Boosting CO2 Hydrogenation by Synergistic Incorporation of Pure Silica 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 (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/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.