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Compared to industry\u2010used cryogenic distillation, adsorption separation would offer a more energy\u2010efficient solution when an efficient adsorbent is available. Herein, a class of C<jats:sub>2<\/jats:sub>H<jats:sub>4<\/jats:sub>\/C<jats:sub>2<\/jats:sub>H<jats:sub>6<\/jats:sub> separation adsorbents, doped carbon molecular sieves (d\u2010CMSs) is reported which are prepared from the polymerization and subsequent carbonization of resorcinol, <jats:italic>m<\/jats:italic>\u2010phenylenediamine, and formaldehyde in ethanol solution. The study demonstrated that the polymer precursor themselves can be a versatile platform for modifying the pore structure and surface functional groups of their derived d\u2010CMSs. The high proportion of pores centered at 3.5\u00a0\u00c5 in d\u2010CMSs contributes significantly to achieving a superior kinetic selectivity of 205 for C<jats:sub>2<\/jats:sub>H<jats:sub>4<\/jats:sub>\/C<jats:sub>2<\/jats:sub>H<jats:sub>6<\/jats:sub> separation. The generated pyrrolic\u2010N and pyridinic\u2010N functional sites in d\u2010CMSs contribute to a remarkable elevation of Henry selectivity to 135 due to the enhancement of the surface polarity in d\u2010CMSs. By balancing the synergistic effects of kinetics and thermodynamics, d\u2010CMSs achieve efficient separation of C<jats:sub>2<\/jats:sub>H<jats:sub>4<\/jats:sub>\/C<jats:sub>2<\/jats:sub>H<jats:sub>6<\/jats:sub>. Polymer\u2010grade C<jats:sub>2<\/jats:sub>H<jats:sub>4<\/jats:sub> of 99.71% purity can be achieved with 75% recovery using the devised d\u2010CMSs as reflected in a two\u2010bed vacuum swing adsorption simulation.<\/jats:p>","DOI":"10.1002\/smll.202401965","type":"journal-article","created":{"date-parts":[[2024,5,13]],"date-time":"2024-05-13T14:36:23Z","timestamp":1715610983000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Balancing the Kinetic and Thermodynamic Synergetic Effect of Doped Carbon Molecular Sieves for Selective Separation of C<sub>2<\/sub>H<sub>4<\/sub>\/C<sub>2<\/sub>H<sub>6<\/sub>"],"prefix":"10.1002","author":[{"given":"Ru\u2010Shuai","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Fine Chemicals Frontier Science Center for Smart Materials Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, and School of Chemical Engineering Dalian University of Technology  Dalian Liaoning 116024 P. 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China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Xue\u2010Jie","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals Frontier Science Center for Smart Materials Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, and School of Chemical Engineering Dalian University of Technology  Dalian Liaoning 116024 P. R. China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Cheng\u2010Tong","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals Frontier Science Center for Smart Materials Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, and School of Chemical Engineering Dalian University of Technology  Dalian Liaoning 116024 P. R. 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