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Enhancing electrochemical reductive defluorination of PFASs using ZIF-67 modified cathode: Mechanistic insights and performance optimization

Xing Zhang,Han Wu,Yue Wang,Yafei Wang,Yangyang Deng,Yanping Zhu,Shengsen Zhang,Huub Rijnaarts,Harry Bruning,Junhao Qin,Qingqi Lin,Zhuobiao Ni,Rongliang Qiu

The effectiveness of electrochemical reductive defluorination is impeded by the low environmental concentrations of per- and polyfluoroalkyl substances (PFASs) and the robust nature of C − F bonds. In this work, we investigate the zeolitic imidazolate framework-67 (ZIF-67) as a promising catalyst for PFASs remediation. We show that ZIF-67 hold promise for simultaneous adsorption and reductive defluorination of 2-(trifluoromethyl) acrylic acid (TFMAA). Following a 48-hour treatment, the ZIF-67 modification significantly improves the adsorption of TFMAA onto the cathode surface, achieving removal and defluorination efficiencies of 99.66 % and 97.16 %, respectively (C 0 = 5 mg L −1 , applied voltage of −1.2 V vs. Ag/AgCl). Furthermore, the atomic H*, catalyzed by the Co−N 4 structure, boosts the reductive defluorination of TFMAA through indirect mechanisms, while the nitrogen loss due to carbonization further enhances the catalytic defluorination efficiency. This research presents a novel electrode material for PFASs defluorination and offers mechanistic insights into the defluorination process.