Durable Ti4O7 Heterojunction Composite Membrane Encapsulating N-Doped Graphene Nanosheets for Efficient Electro-Oxidation of GenX and Other PFAS in Fluorochemical Wastewater

Rational interfacial engineering design of an electrocatalyst, such as a heterojunction structure, can effectively enhance its catalytic activity. This study aims to address a critical challenge associated with the use of carbon material@Ti4O7 heterojunction composite electrodes for wastewater treatment─electrode stability over long-term operation. Herein, we report a highly stabilized interfacial engineering strategy, i.e., the use of conductive inorganic CeO2 as a “cement” to firmly encapsulate N-doped graphene oxide nanosheets (N-GS) on the Ti4O7 surface. The defect-rich N-GS encapsulated on the Ti4O7 surface significantly enhances interfacial charge transfer. This enhancement results in the N-GS/CeO2@Ti4O7 heterojunction composite electrode exhibiting excellent efficiency in the electro-oxidation of hexafluoropropylene oxide dimer acid (HFPO-DA or GenX). Furthermore, a flow-through N-GS/CeO2@Ti4O7 reactive electrochemical membrane system effectively mineralizes other 35 PFASs in a real fluorochemical wastewater sample, achieving a high defluorination rate of 70–90% and exhibiting better performance in PFAS destruction and energy efficiency compared to the UV/KI-SO32– process. Results of this study enhance our understanding of the electrochemical oxidation of PFAS and offer valuable insight into the design of stabilized Ti4O7 heterojunction composites. These findings are instrumental in advancing the development of effective treatments for PFAS-contaminated environments.