标题: Generation of Fe-IV=O and its Contribution to Fenton-Like Reactions on a Single-Atom Iron-N-C Catalyst

作者: Cheng, C (Cheng, Cheng); Ren, W (Ren, Wei); Miao, F (Miao, Fei); Chen, XT (Chen, Xuantong); Chen, XX (Chen, Xiaoxiao); Zhang, H (Zhang, Hui)

来源出版物: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION DOI: 10.1002/anie.202218510 提前访问日期: JAN 2023

摘要: Generating Fe-IV=O on single-atom catalysts by Fenton-like reaction has been established for water treatment; however, the Fe-IV=O generation pathway and oxidation behavior remain obscure. Employing an Fe-N-C catalyst with a typical Fe-N-4 moiety to activate peroxymonosulfate (PMS), we demonstrate that generating Fe-IV=O is mediated by an Fe-N-C-PMS* complex-a well-recognized nonradical species for induction of electron-transfer oxidation-and we determined that adjacent Fe sites with a specific Fe-1-Fe-1 distance are required. After the Fe atoms with an Fe-1-Fe-1 distance <4 angstrom are PMS-saturated, Fe-N-C-PMS* formed on Fe sites with an Fe-1-Fe-1 distance of 4-5 angstrom can coordinate with the adjacent Fe-II-N-4, forming an inter-complex with enhanced charge transfer to produce Fe-IV=O. Fe-IV=O enables the Fenton-like system to efficiently oxidize various pollutants in a substrate-specific, pH-tolerant, and sustainable manner, where its prominent contribution manifests for pollutants with higher one-electron oxidation potential.

作者关键词: Atomic Distance; Fenton-Like Reactions; High-Valent Iron-Oxo Species; Peroxymonosulfate Activation; Single-Atom Catalysts

地址: [Cheng, Cheng; Miao, Fei; Chen, Xuantong; Chen, Xiaoxiao; Zhang, Hui] Wuhan Univ, Sch Resource & Environm Sci, Dept Environm Sci & Engn, Wuhan 430079, Peoples R China.

[Ren, Wei] Nanchang Hangkong Univ, Key Lab Jiangxi Prov Persistent Pollutants Control, Nanchang 330063, Peoples R China.

通讯作者地址: Zhang, H (通讯作者)，Wuhan Univ, Sch Resource & Environm Sci, Dept Environm Sci & Engn, Wuhan 430079, Peoples R China.

电子邮件地址: eeng@whu.edu.cn

影响因子：16.823