Almost 100 % Peroxymonosulfate Conversion to Singlet Oxygen on Single‐Atom CoN 2+2 Sites

作者：Xueyue Mi, Pengfei Wang, Shizhe Xu, Lina Su, Hui Zhong, Haitao Wang, Yi Li, Sihui Zhan · 发表于：Angewandte Chemie International Edition · 年份：2020 · DOI：10.1002/anie.202014472 · 被引用次数：687 · 研究领域：Advanced oxidation water treatment、Environmental remediation with nanomaterials、Industrial Gas Emission Control

Abstract 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 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, CoN 2+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 CoN 2+2 active sites was energetically unfavorable because of the weakly positive Co atoms and CoN 2+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.