Boosting CO2 Hydrogenation by Synergistic Incorporation of Pure Silica Silicalite‐1 Zeolite and CeO2 into Cu Catalysts

Abstract Chemical conversion of CO 2 is providing an opportunity to mitigate the global warming induced by the overconsumption of fossil fuel. Cu has been regarded as one of the most powerful contenders in catalyzing CO 2 conversion, yet the precise manipulation of its surface state and the nearby chemical environment continues to pose a formidable challenge. In this work, we report a high‐efficiency catalyst by utilizing CeO 2 and pure silicon zeolite (S1) to co‐activate Cu species. In CO 2 ‐to‐methanol (CTM) conversion, the space‐time yield of methanol (STY MeOH ) of the obtained CuCe/S1 catalysts reaches 87.23 g kg Cu −1 h −1 , which represents a fivefold increase compared to that of the Cu/CeO 2 catalysts. The following mechanistic investigations reveal that S1 serves as a pivotal stabilizer for the small‐sized CeO 2 particles, thereby significantly enhancing the synergistic interaction between Cu species and CeO 2 . The crafted interaface possesses abundant oxygen vacancies and a high content of Cu + , significantly enhancing the adsorption of CO 2 and inhibiting the formation of CO. Our discovery presents a promising new direction for catalyst upgrading and performance enhancement for CTM processes in the foreseeable future.