Dynamic in-situ reconstruction of active site circulators for photo-Fenton-like reactions

Abstract

Developing efficient and stable heterogeneous catalysts for the continuous activation of oxidants is crucial to mitigating the global water resource crisis. Guided by computational predictions, this research achieved this goal through the synthesis of a modified graphitic carbon nitride with enhanced catalytic activity and stability. Its intrinsic activity was further amplified by dynamic in-situ reconstruction using the I⁻/I₃⁻ redox mediator system during photoreactions. Impressively, this reconstructed catalyst demonstrated the capability for at least 30 regeneration cycles while maintaining high purification efficacy. The mechanism underlying the in-situ reconstruction of active sites for periodate functionalization was elucidated through theoretical calculations, coupled with semi-in-situ X-ray photoelectron spectroscopy (XPS) and electrochemical analyses. The system’s capacity to detoxify recalcitrant pollutants was demonstrated through successful Escherichia coli cultivation and Zebrafish embryo experiments. The economic feasibility and environmental impacts are quantitatively assessed by the Electrical Energy per Order (EE/O) metric and Life Cycle Assessment (LCA), confirming the system’s scalability and applicability in real-world scenarios. This dual-site constrained interlayer insertion, and controllable in-situ catalyst reconstruction achieve durable robustness of the photocatalyst, paving the way for the development of sustainable catalytic water purification technologies.