Enhanced surface Lewis acidity of ZrO₂ by -HSO₄ for efficient CF₄ decomposition

Tetrafluoromethane (CF4), as the simplest and most abundant perfluorocarbon in the atmosphere, is listed in the 'United Nations Framework Convention on Gases' for its strong greenhouse potential. With its increasing atmospheric emissions, catalytic hydrolysis of CF4 as a non-toxic by-product method has been extensively studied. However, the highly symmetric and inert structure of CF4 makes it hard to be adsorbed on the catalyst surface. Herein, we developed a protonated sulfate (-HSO4) modified ZrO2 (S-ZrO2) to enhance CF4 adsorption and achieve its complete decomposition at 650 degrees C, which was superior to common gamma-Al2O3. Combining the surface acidity test, in situ infrared spectroscopy and density function theory simulations, we demonstrated that the introduced -HSO4 effectively enhances the Lewis acidity of adjacent Zr sites, which shows strong CF4 adsorption ability and promotes its decomposition.