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It is feasible to optimize the reaction path selectivity by modifying organic ligands and constructing single\u2010atom systems. At the same time, heterogeneous metal nanosheets with atomic thickness have been shown to significantly enhance the catalytic activity of materials due to their ultra\u2010high exposure of active sites and synergistic effects. Herein, we synthesize an ultra\u2010thin heterogeneous alloy metallene with organic ligand\u2010modified surface Cu single atom by one\u2010pot wet chemical method, and further construct an efficient Cu\u2212Pd active sites. The prepared octanoic acid ligand modified PdCu single\u2010atom alloys metallene (SAA OA\u2212Cu\u2010Pdene) shows excellent catalytic activity and stability, with mass activity up to 5.64\u2005A\u2009mg\n                    <jats:sub>Pd<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    and electrochemical active surface area (ECSA) up to 160.39\u2005m\n                    <jats:sup>2<\/jats:sup>\n                    \u2009g\n                    <jats:sub>Pd<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Structural characterization and in situ experiment jointly indicate that ligand modulation brings about charge transfer, and the accompanying rapid migration of OH\n                    <jats:sup>\u2212<\/jats:sup>\n                    greatly improves the selectivity of non\u2010CO pathways while improving the catalytic activity. The results highlight the importance of adjacent\u2010ligand regulation and provide a new strategy for the design of MOR catalysts with high selectivity of non\u2010CO pathway.\n                  <\/jats:p>","DOI":"10.1002\/anie.202420817","type":"journal-article","created":{"date-parts":[[2024,12,23]],"date-time":"2024-12-23T10:19:23Z","timestamp":1734949163000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":70,"title":["Adjacent\u2010Ligand Tuning of Atomically Precise Cu\u2212Pd Sites Enables Efficient Methanol Electrooxidation with a CO\u2010Free Pathway"],"prefix":"10.1002","volume":"64","author":[{"given":"Yuanlong","family":"Qin","sequence":"first","affiliation":[{"name":"Department of Chemistry Capital Normal University  Beijing 100048 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kedi","family":"Yu","sequence":"additional","affiliation":[{"name":"Department of Chemistry Capital Normal University  Beijing 100048 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guo","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Chemistry Capital Normal University  Beijing 100048 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zechao","family":"Zhuang","sequence":"additional","affiliation":[{"name":"Department of Chemistry Tsinghua University  Beijing 100084 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuhai","family":"Dou","sequence":"additional","affiliation":[{"name":"Institute of Energy Materials Science University of Shanghai for Science and Technology  Shanghai 200093 P. R. 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