Formation of 1,3,8-tribromodibenzo-p-dioxin and 2,4,6,8-tetrabromodibenzofuran in the oxidation of synthetic hydroxylated polybrominated diphenyl ethers by iron and manganese oxides under dry conditions
Formation of 1,3,8-tribromodibenzo-p-dioxin and 2,4,6,8-tetrabromodibenzofuran in the oxidation of synthetic hydroxylated polybrominated diphenyl ethers by iron and manganese oxides under dry conditions
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干燥条件下铁氧化物和锰氧化物氧化合成羟基化多溴二苯醚时形成 1,3,8-三溴二苯并-对二恶英和 2,4,6,8-四溴二苯并呋喃
DOI：
10.1007/s11356-018-2980-4
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发表时间：
2018-08
影响因子：
5.8
通讯作者：
Weirong Zhao
中科院分区：
文献类型：
--
作者：
Jiafeng Ding;Gaoyuan Long;Yang Luo;Runze Sun;Mengxia Chen;Yajun Li;Yanfang Zhou;Xinhua Xu;Weirong Zhao
羟基化多溴联苯醚（OH-PBDEs）是一种普遍存在的高毒性新兴内分泌干扰物，存在于地表和地下土壤和粘土沉积物中。严重的是，它们很容易在光化学过程和焚烧过程中转化为毒性更强的二恶英（PBDD/Fs），但PBDD/Fs的自发形成很少有报道。研究了铁锰氧化物（针铁矿和MnOx）在2′-OH-BDE-68和2,2′-diOH-BB-80的氧化作用下生成1,3,8-三溴二苯并对二恶英（1,3,8- trbdd）和2,4,6,8-四溴二苯并呋喃（2,4,6,8- tebdf）。针铁矿在8 d内对1,3,8- trbdd和2,4,6,8- tebdf的转化率分别为0.09 μmol/kg（2.33%）和0.17 μmol/kg (4.15%)， MnOxin在4 d内的转化率分别为0.15 μmol/kg（3.77%）和0.23 μmol/kg（5.74%）。然而，PBDD/Fs的形成可能是通过Smiles重排和溴消除过程进行的，水的存在极大地抑制了PBDD/Fs的形成。针铁矿和微量氧化物对OH-PBDEs的转化伴随着Fe和Mn离子的释放，并提出了反应产物形成的可能途径。鉴于环境中OH-PBDEs和金属氧化物的普遍存在，针铁矿和mnox介导的OH-PBDEs氧化可能是PBDD/Fs形成的非生物途径。
Hydroxylated polybrominated diphenyl ethers (OH-PBDEs) are ubiquitous and highly toxic emerging endocrine disruptors found in surface and subsurface soils and clay deposits. Seriously, they could be easily transformed to the more toxic dioxins (PBDD/Fs) in photochemical processes and incineration, but the spontaneous formation of PBDD/Fs has rarely been reported. This study focused on the formation of 1,3,8-tribromodibenzo-p-dioxin (1,3,8-TrBDD) and 2,4,6,8-tetrabromodibenzofuran (2,4,6,8-TeBDF) from 2′-OH-BDE-68 and 2,2′-diOH-BB-80 under the oxidization of iron and manganese oxides (goethite and MnOx). Approximately 0.09 μmol/kg (2.33%) and 0.17 μmol/kg (4.15%) were transformed to 1,3,8-TrBDD and 2,4,6,8-TeBDF by goethite in 8 days and a higher conversion 0.15 μmol/kg (3.77%) and 0.23 μmol/kg (5.74%) were observed for MnOxin 4 days. However, the formation of PBDD/Fs, probably proceeding via Smiles rearrangements and bromine elimination processes, was greatly inhibited by the presence of water. Transformation of OH-PBDEs by goethite and MnOxwas accompanied by release of Fe and Mn ions and the possible pathways for the formation of reaction products were proposed. In view of the ubiquity of OH-PBDEs and metal oxides in the environment, oxidation of OH-PBDEs mediated by goethite and MnOxis likely an abiotic route for the formation of PBDD/Fs.
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