Almost 100% peroxymonosulfate conversion to singlet oxygen on single-atom CoN2+2 sites.

By Xueyue Mi, Pengfei Wang, Shizhe Xu, Lina Su, Hui Zhong, Haitao Wang, Yi Li, Sihui Zhan. Angewandte Chemie, 2020

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Single-atom CoN 4 active sites have demonstrated excellent efficiency in peroxymonosulfate activation. However, the identification of CoN 4 active sites and the detailed singlet oxygen generation mechanism in peroxymonosulfate activation still remain ambiguous. In this study, we demonstrated a strategy to regulate the generation of reactive oxygen species by atomically dispersed cobalt anchored on nitrogen-doped carbon. As assisted by experimental and DFT calculations, CoN 2+2 was the definite active sites. Singlet oxygen was the absolutely predominant reactive oxygen species that the proportion was 98.89%. Different from the traditional CoN 4 configuration, the CoN 2+2 active sites transformed the pathway of peroxymonosulfate activation and facilitated the singlet oxygen generation. Spontaneous dissociation of adsorbed peroxymonosulfate on Co single atoms was prevented due to the energy barriers caused by weak positive Co atoms and CoN 2+2 coordination, determining PMS oxidation in non-radical pathway and simultaneous singlet oxygen generation. The generated singlet oxygen showed efficient activity for degradation of several organic pollutants in a broad pH range.

Subfields: Biomedical Engineering, Mechanical Engineering, Water Science and Technology

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