Affiliation:
1. CAS Key Laboratory of Urban Pollutant Conversion Department of Environmental Science and Engineering University of Science & Technology of China Hefei Anhui 230026 P. R. China
2. Department of Colloid Chemistry Max Planck Institute of Colloids and Interfaces 14476 Potsdam Germany
3. CAS Center for Excellence in Nanoscience National Synchrotron Radiation Laboratory University of Science & Technology of China Hefei Anhui 230029 P. R. China
Abstract
AbstractHigh‐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 OH and OO bonds as well as efficient electron transfer. However, the high dissociation energy of OH 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 (CoB1N3) is established to offer a strong local electric field, upon which the cleavage of OH bond is thermodynamically favored via a promoted coupled electron–proton transfer process, which serves an essential step to further allow OO 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.
Funder
National Natural Science Foundation of China
Subject
Mechanical Engineering,Mechanics of Materials,General Materials Science
Cited by
21 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献