Achieving acetone efficient deep decomposition by strengthening reactants adsorption and activation over difunctional...

Realizing the simultaneous adsorption and activation of O₂ and reactants over supported noble metal catalysts is crucial for the oxidation of organic hydrocarbons. Herein, we report a facile one-step ethylene glycol reduction method to synthesize difunctional Au(OH)K_x sites, which were anchored on a hierarchical hollow MFI support and adopted for acetone decomposition. The alkali ion-associated adjacent surface hydroxyl groups were coordinated with Au nanoparticles, resulting in partially oxidized Au¹⁺ sites with improved dispersion. The results obtained from exclusive ex situ and in situ experiments illustrated that the proper content of K and hydroxyl groups significantly enhanced the adsorption of surface O₂ and acetone molecules around the Au sites simultaneously, whereas the excess K species inhibited the catalytic performance by blocking the pore structure and decreasing the acidity of catalysts. The Au(OH)K_0.7/h-MFI catalyst exhibited the highest efficiency for acetone oxidation, over which 1500 ppm acetone can be completely oxidized at just 280 °C with an extremely low activation energy of 32.5 kJ mol^-1. The carbonate species were detected as the main intermediates during acetone decomposition over the difunctional Au(OH)K_x sites through a Langmuir - Hinshelwood (L - H) mechanism. This finding paves the way for designing and constructing efficient functional active sites for the complete oxidation of hydrocarbons.