1. Coordination Number Dependent Catalytic Activity of Single‐Atom Cobalt Catalysts for Fenton‐Like Reaction.
- Author
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Liang, Xiaoying, Wang, Di, Zhao, Zhiyu, Li, Tong, Gao, Yaowen, and Hu, Chun
- Subjects
COBALT catalysts ,CATALYTIC activity ,ELECTRON density ,HABER-Weiss reaction ,ENVIRONMENTAL remediation ,REACTIVE oxygen species ,ATOMS - Abstract
Single‐atom catalysts (SACs) are widely investigated in Fenton‐like reactions for environmental remediation, wherein their catalytic performance can be further improved by coordination structure modulation, but the relevant report is rare. Herein, a series of atomically dispersed cobalt catalysts with diverse coordination numbers (denoted as CoNx, x represents nitrogen coordination number) are synthesized and their peroxymonosulfate (PMS) conversion performance is explored. The catalytic specific activity of CoNx is found to be dependent on coordination number of single atomic Co sites, where the lowest‐coordinated CoN2 catalyst exhibits the highest specific activity in PMS activation, followed by under‐coordinated CoN3 and normal CoN4. Experimental and theoretical results reveal that reducing coordination number can increase the electron density of single Co atom in CoNx, which governs the Fenton‐like performance of CoNx catalysts. Specifically, the entire Co–pyridinic NC motif serves as active centers for PMS conversion, where the single Co atom, and pyridinic N‐bonded C atoms along with nitrogen vacancy neighboring the unsaturated Co–pyridinic N2 moiety account for PMS reduction and oxidation toward radical and singlet oxygen (1O2) generation, respectively. These findings provide a useful avenue to coordination number regulation of SACs for environmental applications. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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