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However, the precise formation mechanism of oxygen vacancies (OVs) and exact roles of hydroxyl groups (InOHs), the two most important surface structures, remain poorly understood due to the limited resolution of currently available characterization methods. Here, by employing an advanced\n                    <jats:sup>17<\/jats:sup>\n                    O labeling strategy combined with high\u2010field solid\u2010state NMR (ssNMR) up to 18.8 T, we achieve exceptionally high spectral resolution of\n                    <jats:sup>17<\/jats:sup>\n                    O NMR, enabling explicit separation of distinct surface oxygen species. This approach allows tracing the thermal evolution of these species and probing their reactivities toward CO\n                    <jats:sub>2<\/jats:sub>\n                    activation and hydrogenation. Notably, surface OIn\n                    <jats:sub>3<\/jats:sub>\n                    sites are identified as the OV precursors, with a formation barrier of approximately 200\u00b0C. Unexpectedly,\n                    <jats:italic>room\u2010temperature oxygen exchange<\/jats:italic>\n                    between In\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>3<\/jats:sub>\n                    and CO\n                    <jats:sub>2<\/jats:sub>\n                    is observed, enabled by the high sensitivity of the new\n                    <jats:sup>17<\/jats:sup>\n                    O NMR method. Further probing with\n                    <jats:sup>13<\/jats:sup>\n                    CO\n                    <jats:sub>2<\/jats:sub>\n                    and\/or H\n                    <jats:sub>2<\/jats:sub>\n                    , at variable temperatures, we are capable of unraveling the roles between OVs, InOHs and surface lattice oxygen species in CO\n                    <jats:sub>2<\/jats:sub>\n                    \/H\n                    <jats:sub>2<\/jats:sub>\n                    activation and their stepwise conversion into formate intermediates and ultimately methanol, which may prompt rational designs to lower the reaction temperature for In\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>3<\/jats:sub>\n                    .\n                  <\/jats:p>","DOI":"10.1002\/anie.2883791","type":"journal-article","created":{"date-parts":[[2026,5,23]],"date-time":"2026-05-23T16:28:57Z","timestamp":1779553737000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Hydrogenation of CO\n                    <sub>2<\/sub>\n                    to Methanol Catalyzed by In\n                    <sub>2<\/sub>\n                    O\n                    <sub>3<\/sub>\n                    : Oxygen Vacancies, Surface Hydroxyl Groups, and Temperature Dependence for Reactivity Revealed by\n                    <sup>17<\/sup>\n                    O NMR"],"prefix":"10.1002","volume":"65","author":[{"given":"Hongyu","family":"Chen","sequence":"first","affiliation":[{"name":"State Key Laboratory of Catalysis Institution Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8216-863X","authenticated-orcid":false,"given":"Guangjin","family":"Hou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis Institution Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian 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