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Theses

Nouveaux catalyseurs confinés pour la valorisation du CO2

Abstract : Azaphosphatranes have rarely been applied as organocatalysts in organic transformations. Nevertheless, they have recently proved to be efficient single-component metal-free catalysts for the production of cyclic carbonates from epoxides and carbon dioxide. The goal of this work is to optimize the reactivity of azaphosphatrane based catalysts towards greater CO2 fixation into cyclic carbonates. First, they have been used in conjunction with mesoporous silica of the SBA family. A positive synergy, depending on the nature of the counter-anion, was demonstrated leading to better yields in cyclic carbonates. Adding a solvent or silica was shown to drive to a change in the reaction mechanism as evidenced by kinetic studies. Then, different activating functional groups were introduced at different position of the catalyst structure to further activate epoxide or carbon dioxide substrates. Finally, the kinetic resolution of racemic epoxides in the presence of CO2 was investigated. Different approaches to chiral induction have been explored including the introduction of asymmetric carbons on azaphosphatranes, the use of induced chirality with cyclotriveratrylene unit in hemicryptophane moiety. Chiral imprinted with amino acids and chiral grafted mesoporous silicas have also been studied.
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https://tel.archives-ouvertes.fr/tel-02103764
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Submitted on : Thursday, April 18, 2019 - 4:47:05 PM
Last modification on : Thursday, January 23, 2020 - 6:22:05 PM

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  • HAL Id : tel-02103764, version 1

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Florian Lagarde. Nouveaux catalyseurs confinés pour la valorisation du CO2. Catalyse. Ecole Centrale Marseille, 2018. Français. ⟨NNT : 2018ECDM0011⟩. ⟨tel-02103764⟩

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