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Apport de la technologie plasma pour le développement de procédés de carbonylation en microréacteur gaz/liquide

Abstract : The carbonylation reaction provides access to many organic molecules with high added value, but involves the use of carbon monoxide, a flammable and highly toxic gas. On the contrary, carbon dioxide is a non-toxic, inexpensive, non-flammable gas, and its use as a raw material to produce CO in situ is therefore an interesting path, both from a safety and environmental point of view. The objective of this thesis was therefore to convert CO2 into CO by plasma, then to use the CO formed to carry out a carbonylation reaction, both steps in microfluidic systems. First, the palladium-catalysed aminocarbonylation reaction was studied in a gas/liquid microreactor, and the operating parameters were optimized to obtain a total conversion of the substrate to amide. Secondly, the decomposition of CO2 into CO in a plasma microreactor was optimized to maximize the volume concentration of CO formed. Finally, the serial combination of the two microreactors allowed the synthesis of the amide starting from CO2 with a conversion of 70%, in a total residence time of less than 2 min, at a temperature of 50 °C and atmospheric pressure. Thus, the association of microfluidics and plasma is proving to be a very promising route for the rapid and clean organic synthesis of carbonyl molecules. Direct aminocarbonylation, without catalyst and by plasma activation, has also been explored, and the first results open up encouraging prospects.
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Marion Gaudeau. Apport de la technologie plasma pour le développement de procédés de carbonylation en microréacteur gaz/liquide. Génie mécanique [physics.class-ph]. Université Paris sciences et lettres, 2020. Français. ⟨NNT : 2020UPSLC015⟩. ⟨tel-03549766⟩

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