Directional Electron Transfer in Island‐Sea Structured Contact‐Electro‐Catalysis Enables Cascade Defluorination of PFAS

promote oxidative mineralization of low-fluorinated intermediates, establishing a cascade redox pathway. This cooperative mechanism achieves 95% degradation and 94.4% defluorination of perfluorooctanoic acid with excellent stability. This study defines β-phase-mediated IEF engineering in polymer/single-atom hybrids as a general concept for directing interfacial electron dynamics in catalytic systems.