期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 54, 期 3, 页码 1573-1582出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.9b05423
关键词
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资金
- National Natural Science Foundation of China [21806073, 21607073, 21577063]
- Natural Science Foundation of Jiangsu Province [BK20160651]
- Fundamental Research Funds for the Central Universities [021114380111]
- Major Science and Technology Program for Water Pollution Control and Treatment of China [2017ZX07301002-03]
Soluble manganese(III), stabilized by ligands as Mn(III)-L complexes, are ubiquitous in natural waters and wastewaters and can potentially serve as both the oxidant and reductant in one-electron transfer reactions with organic contaminants. In this study, the oxidative transformations of 14 phenolic endocrine disrupting chemicals (EDCs) by in situ-formed Mn(III)-L complexes, generated from irradiated water containing Mn(II) and humic acid, were investigated. The pseudo-first-order rate constants (k(obs), h(-1)) of these phenols varied from 1.0 X 10(-4) to 5.9 X 10(-2). A quantitative structure-activity relationship model was developed, which suggests that the electron-donating ability (E-HOMO) of phenolic chemicals was the most important molecular characteristic for the Mn(III)-L-mediated oxidative transformation. Phenol transformation was initiated by the generation of a phenoxyl radical through electron transfer to Mn(III)-L. Subsequent self-coupling reactions between phenoxyl radicals resulted in the formation of self-coupling dimers and trimers. With the addition of simple phenol as a cosubstrate, enhanced transformations of these phenolic EDCs were clearly observed, and cross-coupling products of simple phenol and the substrates were also detected. In addition, a reaction activation energy calculation based on the transition-state theory indicated that the cross-coupling reaction was more likely than the self-coupling reaction to occur in the presence of phenol. This work provides new insights into the environmental fate of phenolic compounds.
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