Abstract
AbstractDevelopment of effective and stable catalysts for CO2 hydrogenation into ethanol remains a challenge. Herein, we report that Rh1/CeTiOx single‐atom catalyst constructed by embedding monoatomic Rh onto Ti‐doped CeO2 support has shown a super high ethanol selectivity (≈99.1 %), record‐breaking turnover frequency (493.1 h−1), and outstanding stability. Synergistic effects of Ti‐doption and monoatomic Rh contribute to this excellent catalytic performance by firstly facilitating oxygen vacancies formation to generate oxygen‐vacancy‐Rh Lewis‐acid‐base pairs, which favor CO2 adsorption and activation, cleavage of C−O bonds in CHxOH* and COOH* into CHx* and CO* species, subsequent C−C coupling and hydrogenation into ethanol, and secondly generating strong Rh−O bond by Ti‐doping‐induced crystal reconstruction, which contributes to striking stability. This work highlights the importance of support elaborating regulation for single‐atom catalyst design to substantially improve the catalytic performance.
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