Fe(III)-Doped g-C3N4 Mediated Peroxymonosulfate Activation for Selective Degradation of Phenolic Compounds via High-Valent Iron-Oxo Species

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State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, P. R. China
Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing 210023, P. R. China
*Tel: +86-25-8968-0390; e-mail: [email protected] (B.P.).
Cite this: Environ. Sci. Technol. 2018, 52, 4, 2197–2205
Publication Date (Web):January 26, 2018
https://doi.org/10.1021/acs.est.7b05563
Copyright © 2018 American Chemical Society
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Abstract

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 (1O2) 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 (≡FeV═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 ≡FeV═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 ≡FeV═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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