期刊
WATER RESEARCH
卷 71, 期 -, 页码 64-73出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.watres.2014.12.047
关键词
Halogenated phenolic compound; Laccase-catalytic oxidation; Tri-metal reduction; Sequential treatment; Detoxification
资金
- National Major Program of Science and Technology for Water Pollution Control and Governance (PR China) [2012ZX07202-005]
- National Natural Science Foundation of China [21207004, 21407138]
- Beijing Natural Science Foundation [8142025]
- China Postdoctoral Science Foundation [2014M550083]
Halogenated phenolic compounds (HPCs) are exerting negative effects on human beings and ecological health. Zero-valence metal reduction can dehalogenate HPCs rapidly but cannot mineralize them. Enzymatic catalysis can oxidize phenolic compounds but fails to dehalogenate efficiently, and sometimes even produces more toxic products. In this study, [Fe vertical bar Ni vertical bar Cu] tri-metallic reduction (TMR) and laccase-catalytic oxidation (LCO) processes were combined to sequentially remove HPCs, including triclosan, tetrabromobisphenol A, and 2-bromo-4-fluorophenol in water. The kinetics, pH and temperature dependences of TMR and LCO were obtained. The detailed TMR, LCO, and TMR-LCO transformation pathways of three HPCs were well described based on the identification of intermediate products and frontier molecular orbitals (FMOs) theory. The results showed that the two-stage process worked synergically: TMR that reductively dehalogenated HPCs followed by LCO that completely removed dehalogenated products. TMR was proven to not only improve biodegradability of HPCs but also reduce the yield of potential carcinogenic by-products. Furthermore, a TMR-LCO flow reactor was assembled and launched for 256 h, during which >95% HPCs and >75% TOC were removed. Meanwhile, monitored by microorganism indicators, 83.2%-92.7% acute toxicity of HPCs was eliminated, and the genotoxicity, produced by LCO, was also avoided by using TMR as pretreatment process. (C) 2015 Elsevier Ltd. All rights reserved.
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