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Rozprawy doktorskie na temat "Couplage photochimique du méthane":
Hu, Di. "Photocatalytic methane conversion into chemicals and fuels under mild conditions". Electronic Thesis or Diss., Université de Lille (2022-....), 2022. http://www.theses.fr/2022ULILR034.
A cascade one-pot photo-chemo-catalytic process for methane oxidation to formic acid has been proposed. A specifically designed photocatalyst and a commercial heterogeneous catalyst were used together in the cascade process. The methane selective conversion into formic acid proceeds first over caesium salt of phosphotungstic acid (CsPW) supported on titania, which photocatalytically oxidizes methane under irradiation into a mixture of C1 liquid oxygenates. The C1 liquid oxygenates produced by photocatalysis are then selectively converted into formic acid over the heterogeneous alumina supported ruthenium catalyst. All reactions of selective oxidation of methane to formic acid occur in the cascade process at room temperature in the same reactor. The cascade process produced formic acid with a productivity of 5000 μmolformic acid g-1photocatalyst and a selectivity of 85 %, as well as a concentration of up to 1.1 mmol L-1.Gold nanoparticles with a size from 6 to 29 nm supported on titania have been prepared for photocatalytic non-oxidative and oxidative methane coupling in both batch and continuous gas flow reactors. The photocatalytic performance is not affected by the nanoparticles size. The methane conversion requires band gap transition in TiO2 excited by UV irradiation. No methane conversion was observed after activation of plasmonic gold nanoparticles by visible light. The plasmonic effect of gold nanoparticles cannot alone drive the methane photocatalytic conversion. The methane activation and oxidation occur over titania oxygen vacancies, while oxygen is likely activated by gold nanoparticles. The methane conversion was facilitated by slower electron-hole recombination in the presence of gold nanoparticles. A hydrocarbon productivity of 1864 μmol g−1 h−1 with a coupling selectivity higher than 86% was achieved in the continuous oxidative methane coupling flow process.Silver salt of phosphotungstic aicd (AgPW) supported on titania has been prepared for photochemical methane coupling. The methane conversion requires band gap transition in both the AgPW and TiO2 by UV irradiation as well the charge transfer between them with intimate contact. Introducing even small amount of AgPW to TiO2 significantly enhanced the coupling rate. During photochemical methane coupling, cationic Ag+ species were reduced to metallic Ag and resulted in photoactivity decrease, while Ag+ species and photoactivity can be regenerated from the spent AgPW-TiO2 exposing to light in the presence of air. The chemical looping process achieved ethane production of 64 μmol/g with coupling selectivity above 95%
Gilbert, Charles-Olivier. "Développement de polymères bidimensionnels par couplage photochimique". Master's thesis, Université Laval, 2019. http://hdl.handle.net/20.500.11794/34998.
Lacombe, Sylvie. "Etude mécanistique du couplage oxydant du méthane sur oxyde de lanthane". Lyon 1, 1993. http://www.theses.fr/1993LYO10276.
Bouqueniaux, David. "Étude mécanistique du couplage oxydant du méthane sur zircones pures et dopées". Lille 1, 1995. http://www.theses.fr/1995LIL10035.
Serres, Thomas. "Oxidative Coupling of Methane followed by Oligomerization to Liquids". Thesis, Lyon 1, 2013. http://www.theses.fr/2013LYO10229.
Rochoux, Marie. "Matériaux conducteurs mixtes ioniques et électroniques pour le couplage oxydant du méthane". Thesis, Lyon 1, 2014. http://www.theses.fr/2014LYO10234/document.
The oxidative coupling of methane (OCM) allowed the direct transformation of methane into ethylene (C2). Until now, the catalytic process does not reach the required criteria of selectivity and yield. The presence of gaseous oxygen at high temperature (T>700°C) favors the total oxidation. The use of a dense membrane reaction (MR), made of mixed ionic and electronic materials, limits the gaseous oxygen in the reaction compartment and thus improve the C2 selectivity. The goal of this PhD is to develop catalytic membranes exhibiting a flux high enough to reach a conversion higher than 25% and of which the catalytic coating leads to a C2 selectivity of 80%. An innovative method, based on a microkinetic approach, has been developed to determine the oxygen flux across a membrane from measurements on corresponding powders (isotopic exchange and TGA). The adsorption and diffusion constants obtained are then introduced in the flux equation simulating the semi-permeability. The methodology, validated on three materials: Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF), La0.6Sr0.4Co0.2Fe0.δ et Ba0.95La0.05FeO3-δ, will allow to accelerate the discovery of new oxygen conducting. The OCM tests have been achieved on BSCF membrane modified by a thin layer of catalyst. Two catalysts have been selected: Mn/NaWO4 highly selective and LaSr/CaO highly active. The yield in membrane reactor cannot overstep 6%. A critical analysis has been achieved in order to design an optimal membrane reactor geometry for this reaction
Djehiche, Mokhtar. "Développement d’un couplage cw-CRDS – chambre de simulation pour la mesure in situ du radical HO2 et d’espèces d’intérêt atmosphérique". Thesis, Lille 1, 2011. http://www.theses.fr/2011LIL10045/document.
The continuous wave-Cavity Ring-Down Spectroscopy (cw-CRDS) is a very sensitive absorption technique used to selectively identify and quantify gaseous species at low concentrations and with a short acquisition time. We have developed an environmental chamber (110L) coupled with a near-IR cw-CRDS spectrometer for the detection of HO2 and other gaseous species. In order to demonstrate the performance of this setup, we have investigated two reaction systems. The first study concerns the methyl nitrite (CH3ONO) photolysis, which is known to generate OH radicals. The HONO product in the OH + CH3ONO reaction has been identified and quantified for the first time, which represents a very important step in the comprehension of this reaction. The formation of HONO and CH2O (a major product in the CH3ONO photolysis) has been studied under different experimental conditions. Secondly, the oxidation of methanol in air by chlorine atoms has been investigated. The HO2 radical has been observed for the first time by in-situ cw-CRDS in an environmental chamber. The kinetics of HO2 disappearance has been studied and the results confirm the rate constant value of the HO2 self reaction. A rather significant loss of HO2 on the walls of reactor has been observed at low pressure. Finally, the measurement of the photolysis frequencies of NO2, CH3ONO and Cl2 by various methods has allowed characterizing the experimental device developed in this work
Tonnet, Nicolas. "Dissociation des hydrates de méthane sédimentaires - Couplage transfert de chaleur / transfert de masse". Phd thesis, Ecole Nationale Supérieure des Mines de Saint-Etienne, 2007. http://tel.archives-ouvertes.fr/tel-00326878.
Dans cette étude, les transferts de masse et de chaleur ont été étudiés numériquement et expérimentalement. Un modèle numérique 2D est proposé dans lequel les transferts de chaleur et de masse gouvernent la dissociation des hydrates de méthane. Les résultats numériques montrent la présence de gradients de pression et de température au sein du milieu poreux et l'évolution de la frontière de dissociation selon le type de sédiment utilisé. Ce modèle est utilisé afin de dimensionner un dispositif expérimental de dissociation de carottes sédimentaires partiellement saturées en hydrates de méthane qui permet un suivi précis de la cinétique de dissociation.
Le montage expérimental est composé de cinq zones cylindriques de même diamètre (1/2 inch) mais de tailles différentes (pour une longueur totale de 2,6 m). Chaque zone est contrôlée en pression et en température. Chaque expérience consiste en une cristallisation d'hydrates de méthane au sein d'un milieu poreux, puis en une dissociation de ces mêmes hydrates par une méthode de contrôle de la pression à une extrémité du dispositif. La cinétique de dissociation est étudiée par le suivi de la pression dans un ballast (situé en aval du dispositif). Les résultats obtenus, via une étude paramétrique, permettent de cibler les paramètres clés de la dissociation de ces hydrates sédimentaires et d'observer leur impact sur la cinétique de dissociation. Deux régimes bien distincts de dissociation sont mis en évidence et caractérisés selon les propriétés du sédiment partiellement saturé en hydrates de méthane. Le rôle de la glace au cours de la dissociation est également étudié pour ces deux types de dissociation.
Enfin, la correspondance des résultats numériques et expérimentaux est mise en évidence par comparaison de courbes de cinétique de dissociation et de courbes d'évolution de la pression au sein du milieu poreux.
Gueritey, Nicolas. "Valorisation chimique du méthane par oxydation catalytique sélective". Vandoeuvre-les-Nancy, INPL, 1996. http://www.theses.fr/1996INPL034N.
El, Baghdadi Abdelkrim. "Évaluation de l'activité catalytique des composés zirconyle phosphates, alumines bêta et perovskites pour le couplage oxydatif du méthane". Thesis, National Library of Canada = Bibliothèque nationale du Canada, 1999. http://www.collectionscanada.ca/obj/s4/f2/dsk1/tape8/PQDD_0018/MQ48851.pdf.