Coordination Number Dependent Catalytic Activity of Single‐Atom Cobalt Catalysts for Fenton‐Like Reaction
At a Glance
Section titled “At a Glance”| Metadata | Details |
|---|---|
| Publication Date | 2022-07-07 |
| Journal | Advanced Functional Materials |
| Authors | Xiaoying Liang, Di Wang, Zhiyu Zhao, Tong Li, Yaowen Gao |
| Institutions | Guangzhou University |
| Citations | 262 |
Abstract
Section titled “Abstract”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 CoN x , x represents nitrogen coordination number) are synthesized and their peroxymonosulfate (PMS) conversion performance is explored. The catalytic specific activity of CoN x is found to be dependent on coordination number of single atomic Co sites, where the lowest‐coordinated CoN 2 catalyst exhibits the highest specific activity in PMS activation, followed by under‐coordinated CoN 3 and normal CoN 4 . Experimental and theoretical results reveal that reducing coordination number can increase the electron density of single Co atom in CoN x , which governs the Fenton‐like performance of CoN x 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 N 2 moiety account for PMS reduction and oxidation toward radical and singlet oxygen ( 1 O 2 ) generation, respectively. These findings provide a useful avenue to coordination number regulation of SACs for environmental applications.