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Herein, an ultramicroporous HOF, HOF\u201036, with pyridine\u2010functionalized pore surfaces, was synthesized from 4,4\u2032,4\u2033,4\u2034\u2010(pyridine\u20102,3,5,6\u2010tetrayl)tetrabenzoic acid. According to the single\u2010component sorption isotherm, the activated HOF\u201036 (HOF\u201036a) exhibits preferential adsorption toward ethane (C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    ) and propylene (C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    ) over C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    , with IAST selectivities of 1.6 for C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    and 13.1 for C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    mixtures at 298\u00a0K, where the C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    selectivity surpasses those of all previously reported HOFs. Dynamic breakthrough experiments demonstrate that HOF\u201036a enables one\u2010step purification of polymer\u2010grade C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (\u2265 99.99%) from binary and ternary MTO\u2010related hydrocarbon mixtures. Notably, HOF\u201036a affords a C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    productivity of 1.1\u00a0L kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    for the challenging ternary C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    \/C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (33.3\/33.3\/33.3,\n                    <jats:italic>v<\/jats:italic>\n                    \/\n                    <jats:italic>v<\/jats:italic>\n                    \/\n                    <jats:italic>v<\/jats:italic>\n                    ) mixture. Moreover, the separation performance remains nearly unchanged under humid conditions and repeated breakthrough cycles. Theoretical calculations reveal that the pyridine\u2010functionalized pore surface strengthens the binding affinity toward C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    and C\n                    <jats:sub>3<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    through enhanced host\u2013guest interactions. This work demonstrates the potential of HOFs for challenging multicomponent olefin separation and highlights pore environment engineering for regulating host\u2013guest interactions.\n                  <\/jats:p>","DOI":"10.1002\/anie.5126918","type":"journal-article","created":{"date-parts":[[2026,9,9]],"date-time":"2026-09-09T04:33:45Z","timestamp":1788928425000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Modulating the Pore Environment of a Hydrogen\u2010Bonded Organic Framework for Efficient Separation of a Ternary Mixture of Methanol\u2010to\u2010Olefin Products"],"prefix":"10.1002","volume":"65","author":[{"given":"Xiantao","family":"Zhong","sequence":"first","affiliation":[{"name":"Guizhou Key Laboratory of Macrocyclic and Supramolecular Chemistry School of Chemistry and Chemical Engineering Guizhou University  Guiyang 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