Asymmetrically Coordinated CoB1 N3 Moieties for Selective Generation of High-Valence Co-Oxo Species via Coupled Electron-Proton Transfer in Fenton-like Reactions

Asymmetrically Coordinated CoB1 N3 Moieties for Selective Generation of High-Valence Co-Oxo Species via Coupled Electron-Proton Transfer in Fenton-like Reactions

© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 23 vom: 16. Juni, Seite e2209552
1. Verfasser: Song, Junsheng (VerfasserIn)
Weitere Verfasser: Hou, Nannan, Liu, Xiaocheng, Antonietti, Markus, Zhang, Pengjun, Ding, Rongrong, Song, Li, Wang, Yang, Mu, Yang
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2023
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article Fenton-like reactions asymmetric coordination coupled electron-proton transfers high-valence metal species single-atom catalysts
Beschreibung
Zusammenfassung:© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.
High-valence metal species generated in peroxymonosulfate (PMS)-based Fenton-like processes are promising candidates for selective degradation of contaminants in water, the formation of which necessitates the cleavage of OH and OO bonds as well as efficient electron transfer. However, the high dissociation energy of OH bond makes its cleavage quite challenging, largely hampering the selective generation of reactive oxygen species. Herein, an asymmetrical configuration characterized by a single cobalt atom coordinated with boron and nitrogen (CoB1 N3 ) is established to offer a strong local electric field, upon which the cleavage of OH bond is thermodynamically favored via a promoted coupled electron-proton transfer process, which serves an essential step to further allow OO bond cleavage and efficient electron transfer. Accordingly, the selective formation of Co(IV)O in a single-atom Co/PMS system enables highly efficient removal performance toward various organic pollutants. The proposed strategy also holds true in other heteroatom doping systems to configure asymmetric coordination, thus paving alternative pathways for specific reactive species conversion by rationalized design of catalysts at atomic level toward environmental applications and more
Beschreibung:Date Completed 08.06.2023
Date Revised 08.06.2023
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202209552