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Here, we investigate the performance of heteroatom\u2010doped Cu\n                    <jats:sub>3<\/jats:sub>\n                    clusters supported on g\u2010C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>4<\/jats:sub>\n                    for CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    conversion. Through DFT calculations and transition\u2010state analysis, we demonstrate that doping with P and Se stabilizes the Cu\n                    <jats:sub>3<\/jats:sub>\n                    clusters, enhances\n                    <jats:sup>*<\/jats:sup>\n                    CO adsorption, and lowers the energy barrier for the rate\u2010determining\n                    <jats:sup>*<\/jats:sup>\n                    CO +\n                    <jats:sup>*<\/jats:sup>\n                    CHO \u2192\n                    <jats:sup>*<\/jats:sup>\n                    COCHO C\u2500C coupling step to 0.84 and 0.92\u00a0eV, respectively. Thermodynamic analysis reveals a preference for ethylene formation over ethanol, with overpotentials as low as 0.33 and 0.10\u00a0V for P\u2010 and Se\u2010doped systems. Electronic structure analysis shows that first\u2010shell substitution with P or Se creates charge\u2010asymmetric sites, strengthens\n                    <jats:sup>*<\/jats:sup>\n                    CO and\n                    <jats:sup>*<\/jats:sup>\n                    CHO binding, and shifts antibonding Cu\u2500CO states to higher energies, thereby promoting efficient C\u2500C coupling. Electrochemically, the Se\u2010modified catalyst delivers a remarkable ethylene Faradaic efficiency of \u223c54% at 250\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , and maintains stable performance for 30 h under flow\u2010cell conditions. This study establishes a synergistic theory\u2010experiment framework for optimizing CO\n                    <jats:sub>2<\/jats:sub>\n                    RR catalysts, emphasizing the critical role of precise cluster engineering and charge\u2010gradient doping in promoting efficient C\u2500C coupling.\n                  <\/jats:p>","DOI":"10.1002\/adma.73318","type":"journal-article","created":{"date-parts":[[2026,5,8]],"date-time":"2026-05-08T04:43:58Z","timestamp":1778215438000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Heteroatom\u2010Engineered Triatomic Cu Cluster on G\u2010C\n                    <sub>3<\/sub>\n                    N\n                    <sub>4<\/sub>\n                    for Selective CO\n                    <sub>2<\/sub>\n                    \u2010to\u2010Ethylene Electrocatalysis"],"prefix":"10.1002","volume":"38","author":[{"given":"Shengjie","family":"Bai","sequence":"first","affiliation":[{"name":"International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University  Shaanxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhizhong","family":"He","sequence":"additional","affiliation":[{"name":"International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University  Shaanxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenyu","family":"Zheng","sequence":"additional","affiliation":[{"name":"International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University  Shaanxi 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