Interfused Graphene Fiber Membranes Enable Volumetric Electron‐Transfer Advanced Oxidation via Interlayer Site Activation

Electron-transfer-involved persulfate-based advanced oxidation processes (ET-AOPs) are attractive for wastewater treatment because of their high selectivity and environmental robustness. However, ET-AOPs are intrinsically dual-site reaction requiring efficient electron transfer between persulfate-binding and pollutant-binding sites. This constraint is often obscured in powder catalysts but becomes critical when reactions in integrated catalytic membranes or devices, where spatial separation of active sites and discontinuous conductive pathways can electronically isolate internal regions, substantially limiting reaction site utilization. Here we report an interfused nitrogen-doped reduced graphene oxide fiber (N-rGOF) membrane that overcomes this by unifying long-range electronic continuity with internal site accessibility. Fused junctions between fibers form a continuous, low resistance conductive network, while the layered rGO structure enables persulfate entry into interlayers to activate otherwise inaccessible internal nitrogen sites through an interlayer entry-induced site activation (IESA) mechanism. The N-rGOF membrane degraded bisphenol A (BPA) ∼5.2 times faster than a noninterfused counterpart and maintained excellent removal of trace organic pollutants in real livestock wastewater with high ionic strength and organic loading. Furthermore, the intrinsic potential difference generated during catalysis enables a floatable, self-powered setup that couples pollutant degradation with real-time electrical signaling, illustrating the conceptional feasibility of integrated monitoring and remediation based on one single system.