N-coordinated single cobalt atoms catalyst triggering concerted radical-nonradical process in catalytic ozonation for efficient water decontamination

Heterogeneous catalytic ozonation (HCO) has been developed as a promising technology for wastewater treatment, while traditional radical-based HCO process still suffers from insufficient mineralization of organic pollutants. Herein, we constructed a N-coordinated single cobalt atoms catalyst (CoSAC-N-C) triggering concerted radical-nonradical process in catalytic ozonation for efficient decontamination of pollutants. Experiments and theoretical calculations proved that mediate O in O3 obtained electrons from electron-rich N sites for hydroxyl radical (·OH) production, and the terminal O in O3 was attracted on electron-deficient Co sites for nonradical *O generation by O-O cleavage. The synergistic oxidation of ·OH and *O enabled excellent pollutants mineralization, surpassing most of conventional HCO catalysts. CoSAC-N-C exhibited excellent treatment performance for the coking wastewater in a continuous-flow reactor with COD reducing from 86 mg/L to less than 50 mg/L. This work provided a viable strategy of developing dual-site HCO catalysts to promote concerted radical-nonradical oxidations for wastewater treatment.