UMR 5182

logo-ensl
You are here: Home / News / Soutenances / Anais Mirabaud

Anais Mirabaud

PhD Defense
When

Dec 08, 2015 à 09:30 AM

Where

Amphithéâtre de Physique Nucléaire, Bâtiment Paul Dirac à la Doua, Villeurbanne.

Development of a host-guest chemistry for the valorization of CO2 through an eco-compatible catalysis

The defense will be followed by a celebration that will be held on the 3rd floor of the CPE building, at the "Mezzanine".

 

The utilization of carbon dioxide (CO2) as a key component in organic transformations has recently drawn much attention as a greener alternative to fossil fuel based resources. The objectives of this work aim at studying the synthesis of cyclic carbonates from the coupling of CO2 with epoxide. Numerous catalysts have been proposed for this reaction among which the ammonium halides providing the nucleophile to initiate the reaction by opening the epoxide. Herein, we propose a new approach based on host-guest chemistry, to improve catalytic reactivity by increasing the nucleophilicity of the halide anion. For this purpose, cavitand molecular receptors able to bind quaternary ammonium ions are used, releasing the anionic nucleophile for the initial epoxide ring-opening reaction. At CO2 atmospheric pressure, our catalytic systems demonstrated a great potential by the dramatic activation of tetramethylammonium halides, whereas when used alone, these catalysts had never shown any activity. The influence of the cavitand structure was investigated through experiments run under 10 bar of CO2 pressure, and revealed that a double activation was possible with cavitand bearing Brönsted acidic hydroxyl functions and optimal recognition properties. The heterogeneization of such catalytic systems was finally studied with the grafting of either ammoniums or cavitands on silica based materials.