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发布时间：2019-03-09

论文类型：期刊论文

发表时间：2015-08-04

发表刊物：ENVIRONMENTAL SCIENCE & TECHNOLOGY

收录刊物：Scopus、ISTIC、PKU、PubMed、EI、SCIE

卷号：49

期号：15

页面范围：9092-9099

ISSN号：0013-936X

摘要：Hydroxylated polybrominated diphenyl ethers (OH-PBDEs) are of great concern due to their higher toxicity compared to PBDEs. However, the abiologic process whereby PBDEs are converted to OH-PBDEs in the aquatic environment is not well understood. To explore the possibility of OH-PBDEs photoformation in natural water, the photohydroxylation of BDE-47 has been investigated in aqueous Fe(III) and/or fulvic acid (FA) solutions and in natural lake water under simulated solar light irradiation. The results showed that 6-0H-BDE-47 and 2'-OH-BDE-68 were generated from BDE47 under these conditions. Based on the identification of derivatives and reactive radicals, OH-PBDEs formation can be ascribed to an addition reaction of ortho-tetra-BDE radical and hydroxyl radical ((OH)-O-center dot), with or without a subsequent Smiles rearrangement reaction. Since the ortho-tetra-BDE radical could be readily produced by the photolysis of BDE-47, even in pure water, (OH)-O-center dot production was considered as critical for the photoformation of OH-PBDEs. Thus, it is reasonable to deduce that the photoreactive components (F4111), FA) in aqueous solution played an important role through influencing (OH)-O-center dot generation. Although the yields of OH-PBDEs did not increase regularly with increasing concentration of these photoreactive components in solution, this study suggests a possible abiotic origin of OH-PBDEs formation in the aquatic environment.