The distribution of dechloranes, a group of chlorinated flame retardants, were investigated in air, soil, and sediment around a newly discovered Dechlorane Plus (DP) production facility in China (Anpon). To date, the only known DP manufacturing plant is located in Niagara Falls, NY (OxyChem). Dechloranes including DP, Dechlorane (Mirex), and the recently discovered Dechlorane 602 (Dec 602) were detected in air, soil, and sediment, while Dechlorane 603 and Dechlorane 604 were below detection limit in all matrices. DP air concentrations near the facility ranged from 7737 to 26 734 pg m(-3), the greatest reported thus far. Soil concentrations in the same area for DP, Dechlorane, and Dec 602 were 1490+/-3580 ng g(-1), 81.6+/-96.5 ng g(-1), and 7.24+/-13.2 ng g(-1) dry weight, respectively. Interestingly, lower concentrations of DP (4.93+/-4.34 ng g(-1)), Dechlorane (30.2+/-19.9 ng g(-1)), and Dec 602 (2.14+/-2.23 ng g(-1)) were found in sediment from a nearby canal. Spatial trends of Dechlorane and Dec 602 in soil were similar to DP, implying that the DP manufacturing plant may also be a source of these other flame retardants. DP soil concentrations surrounding the facility decreased by an order of magnitude within 7.5 km. The syn-DP fractional abundance (fsyn) value (0.40) for the commercial DP product manufactured at Anpon was slightly higher than that (0.20-0.36) produced by OxyChem. The fsyn value in most air samples was largely similar to the Chinese commercial DP mixture, while most soil and sediment abundances were lower, suggesting a stereoselective depletion of syn-DP.
Gas/particle (G/P) partitioning of semi-volatile organic compounds (SVOCs) is an important process that primarily governs their atmospheric fate, long-range atmospheric transport, and their routes of entering the human body. All previous studies on this issue are hypothetically based on equilibrium conditions, the results of which do not predict results from monitoring studies well in most cases. In this study, a steady-state model instead of an equilibrium-state model for the investigation of the G/P partitioning behavior of polybrominated diphenyl ethers (PB-DEs) was established, and an equation for calculating the partition coefficients under steady state (K PS ) of PBDEs (log K PS = log K PE + logα) was developed in which an equilibrium term (log K PE = log K OA + logf OM −11.91 where f OM is organic matter content of the particles) and a nonequilibrium term (log α, caused by dry and wet depositions of particles), both being functions of log K OA (octanol-air partition coefficient), are included. It was found that the equilibrium is a special case of steady state when the nonequilibrium term equals zero. A criterion to classify the equilibrium and non-equilibrium status of PBDEs was also established using two threshold values of log K OA , log K OA1 , and log K OA2 , which divide the range of log K OA into three domains: equilibrium, non-equilibrium, and maximum partition domain. Accordingly, two threshold values of temperature t, t TH1 when log K OA = log K OA1 and t TH2 when log K OA = log K OA2 , were identified, which divide the range of temperature also into the same three domains for each PBDE congener. We predicted the existence of the maximum partition domain (the values of log K PS reach a maximum constant of −1.53) that every PBDE congener can reach when log K OA ≥ log K OA2 , or t ≤ t TH2 . The novel equation developed in this study was applied to predict the G/P partition coefficients of PBDEs for our Chinese persistent organic pollutants (POPs) Soil and Air Monitoring Program, Phase 2 (China-SAMP-II) program and other monitoring programs worldwide, including in Asia, Europe, North America, and the Arctic, and the results matched well with all the monitoring data, except those obtained at e-waste sites due to the unpredictable PBDE emissions at these sites. This study provided evidence that the newly developed steady-state-based equation is superior to the equilibrium-state-based equation that has been used in describing the G/P partitioning behavior over decades. We suggest that the investigation on G/P partitioning behavior for PBDEs should be based on steady state, not equilibrium state, and equilibrium is just a special case of steady state when non-equilibrium factors can be ignored. We also believe that our new equation provides a useful tool for environmental scientists in both monitoring and modeling research on G/P partitioning of PBDEs and can be extended to predict G/P partitioning behavior for other SVOCs as well.
Air samples were concurrently collected using high volume air samplers for 24 h every week from September 2008 to August 2009 at 15 sites (11 urban, 1 suburban, and 3 background/rural) across China. Twelve polybrominated diphenyl ether (PBDE) congeners (BDE-17, -28, -47, -66, -85, -99, -100, -138, -153, -154, -183, and -209) were measured. Total PBDE concentrations (∑12PBDEs) in air (gas + particle phases) were in the range of 11.0-838 pg m(-3) with a mean of 232 ± 72 (mean ± SE) pg m(-3). The site with the highest concentration was Guangzhou (838 ± 126 pg m(-3)), followed by Beijing (781 ± 107 pg m(-3)). Significant positive correlations were found between PBDEs levels and urban population (R = 0.69, P < 0.05) and gross industrial output values (R = 0.87, P < 0.001) as well. BDE-209 was the dominating congener with the contribution of 64 ± 23% to ∑12PBDEs, followed by BDE-47(8 ± 8%) and -99(6 ± 5%) at all urban and suburban sites. At background/rural sites, however, BDE-47 was the dominating congener, followed by BDE-99, together accounting for 52 ± 21% of ∑12PBDEs, while BDE-209 was only 11 ± 2%. It was found that PBDEs at the 15 sites showed a primary distribution and fractionation pattern. This study produced more than 700 pairs of air samples in gaseous and particulate phases with a wide temperature range of ∼60 °C, providing a good opportunity to investigate gas-particle partitioning for individual PBDE congeners. The results of gas-particle partitioning analysis for PBDEs using both subcooled-liquid-vapor pressure (PL)-based and octanol-air partition coefficient (KOA)-based models indicated that PBDEs in air at all sampling sites had not reached equilibrium because the slope values (mO) in the KOA-based equation and the opposite slope values (mP) in the PL-based equation at all 15 sampling sites were less than 1. It also found that both mO and -mP were significantly and positively correlated with the annual average temperatures of sampling sites and also significantly and negatively correlated with the mole masses of PBDE congeners, indicating a general trend that the higher the temperature at the sampling site and the lower the mole mass of the PBDE congeners are, the closer to the equilibrium the congeners approach and vice versa. To our knowledge, this is the first study to report the correlations of the slope values for both the KOA-based and PL-based equations with temperatures at sampling sites and mole masses for individual PBDE congeners.
Polybrominated diphenyl ethers (PBDEs) are ubiquitous environmental pollutants, and, on a global basis, North American populations are exposed to the highest doses of PBDEs. In response to the exponential increase in human exposure to PBDEs during the late 1990s, some PBDE formulations were phased out from production in the early 2000s. The effectiveness of the phase-out of commercial Penta-BDE and Octa-BDE mixtures in 2004 in the U.S. on human exposure levels is not known. Dried blood spots (DBSs), collected for the newborn screening program (NSP) in the U.S., are a valuable resource for the elucidation of trends in exposure to environmental pollutants in newborns. In this study, seven PBDE congeners were determined by gas chromatography-high resolution mass spectrometry (GC-HRMS) in archived DBS samples (in total, 51 blood spot composites from 1,224 newborns) collected from newborns in New York State (NYS) from 1997 to 2011. The most frequently detected PBDE congener was BDE-47, with a detection rate (DR) of 86%, followed by BDE-99 (DR: 45%) and BDE-100 (DR: 43%). The mean concentrations determined during 1997 through 2011 in the whole blood of newborns were 0.128, 0.040, and 0.012 ng/mL for BDEs −47, −99, and −100, respectively. A significant correlation was found among the concentrations of three major congeners (p < 0.001). PBDE concentrations were similar during 1997 through 2002 and, thereafter, decreased significantly, which was similar to the trends observed for perfluorinated compounds (PFCs) in DBS samples. Occurrence of PBDEs in the whole blood of newborns confirms that these compounds do cross the placental barrier.
Indoor window film samples were collected in buildings during 2014-2015 for the determination of six phthalate diesters (PAEs). Linear regression analysis suggested that the film mass was positively and significantly correlated with the duration of film growth (from 7 to 77 days). PAEs were detected in all window film samples (n = 64). For all the samples with growth days ranged from 7 to 77 days, the median concentrations of total six PAEs (∑6PAEs) in winter and summer window film samples were 9900 ng/m(2) film (2000 μg/g film) and 4700 ng/m(2) film (650 μg/g film), respectively. Among PAEs analyzed, di-2-ethyl-hexyl phthalate (DEHP) was the major compound (71 ± 9.7%), followed by di-n-butyl phthalate (DBP; 20 ± 7.4%) and diisobutyl phthalate (DiBP; 5.1 ± 2.2%). Positive correlations among PAEs suggested their common sources in the window film samples. Room temperature and relative humidity were negatively and significantly correlated with PAEs concentations (in ng/m(2)). Poor ventilation in cold winter in Noreastern China significantly influenced the concentrations of PAEs in window film which suggested higher inhalation exposure dose in winter. The median hazard quotient (HQ) values from PAEs exposure were below 1, suggesting that the intake of PAEs via three exposure pathways was considered as acceptable.
Parabens are widely used as preservatives in foods, cosmetics, and pharmaceuticals. However, recent studies have indicated that high and systemic exposure to parabens can be harmful to human health. Although a few studies have reported urinary paraben levels in western countries, studies on paraben exposure in the Chinese population are limited. China is currently a major producer of parabens in the world. In this study, 109 urine samples collected from Chinese young adults (approximately 20 years old) were analyzed for five parabens (methyl-, ethyl-, propyl-, butyl-, and benzyl-parabens) by high-performance liquid chromatography-tandem mass spectrometry. Methyl-, propyl-, and ethyl-parabens were the three major paraben analogues found in all (100%) samples. The concentration of the sum of the five parabens ranged from 0.82 to 728 ng/mL with a geometric mean value of 17.4 ng/mL. Urinary concentration of parabens was 2-fold greater in females than in males. Based on the measured urinary concentrations, daily intake of parabens by the Chinese young adults was estimated and compared with those reported for United States adults. The estimated daily intakes (EDIurine) of parabens were 18.4 and 40.8 μg/kg bw/day for Chinese males and females, respectively, values that were lower than those reported for United States adults (74.7 μg/kg bw/day). Based on the reported concentrations of parabens in foods from China and the United States, the contribution of dietary intake to EDIurine was estimated to be 5.5, 2.6, and 0.42% for Chinese males, Chinese females, and United States adults, respectively, which indicates the significance of nondietary sources of parabens to human exposures.
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