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Thermoreversible associations between multiarm structures based on poly(trilmethylene carbonate) oligomers for materials with potential applications in the biomedical field : structure-properties relationships

Abstract : This ph-D describes the functionalization of poly(trimethylene carbonate) (PTMC) by hydrogen bonding motifs (HBMs) and Diels-Alder (DA) reactions to obtain thermoreversible networks and to reveal their structure-property relationships. Linear PTMC oligomers were first synthesized by ring-opening polymerization. PTMC-based multiarm supramolecular polymers bearing telechelic triuret and tetrauret HBMs were then synthesized using urea and a diisocyanate as a linker. Association constants (Ka) of triuret and tetrauret HBMs were determined by NMR in CDCl3. Increasing the HBM functionality or reducing PTMC chain length endowed networks with better creep resistance and higher Young’s modulus in tensile tests. The morphologies and dynamics of these supramolecular polymers were investigated in the melt state to reveal two relaxation modes corresponding to two microdomains, induced by hydrogen bonding between urethane groups and HBMs.. By the association dynamics study of bifunctional linear supramolecular PTMC in bulk, as a model, it was revealed, only dimers were formed between triuret HBMs at short times, leading to the linear chain extension equivalent to a polycondensation. Ka of triuret HBMs were then calculated from a simple and original model based on viscosity measurements in the molten state. Equivalent networks with different densities were also obtained by Diels-Alder reaction between furan-functionalized PTMC and a bismaleimide. Perfect network structures were obtained and the effects of furan functionality on network density and properties were evidenced. The thermoreversibility was found to occur from 130 °C to 160 °C based on their densities.
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Xiang Li. Thermoreversible associations between multiarm structures based on poly(trilmethylene carbonate) oligomers for materials with potential applications in the biomedical field : structure-properties relationships. Polymers. Université de Lyon, 2019. English. ⟨NNT : 2019LYSES008⟩. ⟨tel-02458166⟩

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