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Host-Guest Binding Hierarchy within Redox- and Luminescence Responsive Supramolecular Self-Assembly Based on Chalcogenide Clusters and γ-Cyclodextrin.

著者 Ivanov AA , Falaise C , Abramov PA , Shestopalov MA , Kirakci K , Lang K , Moussawi MA , Sokolov MN , Naumov NG , Floquet S , Landy D , Haouas M , Brylev KA , Mironov YV , Molard Y , Cordier S , Cadot E
Chemistry.2018 Jun 12 ; ():.
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Water-soluble salts of anionic [Re6Q8(CN)6]4- (Q = S, Se, Te) chalcogenide octahedral rhenium clusters react with γ-cyclodextrin (γ-CD) producing a new type of inclusion compounds. Crystal structures determined through single-crystal X-ray diffraction analysis revealed supramolecular host-guest assemblies resulting from close encapsulations of the octahedral cluster within two γ-CDs. Interestingly, nature of the inner Q ligands influences strongly the host-guest conformation. The cluster [Re₆S₈(CN)6]4- interacts preferentially with the primary faces of the γ-CD while the bulkier clusters [Re6Se8(CN)6]4- and [Re6Te8(CN)6]4- exhibit specific interactions with the secondary faces of the cyclic host. Furthermore, analysis of the crystal packing reveals additional supramolecular interactions that lead to 2D infinite arrangements with [Re6S8(CN)6]4- or to 1D "bamboo-like" columns with [Re6Se8(CN)₆]4- and [Re6Te8(CN)6]4- species. Solution studies, using multinuclear NMR methods, ESI-MS and Isothermal titration calorimetry (ITC) corroborates nicely the solid state investigations showing that supramolecular pre-organization is retained in aqueous solution even in diluted conditions. Furthermore, ITC analysis showed that host-guest stability increases significantly ongoing from S to Te. At last, we report herein that deep inclusion alters significantly the intrinsic physical-chemical properties of the octahedral clusters, allowing redox tuning and near IR luminescence enhancement.
PMID: 29894019 [PubMed - as supplied by publisher]
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