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Cu has been regarded as one of the most powerful contenders in catalyzing CO<jats:sub>2<\/jats:sub> 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\u2010efficiency catalyst by utilizing CeO<jats:sub>2<\/jats:sub> and pure silicon zeolite (S1) to co\u2010activate Cu species. In CO<jats:sub>2<\/jats:sub>\u2010to\u2010methanol (CTM) conversion, the space\u2010time yield of methanol (STY<jats:sub>MeOH<\/jats:sub>) of the obtained CuCe\/S1 catalysts reaches 87.23\u2005g\u2009kg<jats:sub>Cu<\/jats:sub><jats:sup>\u22121<\/jats:sup>\u2009h<jats:sup>\u22121<\/jats:sup>, which represents a fivefold increase compared to that of the Cu\/CeO<jats:sub>2<\/jats:sub> catalysts. The following mechanistic investigations reveal that S1 serves as a pivotal stabilizer for the small\u2010sized CeO<jats:sub>2<\/jats:sub> particles, thereby significantly enhancing the synergistic interaction between Cu species and CeO<jats:sub>2<\/jats:sub>. The crafted interaface possesses abundant oxygen vacancies and a high content of Cu<jats:sup>+<\/jats:sup>, significantly enhancing the adsorption of CO<jats:sub>2<\/jats:sub> 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.<\/jats:p>","DOI":"10.1002\/anie.202423438","type":"journal-article","created":{"date-parts":[[2025,1,25]],"date-time":"2025-01-25T03:05:02Z","timestamp":1737774302000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":20,"title":["Boosting CO<sub>2<\/sub> Hydrogenation by Synergistic Incorporation of Pure Silica Silicalite\u20101 Zeolite and CeO<sub>2<\/sub> into Cu Catalysts"],"prefix":"10.1002","volume":"64","author":[{"given":"Jing","family":"Xu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun 130022 China"},{"name":"School of Applied Chemistry and Engineering University of Science and Technology of China  Hefei 230026 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