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

Abstract

Efficient spontaneous molecular oxygen (O2) 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 O2. Herein, defect‐rich N‐doped reduced graphene oxide/CoFe2O4 (NGCF‐OV) membrane containing asymmetric Co‐OV‐Fe sites is prepared for O2 activation. The intrinsic catalytic activity is that the asymmetric Co‐OV‐Fe sites regulate the O─O bond length, promoting more and faster electron transfer to O2 for selectively producing 1O2. Meanwhile, the adjacent graphitic N sites help confine organics to the surface and thus greatly shorten the reaction distance of 1O2 and improve its utilization efficiency. The NGCF‐OV 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.