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The purification of olefin mixture is an essential part in the MTO process where membrane technology has emerged as a high\u2010efficiency and energy\u2010saving approach. However, it remains a critical challenge to achieve precise sieving of C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    and C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    due to their similar molecular size. Herein, we report an interfacial coordination induced sub\u2010angstrom channel regulation strategy and achieve unprecedented cut\u2010off shift of ZIF\u20108 from C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    \/C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>8<\/jats:sub>\n                    to C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    \/C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    . Ionic covalent organic framework with crystalline structure and high\u2010density sulfonate groups was used as growth template for ZIF\u20108 membrane. The coordination between sulfonate groups and Zn\n                    <jats:sup>2+<\/jats:sup>\n                    ions induced lattice contraction of ZIF\u20108 framework, which is confirmed by XRD patterns and molecular dynamic simulations. The resulting membranes demonstrate a distinct cut\u2010off between C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    and C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    , achieving a C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    permeance of 405 GPU and an exceptional C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    \/C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    selectivity of 45, surpassing the separation performance of all reported membranes. Finally, we demonstrate the excellent scalability of this strategy by fabricating large area flat sheet membrane (&gt;500\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    ) on polymer substrates.\n                  <\/jats:p>","DOI":"10.1002\/anie.202522321","type":"journal-article","created":{"date-parts":[[2025,11,19]],"date-time":"2025-11-19T08:38:23Z","timestamp":1763541503000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Benchmark C\n                    <sub>2<\/sub>\n                    H\n                    <sub>4<\/sub>\n                    \/C\n                    <sub>3<\/sub>\n                    H\n                    <sub>6<\/sub>\n                    Separation in MOF\u2013COF Bilayer Membranes via Interfacial Coordination Induced Sub\u2010Angstrom Channel Regulation"],"prefix":"10.1002","volume":"65","author":[{"given":"Hanze","family":"Ma","sequence":"first","affiliation":[{"name":"Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and Technology, Tianjin University  Tianjin 300072 China"},{"name":"Haihe Laboratory of Sustainable Chemical Transformations  Tianjin 300192 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Heyang","family":"Liu","sequence":"additional","affiliation":[{"name":"Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and Technology, Tianjin University  Tianjin 300072 China"},{"name":"Haihe Laboratory of Sustainable Chemical Transformations  Tianjin 300192 China"},{"name":"Shanxi Research Institute of Huairou Laboratory  Taiyuan 030032 China"},{"name":"Beijing Huairou Laboratory  Beijing 101400 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