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https://hdl.handle.net/2440/138798
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Type: | Journal article |
Title: | The structure-dependent mechanism of single-atom cobalt on macroporous carbon nitride in (photo-)Fenton-like reactions |
Author: | Lin, J. Jiang, L. Tian, W. Yang, Y. Duan, X. Jiao, Y. Zhang, H. Wang, S. |
Citation: | Journal of Materials Chemistry A, 2023; 11(25):13653-13664 |
Publisher: | Royal Society of Chemistry (RSC) |
Issue Date: | 2023 |
ISSN: | 2050-7488 2050-7496 |
Statement of Responsibility: | Jingkai Lin, Lin Jiang, Wenjie Tian, Yangyang Yang, Xiaoguang Duan, Yan Jiao, Huayang Zhang, and Shaobin Wang |
Abstract: | Single-atom catalysts have been believed to be ideal materials for achieving maximum utilization of metal active sites in Fenton-like catalysis for eliminating organic pollutants. However, the relationship between the single-atom structure and catalytic activity remains largely uninvestigated. Herein, a spatial confinement strategy to anchor Co single atoms (0.6–10.2 wt%) on macroporous carbon nitride (MCN) was developed, and the single atom catalysts were tested in peroxymonosulfate activation for (photo-) Fenton-like reactions. Single-atom Co-MCN was discovered to show different molecular structures, and a light-dependent mechanism in Fenton-like catalysis was revealed. Co atoms in Co–N4 configuration present Co–N1+3/Co–N2+2 geometric structures, dependent on a Co load. Co–N1+3 is thermodynamically favorable to form, serving as the main active site. Co–N2+2 possesses an inferior catalytic activity and induces negative effects on the adjacent Co–N1+3 site. Moreover, experimental and theoretical investigations reveal a 100% nonradical reaction pathway that can be photo-switched to a nonradical/radical process by visible light. This work enriches the fundamentals of single-atom catalysis by providing new insights into the atomic metal structure, reaction pathways and mechanisms, and structure–activity relationships in organic degradation. |
Description: | First published 18 May 2023 |
Rights: | © The Royal Society of Chemistry 2023 |
DOI: | 10.1039/d3ta01926h |
Grant ID: | http://purl.org/au-research/grants/arc/DP200103206 http://purl.org/au-research/grants/arc/DE220101074 |
Published version: | http://dx.doi.org/10.1039/d3ta01926h |
Appears in Collections: | Chemical Engineering publications |
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