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Based on theoretical and experimental analyses, we show that an inherent trade\u2010off exists: increasing cation concentrations improves Faradaic efficiency (FE) toward CO\n                    <jats:sub>2<\/jats:sub>\n                    R products but comes at the expense of reduced SPCE. We demonstrate a polyimide\u2010modification strategy to overcome this trade\u2010off by taking advantage of the amino groups that can effectively capture protons, creating a local alkaline microenvironment surrounding the electrode surface. In a proof\u2010of\u2010concept experiment, SnO\n                    <jats:sub>2<\/jats:sub>\n                    nanoparticles were modified with polyimide and acted as a CO\n                    <jats:sub>2<\/jats:sub>\n                    R catalyst, which achieved, simultaneously, near\u2010ideal SPCE of 95.7% and FE of 96% (toward HCOOH) at pH 1.36 with dilute potassium ions down to even 0.1\u00a0M. We expect that these findings will accelerate the development of carbon\u2010 and electron\u2010efficient acidic CO\n                    <jats:sub>2<\/jats:sub>\n                    electrolysis.\n                  <\/jats:p>","DOI":"10.1002\/anie.202503539","type":"journal-article","created":{"date-parts":[[2025,4,14]],"date-time":"2025-04-14T22:44:37Z","timestamp":1744670677000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":42,"title":["Acidic CO\n                    <sub>2<\/sub>\n                    Electrolysis With Near\u2010Ideal Selectivity and Carbon Efficiency Enabled by Overcoming Its Inherent Trade\u2010Off"],"prefix":"10.1002","volume":"64","author":[{"given":"Li\u2010Ping","family":"Chi","sequence":"first","affiliation":[{"name":"Division of Nanomaterials &amp; Chemistry, Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 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Microscale University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ye\u2010Cheng","family":"Li","sequence":"additional","affiliation":[{"name":"Division of Nanomaterials &amp; Chemistry, Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tian\u2010Yun","family":"Zhang","sequence":"additional","affiliation":[{"name":"Division of Nanomaterials &amp; Chemistry, Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shu\u2010Ping","family":"Sun","sequence":"additional","affiliation":[{"name":"Division of Nanomaterials &amp; Chemistry, Hefei National Research Center for Physical Sciences at the Microscale University of 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