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Here, we elaborate that redox\u2010active isoindigo, acting as a multifunctional co\u2010catalyst, can pre\u2010activate CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010bound intermediates and suppress HER upon the synergistic effects of Lewis acid\u2010base adduct formation, intramolecular hydrogen\u2010bond interaction, and interfacial water structure modulation. Modifying a silver catalyst with isoindigo substantially decreases the energy barrier for CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010to\u2010*COOH conversion, which is regarded as the potential\u2010limiting step of carbon monoxide production. Accordingly, superior catalytic performances are obtained at pH 2, where Faradaic efficiencies surpass 99% at industrial\u2010relevant current densities. Moreover, we find that assembling an additional polyamine\u2010coated layer in front of gas flow channels improves CO\n                    <jats:sub>2<\/jats:sub>\n                    transport to the catalyst layer, optimizing the trade\u2010off of conversion and selectivity at low flow rates.\n                  <\/jats:p>","DOI":"10.1002\/anie.202514111","type":"journal-article","created":{"date-parts":[[2025,9,5]],"date-time":"2025-09-05T06:33:10Z","timestamp":1757053990000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Multifunctional Binding Interface Drives Near\u2010Unity CO Selectivity in Acidic CO\n                    <sub>2<\/sub>\n                    Electrolysis"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1525-4981","authenticated-orcid":false,"given":"Zhengyuan","family":"Li","sequence":"first","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Johns Hopkins University  Baltimore Maryland 21218 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuting","family":"Xu","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering Worcester Polytechnic Institute  Worcester Massachusetts 01609 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xing","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering Johns Hopkins University  Baltimore Maryland 21218 USA"},{"name":"Department of Chemistry City University of Hong Kong  Hong Kong 999077 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gregory D. 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