With the gradual phasing out of polybrominated diphenyl ethers (PBDEs), market demands for alternative halogenated flame retardants (HFRs) are increasing. The Laizhou Bay area is the biggest manufacturing base for brominated flame retardants (BFRs) in China, and the Xiaoqing River is the largest and most heavily contaminated river in this region. Water and sediment samples were collected from the headwaters to the estuary of the Xiaoqing River to investigate the distribution and fate of HFRs [i.e., PBDEs, alternative brominated flame retardants (aBFRs) and dechlorane plus (DPs). In the water samples, DPs was the most abundant flame retardant (median: 11.7ng/L), followed by decabromodiphenylethane (DBDPE) (5.92ng/L). In the sediment samples, DBDPE was the predominant flame retardant (39.5ng/g dw), followed by decabromodiphenyl ether (BDE 209) (2.81ng/g dw). The levels of DBDPE exceeded those of BDE 209 in most samples, indicating the overwhelming replacement of BDE 209 by DBDPE in this area. In the river section of this study, point source and atmospheric deposition followed by land runoff were the major factors influencing the distribution of HFRs, whereas in the estuary, riverine discharge, the estuarine maximum turbidity zone (MTZ), and hydrodynamic parameters played more important roles. Manufacturing is a significant source of contamination of the Xiaoqing River basin through atmospheric deposition and wastewater discharge.

a b s t r a c tThe distribution characteristics and potential sources of polybrominated diphenyl ethers (PBDEs) and alternative brominated flame retardants (aBFRs) were investigated in 54 surface sediment samples from four bays (Taozi Bay, Sishili Bay, Dalian Bay, and Jiaozhou Bay) of North China's Yellow Sea. Of the 54 samples studied, 51 were collected from within the four bays and 3 were from rivers emptying into Jiaozhou Bay. Decabromodiphenylethane (DBDPE) was the predominant flame retardant found, and concentration ranged from 0.16 to 39.7 ng g À1 dw and 1.13e49.9 ng g À1 dw in coastal and riverine sediments, respectively; these levels were followed by those of BDE 209, and its concentrations ranged from n.d. to 10.2 ng g À1 dw and 0.05e7.82 ng g À1 dw in coastal and riverine sediments, respectively. The levels of DBDPE exceeded those of decabromodiphenyl ether (BDE 209) in most of the samples in the study region, whereas the ratio of DBDPE/BDE 209 varied among the four bays. This is indicative of different usage patterns of brominated flame retardants (BFRs) and also different hydrodynamic conditions among these bay areas. The spatial distribution and composition profile analysis indicated that BFRs in Jiaozhou Bay and Dalian Bay were mainly from local sources, whereas transport from Laizhou Bay by coastal currents was the major source of BFRs in Taozi Bay and Sishili Bay. Both the P PBDEs and P aBFRs (sum of pentabromotoluene (PBT), 2,3-diphenylpropyl-2,4,6-tribromophenyl ether (DPTE), pentabromoethylbenzene (PBEB), and hexabromobenzene (HBB)) were at low concentrations in all the sediments. This is probably attributable to a combination of factors such as low regional usage of these products, atmospheric deposition patterns, coastal currents transportation patterns, and degradation processes for higher BDE congeners. This paper is the first study that has investigated the levels of DBDPE in the coastal sediments of China's Yellow Sea.

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