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Current metal\u2013organic frameworks (MOFs) lack the ideal CO\n                    <jats:sub>2<\/jats:sub>\n                    \u00a0&gt;\u00a0C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    \u00a0&gt;\u00a0C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    adsorption sequence necessary for stepwise removal of impurities. Herein, we address this gap through precise pore environment tuning within an isoreticular series of zinc\u2013triazole MOFs. By modulating the number and position of \u2500NH\n                    <jats:sub>2<\/jats:sub>\n                    \/\u2500CH\n                    <jats:sub>3<\/jats:sub>\n                    groups on the ligand, we precisely control pore chemistry from one\u2010dimensional (1D) channels to two\u2010dimensional (2D) interconnected channels, which successfully achieves the targeted adsorption order. The unilateral amino groups in the optimized MOF,\n                    <jats:bold>ZSTU\u201030<\/jats:bold>\n                    , create unique supramolecular interlocking sites that strongly bind CO\n                    <jats:sub>2<\/jats:sub>\n                    while mitigating interactions with C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    and C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    . Consequently,\n                    <jats:bold>ZSTU\u201030<\/jats:bold>\n                    enables the direct production of polymer\u2010grade C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (&gt; 99.9%) from a ternary gas mixture in a single step, with an exceptional C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    productivity of 3.18\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    . The CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2013host interaction mechanism is elucidated by in situ single\u2010crystal X\u2010ray diffraction and theoretical calculations, which reveal multiple supramolecular interactions at the adsorption sites. Combining excellent water and pH stability,\n                    <jats:bold>ZSTU\u201030<\/jats:bold>\n                    stands out as a robust and promising physisorbent for one\u2010step C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    purification.\n                  <\/jats:p>","DOI":"10.1002\/anie.202522675","type":"journal-article","created":{"date-parts":[[2025,11,20]],"date-time":"2025-11-20T07:14:56Z","timestamp":1763622896000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":31,"title":["Programmed Pore Engineering in an Isoreticular Triazole\u2013MOF Series for One\u2010Step Ethylene Separation"],"prefix":"10.1002","volume":"65","author":[{"given":"Xue","family":"Wang","sequence":"first","affiliation":[{"name":"China\u2010Uzbekistan Joint Laboratory on Advanced Porous Materials State Key Laboratory of Bio\u2010based Fiber Materials School of Materials Science and Engineering Zhejiang Sci\u2010Tech University  Hangzhou 310018 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tao","family":"Zhao","sequence":"additional","affiliation":[{"name":"China\u2010Uzbekistan Joint Laboratory on Advanced Porous Materials State Key Laboratory of Bio\u2010based Fiber Materials School of Materials Science and Engineering Zhejiang Sci\u2010Tech University  Hangzhou 310018 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiacheng","family":"Li","sequence":"additional","affiliation":[{"name":"China\u2010Uzbekistan Joint Laboratory on Advanced Porous Materials State Key Laboratory of Bio\u2010based Fiber Materials School of Materials Science and Engineering Zhejiang Sci\u2010Tech University  Hangzhou 310018 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruizhi","family":"Wei","sequence":"additional","affiliation":[{"name":"China\u2010Uzbekistan Joint Laboratory on Advanced Porous Materials State Key Laboratory of Bio\u2010based Fiber Materials School of Materials Science and Engineering Zhejiang Sci\u2010Tech University  Hangzhou 310018 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xianlong","family":"Xia","sequence":"additional","affiliation":[{"name":"China\u2010Uzbekistan Joint Laboratory on Advanced Porous Materials State Key Laboratory of Bio\u2010based Fiber Materials School of Materials Science and Engineering Zhejiang Sci\u2010Tech University  Hangzhou 310018 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9778-4312","authenticated-orcid":false,"given":"Junkuo","family":"Gao","sequence":"additional","affiliation":[{"name":"China\u2010Uzbekistan Joint Laboratory on Advanced Porous Materials State Key Laboratory of Bio\u2010based Fiber Materials School of Materials Science and Engineering Zhejiang Sci\u2010Tech University  Hangzhou 310018 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,11,19]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2025.216833"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201057489\u2010z"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201908275"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/532435a"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c15141"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202422135"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsmaterialslett.4c02230"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010020\u20100431\u20103"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2025.162717"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929\u2010024\u201001250\u20100"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1039\/C9CS00756C"},{"key":"e_1_2_7_12_1","first-page":"259","volume":"6","author":"Zhang X.\u2010W.","year":"2025","journal-title":"Acc. 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