Hang Zhang, Tao Luo, Yingkang Chen, Xiaojian Wang, Edoardo Mariani, Kang Liu, Junwei Fu, Changxu Liu, Hui Liu, Zhang Lin, Liyuan Chai, Michelle L. Coote, Emiliano Cortés, Min Liu
Abstract Catalytic hydrolysis is an effective strategy for decomposing tetrafluoromethane (CF 4 ), one of the most chemically inert per- and polyfluoroalkyl substances (PFAS). A key challenge in this process lies in enhancing proton availability to facilitate efficient and stable C–F bond activation while ensuring long-term catalyst stability. Here we present an SO 2 -driven approach to significantly enhance H 2 O dissociation and proton-supplying through the in situ formation of Al–HSO 4 and Ga–HS species. Combined experimental and theoretical investigations reveal that these species not only lower the energy barrier for C–F bond activation but also promote active site regeneration by facilitating defluorination, thus effectively overcoming catalyst deactivation. As a result, the optimized catalyst enables complete CF 4 decomposition at a low temperature of 550°C, with stable operation for over 2500 hours. This work establishes a new paradigm for regulating proton transfer and offers a viable route for the efficient, durable degradation of gaseous PFAS.