Enhanced C-F Activation and Proton Supply over Al2O3-Embedded RuOx Clusters Boost Perfluorocarbon Hydrolysis

The catalytic hydrolysis of per- and polyfluoroalkyl substances (PFAS) holds significant potential for environmental remediation; however, the chemically inert C-F bond poses substantial challenges for achieving efficient low-temperature activity. Herein, we demonstrate that RuOx clusters embedded in mesoporous Al2O3 nanosheet (RuOx/Al2O3) catalysts achieved the complete decomposition of CF4, one of the most chemically inert PFAS, at an unprecedented low temperature of 450 °C, outperforming all catalysts reported to date. The extraordinary CF4 hydrolysis performance is attributed to synergistically enhanced C-F bond activation and proton supply. Specifically, the strong electronic interaction between RuOx clusters and Al2O3 promotes the CF4 adsorption and C-F cleavage on Al sites in RuOx/Al2O3. Furthermore, the Ru sites in RuOx/Al2O3 promote H2O dissociation into *H and *OH, which enables the continuous regeneration of adjacent Al-OH groups and supplies sufficient protons for defluorination in the CF4 hydrolysis reaction. This study paves the way for designing and developing highly efficient catalysts for low-temperature catalytic hydrolysis of PFAS.