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作 者:Lin Zhang Jia-Qi Ma Yi-Zhao Guo Xiu-Yuan Li Lei Hou Yao-Yu Wang Zhonghua Zhu
机构地区:[1]Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education,College of Chemistry&Materials Science,Northwest University,Xi’an 710069,China [2]School of Chemical Engineering,The University of Queensland,Brisbane 4072,Australia
出 处:《Science China Chemistry》2025年第3期967-973,共7页中国科学(化学英文版)
基 金:supported by the National Natural Science Foundation of China (22371226);the Natural Science Basic Research Program of Shaanxi (2024JC-JCQN-18);the Shaanxi Fundamental Science Research Project for Chemistry&Biology (23JHZ004)。
摘 要:Ethylene(C_(2)H_(4)) and propylene(C_(3)H_(6)) produced by methanol to olefin(MTO) technology are important chemical raw materials.However,the purification and separation between C_(2)H_(4) and C_(3)H_(6) mixtures is very challenging.Herein,a novel microporous metal-organic framework(MOF) adsorbent Co_(2)(OATA)(DPA) was fabricated through mixed linkers of 5,5'-(oxalylbis(azanediyl))diisophthalic acid(H_(4)OATA) and V-shaped di(pyridin-4-yl)amine(DPA) with -NHCO- and -NH- functional groups,which was endowed with ideal small pore size,large cavity,and interesting C_(3)H_(6) trap constructed by four sets of -NH- groups.Under 298 K and a crucial low pressure(0.05 bar) for the separation in microporous materials,the MOF shows ultra-high C_(3)H_(6) preferential adsorption(97.8 cm^(3)g^(-1)) and considerable C_(3)H_(6)/C_(2)H_(4) selectivity(about 22),representing an advanced material for the reported porous materials with C_(3)H_(6)/C_(2)H_(4) separation function.The studies of single crystal X-ray diffraction and simulations showed that the customized pore limitation in the MOF provided stronger multiple attractive interactions with C_(3)H_(6),leading to significant adsorption selectivity in the process of competing adsorption for C_(3)H_(6) and C_(2)H_(4).In one separation step,the MOF generated highly pure C_(2)H_(4)(≥99.9%) and C_(3)H_(6)(≥99.6%) products respectively from C_(2)H_(4)/C_(3)H_(6) mixtures at different ratios,pressures,and temperatures.
关 键 词:metal-organic framework solvothermal synthesis crystal structure gas adsorption and separation olefins purification
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