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Here, the correlation dynamics intrinsic to layered M(pbe)\u2010\u03b1 (M = Co\n                    <jats:sup>2+<\/jats:sup>\n                    , Zn\n                    <jats:sup>2+<\/jats:sup>\n                    , Cu\n                    <jats:sup>2+<\/jats:sup>\n                    ), transmitting from mono\u2010vertex to strained\u2010linker and to self\u2010adaptive grid\/stack, are orchestrated into node\u2010encoded flexibility. In\u2010situ tracking of dynamic structural evolution (including vertex distortion, linker rotation, layer motion, and pore resculpting) reveals the cation\u2010induced flexibility gradient Co &gt; Zn &gt; Cu, evidenced by changes in coordination bond lengths, unit cell volumes, and inter\/intra\u2010layer interactions. The activated phase Co(pbe)\u2010\u03b2 exhibits strong flexibility, undergoing a polarizability\u2010driven response for acetylene, achieving a record acetylene\/carbon dioxide uptake ratio of 75. Zn(pbe)\u2010\u03b2 with moderate flexibility displays a marked difference in response to propylene versus propane. Cu(pbe)\u2010\u03b2 with the weakest flexibility shows high selectivity for dispersion\u2010driven adsorption of butadiene over n\u2010butene. Breakthrough experiments confirm exceptional separation and cyclic performance, where efficient desorption yields high\u2010purity (\u2265 99.5%) acetylene, propylene, and butadiene. Thus, correlating the local dynamic extent of coordination bonds with weak interaction constraints, as well as global cell volume expansion extent in these finely fabricated layered soft crystals, enables customized flexibility for the matched separation of challenging C2\u2010C4 mixtures.\n                  <\/jats:p>","DOI":"10.1002\/anie.3591838","type":"journal-article","created":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T05:07:01Z","timestamp":1790658421000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Customized Flexibility in Soft Porous Crystals with Coupled Dynamics for Matching Separation of Light Hydrocarbons"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-9377-2578","authenticated-orcid":false,"given":"Qiubing","family":"Dong","sequence":"first","affiliation":[{"name":"Department of Chemistry and Chemical Engineering Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Shantou University  Shantou China"},{"name":"Key Laboratory of Functional Molecular Solids (Ministry of Education of China), Anhui Key Laboratory of Molecule\u2010Based Materials, College of Chemistry and Molecular Sciences College of Chemistry and Molecular Sciences Anhui Normal University  Wuhu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lei","family":"Shi","sequence":"additional","affiliation":[{"name":"Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources (Ministry of Education of China) Guangxi Key Laboratory of Chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical Sciences Guangxi Normal University  Guilin China"},{"name":"Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Key Laboratory for the Synthesis and Application of Organic Functional Molecules (Ministry of Education of China) College of Chemistry and Chemical Engineering Hubei University  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jingdi","family":"Li","sequence":"additional","affiliation":[{"name":"Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources (Ministry of Education of China) Guangxi Key Laboratory of Chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical Sciences Guangxi Normal University  Guilin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9985-8511","authenticated-orcid":false,"given":"Zheng","family":"Yin","sequence":"additional","affiliation":[{"name":"Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources (Ministry of Education of China) Guangxi Key Laboratory of Chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical Sciences Guangxi Normal University  Guilin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8218-1487","authenticated-orcid":false,"given":"Jingui","family":"Duan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemistry and Utilization of Carbon\u2010Based Energy Resources, College of Chemistry Xinjiang University  Urumqi China"},{"name":"Nanjing Tech University Suzhou Future Membrane Technology Innovation Center  Suzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7227-7688","authenticated-orcid":false,"given":"Ming\u2010Hua","family":"Zeng","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Engineering Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Shantou University  Shantou China"},{"name":"Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources (Ministry of Education of China) Guangxi Key Laboratory of Chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical Sciences Guangxi Normal University  Guilin 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These data are provided free of charge by the joint Cambridge Crystallographic Data Centre and Fachinformationszentrum Karlsruhe Access Structures service."},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202504895"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1002\/jcc.26812"},{"key":"e_1_2_8_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/jcc.22885"},{"key":"e_1_2_8_45_1","volume-title":"Supramolecular Chemistry","author":"Atwood J. 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