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Here, we propose a direct high\u2010purity CO electrosynthesis strategy employing an innovative electrolyte, termed porous electrolyte (PE), based on \u201cporous water\u201d. Zeolite nanocrystals within PE provide permanent pores in the liquid phase, enabling physical CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption through an intraparticle diffusion model, as demonstrated by molecular dynamics simulations and in situ spectral analysis. Captured CO\n                    <jats:sub>2<\/jats:sub>\n                    spontaneously desorbs under applied reductive potential, driven by the interfacial CO\n                    <jats:sub>2<\/jats:sub>\n                    concentration gradient, and is subsequently reduced electrochemically. The high CO\n                    <jats:sub>2<\/jats:sub>\n                    concentration in PE enhances mass transfer, and surface ion exchange between Si\u2212OH groups and K\n                    <jats:sup>+<\/jats:sup>\n                    ions on the zeolite surface generates a stronger interfacial electric field, promoting electron transfer steps. This optimized kinetics for mass and electron transfer confers heightened intrinsic activity toward CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction. The PE\u2010based electrolysis system demonstrated superior CO Faradaic efficiency and partial current density compared to the conventional CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010fed system. A circular system using PE and a Ni\u2212N\/C cathode realized continuous production of high\u2010purity CO (97.0\u2005wt\u2009%) from dilute CO\n                    <jats:sub>2<\/jats:sub>\n                    (15\u2009%) and maintained &gt;90.0\u2005wt\u2009% under 150\u2005mA\u2009cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , with significantly reduced energy consumption and costs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202424104","type":"journal-article","created":{"date-parts":[[2025,2,5]],"date-time":"2025-02-05T23:10:16Z","timestamp":1738797016000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Electrolyte Design Using \u201cPorous Water\u201d for High\u2010purity Carbon Monoxide Electrosynthesis from Dilute Carbon Dioxide"],"prefix":"10.1002","volume":"64","author":[{"given":"Wei","family":"Zhang","sequence":"first","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha 410004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Minyang","family":"Dai","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha 410004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhouliangzi","family":"Zeng","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha 410004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yahan","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha 410004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yan","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha 410004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenpeng","family":"Ni","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha 410004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuangyin","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chem\/Bio-Sensing and Chemometrics Advanced Catalytic Engineering Research Center of the Ministry of Education College of Chemistry and Chemical Engineering Hunan University  Changsha 410082 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6651-2752","authenticated-orcid":false,"given":"Shiguo","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha 410004 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,2,12]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-50118-1"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202205262"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2018.10.015"},{"key":"e_1_2_7_5_1","unstructured":"\u00a0"},{"key":"e_1_2_7_6_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-019-1681-6"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1038\/nclimate3231"},{"key":"e_1_2_7_8_2","author":"Ma X.","year":"2024","journal-title":"Nat. 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