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Consequently, conventional alloy catalysts often suffer from an activity\u2013selectivity trade\u2010off, failing to stabilize C\u2500C coupling intermediates without poisoning active sites. Herein, we circumvent this thermodynamic limit by constructing atomically asymmetric Pd\n                    <jats:sub>1<\/jats:sub>\n                    \u2500O\u2500Cu interfaces derived from the partial\n                    <jats:italic>operando<\/jats:italic>\n                    reconstruction of a metal\u2212organic framework (\n                    <jats:bold>CuPd\u2010THQ<\/jats:bold>\n                    ), where isolated Pd single atoms are anchored on Cu\n                    <jats:sub>2<\/jats:sub>\n                    O nanoislands (\n                    <jats:bold>\n                      Pd\/Cu\n                      <jats:sub>2<\/jats:sub>\n                      O\/CuPd\u2010THQ\n                    <\/jats:bold>\n                    ). The strong CO affinity of Pd drives the migration of remote *CO species toward the Pd center via a spillover effect. This catalyst achieves an industrial\u2010level acetate Faradaic efficiency of 82.3% (purity of 96%) and sustains performance for over 400 h at 250\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    under \u22121.0\u00a0V versus RHE, significantly outperforming conventional Cu\u2010based catalysts. Furthermore, in a membrane electrode assembly (MEA) system, it delivers a remarkable acetate yield rate of 6367.7\u00a0mg L\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , demonstrating scalable viability. Mechanism studies reveal that this atomic\u2010scale geometric isolation allows for the independent optimization of *CO and *CCO binding energetics. Our findings provide a generalizable strategy for breaking scaling relations in complex multi\u2010electron electrocatalysis.\n                  <\/jats:p>","DOI":"10.1002\/anie.1174032","type":"journal-article","created":{"date-parts":[[2026,8,13]],"date-time":"2026-08-13T15:49:16Z","timestamp":1786636156000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Atomically Asymmetric Pd\n                    <sub>1<\/sub>\n                    \u2500O\u2500Cu Interfaces Break the Activity\u2013Selectivity Limit in CO\u2010to\u2010Acetate Conversion"],"prefix":"10.1002","volume":"65","author":[{"given":"Zhi\u2010Xin","family":"Li","sequence":"first","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE For Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2013Sen University  Guangzhou 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