Supramolecular binding and separation of hydrocarbons within a functionalized porous metal-organic framework
Supramolecular binding and separation of hydrocarbons within a functionalized porous metal-organic framework
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DOI：
10.1038/nchem.2114
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发表时间：
2015-02-01
期刊：
影响因子：
21.8
通讯作者：
Schroeder, Martin
中科院分区：
文献类型：
--
作者：
Yang, Sihai;Ramirez-Cuesta, Anibal J.;Schroeder, Martin
在许多化学和生物过程中，超分子相互作用是主客体结合的基础。在主客体系统中直接可视化这种超分子相互作用是非常具有挑战性的，但对于理解它们的功能至关重要。我们报道了一项结合了中子散射、同步加速器X射线和中子衍射以及计算模型的综合研究，以定义多孔主体Nott-300中乙炔、乙烯和乙烷在分子水平上的详细结合。这项研究揭示了乙炔和乙烯结合中的同时和协同氢键、pi中心点pi堆积作用和分子间偶极相互作用，从而放弃了在主体内排列的多达12个单独的弱超分子相互作用，形成了烃类选择性结合的最佳几何构型。我们还报道了乙炔和乙烯混合物在多孔主体中的协同结合，以及相应的突破实验和对混合气体的吸附等温线的分析。
Supramolecular interactions are fundamental to host-guest binding in many chemical and biological processes. Direct visualization of such supramolecular interactions within host-guest systems is extremely challenging, but crucial to understanding their function. We report a comprehensive study that combines neutron scattering, synchrotron X-ray and neutron diffraction, and computational modelling to define the detailed binding at a molecular level of acetylene, ethylene and ethane within the porous host NOTT-300. This study reveals simultaneous and cooperative hydrogen-bonding, pi center dot center dot center dot pi stacking interactions and intermolecular dipole interactions in the binding of acetylene and ethylene to give up to 12 individual weak supramolecular interactions aligned within the host to form an optimal geometry for the selective binding of hydrocarbons. We also report the cooperative binding of a mixture of acetylene and ethylene within the porous host, together with the corresponding breakthrough experiments and analysis of adsorption isotherms of gas mixtures.