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Herein, we reported a cage engineering strategy in anion\u2010pillared metal\u2010organic frameworks (APMOFs) for efficient C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    and CO\n                    <jats:sub>2<\/jats:sub>\n                    capture simultaneously. Specifically, two stable ZrF\n                    <jats:sub>6<\/jats:sub>\n                    <jats:sup>2\u2212<\/jats:sup>\n                    anion\u2010pillared cage\u2010type MOFs (ZNU\u201017 and ZNU\u201027) are prepared with both ultramicroporous (\u223c4\u00a0\u00c5) and microporous (&gt;7\u00a0\u00c5) cages but featuring different shapes. While ZNU\u201017 allows the efficient binary 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                    separation, ZNU\u201027 enables the benchmark ternary C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    separation by increasing the adsorption affinity toward CO\n                    <jats:sub>2<\/jats:sub>\n                    . Notably, remarkably increased C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    (170.1\u00a0cm\n                    <jats:sup>3<\/jats:sup>\n                    \u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0versus 120.1 cm\n                    <jats:sup>3<\/jats:sup>\n                    \u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and CO\n                    <jats:sub>2<\/jats:sub>\n                    (91.8\u00a0cm\n                    <jats:sup>3<\/jats:sup>\n                    \u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0versus 64.5 cm\n                    <jats:sup>3<\/jats:sup>\n                    \u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) adsorption capacities are achieved in ZNU\u201027, and the IAST selectivity of ZNU\u201027 for CO\n                    <jats:sub>2<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    is 4.3 times as high as that of ZNU\u201017 (6.5\u00a0versus 1.5). The 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>4<\/jats:sub>\n                    binding sites in ZNU\u201027 are studied by gas loaded in situ single crystal structure and density functional theory (DFT) calculation, which revealed that the unique fluorinated 8.5\u00a0\u00c5 spherical cages provide strong hydrogen binding or electrostatic interactions for C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    and CO\n                    <jats:sub>2<\/jats:sub>\n                    . Dynamic breakthrough tests show that from a C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (1\/9\/90) mixture, polymer\u2010grade C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (\u226599.99%) can be obtained in ZNU\u201027 with a high productivity of 12.04\u00a0mol\u00a0kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    .\n                  <\/jats:p>","DOI":"10.1002\/anie.202514808","type":"journal-article","created":{"date-parts":[[2025,8,4]],"date-time":"2025-08-04T07:20:32Z","timestamp":1754292032000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":21,"title":["Cage Engineering in Anion\u2010Pillared MOFs for Benchmark One\u2010Step C\n                    <sub>2<\/sub>\n                    H\n                    <sub>4<\/sub>\n                    Purification from Ternary C\n                    <sub>2<\/sub>\n                    H\n                    <sub>2<\/sub>\n                    \/CO\n                    <sub>2<\/sub>\n                    \/C\n                    <sub>2<\/sub>\n                    H\n                    <sub>4<\/sub>\n                    Mixtures"],"prefix":"10.1002","volume":"64","author":[{"given":"Lingyao","family":"Wang","sequence":"first","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Catalysis and Adsorption Materials, Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science Zhejiang Normal University  Jinhua 321004 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huirong","family":"Chen","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Catalysis and Adsorption Materials, Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science Zhejiang Normal University  Jinhua 321004 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chengye","family":"Lou","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Catalysis and Adsorption Materials, Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science Zhejiang Normal University  Jinhua 321004 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guangzu","family":"Xiong","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Catalysis and Adsorption Materials, Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science Zhejiang Normal University  Jinhua 321004 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunjia","family":"Jiang","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Catalysis and Adsorption Materials, Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science Zhejiang Normal University  Jinhua 321004 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Banglin","family":"Chen","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Catalysis and Adsorption Materials, Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science Zhejiang Normal University  Jinhua 321004 P.R. China"},{"name":"Fujian Provincial Key Laboratory of Polymer Materials, College of Chemistry &amp; Materials Science Fujian Normal University  Fuzhou 350007 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8268-384X","authenticated-orcid":false,"given":"Yuanbin","family":"Zhang","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Advanced Catalysis and Adsorption Materials, Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science Zhejiang Normal University  Jinhua 321004 P.R. 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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.202514808","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,10,14]],"date-time":"2025-10-14T12:04:10Z","timestamp":1760443450000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/anie.202514808"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2025,8,4]]},"references-count":58,"journal-issue":{"issue":"40","published-print":{"date-parts":[[2025,9,26]]}},"alternative-id":["10.1002\/anie.202514808"],"URL":"https:\/\/doi.org\/10.1002\/anie.202514808","archive":["Portico"],"relation":{},"ISSN":["1433-7851","1521-3773"],"issn-type":[{"value":"1433-7851","type":"print"},{"value":"1521-3773","type":"electronic"}],"subject":[],"published":{"date-parts":[[2025,8,4]]},"assertion":[{"value":"2025-07-07","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-07-28","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-08-04","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e202514808"}}