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In this study, we report an isoreticular design strategy to fine\u2010tune the local pore chemistry of metal\u2010organic frameworks (MOFs), enabling the simultaneous selective adsorption of CO\n                    <jats:sub>2<\/jats:sub>\n                    and C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    . Through rational organic ligand engineering, the hydroxyl\u2010functionalized analogue PCP\u2010TPA\u20102OH (also termed as ZU\u2010925, ZU represents Zhejiang University) breaks the bottleneck of only C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    capture exhibited by the parent PCP\u2010TPA. The tailored synergistic binding environment of ZU\u2010925 makes it be new benchmark in one\u2010step C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    purification from CO\n                    <jats:sub>2<\/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                    ternary mixtures. Ultra\u2010purity C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    (99.99%) along with high productivity of 17.8\u00a0L kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    could be realized through only one\u2010step adsorption. Molecular simulations reveal that the preferential binding of C\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    arises from a tailored pore environment featuring aligned aromatic units and electronegative oxygen atoms, while Lewis basic hydroxyl groups locally modulate the pore chemistry, contributing to enhanced CO\n                    <jats:sub>2<\/jats:sub>\n                    capture. This study provides valuable insights into the design of advanced adsorbents for multiple impurity removal via isoreticular chemistry.\n                  <\/jats:p>","DOI":"10.1002\/anie.202518996","type":"journal-article","created":{"date-parts":[[2025,10,31]],"date-time":"2025-10-31T07:11:21Z","timestamp":1761894681000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Tailored Synergistic Binding Environment in Metal\u2010Organic Frameworks for Record One\u2010Step Ethylene Purification from Multicomponent Mixtures"],"prefix":"10.1002","volume":"64","author":[{"given":"Peixin","family":"Zhang","sequence":"first","affiliation":[{"name":"Zhejiang Key Laboratory of Intelligent Manufacturing for Functional Chemicals College of Chemical and Biological Engineering Zhejiang University  Hangzhou 310012 China"},{"name":"Engineering Research Center of Functional Materials Intelligent Manufacturing of Zhejiang Province Institute for Intelligent Bio\/Chem Manufacturing ZJU\u2010Hangzhou Global Scientific and Technological Innovation Center  Hangzhou 311200 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dengzhuo","family":"Zhou","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Intelligent Manufacturing for Functional Chemicals College of Chemical and Biological Engineering Zhejiang University  Hangzhou 310012 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xian","family":"Suo","sequence":"additional","affiliation":[{"name":"Engineering Research Center of Functional Materials Intelligent Manufacturing of Zhejiang Province Institute for Intelligent Bio\/Chem Manufacturing ZJU\u2010Hangzhou Global Scientific and Technological Innovation Center  Hangzhou 311200 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xili","family":"Cui","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Intelligent Manufacturing for Functional Chemicals College of Chemical and Biological Engineering Zhejiang University  Hangzhou 310012 China"},{"name":"Engineering Research Center of Functional Materials Intelligent Manufacturing of Zhejiang Province Institute for Intelligent Bio\/Chem Manufacturing ZJU\u2010Hangzhou Global Scientific and Technological Innovation Center  Hangzhou 311200 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2810-3023","authenticated-orcid":false,"given":"Lifeng","family":"Yang","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Intelligent Manufacturing for Functional Chemicals College of Chemical and Biological Engineering Zhejiang University  Hangzhou 310012 China"},{"name":"State Key Laboratory of Silicon Materials School of Materials Science and Engineering Zhejiang University  Hangzhou 310027 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7418-0046","authenticated-orcid":false,"given":"Huabin","family":"Xing","sequence":"additional","affiliation":[{"name":"Zhejiang Key Laboratory of Intelligent Manufacturing for Functional Chemicals College of Chemical and Biological Engineering Zhejiang University  Hangzhou 310012 China"},{"name":"Engineering Research Center of Functional Materials Intelligent Manufacturing of Zhejiang Province Institute for Intelligent Bio\/Chem Manufacturing ZJU\u2010Hangzhou Global Scientific and Technological Innovation Center  Hangzhou 311200 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,10,30]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/532435a"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44286\u2010023\u201000004\u20102"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adg2491"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8EE01332B"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202218027"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c15141"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563\u2010018\u20100206\u20102"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202104318"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abi7281"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1039\/C9CS00756C"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201806445"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/cbe.4c00035"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1039\/C7CS00153C"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aam7232"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr200190s"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3CS01163A"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202002563"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abn8418"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010021\u201003627\u20108"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaf6323"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c08726"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.202500851"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2025.162121"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202401693"},{"key":"e_1_2_7_25_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8EE01332B"},{"key":"e_1_2_7_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.iecr.9b05665"},{"key":"e_1_2_7_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/aic.18396"},{"key":"e_1_2_7_28_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaf2458"},{"key":"e_1_2_7_29_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adh0135"},{"key":"e_1_2_7_30_1","doi-asserted-by":"publisher","DOI":"10.1021\/cbe.3c00093"},{"key":"e_1_2_7_31_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.9b10923"},{"key":"e_1_2_7_32_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aat0586"},{"key":"e_1_2_7_33_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.9b00913"},{"key":"e_1_2_7_34_1","doi-asserted-by":"publisher","DOI":"10.1021\/cbe.4c00113"},{"key":"e_1_2_7_35_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010024\u201045004\u20109"},{"key":"e_1_2_7_36_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-26473-8"},{"key":"e_1_2_7_37_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202208182"},{"key":"e_1_2_7_38_1","doi-asserted-by":"publisher","DOI":"10.1002\/aic.18312"},{"key":"e_1_2_7_39_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aax8666"},{"key":"e_1_2_7_40_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.abn9231"},{"key":"e_1_2_7_41_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c10973"},{"key":"e_1_2_7_42_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202016673"},{"key":"e_1_2_7_43_1","unstructured":"Deposition 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These data can be obtained free of charge from the Cambridge Crystallographic Data Centre."},{"key":"e_1_2_7_44_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2020.126937"},{"key":"e_1_2_7_45_1","doi-asserted-by":"publisher","DOI":"10.1007\/s40843-020-1471-0"},{"key":"e_1_2_7_46_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aab1680"},{"key":"e_1_2_7_47_1","doi-asserted-by":"publisher","DOI":"10.1002\/aic.690110125"},{"key":"e_1_2_7_48_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010022\u201032677\u20103"},{"key":"e_1_2_7_49_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.2c13905"},{"key":"e_1_2_7_50_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ces.2017.09.032"},{"key":"e_1_2_7_51_1","doi-asserted-by":"publisher","DOI":"10.1002\/aic.18676"},{"key":"e_1_2_7_52_1","doi-asserted-by":"publisher","DOI":"10.1038\/ncomms9697"},{"key":"e_1_2_7_53_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c02108"},{"key":"e_1_2_7_54_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202403345"},{"key":"e_1_2_7_55_1","doi-asserted-by":"publisher","DOI":"10.1088\/0953-8984\/14\/11\/301"},{"key":"e_1_2_7_56_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202100342"},{"key":"e_1_2_7_57_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557\u2010021\u201000740\u2010z"},{"key":"e_1_2_7_58_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2024.157054"}],"container-title":["Angewandte Chemie International Edition"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.202518996","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/full-xml\/10.1002\/anie.202518996","content-type":"application\/xml","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.202518996","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,6,1]],"date-time":"2026-06-01T12:47:40Z","timestamp":1780318060000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/anie.202518996"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2025,10,30]]},"references-count":58,"journal-issue":{"issue":"52","published-print":{"date-parts":[[2025,12,22]]}},"alternative-id":["10.1002\/anie.202518996"],"URL":"https:\/\/doi.org\/10.1002\/anie.202518996","archive":["Portico"],"relation":{},"ISSN":["1433-7851","1521-3773"],"issn-type":[{"value":"1433-7851","type":"print"},{"value":"1521-3773","type":"electronic"}],"subject":[],"published":{"date-parts":[[2025,10,30]]},"assertion":[{"value":"2025-08-29","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-10-20","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-10-30","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e18996"}}