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Activation of peroxymonosulfate via mediated electron transfer mechanism on single-atom Fe catalyst for effective organic pollutants removal

Cheap and abundant Fe based catalysts in advanced oxidation progresses (AOPs) usually exhibit radicals or high-valent Fe species (HV-Fe) dominated activation mechanism. In this contribution, the atomically dispersed Fe on g-C3N4 (SAFe-CN) was fabricated for peroxymonosulfate (PMS) activation to degr...

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Published in:Applied catalysis. B, Environmental Environmental, 2021-12, Vol.299, p.120714, Article 120714
Main Authors: Duan, Pijun, Pan, Jingwen, Du, Weiyan, Yue, Qinyan, Gao, Baoyu, Xu, Xing
Format: Article
Language:English
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Summary:Cheap and abundant Fe based catalysts in advanced oxidation progresses (AOPs) usually exhibit radicals or high-valent Fe species (HV-Fe) dominated activation mechanism. In this contribution, the atomically dispersed Fe on g-C3N4 (SAFe-CN) was fabricated for peroxymonosulfate (PMS) activation to degrade o-phenylphenol (OPP). OPP removal was not impeded by common radical scavengers, indicating the absence of SO4•− and •OH. The involvement of 1O2 and HV–Fe was excluded and the mediated electron transfer was finally identified as the dominated mechanism. Atomically dispersed Fe sites in SAFe-CN were verified as active sites for reacting with OO bond of PMS and ulteriorly electron shuttling in pollutants degradation. A water treatment filter was fabricated using SAFe-CN and it remained 100% of OPP removal after 100 h of operation. These results provide new insights into the mechanism of mediated electron transfer as well as potential application of non-radical dominated process at device level. [Display omitted] Peroxymonosulfate was activated on atomically dispersed Fe on g-C3N4 for o-phenylphenol removal via mediated electron transfer mechanism. •PMS was activated on SAFe-CN via mediated electron transfer mechanism.•SAFe-CN/PMS system exhibited outstanding salt tolerance and more efficient utilization of PMS.•Single-atom Fe served as the active sites for PMS adsorption and activation.•SAFe-CN coated water treatment filter exhibited 100% pollutants removal after 100 h of operation.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2021.120714