toxic Identification and Evaluation of Androgen Receptor Antagonistic Activities in Acid-Treated Liver Extracts of High-Trophic Level Wild Animals from Japan

  Kentaro Misaki, Go Suzuki, Nguyen Minh Tue, Shin Takahashi, Masayuki Someya, Hidetaka Takigami, Yuko Tajima, Tadasu K. Yamada, Masao Amano, Tomohiko Isobe, Shinsuke Tanabe

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 49 (19) 11840 - 11848 0013-936X 2015/10 Scientific journal 

  Sulfuric acid-treated liver extracts of representative high-trophic level Japanese animals were analyzed by toxic identification and evaluation (TIE) with chemically activated luciferase expression (CALUX) and chemical analysis to elucidate androgen receptor (AR) antagonistic activities and potential contributions of organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs). The activities were detected in striped dolphins (n = 5), Stejneger's beaked whales (n = 6), golden eagle (n = 1), and Steller's sea eagle (n = 1) with CALUX-flutamide equivalents (FluEQs) as follow: 38 (20-52), 47 (21-96), 5.0, and 80 mu g FluEQ/g-lipid, respectively. The AR antagonism was detected in limited number of specimens at lower levels for finless porpoise, raccoon dog, and common cormorant. Theoretical activities (Theo-FluEQs) were calculated using the concentration of OCPs and PCBs and their IC25-based relative potency (REP) values. These total contribution to CALUX-FluEQ was 126%, 84%, 53%, 55%, and 44% for striped dolphin, Steller's sea eagle, Stejneger's beaked whale, finless porpoise, and golden eagle, respectively, and the main contributor was p,p'-DDE. However, most of the activities for raccoon dog (7.6%) and common cormorant (17%) could not be explained by OCPs and PCBs. This suggests other unknown compounds could function as AR antagonists in these terrestrial species.
• Flame retardant emission from e-waste recycling operation in northern Vietnam: Environmental occurrence of emerging organophosphorus esters used as alternatives for PBDEs

  Hidenori Matsukami, Nguyen Minh Tue, Go Suzuki, Masayuki Someya, Le Huu Tuyen, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe, Hidetaka Takigami

  SCIENCE OF THE TOTAL ENVIRONMENT 514 492 - 499 0048-9697 2015/05 Scientific journal 

  Three oligomeric organophosphorus flame retardants (o-PERs), eight monomeric PFRs (m-PFRs), tetrabromobisphenol A (TBBPA), and polybrominated diphenyl ethers (PBDEs) were identified and quantified in surface soils and river sediments around the e-waste recycling area in Bui Dau, northern Vietnam. Around the e-waste recycling workshops, 1,3-phenylene bis(diphenyl phosphate) (PBDPP), bisphenol A bis(diphenyl phosphate) (BPA-BDPP), triphenyl phosphate (TPHP),TBBPA, and PBDEs were dominant among the investigated flame retardants (FRs). The respective concentrations of PBDPP, BPA-BDPP, TPHP, TBBPA and the total PBDEs were 6.6-14000 ng/g-dry, <2-1500 ng/g-dry, 11-3300 ng/g-dry, <5-2900 ng/g-dry, and 67-9200 ng/g-dry in surface soils, and 4.4-78 ng/g-dry, <2-20 ng/g-dry, 73-38 ng/g-dry, 6.0-44 ng/g-dry and 100-350 ng/g-dry in river sediments. Near the open burning site of e-waste, tris(methylphenyl) phosphate (TMPP), (2-ethylhexyl) diphenyl phosphate (EHDPP), TPHP, and the total PBDEs were abundantly with respective concentrations of <2-190 ng/g-dry, <2-69 ng/g-dry, <3-51 ng/g-dry and 1.7-67 ng/g-dry in surface soils. Open storage and burning of e-waste have been determined to be important factors contributing to the emissions of FRs. The environmental occurrence of emerging FRs, especially o-PERs, indicates that the alternation of FRs addition in electronic products is shifting in response to domestic and international regulations of PBDEs. The emissions of alternatives from open storage and burning of e-waste might become greater than those of PBDEs in the following years. The presence and environmental effects of alternatives should be regarded as a risk factor along with e-waste recycling. (C) 2015 Elsevier B.V. All rights reserved.
• Residue profiles of organohalogen compounds in human serum from e-waste recycling sites in North Vietnam: Association with thyroid hormone levels

  Akifumi Eguchi, Kei Nomiyama, Nguyen Minh Tue, Pham Thi Kim Trang, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe

  ENVIRONMENTAL RESEARCH 137 440 - 449 0013-9351 2015/02 Scientific journal 

  This study demonstrated the contamination levels of polychlorinated biphenyls (PCBs), hydroxylated PCBs (OH-PCBs), polybrominated diphenyl ethers (PBDEs), methoxylated PBDEs (MeO-PBDEs), hydroxylated PBDEs (OH-PBDEs), and bromophenols (BPhs), and their relationships with thyroid hormones (THs), in the serum of human donors from an e-waste recycling site and a rural site in Hung Yen province, Vietnam. Occupationally related exposure was indicated by significantly higher residue levels of PCBs, OH-PCBs, PBDEs, and BPhs in the serum of donors from the e-waste recycling site (median: 420, 160, 290, and 300 pg g(-1) wet wt, respectively) than those in the serum of donors from the rural site (median: 290, 82, 230, and 200 pg g(-1) wet wt, respectively). On the other hand, levels of OH-/MeO-PBDEs were significantly higher in serum of donors from the reference site (median: 160 and 20 pg g(-1) wet wt, respectively) than in those from the e-waste recycling site (median: 43 and 0.52 pg g(-1) wet wt, respectively). In addition, we implemented stepwise generalized linear models to assess the association between the levels of TH and PCBs, PBDEs, and their related compounds. In females, we found positive associations of PCBs and OH-PCB concentrations with total thyroxine, free thyroxine, total triiodothyronine, and free triiodothyronine, and a negative association with thyroid-stimulating hormone concentrations. (C) 2015 Elsevier Inc. All rights reserved.
• Arsenic (+3 oxidation state) methyltransferase (AS3MT)遺伝子多型と無機ヒ素のメチル化能力との関連

  阿草哲郎, 國頭 恭, N.M. Tue, V.T.M. Lan, T.B. Minh, P.T.K. Trang, 藤原純子, 竹下治男, 高橋 真, P.H. Viet, 田辺信介, 岩田久人

  日衛誌 70 (3) 186-196  2015 [Peer-reviewed]
  
• Haptoglobin genotyping of Vietnamese: Global distribution of HPdel, complete deletion allele of the HP gene

  Mikiko Soejima, Tetsuro Agusa, Hisato Iwata, Junko Fujihara, Takashi Kunito, Haruo Takeshita, Vi Thi Mai Lan, Tu Binh Minh, Shin Takahashi, Pham Thi Kim Trang, Pham Hung Viet, Shinsuke Tanabe, Yoshiro Koda

  LEGAL MEDICINE 17 (1) 14 - 16 1344-6223 2015/01 Scientific journal 

  The haptoglobin (HP) gene deletion allele (HPdel) is responsible for anhaptoglobinemia and a genetic risk factor for anaphylaxis reaction after transfusion due to production of the anti-HP antibody. The distribution of this allele has been explored by several groups including ours. Here, we studied the frequency of HPdel in addition to the distribution of common HP genotypes in 293 Vietnamese. The HPdel was encountered with the frequency of 0.020. The present result suggested that this deletion allele is restricted to East and Southeast Asians. Thus, this allele seems to be a potential ancestry informative marker for these populations. (C) 2014 Elsevier Ireland Ltd. All rights reserved.
• Organophosphorus flame retardants (PFRs) in human breast milk from several Asian countries

  Joon-Woo Kim, Tomohiko Isobe, Mamoru Muto, Nguyen Minh Tue, Kana Katsura, Govindan Malarvannan, Agus Sudaryanto, Kwang-Hyeon Chang, Maricar Prudente, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe

  CHEMOSPHERE 116 91 - 97 0045-6535 2014/12 Scientific journal 

  In this study, the concentrations of 10 organophosphorus flame retardants (PFRs) were determined in 89 human breast milk samples collected from Japan, the Philippines and Vietnam. Among the targeted PFRs, tris(2-chloroexyl) phosphate (TCEP) and triphenyl phosphate (TPHP) were the predominant compounds and were detected in more than 60% of samples in all three countries. The concentrations of PFRs in human breast milk were significantly higher (p < 0.05) in the Philippines (median 70 ng g(-1) lipid wt.) than those in Japan (median 22 ng g-1 lipid wt.) and Vietnam (median 10 ng g-1 lipid wt.). The present results suggest that the usage of products containing PFRs in the Philippines is higher than those of Japan and Vietnam. Comparing with a previous literature survey in Sweden, the levels of PERs in human breast milk from the Philippines were 1.5-2 times higher, whereas levels in Japan and Vietnam were 4-20 times lower, suggesting that these differences might be due to their variation in the usage of flame-retarded products utilized in each country. When daily intake of PFRs to infants via human breast milk was estimated, some individuals accumulated tris(2-butoxyethyl) phosphate (TBOEP) and TCEP were close to reference dose (RfD). This is the first report to identify PFRs in human breast milk samples from Asian countries. (C) 2014 Elsevier Ltd. All rights reserved.
• Methylated and unsubstituted polycyclic aromatic hydrocarbons in street dust from Vietnam and India: Occurrence, distribution and in vitro toxicity evaluation

  Le Huu Tuyen, Nguyen Minh Tue, Shin Takahashi, Go Suzuki, Pham Hung Viet, Annamalai Subramanian, Kesav A. Bulbule, Peethambaram Parthasarathy, Alagappan Ramanathan, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 194 272 - 280 0269-7491 2014/11 Scientific journal 

  Methylated polycyclic aromatic hydrocarbons (MePAHs), unsubstituted PAHs and AhR-mediated activities were determined in street dust collected from Vietnam and India using a combined approach of chemical analysis and in vitro reporter gene assay. MePAHs and PAHs diagnostic ratios indicated that the main sources of MePAHs in Vietnam were pyrogenic emissions, whereas in India there were mixed sources of pyrogenic and petrogenic emissions. AhR-mediated activities determined by using DR-CALUX assay were observed in urban street dust at mean 40,29 and 20 ng CALUX-TEQ/g dw for Hanoi, Bangalore and New Delhi, respectively. MePAHs and PAHs contributed only 5% or less to AhR-mediated activity in street dust, indicating the occurrence of unknown AhR agonists. The principal contributors to Theoretical-TEQs among target compounds were methyl benz[a]anthracene, benzo[b]- and benzo[k] fluoranthene. The present study indicates importance of MePAHs in evaluation of toxic risk related to AhR-mediated activity in urban polluted areas. (C) 2014 Elsevier Ltd. All rights reserved.
• Aryl hydrocarbon receptor mediated activities in road dust from a metropolitan area, Hanoi-Vietnam: Contribution of polycyclic aromatic hydrocarbons (PAHs) and human risk assessment

  Le Huu Tuyen, Nguyen Minh Tue, Go Suzuki, Kentaro Misaki, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe

  SCIENCE OF THE TOTAL ENVIRONMENT 491 246 - 254 0048-9697 2014/09 Scientific journal 

  Dioxin-Responsive Chemical-Activated LUciferase gene eXpression assay (DR-CALUX) was applied to assess the total toxic activity of the mixture of PAHs and related compounds as well as dioxin-related compounds in road dust from urban areas of Hanoi, Vietnam. Road dust from Hanoi contained significantly higher DR-CALUX activities (3 to 39, mean 20 ng CALUX-TEQ/g dw) than those from a rural site (2 to 13, mean 5 ng CALUX-TEQ/g dw). The total concentrations of 24 major PAHs (Sigma(24)PAHs) in urban road dust (0.1 to 5.5, mean 2.5 mu g/g dw) were also 6 times higher than those in rural road dust (0.08 to 1.5, mean 0.4 mu g/g dw). Diagnostic ratios of PAHs indicated vehicular engine combustion as the major PAH emission source in both sites. PAHs accounted for 0.8 to 60% (mean 10%) and 2 to 76% (mean 20%) of the measured CALUX-TEQs in road dust for Hanoi the rural site, respectively. Benzo[b]-/benzo[k]fluoranthenes were the major TEQ contributors among PAHs, whereas DRCs contributed <0.1% to CALUX-TEQs for both rural and urban sites. These results suggest TEQ contribution of other aryl hydrocarbon receptor agonists in road dust. Significant PAH concentrations in urban dust indicated high mutagenic and carcinogenic potencies. Estimated results of incremental life time cancer risk (ILCR) indicated that Vietnamese populations, especially those in urban areas such as Hanoi, are potentially exposed to high cancer risk via both dust ingestion and dermal contact. This is the first study on the exposure risk of AhR agonists, including PAHs and DRCs, in urban road dust from a developing country using a combined bio-chemical analytical approach. (C) 2014 Elsevier B.V. All rights reserved.
• Dioxin-related compounds in breast milk of women from Vietnamese e-waste recycling sites: Levels, toxic equivalents and relevance of non-dietary exposure

  Nguyen Minh Tue, Kana Katsura, Go Suzuki, Le Huu Tuyen, Takurni Takasuga, Shin Takahashi, Pham Hung Viet, Shinsuke Tanabe

  ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY 106 220 - 225 0147-6513 2014/08 Scientific journal 

  Although informal e-waste recycling sites (EWRSs) are hotspots of both polychlorinated and poly-brominated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs and PBDD/Fs), human exposure to the latter has not been studied in details. This study investigated the accumulation levels and profiles of dioxin-related compounds (DRCs) in breast milk samples from women living in two Vietnamese EWRSs and estimated the intake contribution from e-waste-related exposure. Screening results using Dioxin-Responsive Chemically Activated LUciferase gene eXpression assay (DR-CALUX) showed higher dioxin-like (DL) activities in samples from the EWRS Bui Dau than in those from the EWRS Trang Minh and a reference site (2.3-10 vs 1.7-4.8 and 0.60-5.7 pg CALUX-TEQ/g lipid, n=10, 6 and 9, respectively). Chemical analysis results of selected samples show that the WHO-TEQ levels of PCDD/Fs, DL-PCBs and PBDD/Fs in EWRS samples were not significantly higher than in those from the reference site (0.22-7.4 vs 1.1-3.0 pg/g lipid) and within the Vietnamese background range, but women involved in recycling accumulated higher concentrations of PCDFs (13-15 vs 2.3-8.8 pg/g lipid) and PBDFs (1.1-1.5 vs <1.1 pg/g lipid). By comparing the DRC profile in milk of these women with the reported profile in house dust from the same site, dust ingestion was estimated to contribute most of the intake for tetraBDF, 37 per cent to 55 per cent for penta octaCDFs, but less than twenty per cent for PCDDs and DL-PCBs, and 26 per cent for total WHO-TEQs. The DL activities in some EWRS milk samples were not fully explained by chemical data, suggesting contribution from unidentified compounds. The estimated WHO-TEQ intake doses for breastfed infants (1.3-33 pg/kg/d) mostly exceeded the tolerable value, especially for those living in the EWRSs; and unidentified DRCs might increase further the dioxin-related health risk. (C) 2014 Elsevier Inc. All rights reserved.
• A microcosm approach to evaluate the degradation of tributyltin (TBT) by Aeromonas molluscorum Av27 in estuarine sediments

  Andreia Cruz, Isabel Henriques, Ana C. A. Sousa, Ines Baptista, Adelaide Almeida, Shin Takahashi, Shinsuke Tanabe, Antonio Correia, Satoru Suzuki, Ana Maria Anselmo, Sonia Mendo

  ENVIRONMENTAL RESEARCH 132 430 - 437 0013-9351 2014/07 Scientific journal 

  Tributyltin (TBT) is a biocide extremely toxic to a wide range of organisms, which has been used for decades in antifouling paints. Despite its global ban in 2008, TBT is still a problem of great concern due to the high levels trapped in sediments. Aeromonas molluscorum Av27 is a TBT degrading bacterium that was isolated from an estuarine system. We investigated the ability and the role of this bacterium on TBT degradation in this estuarine system, using a microcosm approach in order to mimic environmental conditions. The experiment was established and followed for 150 days. Simultaneously, changes in the indigenous bacterial community structure were also investigated. The results revealed a maximum TBT degradation rate of 28% accompanied by the detection of the degradation products over time. Additionally, it was observed that TBT degradation was significantly enhanced by the presence of Av27. In addition a significantly higher TBT degradation occurred when the concentration of Av27 was higher. TBT degradation affected the bacterial community composition as revealed by the changes in the prevalence of Proteobacteria subdivisions, namely the increase of Deltaproteobacteria and the onset of Epsilonproteobacteria. However, the addition of Av27 strain did not affect the dominant phylotypes. Total bacterial number, bacterial biomass productivity, 16S rRNA gene and denaturing gradient gel electrophoresis (DGGE) analyses also indicated alterations on the bacterial community structure over time, with bacteria non-tolerant to pollutants increasing their representativeness, as, for instance, the increase of the number of Alphaproteobacteria clones from 6% in the beginning to 12% at the end of the experiment. The work herein presented confirms the potential of Av27 strain to be used in the decontamination of TBT-polluted environments. (C) 2014 Elsevier Inc. All rights reserved.
• An international comparative study of end-of-life vehicle (ELV) recycling systems

  Shin-ichi Sakai, Hideto Yoshida, Jiro Hiratsuka, Carlo Vandecasteele, Regina Kohlmeyer, Vera Susanne Rotter, Fabrizio Passarini, Alessandro Santini, Maria Peeler, Jinhui Li, Gil-Jong Oh, Ngo Kim Chi, Lawin Bastian, Stephen Moore, Natsuko Kajiwara, Hidetaka Takigami, Takaaki Itai, Shin Takahashi, Shinsuke Tanabe, Keijiro Tomoda, Takashi Hirakawa, Yasuhiro Hirai, Misuzu Asari, Junya Yano

  JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 16 (1) 1 - 20 1438-4957 2014/02 

  End-of-life vehicles (ELV) have become a global concern as automobiles have become popular worldwide. An international workshop was held to gather data and to discuss 3R policies and ELV recycling systems, their background and present situation, outcomes of related policies and programs, the framework of recycling and waste management, and case studies on related topics in several countries and regions, as well as the essential points of the comparison. Legislative ELV recycling systems are established in the EU, Japan, Korea, and China, while in the US, ELV recycling is managed under existing laws on environmental protection. Since automobile shredding residue (ASR) has a high calorific value and ash content, and includes heavy metals as well as a mass of unclassified fine particles, recycling ASR is considered highly difficult. Countries with a legislative ELV system commonly set a target for recovery rates, with many aiming for more than 95 % recovery. In order to reach this target, higher efficiency in ASR recovery is needed, in addition to material recycling of collectable components and metals. Environmentally friendly design was considered necessary at the planning and manufacturing stages, and the development of recycling systems and techniques in line with these changes are required for sound ELV management.
• Exposure assessment of lead to workers and children in the battery recycling craft village, Dong Mai, Vietnam

  Takako Noguchi, Takaaki Itai, Nguyen Minh Tue, Tetsuro Agusa, Nguyen Ngoc Ha, Sawako Horai, Pham Thi Kim Trang, Pham Hung Viet, Shin Takahashi, Shinsuke Tanabe

  JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 16 (1) 46 - 51 1438-4957 2014/02 Scientific journal 

  Human exposure to lead (Pb) due to uncontrolled Pb-acid battery recycling has been an environmental health issue in newly developed industrial regions. We conducted a human monitoring survey in Dong Mai, a battery recycling village in Vietnam, to assess exposure status to Pb. Lead level was measured in hair, blood and urine samples of residents in Dong Mai and two reference sites during 4 years spanning 2007-2011. In Dong Mai, Pb levels in three matrixes were significantly higher than those in reference sites. Blood Pb levels of all adults and children exceeded 10 mu g/dL, the Centers for Disease Control and Prevention definition of an elevated blood Pb level. Clear increase of urinary delta-aminolevulinic acid (ALA) level with increasing blood Pb level indicated disruption of heme synthesis. One adult exceeded 100 mu g/dL of blood Pb, where encephalopathy is of concern. The blood Pb levels achieved various toxic effect threshold values, and elevated blood Pb was not limited to recycling workers, but was also in children and women of reproductive age. Serious pollution status of Dong Mai village suggests an importance of further monitoring surveys in various developing Asian countries.
• Effect-based Hazard Identification of House Dust by In Vitro Assays Detecting Dioxin-like Compounds, Thyroid and Reproductive Toxicants

  Go Suzuki, Nguyen M. Tue, Shin Takahashi, Shinsuke Tanabe, Shin-ichi Sakai, Hidetaka Takigami

  CURRENT ORGANIC CHEMISTRY 18 (17) 2231 - 2239 1385-2728 2014 Scientific journal 

  Indoor dust is a sink for many kinds of pollutants, including flame retardants (FRs), plasticizers and various degradation products, derived from household products. Recently, we have put particular emphasis on the evaluation of indoor dust as an excellent indicator of important contaminants for chemical risk management throughout the lifecycle of household product. Our research has focused on effect-based approach using in vitro bioassays together with instrumental analyses in an attempt to conduct hazard characterization determining the presence and activity profile of contaminants detected in house dust. This approach will lead to a determination of priority pollutants, their impurities and by-products for further assessment from the list of chemicals manufactured and distributed worldwide. Here, we introduce some background studies and results obtained by using effect-based approach for house dust, revealing importance of dioxin-like compounds, thyroid and reproductive toxicants used and contained in household products. Based on outcomes from previous studies here summarized, it can be suggested that effect-based approach is a useful scheme to determine contaminants and endpoints in indoor dust for priority assessment on in vitro toxicological point of view. Further integration of exposure and effect analysis for indoor dust will lead to appropriate chemical risk management throughout various household products' lifecycles.
• Dioxin-related compounds in house dust from New York State: Occurrence, in vitro toxic evaluation and implications for indoor exposure

  Nguyen Minh Tue, Go Suzuki, Shin Takahashi, Kurunthachalam Kannan, Hidetaka Takigami, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 181 75 - 80 0269-7491 2013/10 Scientific journal 

  This study analysed sulphuric-acid-treated extracts of house dust from New York State with DR-CALUX assay and HRGC-HRMS to elucidate the total dioxin-like (DL) activities, the occurrence of various dioxin-related compounds (DRCs), including PBDD/Fs, and their toxic contribution. The DL activities were 30 -8000, median 210 pg CALUX-TEQ/g. PCDD/Fs, PBDD/Fs and DL-PCBs were detected with a large variation in concentrations (0.12-80, 0.33-150, 0.46-35, medians 1.7, 2.1 and 5.6 ng/g, respectively) and profiles, indicating the existence of multiple contamination sources in homes. PCDD/Fs, PBDD/Fs and DL-PCBs with known potency theoretically contributed <1%-130%, <1%-21% and <1%-6.8%, respectively, of the measured CALUX-TEQs. These results and those from DR-CALUX assays with fractionated dust extracts indicated that a substantial portion of the CALUX-TEQs could be caused by unknown dust contaminants. Considering that the DRC intake from indoor dust ingestion can be significant, identification of unknown DL contaminants in indoor dust is necessary. (C) 2013 Elsevier Ltd. All rights reserved.
• Occurrence of halogenated contaminants in inland and coastal fish from Ghana: Levels, dietary exposure assessment and human health implications

  Kwadwo Ansong Asante, Shin Takahashi, Takaaki Itai, Tomohiko Isobe, Gnanasekaran Devanathan, Mamoru Muto, Seth Koranteng Agyakwah, Sam Adu-Kumi, Annamalai Subramanian, Shinsuke Tanabe

  ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY 94 123 - 130 0147-6513 2013/08 Scientific journal 

  Fish consumption is known to have several health benefits for humans. However, the accumulation of toxic contaminants, such as PCBs, PBDEs and HBCDs in fish could pose health hazards. These contaminants were measured in tilapia fish species collected from Ghana. Mean levels were PCBs (62 ng/g lw), PBDEs (7.3 ng/g lw) and HBCDs (1.2 ng/g lw) and the predominance of CB-153, CB-138, CB-180, BDE-47 and alpha-HBCD is in concordance with scientific literature. The congener profiles of PBDEs and PCBs in the fish suggest that sources of Penta- and Deca-BDE technical mixtures as well as technical PCB mixture (Clophen A60) exist in Ghana, while textile operations and associated release of untreated wastewater are likely to be significant sources of HBCDs. Comparison of the results with some reported studies showed moderate contamination in Ghana although Ghana is a developing country in Africa. Concentrations of PCBs measured in all the specimens in this study were below the food safety guidelines issued by the Food and Drug Administration, USA and the European Commission. The calculated hazard index levels of the target contaminants were below the threshold value of one, indicating that the levels of the target contaminants do not seem to constitute a health risk via fish consumption, with regard to PCBs, PBDEs and HBCDs, based on the limited number of samples that was accounted for in this study. However, due to the continuous discharge of untreated effluents, follow up studies are warranted as the consumption of fish is the primary route of human exposure to PCBs. This maiden report on the status of PBDEs and HBCDs in fish from Ghana will contribute to the knowledge about environmental contamination by POPs in a less industrialized region of the world so far sparsely covered in the literature. (C) 2013 Elsevier Inc. All rights reserved.
• Environmental contamination and human exposure to dioxin-related compounds in e-waste recycling sites of developing countries

  Nguyen Minh Tue, Shin Takahashi, Annamalai Subramanian, Shinichi Sakai, Shinsuke Tanabe

  Environmental Sciences: Processes and Impacts 15 (7) 1326 - 1331 2050-7887 2013/07 Scientific journal 

  E-waste recycling using uncontrolled processes is a major source of dioxin-related compounds (DRCs), including not only the regulated polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs) and dioxin-like polychlorinated biphenyls (DL-PCBs) but also non-regulated brominated and mixed halogenated compounds (PBDD/Fs and PXDD/Fs). Various studies at informal e-waste recycling sites (EWRSs) in Asian developing countries found the soil contamination levels of PCDD/Fs from tens to ten thousand picogram TCDD-equivalents (TEQ) per gram and those of DL-PCBs up to hundreds of picogram TEQ per gram. The air concentration of PCDD/Fs was reported as high as 50 pg TEQ per m3 in Guiyu, the largest Chinese EWRS. Non-regulated compounds also contributed substantially to the total DL toxicity of the DRC mixtures from e-waste, as evidenced by the high TEQ levels estimated for the currently identifiable PBDD/Fs as well as the large portion of unexplained bioassay-derived TEQ levels in soils/dusts from EWRSs. Considering the high exposure levels estimated for EWRS residents, especially children, comprehensive emission inventories of DRCs from informal e-waste recycling, the identities and toxic potencies of unidentified DRCs released, and their impacts on human health need to be investigated in future studies. © 2013 The Royal Society of Chemistry.
• Contamination by perfluorinated compounds in water near waste recycling and disposal sites in Vietnam

  Joon-Woo Kim, Nguyen Minh Tue, Tomohiko Isobe, Kentaro Misaki, Shin Takahashi, Pham Hung Viet, Shinsuke Tanabe

  ENVIRONMENTAL MONITORING AND ASSESSMENT 185 (4) 2909 - 2919 0167-6369 2013/04 Scientific journal 

  There are very few reports on the contamination by perfluorinated chemicals (PFCs) in the environment of developing countries, especially regarding their emission from waste recycling and disposal sites. This is the first study on the occurrence of a wide range of PFCs (17 compounds) in ambient water in Vietnam, including samples collected from a municipal dumping site (MD), an e-waste recycling site (ER), a battery recycling site (BR) and a rural control site. The highest PFC concentration was found in a leachate sample from MD (360 ng/L). The PFC concentrations in ER and BR (mean, 57 and 16 ng/L, respectively) were also significantly higher than those detected in the rural control site (mean, 9.4 ng/L), suggesting that municipal solid waste and waste electrical and electronic equipment are potential contamination sources of PFCs in Vietnam. In general, the most abundant PFCs were perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), and perfluoroundecanoic acid (PFUDA; < 1.4-100, < 1.2-100, and < 0.5-20 ng/L, respectively). Interestingly, there were specific PFC profiles: perfluoroheptanoic acid and perfluorohexanoic acid (88 and 77 ng/L, respectively) were almost as abundant as PFOA in MD leachate (100 ng/L), whereas PFNA was prevalent in ER and BR (mean, 17 and 6.2 ng/L, respectively) and PFUDA was the most abundant in municipal wastewater (mean, 5.6 ng/L), indicating differences in PFC contents in different waste materials.
• Soil contamination by brominated flame retardants in open waste dumping sites in Asian developing countries

  Akifimi Eguchi, Tomohiko Isobe, Karri Ramu, Nguyen Minh Tue, Agus Sudaryanto, Gnanasekaran Devanathan, Pham Hung Viet, Rouch Seang Tana, Shin Takahashi, Annamalai Subramanian, Shinsuke Tanabe

  Chemosphere 90 (9) 2365 - 2371 0045-6535 2013/03 Scientific journal 

  In Asian developing countries, large amounts of municipal wastes are dumped into open dumping sites each day without adequate management. This practice may cause several adverse environmental consequences and increase health risks to local communities. These dumping sites are contaminated with many chemicals including brominated flame retardants (BFRs) such as polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs).BFRs may be released into the environment through production processes and through the disposal of plastics and electronic wastes that contain them. The purpose of this study was to elucidate the status of BFR pollution in municipal waste dumping sites in Asian developing countries. Soil samples were collected from six open waste dumping sites and five reference sites in Cambodia, India, Indonesia, Malaysia, and Vietnam from 1999 to 2007. The results suggest that PBDEs are the dominant contaminants in the dumping sites in Asian developing countries, whereas HBCD contamination remains low. Concentrations of PBDEs and HBCDs ranged from ND to 180 μg/kg dry wt and ND to 1.4 μg/kg dry wt, respectively, in the reference sites and from 0.20 to 430 μg/kg dry wt and ND to 2.5 μg/kg dry wt, respectively, in the dumping sites. Contamination levels of PBDEs in Asian municipal dumping sites were comparable with those reported from electronic waste dismantling areas in Pearl River delta, China. © 2012 Elsevier Ltd.
• Similarities in the Endocrine-Disrupting Potencies of Indoor Dust and Flame Retardants by Using Human Osteosarcoma (U2OS) Cell-Based Reporter Gene Assays

  Go Suzuki, Nguyen Minh Tue, Govindan Malarvannan, Agus Sudaryanto, Shin Takahashi, Shinsuke Tanabe, Shin-ichi Sakai, Abraham Brouwer, Naoto Uramaru, Shigeyuki Kitamura, Hidetaka Taldgami

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 47 (6) 2898 - 2908 0013-936X 2013/03 Scientific journal 

  Indoor dust is a sink for many kinds of pollutants, including flame retardants (FRs), plasticizers, and their contaminants and degradation products. These pollutants can be migrated to indoor dust from household items such as televisions and computers. To reveal high-priority end points of and contaminant candidates in indoor dust, using CALUX reporter gene assays based on human osteosarcoma (U2OS) cell lines, we evaluated and characterized the endocrine-disrupting potencies of crude extracts of indoor dust collected from Japan (n = 8), the United States (n = 21), Vietnam (n = 10), the Philippines (n = 17), and Indonesia (n = 10) and for 23 selected FRs. The CALUX reporter gene assays used were specific for compounds interacting with the human androgen receptor (AR), estrogen receptor alpha (ER alpha), progesterone receptor (PR), glucocorticoid receptor (GR), and peroxisome proliferator-activated receptor gamma 2 (PPAR gamma 2). Indoor dust extracts were agonistic to ER alpha, GR, and PPAR gamma 2 and antagonistic against AR, PR, GB., and PPAR gamma 2. In comparison, a majority of FRs was agonistic to ER alpha and PPAR gamma 2 only, and some FRs demonstrated receptor-specific antagonism against all tested nuclear receptors. Hierarchical clustering clearly indicated that agonism of ER alpha and antagonism of AR and PR were common, frequently detected end points for indoor dust and tested FRs. Given our previous results regarding the concentrations of FRs in indoor dust and in light of our current results, candidate contributors to these effects include not only internationally controlled brominated FRs but also alternatives such as some phosphorus-containing FRs. In the context of indoor pollution, high-frequency effects of FRs such as agonism of ER alpha and antagonism of AR and PR are candidate high-priority end points for further investigation.
• Organotin Compounds from Snails to Humans

  Ana C. A. Sousa, M. Ramiro Pastorinho, Shin Takahashi, Shinsuke Tanabe

  Springer Science + Business Media 215 - 275 2213-7114 2013 [Peer-reviewed]
  
• Contamination of indoor dust and air by polychlorinated biphenyls and brominated flame retardants and relevance of non-dietary exposure in Vietnamese informal e-waste recycling sites

  Nguyen Minh Tue, Shin Takahashi, Go Suzuki, Tomohiko Isobe, Pham Hung Viet, Yuso Kobara, Nobuyasu Seike, Gan Zhang, Agus Sudaryanto, Shinsuke Tanabe

  ENVIRONMENT INTERNATIONAL 51 160 - 167 0160-4120 2013/01 Scientific journal 

  This study investigated the occurrence of polychlorinated biphenyls (PCBs), and several additive brominated flame retardants (BFRs) in indoor dust and air from two Vietnamese informal e-waste recycling sites (EWRSs) and an urban site in order to assess the relevance of these media for human exposure. The levels of polybrominated diphenyl ethers (PBDEs), hexabromocyclododecane (HBCD), 1,2-bis-(2,4,6-tribromophenoxy) ethane (BTBPE) and decabromodiphenyl ethane (DBDPE) in settled house dust from the EWRSs (130-12,000, 5.4-400, 5.2-620 and 31-1400 ng g(-1), respectively) were significantly higher than in urban house dust but the levels of PCBs (4.8-320 ng g(-1)) were not higher. The levels of PCBs and PBDEs in air at e-waste recycling houses (1000-1800 and 620-720 pg m(-3), respectively), determined using passive sampling, were also higher compared with non-e-waste houses. The composition of BFRs in EWRS samples suggests the influence from high-temperature processes and occurrence of waste materials containing older BFR formulations. Results of daily intake estimation for e-waste recycling workers are in good agreement with the accumulation patterns previously observed in human milk and indicate that dust ingestion contributes a large portion of the PBDE intake (60%-88%), and air inhalation to the low-chlorinated PCB intake (>80% for triCBs) due to their high levels in dust and air, respectively. Further investigation of both indoor dust and air as the exposure media for other e-waste recycling-related contaminants and assessment of health risk associated with exposure to these contaminant mixtures is necessary. (C) 2012 Elsevier Ltd. All rights reserved.
• A numerical study on the seasonal variability of polychlorinated biphenyls from the atmosphere in the East China Sea

  Jun Ono, Daisuke Takahashi, Xinyu Guo, Shin Takahashi, Hidetaka Takeoka

  CHEMOSPHERE 89 (4) 389 - 397 0045-6535 2012/10 Scientific journal 

  A three-dimensional/high-resolution transport model for persistent organic pollutants (POPs) has been developed for the East China Sea (ECS). The POPs model has four compartments (gaseous, dissolved, phytoplankton-bound, and detritus-bound phases) and includes processes for diffusive air-water exchange, phytoplankton uptake/depuration to POPs, decomposition of dissolved phase, vertical sinking of phytoplankton, detritus production by phytoplankton mortality, and vertical sinking and decomposition of detritus. The POPs model is coupled with an ocean circulation model that can reproduce the seasonal variation in physical variables to represent the advection and diffusion of POPs. We applied the POPs model to the polychlorinated biphenyl congener 153 (PCB 153) from the atmosphere and examined the behavior of PCB 153 in the ocean. The model showed a remarkable seasonal variability of PCB 153. Concentrations in the dissolved and particulate phases are high in winter (January-March) and low in summer (July-September). In coastal regions, where chlorophyll a concentration is high, horizontal and vertical distributions in the dissolved and particulate PCB 153 concentrations are strongly affected by phytoplankton uptake. The sensitivity experiments on the dynamics of PCB 153 suggested that a change of Henry's law constant associated with water temperature is the major factor controlling the seasonal variability of PCB 153. The model-based yearly mass balance of PCB 153 in the ECS indicated that most of the atmospheric input (35.5 kg year(-1)) is removed by the horizontal advection outside the ECS (19.0 kg year(-1)) and accumulates to the sea bottom by vertical sinking (15.7 kg year(-1)). For comparison with PCB 153, we also conducted simulations for PCB 52, 101, and 180. The seasonal variations are similar to that of PCB 153. The mass balance of PCB 52 that has short half-life time and less hydrophobic property shows the different results compared with PCB 101, 153, and 180. (C) 2012 Elsevier Ltd. All rights reserved.
• Different profiles of anthropogenic and naturally produced organohalogen compounds in serum from residents living near a coastal area and e-waste recycling workers in India

  Akifumi Eguchi, Kei Nomiyama, Gnanasekaran Devanathan, Annamalai Subramanian, Kesav A. Bulbule, Peethambaram Parthasarathy, Shin Takahashi, Shinsuke Tanabe

  ENVIRONMENT INTERNATIONAL 47 8 - 16 0160-4120 2012/10 Scientific journal 

  We determined the contamination status and accumulation profiles of polychlorinated biphenyls (PCBs), hydroxylated PCB congeners (OH-PCBs), polybrominated diphenyl ethers (PBDEs), hydroxylated PBDEs (OH-PBDEs), methoxylated PBDEs (MeO-PBDEs), and bromophenols (BPhs) in serum from e-waste recycling workers and residents near a coastal area in India. Residue levels of penta- to octa-chlorinated PCBs, penta- to octa-chlorinated OH-PCBs, 6MeO-BDE47, 6OH-BDE47, and 2,4,6-tri-BPh in serum from residents living near the coastal area were significantly higher than those in serum from e-waste recycling workers. Residue levels of tri- to tetra-chlorinated PCBs, tri- to tetra-chlorinated OH-PCBs. PBDEs. octa-brominated OH-PBDEs, and tetra-BPhs in serum from e-waste recycling workers were higher than those in serum from residents living near the coastal area. Principal component analysis revealed that residents living near the coastal area and e-waste recycling workers had different serum profiles of chlorinated and brominated compounds. (C) 2012 Elsevier Ltd. All rights reserved.
• Quantification of Toxic Metals Derived from Macroplastic Litter on Ookushi Beach, Japan

  Etsuko Nakashima, Atsuhiko Isobe, Shin'ichiro Kako, Takaaki Itai, Shin Takahashi

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 46 (18) 10099 - 10105 0013-936X 2012/09 Scientific journal 

  The potential risk of toxic metals that could leach into a beach environment from plastic litter washed ashore on Ookushi Beach, Goto Islands, Japan was estimated by balloon aerial photography, in situ beach surveys, and leaching experiments in conjunction with a Fickian diffusion model analysis. Chromium (Cr), cadmium (Cd), tin (Sn), antimony (Sb), and lead (Pb) were detected in plastic litter collected during the beach surveys. Polyvinyl chloride (PVC) fishing floats contained the highest quantity of Pb. Balloon aerial photography in conjunction with a beach survey gave an estimated mass of Pb derived from plastic litter of 313 +/- 247 g. Lead leaching experiments on collected PVC floats showed that Pb in the plastic litter could leach into surrounding water on the actual beach, and that plastic litter may act as a "transport vector" of toxic metals to the beach environment. Using the experimental data, the total mass of Pb that could leach from PVC plastic litter over a year onto Ookushi Beach was estimated as 0.6 +/- 0.6 g/year, suggesting that toxic metals derived from plastic beach litter are a potential "pathway" to contamination of the beach environment due to their accumulation in beach soil over time.
• Multi-trace element levels and arsenic speciation in urine of e-waste recycling workers from Agbogbloshie, Accra in Ghana

  Kwadwo Ansong Asante, Tetsuro Agusa, Charles Augustus Biney, William Atuobi Agyekum, Mohammed Bello, Masanari Otsuka, Takaaki Itai, Shin Takahashi, Shinsuke Tanabe

  SCIENCE OF THE TOTAL ENVIRONMENT 424 63 - 73 0048-9697 2012/05 Scientific journal 

  To understand human contamination by multi-trace elements (TEs) in electrical and electronic waste (e-waste) recycling site at Agbogbloshie, Accra in Ghana, this study analyzed TEs and As speciation in urine of e-waste recycling workers. Concentrations of Fe, Sb, and Pb in urine of e-waste recycling workers were significantly higher than those of reference sites after consideration of interaction by age, indicating that the recycling workers are exposed to these TEs through the recycling activity. Urinary As concentration was relatively high, although the level in drinking water was quite low. Speciation analysis of As in human urine revealed that arsenobetaine and dimethylarsinic acid were the predominant As species and concentrations of both species were positively correlated with total As concentration as well as between each other. These results suggest that such compounds may be derived from the same source, probably fish and shellfish and greatly influence As exposure levels. To our knowledge, this is the first study on human contamination resulting from the primitive recycling of e-waste in Ghana. This study will contribute to the knowledge about human exposure to trace elements from an e-waste site in a less industrialized region so far scantly covered in the literature. (c) 2012 Elsevier B.V. All rights reserved.
• Organotin levels in Nazare canyon (west Iberian Margin, NE Atlantic) and adjacent coastal area

  Ana C. A. Sousa, Isabel B. Oliveira, Filipe Laranjeiro, Shin Takahashi, Shinsuke Tanabe, Marina R. Cunha, Carlos M. Barroso

  MARINE POLLUTION BULLETIN 64 (2) 422 - 426 0025-326X 2012/02 Scientific journal 

  Organotin compounds (OTs) are ubiquitous in the marine environment and high concentrations (mu g g(-1) range) in sediments from different coastal areas around the world have been reported. However, few reports have described the OTs contamination status in the offshore and deep sea environment. This work investigated organotin levels in Nazare canyon for the first time. Levels of monobutyltin (MBT), dibutyltin (DBT), tributyltin (TBT), diphenyltin (DPT), triphenyltin (TPT), dioctyltin (DOT) and trioctyltin (TOT) were quantified in sediment samples from the upper flanks of the canyon and from the adjacent coastal area. TBT levels detected in the canyon flanks are about two to three orders of magnitude lower than those found in the coastal area. Nevertheless, when quantifiable. TBT levels in the canyon samples were higher than the Environmental Assessment Criteria set for TBT in sediments by the OSPAR Commission indicating that at those locations negative ecological impacts are likely to occur. (C) 2011 Elsevier Ltd. All rights reserved.
• Brominated flame retardants and polychlorinated biphenyls in human breast milk from several locations in India: Potential contaminant sources in a municipal dumping site

  Gnanasekaran Devanathan, Annamalai Subramanian, Agus Sudaryanto, Shin Takahashi, Tomohiko Isobe, Shinsuke Tanabe

  ENVIRONMENT INTERNATIONAL 39 (1) 87 - 95 0160-4120 2012/02 Scientific journal 

  This study investigated the status of contamination of organohalogen compounds (OCs) such as polychlorinated biphenyls (PCBs) and brominated flame retardant (BFRs), including polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs) in human milk samples from several locations in India. The levels of OCs were significantly higher in the milk of mothers living in and near municipal dumping site than other locations indicating that the open dumping sites for municipal wastes act as potential sources of these contaminants in India. The PCB concentrations observed in this study tended to decrease compared to those in the matched locations reported previously, probably due to the restriction of technical PCB usage in India. PBDE levels in human milk were two to three folds lower than those of PCBs in all the sampling locations investigated. Congener profiles of PCBs and PBDEs were different between samples from the dumping site mothers and general populations in other areas suggesting the presence of region-specific sources and pathways. HBCDs were detected in human milk from only two sites, with much lower concentrations and detection frequencies compared to PCBs and PBDEs. When hazard quotients (HQs) of PCBs and PBDEs were estimated for infant health risk, the HQs in some milk samples from the dumping site exceeded the threshold value (HQ>1) of PCBs, indicating the potential risk for infants in the specific site. (C) 2011 Elsevier Ltd. All rights reserved.
• Bioaccumulation of trace elements in marine organisms from deep-waters of Off-Sanninn and Off-Hokuriku, Japan

  Adachi, H, Itai, T, Takahashi, S, Kubodera, T, Haruta, S, Tanabe, S

  Interdisciplinary Studies on Environmental Chemistry 6 2012 [Peer-reviewed]
   International conference proceedings
• Applicability of human hair as a bioindicator for trace elements exposure

  Noguchi, T, Itai, T, Kawaguchi, M, Takahashi, S, Tanabe, S

  Interdisciplinary Studies on Environmental Chemistry 6 2012 [Peer-reviewed]
   International conference proceedings
• Toxic metals derived from plastic litter on a beach

  Nakashima, E, Isobe, A, Kako, S, Itai, T, Takahashi, S

  Interdisciplinary Studies on Environmental Chemistry 6 2012 [Peer-reviewed]
   International conference proceedings
• A comparative study on temporal trends of trace elements in harbor porpoise (Phocoena phocoena) from coastal waters of North Japan

  Yasuda Y, Hirata S, Itai T, Isobe T, Matsuishi T, Yamada TK, Tajima Y, Takahashi S, Tanabe S

  Interdisciplinary Studies on Environmental Chemistry-Environmental Pollution and Ecotoxicology 151 - 159 2012 [Peer-reviewed]
   International conference proceedings 

  Proceedings of interdisciplinary studies on environmental chemistry Vol. 6 Environmental pollution and ecotoxicology, Eds., M. Kawaguchi, K. Misaki, H. Sato, T. Yokokawa, T. Itai, T. M. Nguyen, J. Ono and S. Tanabe
• Individual variations in arsenic metabolism in Vietnamese: the association with arsenic exposure and GSTP1 genetic polymorphism

  Tetsuro Agusa, Takashi Kunito, Nguyen Minh Tue, Vi Thi Mai Lan, Junko Fujihara, Haruo Takeshita, Tu Binh Minh, Pham Thi Kim Trang, Shin Takahashi, Pham Hung Viet, Shinsuke Tanabe, Hisato Iwata

  METALLOMICS 4 (1) 91 - 100 1756-5901 2012 Scientific journal 

  We investigated the association of As exposure and genetic polymorphism in glutathione S-transferase pi 1 (GSTP1) with As metabolism in 190 local residents from the As contaminated groundwater areas in the Red River Delta, Vietnam. Total As concentrations in groundwater ranged from <0.1 to 502 mu g l(-1). Concentrations of dimethylarsinic acid (DMA(V)), monomethylarsonic acid (MMA(V)), and arsenite (As(III)) in human urine were positively correlated with total As levels in the groundwater, suggesting that people in these areas may be exposed to As through the groundwater. The concentration ratios of urinary As(III) /arsenate (As(V)) and MMA(V) /inorganic As (IA; As(III) + As(V))(M/I), which are indicators of As metabolism, increased with the urinary As level. Concentration and proportion of As(III) were high in the wild type of GSTP1 Ile105Val compared with the hetero type, and these trends were more pronounced in the higher As exposure group (>56 mu g l(-1) creatinine in urine), but not in the lower exposure group. In the high As exposure group, As(III)/As(V) ratios in the urine of wild type of GSTP1 Ile105Val were significantly higher than those of the hetero type, while the opposite trend was observed for M/I. These results suggest that the excretion and metabolism of IA may depend on both the As exposure level and the GSTP1 Ile105Val genotype.
• Identification of Major Dioxin-Like Compounds and Androgen Receptor Antagonist in Acid-Treated Tissue Extracts of High Trophic-Level Animals

  Go Suzuki, Nguyen M. Tue, Sander van der Linden, Abraham Brouwer, Bart van der Burg, Martin van Velzen, Marja Lamoree, Masayuki Someya, Shin Takahashi, Tomohiko Isobe, Yuko Tajima, Tadasu K. Yamada, Hidetaka Takigami, Shinsuke Tanabe

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 45 (23) 10203 - 10211 0013-936X 2011/12 Scientific journal 

  We evaluated the applicability of combining in vitro bioassays with instrument analyses to identify potential endocrine disrupting pollutants in sulfuric acid-treated extracts of liver and/or blubber of high trophic-level animals. Dioxin-like and androgen receptor (AR) antagonistic activities were observed in Baikal seals, common cormorants, raccoon dogs, and finless porpoises by using a panel of rat and human cell-based chemical-activated luciferase gene expression (CALUX) reporter gene bioassays. On the other hand, no activity was detected in estrogen receptor alpha (ER alpha)-, glucocorticoid receptor (GR)-, progesterone receptor (PR)-, and peroxisome proliferator-activated receptor gamma 2 (PPAR gamma 2)-CALUX assays with the sample amount applied. All individual samples (n = 66) showed dioxin-like activity, with values ranging from 21 to 5500 pg CALUX-2,3,7,8-tetrachlorodibenzo-p-dioxin equivalent (TEQ)/g-lipid. Because dioxins are expected to be strong contributors to CALUX-TEQs, the median theoretical contribution of dioxins calculated from the result of chemical analysis to the experimental CALUX-TEQs was estimated to explain up to 130% for all the tested samples (n = 54). Baikal seal extracts (n = 31), but not other extracts, induced AR antagonistic activities that were 8-150 mu g CALUX-flutamide equivalent (FluEQ)/g-lipid. p,p'-DDE was identified as an important causative compound for the activity, and its median theoretical contribution to the experimental CALUX-FluEQs was 59% for the tested Baikal seal tissues (n = 25). Our results demonstrate that combining in vitro CALUX assays with instrument analysis is useful for identifying persistent organic pollutant-like compounds in the tissue of wild animals on the basis of in vitro endocrine disruption toxicity.
• Human exposure to PCBs, PBDEs and HBCDs in Ghana: Temporal variation, sources of exposure and estimation of daily intakes by infants

  Kwadwo Ansong Asante, Sam Adu-Kumi, Kenta Nakahiro, Shin Takahashi, Tomohiko Isobe, Agus Sudaryanto, Gnanasekaran Devanathan, Edith Clarke, Osmund Duodu Ansa-Asare, Stephen Dapaah-Siakwan, Shinsuke Tanabe

  ENVIRONMENT INTERNATIONAL 37 (5) 921 - 928 0160-4120 2011/07 Scientific journal 

  Human exposure to polychlorinated biphenyls (PCBs) and brominated flame retardants (BFRs) such as polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs) was evaluated in Ghana using breast milk samples collected in 2004 and 2009. Mean levels and ranges of PBDEs (4.5; 0.86-18 ng/g lw) and PCBs (62; 15-160 ng/g lw) observed in the present study were unexpectedly high, in spite of the fact that Ghana is a non-industrialized country when compared with many of the Asian and European countries. Significant increases were found in the concentrations of PCBs and PBDEs over the years, while no significant increase was observed for HBCDs. Estimated hazard quotient (HQ) showed that all the mothers had HQ values exceeding the threshold of 1 for PCBs, indicating potential health risk for their children. PCBs in dirty oils and obsolete equipment should be of concern as potential sources in Ghana, and e-waste recycling with little or no experience in safe handling could be a threat to this sub-region noted for unregulated disposal of e-waste. The results may point towards an increase in trends in human milk in Ghana, especially in the larger cities but further analysis would be required to confirm this upward trend in levels. This is the first study to report BFRs in human breast milk from Africa, and undoubtedly from Ghana. (C) 2011 Elsevier Ltd. All rights reserved.
• Characterization of polychlorinated biphenyls and brominated flame retardants in surface soils from Surabaya, Indonesia

  Muhammad Ilyas, Agus Sudaryanto, Iwan Eka Setiawan, Adi Slamet Riyadi, Tomohiko Isobe, Shohei Ogawa, Shin Takahashi, Shinsuke Tanabe

  CHEMOSPHERE 83 (6) 783 - 791 0045-6535 2011/04 Scientific journal 

  In this study, soil contamination by PCBs, PBDEs, HBCDs and two novel BFRs such as 1,2-bis-(2,4,6-tribromopenoxy) ethane (BTBPE) and decabromodiphenyl ethane (DBDPE) in various locations such as industrial, urban, rural, dumping site and agricultural areas of Surabaya, Indonesia has been characterized in order to evaluate their contamination status, profiles, potential sources, fate and behavior. Range and median concentrations of PCBs, PBDEs, HBCDs, BTBPE and DBDPE were ND - 9.6(1.2), 0.069 - 24(7.4). ND - 1.8 (0.48), ND - 1.7 (0.14) and ND - 7.6 (2.2) ng g(-1) dw, respectively. Industrial, urban and dumping areas were inventoried as the main sources of these pollutants. Decreasing gradient levels were observed for these contaminants from industrial district, urban, dumping site, rural and agricultural areas, in that order. Furthermore, organic carbon contents and proximity to the point sources were found as the major controlling factors. Contaminant profiles were characterized by the predominance of hexa-, hepta- and penta-homologues for PCBs; deca-, nona- and octa- for PBDEs and a-isomer for HBCDs. Product mixtures such as Ar1260/KC600 and Ar1254/KC500 for PCBs, deca- and octa-BDEs for PBDEs were the possible common formulations used in study area. To our knowledge, this is a first comprehensive study on characterization of soil contamination by PCBs, PBDEs and HBCDs together with two novel BFRs in a highly industrialized city located in tropical region. This study provides baseline information for establishing national monitoring programs in Indonesia. (C) 2011 Elsevier Ltd. All rights reserved.
• Process study on numerical simulation for persistent organic pollutants in the East China Sea.

  Ono, J, Takahashi, D, Guo, X, Takahashi, S, Takeoka, H

  Interdisciplinary Studies on Environmental Chemistry, Vol. 5, Modeling and Analysis of Marine Environmental Problems 197 - 204 2011/03 [Peer-reviewed]
   International conference proceedings
• Toxic metals in polyethylene plastic litter

  Nakashima, E, Isobe, A, Kako, S, Magome, S, Deki, N, Itai, T, Takahashi, S

  Interdisciplinary Studies on Environmental Chemistry 5 271 - 277 2011 [Peer-reviewed]
   International conference proceedings
• Assessment of persistent organic pollutants in sediments from Lower Mekong River Basin

  Agus Sudaryanto, Tomohiko Isobe, Shin Takahashi, Shinsuke Tanabe

  CHEMOSPHERE 82 (5) 679 - 686 0045-6535 2011/01 Scientific journal 

  Organochlorine compounds (OCs) in sediments collected from various locations in Lower Mekong River Basin (MRB) in Laos and Thailand were examined to elucidate their occurrence, distribution and potential ecological risk. Concentration of PCBs and DDTs were higher than other OCs, ranging from 0.18 to 310 mu g kg(-1) dry wt. and from 0.027 to 52 mu g kg(-1) dry wt., respectively, whereas CHLs, HCHs and HCB were 1-3 orders of magnitude lower. Geographical distribution indicates that levels of PCBs, DDTs and CHLs in the Vientiane canal were significantly higher than those in mainstream of Mekong River, Phong River and its surrounding areas, indicating significant sources of these compounds in urbanized areas. Comparison with other parts of MRB indicates that PCBs were higher in Laos, whereas DDTs were more prevalent in Mekong Delta, indicating location specific contaminations of these compounds in MRB. The ratios of DDTs composition indicate possible difference in the historical input of DDT among locations in and around Mekong River. Hazard assessment of PCBs and DDTs indicate possible toxic potential particularly in areas close to point sources such as intensive human activities and agricultural areas which highlight the need for further study. (C) 2010 Elsevier Ltd. All rights reserved.
• Characterization of polychlorinated biphenyls and brominated flame retardants in sediments from riverine and coastal waters of Surabaya, Indonesia

  Muhammad Ilyas, Agus Sudaryanto, Iwan Eka Setiawan, Adi Slamet Riyadi, Tomohiko Isobe, Shin Takahashi, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 62 (1) 89 - 98 0025-326X 2011/01 Scientific journal 

  A total of 33 surficial sediments from riverine and coastal waters from Surabaya, Indonesia were analyzed for PCBs and BFRs. Concentrations of PCBs (62 congeners), PBDEs (14 congeners) and HBCDs (3 isomers) varied from <DL-420, <DL-35 and <DL-5.4 ng g(-1) dw, respectively. Higher concentrations of these compounds were found in riverine than coastal sediments. Their levels and distribution were influenced by proximity to the point sources and TOC. The predominant congeners were CB-153, -28, -138, -149, -180, -33 and BDE-209, -207, -206, -197, -196, -183, -99, -47 for PCBs and PBDEs, respectively, and gamma-isomer for HBCDs. Debromination of BDE-209 might be taking place producing lower toxic congeners in sediment. Levels of PCBs in riverine sediments were comparable with some polluted areas worldwide, but PBDEs and HBCDs were lower. Hazard assessment of PCBs indicated possible toxic potential, particularly in areas close to point sources. (C) 2010 Elsevier Ltd. All rights reserved.
• Contamination status and spatial distribution of organochlorine compounds in fishes from Nansei Islands, Japan

  Govindan Malarvannan, Shin Takahashi, Tokutaka Ikemoto, Tomohiko Isobe, Tatsuya Kunisue, Agus Sudaryanto, Toshihiko Miyagi, Masaru Nakamura, Shigeki Yasumura, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 63 (5-12) 541 - 547 0025-326X 2011 Scientific journal 

  Two species of fishes (n =52; tilapia and mullet) from industrialized and urbanized areas of Okinawa Island (Manko-Noha river, Hija river and Shikaza river) and from a remote area of Ishigaki Island (Anparu mudflat), Japan were collected between August 2005 and July 2006, and analyzed for five organochlorine compounds (OCs), viz., DDTs, PCBs, CHLs, HCHs and HCB. Concentrations and the contamination patterns of OCs in fishes varied between locations. Considerable residue levels of OCs, especially CHLs and DDTs were found in both fishes from the main Okinawa Island. These levels were relatively higher than the reported values for seafood from Japanese coasts, indicating that even now pollution sources of these contaminants still exist in this region. On the other hand, lower concentrations of OCs were detected in fishes from Ishigaki Island waters than those of other Japanese coastal waters, suggesting that this region is less contaminated by OC contaminants. (C) 2011 Elsevier Ltd. All rights reserved.
• Levels and distribution of polybrominated diphenyl ethers and organochlorine compounds in sea turtles from Japan

  Govindan Malarvannan, Shin Takahashi, Tomohiko Isobe, Tatsuya Kunisue, Agus Sudaryanto, Toshihiko Miyagi, Masaru Nakamura, Shigeki Yasumura, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 63 (5-12) 172 - 178 0025-326X 2011 Scientific journal 

  Three species of sea turtles (green. hawksbill and loggerhead turtles) stranded along the coasts or caught (by-catch) around Ishigaki Island and Kochi, Japan were collected between 1998 and 2006 and analyzed for six organohalogen compounds viz., PBDEs, PCBs, DDTs, CHLs, HCHs and HCB. The present study is the first and foremost to report the occurrence of organohalogen compounds in the sea turtles from Japan. Among the compounds analyzed, concentrations of PCBs, DDTs and CHLs were the highest in all the turtle samples. PBDEs were ubiquitously present in all the turtle species. Comparing with the other two species, concentrations of organohalogens in green turtle were relatively low and decreasing trend in the concentrations were noted with increasing carapace length. Concentrations of OCs in sea turtles from the coasts of Ishigaki Island and Kochi were relatively low as compared to those from other locations in the world. (C) 2011 Elsevier Ltd. All rights reserved.
• Evaluation of Dioxin-Like Activities in Settled House Dust from Vietnamese E-Waste Recycling Sites: Relevance of Polychlorinated/Brominated Dibenzo-p-Dioxin/Furans and Dioxin-Like PCBs

  Nguyen M. Tue, Go Suzuki, Shin Takahashi, Tomohiko Isobe, Pham T. K. Trang, Pham H. Viet, Shinsuke Tanabe

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 44 (23) 9195 - 9200 0013-936X 2010/12 Scientific journal 

  Few studies have investigated the human exposure to the ensemble of dioxin-related compounds (DRCs) released from uncontrolled e-waste recycling, especially from a toxic effect standpoint This study evaluated the TCDD toxic equivalents (TEQs) in persistent extracts of settled house dust from two Vietnamese e-waste recycling sites (EWRSs) using the Dioxin-Responsive Chemically Activated LUciferase gene eXpression assay (DR-CALUX), combined with chemical analysis of PCDD/Fs, DL-PCBs, PBDD/Fs, and monobromo PCDD/Fs to determine their TEQ contribution. The CALUX-TEQ levels in house dust ranged from 370 to 1000 pg g(-1) in the EWRSs, approximately 3.5-fold higher than in the urban control site. In EWRS house dust, the concentrations of the unregulated PBDFs were 7.7-63 ng g(-1), an order of magnitude higher than those of regulated DRCs (PCDD/Fs and DL-PCBs), and PBDFs were also principal CALUX-TEQ contributors (4.2-22%), comparable to PCDD/Fs (8.1-29%). The CALUX-TEQ contribution of DRCs varied, possibly depending on thermal processing activities (higher PCDD/F-TEQs) and PBDE content in the waste (higher PBDF-TEQs). However, the percentage of unknown dioxin-like activities was high in all dust samples, indicating large contribution from unidentified DRCs and/or synergy among contaminants. Estimates of TEQ intake from dust ingestion suggest that children in the EWRSs may be adversely affected by DRCs from dust.
• Dioxin-like Activity in Japanese Indoor Dusts Evaluated by Means of in Vitro Bioassay and Instrumental Analysis: Brominated Dibenzofurans Are an Important Contributor

  Go Suzuki, Masayuki Someya, Shin Takahashi, Shinsuke Tanabe, Shin-ichi Sakai, Hidetaka Takigami

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 44 (21) 8330 - 8336 0013-936X 2010/11 Scientific journal 

  In our previous study, we demonstrated that dioxin-like activity in sulfuric-acid-treated extracts of Japanese indoor dust was higher than the activity in contaminated sediments. In the current study, we used high-performance liquid chromatography (HPLC) fractionation in combination with the dioxin-responsive chemical-activated luciferase gene expression (DR-CALUX) assay and gas chromatography-high-resolution mass spectrometry (GC-HRMS) to quantitatively evaluate dioxin-like compounds in indoor dusts. Selected four sulfuric-acid-treated extracts of indoor dusts were fractionated into seven fractions by means of HPLC with a nitrophenylpropylsilica column, and the activity in the first fraction of each extract was much higher than the activities in the other fractions. Therefore, each of the first fractions was further fractionated into 90 fractions by HPLC with an octadecylsilica column, and all the fractions were analyzed by means of the DR-CALUX assay. On the basis of elution characteristics, the active compounds in the fractions showing high activity were determined to be polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), coplanar polychlorinated biphenyls (Co-PCBs), and polychlorinated naphthalenes (PCNs), or supposed to be polybrominated dibenzo-p-dioxins and dibenzofurans (PBDD/Fs). These compounds in the 33 dusts extracts were quantified by means of GC-HRMS, and their median-based contributions of the theoretical CALUX-TEQs [2,3,7,8-tetrachlorodibenzo-p-dioxin (2,3,7,8-tetraCDD) equivalent] chemically calculated for PBDFs, PCDDs, PCDFs, non-ortho Co-PCBs, PCNs, and mono-ortho Co-PCBs to the experimental values (38-1400 pg/g, median 160 pg/g) were 17%, 14%, 8.8%, 0.98%, 0.10%, and 0.019%, respectively. Our results indicate that PBDFs, which are not internationally regulated dioxins, were important contributors to dioxin-like activity in Japanese dust and that further analysis of PBDFs in indoor dust is required so that the risk of exposure to these compounds via dust can be assessed.
• Kinetic differences of legacy organochlorine pesticides and polychlorinated biphenyls in Vietnamese human breast milk

  Nguyen Minh Tue, Agus Sudaryanto, Tu Binh Minh, Bui Hong Nhat, Tomohiko Isobe, Shin Takahashi, Pham Hung Viet, Shinsuke Tanabe

  CHEMOSPHERE 81 (8) 1006 - 1011 0045-6535 2010/11 Scientific journal 

  The present study investigated the current contamination status and evaluated several kinetic-related features of organochlorine pesticides (OCPs) and PCBs in human breast milk collected from northern Vietnam. The variation in the levels of these contaminants was found to be strongly associated with total lactation time and dietary habits. OCPs exhibited the characteristics of steadily declining compounds: the overall levels of DDTs and HCHs in the population decreased with a half-time of only 5 years and it can be suggested that OCPs depurated relatively fast with breastfeeding (5% per month). PCBs were slower in both regards, with a temporal decrease half-time of 12 years and a suggested depuration rate via breastfeeding of 2.5% per month, indicating that the exposure level was still high relative to the human body burden. It was found that the PCB exposure levels of infant from breastfeeding exceeded the reference dose, and this situation may continue for the next two or three decades. Knowledge of these kinetic-related characteristics not only is useful for risk assessment and prediction of future trends of legacy contaminants but also may provide insight regarding similar kinetic processes of emerging persistent pollutants. (C) 2010 Elsevier Ltd. All rights reserved.
• Organotin Compounds, Including Butyltins and Octyltins, in House Dust from Albany, New York, USA

  Kurunthachalam Kannan, Shin Takahashi, Naohiro Fujiwara, Hazuki Mizukawa, Shinsuke Tanabe

  ARCHIVES OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY 58 (4) 901 - 907 0090-4341 2010/05 Scientific journal 

  Organotin compounds (OTs) have been used in a wide variety of consumer products. Despite this, very few studies have reported the occurrence of OTs in house dust or exposure of humans to OTs through the ingestion of house dust. In the present study, concentrations of monobutyltin (MBT), dibutyltin (DBT), tributyltin (TBT), monooctyltin (MOT), dioctyltin (DOT), trioctyltin (TOT), diphenyltin (DPT), and triphenyltin (TPT) were measured in dust collected from 24 houses in Albany, New York, USA. In addition, a few household products, such as wallpaper, floor tile, vinyl window blinds, and handbags were analyzed for the presence of OTs. Organotins were found in all of the house dust samples analyzed, and total OT concentrations varied from 390 to 28,000 ng/g (mean +/- A SD: 6700 +/- A 6200; median: 5000). Relative abundances of OTs in house dust were in the order MBT > MOT > DBT > DOT > TBT. TOT, DPT, and TPT were not found in any of the samples at concentrations above their corresponding detection limits. MBT accounted for, on average, 51% of the total OT concentrations. Mean concentrations of total OTs found in house dust samples from our study were two to five times higher than concentrations that have been reported for dust samples from several European countries. Calculations indicate that dust ingestion by children account for, on average, 15-18% of the tolerable daily intake proposed by the World Health Organization (WHO). The estimated rates of OT intake by children via dust ingestion were, on average, eightfold higher than the intake rates calculated for adults. Household products, such as wallpaper, contained total OT concentrations as high as 780,000 ng/g.
• Polychlorinated Biphenyls and Their Hydroxylated Metabolites (OH-PCBs) in the Blood of Toothed and Baleen Whales Stranded along Japanese Coastal Waters

  Kei Nomiyama, Satoko Murata, Tatsuya Kunisue, Tadasu K. Yamada, Hazuki Mizukawa, Shin Takahashi, Shinsuke Tanabe

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 44 (10) 3732 - 3738 0013-936X 2010/05 Scientific journal 

  In this study, we determined the residue levels and patterns of polychlorinated biphenyls (PCBs) and hydroxylated PCBs (OH-PCBs) in the blood from eight species of toothed whales and three species of baleen whales stranded along the Japanese coast during 1999-2007. Penta- through hepta-chlorinated PCB congeners were the dominant homologue groups in all cetaceans. In contrast, specific differences in the distribution of dominant OH-PCB isomers and homologues were found among the cetacean species. In five species of toothed whales (melon-headed whale, Stejneger's beaked whale, Pacific white-sided dolphin, Blainville's beaked whale, and killer whale), the predominant homologues were OH-penta-PCBs followed by OH-tetra-PCBs and OH-tri-PCBs. The predominant homologues of finless porpoise and beluga whale were OH-penta-PCBs followed by OH-hexa-PCBs and OH-tri-PCBs. The predominant OH-PCB isomers were para-OH-PCBs such as 4'OH-CB26, 4'OH-CB25/4'OH-CB26/4OH-CB31, 4OH-CB70, 4'OH-CB72, 4'OH-CB97, 4'OH-CB101/4'OH-CB120, and 4OH-CB107/4'OH-CB108 in toothed whales. In three baleen whales (common minke whale, Bryde's whale, and humpback whale) and in sperm whale (which is a toothed whale), OH-octa-PCB (4OH-CB202) was the predominant homologue group accounting for 40-80% of the total OH-PCB concentrations. The differences in concentrations and profiles of OH-PCBs may suggest species-specific diets, metabolic capability, and the transthyretin (TTR) binding specificity. These results reveal that the accumulation profiles of OH-PCBs in cetacean blood are entirely different from the profiles found in pinnipeds, polar bear, and humans.
• Spatial distribution of polybrominated diphenyl ethers and hexabromocyclododecanes in sediments from coastal waters of Korea

  Karri Ramu, Tomohiko Isobe, Shin Takahashi, Eun-Young Kim, Byung-Yoon Min, Sung-Ug We, Shinsuke Tanabe

  CHEMOSPHERE 79 (7) 713 - 719 0045-6535 2010/04 Scientific journal 

  Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs) were determined in surface sediments collected from 24 coastal locations in Korea. The concentrations of Sigma(PBDEs) (defined as the sum of all targeted PBDE congeners except for BDE-209) and BDE-209 ranged from 0.05 to 32 ng g(-1) dry wt. and from 0.40 to 98 ng g(-1) dry wt., respectively. The PBDE congener compositions were dominated by BDE-209, which is in accordance with the consumption of decaBDE mixture in Korea. HBCD concentrations ranged from 0.39 to 59 ng g(-1) dry wt. Concentrations of PBDEs and HBCDs were found to be higher near locations with industrial complexes and harbors, associating these compounds to urbanization and industrialization. Significant positive correlations between PBDE and HBCD concentrations and organic carbon content in sediments imply the role played by organic matter in the contaminant transport and trapping in the aquatic environment. (C) 2010 Elsevier Ltd. All rights reserved.
• Accumulation of polychlorinated biphenyls and brominated flame retardants in breast milk from women living in Vietnamese e-waste recycling sites

  Nguyen Minh Tue, Agus Sudaryanto, Tu Binh Minh, Tomohiko Isobe, Shin Takahashi, Pham Hung Viet, Shinsuke Tanabe

  SCIENCE OF THE TOTAL ENVIRONMENT 408 (9) 2155 - 2162 0048-9697 2010/04 Scientific journal 

  This study investigated the contamination status of PCBs, PBDEs and HBCDs in human and possible exposure pathways in three Vietnamese e-waste recycling sites: Trang Minh (suburb of Hai Phong city), Dung Mai and Bui Dau (Hung Yen province), and one reference site (capital city Hanoi) by analysing human breast milk samples and examining the relationships between contaminant levels and lifestyle factors. Levels of PBDEs, but not PCBs and HBCDs, were significantly higher in Trang Minh and Bui Dau than in the reference site. The recyclers from Bui Dau had the highest levels of PBDEs (20-250 ng g(-1) lipid wt.), higher than in the reference group by two orders of magnitude and more abundant than PCBs (28-59 ng g(-1) lipid wt.), and were also the only group with significant exposure to HBCDs (1.4-7.6 ng g(-1) lipid wt.). A specific accumulation, unrelated to diet, of low-chlorinated PCBs and high-brominated PBDEs was observed in e-waste recyclers, suggesting extensive exposure to these compounds during e-waste recycling activities, possibly through inhalation and ingestion of dust. The estimated infant intake dose of PBDEs from breast milk of some mothers occupationally involved in e-waste recycling were close to or higher than the reference doses issued by the U.S. EPA. (C) 2010 Elsevier B.V. All rights reserved.
• Organohalogen compounds in deep-sea fishes from the western North Pacific, off-Tohoku, Japan: Contamination status and bioaccumulation profiles

  Shin Takahashi, Tomoko Oshihoi, Karri Ramu, Tomohiko Isobe, Koji Ohmori, Tsunemi Kubodera, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 60 (2) 187 - 196 0025-326X 2010/02 Scientific journal 

  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 N-15 (parts per thousand) and PCBs, DDTs and PBDEs suggest the high biomagnification potential of these contaminants in food web. The large variation in delta C-13 (parts 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. (C) 2009 Elsevier Ltd. All rights reserved.
• Biomagnification of arsenic species in the deep-sea ecosystem of the Sagami Bay, Japan

  Hayase, D, Agusa, T, Toyoshima, S, Takahashi, S, Hirata, S. H, Itai, T, Omori, K, Nishida, S, Tanabe, S

  Interdisciplinary Studies on Environmental Chemistry 4 199 - 204 2010 [Peer-reviewed]
   International conference proceedings
• Persistent organic pollutants in breast milk of mothers residing around an open dumping site in Kolkata, India: Specific dioxin-like PCB levels and fish as a potential source

  Masayuki Someya, Masako Ohtake, Tatsuya Kunisue, Annamalai Subramanian, Shin Takahashi, Paromita Chakraborty, Ramesh Ramachandran, Shinsuke Tanabe

  ENVIRONMENT INTERNATIONAL 36 (1) 27 - 35 0160-4120 2010/01 Scientific journal 

  Concentrations of persistent organic Pollutants (POPs) such as polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), polychlorinated biphenyls (PCBs) and organochlorine pesticides were measured in human breast milk collected from mothers residing near an open dumping site and a reference site in Kolkata, India during 2004-2005. POPs were detected in all the human milk samples analyzed, suggesting that residents of Kolkata are widely exposed to these contaminants. Concentrations of dioxin-like PCBs in the samples from the dumping site were significantly higher than in the reference site samples, whereas no such difference was found for PCDDs and PCDFs. In addition, significantly higher concentrations of total PCBs were also observed in the samples from the dumping site than the reference site. Interestingly, concentrations of total and dioxin-like PCBs in the breast milk of mothers from the dumping site significantly increased with the number of years of residence near the dumping site. These results indicate that significant pollution sources of PCBs are present in the dumping site of Kolkata and the residents living around are exposed to relatively higher levels of PCBs. When the residue levels of dioxins and related compounds in fish collected from ponds near the Kolkata dumping site and the reference site were measured, it was found that dioxin-like PCB and TEQ levels in fish from the dumping site were notably higher than those from the reference site. This result indicates that fish is a potential source of PCBs for residents living near the Kolkata dumping site. (C) 2009 Elsevier Ltd. All rights reserved.
• Temporal and spatial trends of organotin contamination in the livers of finless porpoises (Neophocaena phocaenoides) and their association with parasitic infection status

  Kei Nakayama, Chiho Matsudaira, Yuko Tajima, Tadasu K. Yamada, Motoi Yoshioka, Tomohiko Isobe, Shin Takahashi, Shinsuke Tanabe

  SCIENCE OF THE TOTAL ENVIRONMENT 407 (24) 6173 - 6178 0048-9697 2009/12 Scientific journal 

  Organotins (OTs) are globally ubiquitous contaminants. Contamination of OTs, particularly butyltins (BTs). has been suspected to Cause immunosuppressive effects leading to subsequent infectious diseases or opportunistic infection by pathogens in marine mammals. In the present study, we collected individuals from five different populations of finless porpoises (Neophocaena phocaenoides) from coastal areas of Japan (Seto Inland Sea, Ise Bay, Omura Bay, and Pacific coast) and Hong Kong. and measured OT concentrations in their livers. In addition, infection status of lung nematodes and liver trematodes was also observed to analyze the relationship between OT contamination and parasitic infection in finless porpoises. Hepatic OT concentrations were highest in the Hong Kong population, while levels in the Japanese populations were equivalent to those of other cetaceans from different locations. OT levels in Japan have been decreasing in the past few decades. while OT contamination has shown little improvement in Hong Kong. Observation of parasite infection in Seto Inland Sea porpoises revealed that 16 and 11 out of 22 individuals were infected by lung nematodes and liver trematodes, respectively. Additionally, a significant association between BT levels and parasitic infection status of lung nematodes was detected. Thus, the present study suggests that BTs could be a factor affecting parasitic infection. especially the presence or severity of lung nematodes in finless porpoises. Since chemical exposure may alter the susceptibility of organisms to infectious diseases. the interaction of chemical contamination with infectious diseases needs to be investigated in greater depth to understand the risk of population decline due to these factors in marine mammals. (C) 2009 Elsevier B.V. All rights reserved.
• Imposex and organotin prevalence in a European post-legislative scenario: Temporal trends from 2003 to 2008

  Ana Sousa, Filipe Laranjeiro, Shin Takahashi, Shinsuke Tanabe, Carlos M. Barroso

  CHEMOSPHERE 77 (4) 566 - 573 0045-6535 2009/10 Scientific journal 

  Imposex levels and organotin tissue concentrations were assessed in Nassarius reticulatus females collected between June and August 2008 at 23 sites along the Portuguese coast. Females with imposex were present at all sampling sites with highest levels inside main harbors. Imposex parameters across sampling stations varied between 6.3% and 100% for %I. 0.2-4.4 for VDSI, 0.1-7.8 mm for FPL 0.3-88.9% for RPLI and 0.0-1.1 for AOS. TBT levels varied between 3.5 and 380 ng Sn g(-1) dw, representing an average proportion of 50.4% of total butyltins (Sigma BTs = MBT + DBT + TBT). Sterile females were detected at two locations. Highly significant correlations between imposex and TBT levels were found. The efficacy of the EU legislation banning the use of TBT-based antifouling paints since 2003 (EC Regulation 782/2003) was evaluated by comparing the levels of imposex observed in 2008 with those reported for 2003. OTs tissue concentrations were also determined in preserved samples collected in 2003. There was a decrease in imposex and TBT tissue contamination between 2003 and 2008 indicating that a decline in TBT pollution has occurred in the Portuguese coast since the implementation of the legislation. Considering that the EC Regulation 782/2003 is an anticipation of the IMO AFS Convention, a global scale decrease in TBT pollution can be expected in the near future. Despite the rapid amelioration in the Portuguese coast, TBT pollution is still a problem as the Ecological Quality Objective (EcoQO) proposed by OSPAR Commission was not achieved in 91% of the surveyed sites. (C) 2009 Elsevier Ltd. All rights reserved.
• Development of a mathematical model for 3D-dynamics of persistent organic pollutant in the East China Sea.

  Ono, J, Takahashi, D, Guo, X, Takahashi, S, Takeoka, H

  Organohalogen Compounds 71 (2) 1314 - 1317 2009/08 [Peer-reviewed]
   Scientific journal
• Distribution of synthetic organotins and total tin levels in Mytilus galloprovincialis along the Portuguese coast

  Ana Sousa, Tokutaka Ikemoto, Shin Takahashi, Carlos Barroso, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 58 (8) 1130 - 1136 0025-326X 2009/08 Scientific journal 

  Despite the huge amount of literature available on butyltins (BuTs), few studies addressed the environmental levels of phenyltins (PhTs), octyltins (OcTs) and total tin (Sn-T) in environmental samples. In 2006 a mussel watch survey was developed for the Portuguese coast (total of 29 sampling sites) in order to describe the concentrations of BuTs, PhTs, OcTs and SnT in the whole tissues of Mytilus galloprovincialis (Lamarck, 1819). BuTs were detected in all analyzed samples accounting, in average, for 98.6% of total organotins (Sigma OTs = BuTs + PhTs + OcTs), and presented highest values in the vicinity of harbors. Tributyltin (TBT) was the dominant butyltin, representing, in average, 62% of Sigma BuTs (Sigma BuTs = TBT + DBT + MBT) suggesting that fresh inputs of TBT are still occurring in the Portuguese coast, particularly near harbors. The contribution of organotin compounds derived from antifouling paints to the total tin levels in M. galloprovincialis is discussed. (C) 2009 Elsevier Ltd. All rights reserved.
• Organohalogen contaminants in striped dolphins (Stenella coeruleoalba) from Japan: Present contamination status, body distribution and temporal trends (1978-2003)

  Tomohiko Isobe, Yoko Ochi, Karri Ramu, Takahito Yamamoto, Yuko Tajima, Tadasu K. Yamada, Masao Amano, Nobuyuki Miyazaki, Shin Takahashi, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 58 (3) 396 - 401 0025-326X 2009/08 Scientific journal 

  Organohalogen contaminants including PCBs, DDTs, CHLs, HCHs, HCB, PBDEs and HBCDs were determined in striped dolphins (Stenella coeruleoalba) found stranded at Gogo-shima (n = 6, 2003) and collected from Taiji (n = 15, 1978-1992) in Japan. All target compounds were significantly detected in all the specimens, indicating ubiquitous contamination of oceanic cetaceans in northwest Pacific Ocean. Examination of body distribution of organohalogens in the six specimens from Gogo-shima showed no significant difference in concentrations among the analyzed tissues, except for brain, which had lower levels possibly due to the existence of blood-brain barrier. For evaluating temporal trends, archived blubber samples of adult male stripped dolphins collected in 1978,1979,1986 and 1992 were analyzed. Concentrations of PCBs, DDTs and HCHs did not change significantly during 1978-2003. In contrast, remarkable increasing trends of PBDEs and HBCDs were observed, suggesting growing consumption in Japan and surrounding countries in recent years. (C) 2008 Elsevier Ltd. All rights reserved.
• Contamination by trace elements at e-waste recycling sites in Bangalore, India

  Nguyen Ngoc Ha, Tetsuro Agusa, Karri Ramu, Nguyen Phuc Cam Tu, Satoko Murata, Keshav A. Bulbule, Peethmbaram Parthasaraty, Shin Takahashi, Annamalai Subramanian, Shinsuke Tanabe

  CHEMOSPHERE 76 (1) 9 - 15 0045-6535 2009/06 Scientific journal 

  The recycling and disposal of electronic waste (e-waste) in developing countries is causing an increasing concern due to its effects on the environment and associated human health risks. To understand the contamination status, we measured trace elements (TEs) in soil, air dust, and human hair collected from e-waste recycling sites (a recycling facility and backyard recycling units) and the reference sites in Bangalore and Chennai in India. Concentrations of Cu, Zn, Ag, Cd, In, Sn, Sb, Hg, Pb, and Bi were higher in soil from e-waste recycling sites compared to reference sites. For Cu, Sb, Hg, and Pb in some soils from e-waste sites, the levels exceeded screening values proposed by US Environmental Protection Agency (EPA). Concentrations of Cr, Mn, Co, Cu, In, Sn, Sb, Tl, Pb and Bi in air from the e-waste recycling facility were relatively higher than the levels in Chennai city. High levels of Cu, Mo, Ag, Cd, In, Sb, Tl, and Pb were observed in hair of male workers from e-waste recycling sites. Our results suggest that e-waste recycling and its disposal may lead to the environmental and human contamination by some TEs. To our knowledge, this is the first study on TE contamination at e-waste recycling sites in Bangalore, India. (C) 2009 Elsevier Ltd. All rights reserved.
• Organohalogen compounds in human breast milk from mothers living in Payatas and Malate, the Philippines: Levels, accumulation kinetics and infant health risk

  Govindan Malarvannan, Tatsuya Kunisue, Tomohiko Isobe, Agus Sudaryanto, Shin Takahashi, Maricar Prudente, Annamalai Subramanian, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 157 (6) 1924 - 1932 0269-7491 2009/06 Scientific journal 

  Human breast milk samples (n = 33) from primipara and multipara mothers from Payatas a waste dump site, and Malate a reference site in the Phillipines were collected in 2004 and analyzed for eight organohalogen compounds, viz., PCBs, DDTs, CHLs, HCHs, HCB, TCPMe, PBDEs and HBCDs. DDTs and PCBs were predominant in all the samples. Overall mean concentrations of PBDEs found in our study were higher (7.5 ng/g lipid wt.) than those reported for Japan and many other Asian countries. Primipara mothers had significantly higher levels of DDTs, CHLs and HCHs than multipara mothers, but not PBDEs and HBCDs. A few individuals accumulated CHLs close to or even higher than the tolerable daily intake guidelines proposed by Health Canada. (C) 2009 Elsevier Ltd. All rights reserved.
• Polybrominated, polychlorinated and monobromo-polychlorinated dibenzo-p-dioxins/dibenzofurans and dioxin-like polychlorinated biphenyls in marine surface sediments from Hong Kong and Korea

  Hidenori Terauchi, Shin Takahashi, Paul K. S. Lam, Byung-Yoon Min, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 157 (3) 724 - 730 0269-7491 2009/03 Scientific journal 

  In this study we investigated occurrences and distribution patterns of dioxin-related compounds (DRCs) such as polybrominated dibenzo-p-dioxins/dibenzofurans (PBDD/Fs), polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs), monobromo-polychlorinated dibenzo-p-dioxins/dibenzofurans (MoBPCDD/Fs) and dioxin-like polychlorinated biphenyls (DL-PCBs) in marine surface sediments collected from the coastal waters of Hong Kong and Korea. In most sampling sites, concentrations of PCDDs were the highest, followed by DL-PCBs, PCDFs, PBDFs, PBDDs, MoBPCDDs and MoBPCDFs in this order. Levels of PBDD/Fs were generally 1-2 orders of magnitude lower than chlorinated analogues. Levels of PCDDs are higher than PCDFs in Hong Kong while levels of PBDFs are higher than PBDDs in Korea (p < 0.05). Report of PBDD/Fs and MoBPCDD/Fs in sediments from East Asian countries is novel and original. Environmental levels of PBDD/Fs are supposed to start increasing in accordance with rising production, use and disposal of brominated flame retardants (BFRs) and recycling processes of e-waste in Asian developing countries. (C) 2008 Elsevier Ltd. All rights reserved.
• Accumulation features and temporal trends of PCDDs, PCDFs and PCBs in Baikal seals (Pusa sibirica)

  Daisuke Imaeda, Tatsuya Kunisue, Yoko Ochi, Hisato Iwata, Oyuna Tsydenova, Shin Takahashi, Masao Amano, Evgeny A. Petrov, Valeriy B. Batoev, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 157 (3) 737 - 747 0269-7491 2009/03 Scientific journal 

  This study investigated the accumulation features and temporal trends of PCDD/Fs, dioxin-like PCBs (DL-PCBs) and non-dioxin-like PCBs (NDL-PCBs) in the blubber of Baikal seals collected in 1992 and 2005. DL-PCBs (480-3600 ng/g) and NDL-PCBs (980-35,000 ng/g) were dominant contaminants. Concentrations of PCDDs and PCBs in males were significantly higher than in females. In males, age-dependent accumulation was observed for PCDDs, mono-ortho PCBs and NDL-PCBs. PCDFs and non-ortho PCBs showed no such trends, implying that exposure of seals to these contaminants has been decreasing in recent years. No decreasing temporal trend was observed for PCDDs, mono-ortho PCBs and NDL-PCBs, suggesting that Baikal seals are still exposed to PCDDs and PCBs. TEQs of PCDDs and mono-ortho PCBs in seals collected in 2005 accounted for 62-77% of total TEQs. The TEQ levels in 40% of the specimens exceeded the threshold level for immunosuppression observed in harbor seals (209 pg/g). (C) 2008 Elsevier Ltd. All rights reserved.
• Goiter-Like Changes in the Thyroid Gland of Mass Stranded Striped Dolphins (Stenella coeruleoalba)

  真柄真実, 田島木綿子, 山田格, 磯部友彦, 高橋真, 田辺信介, 島田章則

  日本獣医師会雑誌 62 (2) 155 - 160 0446-6454 2009/02 

  2003年3月、愛媛県興居島にて7頭のスジイルカ（Stenella coeruleoalba）が集団座礁し、そのうち6頭について全身解剖および病理組織学的検索を行った。体長などからいずれも成体であることが推測された。各個体の直接的な死因は、肺における重度のうっ血水腫と思われるが、これらの症例に共通する漂着の原因を示す所見は確定できなかった。2例の甲状腺に、コロイドの大量貯留による濾胞拡張および結節形成を伴う、いわゆる甲状腺腫に類似した所見が認められた。脂皮内の有機ハロゲン化合物の分析の結果は、日本国内でこれまで報告されている海棲哺乳類における蓄積パターンとおおむね一致していた。一部の有機ハロゲン化合物の高濃度の蓄積が認められた。
• Goiter-Like Changes in the Thyroid Gland of Mass Stranded Striped Dolphins (Stenella coeruleoalba)

  真柄真実, 田島木綿子, 山田格, 磯部友彦, 高橋真, 田辺信介, 島田章則

  日本獣医師会雑誌 日本獸医師会 62 (2) 155 - 160 0446-6454 2009/02 

  2003年3月、愛媛県興居島にて7頭のスジイルカ（Stenella coeruleoalba）が集団座礁し、そのうち6頭について全身解剖および病理組織学的検索を行った。体長などからいずれも成体であることが推測された。各個体の直接的な死因は、肺における重度のうっ血水腫と思われるが、これらの症例に共通する漂着の原因を示す所見は確定できなかった。2例の甲状腺に、コロイドの大量貯留による濾胞拡張および結節形成を伴う、いわゆる甲状腺腫に類似した所見が認められた。脂皮内の有機ハロゲン化合物の分析の結果は、日本国内でこれまで報告されている海棲哺乳類における蓄積パターンとおおむね一致していた。一部の有機ハロゲン化合物の高濃度の蓄積が認められた。
• Radionuclide (Cs-137 and K-40) concentrations in the muscle of Baikal seal (Pusa sibirica) from Lake Baikal

  M. Udaka, T. Ikemoto, H. Zenke, S. Takahashi, V. B. Batoev, E. A. Petrov, S. Tanabe

  MARINE POLLUTION BULLETIN 58 (2) 290 - 294 0025-326X 2009/02 Scientific journal
• Persistent organochlorines in human breast milk from major metropolitan cities in India

  Gnanasekaran Devanathan, Annamalai Subramanian, Masayuki Someya, Agus Sudaryanto, Tomohiko Isobe, Shin Takahashi, Paromita Chakraborty, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 157 (1) 148 - 154 0269-7491 2009/01 Scientific journal 

  The present study was carried out to understand the current contamination status of organochlorine compounds (OCs) in human breast milk from three metropolitan cities in India (New Delhi, Mumbai and Kolkata). Among the OCs analyzed, DDTs were predominant followed by HCHs and PCBs. CHLs and HCB levels were much lower. Contamination patterns were different in human milk found in our previous study in Chennai, a metropolitan city in southern India, indicating region specific exposure routes and variable sources. In comparison with previous data, levels of DDTs and HCHs generally declined with time, implying the effect of various bans and restrictions on their usage. No association between concentrations of OCs and demographic characteristics such as parity and age of mothers was observed which might be due to narrow range of mother's age. Estimated daily intake shows that some infants are exposed to OCs to a greater extent, particularly HCHs than the guideline standard. (C) 2008 Elsevier Ltd. All rights reserved.
• Spatial and temporal evolution of imposex in dogwhelk Nucella lapillus (L.) populations from North Wales, UK

  Isabel Benta Oliveira, Christopher Allan Richardson, Ana Catarina Sousa, Shin Takahashi, Shinsuke Tanabe, Carlos Miguez Barroso

  JOURNAL OF ENVIRONMENTAL MONITORING 11 (8) 1462 - 1468 1464-0325 2009 Scientific journal 

  Nucella lapillus imposex and organotin tissue contamination were assessed, during 2006, at twenty sites in North Wales, between Anglesey and Shell Island on the Lleyn Peninsula. Vas Deferens Sequence Index (VDSI), Relative Penis Size Index (RPSI) and the percentage of affected females (%I) were used to assess imposex levels which varied between 0.5 and 3.8 for VDSI, 0.0 and 11.5% for RPSI and 49 and 100% for %I. Tributyltin (TBT) and triphenyltin (TPT) concentrations in whole tissues varied between 0.8 and 39 and 0.4 and 2.1ng Sn/g dry weight, respectively. TBT represented the higher fraction of butyltin compounds in the tissues, suggesting that TBT inputs continue to occur. Comparisons with nineteen years of data collected during previous studies demonstrated that there had been a significant reduction in imposex levels over the last two decades following the introduction of legislative restrictions in the U. K. regarding the use of organotin based antifouling paints.
• Hexabromocyclododecanes in human adipose tissue from Japan

  Tomohiko Isobe, Hiroko Oda, Nozomi Takayanagi, Tatsuya Kunisue, Hiroaki Komori, Norimasa Arita, Norifumi Ueda, Masato Nose, Taketo Yamada, Shin Takahashi, Shinsuke Tanabe

  ENVIRONMENTAL CHEMISTRY 6 (4) 328 - 333 1448-2517 2009 Scientific journal 

  Residue levels of hexabromocyclododecanes (HBCDs) were measured using LC-MS/MS in the Japanese human adipose tissue samples collected during 2003-2004 from Ehime prefecture (n=26) and Kanto region (n = 9) of Japan. Concentrations of HBCDs (0.85 39 ng g(-1) lipid) in the adipose tissue samples were 1 2 orders of magnitude lower than those of organochlorines (OCs). Regional differences between HBCD levels in Ehime prefecture and Kanto region were not significant. No age-dependent accumulation of HBCDs was observed. HBCD levels in men were significantly higher than those in women. Significant positive correlation between polybrominated diphenyl ethers (PBDEs) and HBCDs implies similar routes of exposure to these contaminants for Japanese citizens. alpha-HBCD was predominant among the three isomers, which is consistent with the other reports on bioaccumulation of alpha-HBCD in higher trophic animals.
• バイカルアザラシ(Pusa sibirica)の肝臓および筋肉における微量元素の蓄積特性

  宇高真行, 池本徳孝, 高橋真, 岩田久人, BATOEV Valeriy B, PETROV Evgeny A, 田辺信介

  環境毒性学会誌 11 (2) 117 - 131 1344-0667 2008/12
• バイカルアザラシ(Pusa sibirica)の肝臓および筋肉における微量元素の蓄積特性

  宇高真行, 池本徳孝, 高橋真, 岩田久人, BATOEV Valeriy B, PETROV Evgeny A, 田辺信介

  環境毒性学会誌 日本環境毒性学会 11 (2) 117 - 131 1344-0667 2008/12
• Trace elements and stable isotopes (delta C-13 and delta N-15) in shallow and deep-water organisms from the East China Sea

  Kwadwo Ansong Asante, Tetsuro Agusa, Hiroko Mochizuki, Karri Ramu, Suguru Inoue, Tsunemi Kubodera, Shin Takahashi, Annamalai Subramanian, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 156 (3) 862 - 873 0269-7491 2008/12 Scientific journal 

  Trace elements (22) and stable isotope ratios (delta N-15 and delta C-13) were analyzed in marine organisms from shallow (SW) and deep-water (DW) of the East China Sea to understand biomagnification and prey source of trace elements. In the benthic marine organisms from DW, delta N-15 values were negatively correlated with Ba, Cu, Ag, Mo, Sr, As. and Co concentrations. This may be due to the specific accumulation in lower trophic animals and/or the biodilution through the food web in DW. Relationships between delta N-15 and concentrations of Co, Cr, Bi, and Tl in fish and Ag, Bi, V, Hg, and Tl in crustaceans showed positive correlations, suggesting that trophic position was affecting the concentrations of those elements in phyla, with higher trophic animals retaining higher concentrations than the lower trophic animals. Positive correlations between delta C-13 and Rb were observed in marine organisms. Therefore, Rb may be a possible substitute of delta C-13 as tracer of prey source in the East China Sea although further investigation is required. (C) 2008 Elsevier Ltd. All rights reserved.
• Levels and congener specific profiles of PBDEs in human breast milk from China: Implication on exposure sources and pathways

  Agus Sudaryanto, Natsuko Kajiwara, Oyuna V. Tsydenova, Tomohiko Isobe, Hongxia Yu, Shin Takahashi, Shinsuke Tanabe

  CHEMOSPHERE 73 (10) 1661 - 1668 0045-6535 2008/11 Scientific journal 

  Fourteen PBDE congeners from mono- to deca-BDE were determined in breast milk of primiparous mothers from two locations in East China, i.e. Nanjing (n =9), an urban area, and Zhoushan (n - 10). a semi rural coastal area. PBDEs were detected in all the human breast milk samples of the present study, indicating that general Population in these two locations are widely exposed to these pollutants. Relatively higher concentrations of PBDEs were found in the milk of mothers from Nanjing than Zhoushan, suggesting the existence of significant sources of PBDEs in urban areas. PBDE levels in the present study were similar to those in European countries, but one or two orders of magnitude lower than in North America. Except for BDE-3, all congeners from di- to deca-BDE were detected in the samples of the present study. BDE-209, a congener considered to have less bioavailability, was detected in about 50% of the samples at concentrations higher than that of other congeners. Other higher brominated congeners, such as BDE-153, -197 and -207, were also prominent in the present study, which is different from the pattern generally observed in previous studies on human milk as well as biota samples. These results may indicate that the inhabitants of Nanjing and Zhoushan are exposed to location specific sources of PBDEs. (C) 2008 Elsevier Ltd. All rights reserved.
• Passive Atmospheric Sampling of Organochlorine Pesticides, Polychlorinated Biphenyls, and Polybrominated Diphenyl Ethers in Urban, Rural, and Wetland Sites along the Coastal Length of India

  Gan Zhang, Paromita Chakraborty, Jun Li, Pichai Sampathkumar, Thangavel Balasubramanian, Kandasamy Kathiresan, Shin Takahashi, Annamalai Subramanian, Shinsuke Tanabe, Kevin C. Jones

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 42 (22) 8218 - 8223 0013-936X 2008/11 Scientific journal 

  India is of prime interest due to the large past and ongoing use of pesticidal persistent organic pollutants (POPS). Rapid dissipation of POPS to the atmosphere in the tropical climate of India infers an atmospheric outflow of these chemicals. Yet data on POPS in the atmosphere of India are sparse. Passive air samplers consisting of polyurethane foam disks were therefore deployed concurrently at 18 locations and exposed for 6 weeks from July 30, 2006, to September 26, 2006, along the coastal length of India to screen for POPS in the atmosphere. The sampling sites were selected to form categories of urban, rural, and background (mangrove/wetlands) locations. Derived air concentrations (pg/m(3)) ranged as follows: the sum of 28 PCB congeners, 120-1080; DOTS, 16-2950; HCHs, 66-5400; chlordanes, 9-921; endosulfans, 0.45-1120; and the sum of 9 PBDE congeners, 1-181. The highest levels of all the detected POPS (except endosulfan) were observed at the urban sites, indicating the dominant areas of usage and emissions. An urban-rural composition fractionation of PCBs indicates their atmospheric movement. The gamma-HCH levels were more than double those of alpha-HCH, indicating the sporadic use of lindane. DDT concentrations were elevated, at levels comparable to China, but with much higher percentages of p,p'-DDE, reflecting a more 'weathered' feature. Although no dicofol use was recorded in India, the o,p'-/p,p'-DDT ratios were observed to be even higher than in China. Chlordanes showed high trans-/cis-chlordane (TC/CC) ratios, indicative of the current use of technical chlordane and a contribution from heptachlor usage.
• Time trends and transplacental transfer of perfluorinated compounds in melon-headed whales stranded along the Japanese coast in 1982, 2001/2002, and 2006

  Kimberly Hart, Kurunthachalam Kannan, Tomohiko Isobe, Shin Takahashi, Tadasu K. Yamada, Nobuyuki Miyazaki, Shinsuke Tanabe

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 42 (19) 7132 - 7137 0013-936X 2008/10 Scientific journal 

  As a result of the phase-out of production of perfluorooctanesulfonyl-based compounds by a major producer, concentrations of perfluorooctanesulfonate (PFOS) in marine mammals from North American and European coastal waters have been declining since the early 2000s. Nevertheless, temporal trends in perfluorochemical (PFC) concentrations in marine mammals from Asian coastal waters have not been examined. In this study, PFCs were determined in livers of melon-headed whales (Peponocephala electra) collected along the coast of Japan, from three mass strandings that occurred during the past 25 years. Concentrations of nine PFCs were determined in livers of 48 melon-headed whales that were collected during strandings in 1982, 2001/2002, and 2006. In addition, concentrations in liver tissues obtained from two pregnant females and their fetuses were compared for determination of transplacental transfer rates of PFCs during gestation. PFOS and perfluorooctanesulfonamide (PFOSA) were the predominant PFCs found in livers of melon-headed whales collected in 1982 (n = 22). PFOS, PFOSA, perfluoroundecanoate (PFUnDA), perfluorododecanoate (PFDoDA), perfluorodecanoate (PFDA), and perfluorononanoate (PFNA) were found in whales collected in 2001/2002 In = 21) and in 2006 (n = 5). Concentrations of PFOS and PFOSA were approximately 10-fold higher in 2001/2002 than in 1982. Whereas concentrations of PFOSA then declined by 2-fold from 2001/2002 to 2006, concentrations of PFOS and perfluorocarboxylates did not decline after 2001/2002. Conversely, concentrations of PFNA and PFDA increased significantly from 2001/2002 to 2006. The proportion of perfluoroalkylsulfonates in total PFC concentrations decreased from 75% in 1982 to 51% in 2006. Conversely,the contribution of perfluorocarboxylates to total PFC concentrations increased from 25% in 1982 to 49% in 2006. PFUnDA was the major perfluorocarboxylate found in whale livers collected after 2000. Analysis of paired samples of mother-fetus demonstrated that the transplacental transfer rates of PFCs were higher than those for PCBs and PBDEs.
• Brominated flame retardants and heavy metals in automobile shredder residue (ASR) and their behavior in the melting process

  Morihiro Osada, Nobuhiro Tanigaki, Shin Takahashi, Shin-ichi Sakai

  JOURNAL OF MATERIAL CYCLES AND WASTE MANAGEMENT 10 (2) 93 - 101 1438-4957 2008/09 Scientific journal 

  The End-of-life Vehicles Recycling Act went into effect on January 1, 2005, in Japan and requires the proper treatment of airbags, chlorofluorocarbons (CFCs), and automobile shredder residue (ASR). The need for optimal treatment and recycling of ASR, in particular, has been increasing year after year because ASR is regarded as being difficult to treat. Dioxin-related compounds, brominated flame retardants (BFRs), heavy metals, chlorine and organotin compounds are all present in high concentrations in ASR. The authors conducted ASR melting treatment tests using a 10-tons/day-scale direct melting system (DMS), which employs shaft-type gasification and melting technology. The results obtained showed that dioxin-related compounds and BFRs were decomposed by this melting treatment. The high-temperature reducing atmosphere in the melting furnace moved volatile heavy metals such as lead and zinc into the fly ash where they were distributed at a rate of more than 90% of the input amount. This treatment was also found to be effective in the decomposition of organotin, with a rate of decomposition higher than 99.996% of the input amount. Via the recovery of heavy metals concentrated in the fly ash, all the products discharged from this treatment system were utilized effectively for the complete realization of an ASR recycling system that requires no final disposal sites.
• Skipjack tuna as a bioindicator of contamination by perfluorinated compounds in the oceans

  Kimberly Hart, Kurunthachalam Kannan, Lin Tao, Shin Takahashi, Shinsuke Tanabe

  SCIENCE OF THE TOTAL ENVIRONMENT 403 (1-3) 215 - 221 0048-9697 2008/09 Scientific journal 

  Perfluorinated chemicals (PFCs) have emerged as global environmental contaminants. Studies have reported the widespread occurrence of PFCs in biota from marine coastal waters and in remote polar regions. However, few studies have reported the distribution of PFCs in biota from offshore waters and open oceans. In this study, concentrations of nine PFCs were determined in the livers of 60 skipjack tuna (Katsuworius pelamis) collected from offshore waters and the open ocean along the Pacific Rim, including the Sea of Japan, the East China Sea, the Indian Ocean, and the Western North Pacific Ocean, during 1997-1999. At least one of the nine PFCs was found in every tuna sample analyzed. Overall, perfluorooctanesulfonate (PFOS) and perfluoroundecanoic acid (PFUnDA) were the predominant compounds found in livers of tuna at concentrations of <1-58.9 and <1-31.6 ng/g, wet wt, respectively. Long-chain perfluorocarboxylates such as perfluorodecanoic acid (PFDA) and perfluorododecanoic acid (PFDoDA) were common in the tuna livers. In livers of tuna from several offshore and open-ocean locations, concentrations of PFUnDA were greater than the concentrations of PFOS. The profiles and concentrations of PFCs in tuna livers suggest that the sources in East Asia are dominated by long-chain perfluorocarboxylates, especially PFUnDA. High concentrations of PFUnDA in tuna may indicate a shift in sources of PFCs in East Asia. The spatial distribution of PFOS in skipjack tuna reflected the concentrations previously reported in seawater samples from the Pacific and Indian Oceans, suggesting that tuna are good bioindicators of pollution by PFOS. Despite its predominance in ocean waters, PFOA was rarely found in tuna livers, indicative of the low bioaccumulation potential of this compound. Our study establishes baseline concentrations of PFCs in skipjack tuna from the oceans of the Asia-Pacific region, enabling future temporal trend studies of PFCs in oceans. (C) 2008 Elsevier B.V. All rights reserved.
• Inshore/offshore gradients of imposex and organotin contamination in Nassarius reticulatus (L.) along the Portuguese coast

  Milene Rato, Miguel B. Gaspar, Shin Takahashi, Shinichi Yano, Shinsuke Tanabe, Carlos Barroso

  MARINE POLLUTION BULLETIN 56 (7) 1323 - 1331 0025-326X 2008/07 Scientific journal 

  Imposex and organotin (OT) tissue contamination of the netted whelk Nassanus reticulatus (L.) were assessed in the continental shelves around the main estuaries of the central coast of Portugal (Lisbon: Tagus estuary; Setubal: Sado estuary) and the main coastal lagoon in the Southern of Portugal (Faro: Ria Formosa). Pollution levels were higher in areas of more intense boat traffic and shipyard activities and imposex showed a clear decreasing gradient from the estuaries to the offshore, in relation to a similar gradient of tissue contamination by tributyltin. Remarkably, imposex was extensively spread over the adjacent continental shelves of Tagus and Sado estuaries. The current work shows that TBT pollution is undoubtedly a matter of concern not only for the above estuaries where harbours are implanted but also for the adjacent continental shelves, regardless the massive dilution of contaminants that may occur in these deeper areas. (c) 2008 Elsevier Ltd. All rights reserved.
• Spatial trends of polybrominated diphenyl ethers in avian species: Utilization of stored samples in the Environmental Specimen Bank of Ehime University (es-Bank)

  Tatsuya Kunisue, Yumi Higaki, Tomohiko Isobe, Shin Takahashi, Annamalai Subramanian, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 154 (2) 272 - 282 0269-7491 2008/07 Scientific journal 

  The present study determined concentrations and patterns of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) in specimens of open sea, and Japanese coastal and inland avian species, which have been stored in the Environmental Specimen Bank of Ehime University (es-Bank), to examine the spatial trends. PBDEs and PCBs were detected in all the muscle samples analyzed, suggesting that PBDE pollution has spread even to the remote open sea areas, as in the case of PCBs. Japanese coastal and inland birds accumulated higher concentrations of PBDEs than open sea birds. In addition, higher PBDE/PCB concentration ratios were observed in Japanese coastal and inland birds than in open sea birds, indicating the input of PBDEs into the Japanese terrestrial environment. Compositions of PBDEs varied among avian species with a predominance of BDE47 or BDE153. This could be due to differences in their habitat, food habit and/or biotransformation capacity of PBDEs. (C) 2007 Elsevier Ltd. All rights reserved.
• Contamination status and accumulation profiles of organotins in sea otters (Enhydra lutris) found dead along the coasts of California, Washington, Alaska (USA), and Kamchatka (Russia)

  Satoko Murata, Shin Takahashi, Tetsuro Agusa, Nancy J. Thomas, Kurunthachalam Kannan, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 56 (4) 641 - 649 0025-326X 2008/04 Scientific journal 

  Organotin compounds (OTs) including mono- to tri-butyltins, -phenyltins, and -octyltins were determined in the liver of adult sea otters (Enhydra lutris) found dead along the coasts of California, Washington, and Alaska in the USA and Kamchatka, Russia. Total concentrations of OTs in sea otters from California ranged from 34 to 4100 ng/g on a wet weight basis. The order of concentrations of OTs in sea otters was total butyltins >> total octyltins >= total phenyltins. Elevated concentrations of butyltins (BTs) were found in some otters classified under 'infectious-disease' mortality category. Concentrations of BTs in few of these otters were close to or above the threshold levels for adverse health effects. Total butyltin concentrations decreased significantly in the livers of California sea otters since the 1990s. Based on the concentrations of organotins in sea otters collected from 1992 to 2002, the half-lives of tributyltin and total butyltins in sea otters were estimated to be approximately three years. (c) 2008 Elsevier Ltd. All rights reserved.
• Characteristics and Sources of Polycyclic Aromatic Hydrocarbons in Ehime Prefecture

  二宮久, 藤田慎二郎, 宇野克之, 泉喜子, 青木平八郎, 高橋真, 田辺信介

  環境化学 18 (1) 29 - 42 0917-2408 2008/03
• Characteristics and Sources of Polycyclic Aromatic Hydrocarbons in Ehime Prefecture

  二宮久, 藤田慎二郎, 宇野克之, 泉喜子, 青木平八郎, 高橋真, 田辺信介

  環境化学 日本環境化学会 18 (1) 29 - 42 0917-2408 2008/03
• Levels and body distribution of polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs) in freshwater fishes from the Yangtze River, China

  Qiming Xian, Karri Ramu, Tomohiko Isobe, Agus Sudaryanto, Xiaohua Liu, Zishen Gao, Shin Takahashi, Hongxia Yu, Shinsuke Tanabe

  CHEMOSPHERE 71 (2) 268 - 276 0045-6535 2008/03 Scientific journal 

  Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs) were determined in muscle, liver and eggs of freshwater fishes from the lower reach of the Yangtze River, China. The present study is the first to report HBCD concentrations in the environment of China. The concentrations of PBDEs and HBCDs in muscle of freshwater fishes from the Yangtze River ranged from IS to I 100 ng/g and 12 to 330 ng/g lipid weight (wt.), respectively. When compared with other regions of the world, the contamination of PBDEs in biota could be regarded as moderate, whereas contamination of HBCDs in biota was relatively high. The PBDE congener profiles in fishes of the present Study were markedly different from those observed in freshwater and marine fishes from other regions of the world. In the present study, BDE-15 BDE-28 and BDE-47 were the predominant congeners in the fishes. This particular congener profile in fishes from the Yangtze River revealed that a specific commercial PBDE formulation (probably made in China) might have been used in the Yangtze River Delta region. (c) 2007 Elsevier Ltd. All rights reserved.
• Identification of brominated and chlorinated phenols as potential thyroid-disrupting compounds in indoor dusts

  Go Suzuki, Hidetaka Takigami, Mafumi Watanabe, Shin Takahashi, Kazutoshi Nose, Misuzu Asari, Shin-Ichi Sakai

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 42 (5) 1794 - 1800 0013-936X 2008/03 Scientific journal 

  Our previous study demonstrated that compounds in indoor dusts strongly inhibit thyroxine (T4) binding to the human thyroid hormone transport protein transthyretin (TTR) in vitro. Exposure assessment indicated that house dust is an important medium of exposure of children to TrR-binding compounds when binding potency and dust ingestion rates are high. Here, we used chemical fractionation with in vitro competitive human TTR-binding assay and GC-MS to analyze the TTR-binding compounds in a sulfuric-acid-treated dust extract. 2,4,6-Tribromophenol (TriBPh) and 2,3,4,5,6-pentachlorophenol (PeCPh) were potent TTR-binding compounds in all dust samples. 2,4,6-TriBPh- and 23,45,6-PeCPh-derived theoretical T4 equivalents (T4EQs), calculated arithmetically from the concentrations and relative potencies, accounted for about 40-70% of experimental T4EQs detected in indoor dusts, indicating that these compounds contributed strongly to the TTR-binding potency of indoor dust. Indoor sources of 2,4,6-TriBPh might be brominated flame retardants currently used in household materials such as electrical appliances. In contrast, the 2,3,4,5,6-PeCPh might be trace evidence of past use in agricultural chemicals and preservatives in indoor or outdoor environments, because its use has been banned since 1990 in Japan. 2,4,6-TriBPh and 2,3,4,5,6-PeCPh are ubiquitous potential thyroid-disrupting compounds in the home and work environments of Japan and other countries.
• Regional trend and tissue distribution of brominated flame retardants and persistent organochlorines in raccoon dogs (Nyctereutes procyonoides) from Japan

  Tatsuya Kunisue, Nozomi Takayanagi, Tomohiko Isobe, Shin Takahashi, Susumu Nakatsu, Toshio Tsubota, Keisuke Okumoto, Sumio Bushisue, Kazuyuki Shindo, Shinsuke Tanabe

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 42 (3) 685 - 691 0013-936X 2008/02 Scientific journal 

  The present study investigated concentrations and patterns of brominated flame retardants, such as polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs), and persistent organochlorines (OCs) in liver and adipose tissues of raccoon dogs (RD: Nyctereutes procyonoides) collected from two metropolises and a local prefecture in Japan during 2001-2006. Relatively high concentrations of PBDEs were found in RD livers, while HBCD levels were the lowest among the measured organohalogen compounds. Among PBDE congeners, BDE 209 was predominant in RDs from all the regions, indicating that pollution derived from the technical decaBDE product is extensive across Japan. On the other hand, concentrations of tetra- to nona-BDE congeners in RDs from a metropolis were significantly higher than those from the other two regions, implying that there were regional differences in the past usage of the technical tetraBDE and octaBDE products. Such a regional difference was also observed for HBCD levels. Lipid-normalized concentration ratios of liver to adipose tissue L/A ratio) for tri to hepta-BDE congeners were lower than 1.0 in the investigated eight RDs, suggesting lipid-dependent accumulation. However, the L/A ratios of BDE 209 exceeded 1.0 in all the specimens, suggesting hepatic retention of this compound. In addition, lipid-dependent accumulation of alpha-HBCD was observed, but the L/A ratios of gamma-HBCD were greater than 1.0 in some specimens. These results indicate that Japanese RDs have been recently exposed to BDE 209 and gamma-HBCD and accumulated both these compounds preferentially in blood-rich organs, probably due to their binding to proteins and/or rapid biotransformation, as reported in experimental rodents.
• Hydroxylated polychlorinated biphenyls in the blood of Baikal seals (Pusa Sibirica)

  Imaeda, D, Kunisue, T, Iwata, H, Tsydenova, O, Takahashi, S, Nomiyama, K, Amano, M, Petrov, A.E, Batoev, B.V, Tanabe, S

  Organohalogen Compounds 70 1475 - 1478 2008 [Peer-reviewed]
   

  Proceedings
• Characteristics and Sources of Polycyclic Aromatic Hydrocarbons in Ehime Prefecture

  NINOMIYA Hisashi, FUJITA Shinjiro, UNO Katsuyuki, IZUMI Yoshiko, AOKI Heihachirou, TAKAHASHI Shin, TANABE Shinsuke

  JEC Japan Society for Environmental Chemistry 18 (1) 29 - 42 0917-2408 2008 

  Concentrations of particulate polycyclic aromatic hydrocarbons(PAHs) in ambient air were investigated every month during the period Apr. 2004 to Mar. 2006 at two sampling sites in Ehime Prefecture; Site-N in Niihama city industrial area and Site-U in Uwajima city nonindustrial area. The sampling was carried out by high volume air sampler on quarts filters, extracted with dichloromethane and analyzed by HPLC with programmable fluorescence detection. Heavy metals and water soluble ios in particulate samples and benzene in air samples were also analyzed in this study. Annual average of total PAHs concentrations ranged from 4.5 to 4.7 ng/m<SUP>3</SUP> at Site-N, higher than in Site-U (2.0∼3.4 ng/m<SUP>3</SUP>). Estimated risks of each PAHs based on unit risk were in the order of 10<SUP>-7</SUP>∼10<SUP>-5</SUP>, but overall risk was higher than objective criteria suggested by Central Environmental Council, Japan. B[a]P contributed above 50 % followed by DB[a,h]A. To have a complete knowledge on PAHs in atmosphere, their levels in the gaseous phase should also be monitored. Major source of PAHs would be vehicles especially diesel cars because of their diagnostic ratios of B[ghi]P/IP, IP/(IP+B[ghi]P) and (B[b]F+B[k]F)/B[ghi]P ranged within values reported for diesel exhausts so far. This view can be substantiated by the observed high correlation of PAHs with benzene and carbon oxide. Indexes of sources were selected by hierarchical cluster analysis on datasets of PAHs, metals and ions at Site-U which has no significant sources from industries. Then temporal variations of them and back trajectories at points in time were analyzed. It appears that high concentrations of anthropogenic metals and NH<SUB>4</SUB>SO<SUB>4</SUB> are observed when the air mass was originated and passed through low-altitudes on industrial regions of China. Although PAHs showed significant correlation with these metals, they would be increased mainly by the effect of atmospheric stability.
• バイカルアザラシ（Ｐｕｓａ ｓｉｂｉｒｉｃａ）の肝臓および筋肉における微量元素の蓄積特性

  宇高 真行, 池本 徳孝, 高橋 真, 岩田 久人, BATOEV Valeriy, PETROV Evgeny, 田辺 信介

  環境毒性学会誌 日本環境毒性学会 11 (2) 117 - 131 1344-0667 2008 

  Concentrations of 21 trace elements (V, Cr, Mn, Co, Cu, Zn, Se, Rb, Sr, Mo, Ag, Cd, In, Sn, Sb, Cs, Ba, Hg, Tl, Pb and Bi) were determined in the liver and muscle of Baikal seals (<I>Pusa sibirica</I>) (<I>n</I> = 44) collected from Lake Baikal, Russia in 2005. Most of the elements, such as V, Mn, Cu, Zn, Se, Hg and Mo, showed higher concentrations in liver than in muscle. However, Cs was found at higher levels in muscle than in liver. Liver and muscle concentrations of essential elements Cu and Zn were higher than other essential elements in Baikal seals. On the other hand the levels of non-essential elements Cd and Hg were comparable to or lower than the corresponding levels in other seal species. Significant age dependent accumulation was observed for Mn, Cu, Sr, Cd and Hg in liver and muscle, V, Se, Mo and Ba in liver, and Zn in muscle. Significant correlations were observed between concentrations of the following trace elements V-Cd, Mn-Cu, Mn-Cd, Cu-Sr, Cu-Cd, Cu-Hg, Rb-Cs, Sr-Ba, Sb-Tl, Ba-Pb and Tl-Bi in both liver and muscle. Generally, the molar ratio between Se and Hg is known to be 1:1 in marine mammals which show high levels of Se and Hg, however no such pattern was observed in the present study due to the low level of these elements. Concentrations of V, Cr, Mn, Co, Cu, Zn, Se, Sr, Mo, Ag, Cd, Sb, Cs, Hg, and Tl in Baikal seals collected in 2005 were comparable to those in the seals collected in 1992. On the other hand, concentrations of Rb were significantly higher in 2005 samples, suggesting that environmental contamination by Rb in Lake Baikal seems to have increased during the last decade.
• Geographical distribution and accumulation features of PBDEs in human breast milk from Indonesia

  Agus Sudaryanto, Natsuko Kajiwara, Shin Takahashi, Muawanah, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 151 (1) 130 - 138 0269-7491 2008/01 Scientific journal 

  The present study reports concentrations of polybrominated diphenyl ethers (PBDEs) and organochlorines (OCs) in human breast milk from Indonesia covering urban, suburban and rural areas. PBDEs were detected in all the samples of the present study with total concentrations ranging from 0.49 to 13 ng/g lipid wt. Geographical distribution showed that concentrations of PBDEs were relatively uniform (p > 0.05) and the levels were in the same order as those in Japan and some European countries, but were one or two order lower than North America. When compared to OCs, the level of total PBDEs was lower. The congener pattern was in accordance with other studies on human matrices, in which BDE-47 was the most abundant congener. Variations of PBDE congeners in human breast milk were further discussed to elucidate the potential exposure source(s) and pathways. (C) 2007 Elsevier Ltd. All rights reserved.
• Polybrominated diphenyl ethers and persistent organochlorines in Japanese human adipose tissues

  Tatsuya Kunisue, Nozomi Takayanagi, Tomohiko Isobe, Shin Takahashi, Masato Nose, Taketo Yamada, Hiroaki Komori, Nonimasa Arita, Norifumi Ueda, Shinsuke Tanabe

  ENVIRONMENT INTERNATIONAL 33 (8) 1048 - 1056 0160-4120 2007/11 Scientific journal 

  The present study determined concentrations of polybrominated diphenyl ethers (PBDEs) and persistent organochlorines (OCs) in Japanese human adipose tissues collected during 2003-2004. Concentrations of PBDEs in adipose tissues were 1-2 orders of magnitude lower than those of OCs. However, observed PBDE congener levels in this study were relatively higher than those in Japanese human adipose tissues collected during 2000 reported previously, while OC levels were comparable to those in specimens collected during 1999 reported by our group. In addition, no age-dependent accumulation of PBDEs was observed, while OC levels except chlordane compounds increased with age. These results indicate recent human exposure to PBDEs in Japan. Among PBDE congeners accumulated in Japanese adipose tissues, BDE-153 was dominant, but this trend was different from those in human milk (BDE-47) and blood (BDE-209) reported previously in Japan, implying the congener-specific kinetics in human bodies. The significant positive correlations between PBDEs and OCs were observed in Japanese adipose tissues, indicating the similar exposure route of these contaminants for Japanese citizens, probably via fish intake. (C) 2007 Elsevier Ltd. All rights reserved.
• Integrative assessment of organotin contamination in a southern European estuarine system (Ria de Aveiro, NW Portugal): Tracking temporal trends in order to evaluate the effectiveness of the EU ban

  Ana Sousa, Chiho Matsudaira, Shin Takahashi, Shinsuke Tanabe, Carlos Barroso

  MARINE POLLUTION BULLETIN 54 (10) 1645 - 1653 0025-326X 2007/10 Scientific journal 

  Organotin (OT) compounds have been used as biocide agents in antifouling paints since the mid 1960s and are now ubiquitous in the marine environment. Due to their high toxicity to non-target species they were banned from antifouling paints in the European Union in 2003 (2002/62/EC directive). The aim of the present work is to assess any obvious decline of the OT environmental levels at Ria de Aveiro (NW Portugal) after the ban. The organotins - monobutyltin (MBT), dibutyltin (DBT), tributyltin TBT), monophenyltin (MPT), diphenyltin (DPT), triphenyltin (TPT), monoctyltin (MOT), dioctyltin (DOT) and trioctyltin (TOT) - were quantified in the gastropod Nassarius reticulatus, in the mussel Mytilus galloprovincialis and in sediments. Imposex (imposition of male characters on females of gonochorist gastropods) in N. reticulatus was additionally used as a biomarker of TBT pollution. Time comparisons show a slight decrease of imposex between 2003 and 2005 probably as a consequence of the EU ban, though in some cases this trend seems to have started earlier since 2000. The fraction of TBT relatively to its metabolites has been decreasing over the last years but still remains high suggesting that there are still recent inputs of this compound into the study area. (C) 2007 Elsevier Ltd. All rights reserved.
• Levels and distribution of organochlorines in fish from Indonesia

  Agus Sudaryanto, In Monirith, Natsuko Kajiwara, Shin Takahashi, Philippus Hartono, Muawanah, Koji Omori, Hidetaka Takeoka, Shinsuke Tanabe

  ENVIRONMENT INTERNATIONAL 33 (6) 750 - 758 0160-4120 2007/08 Scientific journal 

  Organochlorines such as PCBs, DDTs, HCHs, CHLs and HCB were determined in pooled whole body homogenized of fish samples collected from five locations during 1998 and 2003 in order to understand their contamination status, temporal and spatial variation in Indonesian waters. PCBs and DDTs were the predominant contaminants with concentrations from 9.7 to 2700 ng/g lipid wt. and 12 to 1100 ng/g lipid wt., respectively, while HCHs (nd-24 ng/g lipid wt.), CHL compounds (nd-81 ng/g lipid wt.) and HCB (0.22-28 ng/g lipid wt.) were one to two orders of magnitude lower. Among the locations, PCBs and CHLs were higher in the samples from highly industrialized and thickly populated-locations, whereas OC pesticides such as DDTs and HCHs were particularly more prominent in suburban and rural areas. Levels of OCs observed in the waters surrounding Java Island were higher than those in Sumatra Island, implying significant use of OCs in highly populated Java Island. Concentrations of PCBs and DDTs in fish from Jakarta Bay were significantly lower in the samples collected in 2003 as compared to fish in 1998, indicating decreasing trend of these compounds in the Indonesian environment. Recent estimated average daily intakes of PCBs (0.81 mu g/person/ day), DDTs (1.1 mu g/person/day), HCHs (0.018 (mu g/person/day), CHLs (0.010 mu g/person/day) were much lower than the threshold values recommended by various agencies, suggesting minimal risk of this compound via fish ingestion to Indonesians. (c) 2007 Elsevier Ltd. All rights reserved.
• Isomer specific determination of hexabromocyclododecanes (HBCDs) in small cetaceans from the South China Sea - Levels and temporal variation

  Tomohiko Isobe, Karri Ramu, Natsuko Kajiwara, Shin Takahashi, Paul K. S. Lam, Thomas A. Jefferson, Kaiya Zhou, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 54 (8) 1139 - 1145 0025-326X 2007/08 Scientific journal 

  A diastereoisomer (alpha, beta, and gamma) specific analytical method for measuring hexabromocyclododecanes (HBCDs) was developed using liquid chromatography-tandem mass spectrometry (LC-MS-MS). The method developed was applied to analyze blubber of small cetaceans to divulge the distribution and temporal variation of HBCDs in the Asian marine environment. HBCDs were detected in all the blubber samples of finless porpoises (Neophocaena phocaenoides) and Indo-Pacific humpback dolphins (Sousa chinensis) collected from the South China Sea during 1990-2001. Concentrations of HBCDs were higher in humpback dolphins (31-380 ng/g lipid) than in finless porpoises (4.7-55 ng/g lipid), which can be attributed to habitat differences. Average concentrations of alpha-HBCD in finless porpoises increased from 9.5 ng/g lipid in 1990 to 35 ng/g lipid in 2000/01. alpha-HBCD was predominant among the three isomers with some exceptions in finless porpoises collected in 1990. This is the first report on HBCDs contamination in marine mammals from Southeast Asia. (C) 2007 Elsevier Ltd. All rights reserved.
• Occurrence of hydroxylated polychlorinated biphenyls in the brain of cetaceans stranded along the Japanese coast

  Tatsuya Kunisue, Takanori Sakiyama, Tadasu K. Yamada, Shin Takahashi, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 54 (7) 963 - 973 0025-326X 2007/07 Scientific journal 

  Levels of hydroxylated polychlorinated biphenyls (OH-PCBs) and PCBs were measured in the brain of melon-headed whales (MW: Peponocephala electra), striped dolphins (SD: Stenella coerideoalba) and finless porpoises (FP: Neophocaena phocaenoides) stranded along the Japanese coast during 2002-2003. Levels of OH-PCBs (including identified and unknown OH-P5CB, -H6CB, -H7CB and O8CB congeners) in the brain of MW, SD and FP were in the range of 20-290, 21-330 and 170-240 pg/g wet wt., respectively. Observed OH-PCB levels were 2-3 orders of magnitude lower than PCBs in the same individuals. OH-PCBs/PCBs ratios in MW, SD and FP brain were lower than those in blood of humans and wildlife and in the brain of polar bears reported previously. OH-PCBs were also detected in maternal and fetal brain of SID (1 pair), suggesting transfer of OH-PCBs into the fetal brain of odontocete cetaceans. When fetus/dam concentration ratios of 0H-PCB congeners detected in maternal and fetal brain were estimated, the values were higher than those of PCB congeners, implying that OH-PCBs in maternal blood could be more easily transferred into fetal brain via placenta than PCBs. (c) 2007 Elsevier Ltd. All rights reserved.
• Asian mussel watch program: Contamination status of polyhrominated diphenyl ethers and organochlorines in coastal waters of Asian countries

  Karri Ramu, Natsuko Kajiwara, Agus Sudaryanto, Tomohiko Isobe, Shin Takahashi, Annamalai Subramanian, Daisuke Ueno, Gene J. Zheng, Paul K. S. Lam, Hideshige Takada, Mohamad Pauzi Zakaria, Pham Hung Viet, Maricar Prudente, Touch Seang Tana, Shinsuke Tanabe

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 41 (13) 4580 - 4586 0013-936X 2007/07 Scientific journal 

  Mussel samples were used in this study to measure the levels of polybrominated diphenyl ethers (PBDEs) and organochlorines (OCs) in the coastal waters of Asian countries like Cambodia, China, Hong Kong, India, Indonesia, Japan, Korea, Malaysia, the Philippines, and Vietnam. PBDEs were detected in all the samples analyzed, and the concentrations ranged from 0.66 to 440 ng/g lipid wt. Apparently higher concentrations of PBDEs were found in mussels from the coastal waters of Korea, Hong Kong, China, and the Philippines, which suggests that significant sources of these chemicals exist in and around this region. With regard to the composition of PBDE congeners, BDE-47, BDE-99, and BDE-100 were the dominant congeners in most of the samples. Among the OCs analyzed, concentrations of DDTs were the highest followed by PCBs > CHILs > HCHs > HCB. Total concentrations of DDTs, PCBs, CHLs, and HCHs in mussel samples ranged from 21 to 58 000, 3.8 to 2000, 0.93 to 900, and 0.90 to 230 ng/g lipid wt., respectively. High levels of DDTs were in mussels from Hong Kong, Vietnam, and China; PCBs were found in Japan, Hong Kong, and industrialized/urbanized locations in Korea, Indonesia, the Philippines, and India; CHLs were found in Japan and Hong Kong; HCHs were found in India and China. These countries seem to play a role as probable emission sources of corresponding contaminants in Asia and, in turn, may influence their global distribution.
• Spatial distribution and vertical profile of polybrominated diphenyl ethers and hexabromocyclododecanes in sediment core from Tokyo Bay, Japan

  Nguyen Hung Minh, Tomohiko Isobe, Daisuke Ueno, Keizo Matsumoto, Masayuki Mine, Natsuko Kajiwara, Shin Takahashi, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 148 (2) 409 - 417 0269-7491 2007/07 Scientific journal 

  Brominated flame retardants (BFRs), hexabromocyclododecanes (HBCDs) and polybrominated diethyl ethers (PBDEs) were detected in three sediment cores and six surface sediments of Tokyo Bay, Japan. HBCDs were detected for the first time in this region with concentrations ranging from 0.056 to 2.3 ng/g dry wt, implying their widespread contamination, even though their concentrations were lower than Sigma PBDEs (di- to nona-BDEs) and BDE-209. Levels of these compounds were higher near to the highly populated industrial area of the bay implicating industrial and human activities as sources of these compounds. Sigma PBDEs increased in the sediment layer up to the mid-1990s and decreased afterwards, whereas BDE-209 showed an increasing trend until now, following the usage of different commercial BDE mixtures. HBCDs first appeared in the mid-1970s and increased until today. The annual surficial flux of HBCDs (0.62-2.4 ng/cm(2)/yr) is equal to Sigma PBDEs (0.95-2.6 ng/cm(2)/yr) but lower than that of BDE-209 (17-58 ng/cm(2)/yr). (c) 2007 Elsevier Ltd. All rights reserved.
• Spatial distribution and accumulation of brominated flame retardants, polychlorinated biphenyls and organochlorine pesticides in blue mussels (Mytilus edulis) from coastal waters of Korea

  Karri Ramu, Natsuko Kajiwara, Tomohiko Isobe, Shin Takahashi, Eun-Young Kim, Byung-Yoon Min, Sung-Ug We, Shinsuke Tanabe

  ENVIRONMENTAL POLLUTION 148 (2) 562 - 569 0269-7491 2007/07 Scientific journal 

  Blue mussels (Mytilus edulis) from 20 locations along the coastal waters of Korea were analyzed to elucidate the characteristic distribution and contamination status of polybrominated diphenyl ethers (PBDEs), hexabromocyclododecanes (HBCDs), polychlorinated biphenyls (PCBs) and organochlorine pesticides. To our knowledge, this is the first study to report on the contamination status of HBCDs from Korea. PBDEs and HBCDs were found in mussels at levels ranging from 6.6 to 440 and from 6.0 to 500 ng/g lipid wt., respectively. Concentrations of PBDEs in mussels from Korea were higher or comparable to available data in mussels from other countries. Among the organochlorine compounds (OCs) analyzed, levels of PCBs and DDTs were the highest followed by CHLs, HCHs and hexachlorobenzene. For all the compounds, higher concentrations were found in mussels from southeastern coast of Korea. The present study shows the importance of mussels as bioindicators for monitoring contaminants in coastal waters. (c) 2006 Elsevier Ltd. All rights reserved.
• Degradation pathways of decabromodiphenyl ether during hydrothermal treatment

  Kazutoshi Nose, Shunji Hashimoto, Shin Takahashi, Yukio Noma, Shin-ichi Sakai

  CHEMOSPHERE 68 (1) 120 - 125 0045-6535 2007/05 Scientific journal 

  The hydrothermal degradation pathways of decabromodiphenyl ether during hydrothermal treatment were investigated. After an initial "Heating time", the reaction runs were carried out at constant temperature (heating to 300 degrees C and keeping temperature) and pressure (8 MPa) in a SUS316 stainless steel micro autoclave filled with water. Some decomposition of decabromodiphenyl ether was observed over 200 degrees C, and it was decomposed by more than 99% after 10 min at 300 degrees C. The reactivities of bromine on para and meta substituents were relatively high, while its reactivity on ortho bromine was extremely low. The formations of polybrominated dibenzo-p-dioxins and furans (PBDD/DFs) were observed in the early stages of the reactions at around 300 degrees C. The TCDD toxicity equivalency (TCDD-EQs) of the by-products was determined based on relative potencies (REPs EC5TCDD) with the Dioxin-Responsive-Chemical Activated Luciferase gene eXpression (DR-CALUX) bioassays technology. These results indicated that the risk of formation of PBDD/DFs in the hydrothermal degradation of deca-BDE was low, and it would be possible to reduce the TCDD-EQs value by adding some catalyst or alkali, or extending processing time. (C) 2006 Elsevier Ltd. All rights reserved.
• Persistent organic pollutants in sediments from Sai Gon-Dong Nai River Basin, Vietnam: Levels and temporal trends

  Nguyen Hung Minh, Tu Binh Minh, Hisato Iwata, Natsuko Kajiwara, Tatsuya Kunisue, Shin Takahashi, Pham Hung Viet, Bui Cach Tuyen, Shinsuke Tanabe

  ARCHIVES OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY 52 (4) 458 - 465 0090-4341 2007/05 Scientific journal 

  Surficial sediment samples were collected from Hochiminh City canals, the Sai Gon-Dong Nai River, and its estuary, one of the most predominant industrial areas in Hochiminh City, southern Vietnam, for determination of selected persistent organic pollutants (POPs). Contamination pattern was as follows: PCBs >= DDTs > HCB > CHLs > HCHs. Concentrations of PCBs and DDTs ranged from 0.50-150 ng/g and 0.15-72 ng/g dry wt, respectively. On the other hand, concentrations of CHLs, HCHs, and HCB were mostly < 2 ng/g dry wt. Levels of the all organochlorines (OCs) in Hochiminh City canals were significantly higher than those in the other areas, indicating the urban areas as major pollution sources to the aquatic environment. The contamination pattern was PCBs > DDTs in the city canals but PCBs < DDTs in the downstream and the estuary, suggesting particularly high contamination by PCBs in the city. Examination of DDTs composition and their ratios demonstrated continuous input of this pesticide to the city canals. However, the combination of our data and those from available literature implies a decreasing trend of PCBs and DDTs in the environment. DDTs concentrations have been reduced 50% after approximately 5 years. Composition of CHLs in the sediment from Hochiminh City canals was comparable to those of common technical mixtures, suggesting continuous input of CHLs to the environment. CHLs might be in use for purposes like termite control, wood preservation, and protection of underground cables. Hazard assessment implies high toxic potential of DDTs for sediments from Hochiminh City canals and suggests the need for better management of municipal discharges.
• Dioxin-like and transthyretin-binding compounds in indoor dusts collected from Japan: Average daily dose and possible implications for children

  Go Suzuki, Hidetaka Takigami, Kazutoshi Nose, Shin Takahashi, Misuzu Asari, Shin-ichi Sakai

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 41 (4) 1487 - 1493 0013-936X 2007/02 Scientific journal 

  Many researchers are increasingly interested in human exposure to house dust containing household compounds such as polybrominated diphenylethers (PBDEs). Nevertheless, no investigations have addressed the endocrine-disrupting potencies of compounds contained in indoor dust. This study specifically addresses endocrine-disrupting potencies such as dioxin-like activity and human transthyretin (TTR)-binding potencies. Using in vitro bioassays, we investigated these activity levels in indoor dusts. We performed exposure assessments of active compounds that are contained in house dust for subsequent evaluation of house dusts' risks to humans. Dioxin-like and TTR-binding activities in sulfuric acid treatment extracts of house and office dust were investigated using Dioxin-Responsive Chemical-Activated LUciferase gene eXpression assay (DR-CALUX) and TTR-binding assay (in vitro competitive human TTR-binding assay). Dioxin-like activities in indoor dust were 38-1400 pg CALUX-TEQ (2,3,7,8-TCDD equivalent)/g (median 160 pg CALUX-TEQ/g) and TTR-binding potencies were 300-5000 pmol T4EQ (thyroxine (T4) equivalent)/g (median 1000 pmol T4EQ/g), which are higher values than those in other environmental samples, e.g., contaminated sediments. These exposure results suggest that children might be affected by both dioxin-like compounds and TTR-binding compounds via house dust. When the ingestion rate, CALUX-TEQ, and T4EQ for house dust are high, thyroid hormone homeostasis in children may be disrupted.
• Occurrence of organochlorine pesticides, polychlorinated biphenyls and polybrominated diphenyl ethers in deep-sea fishes from the Sulu Sea

  Karri Ramu, Natsuko Kajiwara, Hiroko Mochizuki, Hitoshi Miyasaka, Kwadwo Ansong Asante, Shin Takahashi, Suguru Ota, Hsin-Ming Yeh, Shuhei Nishida, Shinsuke Tanabe

  MARINE POLLUTION BULLETIN 52 (12) 1827 - 1832 0025-326X 2006/12 Scientific journal
• Perfluorooctanesulfonate and related fluorochemicals in albatrosses, elephant seals, penguins, and Polar Skuas from the Southern Ocean

  Lin Tao, Kurunthachalam Kannan, Natsuko Kajiwara, Monica M. Costa, Gilberto Fillmann, Shin Takahashi, Shinsuke Tanabe

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 40 (24) 7642 - 7648 0013-936X 2006/12 Scientific journal 

  Perfluorinated chemicals (PFCs) have been used as surfactants in industrial and commercial products for over 50 years. Earlier studies of the geographical distribution of PFCs focused primarily on the Northern Hemisphere, while little attention was paid to the Southern Hemisphere. In this study, livers from eight species of albatrosses, blood from elephant seal, and blood and eggs from penguins and polar skua collected from the Southern Ocean and the Antarctic during 1995 - 2005 were analyzed for 10 PFCs. In addition, for comparison with the Southern Ocean samples, we analyzed liver, sera, and eggs from two species of albatrosses from Midway Atoll in the North Pacific Ocean. Perfluorooctanesulfonate (PFOS) and perfluorooctanoic acid (PFOA) were found in livers of albatrosses from the Southern Ocean. PFOS was the major contaminant, although the concentrations were < 5 ng/g, wet wt, in 92% of the albatross livers analyzed. PFOA was detected in 30% of the albatross livers, with a concentration range of < 0.6 - 2.45 ng/g, wet wt. Other PFCs, including long-chain perfluorocarboxylates (PFCAs), were below the limits of quantitation in livers of albatrosses from the Southern Ocean. In liver, sera, and eggs of albatrosses from the North Pacific Ocean, long-chain PFCAs (perfluorononanoate, perfluorodecanoate, perfluoroundecanoate, and perfluorododecanoate) were found at concentrations similar to those of PFOS and PFOA. The mean concentration of PFOS in livers of Laysan albatrosses from the North Pacific Ocean (5.1 ng/g, wet wt) was higher than that in several species of albatrosses from the Southern Ocean (2.2 ng/g, wet wt). Species-specific differences in the concentrations of PFOS were noted among Southern Ocean albatrosses, whereas geographical differences in PFOS concentrations among the Indian Ocean, South Pacific Ocean, and South Atlantic Ocean were insignificant. Concentrations of PFOS and PFOA were, respectively, 2- and 17-fold higher in liver than in sera of Laysan albatrosses. PFOS was found in the blood of elephant seals from Antarctica at concentrations ranging from < 0.08 to 3.52 ng/mL. PFOS was found in eggs (2.1 - 3.1 ng/g) and blood (< 0.24 - 1.4 ng/mL) of polar skuas but was not detected in penguins from Antarctica. Our study documents the existence of low but detectable levels of PFOS and PFOA in Southern Hemisphere fauna, suggesting distribution of these compounds on a global scale.
• PBDEs and organochlorines in farmed and wild grouper (Epinephelus fuscoguttatus) from Lampung Mariculture area, Indonesia

  Agus Sudaryanto, Natsuko Kajiwara, Shin Takahashi, Phillipus Hartono, Ir. Muawanah, Koji Omoril, Shinsuke Tanabe

  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY 232 670 - 670 0065-7727 2006/09 [Peer-reviewed]
  
• Contamination status of PBDEs in the Asia-Pacific region: A review of recent studies on marine mammals, fish/shellfish, human breast milk and terrestrial environments including waste dumping sites

  Shin Takahashi, Tomohiko Isobe, Agus Sudaryanto, Karri Ramu, Tatusya Kunisue, Nguyen Hung Minh, Tu Binh Minh, Annamalai Subramanian, Natsuko Kajiwara, Daisuke Ueno, Shin-ichi Sakai, Shinsuke Tanabe

  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY 232 664 - 664 0065-7727 2006/09 [Peer-reviewed]
  
• Levels and distribution of organohalogen compounds in blue mussels (Mytilus edulis) from coastal waters of Korea

  Karri Ramu, Natsuko Kajiwara, Tomohiko Isobe, Shin Takahashi, Eun-Young Kim, Byung-Yoon Min, Sung-Ug We, Shinsuke Tanabe

  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY 232 665 - 665 0065-7727 2006/09 [Peer-reviewed]
  
• Vertical profiles of brominated flame retardants, polybrominated diphenyl ethers and hexabromocyclododecane in the sediment core from Tokyo Bay

  Tomohiko Isobe, Nguyen Hung Minh, Daisuke Ueno, Keizo Matsumoto, Natsuko Kajiwara, Shin Takahashi, Shinsuke Tanabe

  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY 232 671 - 671 0065-7727 2006/09 [Peer-reviewed]
  
• Brominated flame retardants in the environment of Indonesia

  Agus Sudaryanto, Tomohiko Isobe, Shin Takahashi, Shinsuke Tanabe

  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY 232 669 - 669 0065-7727 2006/09 [Peer-reviewed]
  
• Human blood monitoring program in Japan: Contamination and bioaccumulation of persistent organochlorines in Japanese residents

  T. B. Minh, M. Watanabe, N. Kajiwara, H. Iwata, S. Takahashi, A. Subramanian, S. Tanabe, S. Watanabe, T. Yamada, J. Hata

  ARCHIVES OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY 51 (2) 296 - 313 0090-4341 2006/08 Scientific journal 

  Concentrations of persistent organochlorines (OCs)-such as polychlorinated biphenyls (PCBs), 1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane (DDT) and its metabolites (DDTs), hexachlorocyclohexane isomers (HCHs), chlordane compounds (CHLs), hexachlorobenzene, and tris(4-chlorophenyl)methane [TCPMe]-were determined in plasma samples from residents of three sub-metropolitan locations in Japan (Miyako, Saku, and Tottori) for the purpose of studying the geographic variation and specific accumulation of OCs. Residue concentrations of PCBs and DDTs were the highest in samples collected in Saku (400 and 370 ng/g lipid wt, respectively) whereas samples from Miyako contained greater CHL residues (70 ng/g lipid wt) than those from the other two locations. This contamination pattern reflects the historic use of OCs in each area. For the first time, tris (4-chlorophenyl) methane (TCPMe) concentrations were detected in most of the plasma sample analyzed. Concentrations of TCPMe which ranged from < 0.1 to 8.1 ng/g lipid wt eight, were lower than those previouly reported in other human tissue. Larger geographic differences in OC accumulation were observed for PCBs and CHLs, whereas DDTs and HCHs exhibited little variability. PCB concentrations in samples from Saku residents were higher than those from residents of countries in the circumpolar Arctic region but lower than those reported for some populations in the United States and Western European countries. Interestingly, CHL residue concentrations in human blood from Japan are among the highest values reported for the countries examined, suggesting continued increased exposure to CHLs of the Japanese population. Time-trend analysis of CHLs in human blood samples from Miyako (Okinawa prefecture) showed that CHL residues have decreased substantially during the last decade, indicating the effect of the official ban of CHLs in 1986 in Japan. Isomer-specific analysis of PCBs revealed lower proportions of higher chlorinated congeners such as hepta- and octachlorobiphenyls in women than in men, suggesting the possibility of preferential elimination of higher chlorinated biphenyls in women. The difference in sex-dependent accumulation of OC compounds in healthy and ill persons was suggested. To our knowledge, this is the first report on the specific accumulation of persistent QCs, including TCPMe, in human blood samples from Japan.
• An intercalibration study on organobromine compounds: Results on polybrominated diphenylethers and related dioxin-like compounds

  Shin Takahashi, Shin-ichi Sakai, Isao Watanabe

  CHEMOSPHERE 64 (2) 234 - 244 0045-6535 2006/06 Scientific journal 

  An intercalibration study on organobromine compounds has been conducted to evaluate the accuracy and reliability in the analysis of brominated flame retardants (BFRs) such as polybrominated diphenyl ethers (PBDEs) and their related compounds like polybrominated and monobromo-polychlorinated dibenzodioxins and -furans (PBDDs/DFs, MoBPCDDs/DFs). This paper reports the results for these compounds in 'Mixed Standard Solutions' and 'Air-Dried Sediment'. The relative standard deviations (RSDs) for PBDEs, PBDDs/DFs and MoBPCDDs/DFs in mixed standard solutions ranged from 9% to 24%, 4% to 20% and 8% to 27%, respectively. The results of this study are better than those reported in earlier international interlaboratory studies due to general improvement in analytical methods and an increasing number of available authentic standards, particularly for PBDEs. In the analysis for higher brominated compounds such as octabromodibenzodioxin, the participants were advised to optimize the calibration curves befitting the range of concentrations found in samples because variation of relative response factors was noted. The results for 'Air-Dried Sediment' were also reasonable with RSDs from 10% to 38% for PBDEs, 8% to 38% for PBDDs/DFs and 17% to 36% for MoBPCDDs/DFs. In the sediment sample, possible errors in the sample pretreatment and/or interference by other compounds/impurities were indicated. The concentrations of pentabromodiphenylether, BDE100, varied more than the other PBDE isomers due to its poor separation in some chromatographic conditions. In addition, interference by PBDEs was observed in the analysis for PBDFs. Potential degradation/secondary formulation of PBDEs and PBDFs during the Soxhlet extraction were suggested when copper powder was added into the sediment samples. Inspite of these observations, the results in this study are better than those reported in other interlaboratory studies due to the advice given to participants for improving the results. Compared with the results for PCDDs/DFs (5-23% RSDs) and Co-PCBs (6 24% RSDs), the RSDs for most of the organobromine compounds were high, indicating an immature QA/QC approach for the analysis of PBDEs and related compounds in comparison to common chlorinated dioxins. (c) 2006 Elsevier Ltd. All rights reserved.
• Organotin residues and the role of anthropogenic tin sources in the coastal marine environment of Indonesia

  A Sudaryanto, S Takahashi, H Iwata, S Tanabe, M Muchtar, H Razak

  MARINE POLLUTION BULLETIN 50 (2) 227 - 236 0025-326X 2005/02 Scientific journal
• Status of butyltin pollution along the coasts of western Japan in 2001, 11 years after partial restrictions on the usage of tributyltin

  R Murai, S Takahashi, S Tanabe, Takeuchi, I

  MARINE POLLUTION BULLETIN 51 (8-12) 940 - 949 0025-326X 2005 Scientific journal 

  Restrictions on the use of tributyltin (TBT) in aquaculture and on boats in coastal regions, except for ocean-going vessels, have been in place in Japan since 1990 due to the strong toxic effects of TBT on marine organisms. However, TBT pollution along the Japanese coasts has been reported after this legislation was enacted. In order to elucidate the present status of contamination by butyltin (BT) compounds, we measured the levels of BTs [monobutyltin (MBT), dibutyltin (DBT) and TBT] in seawater and Caprella spp. samples obtained from the western part of Seto Inland Sea, Uwa Sea and Uranouchi Bay in western Japan during March to September, 2001. Butyltins were detected in more than 90% of the seawater samples (n = 59), with average concentrations of 8.2 +/- 9.2 (SID) ng MBT L-1, 3.3 +/- 3.0 ng DBT L-1 and 9.0 +/- 7.0 ng TBT L-1. Among 41 stations situated on coastal lines, a sufficient number of Caprella organisms for chemical analysis could be collected from only 16 stations. The butyltin concentrations in seawater and Caprella samples from Uwa Sea and Uranouchi Bay, in which the dominant industry in both waters is aquaculture, showed significantly higher than or no significant differences from those samples from the western part of Seto Inland Sea, a major heavy-industry area in Japan. As the TBT concentration in seawater increased, the number of Caprella organisms collected decreased. The mean TBT concentration among the seawater samples was above the estimated lowest observable effect concentration (LOEC) that reduces the survival rate of Caprella dandevskii. Thus, the present study indicates that TBT is still a potential ecological hazard to the survival of marine invertebrates inhabiting coasts along western Japan, even I I years after the partial ban on TBT usage was implemented. (c) 2005 Elsevier Ltd. All rights reserved.
• Decline of butyltin levels in Caprella spp. (Crustacea : Amphipoda) inhabiting the Sargassum community in Otsuchi Bay, Japan from 1994 to 2001

  Takeuchi, I, S Takahashi, S Tanabe

  JOURNAL OF THE MARINE BIOLOGICAL ASSOCIATION OF THE UNITED KINGDOM 84 (5) 911 - 918 0025-3154 2004/10 Scientific journal 

  Caprella spp. (Crustacea: Amphipoda) inhabiting the Satgassum algal community in Otsuchi Bay near unpopulated areas of northern Japan, were collected froth 1994 to 2001 and subjected to analysis of butyltin (BT) concentrations. The period from 1994 to 2001 corresponds to four to 11 years after legislation limiting the use of tributyltin (TBT) on small boats and aquaculture facilities was passed in Japan. Butyltin compounds including TBT, dibutyltin (DBT) and monobutyltin (MBT) were detected in all samples of Capzella spp., although the three BTs were not detected in seawater samples collected from the same area between 1997 and 1999. The concentration of total BTs (BTs=MBT+DBT+TBI') in Caprella spp. significantly decreased froth 84 ng BTs/g wet wt in 1994 to 7.4 ng/g wet wt in 2001. The concentrations of BTs in Caprella spp., which have a high bioconcentration factor for TBh are thought to reflect the average concentrations of BTs in the surrounding seawater in the previous few months. The half-life of BTs and TB 1, in Capzella spp. was 2.38 years and 2.07 years, respectively, which are less than half of that of TBT in seawater based on the national survey of The Ministry of the Environment, Japan. Illegal usage of TBT near the studied area may have decreased due to monitoring of BTs.
• Contamination of butyltin compounds in Malaysian marine environments

  A Sudaryanto, S Takahashi, H Iwata, S Tanabe, A Ismail

  ENVIRONMENTAL POLLUTION 130 (3) 347 - 358 0269-7491 2004/08 Scientific journal 

  Concentration of butyltin compounds (BTs), including tributyltin (TBT), dibutyltin (DBT) and monobutyltin (MBT) and total tin (SigmaSn) were determined in green mussel (Perna viridis), 10 species Of Muscle fish and sediment from coastal waters of Malaysia. BTs were detected in all these samples ranging from 3.6 to 900 ng/g wet wt., 3.6 to 210 ng/g wet wt., and 18 to 1400 ng/g dry wt. for mussels, fish and sediments, respectively. The concentrations of BTs in several locations of this study were comparable with the reported values from some developed countries and highest among Asian developing nations. Considerable concentration of BTs in several locations might have ecotoxicological consequences and may cause concern to human health. The parent compound TBT was found to be highest than those of its degradation compounds, DBT and MBT, suggesting recent input of TBT to the Malaysian marine environment. Significant positive correlation (Spearman rank correlation: r(2) = 0.82, P < 0.0001) was found between BTs and SigmaSn, implying considerable anthropogenic input of butyltin compounds to total tin contamination levels. Enormous boating activities may be a major source of BTs in this country, although aquaculture activities may not be ignored. (C) 2004 Elsevier Ltd. All rights reserved.
• Butyltin concentrations along the Japanese coast from 1997 to 1999 monitored by Caprella spp. (Crustacea : Amphipoda)

  Takeuchi, I, S Takahashi, S Tanabe, N Miyazaki

  MARINE ENVIRONMENTAL RESEARCH 57 (5) 397 - 414 0141-1136 2004/06 Scientific journal 

  The concentrations of butyltins along the Japanese coastline were investigated from 1997 to 1999, 7 to 9 years after implemantion of legislation limiting the use of tributyltin (TBT) in Japan. Seawater was sampled at 0.5 m depth, and Caprella spp. were collected from Sargassum spp. and aquaculture facilities from 18 areas within four broad areas along the coastline of Japan, i.e., the Pacific coast of northern Japan, the coast along the Sea of Japan, Tokyo Bay and adjacent areas, and western Japan. Butyltins (MBT, DBT and TBT) were detected in 32 of the 63 seawater samples with average concentrations of 4.6 ng MBT/l, 4.5 ng DBT/l and 6.8 ng TBT/l, respectively. Butyltin concentrations in seawater from western Japan indicate "hot spots" even in unpopulated areas. Butyltins (MBT, DBT and TBT) were detected in all samples of Caprella spp., varying from 2.3 ng BTs/g wet wt in C. penantis R-type from Tobishima Island in the Sea of Japan to 464 ng BTs Ig wet wt in C. decipiens Mayer from Amakusa, western Kyushu. The BT concentrations in Caprella spp. form western Japan were significantly higher than those from other areas, including Tokyo Bay and adjacent areas, where large scale industry and international ports are located. These results indicate that butyltin contamination still remains even in unpopulated areas after the regulation on TBT usage, and that the regulation govering TBT usage since 1990 has not been effective enough to concede recovery of shallow water ecosystems around Japan. (C) 2004 Elsevier LTD. All rights reserved.
• Global pollution monitoring of butyltin compounds using skipjack tuna as a bioindicator

  D Ueno, S Inoue, S Takahashi, K Ikeda, H Tanaka, AN Subramanian, G Fillmann, PKS Lam, J Zheng, M Muchtar, M Prudente, K Chung, S Tanabe

  ENVIRONMENTAL POLLUTION 127 (1) 1 - 12 0269-7491 2004 Scientific journal 

  Butyltin compounds (BTs) including mono- (MBT), di- (DBT), tri-butyltin (TBT) and total tin (SigmaSn), were determined in the liver of skipjack tuna (Katsuwonus pelamis) collected from Asian offshore waters (off-Japan, the Japan Sea, off-Taiwan, the East China Sea. the South China Sea, off-Philippines, off-Indonesia, the Bay of Bengal), off-Seychelles, off-Brazil and open seas (the North Pacific). BTs were detected in all the skipjack tuna collected, suggesting widespread contamination of BTs even in offshore waters and open seas on a global scale. Considering specific accumulation, Sex-, body length- differences and migration of skipjack tuna did not seem to affect BT concentrations, indicating rapid reflection of the pollution levels in seawater where and when they were collected. Skipjack tuna is a suitable bioindicator for monitoring the global distribution of BTs in offshore waters and open seas. High concentrations of BTs were observed in skipjack tuna from offshore waters around Japan, a highly developed and industrialized region (up to 400 ng/g wet weight). Moreover skipjack tuna collected from offshore waters around Asian developing countries also revealed the levels comparable to those in Japan (up to 270 ng/g wet weight) which may be due to the recent improvement in economic status in Asian developing countries. High percentages (almost 90%) of BTs in total tin (SigmaSn: sum of inorganic tin+ organic tin) were found in the liver of skipjack tuna from offshore waters around Asian developing countries. This finding suggests that the anthropogenic BTs represent the major source of Sri accumulation in skipjack tuna from these regions. (C) 2003 Elsevier Ltd. All rights reserved.
• Global pollution monitoring of PCBs and organochlorine pesticides using skipjack tuna as a bioindicator

  D Ueno, S Takahashi, H Tanaka, AN Subramanian, G Fillmann, H Nakata, PKS Lam, J Zheng, M Muchtar, M Prudente, KH Chung, S Tanabe

  ARCHIVES OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY 45 (3) 378 - 389 0090-4341 2003/10 Scientific journal 

  Concentrations of organochlorines (OCs) representing persistent organic pollutants (POPS), such as polychlorinated biphenyls (PCBs), dichlorodiphenyl trichloroethane and its metabolites (DDTs), chlordane compounds (CHLs), hexachlorocyclohexane isomers (HCHs), and hexachlorobenzene (HCB), were determined in the liver of skipjack tuna (Katsuwonus pelamis) collected from the offshore waters of various regions in the world (offshore waters around Japan, Taiwan, Philippines, Indonesia, Seychelles, and Brazil, and the Japan Sea, the East China Sea, the South China Sea, the Bay of Bengal, and the North Pacific Ocean). OCs were detected in livers of all of the skipjack tuna collected from the locations surveyed, supporting the thesis that there is widespread contamination of persistent OCs in the marine environment. Within a location, no significant relationship between growth-stage (body length and weight) and OC concentrations (lipid weight basis) was observed, and the OC residue levels were rather uniform among the individuals. Interestingly, the distribution of OC concentrations in skipjack tuna was similar to those in surface seawaters from which they were taken. These results suggest that OC concentrations in skipjack tuna could reflect the pollution levels in seawater from which they are collected and that this species is a suitable bioindicator for monitoring the global distribution of OCs in offshore waters and the open ocean. Concentrations of PCBs and CHLs in skipjack tuna were higher in offshore waters around Japan (up to 1100 and 250 ng/g lipid wt, respectively), suggesting the presence of sources of PCBs and CHLs in Japan. High concentrations of DDTs and HCHs were observed in samples from the Japan Sea, the East China Sea, the South China Sea, and the Bay of Bengal (up to 1300 and 22 ng/g lipid wt, respectively). This result suggests recent use of technical DDT and HCH for agricultural and/or public health purposes in Russia, China, India, and some other developing Asian countries. Relatively high concentrations of PCBs, CHLs, HCHs, and HCB were also observed in samples collected from some locations in the middle of the Pacific Ocean, indicating the expansion of OC contamination on a global scale. Considering these facts, continuous studies monitoring these compounds in offshore waters and the open seas, using skipjack tuna as a bioindicator, are needed to further understand the future trend of contamination.
• Asia-Pacific mussel watch: monitoring contamination of persistent organochlorine compounds in coastal waters of Asian countries

  Monirith, I, D Ueno, S Takahashi, H Nakata, A Sudaryanto, A Subramanian, S Karuppiah, A Ismail, M Muchtar, JS Zheng, BJ Richardson, M Prudente, ND Hue, TS Tana, AV Tkalin, S Tanabe

  MARINE POLLUTION BULLETIN 46 (3) 281 - 300 0025-326X 2003/03 

  Contamination of persistent organochlorines (OCs) such as PCBs (polychlorinated biphenyls), DDT and its metabolites (DDTs), HCH (hexachlorocyclohexane) isomers (HCHs), chlordane compounds (CHLs), and HCB (hexachlorobenzene) were examined in mussels collected from coastal waters of Asian countries such as Cambodia, China, Hong Kong, India, Indonesia, Japan, Korea, Malaysia, Philippines, Far East Russia, Singapore, and Vietnam in 1994, 1997, 1998, 1999, and 2001 to elucidate the contamination status, distribution and possible pollution sources and to assess the risks on aquatic organisms and human. OCs were detected in all mussels collected from all the sampling sites investigated. Considerable residue levels of p,p'-DDT and alpha-HCH were found in mussels and the concentrations of DDTs and HCHs found in mussels from Asian developing countries were higher than those in developed nations suggesting present usage of DDTs and HCHs along the coastal waters of Asian developing countries. On the other hand, lower concentrations of PCBs detected in mussels from Asian developing countries than those in developed countries indicate that PCBs contamination in mussels is strongly related to industrial and activities. To our knowledge, this is a first comprehensive report on monitoring OCs pollution in the Asia-Pacific region. (C) 2002 Elsevier Science Ltd. All rights reserved.
• Contamination by butyltin compounds in sediments, cultured fishes (Seriola quinqueradiata and Pagrus major) and pearl oysters (Pinctada martensii) collected from Uwa Sea, Japan

  H Sakai, R Kasai, S Takahashi, S Tanabe

  NIPPON SUISAN GAKKAISHI 69 (1) 10 - 22 0021-5392 2003/01 Scientific journal 

  Butyltin compounds (MBT, DBT, TBT) were determined in surface sediments, sediment cores, cultured fishes and pearl oysters collected from Uwa Sea, Japan. TBT concentrations in surface sediments ranged from 2.8 to 930 ng/g dry wt, which were comparable to those in urban regions such as Tokyo Bay, Osaka Bay and Dokai Bay. SigmaBTs (MBT + DBT + TBT) concentrations in surface sediments from fish culture areas were significantly higher than those from pearl oyster areas. In case of sediment cores, BTs concentration was the highest in the surface layer and decreased with core depth. SigmaBTs concentrations in pearl oysters were lower than those in other species of bivalves from various coastal waters around the world, whereas SigmaBTs concentrations in cultured fish from Uwa Sea were comparable to those reported in Osaka Bay. Higher proportions of TBT in SigmaBTs residues were found in fish and pearl oysters than in sediments. Although TBT concentrations found in cultured fishes were less than the tolerable level estimated from ADI suggested by the Ministry of Health and Welfare, efforts to reduce the residue levels are needed for the conservation of ecosystems.
• Contamination by butyltin compounds in sediments, cultured fishes (Seriola quinqueradiata and Pagrus major) and pearl oysters (Pinctada martensii) collected from Uwa Sea, Japan

  H Sakai, R Kasai, S Takahashi, S Tanabe

  NIPPON SUISAN GAKKAISHI 公益社団法人日本水産学会 69 (1) 10 - 22 0021-5392 2003/01 Scientific journal 

  Butyltin compounds (MBT, DBT, TBT) were determined in surface sediments, sediment cores, cultured fishes and pearl oysters collected from Uwa Sea, Japan. TBT concentrations in surface sediments ranged from 2.8 to 930 ng/g dry wt, which were comparable to those in urban regions such as Tokyo Bay, Osaka Bay and Dokai Bay. SigmaBTs (MBT + DBT + TBT) concentrations in surface sediments from fish culture areas were significantly higher than those from pearl oyster areas. In case of sediment cores, BTs concentration was the highest in the surface layer and decreased with core depth. SigmaBTs concentrations in pearl oysters were lower than those in other species of bivalves from various coastal waters around the world, whereas SigmaBTs concentrations in cultured fish from Uwa Sea were comparable to those reported in Osaka Bay. Higher proportions of TBT in SigmaBTs residues were found in fish and pearl oysters than in sediments. Although TBT concentrations found in cultured fishes were less than the tolerable level estimated from ADI suggested by the Ministry of Health and Welfare, efforts to reduce the residue levels are needed for the conservation of ecosystems.
• Asia-Pacific mussel watch: Monitoring of butyltin contamination in coastal waters of Asian developing countries

  A Sudaryanto, S Takahashi, Monirith, I, A Ismail, M Muchtar, J Zheng, BJ Richardson, A Subramanian, M Prudente, ND Hue, S Tanabe

  ENVIRONMENTAL TOXICOLOGY AND CHEMISTRY 21 (10) 2119 - 2130 0730-7268 2002/10 [Peer-reviewed]
   Scientific journal 

  Butyltin compounds (BTs) including mono-, di-, and tributyltin and total tin (SigmaSn), were determined in green mussels (Perna viridis) from various Asian developing countries, such as Cambodia, China (Hong Kong and southern China), Malaysia, India, Indonesia, the Philippines, and Vietnam. to elucidate the contamination status, distribution, and possible sources and to assess the risks on aquatic organisms and humans. Butyltin compounds were detected in green mussels collected from all the sampling location investigated, suggesting widespread contamination of BTs along the coastal waters of Asian developing countries. Among butyltin derivatives, tributyltin (TBT) was the predominant compound, indicating its ongoing usage and recent exposures in Asian coastal waters. Higher concentrations of BTs were found in mussels collected at locations with intensive maritime activities, implying that the usage of TBT as a biocide in antifouling paints was a major source of BTs. In addition, relatively high concentrations of BTs were observed in mussels from aquaculture areas in Hong Kong and Malaysia, as it has been reported in Thailand. With the recent improvement in economic status in Asia, it is probable that an increase in TBT usage will occur in aquaculture, Although contamination levels were generally low in mussel samples from most of the Asian developing countries, some of those from polluted areas in Hong Kong, India. Malaysia, the Philippines, and Thailand revealed levels, comparable to those in developed nations. Furthermore, the concentrations of TBT in some mussels from polluted areas exceeded the threshold for toxic effects on organisms and estimated tolerable average residue levels as seafoods for human consumption, A significant correlation was observed between the concentrations of SigmaBTs and SigmaSn in mussels, and SigmaBTs were made up mostly 100% of SigmaSn in mussels taken from locations having intensive maritime/human activities. This suggests that anthropogenic BTs represent the major source of tin accumulation in mussels. To our knowledge, this is a first comprehensive report on butyltin pollution monitoring in developing countries in the Asia-Pacific region.
• Contamination by organochlorine compounds in walleye pollock (Theragra chalcogramma) from the Bering Sea, Gulf of Alaska and the Japan Sea

  APX de Brito, D Ueno, S Takahashi, S Tanabe

  MARINE POLLUTION BULLETIN 44 (2) 172 - 177 0025-326X 2002/02 [Peer-reviewed]
   Scientific journal
• Organochlorine and butyltin residues in deep-sea organisms collected from the western North Pacific, off-Tohoku, Japan

  APX de Brito, S Takahashi, D Ueno, H Iwata, S Tanabe, T Kubodera

  MARINE POLLUTION BULLETIN 45 (1-12) 348 - 361 0025-326X 2002 [Peer-reviewed]
   Scientific journal 

  Organochlorine (OCs) and butyltin (BTs) residues were determined in deep-sea organisms collected from the western North Pacific, off-Tolioku, Japan. Among OCs, concentrations of polychlorinated biphenyls (PCBs') and DDTs (DDTs and its metabolites) were the highest in deep-sea organisms (maximum concentrations of 6700 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 front 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 mug/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 (similar to1000 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. (C) 2002 Elsevier Science Ltd. All rights reserved.
• Organochlorine and organotin compounds in Caspian seals (Phoca caspica) collected during an unusual mortality event in the Caspian Sea in 2000

  N Kajiwara, S Niimi, M Watanabe, Y Ito, S Takahashi, S Tanabe, LS Khuraskin, N Miyazaki

  ENVIRONMENTAL POLLUTION 117 (3) 391 - 402 0269-7491 2002 [Peer-reviewed]
   Scientific journal 

  Polychlorinated biphenyls (PCBs), organochlorine pesticides and organotin compounds were determined in the blubber and liver of Caspian seals (Phoca caspica) found stranded on the coast of the Caspian Sea during an outbreak of canine distemper virus (CDV) in 2000. Among organochlorines analyzed, DDTs were the most dominant contaminants with concentrations ranging from 6.3 to 470 mug/g on a lipid-weight basis. Caspian seals collected in 2000 during the epizootic had higher concentrations of organochlorines than healthy individuals sampled in 1998. However, the blubber layer was generally thinner in the seals collected in 2000 than those in the previous surveys. Although compositions of organochlorine pesticides in seals suggested that the contamination status in the Caspian Sea is improving, the levels found in Caspian seals in 2000 were comparable to those in other marine mammals that have suffered from epizootics. This implies that the present status of contamination found in Caspian seals poses a risk of immunosuppression. Concentrations of butyltin compounds in livers of seals ranged from 0.49 to 17 ng/g on a wet-weight basis and octyltin compounds were below limit of detection in all the samples analyzed, suggesting less contamination by organotin compounds in the Caspian Sea. (C) 2002 Elsevier Science Ltd. All rights reserved.
• Differences in the acute toxicities of tributyltin between the Caprellidea and the Gammaridea (Crustacea : Amphipoda)

  M Ohji, Takeuchi, I, S Takahashi, S Tanabe, N Miyazaki

  MARINE POLLUTION BULLETIN 44 (1) 16 - 24 0025-326X 2002/01 Scientific journal 

  Tests for the acute toxicity of tributyltin (TBT) were conducted on amphipod crustaceans collected from Otsuchi Bay, Japan. Five species of caprellids and three species of gammarids, which belong to a closely related ecological niche, were used for the exposure experiments at seven test concentrations (0, 0.001, 0.01, 0.1, 1, 10 and 100 mug TBTCl/l) for 48 h at 20degreesC. The 48-h LC50 values of the caprellids were 1.2-6.6 mug TBTCl/l, and these were significantly lower than those of the gammarids (17.8-23.1 mug TBTCl/l). This suggests that caprellids are more sensitive to TBT than gammarids. Furthermore, the proportions of TBT and its derivatives, dibutyltin (DBT) and monobutyltin (MBT), were measured in the amphipods collected from Otsuchi Bay. In the caprellids, TBT was the predominant compound. accounting for 72% of the total butyltin which reflected the butyltin ratio in seawater, while in the gammarids, TBT's breakdown products (DBT and MBT) predominated, accounting for 75% of the total butyltin. This difference suggests that caprellids may have lower metabolic capacity to degrade TBT than gammarids. Therefore, the difference in sensitivity to TBT among the amphipods is thought to be related to the species-specific capacity to metabolize TBT. (C) 2002 Elsevier Science Ltd. All rights reserved.
• Organochlorine and butyltin residues in walleye pollock (Theragra chalcogramma) from Bering Sea, Gulf of Alaska and Japan Sea

  APX de Brito, D Ueno, S Takahashi, S Tanabe

  CHEMOSPHERE 46 (3) 401 - 411 0045-6535 2002/01 [Peer-reviewed]
   Scientific journal 

  Persistent organochlorine (OC) and toxic butyltin compounds (BTs) were determined in walleye pollock (Theragra chalcogramma) collected from Gulf of Alaska, Bering Sea and Japan Sea, during 1991 and 1992. Polychlorinated biphenyls (PCBs) and dichlorodiphenyltrichloroethane (DDTs) and its metabolites were the most abundant compounds ranging up to 3200 and 2500 ng/g on lipid weight, respectively, followed by chlordane compounds (CHLs), hexachlorocyclohexane isomers (HCHs) and hexachloro benzene (HCB) in the liver of walleye pollock. Concentrations of HCHs and HCB in walleye pollock from these remote areas were higher than those in fishes from the western North Pacific and Japanese coastal waters, indicating atmospheric transport of these compounds to higher latitude regions such as Bering Sea and Gulf of Alaska and/or local input around northern Japan Sea. The concentrations of other OCs were generally comparable to those in fishes from North Pacific Ocean and Japanese waters but significantly lower than in cod-like fishes from North Atlantic and European countries. Among sampling locations, walleye pollock from Japan Sea showed higher concentrations of DDTs and HCHs compared to fishes from Bering Sea and Gulf of Alaska, suggesting greater input of these compounds around Japan Sea. Slower declining trend of DDTs and CHLs and an increasing pattern of PCBs concentrations were found in walleye pollock from Bering Sea during 1982-1992. This may imply a continuous input of these compounds by long-range transport and/or long-term persistency in these cold regions. Compared to the fishes from Japan Sea, walleye pollock from Bering Sea and Gulf of Alaska showed higher proportions of alpha-HCH and p,p'-DDE in the composition of HCH isomers and DDT compounds, respectively. This suggests selective transportability of these compounds during long-range transport to higher latitude remote areas. Concentrations of tributyltin (TBT) in the muscle of walleye pollock ranged from 1.1 to 5.5 ng/g on wet weight. Concentrations of TBT in deep-sea walleye pollock from Gulf of Alaska and Bering Sea were lower than those in Japan Sea. (C) 2002 Elsevier Science Ltd. All rights reserved.
• Butyltin residues in blue mussels (Mytilus edulis) and arkshells (Scapharca broughtonii) collected from Korean coastal waters

  HK Hong, S Takahashi, BY Min, S Tanabe

  ENVIRONMENTAL POLLUTION 117 (3) 475 - 486 0269-7491 2002 [Peer-reviewed]
   Scientific journal 

  Butyltin compounds (BTs) including tributyltin (TBT) and its degradation products, di- (DBT) and mono-butyltin (MBT), were determined in bivalves such as blue mussels (Mytilus edulis) and arkshells (Scapharca broughtonii) collected from Korean coastal waters. BTs were detected in all the blue mussels and arkshells analyzed. The concentrations of total butyltin (SigmaBTs: MBT + DBT + TBT) in blue mussels and arkshells ranged from 49 to 2500 ng/g and 29 to 87 ng/g wet weight, respectively. Higher concentrations of BTs were found in blue mussels collected from Okpo and Kohyonsong Bays and Jangsengpo Harbor where large shipyards and harbors are located with dry-dock facilities. This suggested that maritime activities nearby the harbors play a major role as the source of BTs. Concentrations of TBT in mussels collected from Korea were one of the highest values reported, suggesting ongoing TBT contamination in Korea. Among BTs, TBT was the predominant compound both in blue mussels and arkshells collected from almost all the sampling locations, indicating the fresh input of TBT in Korean coastal waters. Smaller mussels tended to accumulate BTs at higher concentrations than larger ones, which may be due to higher filtration rate of small mussels and/or contact with surface microlayer in intertidal zones. (C) 2002 Elsevier Science Ltd. All rights reserved.
• Variations of organochlorine concentrations in blue mussels associated with season, size and vertical habitat

  D Ueno, S Takahashi, S Tanabe, K Ikeda, J Koyama, H Yamada

  NIPPON SUISAN GAKKAISHI 67 (5) 887 - 893 0021-5392 2001/09 Scientific journal 

  Live speciments of the blue mussel Mytilus galloprovincialis were collected from the southwestern coastal region of Tokyo Bay and examined for seasonal, size-dependent and spatial variations in the concentrations of organochlorine compounds (OCs) such as PCBs (polychlorinated biphenyls), DDTs (DDT and its metabolites), CHLs (chlordane and related compounds), HCHs (hexachlorocyclohexane isomers) and HCB (hexachlorobenzene), Seasonal variations in OCs concentrations (fat weight base) appeared to reflect the levels in an ambient water rather than seasonal physiological changes of mussels. Neither shell size nor vertical habitation of mussels resulted in significant differences in their concentrations (fat weight base). These results suggest that the variable factors examined did not significantly affect the availability and suitability of mussels as bioindicators for monitoring of contamination with OCs.
• Variations of organochlorine concentrations in blue mussels associated with season, size and vertical habitat

  D Ueno, S Takahashi, S Tanabe, K Ikeda, J Koyama, H Yamada

  NIPPON SUISAN GAKKAISHI 公益社団法人日本水産学会 67 (5) 887 - 893 0021-5392 2001/09 Scientific journal 

  Live speciments of the blue mussel Mytilus galloprovincialis were collected from the southwestern coastal region of Tokyo Bay and examined for seasonal, size-dependent and spatial variations in the concentrations of organochlorine compounds (OCs) such as PCBs (polychlorinated biphenyls), DDTs (DDT and its metabolites), CHLs (chlordane and related compounds), HCHs (hexachlorocyclohexane isomers) and HCB (hexachlorobenzene), Seasonal variations in OCs concentrations (fat weight base) appeared to reflect the levels in an ambient water rather than seasonal physiological changes of mussels. Neither shell size nor vertical habitation of mussels resulted in significant differences in their concentrations (fat weight base). These results suggest that the variable factors examined did not significantly affect the availability and suitability of mussels as bioindicators for monitoring of contamination with OCs.
• Caprella watch: a new approach for monitoring butyltin residues in the ocean

  A Takeuchi, S Takahashi, S Tanabe, N Miyazaki

  MARINE ENVIRONMENTAL RESEARCH 52 (2) 97 - 113 0141-1136 2001/08 Scientific journal 

  A comparative study on the butyltin levels in various organisms showed that marked bioaccumulation occurs in certain lower trophic levels; i.e. from seawater to phytoplankton and into caprellid amphipods, Caprella spp. Caprella spp., which inhabit al.-al communities and aquaculture beds in the subtidal zone, are small crustaceans with reduced movement and a life-span of less than 3 months. These characteristics indicate that Caprella spp. may be well-suited for monitoring butyltin residue changes over small spatial and temporal scales. Two groups of organisms, mussels and neogastropods, have been mainly used for monitoring butyltin in shallow water ecosystems. These invertebrates mainly inhabit the intertidal zone where the butyltin levels vary widely depending on the immersion period and exposure to the sea surface microlayer. Monitoring using neogastropods may also over estimate exposures after restrictions on tributyltin, since neogastropods show an irreversible response to residue changes owing to their long life-spans. Thus, we propose usage of Caprella spp. to monitor temporal and spatial changes in baseline concentrations of butyltins. (C) 2001 Elsevier Science Ltd. All rights reserved.
• Organochlorine pesticides, polychlorinated biphenyls, and butyltin compounds in blubber and livers of stranded California sea lions, elephant seals, and harbor seals from coastal California, USA

  N Kajiwara, K Kannan, M Muraoka, M Watanabe, S Takahashi, F Gulland, H Olsen, AL Blankenship, PD Jones, S Tanabe, JP Giesy

  ARCHIVES OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY 41 (1) 90 - 99 0090-4341 2001/07 [Peer-reviewed]
   Scientific journal 

  Concentrations of polychlorinated biphenyls (PCBs), DDTs (p,p ' -DDE, p,p ' -DDD, p,p ' -DDT), chlordanes (CHLs; cis-chlordane, cis-nonachlor, trans-nonachlor, and oxychlordane), hexachlorocyclohexane isomers (HCHs), hexachlorobenzene (HCB), tris(4-chlorophenyl)methane (TCPMe), tris(4-chlorophenyl)methanol (TCPMOH), and mono- (MBT), di-(DBT), and tri-butyltin (TBT) were determined in blubber and livers of 15 California sea lions (Zalophus californianus), 6 northern elephant seals (Mirounga augustirostris), and 10 harbor seals (Phoca vitulina) found stranded along the coasts of California, USA, during 1991-1997. Among the organochlorines analyzed, DDTs were predominant, followed in decreasing order by PCBs, CHLs, TCPMe, TCPMOH, HCHs, and HCB. The greatest concentrations of organochlorines were found in California sea lions. The highest DDT and PCB concentrations found in the blubber of California sea lions were 2,900 and 1,300 mug/g, lipid weight, respectively. Concentrations of TCPMe and TCPMOH in California sea lions were correlated significantly with DDT concentrations. Concentration ratios of various organochlorines in harbor seal livers were different from those in California sea lions and elephant seals, which suggested that the sources of exposure of harbor seals to organochlorines were different from those in the other two species. Concentrations of butyltin compounds in livers of pinniped species ranged from 2 to 99 ng/g, wet weight, which were less than those observed in cetaceans and in California sea otters.
• Organochlorine and butyltin residues in mesopelagic myctophid fishes from the western North Pacific

  S Takahashi, S Tanabe, K Kawaguchi

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 34 (24) 5129 - 5136 0013-936X 2000/12 [Peer-reviewed]
   Scientific journal 

  Organochlorine (OCs) and butyltin (BTs) residues were determined in mesopelagic myctophid fishes collected from the western North Pacific to elucidate contamination status, accumulation patterns, and distribution. Among OCs, concentrations of PCBs (polychlorinated biphenyls) and DDTs (DDT and its metabolites) were the highest in myctophids (at maximum concentrations bf 370 ng/g and 280 ng/g lipid wt, respectively). CHLs (chlordane compounds) or HCHs (hexachlorocyclohexanes) were the next most abundant OCs, and HCB (hexachlorobenzene) was the lowest. The maximum concentration of total butyltin (Sigma BTs = MBT + DBT + TBT) in fish was 46 ng/g wet wt. Concentrations of PCBs, CHLs, and BTs were significantly lower in oceanic myctophids than those in fishes from Japanese coastal water, Suruga Bay. The residue pattern of OCs and BTs showed a specific trend according to diel vertical migration of myctophids. Relatively high concentrations of PCBs, DDTs, and CHLs were found in nonmigratory species living in deeper waters, whereas concentrations of HCHs, HCB, and BTs were high in migratory species, which migrate up to the upper 200 m at night for feeding. These patterns are also influenced by the vertical distributions of OCs and BTs in the subarctic and transitional waters of the western North Pacific, where intrusion of watermass from the Okhotsk Sea has been suggested. Temporal variation in the residue level and composition of OCs found in myctophids indicated a significant decrease in the input of DDTs into the marine environment while HCHs declined at a slower rate.
• Accumulation of butyltin compounds and total tin in marine mammals

  S Takahashi, LTH Le, H Saeki, N Nakatani, S Tanabe, N Miyazaki, Y Fujise

  WATER SCIENCE AND TECHNOLOGY 42 (7-8) 97 - 108 0273-1223 2000 [Peer-reviewed]
   

  Concentrations of butyltin compounds (BTs), including tributyltin (TBT) and its metabolites, di-(DBT) and monobutyltin (MBT), and total tin (n=organic +inorganic tin) were determined in various tissues and organs of marine mammals collected from Japanese coastal waters. Some marine mammal species from Hong Kong, India, Philippines, Black Sea and North Pacific Ocean were analyzed for comparison. Among the organs and tissues analyzed. concentrations of Sigma BTs (TBT+DBT+MBT) and Sigma Sn were the highest in the liver. Concentrations of Sigma BTs and Sigma Sn in most coastal species were higher than those in offshore species, indicating a greater input of tin compounds in coastal waters. Lower hepatic concentrations of Sigma BTs and ratio of Sigma BTs to Sigma Sn observed in pinnipeds may be attributed to higher metabolic capacity to degrade BTs and to their excretion through hair shedding. Age trends in accumulation of both Sigma BTs and Sigma Sn showed increasing concentrations in immature growth stage and stable levels in mature animals. A significant correlation was observed between the hepatic concentrations of Sigma BTs and Sigma Sn in marine mammals. These findings suggest a significant input and/or bioaccumulation of anthropogenic tin. A significant correlation was found between concentrations of Sigma BTs (as wen as Sigma Sn) in hair and liver of pinnipeds, suggesting that hair can be used as an indicator for monitoring butyltin contamination in the body of pinnipeds under non-killing condition.
• Organochlorine contamination in fish and mussels from Cambodia and other Asian countries

  Monirith, I, H Nakata, M Watanabe, S Takahashi, S Tanabe, TS Tana

  WATER SCIENCE AND TECHNOLOGY 42 (7-8) 241 - 252 0273-1223 2000 [Peer-reviewed]
   

  Contamination by organochlorine compounds (OCs) was examined in fish and mussels collected from Cambodia and other Asian developing countries in 1997 and 1998. DDT and its metabolites were the predominantly detected compound in both fish and mussel samples. PCBs were second highest, followed by HCHs, CHLs, and HCB. Freshwater fish contained higher concentrations of DDTs than marine fish and mussels, implying that the source of DDTs originated from inland watersheds such as the Mekong River, Basac River, Tonlesap River, and Tonlesap Great Lake. Comparison of the OC residue levels in fish and mussels from Cambodia with those in other Asian and Oceanic regions suggested that Cambodia is one of the countries least contaminated by OCs. In other words, it can be concluded that among Asian and Oceanic countries Cambodia has kept a "Clean Environment".
• Occurrence of butyltin compounds in mussels from Indonesian coastal waters and some Asian countries

  A Sudaryanto, S Takahashi, S Tanabe, M Muchtar, H Razak

  WATER SCIENCE AND TECHNOLOGY 42 (7-8) 71 - 79 0273-1223 2000 [Peer-reviewed]
   

  The green mussel (Perna viridis) samples were collected from Indonesian coastal waters and some other Asian countries in the period of 1997-1998 to elucidate the present status of marine pollution by butyltin compounds (BTs) including mono- (MBT), di- (DBT), and tributyltin (TBT). BTs were detected in all the mussel samples from Indonesian coastal waters in the range of 3.7 to 64 ng/g wet wt as total butyltins (Sigma BTs = MBT+DBT+TBT). The highest concentrations were found in green mussels from Jakarta Bay and Surabaya coastal waters. Relatively higher concentrations of BTs were detected in the mussels from adjacent areas of high maritime activities such as marina, harbour and fishing port. This suggests pollution of BTs arising from TBT usage in antifouling paints. BTs were also detected in mussels from aquaculture areas, implying TBT usage for fisheries activity. The composition of butyltin derivatives in green mussels from Indonesian coastal waters were in the order of TBT>MBT>DBT, suggesting fresh input of TBT in the marine environment. The contamination levels of BTs in green mussels from Indonesia were comparable or lower than those from other Asian developing countries. The elevated concentrations of BTs ware found in mussels from some areas of Thailand, Philippines, India and Malaysia where residue levels of BTs were comparable to those in developed nations.
• Distribution and specific bioaccumulation of butyltin compounds in a marine ecosystem

  S Takahashi, S Tanabe, Takeuchi, I, N Miyazaki

  ARCHIVES OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY 37 (1) 50 - 61 0090-4341 1999/07 Scientific journal 

  Butyltin compounds (BTs), including tributyltin (TBT) and its breakdown products, di- (DBT) and monobutyltin (MBT), were determined in sea water, sediment, and biota at various trophic levels in the food chain collected from Otsuchi Bay, Japan, for understanding distribution and bioaccumulation of BTs in natural marine ecosystems. BT residues were detected in all the compartments analyzed, although their concentrations appeared to be less than those in polluted areas. Concentrations of BTs in sea water were higher in locations near Otsuchi Port, indicating that maritime activities in the harbor has been a major source of BTs in this bay. A specific peak in BT residue levels was found in sediment cores at an estimated depth that dated to be from the 1980s. Lack of significant variation in the composition of BTs at different depths of cores suggests slow degradation rate of these compounds in sediments. BTs were accumulated in plankton and other organisms up to similar to 70,000 times higher than in sea water. However, no considerable biomagnification was observed for BTs through the food chain. Relatively high concentrations were found in caprellids and smaller fish, such as gunnels. These organisms accumulated TBT as the predominant compound among BT derivatives and showed higher bioconcentration factors for TBT than in other species reported so far. Our results suggest that certain organisms in the food chain may have a less capacity to degrade TBT, and therefore may accumulate BTs at elevated levels.
• High percentage of butyltin residues in total tin in the livers of cetaceans from Japanese coastal waters

  LTH Le, S Takahashi, K Saeki, N Nakatani, S Tanabe, N Miyazaki, Y Fujise

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 33 (11) 1781 - 1786 0013-936X 1999/06 [Peer-reviewed]
   Scientific journal 

  There have been few reports on quantitative discussion of organic tin compounds based on total tin in environmental media and biota. The present study determined concentrations of total tin (Sigma Sn = organic + inorganic) and butyltin compounds (Sigma BTs = MBT + DBT + TBT) in the livers of cetaceans collected from Japanese coastal waters in order to estimate the ratio of Sigma BTs:Sigma Sn and to elucidate the role of anthropogenic butyltins in the view of total tin accumulation in these higher trophic organisms. Additionally, some cetacean species from open seas and oceans were also subjected to analyses for comparison purposes. Higher concentrations of Sigma Sn and Sigma BTs were found in coastal species than in offshore species, indicating greater input of tin compounds in coastal waters surrounding Japan. Sigma Sn concentrations increased with an increase in Sigma BTs residues in all species analyzed (r = 0.95, p < 0.001). Furthermore, Sigma BTs made up considerably higher percentages of the hepatic Sigma Sn in coastal species, with up to 74% in finless porpoise (Neophocaena phocaenoides) and 90% in bottlenose dolphin (Tursiops troncatus). These findings suggest that hepatic tin in coastal cetaceans predominantly exists in organic form such as butyltin compounds, implying that tin residues in marine mammals reflect mostly the input from anthropogenic sources. Despite some similar features expected between the residues of tin and mercury, anthropogenic exposure to tin compounds seems to be more apparent than exposure to mercury, which generally originates from natural exposure.
• Butyltin residues in livers of humans and wild terrestrial mammals and in plastic products

  S Takahashi, H Mukai, S Tanabe, K Sakayama, T Miyazaki, H Masuno

  ENVIRONMENTAL POLLUTION 106 (2) 213 - 218 0269-7491 1999 [Peer-reviewed]
   Scientific journal 

  Butyltin compounds (BTs) including mono-(MBT), di-(DBT) and tributyltin (TBT) were determined in livers of humans and wild terrestrial mammals, such as raccoon dogs (Nyctereutes procyonoids) and monkeys (Macaca fuscata) from Japan. In addition, 22 samples of plastic products were analyzed. BT residues were detected in all the liver samples of humans and raccoon dogs, with concentrations of < 360 ng/g wet wt, whereas concentrations in the liver of monkeys were either less than the detection limit or were only in trace levels. Elevated concentrations of BTs, particularly DBT (< 140,000 ng/g) and MBT (< 130,000 ng/g), were found in some plastic products, such as baking parchments made from siliconized paper and gloves made up from polyurethane. The results of a cooking test using the above baking parchment indicated the transfer of BTs to foodstuffs. These observations suggest expansion of BT contamination among terrestrial mammals. BT pollution from industrial appliances, such as plastic stabilizers and catalysts other than those of marine origin as antifouling agents, are suggested as alternative sources of exposure. (C) 1999 Elsevier Science Ltd. All rights reserved.
• Uptake Kinetics of Persistent Organochlorines in Mussels through the Transplantation Experiment.

  UENO Daisuke, TAKAHASHI Shin, TANABE Shinsuke, IKEDA Kumiko, KOYAMA Jirou

  JEC Japan Society for Environmental Chemistry 9 (2) 369 - 378 0917-2408 1999 

  The uptake kinetics of PCBs (polychlorinated biphenyls), DDTs (DDT and its metabo lites), CHLs (chlordane and related compounds), HCHs (hexachlorocyclohexane isomers) and HCB (hexachlorobenzene) were examined in blue and green mussels through the transplantation experiment that was conducted in Aburatsubo Bay and Tokyo Bay in a period of 8 weeks from July to October, 1998. Concentration levels of PCBs and DDTs in the transplanted mussels reached those in native mussels and oysters after 2 weeks of transplantation. The compositions of DDT-related compounds and chlordane-related compounds also changed similar to the native ones with the same period. This observation suggests that these blue and green mussels have the ability to respond rapidly to changes in ambient levels of organochlorines. Thus, these species could be considered as good bioindicators for understanding short-term variable pollution. No significant difference was observed for organochlorine concentrations and compositions between blue and green mussels in the overall transplantation experiment, implying that in marine pollution monitoring, it is not always necessary to use single species of mussels as bioindicator.
• Contamination and specific accumulation of organochlorine and butyltin compounds in deep-sea organisms collected from Suruga Bay, Japan

  S Takahashi, JS Lee, S Tanabe, T Kubodera

  SCIENCE OF THE TOTAL ENVIRONMENT 214 (1-3) 49 - 64 0048-9697 1998/06 [Peer-reviewed]
   Scientific journal 

  Organochlorine (OC) and butyltin (BT) residues were detected in deep-sea and shallow water organisms collected from Suruga Bay, Japan. Among OCs, residue levels of polychlorinated biphenyls (PCBs) were highest in deep-sea organisms with up to 2800 ng/g lipid wt. Total butyltin (CBT) concentrations in deep-sea organisms were found to be 980 ng/g wet wt. at maximum levels. Residue levels of OCs in both deep-sea and shallow water organisms from Suruga Bay were lower than those in industrialized areas like Tokyo Bay, whereas residue levels of BTs were comparable or higher. These facts clearly indicate the expansion of BT pollution in deep-sea ecosystems. The deep-sea organisms showed no consistent trend between OC concentrations and prey-predator relationships, while the accumulative pattern of BTs appeared to be influenced by food-chain magnification and feeding habits of the organisms. OC compositions in deep-sea organisms showed a higher ratio of p,p'-DDE, trans-nonachlor and beta-HCH among their related compounds and isomers. Whereas TBT (tributyltin) as a parent compound of BT was predominant in deep-sea organisms, suggesting a fresh input of TBT into the deep-sea environment. (C) 1998 Elsevier Science B.V.
• Butyltin residues in deep sea organisms collected from Surnga Bay, Japan

  S Takahashi, S Tanabe, T Kubodera

  ENVIRONMENTAL SCIENCE & TECHNOLOGY 31 (11) 3103 - 3109 0013-936X 1997/11 [Peer-reviewed]
   Scientific journal 

  Aquatic pollution resulting from extensive usage of organotin compounds has been of great concern due to their deleterious effects in organisms. However, organotin contamination in deep-sea ecosystems has not yet been studied. The present study was attempted to determine butyltin compounds (BTs), including mono- (MBT), di- (DBT), and tributyltin (TBT) in deep-sea organisms collected from Suruga Bay, Japan, in order to elucidate the contamination status and accumulation characteristics. The organisms were collected between 135 and 980 m in the aphotic bathyal zone and compared with those collected from shallow waters. Total butyltin (Sigma BT: MBT + DBT + TBT) concentrations in the tissues of deep-sea fish, crustaceans, cephalopods, echinoderms, and gastropods were up to 980, 460, 460, 130, and 21 ng/g wet wt, respectively. These levels were lower than those in shallow-water organisms from the same bay but comparable to those reported in industrialized areas like Tokyo Bay, suggesting the expansion of BT pollution in deep-sea ecosystems. Deep-sea organisms from Suruga Bay contained much higher levels of BTs than previously reported organochlorine concentrations. BT accumulation appeared to be less lipid dependent. Among BTs, TBT was the predominant compound except in cephalopods, suggesting a fresh input of TBT into the deep-sea environment. To our knowledge, this is the first report on the detection of organotin residues in deep-sea organisms.
• Contamination of deep-sea organisms from Suruga Bay, Japan by organochlorine and butyltin compounds.

  Takahashi, S, Lee, J.s, Tanabe, S, Kubodera, T

  National Science Museum Monographs (12) 319 - 336 1997
• Elevated accumulation of tributyltin and its breakdown products in bottlenose dolphins (Tursiops truncatus) found stranded along the U.S. Atlantic and Gulf Coasts

  K. Kannan, K. Senthilkumar, B. G. Loganathan, S. Takahashi, D. K. Odell, S. Tanabe

  Environmental Science and Technology 31 (1) 296 - 301 0013-936X 1997/01 [Peer-reviewed]
   Scientific journal 

  Butyltin compounds, including mono- (MBT), di- (DBT), and tributyltin (TBT), were determined in the liver, kidney, and muscle of bottlenose dolphins (Tursiops truncatus) found stranded along the southeast U.S. Atlantic and Gulf coasts during 1989-1994. Total butyltin (BTs: MBT + DBT + TBT) concentrations in dolphin liver ranged between 110 and 11 340 ng/g (wet wt) with a mean value of 1400 ng/g. Butyltin concentrations in bottlenose dolphins were higher than those reported from other locations. The liver of a adult male dolphin collected in 1989 had the highest BT concentration (11 340 ng/g wet wt) reported. The concentrations of butyltins increased during the early life stages until maturity, for both sexes, and then tended to remain constant. Analysis of fish muscle collected from the Gulf of Mexico indicated the existence of recent inputs of TBT. The biomagnification factor of BTs in dolphins, on average, was 1.0 with the highest value of 6.8. In addition to polychlorinated biphenyls (PCBs), the presence of noticeable concentrations of TBT and DBT, which are potential immunosuppressing agents, might have also contributed to bottlenose dolphin mortality events in the U.S. Atlantic and Gulf coasts.
• Spatial profile of trace elements in marine sediments from Jakarta Bay, Indonesia.

  Riyadi, A. S, Itai, T, Isobe, T, Ilyas, M, Sudaryanto, A, Setiawan, I. E, Takahashi, S, Tanabe, S

  Interdisciplinary Studies on Environmental Chemistry 6 [Peer-reviewed]
   International conference proceedings

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