期刊
WATER RESEARCH
卷 143, 期 -, 页码 176-187出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.watres.2018.06.038
关键词
Persulfate activation; Nitrogen doping; Carbonaceous materials; 2,4,4 '-HBP; Reaction mechanisms
资金
- National Natural Science Foundation of China [21607073, 21577063]
- Natural Science Foundation of Jiangsu Province [BK20160651]
- National Key Program for the Introduction of Renowned Overseas Professors of P.R. China [MS2017NJDX017]
In this work, we systematically investigated the persulfate (PS) activation potential of a series of nitrogen doped carbonaceous materials for the degradation of 2,4,4'-trihydroxybenzophenone (2,4,4'-HBP), an additive in polyvinyl acetate films and personal care products. Nitrogen originating from urea, NH4NO3, indole and polyaniline was doped into carbonaceous materials, including hydroxylated multi-walled carbon nanotubes (CNT-OH), large-inner thin-walled carboxylated carbon nanotubes (CNT-COOH) and graphite oxide (GO), to examine the catalytic effect. The NH4NO3-CNT-OH catalyst, which showed the best catalytic performance in 2,4,4'-HBP removal, was characterized by SEM, TEM, FT-IR, Raman, BET surface area, XRD and XPS, and pyrrolic nitrogen was found to play a highly important role in the activation of PS. Under the conditions of [2,4,4'-HBP](0): [PS](0) = 1: 500, T = 25 degrees C, pH(0) = 7.0, concentration of catalyst = 100 mg L-1, 43.48 mu M 2,4,4'-HBP was completely removed in 2 h. According to electron paramagnetic resonance (EPR) spectra and radical quenching experiments, hydroxyl and sulfate radicals on the surface of the catalyst contributed to the substrate oxidation. Cleavage of C-C bridge bond, hydroxylation and polymerization were mainly involved in the oxidation process, leading to the formation of 10 intermediates (e.g., dimers), as detected by the MS/MS spectra. To the best of our knowledge, this report is the first to describe the transformation mechanism of 2,4,4'-HBP in nitrogen doped carbonaceous materials catalyzed PS system. (C) 2018 Elsevier Ltd. All rights reserved.
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