Carbon nitride with a tailored electronic structure toward peroxymonosulfate activation: A direct electron transfer mechanism for organic pollutant degradation

The persulfate-based nonradical reaction process has gained increasing attention in removing organic contaminants, and the process dramatically needs affordable, robust, high-performance heterogeneous catalysts. Herein, dimethyl formamide (DMF) incorporated graphitic carbon nitride (DCN) was synthesized. The molecular engineering of the heptazine unit in DCN improves the electron mobility, strengthens the built-in electric field, and provides abundant active sites, thus enabling DCN to efficiently activate PMS for organic degradation, with 100% removal of BPA within 12 min. The investigation of the reactive species and electrochemical properties confirmed the direct electron transfer in the PMS activation for organic degradation over DCN. More importantly, DCN can be used as a membrane catalyst in a flowing catalytic unit, enabling continuous water purification and catalyst regeneration. This work provides novel guidance for metal-free catalyst design and profound insights into the persulfate-based heterogeneous catalytic oxidation process for water decontamination technology.