Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 52, Issue 4, Pages 2197-2205Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.7b05563
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Funding
- Natural Science Foundation of China [51578280/51761165011]
- National Key Research and Development Program of China [2016YFA0203104]
- Natural Science Foundation of Jiangsu Province [BK20160653]
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Herein, we proposed a new peroxymonosulfate (PMS) activation system employing the Fe(III) doped g-C3N4 (CNF) as catalyst. Quite different from traditional sulfate radical-based advanced oxidation processes (SR-AOPs), the PMS/CNF system was capable of selectively degrading phenolic compounds (e.g., p-chlorophenol, 4-CP) in a wide pH range (3-9) via nonradical pathway. The generated singlet oxygen (O-1(2)) in the PMS/CNF3 (3.46 wt % Fe) system played negligible role in removing 4-CP, and high-valent iron-oxo species fixated in the nitrogen pots of g-C3N4 ( Fe-V= O) was proposed as the dominant reactive species by using dimethyl sulfoxide as a probe compound. The mechanism was hypothesized that PMS was first bound to the Fe(III)-N moieties to generate Fe-V=O, which effectively reacted with 4-CP via electron transfer. GC-MS analysis indicated that 4-chlorocatechol and 1,4-benzoquinone were the major intermediates, which could be further degraded to carboxylates. The kinetic results suggested that the formation of Fe-V=O was proportional to the dosages of PMS and CNF3 under the experimental conditions. Also, the PMS/CNF3 system exhibited satisfactory removal of 4-CP in the presence of inorganic anions and natural organic matters. We believe that this study will provide a new routine for effective PMS activation by heterogeneous iron-complexed catalysts to efficiently degrade organic contaminants via nonradical pathway.
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