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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 and0.02 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.

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.

Phthalates are anti-androgenic chemicals and may cause long-lasting adverse effects on growing fetuses. Understanding their exposure profile during pregnancy, therefore, is of public health importance. Because both behavioral and physiological changes of pregnant women are expected to be substantial, the amount of phthalate exposure is expected to vary significantly over the course of pregnancy. Temporal trend of phthalate exposure during pregnancy, however, is largely unknown, especially in Asian women. The purpose of this study is to investigate the urinary concentrations of metabolites for major phthalates and alternative plasticizers over the course of pregnancy among Korean (n = 81) and Thai women (n = 102). Twenty-four metabolites from 15 plasticizers, such as dimethyl phthalate (DMP), diethyl phthalate (DEP), di-isobutyl phthalate (DiBP), di-n-butyl phthalate (DnBP), benzyl butyl phthalate (BBzP), di(2-ethylhexyl) phthalate (DEHP), dioctyl phthalate (DnOP), diisononyl phthalate (DiNP), diisodecyl phthalate (DiDP), di(2-ethylhexyl) terephthalate (DEHTP), and di-(iso-nonyl)-cyclohexane-1,2-dicarboxylate (DINCH), were measured in urine samples collected in each trimester from pregnant women. While the levels of several phthalate metabolites were significantly different by trimester among Korean women, those of Thai women were relatively consistent. Urinary metabolites of DEP and DnOP were higher in Thai pregnant women compared to Korean pregnant women. The detection frequencies of the DINCH metabolite were 67.4% and 44.9% among Korean and Thai pregnant women, respectively. However, the ratio of DINCH to DEHP metabolites was significantly higher in Thai women. According to risk assessment, 11.9% of Korean and 5.3% of Thai women were considered at risk due to phthalate exposure, and DEHP, DnBP and DiBP were identified as major risk drivers. Considering the vulnerability of growing fetuses, further studies are warranted to identify major sources of exposure to these plasticizers during pregnancy.

Phthalates are endocrine-disrupting chemicals that cause adverse health effects in wildlife and humans. Due to domestic and global regulations of phthalates in commercial products, non-phthalate plasticizers (NPPs) have been introduced into industrial markets. Few studies have been conducted on the occurrence of phthalates and NPPs in sludge from wastewater treatment plants (WWTPs). In this study, sludge samples were collected from 40 WWTPs in Korea to investigate the occurrence, compositional profiles, and emission flux of phthalates and NPPs. Total concentrations of phthalates and NPPs in sludge ranged from 4.7 to 1400 (mean: 110) μg/g dry weight and from 0.17 to 780 (mean: 28.0) μg/g dry weight, respectively. Di(2-ethylhexyl)phthalate (DEHP) was a predominant compound, suggesting widespread consumption in Korea. Di(2-ethylhexyl)terephthalate (DEHT) was dominant in industrial sludge samples, whereas di-isononyl cyclohexane-1,2-dicarboxylate (DINCH) and trioctyl trimellitate (TOTM) were dominant in domestic sludge. This implies different consumption patterns of phthalate alternatives by industry and domestic activities. Concentrations of NPPs were significantly correlated with those of high-molecular-weight (HMW) phthalates, indicating that HMW phthalates were preferentially replaced by NPPs. The emission fluxes of phthalates via domestic WWTP activities were higher than those measured for industrial WWTPs, while the emission fluxes of NPPs via industrial WWTPs were higher than those found for domestic and industrial WWTPs. This indicates that phthalate emissions are associated with household activities, while NPP emissions are associated with industrial activities.

The placenta is a crucial organ for the supply of oxygen and nutritional elements from mother to fetus. Several studies have reported evidence of the placental transfer of persistent organic pollutants (POPs). Despite the importance of prenatal exposure to POPs, the transport process of POPs via the human placenta is not well understood. To investigate the transport processes of these contaminants and to assess the feasibility of the placenta as a non-invasive biological matrix, we measured 19 polychlorinated biphenyls (PCBs), 18 organochlorine pesticides (OCPs), and 24 polybrominated diphenyl ethers (PBDEs) in placenta tissues. The total concentrations of PCBs, OCPs, and PBDEs in placental tissues ranged from 0.36 to 75.2 (median: 5.85) ng/g lipid wt, 1.37 to 250 (63.5) ng/g lipid wt, and 1.21 to 427 (11.7) ng/g lipid wt, respectively. The BDE 209 concentrations were higher than those reported in previous studies presumably because of the high consumption of deca-BDE technical mixtures in Korea. The concentrations of all of the POPs in placental tissues correlated significantly with each other, but BDE 209 concentration did not correlate with that of any other contaminants possibly because of different exposure sources and kinetics. Maternal age, body mass index, and parity were contributors to the accumulation of several POPs in the placenta. Partitioning ratios between maternal blood-placenta-cord blood showed that lower molecular-weight and hydrophobic POPs were preferentially transported from maternal blood to the placenta and that higher molecular-weight and hydrophobic contaminants tended to remain in placental tissues. Regression analysis showed significant relationships between the POP concentrations in multiple biological matrices such as maternal blood, placenta, cord blood, and meconium. These relationships suggest that the placenta can be used as a non-invasive matrix for biomonitoring prenatal exposure to several POPs. (C) 2017 Elsevier B.V. All rights reserved.

Several studies suggested potential links of phthalates to stress-related outcomes. However, limited evidence has been available for the relationships between phthalate metabolites and free cortisol and 8-hydroxy-2'-deoxyguanosine (8-OHdG) in perinatal and postnatal environments. Therefore, we evaluated the relationships between phthalate metabolites and free cortisol and 8-OHdG in mother-child pairs. We repeatedly collected urine samples of 287 mother-child pairs from just before delivery to 15 months of age to measure the levels of four phthalate metabolites - mono-(2-ethyl-5-hydroxyhexyl) phthalate (MEHHP), mono-(2-ethyl-5-oxohexyl) phthalate (MEOHP), mono-isobutyl phthalate (MiBP), and mono-n-butyl phthalate (MnBP) - and free cortisol and 8-OHdG. We used linear mixed effect models and generalized additive mixed models to estimate the relationship between the phthalate metabolites and free cortisol and 8-OHdG after adjusting for the child's gender, urine collection time, and maternal smoking status. The four phthalate metabolite levels were strongly correlated each other (all, p .0001), and intra-class correlation for each metabolite in children ranged from 0.18 to 0.96. All four phthalate metabolites were positively associated with both free cortisol (MEHHP, β = 0.18 and p .0001; MEOHP, β = 0.17 and p .0001; MiBP, β = 0.13 and p = .0001; MnBP, β = 0.21 and p .0001; and molar sum of metabolites, β = 0.21 and p .0001) and 8-OHdG (MEHHP, β = 0.20 and p .0001; MEOHP, β = 0.18 and p .0001; MiBP, β = 0.23 and p .0001; MnBP, β = 0.28 and p .0001; and molar sum of metabolites, β = 0.29 and p .0001) in childhood. Our findings suggest that phthalate exposures increase free cortisol and 8-OHdG levels in early childhood.

Despite the global ban, organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) have been a persistent and significant environmental health issue worldwide. Prenatal exposure to these persistent organic pollutants (POPs) has been identified as a major route of exposure among developing fetuses and newborn infants. Among Children's Health and Environmental Health of Korea (CHECK) cohort population, pregnant females (n=148) and their matching newborn infants (n=117) recruited from four cities of Korea in 2011 were investigated. The blood serum and cord blood serum were sampled at delivery, and measured for 19 OCPs and 19 PCBs. In addition, a questionnaire regarding demographic characteristics, and dietary habits were conducted. The most frequently detected POPs in both maternal blood and cord blood were p,p'-dichlorodiphenyl dichloroethylene (DDE) (99% detection in maternal, and 98% in cord blood serum) and PCB153 (95% in maternal, 74% in cord blood serum). The levels of dichlorodiphenyl trichloroethanes (DDTs) in both maternal (average 82.5ng/g lw) and cord blood serum (average 77.5ng/g lw) were comparable to or greater than those reported in Japan about a decade ago. Approximately two thirds of the pregnant women and newborn infants showed the p,p'-DDE concentrations exceeding the biological equivalent (BE) corresponding to 10-6 excess cancer risk. In addition, less chlorinated PCBs were detected higher in both maternal and cord serum. Less chlorinated PCBs also showed greater transplacental ratio. Dairy consumption among the subjects was positively associated, and tea consumption was negatively associated with serum levels of several POPs. Our results show that the exposure to legacy POPs, especially DDTs, among pregnant women and newborn infants is still prevailing, thus warrants measures for exposure mitigation among these vulnerable populations.

In utero exposure to lead is known to cause various adverse health outcomes and early life obesity can affect permanent metabolic alterations leading to adverse health outcomes. To examine the relation between perinatal lead exposure and childhood obesity, lead level in cord bloods and growth- and obesity-related markers at birth were measured from 280 mother-child pairs. The weight, height, and body mass index (BMI) of children were measured at birth and followed up several times up to 27months of age. The relations between lead level and growth- and obesity-related markers were evaluated using a generalized linear model after adjustment for maternal age, maternal BMI, gestational period, cesarean section, and smoking status. The changes of child weight, height, and BMI z-scores at followed-up months of age after birth by lead exposure were evaluated using a generalized linear model after adjustment for covariates used in the analyses for growth- and obesity-related markers and child's gender. The lead level was positively associated with an increase of birth height (p=0.019) and a decrease of ponderal index at birth (p=0.027) in boys, but not in girls. Moreover, the lead level was positively associated with increases of BMI z-score after 18months of age (p=0.070 at 18months of age; p=0.003 at 24months of age; and p=0.002 at 27months of age). Perinatal lead exposure affected accelerated body mass increases at specific times of the children' development.

In utero exposure to mercury and lead has been linked to various adverse health effects related to growth and development. However, there was no evidence on the relationship between food consumption during pregnancy and mercury or lead level in cord blood. Therefore we measured mercury and lead levels in bloods, urines, and cord bloods obtained from 302 pregnant women and estimated relationships between food consumption during pregnancy and mercury or lead level in cord blood to identify perinatal mercury and lead exposures originated from foods during pregnancy. Relationship between food consumption and mercury or lead level was estimated using a generalized linear model after adjustment for body mass index (BMI), delivery experience, income, recruitment year, and other dietary factors for mercury and age, BMI, cesarean section, delivery experience, recruitment year, and other dietary factors for lead. Fish consumption was positively associated with mercury level in cord blood (p=0.0135), while cereal and vegetable consumptions were positively associated with lead level in cord blood (p=0.0517 for cereal and p=0.0504 for vegetable). Furthermore, tea consumption restrained increase of lead level in cord blood (p=0.0014). Our findings support that mercury or lead exposure in Korean pregnant women may come from frequent fish and cereal or vegetable consumption while tea consumption may decrease lead exposure in pregnant women. Therefore, careful intervention through food consumption should be considered.

Phthalates have been associated with endocrine disruption and developmental effects in many experimental and epidemiological studies. Developing infants are among the most susceptible populations to endocrine disruption. However, limited information is available on phthalate exposure and its associated risks among breast-fed newborn infants. In the present study, breast milk samples were collected from 62 lactating mothers at 1 month post-partum from four cities of Korea in 2012 and were evaluated for six phthalate metabolites (mono-isobutyl phthalate (MiBP), mono-n-butyl phthalate (MnBP), mono(2-ethyl-hexyl) phthalate (MEHP), mono-(2-ethyl-5-hydroxyhexyl) phthalate (MEHHP), mono-(2-ethyl-5-oxohexyl) phthalate (MEOHP) and monoethyl phthalate (MEP)). MEP was detected in all breast milk samples, with a median concentration of 0.37 μg/L, and MiBP, MnBP and MEHP were detected in 79-89% of samples, with median concentrations of 1.10, 1.70, and 2.08 μg/L, respectively. However, MEHHP and MEOHP, the oxidized forms of di-ethyl-hexyl phthalate (DEHP), were detected in only one sample. For exposure assessment, the levels of phthalate diesters were estimated based on the parent:metabolite ratios in the breast milk that are reported elsewhere. For risk assessment, the endocrine-related toxicity of the monoester was assumed to be the same as that of its diester form. Median daily intake estimates of phthalates, including both monoester and diester forms, through breast milk consumption ranged between 0.91 and 6.52 μg/kg body weight (bw) for DEHP and between 0.38 and 1.43 μg/kg bw for di-n-butyl phthalate (DnBP). Based on the estimated daily intake, up to 8% of infants exceeded the reference dose of anti-androgenicity (RfD AA) for DEHP, and 6% of infants exceeded the tolerable daily intake (TDI) for DnBP. Breast milk MiBP and MnBP concentrations showed significant positive associations with maternal consumption of whipped cream or purified water. Considering vulnerability of young infants, efforts to mitigate phthalate exposure among lactating women are warranted.

Siloxanes are widely used in various industrial applications as well as in personal care products. Despite their widespread use and potential toxic effects, few studies have reported on the occurrence of siloxanes in the environment. In this study, we determined the concentrations of 5 cyclic and 15 linear siloxanes in sludge collected from 40 representative wastewater treatment plants (WWTPs) in Korea. Total concentrations of 20 siloxanes (Σsiloxane) in sludge ranged from 0.05 to 142 (mean: 45.7) μg/g dry weight, similar to the concentrations reported in European countries but higher than those reported in China. The concentrations of siloxanes in sludge from domestic WWTPs were significantly (p

Data on the residue levels of persistent organic pollutants (POPs) in baby food samples are scarce. This is the first study to explore current contamination status and exposure assessment of organochlorines (OCs), including polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs), in baby food from Korea In this study, the concentrations of OCs were determined in homemade baby food samples (n = 100) collected from 6-, 9-, 12- and 15-month-old infant groups. The average concentrations of PCBs, dichloro-diphenyl-trichloroethanes (DDTs), hexachlorocyclohexanes (HCHs) and chlordanes (CHLs) in baby food samples were 37.5, 96.6, 26.0, and 132 pg/g fresh weight, respectively. The major compounds were CBs 28, 153, 52, and 33 for PCBs and p,p'-DDE, p,p'-DDT and beta-HCH for OCPs. The contribution of DDTs to the total OC concentrations increased from 30% (6-month-old infants) to 67% (15-month-old infants) with increasing infant age, while the concentrations of PCBs, HCHs and CHLs gradually decreased with increasing infant age, suggesting that highest priority for risk reduction of DDTs. The estimated daily intakes (EDIs) of OCs in Korean infants from baby food consumption were lower than the thresholds proposed by the United States Environmental Protection Agency and Health Canada, implying limited potential health risks. However, considering simultaneous exposure from baby food and breast milk consumption, chlordanes and heptachlor epoxide posed potential health risks. Considering the importance of early development and the vulnerability of infants, it is essential to perform systematic monitoring and management programs of OCs in baby food for risk reduction in Korean infants. (C) 2013 Elsevier B.V. All rights reserved.

Concentrations of polybrominated diphenyl ethers (PBDEs) were determined in commonly consumed seafood and house dust collected from Korea. Total concentrations of PBDEs in seafood and house dust samples were in the ranges of 0.06 to 6.25 ng/g wet weight and 80 to 16,000 ng/g dry weight, respectively. Predominant congeners in seafood were BDEs 47, 99 and 100 and those in dust samples were BDE 209. Estimated daily intakes (EDIs) of PBDEs through seafood consumption and dust ingestion for adults (20 years) and toddlers (2 years) were 1.83 and 11.4 ng/kg body weight/day, respectively. In comparison with the EDIs reported for PBDEs by general population in several countries, the contribution of seafood consumption to PBDE intake in Korea was the highest. Seafood consumption and dust ingestion contributed equally to the total PBDE intakes in Korean adults, while dust ingestion was the major contributor to toddlers. This study was the first to assess exposure of humans to PBDEs through two major exposure pathways.