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As a class of plasticizers widely used in consumer products, some phthalate esters (PAEs) have been restricted due to their adverse health effects and ubiquitous presence, leading to the introduction of alternative non-phthalates plasticizers (NPPs) to the market. However, few studies focus on the influence of environmental parameters on the presence of these plasticizers and the potential human health risks for people living in poorly ventilated indoor spaces in cold regions. We investigated the trends of PAEs and NPPs in air in a typical indoor residence in northern China for over one year. The air concentrations of PAEs were significantly higher than those of NPPs (p0.05), indicating that PAEs are still the dominant plasticizers currently being used in the studied residence. PAEs showed seasonal fluctuation patterns of the highest levels found in summer and autumn. The temperature and relative humidity dependence for most PAEs and NPPs decreased with decreasing vapor pressure. Concentrations of the high molecular weight NPPs and PAEs positively correlated with total suspended particles (TSP). It is worth noting that the peak concentrations of PAEs and NPPs were found when the haze occurred in autumn. Principal component analysis (PCA) suggested the diverse applications of PAEs and NPPs in the indoor environment. The hazard index (HI) values observed in this study were all below international guidelines (1); however, the average carcinogenic risk (CR) values for some compounds exceeded acceptable levels (One in a million), which raised concerns about the possibility of carcinogenicity for people living indoors for long periods of time in cold regions.

Clothing easily adsorbed the chemicals in the environment, and became a source of human exposure to chemicals. However, large contacted surface area and long exposure duration have elevated human exposure to chemicals from clothing, such as phthalates. Among them, cotton clothing, which infants prefer to wear, has been proven to adsorb phthalates more easily than other fabrics. While infants are developing, they are easily affected by phthalates. In this study, in order to study accumulation of phthalates in infant cotton clothing during the whole process from production to the first wearing, 24 infant cotton clothing samples were collected from shopping malls in Harbin, China. High detection rates and concentrations suggest that phthalates in the environment are widely adsorbed to infant cotton clothing, and traditional laundering for infant clothing cannot remove phthalates completely. The median concentration of the total phthalates was 4.15 μg/g. Di-(2-ethylhexyl) phthalate (DEHP) has become the dominant phthalate. For the estimated daily intakes (EDIs) for infants, dibutyl phthalate (DBP) had the highest contribution, followed by di-iso-butyl phthalate (DiBP) and DEHP. Dermal absorption has become the main route of infant exposure to phthalates, and ingestion contributed very little. The result of comparing with the EDIs via dermal absorption from house air and dust suggests that clothing plays an important role of dermal absorption exposure to phthalates. For risk assessment, the carcinogenic risk of BBP and DEHP indicates that the level of DEHP in infant cotton clothing might pose potential adverse effects to infant health.

The gas/particle (G/P) partition of organochlorine pesticides (OCPs) has been widely investigated and well documented, but rare at low temperature. In this study, seventy-four pairs of air samples in two sampling sites in northeastern China at a wide ambient temperature range of ~63 °C (−40 to +23 °C) were simultaneously collected in both gaseous and particulate phases and eighteen OCPs in these samples were measured and analyzed, among which, partition quotient (KP) values for fifteen OCPs were determined. Seven models including those have never been used for OCPs were applied to predict the values of KP, and the results were compared with the monitoring data for the fifteen OCPs. It was found out that, L-M-Y model provided advantages over the other models, with the best agreement to the monitoring data for analyzed OCPs (90.1 ± 11.1% data points within ±1 log unit, RMSE: 0.53 ± 0.18). The predicted maximum partition (MP) domain for eleven OCPs was observed with high values of their logarithm of octanol-air partition coefficient (log KOA > 12.5), where the log KP values become a constant (−1.53), indicating that the G/P partition of OCPs is in steady state but not the equilibrium. The Li-Ma-Yang (L-M-Y model) model, considering the wet and dry depositions of particles, elucidates the necessity of non-equilibrium term for the OCPs at low temperature. These results indicate that the L-M-Y model is valid for OCPs, which renders it highly promising for describing the partition behaviors in atmosphere for SVOCs, particularly at low temperature. An equation to calculate the condensation temperature TC was also derived, which gave a new understanding on the situation of chemicals with equal distribution between gaseous and particulate phases of OCPs and other similar SVOCs, especially in Polar Regions.

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.

The study of the fate of organophosphate esters (OPEs) in the interior environment is vital because of the growing use of OPEs. Organic films on glass are both sink and sources of indoor pollutants. Indoor window films have been employed as passive air samplers to collect OPEs in the indoor air. Nevertheless, little is known about the development and equilibrium condition of OPEs on indoor window films during the film formation process. In this study, the concentrations of twelve OPEs in indoor window films from different buildings on a university campus and the growth thickness of the films as a function of sampling time were investigated in different seasons. Ten out of the 12 OPEs were detected in window film with50 % frequency. Tris (2-chloroethyl) phosphate (TCEP) and tris (1-chloro-2-propyl) phosphate (TCPP), which are chlorinated and toxic OPEs, were the dominant OPEs found in the winter. The majority of OPEs in window films exhibited linear growth patterns within 77 days. Temperature, humidity, ventilation, and seasonality all affected the concentrations of various OPEs in the window films. Low molecular weight OPEs, such as tri-n-butyl phosphate and TCEP, attained equilibrium between indoor air and window films within 49 or 77 days. The indoor air concentrations of OPEs were estimated from their film concentrations based on the theoretical approach for the passive air sampler. In winter, the predicted gas-phase air concentrations of OPEs (3.7 ng/m

Active air samples were collected in Lhasa, one of the highest cities in the world (3650m above sea level) located in the Tibetan Plateau, and were analyzed for 38 halogenated flame retardants (HFRs), including polybrominated diphenyl ethers (PBDEs), non-PBDE brominated flame retardants (NBFRs) and dechlorane plus (DPs). The median concentrations of PBDEs, NBFRs and DPs were 40, 23 and 0.21pg/m3, respectively. Correlation analysis indicated the common source and/or similar environmental behavior for several HFRs. The Clausius-Clapeyron equation was applied to diagnose the sources of lower molecular weight HFRs (LMW-HFRs), which suggested that the gaseous LMW-HFRs at Lhasa were more controlled by regional or long-range atmospheric transport rather than the temperature-driven evaporation from local contaminated surfaces. Finally, the potential source contribution function model was applied to assess the influences of air parcels on the atmospheric concentrations of HFRs in Lhasa, which suggested that the sources of higher molecular weight HFRs (HMW-HFRs) were mostly originated from local emissions, while the others were originated from long-range atmospheric transport.

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.

Phthalates are widely used chemicals in household products, which severely affect human health. However, there were limited studies emphasized on young adults' exposure to phthalates in dormitories. In this study, seven phthalates were extracted from indoor dust that collected in university dormitories in Harbin, Shenyang, and Baoding, in the north of China. Dust samples were also collected in houses in Harbin for comparison. The total concentrations of phthalates in dormitory dust in Harbin and Shenyang samples were significantly higher than those in Baoding samples. The total geometric mean concentration of phthalates in dormitory dust in Harbin was lower than in house dust. Di-(2-ethylhexyl) phthalate (DEHP) was the most abundant phthalate in both dormitory and house dust. The daily intakes of the total phthalates, carcinogenic risk (CR) of DEHP, hazard index (HI) of di-isobutyl phthalate (DiBP), dibutyl phthalate (DBP), and DEHP were estimated, the median values for all students in dormitories were lower than adults who live in the houses. Monte Carlo simulation was applied to predict the human exposure risk of phthalates. HI of DiBP, DBP, and DEHP was predicted according to the reference doses (RfD) provided by the United States Environmental Protection Agency (U.S.EPA) and the reference doses for anti-androgenicity (RfD AA) developed by Kortenkamp and Faust. The results indicated that the risks of some students had exceeded the limitation, however, the measured results were not exceeded the limitation. Risk quotients (RQ) of DEHP were predicted based on China specific No Significant Risk Level (NSRL) and Maximum Allowable Dose Level (MADL). The predicted results of CR and RQ of DEHP suggested that DEHP could pose a health risk through intake of indoor dust.

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 Σ12OPEs concentrations ranged from 0.41 ng/m3 to 940 ng/m3. Tris(1-chloro-2-propyl) phosphate (TCIPP) was the most abundant OPE and accounted for 83.2% of the total OPEs. The Σ12OPEs 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 KOA > 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.

Phthalates are widely used in consumer products. People are frequently exposed to phthalates due to their applications in daily life. In this study, 14 phthalate metabolites were analyzed in 108 urine samples collected from Chinese young adults using high-performance liquid chromatography-tandem mass spectrometry. The total concentrations of 14 phthalate metabolites ranged from 71.3 to 2670 ng/mL, with the geometric mean concentration of 306 ng/mL. mBP and miBP were the two most abundant compounds, accounting for 48% of the total concentrations. Principal component analysis suggested two major sources of phthalates: one dominated by the DEHP metabolites and one by the group of mCPP, mBP and miBP metabolites. The estimated daily intakes of DMP, DEP, DBP, DiBP and DEHP were 1.68, 2.14, 4.12, 3.52 and 1.26-2.98 μg/kg-bw/day, respectively. In a sensitivity analysis, urinary concentration and body weight were the most influential variables for human exposure estimation. Furthermore, cumulative risk for hazard quotient (HQ) and hazard index (HI) were evaluated. Nearly half of Chinese young adults had high HI values exceeding the safe threshold. This is the first study on the occurrence and human exposure to urinary phthalate metabolites with Chinese young adults.

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.

Emission inventories for polychlorinated biphenyls (PCBs) are crucial input data for atmospheric transport modeling and for the study of source-receptor relationships and the environmental behavior of these chemicals. Three types of primary PCB sources are considered in this study: intentionally produced PCBs (IP-PCBs), unintentionally produced PCBs (UP-PCBs), and PCB emissions from two e-waste sites (EW-PCBs). This study presents the historical emissions of all IP-, UP- and EW-PCBs into the air in China and the gridded Chinese emission inventories at a resolution of 1/6° latitude×1/4° longitude from 1950 to 2010. The UP-TPCB emissions from 1950 to 2010 were re-estimated to be 8.56t from eight emission sources comprising 96.3% of the Chinese UP-TPCB emissions. The EW-TPCB emissions from 1990 to 2010 were estimated to be 103.5 t, of which 7.1t and 12.3t were EW-PCB28 and EW-7PCB congeners (i.e., indicator-PCB28, 52, 101, 118, 138, 153, 180), respectively. The IP-PCB28 and IP-7PCB congener emissions from 1965 to 2010 were estimated to be 57.4 t and 130.1t, respectively. A significant correlation was found between congener PCB28 and 7PCBs (R(2)=0.988 and P=0.000), which suggests that PCB28 is a good marker congener for describing the emission trends of all 7PCB emission sources. The gridded emission data were compared with published measured atmospheric concentrations for 2004 and 2008, and a significant correlation was found between the modeled emissions and monitoring data. To our knowledge, this study presents the first comprehensive gridded emission inventories that include all IP-, UP-, and EW-PCBs on a national scale.

Indoor dust samples were collected across China in the winter of 2010 from 45 private domiciles and 36 public buildings. 16 polycyclic aromatic hydrocarbons (PAHs) were determined by GC-MS. Total concentrations of PAHs ranged from 1.00 μg/g to 470 μg/g with a mean value of 30.9 μg/g. High-molecular weight (HMW) PAHs (4 to 6 rings) are the predominant PAHs found in indoor dust, accounting for 68% of the total PAH concentration in private domiciles, and 84.6% in public buildings. Traffic conditions and cooking methods were the two key factors controlling PAH levels, especially for coal combustion and vehicular traffic emission sources. A significant positive correlation was observed between PAH concentrations in indoor dust and based on location (latitude and longitude). The latitudinal distribution indicated a higher usage of coal for heating in Northern China than in Southern China. The longitudinal distribution indicated that the usage of oil and mineral fuels as well as economic development and population density increased from West China to East China. In addition, diagnostic ratios and principal component analysis (PCA) were used to explore source apportion, as indicated in both the pyrogenic and petrogenic sources of PAHs in indoor dust in China. Furthermore, the BaP equivalent was applied to assess the carcinogenic risk of PAHs, which also indicated that traffic emissions and coal combustion were the two major contributions to carcinogenic risk of PAHs in indoor dust in China.

The gas/particle (G/P) partitioning behavior is an important factor for the environmental fate of polycyclic aromatic hydrocarbons (PAHs) in atmosphere. Based on one year monitoring program at 11 urban sites across China, 7647 pairs of gaseous and particulate concentrations were obtained for 16 priority PAHs, which provided a good opportunity to study the G/P partitioning behavior of PAHs. The concentrations of PAHs in both gas and particle phases were not in the same level among the 11 sites with a difference of more than one orders of magnitude. Along with the increase of molar weight of PAHs, the proportion of concentration in particle phase was increasing. In particle phase, the concentrations of ∑16PAHs in northern Chinese cities were significantly (p