School of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD, UK.
The Chemical and Engineering Materials Division (CEMD), Neutron Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
Nat Chem. 2014 Feb;7(2):121-9. doi: 10.1038/nchem.2114. Epub 2014 Dec 1.
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, π···π 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.
超分子相互作用是许多化学和生物过程中主体-客体结合的基础。在主体-客体体系中直接观察这种超分子相互作用极具挑战性，但对于理解其功能至关重要。我们报告了一项综合研究，该研究结合了中子散射、同步加速器 X 射线和中子衍射以及计算建模，以在分子水平上定义乙炔、乙烯和乙烷在多孔宿主 NOTT-300 中的详细结合情况。这项研究揭示了乙炔和乙烯与多孔宿主相互作用时同时发生的协同氢键、π···π 堆积相互作用和分子间偶极相互作用，形成多达 12 个单独的弱超分子相互作用，这些相互作用在宿主内排列成最佳几何形状，以实现对烃类的选择性结合。我们还报告了多孔宿主中乙炔和乙烯混合物的协同结合，以及相应的突破实验和混合气体吸附等温线分析。
