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The central issue is the lack of quantitative understanding of how the interfacial\n                    <jats:sup>*<\/jats:sup>\n                    CO and\n                    <jats:sup>*<\/jats:sup>\n                    H intermediates jointly govern product selectivity. Here, we establish an interfacial coverage regulation strategy by embedding Cu nanoparticles into an imine\u2010functionalized covalent organic framework (Cu\/Im\u2010COF). The imine\u2010rich interface enriches CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption while modulating proton transfer, enabling a balanced surface coverage of\n                    <jats:sup>*<\/jats:sup>\n                    CO and\n                    <jats:sup>*<\/jats:sup>\n                    H, identified as the key selectivity descriptor (\n                    <jats:italic>\u03b8<\/jats:italic>\n                    <jats:sub>*CO\/*H<\/jats:sub>\n                    ) for ethanol formation. Operando Raman spectroscopy, density functional theory calculations, confirms that an optimized\n                    <jats:italic>\u03b8<\/jats:italic>\n                    <jats:sub>*CO\/*H<\/jats:sub>\n                    stabilizes the\n                    <jats:sup>*<\/jats:sup>\n                    HCCHOH intermediate and lowers its formation barrier. Quantitative integration of Raman features allows direct determination of\n                    <jats:italic>\u03b8<\/jats:italic>\n                    <jats:sub>*CO\/*H<\/jats:sub>\n                    , revealing a volcano\u2010type dependence of ethanol selectivity on this descriptor. A maximum ethanol Faradaic efficiency of 56% is achieved at log(\n                    <jats:italic>\u03b8<\/jats:italic>\n                    <jats:sub>*CO\/*H<\/jats:sub>\n                    ) \u2248 3.0, a current density of 700\u00a0mA cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    , and a 15% CO\n                    <jats:sub>2<\/jats:sub>\n                    feed. This work establishes\n                    <jats:italic>\u03b8<\/jats:italic>\n                    <jats:sub>*CO\/*H<\/jats:sub>\n                    as a quantitative bridge between intermediate coverage and reaction kinetics, providing a mechanistic framework for rational design of CO\n                    <jats:sub>2<\/jats:sub>\n                    RR catalysts with high ethanol selectivity under CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010constrained conditions.\n                  <\/jats:p>","DOI":"10.1002\/smtd.202502409","type":"journal-article","created":{"date-parts":[[2026,2,21]],"date-time":"2026-02-21T09:01:23Z","timestamp":1771664483000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Establishing\n                    <sup>*<\/sup>\n                    CO\/\n                    <sup>*<\/sup>\n                    H Intermediate Descriptor for Selective CO\n                    <sub>2<\/sub>\n                    \u2010to\u2010Ethanol Electroreduction Under Limited CO\n                    <sub>2<\/sub>\n                    Supply"],"prefix":"10.1002","volume":"10","author":[{"given":"Xiaochen","family":"Feng","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science School of Chemistry Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zihao","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science School of Chemistry Beihang University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingwei","family":"Fang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science School of Chemistry Beihang University  Beijing 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Laboratory of Bioinspired Interfacial Materials Science School of Chemistry Beihang University  Beijing China"},{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science Bioinspired Science Innovation Center Hangzhou International Innovation Institute Beihang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lei","family":"Jiang","sequence":"additional","affiliation":[{"name":"CAS Key Laboratory of Bio\u2010Inspired Materials and Interface Science Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing 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