Strong hetero-interfacial interactions mediated photocatalytic 3-electron oxygen reduction to hydroxyl radicals for wastewater decontamination

In this work, we synthesized perylene-3,4,9,10-tetracarboximide/WO 3 (PDINH/WO 3 ) with strong hetero-interfacial interactions (SHIs) to enhance the three-electron oxygen reduction reaction (3e - ORR) for hydroxyl radicals (•OH) generation toward micropollutants degradation and antibacterial applications. Experimental and density functional theory (DFT) computational results revealed that WO 3 facilitates the 2e - oxygen reduction pathway for H 2 O 2 production, while the organic PDINH component strengthens the adsorption of *H 2 O 2 intermediates, promoting their subsequent 1e - reduction to •OH. The optimized system enabled exceptional •OH production, with excellent tetracycline degradation and robust antibacterial activity, alongside 120 h stability with < 5 % activity loss in continuous-flow wastewater treatment, even under high-salinity, extreme pH, and natural organic matter interference. This work establishes SHIs as a universal design principle for steering 3e - ORR pathways. The findings offer transformative opportunities for energy-efficient environmental remediation, demonstrating exceptional resilience in complex real-world wastewater systems.