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Herein, inspired by the activation mechanism of natural carbon monoxide dehydrogenase, we fabricated a Re\u2010Ni dual\u2010atom catalyst supported on a nitrogen\u2010doped carbon catalyst (ReNi\u2010N\/C), featuring adjacent Re\u2010Ni atomic pairs, that exhibits outstanding eCO\n                    <jats:sub>2<\/jats:sub>\n                    R performance with a CO partial current density of \u2212427.6\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and near 100% Faradaic efficiency for CO (FE\n                    <jats:sub>CO<\/jats:sub>\n                    ). Notably, it operates at an ultralow overpotential of 0.16\u00a0V to achieve a CO partial current density of \u221227.0\u00a0mA cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    and maintains over 95% FE\n                    <jats:sub>CO<\/jats:sub>\n                    within a broad potential range from \u22120.27\u00a0V to \u22120.80\u00a0V. In situ spectroscopy and density functional theory (DFT) calculations reveal that the formation of Re\u2010Ni pairs not only induces a downshift by 0.22\u00a0eV of the Ni d\u2010band center but also enables a bidentate adsorption configuration of the *COOH intermediate on the Ni\u2212Re site, which accelerates *COOH formation and *CO desorption, thereby achieving high activity and selectivity in eCO\n                    <jats:sub>2<\/jats:sub>\n                    R. This work demonstrates a new strategy and theoretical basis for the rational design of bimetallic sites toward efficient CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction electrocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.1716945","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T11:48:07Z","timestamp":1784116087000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["The Bidentate Adsorption Mode of Re\u2010Ni Atomic Pairs Inducing the Ultralow Overpotential in CO\n                    <sub>2<\/sub>\n                    Electroreduction"],"prefix":"10.1002","volume":"65","author":[{"given":"Jianping","family":"Guan","sequence":"first","affiliation":[{"name":"College of Chemistry and Chemical Engineering Central South University  Changsha P. R. 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