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Asymmetrically Coordinated CoB 1 N 3 Moieties for Selective Generation of High-Valence Co-Oxo Species via Coupled Electron-Proton Transfer in Fenton-like Reactions.

Authors :
Song J
Hou N
Liu X
Antonietti M
Zhang P
Ding R
Song L
Wang Y
Mu Y
Source :
Advanced materials (Deerfield Beach, Fla.) [Adv Mater] 2023 Jun; Vol. 35 (23), pp. e2209552. Date of Electronic Publication: 2023 Apr 27.
Publication Year :
2023

Abstract

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 (CoB <subscript>1</subscript> N <subscript>3</subscript> ) 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.<br /> (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Details

Language :
English
ISSN :
1521-4095
Volume :
35
Issue :
23
Database :
MEDLINE
Journal :
Advanced materials (Deerfield Beach, Fla.)
Publication Type :
Academic Journal
Accession number :
36932043
Full Text :
https://doi.org/10.1002/adma.202209552