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Herein, we demonstrate the systematic design of a pillared\u2010layer MOF series (CPL\u20101) to achieve optimal host\u2013guest fit through increasing the number of bulky groups, progressively enhancing the C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    adsorption performance. The newly synthesized, best\u2010fit\n                    <jats:bold>SXU\u201010<\/jats:bold>\n                    exhibits the most superior very\u2010low\u2010pressure C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    capture\u2014reaching near saturation at just 2\u00a0kPa. With record C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    packing densities of 483.9\u00a0mg cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    at 1\u00a0kPa and 733.97\u00a0mg cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    at 100\u00a0kPa,\n                    <jats:bold>SXU\u201010<\/jats:bold>\n                    exhibits an uptake of 1.18\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    at 1\u00a0kPa 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                    selectivity of 133 for 1\/99 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 (all at 298\u00a0K), along with exceptional stability and humidity tolerance, enabling the production of polymer\u2010grade C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    from trace C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    mixtures under a challenging humid condition (80% RH). The unusual steep\u2010rise\u2010uptake phenomenon and significantly improved performance are attributed to the optimized host\u2013guest shape fit at a sub\u2010\u00e5ngstr\u00f6m precision which constrains the gate\u2010opening flexibility, evidenced via in situ single\u2010crystal X\u2010ray diffraction. The present study sheds light on the molecular\u2010level engineering of bioinspired porous adaptive materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.202524692","type":"journal-article","created":{"date-parts":[[2025,12,27]],"date-time":"2025-12-27T06:34:11Z","timestamp":1766817251000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Optimal Host\u2013Guest Fit in Metal\u2010Organic Frameworks to Achieve Record C\n                    <sub>2<\/sub>\n                    H\n                    <sub>2<\/sub>\n                    Packing Density for Trace Acetylene Capture"],"prefix":"10.1002","volume":"65","author":[{"given":"Jun\u2010Hao","family":"Wang","sequence":"first","affiliation":[{"name":"Institute of Crystalline Materials Shanxi University  Taiyuan 030006 China"},{"name":"Institute of Molecular Science Shanxi University  Taiyuan 030006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu\u2010Chi","family":"Wan","sequence":"additional","affiliation":[{"name":"Institute of Crystalline Materials Shanxi University  Taiyuan 030006 China"},{"name":"Institute of Molecular Science Shanxi University  Taiyuan 030006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ji\u2010Ning","family":"Cao","sequence":"additional","affiliation":[{"name":"Institute of Crystalline Materials Shanxi University  Taiyuan 030006 China"},{"name":"Institute of Molecular Science Shanxi University  Taiyuan 030006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ye\u2010Fan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Institute of Crystalline Materials Shanxi University  Taiyuan 030006 China"},{"name":"Institute of Molecular Science Shanxi University  Taiyuan 030006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui\u2010Min","family":"Wu","sequence":"additional","affiliation":[{"name":"Institute of Crystalline Materials Shanxi University  Taiyuan 030006 China"},{"name":"Institute of Molecular Science Shanxi University  Taiyuan 030006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hai\u2010Feng","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Chemical Engineering Shantou University Chemistry and Chemical Engineering Guangdong Laboratory  Guangdong 515000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xu\u2010Dong","family":"Wu","sequence":"additional","affiliation":[{"name":"College of Chemistry and Chemical Engineering Shantou University Chemistry and Chemical Engineering Guangdong Laboratory  Guangdong 515000 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Numbers 2468384 (for ZU\u2010901\u2010C2H2) 2468385 (for CPL\u20101\u2010C2H2) 2468386 (for ZU\u2010901\u2010H2O) 2468387 (for CPL\u20101) 2468388 (for ZU\u2010901) 2468389 (for SXU\u201010\u2010H2O) 2468390 (for SXU\u201010\u2010C2H2) 2468391 (for SXU\u201010) and 2468392 (for CPL\u20101\u2010H2O)https:\/\/www.ccdc.cam.ac.uk\/services\/structures?id=https:\/\/doi.org\/10.1002\/anie.202524692contains the supplementary crystallographic data for this paper. These data are provided free of charge by the joint Cambridge Crystallographic Data Centre and Fachinformationszentrum Karlsruhehttp:\/\/www.ccdc.cam.ac.uk\/structuresAccess Structures service."}],"container-title":["Angewandte Chemie International Edition"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.202524692","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/full-xml\/10.1002\/anie.202524692","content-type":"application\/xml","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.202524692","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,10,17]],"date-time":"2026-10-17T17:10:41Z","timestamp":1792257041000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/anie.202524692"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2025,12,26]]},"references-count":55,"journal-issue":{"issue":"7","published-print":{"date-parts":[[2026,2,9]]}},"alternative-id":["10.1002\/anie.202524692"],"URL":"https:\/\/doi.org\/10.1002\/anie.202524692","archive":["Portico"],"relation":{},"ISSN":["1433-7851","1521-3773"],"issn-type":[{"value":"1433-7851","type":"print"},{"value":"1521-3773","type":"electronic"}],"subject":[],"published":{"date-parts":[[2025,12,26]]},"assertion":[{"value":"2025-11-08","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-12-21","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-12-26","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e24692"}}