Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 9, Pages 4588-4593Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202014472
Keywords
advanced oxidation processes; CoN2+2 sites; peroxymonosulfate activation; reactive oxygen species; singlet oxygen
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Funding
- National Natural Science Foundation of China [21722702, 22076082, 22006029]
- Tianjin Commission of Science and Technology as key technologies RD projects [19YFZCSF00740, 20YFZCSN01070]
- National Key Basic Research Program of China [2017YFA0403402]
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This study demonstrates a strategy to regulate the generation of reactive oxygen species by atomically dispersed cobalt anchored on nitrogen-doped carbon, with singlet oxygen being the predominant reactive oxygen species. The generated singlet oxygen is capable of degrading various organic pollutants efficiently across a broad pH range, providing new theoretical support for the singlet oxygen generation mechanism in peroxymonosulfate activation.
Single-atom CoN4 active sites have demonstrated excellent efficiency in peroxymonosulfate activation. However, the identification of CoN4 active sites and the detailed singlet oxygen generation mechanism in peroxymonosulfate activation remains ambiguous. We demonstrate a strategy to regulate the generation of reactive oxygen species by atomically dispersed cobalt anchored on nitrogen-doped carbon. As indicated by experiment and DFT calculations, CoN2+2 was the active site and singlet oxygen was the predominant reactive oxygen species with a proportion of 98.89 %. Spontaneous dissociation of adsorbed peroxymonosulfate on the CoN2+2 active sites was energetically unfavorable because of the weakly positive Co atoms and CoN2+2 coordination, which directed PMS oxidation by a non-radical pathway and with simultaneous singlet oxygen generation. The generated singlet oxygen degraded several organic pollutants with high efficiency across a broad pH range.
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