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Direct synthesis of long-chain hydrocarbons by plasma-catalysis from syngas and CH4-CO2 mixtures

Abstract : This thesis deals with the study of Fischer-Tropsch synthesis (FTS) and the direct conversion of CO2 and CH4 into value-added liquid products by a process coupling non-thermal plasma and heterogeneous catalysis. A coaxial dielectric barrier discharge (DBD) plasma-catalytic reactor was designed and tested in this thesis with its analysis and diagnostic devices. The reactor operates under ambient conditions, the catalyst and its support are under the form of granules packaged in the reactor. The support is in silica aerogel and was synthesized by surface treatment and ambient drying. Chapter 3 is dedicated to the experimental study of plasma-catalytic Fischer-Tropsch synthesis. In this chapter, the experiments were first conducted in plasma alone without catalyst, paying particular attention to the influence of the gas flow rate, the H2/CO ratio and the electrical excitation frequency on the syngas conversion. Then, in a second step, the catalyst/support couple (Co/SiO2) was introduced into the reactor in order to study the results of the conversion under plasma-catalytic combination. Chapters 4 and 5 deal with the direct plasma-catalytic conversion of CO2 and CH4 into liquid products and syngas. In Chapter 4, the same approach as in Chapter 3 was used, a comparative study of experiments with and without catalyst was done. The two catalyst/support couples used successively in this chapter are Co/SiO2 and Fe/SiO2. Chapter 5 extends the study by proposing a plasma-catalytic combination with two catalysts at the same time. The effects of packing composite catalysts (Co/SiO2 or Fe/SiO2 with HZSM-5, Co/HZMS-5 and Fe/HZSM-5) were studied. The combination of catalysts has made it possible to increase the liquid products selectivity and to produce new liquid products compared to Chapter 4. Thus alcohols, carboxylic acids and C5+ hydrocarbons were synthesized. The thesis ends with a comparison of the results with those of the literature from close processes; energy efficiency and gross productivity were compared. Some possible ways of reaction have also been proposed to initiate a more theoretical reflection. Finally, recommendations for optimization/improvement of FTS and direct conversion of CO2/CH by plasma-catalytic route are provided and discussed.
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Submitted on : Wednesday, July 15, 2020 - 12:49:10 PM
Last modification on : Wednesday, October 14, 2020 - 4:11:15 AM


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Di Li. Direct synthesis of long-chain hydrocarbons by plasma-catalysis from syngas and CH4-CO2 mixtures. Chemical and Process Engineering. Université Paris sciences et lettres, 2019. English. ⟨NNT : 2019PSLEM059⟩. ⟨tel-02899601⟩



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