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Herein, we report a series of isostructural pillar\u2010layered metal\u2013organic frameworks (MOFs), named JNU\u201013, JNU\u201013\u2010CH\n                    <jats:sub>3<\/jats:sub>\n                    , and JNU\u201013\u2010(CH\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    . These MOFs feature one\u2010dimensional (1D) channels integrated with orthogonally arrayed side pockets, enabling dense packing of C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    molecules while maintaining rapid diffusion pathways. Specifically, JNU\u201013\u2010CH\n                    <jats:sub>3<\/jats:sub>\n                    achieves a high C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    packing density of 360 g L\n                    <jats:sup>\u22121<\/jats:sup>\n                    , a low adsorption enthalpy of 31.61 kJ mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    , and adsorption\/desorption coefficients one to two orders of magnitude higher than other benchmark MOFs. Breakthrough experiments reveal a high C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    capture capacity of 3.46 mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    from an equimolar C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \/CO\n                    <jats:sub>2<\/jats:sub>\n                    mixture at 298 K and 1 bar, even under humid conditions. Moreover, we demonstrate the scale\u2010up synthesis of JNU\u201013\u2010CH\n                    <jats:sub>3<\/jats:sub>\n                    and gas\u2010cylinder collection of high\u2010purity C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    , achieving &gt;99.9% 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                    (95\/5) mixture and &gt;99.7% 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                    \/CH\n                    <jats:sub>4<\/jats:sub>\n                    (95\/2.5\/2.5) mixture. Overall, this study highlights the effectiveness of orthogonal\u2010arrayed side pockets for balancing dense packing and mass transport, offering a promising strategy for energy\u2010efficient C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    purification.\n                  <\/jats:p>","DOI":"10.1002\/anie.202523562","type":"journal-article","created":{"date-parts":[[2025,12,16]],"date-time":"2025-12-16T14:21:31Z","timestamp":1765894891000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["One\u2010Dimensional Channel with Side Pockets for Rapid Diffusion and Efficient C\n                    <sub>2<\/sub>\n                    H\n                    <sub>2<\/sub>\n                    Purification"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6780-8272","authenticated-orcid":false,"given":"Xiao\u2010Jing","family":"Xie","sequence":"first","affiliation":[{"name":"College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou 510632 P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhi\u2010Hao","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou 510632 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yisi","family":"Yang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou 510632 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2298-7347","authenticated-orcid":false,"given":"Heng","family":"Zeng","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou 510632 P.R. 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