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Here, we construct two well\u2010defined model catalysts, single\u2010atomic Pt on CuO\n                    <jats:sub>x<\/jats:sub>\n                    clusters (Pt\n                    <jats:sub>1<\/jats:sub>\n                    \u2010CuO\n                    <jats:sub>x<\/jats:sub>\n                    \/CN) and triple\u2010atomic Pt on CuO\n                    <jats:sub>x<\/jats:sub>\n                    clusters (Pt\n                    <jats:sub>3<\/jats:sub>\n                    \u2010CuO\n                    <jats:sub>x<\/jats:sub>\n                    \/CN), and employ methanol oxidation reaction (MOR) as a probe to unravel the role of atomic assembly in governing catalytic mechanisms. Pt\n                    <jats:sub>1<\/jats:sub>\n                    \u2010CuO\n                    <jats:sub>x<\/jats:sub>\n                    \/CN enables a CO\u2010free pathway, achieving an ultrahigh formate selectivity of 80%\u201399% over a wide potential window (0.6\u20131.0 V vs. RHE). In contrast, Pt\n                    <jats:sub>3<\/jats:sub>\n                    \u2010CuO\n                    <jats:sub>x<\/jats:sub>\n                    \/CN follows a hybrid pathway involving both formate and CO routes, delivering significantly higher mass activity than that of Pt\n                    <jats:sub>1<\/jats:sub>\n                    \u2010CuO\n                    <jats:sub>x<\/jats:sub>\n                    \/CN and the commercial Pt\/C, alongside high resistance to CO poisoning. Isolated Pt sites in Pt\n                    <jats:sub>1<\/jats:sub>\n                    \u2010CuO\n                    <jats:sub>x<\/jats:sub>\n                    \/CN impose a prohibitively uphill free\u2010energy change for the key *COH intermediate (2.15 eV), effectively suppressing CO generation. Conversely, triangular Pt sites in Pt\n                    <jats:sub>3<\/jats:sub>\n                    \u2010CuO\n                    <jats:sub>x<\/jats:sub>\n                    \/CN form a robust electronic localization center via deep 5d orbital hybridization, facilitating d\u2192\u03c0* electron back\u2010donation and stabilizing *COH adsorption in a triple hollow\u2010site configuration, lowering the limiting free\u2010energy requirement for the CO pathway. This work reveals the role of atomic\u2010scale assembly on oxide clusters in dictating catalytic mechanism and performance, opening new avenues for precise design of advanced electrocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.4503768","type":"journal-article","created":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T11:00:40Z","timestamp":1786964440000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Tuning Reaction Pathways by Controlling Atomic Assembly on Oxide Clusters"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-2281-504X","authenticated-orcid":false,"given":"Chenliang","family":"Ye","sequence":"first","affiliation":[{"name":"Hebei Key Laboratory of Energy Storage Technology and Integrated Energy Utilization North China Electric Power University  Baoding Hebei China"},{"name":"College of Materials Science and Engineering Shenzhen University  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiguo","family":"Wang","sequence":"additional","affiliation":[{"name":"Hebei Key Laboratory of Energy Storage Technology and Integrated Energy Utilization North China Electric Power University  Baoding Hebei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiming","family":"Li","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Shenzhen University  Shenzhen China"},{"name":"Key Laboratory of Functional Molecular Solids, Ministry of Education College of Chemistry and Molecular Sciences Anhui Normal University  Wuhu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingyue","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Technology Tianjin University  Tianjin 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Hebei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8873-6295","authenticated-orcid":false,"given":"Mao","family":"Peng","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Technology Tianjin University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0074-7633","authenticated-orcid":false,"given":"Dingsheng","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Chemistry Tsinghua University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3427-191X","authenticated-orcid":false,"given":"Jin","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Shenzhen University  Shenzhen China"},{"name":"Key Laboratory of Functional Molecular Solids, Ministry of Education College of Chemistry and Molecular Sciences 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