[Show abstract][Hide abstract] ABSTRACT: Perchlorate is a widespread environmental contaminant and potent thyroid hormone disrupting compound. Despite this, very little is known with regard to the occurrence of this compound in indoor dust and the exposure of humans to perchlorate through dust ingestion. In this study, 366 indoor dust samples were collected from 12 countries,, during 2010–2014. Dust samples were extracted by 1% (v/v) methylamine in water. Analyte separation was achieved by an ion exchange (AS-21) column and analysis was performed by high performance liquid chro-matography–tandem mass spectrometry (HPLC–MS/MS). The overall concentrations of perchlorate in dust were in the range of 0.02–104 μg/g (geometric mean: 0.41 μg/g). The indoor dust samples from China contained the highest concentrations (geometric mean: 5.38 μg/g). No remarkable differences in perchlorate concentrations in dust were found among various microenvironments (i.e., car, home, office, and laboratory). The estimated median daily intake (EDI) of perchlorate for toddlers through dust ingestion in the USA,.3 ng/kg body weight (bw)/day, respectively. Although high concen-trations of perchlorate were measured in some dust samples, the contribution of dust to total perchlorate intake was b 5% of the total perchlorate intake in humans. This is the first multinational survey on the occurrence of perchlorate in indoor dust.
Environment international 02/2015; 80. DOI:10.1016/j.envint.2014.11.005 · 5.56 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: This paper reported the occurrence and concentrations of macrocyclic-, polycyclic- and nitro musks in cosmetics and household commodities collected from Japan. The high concentrations and detection frequencies of Musk T, habanolide, and exaltolides were found in commercial products, suggesting their large amounts of production and usage in Japan. Polycyclic musks, HHCB and OTNE, also showed high concentrations in cosmetics and products. The estimated dairy intakes of Musk T and HHCB by the dermal exposure to commercial products were 7.8 and 7.9 mu g/kg/day in human, respectively, and perfume and body lotion are dominant exposure sources. We also analyzed synthetic musks in house dusts. Polycyclic musks, HHCB and OTNE, showed high concentrations in samples, but macrocyclic musks were detected only in a few samples, although these types of musks were highly detected in commercial products. This is probably due to easy-degradation of macrocyclic musks in indoor environment. The dairy intakes of HHCB by dust ingestions were 0.22 ng/kg/day in human, which were approximately five orders of magnitudes lower than those of dermal absorption from commercial household commodities.
[Show abstract][Hide abstract] ABSTRACT: Polycyclic aromatic hydrocarbons (PAHs) were analyzed in oysters collected from 18 stations in the Yatsushiro Sea, western Japan. PAHs were detected in all samples analyzed, and the highest concentration (mean 230ng/g wet weight) was found in oysters from Tanoura Bay. The high molecular weight PAHs to low molecular weight PAHs ratios in oysters from Tanoura Bay were higher than at other stations. Sediment samples collected from 42 stations in Tanoura Bay were analyzed for PAHs to understand their concentrations and distribution. Higher concentrations were found in sediment samples at two stations in the southern inner bay (mean 30,200ng/g dry weight), which were approximately two orders of magnitude higher than at a reference site. These observations strongly suggest severe contamination and significant sources of PAHs in Tanoura Bay. Dioxins and dioxin-like compounds (PCDFs, and non- and mono-ortho coplanar PCBs) were analyzed in sediments from eight stations in Tanoura Bay. The concentrations were comparable to, or lower than, at the reference sites, suggesting that there are no specific sources of these compounds in this bay. PAH, dioxins and dioxin-like compounds DR-CALUX relative potencies (REP) were applied to the sediment concentrations to evaluate the potential for toxicological effects on benthic organisms. PAHs made the highest contribution to the total REP concentration, supplying 99% of the total REP, followed by PCDDs (0.18%), PCDFs (0.04%), and PCBs (<0.001%). In this area, PAHs appear to be the most important Ah receptor binding chemicals for potential toxicity to benthic species.
[Show abstract][Hide abstract] ABSTRACT: Organic corrosion inhibitors (OCIs), including ultraviolet light filters, are widely used in plastics, rubbers, colorants, and coatings to increase the performance of products. Derivatives of benzotriazole (BTR), benzothiazole (BTH), and benzophenone (BP) are high-production volume OCIs that have been detected in the environment and human tissues. However, knowledge of their occurrence in indoor environments, as well as human exposure to them, is still lacking. In this study, BTR, BTH, BP and their 12 derivatives were observed in indoor dust for the first time. All three groups of OCIs were found in all 158 indoor dust samples from the U.S. and three East Asian countries (China, Japan, and Korea). The geometric mean (GM) concentration of the sum of six BTRs (GM CΣBTRs) ranged from 20 to 90 ng/g among the four countries studied, with a maximum CΣBTRs of ~2000 ng/g found in a dust sample from China. Tolyltriazole was the major derivative of BTR measured in dust. GM CΣBTHs in indoor dust from the four countries ranged from 600 to 2000 ng/g. 2-OH-BTH was the predominant BTH in dust from the U.S., Japan, and Korea. GM CΣBPs in dust ranged from 80 to 600 ng/g, with 2-OH-4-MeO-BP and 2,4-2OH-BP, contributing to the majority of BP concentrations. Based on the concentrations of three types of OCIs in indoor dust, human exposure through dust ingestion was calculated. Daily intake of OCIs through dust ingestion was higher for people in the U.S., Japan, and Korea than in China; the residents in urban China are exposed to higher levels of OCIs via dust ingestion than are those in rural China.
[Show abstract][Hide abstract] ABSTRACT: Concentrations of 12 hydroxylated polycyclic aromatic hydrocarbons (OH-PAHs) were determined in 306 urine samples collected from seven Asian countries (China, India, Japan, Korea, Kuwait, Malaysia, and Vietnam) by high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS). The total concentrations of OH-PAHs found in the seven Asian countries were in the following increasing order: Malaysia (median: 2260 pg/mL) < Japan (4030 pg/mL) < China (5770 pg/mL) < India (6750 pg/mL) < Vietnam (8560 pg/mL) < Korea (9340 pg/mL) < Kuwait (10 170 pg/mL). The measured urinary concentrations of 1-hydroxypyrene (1-PYR) in samples from Malaysia, Korea, and Japan (∼ 100 pg/mL) were similar to those reported for North America and Western Europe. The concentrations of 1-PYR in urine samples from China, India, and Vietnam were 4-10 times higher than those reported for other countries, thus far. Among the 12 OH-PAH compounds analyzed, hydroxynaphthalene (NAP: sum of 1-hydroxynaphthalene and 2-hydroxynaphthalene) was the dominant compound (accounting for 60-90% of total OH-PAHs), followed by hydroxyphenanthrene (PHEN: sum of 2-hydroxyphenanthrene, 3-hydroxyphenanthrene, 4-hydroxyphenanthrene, and 9-hydroxyphenanthrene [3-16%]), 2-hydroxyfluorene (3-20%), and 1-PYR (2-8%). The total daily intakes (DIs) of PAHs were estimated based on the urinary concentrations of their metabolites. The DIs of naphthalene were found to be higher for populations in Korea, Kuwait, and Vietnam (> 10 μg/day) than those of the other countries studied (∼ 5 μg/day). The DIs of phenanthrene and pyrene (> 10 μg/day) in the populations of China, India, and Vietnam were higher than those estimated for the populations in the other countries studied (∼ 5 μg/day).
[Show abstract][Hide abstract] ABSTRACT: During early 2000, a new analytical procedure for nitrate isotopic measurement, termed the "denitrifier method", was established. With the development of the nitrate isotope tracer method, much research has been reported detailing sources of groundwater nitrate and denitrification mechanisms. However, a shortcoming of these tracer studies has been indicated owing to some overlapping of isotope compositions among different source materials and denitrification trends. In order to reduce these uncertainties, we examined nitrate isotope ratios within a frame of "regional groundwater flow dynamics" to eliminate unnecessary uncertainties in elucidating nitrate sources and behaviors. A total of 361 samples were collected from the Kumamoto area: the circulated groundwater system with a scale of 10(3) km(2) in southern Japan. Subsequently, the nitrate pollution was examined within the above-mentioned framework. As a result, a reasonable identification of the sources and attenuation behaviors (both denitrification and dilution) of groundwater nitrate pollution was obtained over the study area. This study demonstrates that the use of nitrate isotope tracers efficiently improves with a comprehensive understanding of groundwater flow dynamics. The approach emphasized in this study is important and should be applicable in other areas.
Water Research 02/2013; 47(8). DOI:10.1016/j.watres.2013.02.020 · 5.53 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: p-Hydroxybenzoic acid esters (parabens) and bisphenol A diglycidyl ether (BADGE) are widely present in personal care products, food packages, and material coatings. Nevertheless, little is known about the occurrence of these compounds in indoor dust. In this study, we collected 158 indoor dust samples from the U.S., China, Korea, and Japan and determined the concentrations of 11 target chemicals, viz., six parabens and their common hydrolysis product, 4-hydroxybenzoic acid (4-HB), as well as BADGE and its three hydrolysis products (BADGE·H(2)O, BADGE·2H(2)O, and BADGE·HCl·H(2)O). All of the target compounds were found in dust samples from four countries. Concentrations of sum of six parabens in dust were on the order of several hundred to several thousands of nanogram per gram. Geometric mean concentrations of BADGEs in dust ranged from 1300 to 2890 ng/g among four countries. Methyl paraben (MeP), propyl paraben (PrP), BADGE·2H(2)O, and BADGE·HCl·H(2)O were the predominant compounds found in dust samples. This is the first report of BADGE and its hydrolysis products (BADGEs) in indoor dust samples and of parabens in indoor dust from Asian countries. On the basis of the measured concentrations of target chemicals, we estimated the daily intake (EDI) via dust ingestion. The EDIs of parabens via dust ingestion were 5-10 times higher in children than in adults. Among the four countries studied, the EDIs of parabens (5.4 ng/kg-bw/day) and BADGEs (6.5 ng/kg-bw/day) through dust ingestion were the highest for children in Korea and Japan.
[Show abstract][Hide abstract] ABSTRACT: We analyzed 68 green and blue mussels collected from Cambodia, China, Hong Kong, India, Indonesia, Japan, Korea, Malaysia, Philippines, Vietnam and the USA during 2003 and 2007, to elucidate the occurrence and widespread distributions of emerging pollutants, synthetic musks and benzotriazole UV stabilizers (BUVSs) in Asia-Pacific coastal waters. Synthetic musks and BUVSs were detected in mussels from all countries, suggesting their ubiquitous contamination and widespread distribution. High concentrations of musks and BUVSs were detected in mussels from Japan and Korea, where the levels were comparable or greater than those of PCBs, DDTs and PBDEs. Significant correlations were found between the concentrations of HHCB and AHTN, and also between the concentrations of UV-327 and UV-328, which suggest similar sources and compositions of these compounds in commercial and industrial products. To our knowledge, this is the first study of large-scale monitoring of synthetic musks and BUVSs in Asia-Pacific coastal waters.
[Show abstract][Hide abstract] ABSTRACT: Bisphenol A has been reported to be a ubiquitous contaminant in indoor dust, and human exposure to this compound is well documented. Information on the occurrence of and human exposure to other bisphenol analogues is limited. In this study, eight bisphenol analogues, namely 2,2-bis(4-hydroxyphenyl)propane (BPA), 4,4'-(hexafluoroisopropylidene)diphenol (BPAF), 4,4'-(1-phenylethylidene)bisphenol (BPAP), 2,2-bis(4-hydroxyphenyl)butane (BPB), 4,4'-dihydroxydiphenylmethane (BPF), 4,4'-(1,4-phenylenediisopropylidene)bisphenol (BPP), 4,4'- sulfonyldiphenol (BPS), and 4,4'-cyclohexylidenebisphenol (BPZ), were determined in indoor dust samples (n = 156) collected from the United States (U.S.), China, Japan, and Korea. Samples were extracted by solid-liquid extraction, purified by automated solid phase extraction methods, and determined by liquid chromatography-tandem mass spectrometry (LC-MS/MS). The total concentrations of bisphenols (∑BPs; sum of eight bisphenols) in dust were in the range of 0.026-111 μg/g (geometric mean: 2.29 μg/g). BPA, BPS, and BPF were the three major bisphenols, accounting for >98% of the total concentrations. Other bisphenol analogues were rare or not detected, with the exception of BPAF, which was found in 76% of the 41 samples collected in Korea (geometric mean: 0.0039 μg/g). The indoor dust samples from Korea contained the highest concentrations of both individual and total bisphenols. BPA concentrations in dust were compared among three microenvironments (house, office, and laboratory). The estimated median daily intake (EDI) of ∑BPs through dust ingestion in the U.S., China, Japan, and Korea was 12.6, 4.61, 15.8, and 18.6 ng/kg body weight (bw)/day, respectively, for toddlers and 1.72, 0.78, 2.65, and 3.13 ng/kg bw/day, respectively, for adults. This is the first report on the occurrence of bisphenols, other than BPA, in indoor dust.
[Show abstract][Hide abstract] ABSTRACT: As concern regarding the toxic effects of bisphenol A (BPA) grows, BPA in many consumer products is gradually being replaced with compounds such as bisphenol S (BPS). Nevertheless, data on the occurrence of BPS in human specimens are limited. In this study, 315 urine samples, collected from the general populations in the United States, China, India, Japan, Korea, Kuwait, Malaysia, and Vietnam, were analyzed for the presence of total BPS (free plus conjugated) concentrations by high-performance liquid chromatography tandem mass spectrometry (HPLC-MS/MS). BPS was detected in 81% of the urine samples analyzed at concentrations ranging from below the limit of quantitation (LOQ; 0.02 ng/mL) to 21 ng/mL (geometric mean: 0.168 ng/mL). The urinary BPS concentration varied among countries, and the highest geometric mean concentration [1.18 ng/mLor 0.933 μg/g creatinine (Cre)] of BPS was found in urine samples from Japan, followed by the United States (0.299 ng/mL, 0.304 μg/g Cre), China (0.226 ng/mL, 0.223 μg/g Cre), Kuwait (0.172 ng/mL, 0.126 μg/g Cre), and Vietnam (0.160 ng/mL, 0.148 μg/g Cre). Median concentrations of BPS in urine samples from the Asian countries were 1 order of magnitude lower than the median concentrations reported earlier for BPA in the same set of samples, with the exception of samples from Japan. There were no significant differences in BPS concentrations between genders (male versus female), or among age groups (categorized as ≤ 19, 20-29, 30-39, 40-49, and ≥ 50 years), or races (Caucasian versus Asian). The daily intake (EDI) of BPS was estimated on the basis of urinary concentrations using a simple pharmacokinetic approach. The median EDI values of BPS in Japan, China, United States, Kuwait, Vietnam, Malaysia, India, and Korea were 1.67, 0.339, 0.316, 0.292, 0.217, 0.122, 0.084, and 0.023 μg/person, respectively. This is the first study to report the occurrence of BPS in human urine.
[Show abstract][Hide abstract] ABSTRACT: Bisphenol A (BPA) is an industrial chemical used in the manufacture of polycarbonate plastics and epoxy resins. Due to the potential of this compound to disrupt normal endocrinal functions, concerns over human exposure to BPA have been raised. Although several studies have reported human exposure to BPA in Western nations, little is known about exposure in Asian countries. In this study, we determined total urinary BPA concentrations (free plus conjugated) in 296 urine samples (male/female: 153/143) collected from the general population in seven Asian countries, China, India, Japan, Korea, Kuwait, Malaysia, and Vietnam, using high-performance liquid chromatography (HPLC) tandem mass spectrometry (MS/MS). On the basis of urinary BPA concentrations, we estimated the total daily intake. The results indicated that BPA was detected in 94.3% of the samples analyzed, at concentrations ranging from <0.1 to 30.1 ng/mL. The geometric mean concentration of BPA for the entire sample set from seven countries was 1.20 ng/mL. The highest concentration of BPA was found in samples from Kuwait (median: 3.05 ng/mL, 2.45 μg/g creatinine), followed by Korea (2.17 ng/mL, 2.40 μg/g), India (1.71 ng/mL, 2.09 μg/g), Vietnam (1.18 ng/mL, 1.15 μg/g), China (1.10 ng/mL, 1.38 μg/g), Malaysia (1.06 ng/mL, 2.31 μg/g), and Japan (0.95 ng/mL, 0.58 μg/g). Among the five age groups studied (≤ 19, 20-29, 30-39, 40-49, and ≥ 50 years), the highest median concentration of BPA was found in urine samples from the age group of ≤ 19 years. There was no significant difference in BPA concentrations between genders (male and female) or domicile of residence (rural and urban). The estimated median daily intakes of BPA for the populations in Kuwait, Korea, India, China, Vietnam, Malaysia, and Japan were 5.19, 3.69, 2.90, 2.13, 2.01, 1.80, and 1.61 μg/day, respectively. The estimated daily intake of BPA in the seven Asian countries was significantly lower than the tolerable daily intake recommended by the U.S. Environmental Protection Agency. This is the first study to document the occurrence of and human exposure to BPA in several Asian countries.
[Show abstract][Hide abstract] ABSTRACT: The occurrence of 14 phthalate metabolites was found in human urine samples collected from seven Asian countries: China, India, Japan, Korea, Kuwait, Malaysia, and Vietnam. Phthalate metabolites were found in all samples, indicating widespread exposure of humans to phthalates in these Asian countries. The highest total (the sum of 14 phthalates) phthalate metabolite concentrations were found in samples collected from Kuwait (median: 1050 ng/mL), followed in decreasing order by samples from India (389 ng/mL), China (234 ng/mL), Vietnam (133 ng/mL), Japan (120 ng/mL), Korea (117 ng/mL), and Malaysia (94.9 ng/mL). The creatinine-adjusted median concentrations of total phthalates for urine samples from Kuwait, India, China, Vietnam, Japan, Korea, and Malaysia were 692, 506, 289, 119, 103, 104, and 169 μg/g creatinine, respectively. Monomethyl phthalate (mMP), monoethyl phthalate (mEP), mono (2-isobutyl phthalate) (miBP), mono-n-butyl phthalate (mBP), and metabolites of di-(2-ethylhexyl) phthalate (DEHP) were the dominant compounds, collectively accounting for >95% of the total concentrations in the samples from the seven countries. The profiles of urinary phthalate metabolite concentrations varied among the samples collected from the seven countries. Urine samples from Kuwait contained the highest concentrations of mEP (median: 391 ng/mL), mBP (94.1 ng/mL), and the metabolites of DEHP (202 ng/mL), whereas samples from China and Japan contained the highest concentrations of miBP (50.8 ng/mL) and mMP (17.5 ng/mL), respectively. mEP was the predominant metabolite in urine samples from India and Kuwait (accounting for 49% of the total), mBP and miBP were the predominant compounds in samples from China (52%), and DEHP metabolites were the predominant compounds in samples from Korea (46%) and Vietnam (52%). Based on the urinary concentrations of mEP, mBP, miBP, and DEHP metabolites of the samples from the seven Asian countries, we estimated daily intake rates of diethyl phthalate (DEP), dibutyl phthalate (DBP), and DEHP. The results indicated that people in the seven Asian countries are exposed to DEP, DBP, and DEHP at levels well below the reference doses (RfD) suggested as unsafe by the U.S. Environmental Protection Agency (EPA). The estimated exposure doses to DEHP in Kuwait, however, were above the RfD recommended by the EPA.
[Show abstract][Hide abstract] ABSTRACT: Benzotriazole UV stabilizers (BUVSs), such as UV-328 and UV-327, were identified in the blubbers of finless porpoises (Neophocaena phocaenoides) collected from the Ariake Sea, western Japan, by gas chromatography-high resolution mass spectrometry (GC-HRMS). The mean concentrations and standard deviations of UV-328 and UV-327 in five blubber samples were 38 ± 28 ng g(-1) (lipid wt) and 19 ± 19 ng g(-1), respectively. The bioconcentration factor (BCF) of UV-327 between water and finless porpoises was estimated to be 33 300, which is approximately one order of magnitude higher than that found for small fish inhabiting the same regions. The BCF of UV-327 in finless porpoises was similar to that of persistent organochlorine pesticide, hexachlorocyclohexane (HCH: 37 000) in marine mammals from the western North Pacific Ocean. These results suggest that BUVSs appear to be persistent and bioaccumulative in the aquatic food chain. Further investigations on temporal trends, and regional and global monitoring of BUVSs are needed to understand their environmental profiles and potential risks to wildlife and human.
[Show abstract][Hide abstract] ABSTRACT: In order to elucidate the spatial distribution of brominated flame retardants (BFRs) in the Japanese coastal environment, hexabromocyclododecanes (HBCDs), polybrominated diphenyl ethers (PBDEs) and organochlorines (OCs: PCBs, DDTs, CHLs, HCHs, HCB) were determined in bivalves (oysters and mussels) collected from Japanese coastal waters. HBCDs and PBDEs were detected in all samples analyzed. Concentration ranges of HBCDs were 12-5200 ng g(-1) lipid wt., followed by PCBs (20-3100 ng g(-1))>PBDEs (3.1-86 ng g(-1) lipid wt.). The highest concentration of HBCDs was found in the Osaka region. This result indicates that HBCDs are ubiquitous and predominant compounds in bivalves from the Japanese coastal waters. Since no species differences between oysters and mussels were observed for the bioaccumulation properties of HBCDs and PBDEs, oysters could be utilized for BFR contamination monitoring worldwide as an alternative to mussels. Global comparisons between oysters and mussels showed that HBCD concentrations in Japan are among the highest levels reported from Asia and Europe. Estimated dietary exposures of HBCDs and PBDEs through seafood were 0.45-34 ng kg body weight(-1)d(-1), and 0.054-6.8 ng kg body weight(-1)d(-1), respectively. These exposure levels were more than 1000 times lower than the lowest observable effects or no observable adverse effects levels for HBCDs and PBDEs, respectively.
[Show abstract][Hide abstract] ABSTRACT: Benzotriazole UV stabilizers (BUVSs) and polycyclic musks were analyzed in influent, effluent, and sewage sludge samples collected from five wastewater treatment plants (WWTPs) in Japan. BUVSs were detected in most samples analyzed, and UV-326 was the dominant compound in influents (mean: 46 ng/L), followed by UV-328 (34 ng/L). UV-327 was detected in two influents, and UV-320 did not identify in any samples. These results imply a large amount of production and usage of UV-326 compared with other BUVSs in Japan. The high concentrations of polycyclic musks were determined in influents, at mean levels of 1,100 ng/L for HHCB and 450 ng/L for AHTN. The concentrations of BUVSs in the effluents were generally low (<5 ng/L), suggesting an elimination of these compounds during wastewater treatment processes. The removal rates of UV-326 and UV-328 were more than 90% in the effluents, but high concentrations of BUVSs were detected in sewage sludge samples of WWTPs, at the levels of 1,100, 170, and 510 ng/g (dry wt.) for UV-326, UV-327, and UV-328, respectively. This indicates an adsorption of BUVSs with organic carbon in sewage sludge. The mean concentrations of HHCB and AHTN in sludge samples were 21,000 and 7,700 ng/g (dry wt.), which are one to two orders of magnitude higher than those of BUVSs. This study implies that WWTP may be a potential source of BUVSs and polycyclic musks into the aquatic ecosystems. Investigations on mass balance and inventory analysis are needed in order to understand the source and pathway of these compounds in the environment.
[Show abstract][Hide abstract] ABSTRACT: The benzotriazole UV stabilizers, which are used in a variety of plastic products, were analyzed in marine organisms and sediments collected from the Ariake Sea, Japan. The UV stabilizers, such as UV-320, UV-326, UV-327, and UV-328 were detected in all of the samples analyzed, suggesting the production and use of these compounds in Japan. High concentrations of UV stabilizers were found in clams, oysters, and gastropods collected from the tidal flat at concentrations on the order of several hundreds of ng/g on a lipid weight (wt.) basis. The higher trophic species, such as hammerhead sharks and coastal birds, accumulated UV stabilizers, with mean concentrations of 190 ng/g and 74 ng/g (lipid wt.), respectively. These results indicate that benzotriazole UV stabilizers are persistent and bioaccumulative in the marine food-chains. The benzotriazole UV stabilizers were also detected in coastal and river sediments around the Ariake Sea, at concentrations in the range of 7.9-720 ng/g (dry weight basis). Significant correlations were found between concentrations of UV stabilizers and organic carbon content in sediments, implying adsorption of these compounds to organic matter. To our knowledge, this is the first report of ubiquitous contamination and bioaccumulation of benzotriazole UV stabilizers in the marine environment.