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Health risks from exposure to contaminants are generally estimated by evaluating concentrations of the contaminants in environmental matrixes. However, accurate health risk assessment is difficult because of uncertainties regarding exposures. This study aims to utilize data on the concentrations of organophosphate flame retardants (OPFRs) in surface soil across China coupled with Monte Carlo simulations to compensate for uncertainties in exposure to evaluate the health risks associated with contamination of soil with this class of flame retardants. Results revealed that concentrations of ∑OPFRs were 0.793-406 ng/g dry weight (dw) with an average of 23.2 ng/g dw. In terms of spatial distribution, higher OPFRs concentrations were found in economically developed regions. Although the values of health risk of OPFRs in soil across China were below the threshold, the high concentrations of OPFRs in soil in some regions should attract more attentions in future. Sensitivity analysis revealed that concentrations of OPFRs in soil, skin adherence factor, and exposure duration were the most sensitive parameters in health risk assessment. In summary, the study indicated that the national scale soil measurement could provide unique information on OPFRs exposure and health risk assessment, which was useful for the management of soil in China and for better understanding of the environmental fate of OPFRs in the global perspective., (© 2023. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

As the result of the phase-out on polybrominated diphenyl ethers, organophosphate flame retardants (OPFRs) were widely used as substitutes in the world. Previous studies found that OPFRs were frequently detected in environmental, biological, and human samples. Considering their adverse effects, the absorption, bioaccumulation, metabolism and internal exposure processes of OPFRs attracted more attentions recently, especially for aryl-OPFR and Cl-OPFRs. In the present study, the biotransformation, metabolic kinetics and related CYP450 isoforms of typical Cl-OPFR (tris(1,3-dichloro-2-propyl) phosphate: TDCPP) and aryl-OPFR (triphenyl phosphate: TPhP) were studied in vitro by mouse liver microsomes. Metabolomic analysis revealed that TDCPP may be easier to bio-accumulate in organisms than TPhP, which can be explained by their metabolic rates and half-life values (TDCPP: t 1/2  = 1.8083 h; TPhP: t 1/2  = 0.1531 h). CYP2E1, CYP2D6, CYP1A2 and CYP2C19 were suggested to be the specific enzymes for the biotransformation of TDCPP via associated inhibition assay. CYP2E1 was the primary CYP450 isoform of metabolism in vitro for TPhP. These findings may provide new insights for the potential mechanism of hepatotoxicity in mammals induced by OPFRs and the detoxification process of OPFRs in hepatocytes., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

The risk of human exposure to particulate novel brominated flame retardants (NBFRs) in the atmosphere has received increasing attention from scientists and the public, but currently, there is no reliable approach to predict the intake of these compounds on the basis of their size distribution. Here, we develop a reliable approach to predict the size-dependent inhalation intake of particulate NBFRs, based on the gas/particle (G/P) partitioning behavior of the NBFRs. We analyzed the concentrations of eight NBFRs in 363 size-segregated particulate samples and 99 paired samples of gaseous and bulk particles. Using these data, we developed an equation to predict the G/P partitioning quotients of NBFRs in particles in different size ranges ( K P i ) based on particle size. This equation was then successfully applied to predict the size-dependent inhalation intake of particulate NBFRs in combination with an inhalation exposure model. This new approach provides the first demonstration of the effects of the temperature-dependent octanol-air partitioning coefficient ( K OA ) and total suspended particle concentration (TSP) on the intake of particulate NBFRs by inhalation. In an illustrative case where TSP = 100 μg m -3 , inhalation intake of particulate NBFRs exceeded the intake of gaseous NBFRs when log K OA > 11.4.

Organophosphate flame retardants (OPFRs), used extensively as substitutes for polybrominated diphenyl ethers, are ubiquitous environmental contaminants. OPFR pollution in aquatic environments, the main sink of pollutants, has been studied extensively over the past decade. Here, we review the current knowledge on the consumption and applications of OPFRs, and on their ecotoxicity in aquatic environments worldwide. We also synthesize the available evidence on the occurrence of OPFRs in aquatic environments in China (wastewater treatment plant influent and effluent, surface water, sediment, aquatic biota, and drinking water). Across China, the measured concentrations of OPFRs differ by more than three orders of magnitude. Risk assessments based on these measurements indicate a low level of ecological risk from OPFRs in most aquatic environments in China, and a low risk to human health from drinking water and aquatic products. Finally, we identify gaps in the current knowledge and directions for further research on OPFRs in aquatic environments., Competing Interests: Declaration of competing interest The authors declare that they have no known competing interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

To investigate the seasonal variation of organophosphate esters (OPEs) in air particulate matter (PM) and the corresponding influence factors in indoor environment, 104 indoor PM samples were collected in a test home, Harbin, China, from March 2017 to March 2018. The Σ 12 OPEs concentrations ranged from 0.41 ng/m 3 to 940 ng/m 3 . Tris(1-chloro-2-propyl) phosphate (TCIPP) was the most abundant OPE and accounted for 83.2% of the total OPEs. The Σ 12 OPEs concentrations in spring and summer were higher than those in autumn and winter. Outdoor total suspended particles (TSP) were the main factor that affected the concentration variation of OPEs in PM samples in the test home. Comparisons of the gas/particle (G/P) partitioning equilibrium models indicated that the Dachs-Eisenreich (D-E) model estimates were more reliable than the other models in this study. The particle fractions of OPEs with log K OA  > 10.51 that predicted by all four models generally well matched the measured OPE particle fractions in the literatures. To OPEs with lower molecular weight, inhalation was the main exposure route and ingestion contributed mostly to OPEs with higher molecular weight. In addition, the estimated daily intakes (EDIs) and carcinogenic risks (CRs) posed by OPEs were all below the recommended values, indicating that the current OPE levels in the test home were within the safe thresholds., Competing Interests: Declaration of competing interest The authors declare no competing financial interests., (Copyright © 2020 Elsevier B.V. All rights reserved.)

Ten polybrominated diphenyl ethers (PBDEs) and 16 novel brominated flame retardants (NBFRs) were measured in air and dust samples collected in a test home in Harbin, China, from January 2017 to June 2018. The PBDE and NBFR concentrations in indoor air were in the ranges of 0.598-14.5 pg m -3 and 9.28-686 pg m -3 , respectively. The ranges of the PBDE and NBFR concentrations in indoor dust were 221-1060 ng g -1 and 71.9-1160 ng g -1 , respectively. Brominated flame retardant (BFR) concentrations in indoor air were affected by the temperature, relative humidity (RH), and ventilation. The BFR concentrations in indoor dust did not show temperature dependence. All dust samples were sieved into 6 size fractions (F1-F6: 1000-2000 μm, 500-1000 μm, 250-500 μm, 125-250 μm, 63-125 μm, and < 63 μm). The mass percentage of BFRs in F6 was the highest. The BFR concentrations did not increase constantly with a particle size decrease, and the concentrations in F2 were higher than those in F3. The partitioning behavior of BFRs illustrates that the dust-air partitioning coefficient approximately approached equilibrium within F5, F6, and the total dust fraction (FA) in the test home when logK OA was between 9.1 and 11.32. Air-dust fugacity fractions were calculated, and the results suggested that most of the BFRs were mainly transferred from air to dust in the indoor environment for F1-F6.

Organophosphate flame retardants (OPFRs) are widely added to consumer products and building materials, which may pose potential health risk to humans. But information on their contamination and human exposure in the indoor environment especially dormitories in northern China is rare. In this study, twelve OPFRs were investigated in college dormitory dust that collected from Harbin, Shenyang, and Baoding, in northern China. Indoor dust samples were also collected from homes and public microenvironments (PMEs) in Harbin for comparison. The median ∑OPFR concentrations in dormitory dust in Shenyang samples (8690 ng/g) were higher than those in Baoding (6540 ng/g) and Harbin (6190 ng/g). The median ∑OPFR concentrations in home dust (7150 ng/g) were higher than in dormitory and PME dust (5340 ng/g) in Harbin. Tris(2‑chloroethyl) phosphate (TCEP) and tris (2-chloroisopropyl) phosphate (TCIPP) were the most abundant chlorinated OPFRs, while triphenyl phosphate (TPHP) and tris(2‑butoxyethyl) phosphate (TBOEP) were the dominant non-chlorinated OPFRs. The daily intakes of ∑OPFR were estimated, with the median values for female students (2.45 ng/kg-day) higher than those for male students (2.15 ng/kg-day) while were similar to adults (2.45 ng/kg-day) in homes. The estimated daily intakes (EDI) of these OPFRs from indoor dust in Harbin were all below the recommended values. The calculated non-carcinogenic hazard quotients (10 -8 -10 -3 ) from OPFRs were much lower than the theoretical risk threshold. Meanwhile, carcinogenic risk (CR) of tri‑n‑butyl phosphate (TNBP), TCEP, tris(2‑ethylhexyl) phosphate (TEHP), and tris(1,3‑dichloroisopropyl) phosphate (TDCIPP) were also estimated. The highest carcinogenic risk of TCEP for gender-specific and age-specific category range from 1.75 × 10 -7 to 2.46 × 10 -7 from exposure to indoor dust indicated a low potential carcinogenic risk for human exposure., (Copyright © 2019 Elsevier B.V. All rights reserved.)

This paper presents the first comprehensive survey of 19 novel brominated flame retardants (NBFRs) in soil samples collected among five Asian countries. High variability in concentrations of all NBFRs was found in soils with the geometric mean (GM) values ranging from 0.50 ng/g dry weight (dw) in Vietnam to 540 ng/g dw in the vicinity of a BFR manufacturer in China. In urban, rural, and background locations, the GM concentrations of ∑ 19 NBFRs decreased in the order of Japan > South Korea > China > India > Vietnam. Correlations among different NBFR compounds were positive and statistically significant (p < 0.05), suggesting that they originate from similar sources. Evidence for simultaneous application between polybrominated diphenyl ethers (PBDEs) and NBFRs were also noted. Principal component analysis of NBFR concentrations revealed specific pollution sources for different NBFRs coming from urban, BFR-related industrial, and e-waste sites. For the first time, this study demonstrates a "point source fractionation effect" for NBFRs and PBDEs. The concentrations of all NBFRs and PBDEs were negatively and significantly correlated with the distance from BFR-related industrial and e-waste regions. Positive and significant correlation between population density and NBFR concentrations in soils was identified. Our study revealed that the primary sources effects were stronger than the secondary sources effects in controlling the levels and distribution of NBFRs and PBDEs in soils in these five Asian countries.

The occurrence and temporal trends of polybrominated diphenyl ethers (PBDEs) and non-PBDE brominated flame retardants (NBFRs) were investigated in an urban atmosphere of Northeast China in consecutive six years (2008-2013). Among all chemicals, BDE-209, l,2,5,6,9,10-hexabromocyclododecane (HBCD), and decabromodiphenylethane (DBDPE) were the three most dominant compounds. During the period, the levels of pentabromodiphenyl ethers in the gas-phase and octabromodiphenyl ethers in the particle-phase significantly decreased, while the levels of BDE-209 and NBFRs increased in either the gas-phase or particle-phase. Ambient temperature was the most significant variable that influenced the gas-phase and particle-phase concentrations of BFRs, followed by wind speed and relative humidity. A stronger temperature dependence of the atmospheric concentrations was found for lower mass BFRs. Gas-particle partitioning studies suggested PBDEs in the urban atmosphere of Northeast China were at steady-state. Steady-state equation can also well describe the partitioning behavior for NBFRs, suggesting that the atmospheric partitioning behaviors of NBFRs were similar to those of PBDEs., (Copyright © 2016 Elsevier B.V. All rights reserved.)

Wastewater treatment plant (WWTP) is considered to be an important medium for the transport and transformation of organic pollutants. This study attempted to comprehensively investigate polybrominated diphenyl ethers (PBDEs) and novel brominated flame retardants (NBFRs) in a WWTP in Harbin, one of the main "Old Industrial Base" in China. The mean concentrations of the total PBDEs in the influent, effluent, and sludge were 152 ng/L, 16.2 ng/L, and 503 g/g dw, respectively, which were at the low end of the global range. BDE-209 was the most abundant congener, with contributions to the total PBDE ranging from 90.5 to 98.5 %. The level of the total NBFRs ranged from 24.5 to 107 ng/L, 0.95 to 20.3 ng/L, and 305 to 1202 ng/g dw in the influent, effluent, and sludge, respectively. For NBFRs, DBDPE was the most abundant congener (38.8-50.5 %), followed by BEHTBP (11.0-35.0 %). The ratio for DBDPE/BDE-209 (0.62 ± 0.42) was found less than 1 in sludge, which indicated that Deca-BDE is still the major BFR product in this city. Source identification suggested that indoor dust should be an important source of BFRs in the WWTP. Approximately 20.8 and 7.79 kg of PBDEs and NBFRs on annual basis were removed with the sludge. Biodegradation could play an important role on the fate of BFRs in the WWTP, which is required for future research.

Surface soil samples were collected surrounding two brominated flame retardants (BFRs) manufacturing plants in China in August 2014 and analyzed for 23 polybrominated diphenyl ethers (PBDEs) and 8 novel brominated flame retardants (NBFRs). BDE209 and decabromodiphenylethane (DBDPE) were the predominant compounds in soil with the median levels of 1600 and 560 ng/g dw, respectively. The PBDEs profiles in soil samples were consistent with that of commercial product (comDecaBDE). The percentage contributions to total PBDEs decreased from higher to lower brominated homologues. Lower concentrations of NBFRs (excluding DBDPE) were detected in soil surrounding the two plants, suggesting they are byproducts or degradation products of the manufacturing activities. The concentrations of most BFRs dropped exponentially within 3-5 km of the manufacturing plants, suggesting recent deposition of these compounds to the soil. Directional distribution indicated that PBDEs and DBDPE concentrations were highest in the north direction of Plants 1. Three-day air parcel forward trajectories confirmed that the air parcel was responsible for the higher concentration of BFRs in the soil of north direction of the plant., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

This study collected 227 pairs of gas phase and particle phase air samples in a typical urban city of Northeast China from 2008 to 2013. Four alternative halogenated flame retardants for polybrominated diphenyl ethers (PBDEs) were analyzed, namely 2-ethylhexyl 2,3,4,5-tetrabromobenzoate (EHTBB), bis (2-ethylhexyl) tetrabromophthalate (BEHTBP), syn-dechlorane plus (syn-DP) and anti-dechlorane plus (anti-DP). The average concentrations for EHTBB and BEHTBP were 5.2 ± 20 and 30 ± 200 pg/m3, respectively, while for syn-DP and anti-DPwere 1.9±5.1 and 5.8±18 pg/m3, respectively. Generally, they were frequently detected in the particle phase, and the gas/particle partitioning suggested they were the maximum partition chemicals. The fractional abundance of EHTBB (fEHTBB) and syn-DP (fsyn)were comparablewith those in other studies. Strong local sources were identified based on the air parcel backward trajectories and the potential source contribution function. The concentrations of these chemicals were significantly increased during this sampling campaign, possibly suggesting their increasing usages from 2008 to 2013 in China.

Indoor environment is an important source of human exposure to several toxicants, such as brominated flame retardants. Indoor dust samples were collected in winter season in 2010, which covered 23 provinces across China, for the analysis of polybrominated diphenyl ethers (PBDEs). Concentrations of PBDEs (Σ14PBDEs) ranged from 8.92 to 37,500 ng/g, with the mean of 3520 ng/g. BDE-209 was the most dominate congener, followed by BDE-183, BDE-47 and BDE-99. PBDE concentrations and the longitude were significantly correlated (p<0.05), which was consistent with the status of social-economic development and human activities. The results of exposure to PBDEs through dust ingestion and dermal absorption indicated that the toddlers had the highest exposure dose, with the median value of 6.0 ng/kg-bw/day. According to the hazard quotients, health risk of PBDEs via dust ingestion in China is currently acceptable. Monte Carlo simulation was implemented to quantify the uncertainty and sensitivity of exposure models for determining the most influential variables. The results suggested that more specific and accurate parameters should be used for dust ingestion and dermal absorption exposure models in future., (Copyright © 2014 Elsevier Inc. All rights reserved.)

Indoor environment is an important source of human exposure to several toxicants, such as brominated flame retardants. This study presents the concentrations of 22 Non-BDE brominated flame retardants (NBFRs) in 81 indoor dust samples from 23 provinces across China in the winter of 2010. The concentrations of ΣNBFRs ranged from 6.3 to 20,000 ng/g, with a median concentration of 720 ng/g. DBDPE was the dominated compound, followed by HBCD and BEHTBP. Significant differences of concentrations were found between samples from rural and urban areas, and between family and public houses, indicating different applications of NBFRs. The geographical distribution of NBFRs highlighted several hotspots in North China, suggesting the influence of room temperature (heating). The exposure via dust ingestion of NBFRs was 3.8-14 times higher than that of dermal absorption. The toddlers demonstrated the highest exposure dose (9.6 ng/kg-bw/day) of NBFRs through indoor dust among all life stages., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

57 pairs of air samples (gas and particle phases) were collected using a high volume air sampler in a typical city of Northeast China. Brominated flame retardants (BFRs) including 13 polybrominated diphenyl ethers (PBDEs, including BDEs 17, 28, 47, 49, 66, 85, 99, 100, 138, 153, 154, 183, and 209) and 9 alternative BFRs (p-TBX, PBBZ, PBT, PBEB, DPTE, HBBZ, γ-HBCD, BTBPE, and DBDPE) were analyzed. The annual average total concentrations of the 13 PBDEs and the 9 alternative BFRs were 69 pg/m(3) and 180 pg/m(3), respectively. BDE 209 and γ-HBCD were the dominant congeners, according to the one-year study. The partial pressure of BFRs in the gas phase was significantly correlated with the ambient temperature, except for BDE 85, γ-HBCD and DBDPE, indicating the important influence of ambient temperature on the behavior of BFRs in the atmosphere. It was found that the gas-particle partitioning coefficients (logKp) for most low molecular weight BFRs were highly temperature dependent as well. Gas-particle partitioning coefficients (logKp) also correlated with the sub-cooled liquid vapor pressure (logPL(o)). Our results indicated that absorption into organic matter is the main control mechanism for the gas-particle partitioning of atmospheric PBDEs., (Copyright © 2014 Elsevier B.V. All rights reserved.)