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作 者:Lijuan Feng Yan-Xi Tan El-Sayed MEl-Sayed Fenglei Qiu Wenjing Wang Kongzhao Su Daqiang Yuan
机构地区:[1]State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002 [2]College of Chemistry,Fuzhou University,Fuzhou 350116 [3]Chemical Refining Laboratory,Refining Department Egyptian Petroleum Research Institute,Nasr City,Cairo 11727 [4]University of the Chinese Academy of Sciences,Beijing 100049 [5]Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou 350108
出 处:《CCS Chemistry》2024年第9期2264-2274,共11页中国化学会会刊(英文)
基 金:financially supported by the National Nature Science Foundation of China(grant nos.22071244 and 22275191);the Youth Innovation Promotion Association CAS(grant no.2022305);the Natural Science Foundation of Fujian Province of China(grant nos.2022J01503,2020J05087,and 2022I0037).
摘 要:The exploration of ethane(C_(2)H_(6))-selective porous materials for the direct production of polymer-grade ethylene(C_(2)H_(4))from a C_(2)H_(6)/C_(2)H_(4) mixture in a single energy-saving adsorption step is of utmost importance but remains a significant challenge.Thus,developing robust C_(2)H_(6)-selective adsorbents with high C_(2)H_(6) capacity and C_(2)H_(6)/C_(2)H_(4) selectivity is urgently needed for industrial applications.In this study,we have successfully designed and synthesized two novel calix[4]resorcinarene-based porous organic cages(POCs)named CPOC-501 and CPOC-502.The POCs were formed via a Schiff-base reaction involving face-directed[6+8]condensation between a bowlshaped tetratopic tetraformylcalix[4]resorcinarene and triangular tritopic amine synthons.Analysis using single crystal X-ray crystallography revealed that both cages possess large truncated octahedral cavities with a volume of approximately 6500Å3 and 12 accessible rhombic windows with a side length of approximately 10.5Å.Furthermore,the cages exhibited excellent chemical stability under neutral,acidic,and basic conditions and high Brunauer–Emmett–Teller specific surface areas of up to 2175 m^(2) g^(−1) after desolvation.Both POCs demonstrated superior adsorption capabilities for C_(2)H_(6) over C_(2)H_(4).Notably,CPOC-502 exhibited a C_(2)H_(6) capacity and C_(2)H_(6)/C_(2)H_(4) selectivity of 83 cm^(3) g^(−1) and 2.83,respectively,surpassing most of the best-performing C_(2)H_(6)-selective porous organic materials reported to date.Moreover,breakthrough experiments confirmed that both cages efficiently produced polymer-grade C_(2)H_(4)(>99.9%)directly from the C_(2)H_(6)/C_(2)H_(4) mixture,highlighting their outstanding recyclability.
关 键 词:C_(2)H_(6)/C_(2)H_(4)separation porous organic cages resorcinarene gas adsorption and separation host-guest interactions
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