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Étude de la combustion de composés organiques grâce au couplage d'un réacteur parfaitement agité avec des méthodes analytiques spectroscopiques et spectrométriques : application à la détection des hydroperoxydes

Abstract : In recent years, the world is facing a major energetic issue due to the growing primary energy demand and not to mention the emissions of harmful pollutants for the environment. Researchers have been studying alternative pathways to the massive use of fossil fuels, such as the incorporation of biofuels into conventional gasoline or the development of modern technology. New types of engines using a low-temperature combustion are currently under study. They have the advantage of combining both a good performance and a reduction in pollutant emissions (like NOx and soot particles). Significant gaps of knowledge are still remaining, both on the characterization of the reactivity, the emissions and on the low-temperature gas phase oxidation chemistry of biofuels. Main objectives of this thesis are to: ?- Establish an experimental database by identifying reaction products and intermediates and more particularly during the low-temperature oxidation (from 500 to 1100K), ?- Develop and validate detailed kinetic models in order to reproduce the combustion of the fuel. Oxidation experiments were performed using a jet-stirred reactor. Thanks to its homogeneity in both temperature and concentration, it can be considered as an ideal reactor for kinetic studies. The products obtained at the outlet of the reactor have been analyzed using three complementary methods: gas chromatography (GC) and cavity ring-down spectroscopy (CRDS) and mass spectrometry (MS). The GC method is efficient in separating compounds (including isomers) and allows us to analyze a wide range of products. The CRDS method is an absorption spectroscopic technique which allows us to analyze specific species such as HCHO, H2O and H2O2. Finally MS coupled with a soft ionization technique allows us to analyze hydroperoxides products of formula R-OOH. Both H2O2 and hydroperoxides are important reaction intermediates in combustion, but there is very little experimental data available on those species. Due to their weak O-O bond, those compounds are thermolabile and difficult to analyze (undectable using GC). This thesis allowed the study of different fuels oxidation, from hydrocarbons (n-pentane, n-hexane, n-hexenes, n-heptane, iso-octane, n?decane) to oxygenated compounds (dimethyl-ether, 1-hexanol, hexanal, large methyl-esters)
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Anne Rodriguez. Étude de la combustion de composés organiques grâce au couplage d'un réacteur parfaitement agité avec des méthodes analytiques spectroscopiques et spectrométriques : application à la détection des hydroperoxydes. Génie des procédés. Université de Lorraine, 2016. Français. ⟨NNT : 2016LORR0246⟩. ⟨tel-01720491⟩

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