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While the state\u2010of\u2010the\u2010art membranes are CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010selective, CH\n                    <jats:sub>4<\/jats:sub>\n                    \u2010selective membranes remain elusive, with potential applications in the recovery and purification of methane\u2010rich gases such as biogas and landfill gas. Herein, we report a molybdenum\u2010oxygen (Mo\u2500O) functionalized MFI\u2010type zeolite membrane for inverse CH\n                    <jats:sub>4<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    gas separation. A pure\u2010silica MFI\u2010type zeolite membrane is first seeded grown on an alumina support and subsequently functionalized via facile impregnation and calcination of sodium molybdate. The as\u2010prepared membrane features uniform pores (0.5\u00a0nm) and ultrasmall Mo\u2500O clusters (1.6\u00a0nm). The Mo\u2500O\/MFI membrane selectively permeates CH\n                    <jats:sub>4<\/jats:sub>\n                    over CO\n                    <jats:sub>2<\/jats:sub>\n                    , achieving an unprecedented CH\n                    <jats:sub>4<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    separation factor of 11.8 alongside a high CH\n                    <jats:sub>4<\/jats:sub>\n                    permeance of 2.1\u00a0\u00d7\u00a010\n                    <jats:sup>\u22128<\/jats:sup>\n                    \u00a0mol s\n                    <jats:sup>\u22121<\/jats:sup>\n                    m\n                    <jats:sup>\u22122<\/jats:sup>\n                    Pa\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Experimental measurements and theoretical calculations reveal that CH\n                    <jats:sub>4<\/jats:sub>\n                    preferentially adsorbs onto Mo\u2500O clusters via hydrogen bond and diffuses rapidly through MFI zeolite pores. This study represents the first demonstration of porous membranes enabling inverse CH\n                    <jats:sub>4<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    separation and offers guidance for the design of next\u2010generation CH\n                    <jats:sub>4<\/jats:sub>\n                    \u2010selective membranes.\n                  <\/jats:p>","DOI":"10.1002\/anie.202523824","type":"journal-article","created":{"date-parts":[[2025,11,30]],"date-time":"2025-11-30T04:57:18Z","timestamp":1764478638000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["MFI Zeolite Membrane with Surface Mo\u2500O Clusters for Inverse CH\n                    <sub>4<\/sub>\n                    \/CO\n                    <sub>2<\/sub>\n                    Separation"],"prefix":"10.1002","volume":"65","author":[{"given":"Yongyan","family":"Deng","sequence":"first","affiliation":[{"name":"Faculty of Chemistry Northeast Normal University  Changchun 130024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dan","family":"Ma","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry Northeast Normal University  Changchun 130024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Zhang","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry Northeast Normal University  Changchun 130024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaxing","family":"Wu","sequence":"additional","affiliation":[{"name":"School of Energy and Environmental Engineering University of Science and Technology Beijing  Beijing 100083 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