Promoting C–FBond Activation for PerfluorinatedCompounds Decomposition via Atomically Synergistic Lewis and BrønstedAcid Sites

Catalytic hydrolysis is a sustainable method for the degradation of perfluorinated compounds (PFCs) but is challenged by the high reaction temperatures required to cleave strong C–F bonds. Herein, we developed an innovative C–F activation strategy by constructing synergistic Lewis and Brønsted acid pairs over atomically dispersed Zn–O–Al sites to promote C–F bond activation for decomposition of typical PFCs, CF₄. Density functional theory (DFT) calculations demonstrate tricoordinated Al (Al_III) sites and Zn–OH functional, respectively, as Lewis and Brønsted acid sites over Zn–O–Al, synergistically enhancing the adsorption and decomposition of CF₄. X-ray absorption spectroscopy (XAS), pyridine infrared spectroscopy (Py-IR), and ammonia temperature-programmed desorption (NH₃-TPD) verified the presence of both Al_III and Zn–OH on the atomically dispersed Zn–O–Al sites. CF₄-TPD and <i>in situ</i> infrared spectroscopy confirmed that the Zn–O–Al sites facilitate CF₄ adsorption and C–F bond activation. As a result, the Zn–O–Al sites with synergistic Lewis and Brønsted acid pairs achieved 100% CF₄ decomposition at a low temperature of 560 °C and demonstrated outstanding stability for more than 250 h.