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https://hdl.handle.net/2440/138798
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dc.contributor.author | Lin, J. | - |
dc.contributor.author | Jiang, L. | - |
dc.contributor.author | Tian, W. | - |
dc.contributor.author | Yang, Y. | - |
dc.contributor.author | Duan, X. | - |
dc.contributor.author | Jiao, Y. | - |
dc.contributor.author | Zhang, H. | - |
dc.contributor.author | Wang, S. | - |
dc.date.issued | 2023 | - |
dc.identifier.citation | Journal of Materials Chemistry A, 2023; 11(25):13653-13664 | - |
dc.identifier.issn | 2050-7488 | - |
dc.identifier.issn | 2050-7496 | - |
dc.identifier.uri | https://hdl.handle.net/2440/138798 | - |
dc.description | First published 18 May 2023 | - |
dc.description.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. | - |
dc.description.statementofresponsibility | Jingkai Lin, Lin Jiang, Wenjie Tian, Yangyang Yang, Xiaoguang Duan, Yan Jiao, Huayang Zhang, and Shaobin Wang | - |
dc.language.iso | en | - |
dc.publisher | Royal Society of Chemistry (RSC) | - |
dc.rights | © The Royal Society of Chemistry 2023 | - |
dc.source.uri | http://dx.doi.org/10.1039/d3ta01926h | - |
dc.title | The structure-dependent mechanism of single-atom cobalt on macroporous carbon nitride in (photo-)Fenton-like reactions | - |
dc.type | Journal article | - |
dc.identifier.doi | 10.1039/d3ta01926h | - |
dc.relation.grant | http://purl.org/au-research/grants/arc/DP200103206 | - |
dc.relation.grant | http://purl.org/au-research/grants/arc/DE220101074 | - |
pubs.publication-status | Published | - |
dc.identifier.orcid | Lin, J. [0000-0001-6409-0146] | - |
dc.identifier.orcid | Tian, W. [0000-0002-9896-1154] | - |
dc.identifier.orcid | Duan, X. [0000-0001-9635-5807] | - |
dc.identifier.orcid | Jiao, Y. [0000-0003-1329-4290] | - |
dc.identifier.orcid | Wang, S. [0000-0002-1751-9162] | - |
Appears in Collections: | Chemical Engineering publications |
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