Intensify Mass Transfer and Molecular Oxygen Activation by Defect‐Bridged Asymmetric Catalytic Sites Toward Efficient Membrane‐Based Nanoconfined Catalysis

Abstract Efficient spontaneous molecular oxygen (O 2 ) activation is expected in advanced oxidation processes. However, it remains a great challenge to promote the reactants adsorption and accelerate the interfacial electron transfer to boost the activation kinetic of O 2 . Herein, defect‐rich N‐doped reduced graphene oxide/CoFe 2 O 4 (NGCF‐O V ) membrane containing asymmetric Co‐O V ‐Fe sites is prepared for O 2 activation. The intrinsic catalytic activity is that the asymmetric Co‐O V ‐Fe sites regulate the O─O bond length, promoting more and faster electron transfer to O 2 for selectively producing 1 O 2 . Meanwhile, the adjacent graphitic N sites help confine organics to the surface and thus greatly shorten the reaction distance of 1 O 2 and improve its utilization efficiency. The NGCF‐O V membrane demonstrates complete degradation of bisphenol A within a retention time of 86 ms, achieving a k‐value of 0.047 ms −1 , which exceeds the performance of most Fenton‐like systems. This work provides new horizons for designing an efficient and stable catalytic membrane, enriching the domain of advanced wastewater treatment strategies.