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基于尺寸排阻的碳氢化合物分离的孔径控制

Pore Aperture Control Toward Size-Exclusion-Based Hydrocarbon Separations.

作者信息

Lal Bhajan, Idrees Karam B, Xie Haomiao, Smoljan Courtney S, Shafaie Saman, Islamoglu Timur, Farha Omar K

机构信息

Department of Chemistry, Northwestern University, 60208, Evanston, IL, USA.

Institute of Chemistry, Shah Abdul Latif University, 66020, Khairpur, Sindh, Pakistan.

出版信息

Angew Chem Int Ed Engl. 2023 Apr 11;62(16):e202219053. doi: 10.1002/anie.202219053. Epub 2023 Mar 6.

DOI:10.1002/anie.202219053
PMID:36790793
Abstract

Metal-organic frameworks (MOFs) have been proposed as a promising material for non-thermal chemical separations owing to their high structural diversity and tunability. Here, we report the synthesis of a zinc-based MOF containing a three-dimensional (3D) linker, bicyclo[2.2.2]octane-1,4-dicarboxylic acid, with high thermal stability towards the separation of hexane isomers. The incorporation of the 3D linker enhances the structural stability and provides well-defined pore apertures/channels with sub-Ångstrom precision. This precision allowed for the separation of similarly sized hexane isomers based on subtle differences in their kinetic diameters. Multi-component liquid phase batch experiments confirmed the separation of hexanes mixture into linear, monobranched, and dibranched isomers. This work represents a significant milestone in the construction of stable Zn-based MOFs and the incorporation of 3D linkers as a potential solution to challenging separations.

摘要

金属有机框架材料(MOFs)因其高度的结构多样性和可调节性,已被视为一种用于非热化学分离的极具潜力的材料。在此,我们报告了一种含三维(3D)连接体双环[2.2.2]辛烷-1,4-二羧酸的锌基金属有机框架材料的合成,该材料对己烷异构体的分离具有高热稳定性。3D连接体的引入增强了结构稳定性,并提供了具有亚埃精度的明确孔口/通道。这种精度使得基于动力学直径的细微差异对尺寸相近的己烷异构体进行分离成为可能。多组分液相间歇实验证实了己烷混合物可分离为直链、单支链和双支链异构体。这项工作代表了稳定锌基金属有机框架材料构建以及引入3D连接体作为具有挑战性分离问题潜在解决方案方面的一个重要里程碑。

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Synergistic global and local flexibilities in Zr-based metal-organic frameworks enable sequential sieving of hexane isomers.基于锆的金属有机框架中协同的全局和局部灵活性实现了己烷异构体的顺序筛分。
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Selective sorting of hexane isomers by anion-functionalized metal-organic frameworks with optimal energy regulation.
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