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Pore space partition (PSP) has shown promise in enhancing gas adsorption capacity and selectivity by reducing pore size and increasing the density of guest binding sites. Herein, we firstly employ the 2D\u21923D polycatenation strategy to construct a PSP metal\u2010organic framework (MOF)\n                    <jats:bold>Ni\u2010dcpp\u2010bpy<\/jats:bold>\n                    , incorporating functional N\/O sites to enhance C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    purification. The polycatenated framework with optimized pore size and regularity, exhibiting significant improvements over traditional PSP MOFs by resolving the critical contradiction of balancing C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    uptake (98.5\u2005cm\n                    <jats:sup>3<\/jats:sup>\n                    \u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 298\u2009K, 100\u2005kPa) and selectivity 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                    (3.4), 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                    (5.9), and C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/CH\n                    <jats:sub>4<\/jats:sub>\n                    (96.4) in a MOF. Breakthrough experiments confirm high\u2010purity C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (&gt;99.9\u2009%) and high C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    productivity from binary and ternary mixtures. Notably,\n                    <jats:bold>Ni\u2010dcpp\u2010bpy<\/jats:bold>\n                    exhibits excellent water stability, scalability, and regenerability after 20 cycles for separating C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    . Theoretical calculations verify that the strong binding of C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    is mainly attributed to the C\u2212H\u22c5\u22c5\u22c5O\/N interactions between host\n                    <jats:bold>Ni\u2010dcpp\u2010bpy<\/jats:bold>\n                    and guest C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    molecules. The polycatenation strategy not only improved industrial C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    purification efficiency but also enriched the design diversity of customized MOFs for other gas separation applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.202421992","type":"journal-article","created":{"date-parts":[[2024,12,13]],"date-time":"2024-12-13T04:00:49Z","timestamp":1734062449000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":26,"title":["A Scalable Pore\u2010space\u2010partitioned Metal\u2010organic Framework Powered by Polycatenation Strategy for Efficient Acetylene Purification"],"prefix":"10.1002","volume":"64","author":[{"given":"Zhen\u2010Hua","family":"Guo","sequence":"first","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, Shaanxi Key Laboratory of Physico-Inorganic Chemistry, College of Chemistry and Materials Science Northwest University  Xi'an 710127 P. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1283-6334","authenticated-orcid":false,"given":"Dong\u2010Sheng","family":"Li","sequence":"additional","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, Shaanxi Key Laboratory of Physico-Inorganic Chemistry, College of Chemistry and Materials Science Northwest University  Xi'an 710127 P. R. China"},{"name":"College of Materials and Chemical Engineering Hubei Provincial Collaborative Innovation Center for New Energy Microgrid Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials China Three Gorges University  No. 8, Daxue Road Yichang 443002 P. R. 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