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Currently, the prevailing adsorbents are ultramicroporous metal\u2013organic frameworks (MOFs) that feature narrow channels and\/or consist of inorganic anion pillars, which often lead to limited C3H4 uptake capacity and high isosteric enthalpy of adsorption. We report herein a highly porous and robust zirconium metal\u2013organic framework, termed SJTU-520. This MOF incorporates shape-persistent molecular arrays in three-dimensional space derived from cyclotetrabenzoin, which function as selective sites for the preferential entrapment of C3H4 over C3H6, thus enabling high C3H4 capture capacity, record high C3H4\/C3H6 uptake ratio at 1 bar and 298 K, and efficient C3H4\/C3H6 separation at ambient conditions. Compared with the cyclotetrabenzoin and tetraacetate cyclotetrabenzoin-based supramolecular organic crystals, SJTU-520 exhibits significantly higher surface area (3650 m2\/g versus 42 and 570 m2\/g), leading to a C3H4 uptake boost by 6.1-fold and 3.7-fold at 298 K and 1 bar, without any compromise of the C3H4\/C3H6 selectivity. The efficient C3H4\/C3H6 separation was validated by extensive breakthrough experiments under various conditions with great recyclability and high productivity of polymer-grade C3H6 from a 10\/90 C3H4\/C3H6 mixture. Computational simulations revealed that the four benzene walls of the cyclotetrabenzoin macrocycle in SJTU-520 formed equidistant \u03c0\u2013\u03c0 interactions with the C\u2261C triple bond of encapsulated C3H4 molecule. This work illustrates a general and powerful strategy\u2500the reticulation of intrinsically functional organic scaffolds into highly porous frameworks\u2500toward creating bespoke materials with precisely tailored functionalities and enhanced properties.<\/jats:p>","DOI":"10.1021\/jacs.6c05337","type":"journal-article","created":{"date-parts":[[2026,7,16]],"date-time":"2026-07-16T15:26:56Z","timestamp":1784215616000},"page":"30951-30960","source":"Crossref","is-referenced-by-count":0,"title":["Arraying Shape-Persistent\nMolecular Alkynyl Trap into\nHighly Porous and Robust Zirconium Metal\u2013Organic Framework\nfor Propyne Capture and Propyne\/Propylene Separation"],"prefix":"10.1021","volume":"148","author":[{"given":"Yuan","family":"Geng","sequence":"first","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chengye","family":"Lou","sequence":"additional","affiliation":[{"name":"Zhejiang Normal University , , ,","place":["Jinhua, China, 321004"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Min","family":"Mao","sequence":"additional","affiliation":[{"name":"Chongqing University , , ,","place":["Chongqing, China, 400044"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guangzu","family":"Xiong","sequence":"additional","affiliation":[{"name":"Zhejiang Normal University , , ,","place":["Jinhua, China, 321004"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pengfu","family":"Gao","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jingjing","family":"Zhang","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3273-9884","authenticated-orcid":true,"given":"Lingmei","family":"Liu","sequence":"additional","affiliation":[{"name":"Chongqing University , , ,","place":["Chongqing, China, 400044"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8268-384X","authenticated-orcid":true,"given":"Yuanbin","family":"Zhang","sequence":"additional","affiliation":[{"name":"Zhejiang Normal University , , ,","place":["Jinhua, China, 321004"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8707-8115","authenticated-orcid":true,"given":"Banglin","family":"Chen","sequence":"additional","affiliation":[{"name":"Zhejiang Normal University , , ,","place":["Jinhua, China, 321004"]},{"name":"Fujian Normal University , , ,","place":["Fuzhou, China, 350007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1977-0470","authenticated-orcid":true,"given":"Yong","family":"Cui","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1458-054X","authenticated-orcid":true,"given":"Wei","family":"Gong","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,16]]},"reference":[{"key":"2026073021330910600_cit1","doi-asserted-by":"publisher","first-page":"175","DOI":"10.1134\/S2070050415030083","article-title":"Propylene\nProduction Technology: Today and Tomorrow","volume":"7","author":"Lavrenov","year":"2015","journal-title":"Catal.\nInd."},{"key":"2026073021330910600_cit2","doi-asserted-by":"publisher","first-page":"344","DOI":"10.1021\/acs.accounts.0c00628","article-title":"Toward the Copolymerization\nof Propylene with Polar\nComonomers","volume":"54","author":"Luckham","year":"2021","journal-title":"Acc. 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Polym.\nRes."},{"key":"2026073021330910600_cit6","first-page":"613","article-title":"Selective Hydrogenation\nApplied to the Refining of Petrochemical Raw Materials Produced by\nSteam Cracking","volume-title":"Studies in surface science\nand catalysis","author":"Derrien","year":"1986"},{"key":"2026073021330910600_cit7","doi-asserted-by":"crossref","first-page":"149","DOI":"10.1007\/978-3-030-65021-6_5","article-title":"C3-Based Petrochemicals:\nRecent Advances in Processes and Catalysts","volume-title":"Catalysis for Clean Energy and Environmental Sustainability","author":"Samanta","year":"2021"},{"key":"2026073021330910600_cit8","doi-asserted-by":"publisher","first-page":"2390","DOI":"10.1021\/ie00022a024","article-title":"Hybrid Adsorption-Distillation Process\nfor Separating Propane and Propylene","volume":"32","author":"Ghosh","year":"1993","journal-title":"Ind. Eng.\nChem. 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Lett."},{"key":"2026073021330910600_cit15","doi-asserted-by":"publisher","first-page":"1477","DOI":"10.1039\/b802426j","article-title":"Selective\nGas Adsorption and Separation\nin Metal-Organic Frameworks","volume":"38","author":"Li","year":"2009","journal-title":"Chem. Soc. Rev."},{"key":"2026073021330910600_cit16","doi-asserted-by":"publisher","first-page":"869","DOI":"10.1021\/cr200190s","article-title":"Metal-Organic Frameworks for Separations","volume":"112","author":"Li","year":"2012","journal-title":"Chem. Rev."},{"key":"2026073021330910600_cit17","doi-asserted-by":"publisher","first-page":"7124","DOI":"10.1039\/C7CS00575J","article-title":"Metal-Organic Frameworks Based Membranes for Liquid\nSeparation","volume":"46","author":"Li","year":"2017","journal-title":"Chem. Soc. 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Mater."},{"key":"2026073021330910600_cit24","doi-asserted-by":"publisher","first-page":"213968","DOI":"10.1016\/j.ccr.2021.213968","article-title":"Isoreticular\nChemistry within Metal-Organic Frameworks for Gas Storage and Separation","volume":"443","author":"Fan","year":"2021","journal-title":"Coord. Chem. Rev."},{"key":"2026073021330910600_cit25","doi-asserted-by":"publisher","first-page":"42016","DOI":"10.1021\/jacs.5c15577","article-title":"Data-Driven Discovery of Metal-Organic\nFrameworks for Sieving Separation of Quinary C5 Olefin Mixtures","volume":"147","author":"Fang","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026073021330910600_cit26","doi-asserted-by":"publisher","first-page":"657","DOI":"10.1021\/jacs.0c11881","article-title":"Highly Specific Coordination-Driven\nSelf-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented\nJohnson-Type (J51) Nonanuclear Zr-Oxocarboxylate\nClusters","volume":"143","author":"Gong","year":"2021","journal-title":"J. Am. Chem. Soc."},{"key":"2026073021330910600_cit27","doi-asserted-by":"publisher","first-page":"14869","DOI":"10.1021\/jacs.1c07191","article-title":"Efficient C2H2\/CO2 Separation in Ultramicroporous Metal-Organic Frameworks with Record\nC2H2 Storage Density","volume":"143","author":"Gong","year":"2021","journal-title":"J. Am. Chem. 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Soc."},{"key":"2026073021330910600_cit30","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202318475","article-title":"Rational Design\nand Reticulation of Infinite qbe Rod\nSecondary Building Units into Metal-Organic Frameworks Through a Global\nDesymmetrization Approach for Inverse C3H8\/C3H6 Separation","volume":"63","author":"Gong","year":"2024","journal-title":"Angew. Chem.\nInt. Ed"},{"key":"2026073021330910600_cit31","doi-asserted-by":"publisher","first-page":"960","DOI":"10.1126\/science.1234071","article-title":"Separation of Hexane\nIsomers in a\nMetal-Organic Framework with Triangular Channels","volume":"340","author":"Herm","year":"2013","journal-title":"Science"},{"key":"2026073021330910600_cit32","doi-asserted-by":"publisher","first-page":"17795","DOI":"10.1021\/jacs.0c09466","article-title":"An Ultramicroporous\nMetal-Organic Framework for High Sieving Separation\nof Propylene from Propane","volume":"142","author":"Liang","year":"2020","journal-title":"J. Am. Chem. 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Ed."},{"key":"2026073021330910600_cit39","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202200947","article-title":"Comprehensive\nPore Tuning in an Ultrastable Fluorinated Anion Cross-Linked Cage-Like\nMOF for Simultaneous Benchmark Propyne Recovery and Propylene Purification","volume":"61","author":"Jiang","year":"2022","journal-title":"Angew. Chem., Int. Ed."},{"key":"2026073021330910600_cit40","doi-asserted-by":"publisher","first-page":"7733","DOI":"10.1021\/jacs.7b04268","article-title":"Flexible-Robust Metal-Organic\nFramework for Efficient Removal of Propyne from Propylene","volume":"139","author":"Li","year":"2017","journal-title":"J. Am. Chem. Soc."},{"key":"2026073021330910600_cit41","doi-asserted-by":"publisher","first-page":"15403","DOI":"10.1002\/ange.201809869","article-title":"A Metal-Organic\nFramework with Suitable Pore Size and Specific Functional Sites for\nthe Removal of Trace Propyne from Propylene","volume":"130","author":"Li","year":"2018","journal-title":"Angew. Chem."},{"key":"2026073021330910600_cit42","doi-asserted-by":"publisher","first-page":"13716","DOI":"10.1021\/acs.iecr.0c01726","article-title":"Gallate-Based Metal-Organic\nFrameworks for Highly Efficient Removal of Trace Propyne from Propylene","volume":"59","author":"Li","year":"2020","journal-title":"Ind. Eng. Chem. Res."},{"key":"2026073021330910600_cit43","doi-asserted-by":"publisher","first-page":"1705374","DOI":"10.1002\/adma.201705374","article-title":"A Single-Molecule Propyne Trap: Highly Efficient Removal of Propyne\nfrom Propylene with Anion-Pillared Ultramicroporous Materials","volume":"30","author":"Yang","year":"2018","journal-title":"Adv. Mater."},{"key":"2026073021330910600_cit44","doi-asserted-by":"publisher","first-page":"298","DOI":"10.1039\/d2sc05742e","article-title":"Insights into the Thermodynamic-Kinetic Synergistic\nSeparation of Propyne\/Propylene in Anion Pillared Cage MOFs with Entropy-Enthalpy\nBalanced Adsorption Sites","volume":"14","author":"Jiang","year":"2023","journal-title":"Chem. Sci."},{"key":"2026073021330910600_cit45","doi-asserted-by":"publisher","first-page":"43957","DOI":"10.1021\/jacs.5c16526","article-title":"Peristaltic Motion in Structurally Adaptive Molecular\nCrystals Enables Selective Propyne Capture","volume":"147","author":"Lin","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026073021330910600_cit46","doi-asserted-by":"publisher","first-page":"2253","DOI":"10.1021\/acs.orglett.1c00383","article-title":"Cyclobenzoin\nEsters as Hosts for Thin Guests","volume":"23","author":"McHale","year":"2021","journal-title":"Org. Lett."},{"key":"2026073021330910600_cit47","doi-asserted-by":"publisher","first-page":"781","DOI":"10.1021\/acs.orglett.0c04014","article-title":"Expanded Cyclotetrabenzoins","volume":"23","author":"Eisterhold","year":"2021","journal-title":"Org. 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