Elucidating the Mechanistic Origin of a Spin State-Dependent FeN_x-C Catalyst toward Organic Contaminant Oxidation via Peroxymonosulfate Activation

Bofan Zhang; Xianquan Li; Kazuhiko Akiyama

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Elucidating the Mechanistic Origin of a Spin State-Dependent FeN_x-C Catalyst toward Organic Contaminant Oxidation via Peroxymonosulfate Activation

机译：Elucidating the Mechanistic Origin of a Spin State-Dependent FeN_x-C Catalyst toward Organic Contaminant Oxidation via Peroxymonosulfate Activation

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摘要

Atomically dispersed metals on nitrogen-doped carbon matrices have attracted extensive interest in the removal of refractory organic pollutants. However, a thorough exploration of the particular structure for each active site and specific effects of these sites still remains elusive. Herein, an Fe-pyridinic N4 structure in a single-atom catalyst (FeN_x-C) was constructed using a facile pyrolysis strategy, and it exhibited superior catalytic activity in peroxymonosulfate (PMS) activation toward organic contaminant oxidation. The various Fe species and relative amounts of each Fe site in the FeN_x-C catalyst were validated using X-ray absorption spectroscopy and ~(57)Fe Mossbauer spectroscopy, which showed critical dependencies on the precursor ratio and calcination temperature. The positive correlations between relative content of high-spin state species (Fe~II and Fe~III) and catalytic performance were found to determine the reactive species generation and electron transfer pathway in the FeN_x-C/PMS system. Moreover, catalytic performance and theoretical calculation results revealed that Fe~II-N4 in the high-spin state (S = 2) tends to activate PMS to form sulfate and hydroxyl radicals via a one-electron transfer process, while the Fe~III-N4 moiety (S = 5/2) is prone to high-valent iron species generation with lower free energy. Benefiting from finely tuned active sites, a single-atom FeN_x-C catalyst achieved favorable applicability in actual wastewater treatment with efficient resistance of the common water matrix. The present work advances the mechanistic understanding of spin state-dependent persulfate activation in single-atom catalysts and provides guidance to design a superior catalyst based on spin state descriptions.

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《Environmental Science & Technology: ES&T》 |2022年第2期|1321-1330|共10页
作者
Bofan Zhang; Xianquan Li; Kazuhiko Akiyama;
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作者单位

Department of Chemistry, Tokyo Metropolitan University, Tokyo 192-0397, Japan;

CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类环境科学、安全科学;
关键词
refractory organic pollutant; PMS activation; single iron atom; spin state; wastewater;

Elucidating the Mechanistic Origin of a Spin State-Dependent FeN_x-C Catalyst toward Organic Contaminant Oxidation via Peroxymonosulfate Activation

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