Despite the recent efforts to investigate the distribution and fate of persistent organic pollutants in the tropical and subtropical regions of Asia, very little was known about the temporal change of polychlorinated biphenyls (PCBs) in the environmental ecosystem of China. In this study, three dated sediment cores collected from the Pearl River Delta of southern China were analyzed for a large suite of PCB congeners, from which the temporal profiles of PCB abundances, fluxes, and homologue patterns were constructed. The sedimentary inventories of total PCBs at the sampling sites ranged from 480 to 1310 ng/cm2, at the low end of the worldwide figures. Although production and use of PCBs have been banned or highly restricted in China since the early 1980s, the fluxes of total PCBs continued to increase in the Pearl River Delta sediments. There was a concurrent increase of PCB fluxes and gross domestic product per capita in the region from 1980 to 1997, and a decline of agricultural land use was evident at the same time. Apparently, large-scale land transform since the early 1980s as well as emissions from the PCB-containing electrical equipments were responsible for the sharp rise of PCB fluxes in the recent sediments. The difference in the PCB homologue patterns from 1940 to the mid-1970s was probably indicative of the different timelines of PCB usage in Macao/Hong Kong and mainland China and the differenttypes of technical PCBs commercially used. PCBs were detectable in sediments deposited well before the time frame when production of PCBs began (before 1930) and were relatively enriched in the less chlorinated homologue groups (3Cl and 4Cl PCBs), suggesting the downward mobility of lightly chlorinated PCB congeners in the sediment column.

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Air samples were collected in June of 2004 from four sites in the city of Guangzhou, a typical urban center in South China, to determine the levels, compositional profiles, and gas-particle distribution of 11 polybrominated diphenyl ether (PBDE) congeners (BDE-28, -47, -66, -100, -99, -85, -154, -153, -138, -183, and -209). The arithmetic mean atmospheric concentrations of sigmaPBDEs (sum of all target PBDE congeners except for BDE-209) in samples from the urban and city background sites were comparable to or slightly higher than those from other places around the world. The arithmetic mean atmospheric concentrations of BDE-209, however, were higherthan those in North America and Europe, and similar to the values from Japan. Congener compositions were dominated by BDE-209 in all (>70%) but an industrial site, with an average abundance of 48% for BDE-209. The PBDE patterns were generally similar to that in the technical penta-BDE mixture, Bromkal 70-5DE. Partitioning of PBDEs between the gas and particle phases (Kp) was well correlated with the subcooled liquid vapor pressure (PLO) for all of the samples, but the relationship differed between samples from different sites. The measured fractions of PBDEs in the particulate phase were compared to the predictions from the Junge-Pankow adsorption and KOA-based absorption models. The results indicated that the KOA-based model worked better than the Junge-Pankow model that tended to overestimate the particulate fractions for most PBDE congeners.

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Dechlorane Plus (DP), a highly chlorinated flame retardant, has been detected in water, sediment, and aquatic organisms in a reservoir in the vicinity of electronic waste recycling workshops in South China. The biomagnification potential of DP in the food web was assessed and compared with that of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs). DP was detected in all of the aquatic species, with concentrations of 19.1-9630 ng/g lipid wt. A depletion of anti-DP was observed in organisms compared with abiotic samples and the fraction of anti-DP was found to be further decreased upon moving up the trophic levels. This result suggested a stereospecific metabolism of anti-DP and/or isomer-selective uptake of syn-DP was occurring in organisms. Both syn- and anti-DP were significantly biomagnified in the present food web, with trophic magnification factors (TMFs) of 11.3 and 6.6, respectively. The trophic magnification potentials of the DP isomers were generally comparable to or lower than those of the highly recalcitrant PCB congeners in the same food web, but were 2-3 times greater than those of PBDE congeners.

b S Supporting Information ' INTRODUCTION Chlorinated paraffins (CPs) with the formula (C n H 2n+2-z Cl z ) are subdivided into short-chain (C 10 ÀC 13 , SCCPs), mediumchain (C 14 ÀC 17 , MCCPs) and long-chain (C > 17, LCCPs) according to their carbon chain length, where chlorine content ranges from 10% to 72%. 1 Because of their chemical and thermal stability, CPs were widely used as additives in lubricants, as cutting fluids for metal working, as plasticizers and flame retardants in plastics, sealants, and leather. 2 As high production volume chemicals, CPs are inevitably released into the environment during their production, transportation, and usage. CPs have been detected in various environmental matrices including water, sediment, air, soil, biota ,and human beings. 1 It is also suggested that CPs are bioaccumulated and biomagnified in food webs. 3 CPs, especially SCCPs, have attracted increasing attentions in the past decade as they represent a potential "new" category of persistent organic pollutants (POPs). 4 The European Union restricted the usage of SCCPs via the Water Framework Directive based on the SCCP risk assessment. 5,6 Furthermore, SCCPs have been banned for use in Germany since 2003. 1

Several currently used non-polybrominated diphenyl ether (PBDE) brominated flame retardants (BFRs), including hexabromocyclododecanes (HBCDs), 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE), decabromodiphenyl ethane (DBDPE), hexabromobenzene (HBB), pentabromoethylbenzene (PBEB), and pentabromotoluene (PBT), are examined in the components of a freshwater food web from an electronic waste recycling site, South China. All these BFRs are detectable in the food web, with average concentrations of 13.9-868, 1.71-518, < 3.8-338, 197-3099, 3.98-25.6, and 1.20-3.60 ng/g lipid wt for HBCDs, BTBPE, DBDPE, HBB, PBEB, and PBT, respectively. Food web magnification is observed for (+)-alpha-, (-)-alpha-, (+/-)-alpha-, and total HBCDs, and HBB, with trophic magnification factors (TMFs) of 2.22, 2.18, 2.19, 1.82, and 1.46, respectively; whereas there is trophic dilution of BTBPE and PBT through the food web. The TMFs for (+)-alpha-, (-)-alpha-, and (+/-)-alpha-HBCDs are comparable to those of PBDEs detected previously in the same food web. Biota samples show a shift from gamma- toward alpha-HBCD compared with the suspended particles, sediment, and HBCD technical mixtures, with a significant increase of alpha-HBCD on ascending trophic levels. Except for alpha-HBCD in suspended particles and sediment, all the HBCD enantiomers detected are nonracemic in the environmental matrix. In biota, nonracemic residues of alpha-HBCD were observed in mud carp and crucian carp; beta-HBCD in prawn, mud carp, and crucian carp; and gamma-HBCD in water snake, with preferences for (+)-alpha-, (-)-beta-, and (+)-gamma-HBCDs.

The recycling of electrical and electronic waste (e-waste) in developing countries has attracted much attention as a significant source of brominated flame retardants (BFRs). Gaseous and particle-bound BFRs were measured in the atmosphere at e-waste and rural sites in southern China during 2007–2008. The annual average concentrations in the air were 3260 ± 3370 and 219 ± 192 pg/m3 for polybrominated diphenyl ethers (PBDEs) and were 546 ± 547 and 165 ± 144 pg/m3 for non-PBDE BFRs at the e-waste and rural sites, respectively. PBDEs had unusually high relative concentrations of di- and tribrominated congeners at the e-waste site. The Clausius–Clapeyron (CC) plots showed that the gaseous concentrations of less brominated BFRs (di- through hexa-BFRs) were strongly controlled by temperature-driven evaporation from contaminated surfaces (e.g., e-waste, soils, and recycled e-waste remains) except for winter. However, weak temperature dependence at the rural site suggests that regional or long-range atmospheric transport was largely responsible for the air concentrations. Gas-particle partitioning (K P) of PBDEs correlated well with the subcooled liquid vapor pressure (P L o) for most sampling events. The varied slopes of log K P versus log P L o plots for the e-waste site (−0.59 to −1.29) indicated an influence of ambient temperature and atmospheric particle properties on the partitioning behavior of BFRs. The flat slopes (−0.23 to −0.80) for the rural site implied an absorption-dominant partitioning. This paper suggests that e-waste recycling in Asian low-latitude regions is a significant source of less brominated BFRs and has important implications for their global transport from warm to colder climates.