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Such uncontrollable features severely impede the optimization of catalytic performance. In this study, we demonstrate precise control over RMSIs by leveraging the high mobility of InO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    on CeO\n                    <jats:sub>2<\/jats:sub>\n                    support under hydrogen reducing conditions\u2014directly visualized by in situ environmental electron microscopy\u2014in combination with the quantitative tuning of InO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    content via atomic layer deposition. The resulting optimized catalyst delivers an exceptional space\u2010time yield of 1.67 g\n                    <jats:sub>MeOH<\/jats:sub>\n                    \u00b7g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00b7h\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 280\u00b0C in the CO\n                    <jats:sub>2<\/jats:sub>\n                    hydrogenation reaction, surpassing previously reported Ni\u2010based catalysts and even Pd\u2010based noble metal catalysts in the literature. In situ spectroscopic characterization reveals that the controlled RMSIs enables the optimization of InO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    \/NiIn interface, which promotes the selective conversion of HCOO* to CH\n                    <jats:sub>3<\/jats:sub>\n                    O* and subsequently to methanol, thereby significantly enhancing the methanol production. These findings highlight the critical role of precisely regulated RMSIs in the rational design of high\u2010performance catalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.1906096","type":"journal-article","created":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T05:22:02Z","timestamp":1784265722000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Controlled Reactive Metal\u2212Support Interactions in NiIn\/CeO\n                    <sub>2<\/sub>\n                    Catalysts for Enhanced Methanol Synthesis from CO\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"65","author":[{"given":"Qimeng","family":"Sun","sequence":"first","affiliation":[{"name":"Hefei National Research Center for Physical Sciences At the Microscale University of Science and Technology of China  Hefei 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