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作 者:Zi-Ming Ye Xue-Feng Zhang De-Xuan Liu Yan-Tong Xu Chao Wang Kai Zheng Dong-Dong Zhou Chun-Ting He Jie-Peng Zhang
机构地区:[1]Key Laboratory of Bioinorganic and Synthetic Chemistry(Ministry of Education),School of Chemistry,Sun Yat-Sen University,Guangzhou 510275,China [2]Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis,Jiangxi Normal University,Nanchang 330022,China 3.Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development,Guangzhou Institute of Energy Conversion,Chinese Academy of Sciences,Guangzhou 510640,China
出 处:《Science China Chemistry》2022年第8期1552-1558,共7页中国科学(化学英文版)
基 金:supported by the National Natural Science Foundation of China(21731007,22090061,21821003,22161021);the support of Jiangxi Province(jxsq2018106041);the“Young Elite Scientists Sponsorship Program”by CAST。
摘 要:Adsorptive separation of p-xylene(pX)from xylene isomers is a key process in chemical industry,but known adsorbents cannot simultaneously achieve high adsorption selectivity,capacity,and rate.Here,we demonstrate gating ultramicropore as a solution for this challenge.Slight modification of the synthetic condition gives rise to isomeric metal-organic frameworksα-[Zn(pba)](MAF-88,H2pba=4-(1H-pyrazol-4-yl)benzoic acid)andβ-[Zn(pba)](MAF-89)possessing similar pillared-column structures,porosities,and high pX capacities of 2.0 mmol g^(−1),but very different framework/pore topologies,pore sizes,and pX selectivities.For binary and ternary mixtures of liquid xylene isomers,MAF-88 with narrow one-dimensional(1D)channels shows pX selectivity of 11 and 1.6,while MAF-89 with 3D-connected quasi-discrete pores shows pX selectivity up to 221 and 46,respectively.Thermogravimetry,differential scanning calorimetry,and time-dependent separation experiments reveal that the kinetic effects of the gating pores play more important roles than the thermodynamic effects,which is further confirmed by single-crystal X-ray diffraction and computational simulations.
关 键 词:metal-organic frameworks GATING XYLENE ADSORPTION SEPARATION
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