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However, inefficient ion transport limits the efficiency and scalability for CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction under such conditions. Here, we address the limitation through cation effect\u2010engineered electrocatalytic interfaces that optimize hydroxide ion dynamics. By integrating a quaternary ammonia poly(\n                    <jats:italic>N<\/jats:italic>\n                    \u2010methyl\u2010piperidine\u2010co\u2010p\u2010terphenyl) (QAPPT) structural layer with a cation\u2010engineered poly(\n                    <jats:italic>N<\/jats:italic>\n                    \u2010methyl\u2010piperidine\u2010co\u2010biphenyl) (QAPPB) overlayer, we construct a double\u2010layer membrane (DLM) with optimized ion\u2010conduction pathways. The QAPPB overlayer, with ultrahigh ion\u2010exchange capacity, enhances CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction selectivity by accelerating hydroxide mobility under high current densities. This architecture achieves 93% Faradaic efficiency for CO production at 500\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in pure water, sustaining stable operation for over 100 h. Scaling the system to a 100 cm\n                    <jats:sup>2<\/jats:sup>\n                    electrolyzer achieves a CO production rate of 344\u00a0mL min\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 50 A, highlighting system\u2010level robustness. By coupling cationic polymer design with ion\u2010transport kinetics, our work advances electrocatalytic interfaces for efficient pure\u2010water CO\n                    <jats:sub>2<\/jats:sub>\n                    electrolysis.\n                  <\/jats:p>","DOI":"10.1002\/anie.202516321","type":"journal-article","created":{"date-parts":[[2025,12,1]],"date-time":"2025-12-01T09:09:41Z","timestamp":1764580181000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Cation Effect\u2010Engineered Electrocatalytic Interfaces Boost Pure\u2010Water CO\n                    <sub>2<\/sub>\n                    Electrolysis with Optimized Ion Dynamics"],"prefix":"10.1002","volume":"65","author":[{"given":"Haonan","family":"Xu","sequence":"first","affiliation":[{"name":"Department of Chemistry Zhejiang University  Hangzhou 310058 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Zhejiang University  Hangzhou Zhejiang 311200 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6802-3095","authenticated-orcid":false,"given":"Bing","family":"Shan","sequence":"additional","affiliation":[{"name":"Department of Chemistry Zhejiang University  Hangzhou 310058 China"},{"name":"Key Laboratory of Excited\u2010State Materials of Zhejiang Province  Hangzhou 310058 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