A MOF built on 8-connected Y3 nodes demonstrates simultaneous reverse adsorptive separation: ethane over ethylene and propane over propylene

IF 10.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Science China Chemistry Pub Date : 2024-09-27 DOI:10.1007/s11426-024-2185-8

Lu-Lu Ma, Jiaqi Liu, Kang Zhou, Zixuan Cao, Jiafeng Miao, Guo-Ping Yang, Yao-Yu Wang, Jing Li, Hao Wang

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Abstract

Selective adsorption of paraffins over olefins (mostly C2 and C3) by porous solids could offer tremendous advantages for the purification of olefins, which is, however, challenging as it has stringent requirements on the pore dimensions and pore surface chemistry of the adsorbent. We report here a metal-organic framework (MOF) with novel topology, Y₃(μ₃-OH)(TCMPB)₂ (denoted as HIAM-316, TCMPB⁴⁻ = 1,2,4,5-tetra(4-carboxy-3-methylphenyl)benzene), which shows reversed separation of C₂H₆/C₂H₄ and C₃H₈/C₃H₆ simultaneously. The ideal adsorbed solution theory (IAST) selectivities for equimolar binary mixtures of C₂H₆/C₂H₄ and C₃H₈/C₃H₆ were calculated to be 1.67 and 1.23 at 1 bar and 298 K for HIAM-316. Its capability of removing paraffines from paraffin/olefin mixtures is validated by breakthrough measurements. Molecular simulations reveal that the preferential adsorption of paraffins over olefins by HIAM-316 may be attributed to the abundant carboxylate oxygen atoms along its channel.

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以 8 个连接的 Y3 节点为基础构建的 MOF 可同时实现反向吸附分离：乙烷吸附乙烯，丙烷吸附丙烯

多孔固体对烯烃（主要是 C2 和 C3）和石蜡的选择性吸附可为烯烃的提纯提供巨大优势，但这对吸附剂的孔隙尺寸和孔表面化学性质有严格要求，因此具有挑战性。我们在此报告了一种具有新拓扑结构的金属有机框架（MOF）--Y3(μ3-OH)(TCMPB)2（标记为 HIAM-316，TCMPB4- = 1,2,4,5-四（4-羧基-3-甲基苯基）苯），它能同时反向分离 C2H6/C2H4 和 C3H8/C3H6。根据计算，在 1 巴和 298 K 条件下，HIAM-316 对 C2H6/C2H4 和 C3H8/C3H6 等摩尔二元混合物的理想吸附溶液理论（IAST）选择性分别为 1.67 和 1.23。其从石蜡/烯烃混合物中去除石蜡的能力通过突破测量得到了验证。分子模拟显示，HIAM-316 优先吸附石蜡而不是烯烃的原因可能是其通道上有大量的羧酸氧原子。

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来源期刊

Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

14.40

自引率

7.30%

发文量

3787

审稿时长

2.2 months

期刊介绍： Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.