Cobalt Single‐Atom‐Bonded Covalent Heptazine Framework Selectively Generates Nonradicals in Fenton‐Like Catalysis for Rapidly Purifying Organic Wastewater

ABSTRACT Engineering the coordination architecture of cobalt single‐atom catalysts (Co‐SACs) represents a promising strategy to activate peroxymonosulfate (PMS) for sewage purification. In this study, Co single atoms were bonded to a 2,2′‐bipyridine‐bridged covalent heptazine framework (Bpy‐CHF). The obtained Bpy‐CHF‐Co 0.6 catalyst contained highly homogeneous Co‐N active sites and succeeded in achieving efficient generation of 1 O 2 . Density functional theory (DFT) calculations showed that the Co sites tended to adsorb the terminal oxygen of PMS, which facilitated the oxidation of PMS to generate SO 5 •− and achieved efficient generation of 1 O 2 , accompanied by the formation of Co(IV)=O. Furthermore, the catalyst demonstrated durability against a variety of environmental conditions, indicating potential for practical applications, and we fixed it on a PVDF microfiltration membrane to establish a continuous flow system. This study proposes innovative concepts for the advancement of catalysts that facilitate efficient and selective degradation of pollutants, as well as new insights into the selective generation of 1 O 2 and the formation of Co(IV)=O.