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Here, we report the highly efficient separation of C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    and C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    mixtures with isostructural metal\u2010containing hydrogen\u2010bonded organic frameworks (M\u2013HOFs), which feature micropore channels decorated with high\u2010density and uncoordinated carboxyl groups. Single\u2010crystal X\u2010ray diffraction analysis reveals that each free carboxyl group is capable of trapping one C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    molecule through hydrogen bonding. This endows the M\u2013HOFs with excellent C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    capture capability, achieving a benchmark storage density of 396.0\u00a0mg cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    , while simultaneously demonstrating remarkable selectivity over C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (420\u201397) and CO\n                    <jats:sub>2<\/jats:sub>\n                    (188\u201353). Breakthrough experiments confirm that binary gas mixtures can be efficiently separated by M\u2013HOFs, where an impressive C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    productivity (137.4\u00a0mol kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) is realized in the separation of C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (1\/99), and an outstanding separation factor (17) is achieved for C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    (50\/50) splitting. Coupled with their superior chemical stability, these M\u2013HOFs display tremendous potential for practical applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.202514417","type":"journal-article","created":{"date-parts":[[2025,9,30]],"date-time":"2025-09-30T08:01:27Z","timestamp":1759219287000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":22,"title":["Microporous Metal\u2010Containing Hydrogen\u2010Bonded Organic Frameworks with Benchmark C\n                    <sub>2<\/sub>\n                    H\n                    <sub>2<\/sub>\n                    Storage Density for Efficient C\n                    <sub>2<\/sub>\n                    H\n                    <sub>2<\/sub>\n                    \/C\n                    <sub>2<\/sub>\n                    H\n                    <sub>4<\/sub>\n                    and C\n                    <sub>2<\/sub>\n                    H\n                    <sub>2<\/sub>\n                    \/CO\n                    <sub>2<\/sub>\n                    Separations"],"prefix":"10.1002","volume":"64","author":[{"given":"Jiali","family":"Fu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingxue","family":"Hui","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu\u2010Hao","family":"Gu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 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Numbers 2442970 (for Ni\u2013HOF) 2442972 (for acetylene\u2010loaded Ni\u2013HOF) 2463713 (for acetylene\u2010loaded Co\u2013HOF) 2482120 (for empty ethylene\u2010loaded Co\u2013HOF) contain the supplementary crystallographic data for this paper. These data are provided free of charge by the joint Cambridge Crystallographic Data Centre and Fachinformationszentrum Karlsruhe Access Structures service."}],"container-title":["Angewandte Chemie International Edition"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.202514417","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/full-xml\/10.1002\/anie.202514417","content-type":"application\/xml","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.202514417","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T16:04:35Z","timestamp":1790697875000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/anie.202514417"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2025,9,30]]},"references-count":65,"journal-issue":{"issue":"48","published-print":{"date-parts":[[2025,11,24]]}},"alternative-id":["10.1002\/anie.202514417"],"URL":"https:\/\/doi.org\/10.1002\/anie.202514417","archive":["Portico"],"relation":{},"ISSN":["1433-7851","1521-3773"],"issn-type":[{"value":"1433-7851","type":"print"},{"value":"1521-3773","type":"electronic"}],"subject":[],"published":{"date-parts":[[2025,9,30]]},"assertion":[{"value":"2025-07-02","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-09-22","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-09-30","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e202514417"}}