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Caractérisation de polymères supramoléculaires hiérarchiques à base de cyclodextrines fonctionnalisées

Abstract : Molecular systems with nanometer-sized dimensions are involved in a wide variety of processes and biological functions. Understanding the mechanisms controlling their multi-lengthscale structure presents a major interest. For instance, despite this challenge, there is so far no reliable synthetic system forming well-defined tunable fibrillar objects with a monodisperse diameter in aqueous solution. The aim of this work is to develop a tool box of di-functionalized cyclodextrins (CDs) specifically designed to self-assemble into supramolecular rods that could then reach higher levels of hierarchy via interactions mediated by the secondary functionalization. The study of the first level of association of these compounds by viscosimetry, ITC and SANS showed that the use of bridged CDs allows the polymerization by suppressing the self-inclusion phenomenon. As a result, we developed two tunable cationic supramolecular polymers (SMP) based on functionalized β-CD with relatively high polymerization degrees. Their ability to form hierarchical SMP with rigid polyanionic species was then assessed by DLS, spectroscopy and cryo-TEM. In optimized concentration and charge ratio conditions, three different water-soluble hierarchical assemblies were formed. We showed that the first level of association and the high directionality of the secondary interactions are key parameters to achieve these stable, well-defined, hierarchical assemblies. These tunable structures will be therefore used as a platform to get greater insight into hierarchical assembling processes.
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Submitted on : Monday, March 25, 2019 - 3:34:40 PM
Last modification on : Friday, October 23, 2020 - 4:37:25 PM
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  • HAL Id : tel-02078739, version 1


Gaëlle Pembouong. Caractérisation de polymères supramoléculaires hiérarchiques à base de cyclodextrines fonctionnalisées. Chimie-Physique [physics.chem-ph]. Sorbonne Université, 2018. Français. ⟨NNT : 2018SORUS005⟩. ⟨tel-02078739⟩



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