Organophosphate flame retardants (OPFRs) have been widely used as flame retardants and plasticizers in commercial products. Limited data are available on the occurrence and exposure of OPFRs via ...drinking water consumption. In this study, 127 drinking water samples were collected from tap water, purified water (tap water that is passed through in-house filters) and bottled water from major cities in Korea in 2014. The total concentrations of OPFRs (ΣOPFR) in all of the samples ranged from below the method detection limit (MDL) to 1660 (median: 48.7) ng/L. The predominant OPFR compounds in drinking water were tris(2-chloroethyl) phosphate (TCEP), tris(2-chloroethyl) phosphate (TCPP), and tris(2-butoxyethyl) phosphate (TBEP). Significant differences were observed in the levels of TCPP, TBEP and ΣOPFR among various types of drinking water. TCPP is introduced in the drinking water during the water purification process. Regional differences existed in the levels and patterns of OPFRs in water samples, which indicated the existence of diverse sources of these contaminants. Purified water was a significant contributor to the total OPFR intake by humans. The estimated daily intake of OPFRs was lower than the tentative oral reference dose (RfD) values. In comparison with exposure of OPFRs via dust ingestion, water consumption was a significant source of chlorinated PFRs (99% for TCEP and 34% for TCPP to the total intakes) for Koreans.
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•Several OPFRs were detected in various types of drinking water from Korea.•The highest concentrations of OPFRs were found in tap water from industrialized cities.•Diverse contamination patterns of OPFRs were observed in tap water.•Water purifiers are a source of TCPP in purified water.•Water consumption is a significant source of chlorinated PFRs for Koreans.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Domestic and global regulations on phthalates have led to the introduction of non-phthalate plasticizers (NPPs) in industrial markets as alternative plasticizers. In this study, phthalates and NPPs ...from surface and core sediment samples taken from industrialized bays in Korea were measured to determine their distribution, contamination sources, historical records, and the ecological risks they posed. Phthalates and alternative plasticizers were detected in all surface samples and sediment cores, indicating ubiquitous contamination. Predominant phthalates were di(2-ethylhexyl)phthalate (DEHP), diisononyl phthalate (DiNP), and diisodecyl phthalate (DiDP) and di(2-ethylhexyl)terephthalate (DEHT) and tris(2-ethylhexyl)trimellitate (TOTM) were the most common NPPs. The total concentrations of phthalates and NPPs ranged from 76.3 to 59,400 ng/g dry weight and <0.02 to 35,300 ng/g dry weight, respectively. The highest concentrations of phthalates and NPPs were observed in sediment from rivers, streams, and inner parts of bays, with the levels decreasing gradually toward the outer parts of the bays. Our findings suggest that proximity to industrial complexes is crucial for sedimentary distribution for plasticizers. Historical records in a sediment core show clearly increasing trends in phthalate and NPP levels from the 1970s to the 2010s, consistent with their production history. In particular, TOTM has rapidly increased over the last decade, presenting an emerging concern of contaminant in the coastal environment. Industrialization and population growth were suggested as major factors affecting plasticizer contamination. Almost all sediment (>95%) exceeded quality guidelines for DEHP, implying a potential risk for benthic organisms. This is the first report on historical trends of phthalates and alternative plasticizers.
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•TOTM and DEHT were the dominant alternative plasticizers in the sedimentary environment.•Proximity to industrial complexes was crucial for sedimentary distribution of plasticizers.•Clear increasing trends in phthalates and alternative plasticizers were observed over time.•Industrialization and population were major factors affecting plasticizer contamination.•Sedimentary DEHP levels may pose adverse health effects for benthic organisms.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Contamination by organophosphate flame retardants (OPFRs) is an emerging concern in aquatic environments. Concentrations of 18 OPFRs were measured in water and sediments collected from the artificial ...Lake Shihwa. OPFR concentrations in sediments measured in this study were the highest reported worldwide, implying severe OPFR contamination. The highest concentrations of OPFRs were found in creeks taken near industrial complexes, and OPFR concentrations decreased with increasing distance from creeks to inshore or offshore lake waters. On-going OPFR contamination by wastewater treatment plant (WWTP) discharge was evidenced by the clear decrease in OPFRs in water samples collected moving away from WWTP outfall. TBEP and TEP were dominant in water samples, while TDCPP and TCPP were dominant in sediment samples. Differences in contamination profiles with sample matrices are likely due to hydrophobicity of individual OPFRs. Non-parametric multidimensional scaling ordination showed that OPFR contamination was affected by pollution inflow and proximity to industrial complexes.
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•Eighteen OPFRs were measured in water and sediments from industrialized coastal waters.•Concentrations of several OPFRs in creek sediments were the highest reported worldwide.•Clear decrease in OPFRs was found in water collected moving away from WWTP outfall.•TBEP and TEP were dominant in water, while TDCPP and TCPP were dominant in sediments.•Severe OPFR contamination was influenced by inflow of pollution and proximity of industrial complexes.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Siloxanes have been commonly used as additives in a variety of industrial and consumer products. Media and government investigations have revealed that defoamers containing siloxanes are used in the ...effluent of thermal power plants in Korea. However, investigations of the source impact of siloxane contamination from the discharge of thermal power plants into coastal environments are scarce. In this study, sediment and invertebrates were collected around a thermal power plant to assess source impact, seasonal variation, and a potential for bioaccumulation. Although siloxanes were detectable in sediment and invertebrates, the spatial distribution and composition (which differed between the siloxanes found in sediment and invertebrates and those in defoamer used in the plant) suggest they were likely transported by long-distance migration as well as the discharge of thermal power plant. Seasonal differences might affect sedimentary contamination and the bioaccumulation potential of siloxanes. Specifically, octamethylcyclotetrasiloxane (D4) may have limited adsorption capacity and potential for long-distance migration, as its contribution in sediment far from the coastline was greater than that of decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6). However, higher D5 accumulation in invertebrates, and D5 has a potential bioaccumulation. A molecular docking analysis showed that the binding affinity between D5 and the cytochrome enzyme in invertebrates was weaker than that with other siloxanes, which could lead to higher D5 accumulation in invertebrates.
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•Siloxanes were detected in sediment and invertebrates collected around a thermal power plant.•Discharge from the power plant was not the main contributor to siloxane contamination.•Seasonal differences in siloxanes were observed in sediment and invertebrates.•Some siloxanes had the potential for bioaccumulation in benthic invertebrates.•Weak binding between D5 and the cytochrome of invertebrates led to higher bioaccumulation.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Novel halogenated flame retardants (HFRs) were introduced to industrial markets as alternatives to legacy brominated FRs (BFRs), such as polybrominated diphenyl ethers (PBDEs). In the present study, ...PBDEs and their brominated and chlorinated alternatives, novel BFRs (NBFRs) and dechlorane plus (DP), were measured in multiple environmental matrices in a highly industrialized lake in Korea. Legacy and novel HFRs were detected in multiple samples, indicating ubiquitous contamination. Concentrations of HFRs in water and sediment observed in creeks running through machine, textiles, and automobile industrial complexes were significantly higher than those observed in inside and outside of the lake. Higher bioaccumulation levels of HFRs were observed in inshore compared with offshore waters. Results suggest that multi-matrix distribution of legacy and novel HFRs was dependent on the geographical proximity to industrial sources. Compared with previous studies, the highest levels of PBDEs and NBFRs were recorded in water samples on a global scale, implying on-going emissions from industrial activities. Decabromodiphenyl ethane (DBDPE) was a dominant compound in water samples, whereas the concentrations of PBDEs, NBFRs, and DP in sediment were similar to each other. This suggests a shift in consumption from legacy to novel HFRs, preferentially in water environments. A significant declining trend in PBDEs was observed in water and sediment collected between 2008 and 2015, indicating the effectiveness of regulatory actions. Based on their environmental occurrence and bioaccumulation potential, pentabromoethylbenzene and bis(2-ethylhexyl) tetrabromophthalate may pose emerging concerns regarding contamination of aquatic environments.
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•Severe contamination by novel BFRs was observed in creeks running through industrial complexes.•Predominant HFRs in water samples was DBDPE, an alternative of deca-BDE.•Proximity to industrial complexes is crucial for multi-matrix distribution of HFRs.•A significant declining trend in PBDEs indicated the effectiveness of regulatory actions.•PBEB and BEHTBP were suggested as environmental contaminants of emerging concerns.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Human exposure to flame retardants (FRs) in indoor environments is a growing concern. In this study, the concentrations of polybrominated diphenyl ethers (PBDEs) and their alternatives, such as novel ...brominated flame retardants (NBFRs), dechlorane plus (DP), and organophosphate flame retardants (OPFRs), were measured in dust from indoor environments in Korea to investigate their occurrence, contamination profiles, and health risks. Legacy and emerging FRs were detected in dust samples, indicating widespread contamination of indoor environments. The concentrations of alternative FRs were higher in dust from offices compared with house dust, suggesting that office environments are major consumers of alternative FRs. Similar compositional profiles for indoor dust were found for PBDEs in different microenvironments and regions, while OPFR composition varied widely due to disparate applications. The estimated daily intakes of PBDEs, NBFRs, and OPFRs via dust ingestion were lower than the reference doses proposed by previous studies. A multiple-exposure assessment showed that dust ingestion was a major contributor to total PBDEs for toddlers and adults. However, major exposure pathways of BDEs 47 and 209 differed between toddlers and adults. Our study suggests that multiple exposure pathways should be considered in a comprehensive exposure assessment of PBDEs.
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•PBDEs and their alternatives were ubiquitously contaminated in different microenvironments.•Concentrations of alternative flame retardants were higher in offices than in houses.•Compositions of OPFRs in indoor dust varied depending on microenvironment.•Dust ingestion was a major contributor to PBDE exposure through multiple pathways.•Major exposure pathways of BDEs 47 and 209 were different for toddlers and adults.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
•TDCPP and TPP exposure significant reduced reproductive parameters in zebrafish.•TDCPP and TPP increased plasma E2 and VTG levels in both male and female fish.•Gene transcriptions of HPG axis ...corresponded well with hormonal/reproduction changes.
Tris(1,3-dichloro-2-propyl) phosphate (TDCPP) and triphenyl phosphate (TPP) belong to the group of triester organophosphate flame retardants (OPFRs), which have been used in a wide range of consumer products. These chemicals have been frequently detected in effluents, surface water, and fish, and hence their potential adverse effects on aquatic ecosystem are of concern. The present study was conducted to investigate the reproduction-related effects and possible molecular mechanisms of TDCPP and TPP using a 21 day reproduction test employing adult zebrafish (Danio rerio). After 21 d of exposure to TDCPP or TPP, significant decrease in fecundity along with significant increases of plasma 17β-estradiol (E2) concentrations, vitellogenin (VTG) levels, and E2/testosterone (T) and E2/11-ketotestosterone (11-KT) ratios were observed. The transcriptional profiles of several genes of the hypothalamus–pituitary–gonad (HPG) axis changed as well after the exposure, but the trend was sex-dependent. In male fish, gonadotropin-releasing hormone2 (GnRH2), GnRHR3, cytochrome P450 (CYP) 19B, estrogen receptor α (ERα), ER2 β1, and follicle stimulating hormone β (FSHβ) were upregulated in the brain, while luteinizing hormone β (LHβ) and androgen receptor (AR) were downregulated. Corresponding to the upregulation of FSHβ and downregulation of LHβ in the brain, FSHR was upregulated and LHR was downregulated in the testis. Among the genes that regulate the steroidogenesis pathway, transcription of hydroxyl methyl glutaryl CoA reductase (HMGRA), steroidogenic acute regulatory protein (StAR), and 17β-hydroxysteroid dehydrogenase (17βHSD) decreased, while transcription of CYP11A, CYP17, and CYP19A increased. In female fish, transcription ofGnRH2 and GnRHR3 decreased, but FSHβ, LHβ, CYP19B, ERα, ER2β1, and AR transcription increased in the brain. In the ovary, FSHR and LHR were significantly upregulated, and most steroidogenic genes were significantly upregulated. The observed disruption of GnRH and GtHs could be further related to subsequent disruption in both sex steroid hormone balance and plasma VTG levels, as well as reproductive performance. Overall, our observation indicates that both TDCPP and TPP could disturb the sex hormone balance by altering regulatory mechanisms of the HPG axis, eventually leading to disruption of reproductive performance in fish.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Environmental contamination by organophosphate flame retardants (OPFRs) and plasticizers are environmental concerns. In this study, 18 OPFRs were analyzed in sediment and bivalves collected from 50 ...locations along the Korean coast to assess occurrence, geographical distribution, contamination source, and bioaccumulation potential. Tris(1-chloro-2-propanyl) phosphate (TCPP) and tris(2-ethylhexyl) phosphate (TEHP) were highly detected (>80%) OPFRs in sediment and bivalves. Total concentrations of OPFRs and plasticizers in sediment and bivalves ranged from 2.18 to 347 ng/g dry weight and from 6.12 to 206 ng/g dry weight, respectively, which were within the ranges reported for previous studies. Sedimentary organic carbon was a primary factor governing the OPFR distribution. Concentrations of OPFRs and plasticizers in sediments from harbor zones were significantly higher than non-harbor zones, indicating that shipping activity is a contamination source of OPFRs and plasticizers in coastal environments. Biota-sediment accumulation factors <1 for several OPFRs indicated limited potential for bioaccumulation.
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•OPFRs and plasticizers were detected in all sediment and bivalves along the Korean coast.•TCPP was a major OPFR and plasticizer compound in sediment and bivalves.•Shipping activity is a significant OPFR contamination source in coastal environments.•Biota-sediment accumulation factors of OPFRs indicate a limited bioaccumulation potential.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
A total of 20 organophosphate triesters (OPEs), including seven alkyl-OPEs, three chlorinated (Cl)-OPEs, seven aryl-OPEs, and three oligomeric-OPEs were measured in 341 house dust samples collected ...from 12 countries during the period 2010–2014. OPEs were ubiquitous in indoor dust, and the total concentrations of OPEs (∑OPEs; sum of 20 OPEs) ranged from 49.4 to 249,000 ng/g dry weight (dw). Generally, Cl-OPEs were the predominant compounds (51% of total) in indoor dust samples, with a median concentration of 800 ng/g, followed by alkyl-OPEs (31%), aryl-OPEs (17%), and oligomeric-OPEs (1%), with median concentrations of 480, 270, and 21.9 ng/g, respectively. ∑OPE concentrations in indoor dust from more industrialized countries (South Korea: median, 31,300; Japan: 29,800; and the United States: 26,500 ng/g dw) were one or two orders of magnitude higher than those from less industrialized countries (Greece: 7140, Saudi Arabia: 5310, Kuwait: 4420, Romania: 4110, Vietnam: 1190, China: 1120, Colombia: 374, India: 276, and Pakistan: 138 ng/g dw). Statistically significant positive correlations (0.114 < r < 0.748, p < 0.05) were found among the concentrations of 16 OPEs in dust samples, indicating similar sources of these compounds. The median estimated daily intakes of ΣOPEs via dust ingestion for children and adults were in the ranges of 0.29–64.8 and 0.07–14.9 ng/kg bw/day, respectively.
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•OPEs are ubiquitous in house dust samples collected from 12 countries.•Cl-OPEs were the predominant compounds in indoor dust samples.•∑OPEs in dust from industrialized countries were higher than those from less industrialized countries.•Indoor dust ingestion is an important route of human exposure to OPEs.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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