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Here, we report a strategy of adaptive flexibility control. A family of isostructural metal azolate frameworks featuring bent linkers and size\u2010tunable substituents were designed and synthesized. Single\u2010crystal X\u2010ray diffraction and computational simulations unveiled a bending\u2010adsorption coupling mechanism: the stronger ethane binding drives more pronounced linker flattening to reinforce itself. Crucially, bulkier substituents reinforce this adaptive response, further elevating ethane selectivity. Notably, mixture breakthrough experiments demonstrated that navigating the selectivity\u2013capacity trade\u2010off via substituent\u2010tuned adaptive flexibility afforded superior ethylene purification productivity.<\/jats:p>","DOI":"10.1002\/anie.9034981","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T03:41:24Z","timestamp":1790739684000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Controlling Adaptive Flexibility for Efficient Purification of Ethylene From Ethane"],"prefix":"10.1002","author":[{"given":"Xiao\u2010Tong","family":"Lu","sequence":"first","affiliation":[{"name":"MOE Key Laboratory of Bioinorganic and Synthetic Chemistry GBRCE For Functional Molecular Engineering School of Chemistry IGCME Sun Yat\u2010Sen University  Guangzhou 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