| Shanghai is the center for industrial and economic development in China. Recently, all kinds of PBDEs-treated products are used frequently because of rapid increase in population and industry. Available studies have shown that PBDEs are ubiquitous contaminant in different environment mediums from Shanghai. However, little information was available on the emission sources, spatial distribution pattern and temporal trend of PBDEs in Shanghai.In this study, reliable analysis and instrument method for qualitative and quantitative determination of PBDEs in different environment mediums were built up. Roadside soils were collected from different regions in Shanghai to systematically investigate the concentrations, congeners profiles, PBDEs diffusion patterns from urban areas to suburban areas and potential sources in Shanghai including residential districts, industrial park, decoration material markets, incinerators, landfill and waste electrical and electronic equipment (WEEE) recycling and disposal sites. Sewage sludge samples were collected from13wastewater treatment plants in Shanghai to investigate levels, congeners profiles, temporal trend, fate and ecological risks. Meanwhile, soils, vegetation leaves, leachates and workshop-floor dust samples were collected to understand PBDEs behavior, fate and pollution degree in WEEE recycling and disposal sites and landfill, which are main point pollution sources of PBDEs in Shanghai. Finally, the concentrations of PBDEs in migratory waterbirds on the East Asian-Australasian flyway and residential eurasian tree sparrow (Passer montanus) gave an indication of the general exposure and uses of these compounds in Asian-Pacific region and Shanghai, respectively. The major findings are listed below:Sum-PBDEs concentrations in roadside soils from urban and suburban areas ranged14.5-64.2ng/g dw and0.875～68.2ng/g dw. Landfill and WWWE recycling and disposal sites in Shanghai were main emission sources of PBDEs, while ambient environment around industrial parks, residential neighborhoods, incinerators and decoration material markets was less influenced by PBDEs. Different regions in Shanghai had its local sources of PBDEs. Based on the geographic and spatial distribution of soils in Shanghai, the main PBDEs sources in suburban areas in Shanghai were landfill site and industrial parks, but the main ones in urban areas were complicated, including large residential neighborhood, industrial parks and WEEE recycling and disposal sites. The inventory of PBDEs in soil was estimated to be16.4ton and was lower than the result from Pearl River Delta, which was related with the urbanization level, industrialization level and WEEE recycling and disposal activities.BDE47,99,100levels in sewage sludge samples from Shanghai were much lower than those in North America and European. BDE209concentration was higher than those from most of the world, followed by samples from U.S.A and Spain, which indicated that sludge acted as the final sink of PBDEs released from Shanghai. Meanwhile, massive usage of BDE209showed that urbanization and industrial levels in Shanghai were at the high end of global range. No temporal trend was observed in PBDEs concentration in sludge from2010to2012. The inventory of∑7PBDEs and BDE209in sludge in2010was estimated to be8.7kg and1.50ton, respectively. High BDE209concentration in sludge from Shanghai posed possible ecological risk applied to agricultural land and landfill treatment.Sum-PBDEs concentrations in4workshop-floor dust samples from one WWWE recycling site in Pudong New Area followed the order below:coarse crushing workshop for waste printed circuit boards (108177ng/g)> disassembly workshop for waste TVs (95446ng/g)>20m away from disassembly line (21121ng/g)> fine crushing workshop for waste printed circuit boards (17278ng/g). Sum-PBDEs concentration in1floor dust sample from exchange shops of waste home appliances on Quyang Road reached to43064ng/g. Meanwhile, sum-PBDEs concentrations in two soil samples from second hand stores of home on Qiujiang Road were9times higher than those from industrial park and urban districts in Shanghai, which indicated that the pollution levels in second hand business were greater than those in industrial park and urban districts. The open dismantling behaviors in exchange shops and second hand stores were conducive to diffusion of PBDEs.Topsoil and vegetation leaves samples from Shanghai Laogang Municipal Landfill (SLML) proved PBDEs leakage from landfill site and vegetation uptake. PBDEs concentration in leachate samples obtained from SLML were lower than those from USA, Canada and South Africa landfill sites is not surprising since the leachates from SLML were treated by A2/O (Anaerobic-Anoxic-Oxic) and reed wetland process. PBDEs tendency of historical evolution in aged refuse from1989to2002found exponential increase in BDE209concentration, which suggested the increasing market demands for deca-BDE mixture after1990in China. The inventory of PBDEs in SLML was28.7ton, which was related to the landfill amount of waste home appliances. SLML can be considered as one main recipient of PBDEs, receiving inputs predominantly from the PBDEs-containing waste, but also one main emission source of PBDEs to ambient environment.Compared with flyways around the world, migratory waterbirds on the East Asian-Australasian fly way exhibited lower PBDEs burdens than those reported on Black Sea-Mediterranean flyway in Europe and Pacific, Atlantic, Mississippi flyway in North America. Stable nitrogen and carbon isotopes and stomach content analysis indicated shorebirds and ducks had the same dietary composition, but showed different preference to bivalves, gastropods and crustaceans for shorebirds and aquatic plant material for ducks. Migratory species had inherent migratory routes and thus had exposure to PBDEs during their stay in breeding grounds, stopover sites and wintering grounds with high use of different commercial PBDEs mixtures. Higher percentage of BDE209in ducks than shorebirds suggested that breeding ranges and wintering grounds of ducks comprise wetlands in inland and coastal China and Korea where BDE209pollution was serious in Asian-Pacific region. Our findings reveal the influence of migratory behavior on PBDEs distribution and transportation of PBDEs by migratory waterbirds on the East Asian-Australasian flyway.The geographic distribution of sum-PBDEs concentrations in residential eurasian tree sparrow (Parus montanus) samples from different regions in Shanghai followed the order below:landfill> urban> industrial parks> suburban> rural> remote, which indicated that landfill and industrial parks were main emission sources of PBDEs, and also pollution levels in landfill were greater than those in industrial parks. BDE209was the main congener in eurasian tree sparrow samples in Shanghai. Compared with the results from Beijing and Guangdong province, PBDEs levels in eurasian tree sparrow samples in Shanghai were at lower level. However, great attention should be paid to high concentrations samples in landfill, industrial parks and urban areas. |
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