Efficient and stable catalytic hydrolysis of perfluorocarbon enabled by SO2-mediated proton supply.

Catalytic hydrolysis is an effective strategy for decomposing tetrafluoromethane (CF4), 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 SO2-driven approach to significantly enhance H2O dissociation and proton-supplying through the in situ formation of Al-HSO4 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 CF4 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.