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This separation is exceptionally challenging due to their similar physicochemical properties. Herein, we report a novel carborane\u2010based metal\u2010organic framework, ZNU\u201023 (Ni\u2010CB\u2010HPBTA), engineered with a pearl\u2010chain\u2010like pore architecture to achieve unprecedented molecular sieving separation. The narrow pore channel and large cavity in ZNU\u201023 facilitate the high and fast uptake of C\n                    <jats:sub>2<\/jats:sub>\n                    F\n                    <jats:sub>5<\/jats:sub>\n                    H (65.2 cm\n                    <jats:sup>3<\/jats:sup>\n                    \u00b7g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 298 K and 1\u00a0bar) while nearly completely excluding C\n                    <jats:sub>2<\/jats:sub>\n                    F\n                    <jats:sub>6<\/jats:sub>\n                    , leading to a record\u2010high IAST selectivity exceeding 5000 for a C\n                    <jats:sub>2<\/jats:sub>\n                    F\n                    <jats:sub>5<\/jats:sub>\n                    H\/C\n                    <jats:sub>2<\/jats:sub>\n                    F\n                    <jats:sub>6<\/jats:sub>\n                    (1\/99) mixture. Dynamic breakthrough experiments confirm its excellent separation performance across various mixture ratios, remarkable stability under humid and elevated\u2010temperature conditions, and superb recyclability. Mechanistic studies via GCMC simulations and DFT calculations attribute this performance to the multi\u2010site confinement of C\n                    <jats:sub>2<\/jats:sub>\n                    F\n                    <jats:sub>5<\/jats:sub>\n                    H within the pearl\u2010chain pores and the complete steric exclusion of the larger C\n                    <jats:sub>2<\/jats:sub>\n                    F\n                    <jats:sub>6<\/jats:sub>\n                    molecule. The potential C\n                    <jats:sub>2<\/jats:sub>\n                    F\n                    <jats:sub>5<\/jats:sub>\n                    H binding sites within the framework were further revealed by C\n                    <jats:sub>2<\/jats:sub>\n                    F\n                    <jats:sub>5<\/jats:sub>\n                    H\u2010loaded single crystal structure of ZNU\u201023.\n                  <\/jats:p>","DOI":"10.1002\/anie.7710650","type":"journal-article","created":{"date-parts":[[2026,6,18]],"date-time":"2026-06-18T17:41:31Z","timestamp":1781804491000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Novel Carborane Based Metal Organic Framework for Record Electronic Specialty Gas C\n                    <sub>2<\/sub>\n                    F\n                    <sub>6<\/sub>\n                    Purification via Molecular Sieving"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-2497-6232","authenticated-orcid":false,"given":"Jianan","family":"He","sequence":"first","affiliation":[{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials Science Zhejiang Normal University  Jinhua P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lingyao","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials Science Zhejiang Normal University  Jinhua P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guangzu","family":"Xiong","sequence":"additional","affiliation":[{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials Science Zhejiang Normal University  Jinhua P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongxiang","family":"Zhou","sequence":"additional","affiliation":[{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials Science Zhejiang Normal University  Jinhua P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dong","family":"Luo","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8707-8115","authenticated-orcid":false,"given":"Banglin","family":"Chen","sequence":"additional","affiliation":[{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials Science Zhejiang Normal University  Jinhua P.R. China"},{"name":"Fujian Provincial Key Laboratory of Polymer Materials College of Chemistry &amp; Materials Science Fujian Normal University  Fuzhou P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8268-384X","authenticated-orcid":false,"given":"Yuanbin","family":"Zhang","sequence":"additional","affiliation":[{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials Science Zhejiang Normal University  Jinhua P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,6,18]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/app.1986.070320407"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1063\/1.556016"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202505355"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.tsf.2004.03.025"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202513398"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.snb.2024.136335"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.egypro.2017.12.256"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0950\u20104230(01)00067\u20105"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.seppur.2024.128373"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cclet.2025.111478"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202503505"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adj6473"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010024\u201053024\u20108"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2017.03.022"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2024.215697"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2023.09.005"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202522967"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.seppur.2021.119951"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201903600"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201908378"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202414151"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010025\u201057972\u20107"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c03442"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202102585"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2023.144852"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202000323"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202506055"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202417183"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202107963"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202007681"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2023.215093"},{"key":"e_1_2_8_33_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202411744"},{"key":"e_1_2_8_34_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adh0135"},{"key":"e_1_2_8_35_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202514808"},{"key":"e_1_2_8_36_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202309925"},{"key":"e_1_2_8_37_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202215253"},{"key":"e_1_2_8_38_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010023\u201035984\u20105"},{"key":"e_1_2_8_39_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.seppur.2023.124109"},{"key":"e_1_2_8_40_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c12032"},{"key":"e_1_2_8_41_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2025.170631"},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202402382"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202425638"},{"key":"e_1_2_8_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202205427"},{"key":"e_1_2_8_45_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.seppur.2025.134841"},{"key":"e_1_2_8_46_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202003421"},{"key":"e_1_2_8_47_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202403421"},{"key":"e_1_2_8_48_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202200947"},{"key":"e_1_2_8_49_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c03505"},{"key":"e_1_2_8_50_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c14861"},{"key":"e_1_2_8_51_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201902209"},{"key":"e_1_2_8_52_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202406664"},{"key":"e_1_2_8_53_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c08530"},{"key":"e_1_2_8_54_1","doi-asserted-by":"publisher","DOI":"10.1002\/jcc.22885"},{"key":"e_1_2_8_55_1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0216272"},{"key":"e_1_2_8_56_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jmgm.2012.07.004"},{"key":"e_1_2_8_57_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557\u2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