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An analogy to such a function can be drawn conceptually for crystalline porous solids; yet the manifested entities are rare in reticular chemistry. The bottleneck\u2010shaped pores carved out of a metal\u2010organic framework, Zn(MIBA)<jats:sub>2<\/jats:sub> (aka. MAF\u2010stu\u201013), can perfectly accommodate benzene molecules. Remarkably, its framework adapts to the optimal guest binding\u2010the enhanced host\u2013guest interactions in the neck in turn minimize the guest\u2010guest repulsion in the pore to the extent it turns into attraction\u2010as demonstrated by the combined X\u2010ray structural and DFT computational studies. This adaptive material can be used for liquid\u2010phase production of ultrahigh\u2010purity (\u226599\u2009%) cyclohexane, achieving a balance between uptake capacity and separation selectivity and surpassing the performances of other porous and nonporous crystals reported recently (e.g. product purity 99.4\u2009% vs. 97.5\u2009% to date).<\/jats:p>","DOI":"10.1002\/anie.202109964","type":"journal-article","created":{"date-parts":[[2021,8,31]],"date-time":"2021-08-31T11:04:52Z","timestamp":1630407892000},"page":"23590-23595","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":40,"title":["Harnessing Shape Complementarity for Upgraded Cyclohexane Purification through Adaptive Bottlenecked Pores in an Imidazole\u2010Containing MOF"],"prefix":"10.1002","volume":"60","author":[{"given":"Chun\u2010Rong","family":"Ye","sequence":"first","affiliation":[{"name":"Department of Chemistry and Key Laboratory for Preparation and Application 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