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Although single\u2010atom catalysts have shown potential in selectively converting CO\n                    <jats:sub>2<\/jats:sub>\n                    to CH\n                    <jats:sub>4<\/jats:sub>\n                    , their limited active sites often hinder the realization of high current densities, posing a selectivity\u2010activity dilemma. In this study, we developed a single\u2010atom cobalt (Co) doped copper catalyst (Co\n                    <jats:sub>1<\/jats:sub>\n                    Cu) that achieved a CH\n                    <jats:sub>4<\/jats:sub>\n                    Faradaic efficiency exceeding 60\u2009% with a partial current density of \u2212482.7\u2005mA\u2009cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . Mechanistic investigations revealed that the incorporation of single Co atoms enhances the activation and dissociation of H\n                    <jats:sub>2<\/jats:sub>\n                    O molecules, thereby lowering the energy barrier for the hydrogenation of *CO intermediates. In situ spectroscopic experiments and density functional theory simulations further demonstrated that the modulation of the *CO adsorption configuration, with stronger bridge\u2010binding, favours deep reduction to CH\n                    <jats:sub>4<\/jats:sub>\n                    over the C\u2212C coupling or CO desorption pathways. Our findings underscore the potential of Co\n                    <jats:sub>1<\/jats:sub>\n                    Cu catalysts in overcoming the selectivity\u2010activity trade\u2010off, paving the way for efficient and scalable CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010CH\n                    <jats:sub>4<\/jats:sub>\n                    conversion technologies.\n                  <\/jats:p>","DOI":"10.1002\/anie.202417008","type":"journal-article","created":{"date-parts":[[2025,1,13]],"date-time":"2025-01-13T22:15:23Z","timestamp":1736806523000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":50,"title":["Copper\u2010Catalysed Electrochemical CO\n                    <sub>2<\/sub>\n                    Methanation via the Alloying of Single Cobalt Atoms"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9069-7002","authenticated-orcid":false,"given":"Jiawei","family":"Li","sequence":"first","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei Anhui 230026 P. 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