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Fonctionnalisation de molécules organiques modèles en micro-réacteur plasma

Abstract : The use of microfluidics in chemistry is drawing more and more attention to chemists. Its fields of application are expanding, and one sees it as the future of fine organic chemistry, because it allows a very precise control of the reaction and its parameters. On the other hand, plasmas, with its energy and reactivity, becomes an ideal tool for "clean" chemistry synthesis. Indeed, plasma processes exhibits benefits such as being atmospheric, solvent-free, catalysts-free processes. This thesis is located at the intersection of microfluidics technologies and plasma processes. A novel diphasic, microfluidics device integrating generation of a confined, atmospheric plasma, has been developed, designed and manufactured. In these reactors of a new kind, optical and electrical measurements have been able to demonstrate the formation of a plasma in the microstructures. In this plasma are generated many reactive species, including several important radicals, that the use of the COMSOL Multiphysics simulation tool described as reaction intermediates for functionalization of organic molecules. Guided by this numerical simulation, we treated two model liquid, organic molecules, cyclohexane and benzene, with plasmas of argon, oxygen, carbon dioxide and ammonia. GC analysis of the liquid coming out of the reactor attested the effective hydroxylation, carbonylation and amination of these molecules, for conversions and selectivities depending on the nature of the gas and the liquid, as well as many operating conditions such as the voltage and frequency of the electrical signal applied to the reactor, or the temperature of the whole system. The success of these different controlled functionalizations, at atmospheric pressure, without solvent nor catalyst, of a cyclic hydrocarbon opens major stakes on the use of this type of process for industrial synthesis chemistry.
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Aurelien Lepoetre. Fonctionnalisation de molécules organiques modèles en micro-réacteur plasma. Autre. Université Paris sciences et lettres, 2019. Français. ⟨NNT : 2019PSLEC003⟩. ⟨tel-02879723⟩

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