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

Chemical conversion of CO2 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 CO2 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 CeO2 and pure silicon zeolite (S1) to co-activate Cu species. In CO2-to-methanol (CTM) conversion, the space-time yield of methanol (STYMeOH) of the obtained CuCe/S1 catalysts reaches 87.23 g kgCu -1 h-1, which represents a fivefold increase compared to that of the Cu/CeO2 catalysts. The following mechanistic investigations reveal that S1 serves as a pivotal stabilizer for the small-sized CeO2 particles, thereby significantly enhancing the synergistic interaction between Cu species and CeO2. The crafted interaface possesses abundant oxygen vacancies and a high content of Cu+, significantly enhancing the adsorption of CO2 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.