Molecular oxygen cascade reduction to •OH via coplanar dual-electrocatalytic zone achieving electrolyte-free water purification
摘要
As a promising approach for treating emerging organic pollutants in water, the conventional Fenton process faces an inherent limitation: its reliance on the continuous addition of Fenton reagents and supporting electrolytes, which raises operational costs, risks secondary pollution and complicates safe handling. Here, to overcome these challenges, we propose a ‘spatial–temporal dynamic dual-electrocatalytic cascade’ strategy and design an innovative coplanar dual-electrocatalytic zone-structured electrode—integrated with a membrane electrode assembly—that forms a compact reaction system. This system enables the continuous in situ cascading transformation of O2 → H2O2 → •OH without supporting electrolytes and achieves efficient degradation of organic pollutants. Experimental results confirm that the system exhibits exceptional degradation performance for four categories of typical recalcitrant organic pollutants, achieving removal rates exceeding 98%. In terms of energy consumption, it is reduced by ~69.3% compared with the conventional dual-cathode system. Furthermore, this system is effective in five distinct water matrices, and it can achieve effective reduction of total organic carbon in real chemical pharmaceutical wastewater without requiring complex pretreatment. As a reagent-free and electrolyte-free alternative, this integrated coplanar dual-electrocatalytic zone coupled system overcomes the constraints of traditional electro-Fenton technology. It enables decentralized treatment of low-conductivity water matrices, and its broad applicability lays a solid foundation for advancing the practical implementation of electrochemical water treatment technology in complex wastewater remediation.