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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.
Marchal, Éric. "Contribution à l'étude de la réaction catalytique du couplage oxydant du méthane sur des oxydes irradiés par microonde". Nancy 1, 1996. http://www.theses.fr/1996NAN10014.
Bouchoul, Nassim. "Valorisation du dioxyde de carbone par couplage plasma non-thermique et catalyse". Thesis, Poitiers, 2019. http://theses.univ-poitiers.fr/62720/2019-Bouchoul-Nassim-These.
The two main greenhouse gases emitted by human activities are carbon dioxide and methane. Within the context of the current environmental crisis, it has become vital to find a method to valorise these gases. Therefore, this thesis has been conducted to be a part of this process: CO2 and CH4 valorisation. To this end, dry reforming of methane was carried out by coupling non-thermal plasma and catalysts. Metal-based catalysts, such as Ni/Al2O3, are usually used for plasma-catalyst. However, the results are often dissimilar, and even contradictory, as far as conversions and selectivities are concerned. In order to better understand the reasons behind this heterogeneity, the influence of the nature of the solid was studied. For this purpose, metal oxides, such as γ-Al2O3, α-Al2O3, MgO, CaO, La2O3, ZnO, CeO2, SiO2, BaO, TiO2, and a zeolite, were selected because of their respective physicochemical properties (permittivity, acidity, basicity, specific surface). These oxides were submitted to identical tests with identical operational conditions, e.g. a dielectric barrier discharge reactor (DBD), 8W power (800 Hz frequency, 13 and 16 kV tension), a total output of 40 mL.min-1 and a CH4/CO2=0,5 ratio.The study of the physical characteristics of catalysts highlighted the impact of the material’s permittivity or of the size of its grains on the discharge. A high dielectric constant hindered the reaction. When TiO2 (εr=2903) was found in the discharge, it led to a decline in CH4 and CO2 conversions, as they decreased from respectively 20 and 9% without catalyst, to 5 and 2% with TiO2. Furthermore, when grains were too large, there was less surface accessible to plasma, which led to a fall in the reagents’ conversions. Indeed, they dropped from respectively 30 and 15% for CH4 and CO2 for small-sized grains (250-355µm), to 24 and 11% for the largest grains (800-1000µm). In addition to this, the study of the catalysts’ chemical properties showed how basicity influenced the conversions of carbon dioxide. It seemed that when there was a great number of basic sites in a solid, CO2 adsorption was likely to be better. Furthermore, a more detailed study was carried out by coupling calcium oxide with non-thermal plasma. Indeed, the former does not only have a low permittivity, but also a high number of basic sites. Structural and textural modifications appeared after plasma. This was shown by examining the influence of the CH4/CO2 ratio and of the temperature on CaO. When there was a CH4/CO2 = 2 ratio, for a temperature of 300°C, the production of water (reverse water-gas shift reaction) tended to result in the formation of Ca(OH)2 and CaCO3.When water (0,1g.h-1) was added to the reaction mixture, CaO hydroxylation and Ca(OH)2 carbonatation were observed. Furthermore, hydrated calcium hydroxide (Ca(OH)2+ 18% H2O) carbonatation is more likely to occur under plasma. The analysis of gases at the outlet by a mass spectrometer revealed an oscillatory phenomenon associated with CO2 adsorption. A reaction pathway, during which CO2 and H2O adsorption and elimination occur successively, was therefore put forward. A low-energy plasma (4W) is likely to cause carbonatation, as the solid is originally composed of 0,9Ca(OH)2, 0,9 H2O, 0,1 CaCO3, and is made of 0,1Ca(OH)2, 0,9CaCO3 after plasma. Thus, applying a non-thermal plasma seems to encourage CO2 diffusion at the core of Ca(OH)2+ 18% H2O. Carbonatation is a method to store CO2 but it is a slow process, which is often hindered by CO2 diffusion. In this study, plasma was proved to be a highly interesting process, provided that its efficiency could be increased
Araújo, Lima Borges Heloisa de. "Optimisation de catalyseurs à base de lanthane en couplage oxydant du méthane par modification chimique et par mise en oeuvre d'un réacteur à membrane". Lyon 1, 1995. http://www.theses.fr/1995LYO10009.
Barbe, Pascal. "Étude expérimentale de la réaction de couplage oxydant du méthane à l'aide d'un réacteur continu agité à surface catalytique variable". Vandoeuvre-les-Nancy, INPL, 1993. http://www.theses.fr/1993INPL104N.
Olivier, Louis. "Étude du couplage oxydant du méthane : approche combinée de la formulation des catalyseurs, de la cinétique de la réaction et de l'ingénierie des réacteurs". Thesis, Lyon 1, 2010. http://www.theses.fr/2010LYO10051.
The oxidative coupling of methane (OCM) is a complex heterogeneous catalytic reaction allowing the direct conversion of methane to ethylene, at a lower energetic cost than the current industrial processes. OCM requires a temperature higher than 700°C at atmospheric pressure. Hence, there is competition with total oxidation. In the numerous studies reported in literature, the limit of 25% C2 (ethane + ethylene) yield could not be overtaken. Proposed mechanisms are not relevant for all active materials or on all operating condition ranges. A new way to approach the reaction would be to take into account the wider possible panel of parameters involved in this process, from formulation to reactors targeting at process optimisation. The present study permitted to extract relevant descriptors of OCM process from experimental data and establish relationships between descriptors and performances. LaSrCaO catalysts were selected and tested in a parallel fixed-bed reactor and the data obtained were used to validate a micro-kinetic model in this reactor. Experiments were also performed successfully in a dense membrane reactor to improve ethylene productivity. The role played catalyst surface composition was also identified and a critical analysis of the global method implemented concludes this work
Crunelle, Benoît. "Étude de flammes basse pression de méthane et d'éthane par couplage faisceau moléculaire : spectrométrie de masse avec ionisation par impact électronique ou multiphotonique et par modélisation". Lille 1, 1995. http://www.theses.fr/1995LIL10163.
Gasnot, Laurent. "Application du couplage de la fluorescence induite par laser et de la chromatographie à l'étude de la formation de NO dans des flammes basse pression méthane/air". Lille 1, 1995. http://www.theses.fr/1995LIL10140.
Manzalji, Tammam. "Conversion du propylène en acrylonitrile au moyen de NO sur des catalyseurs supportés à base d'oxyde de plomb et couplage oxydant du méthane en éthane en présence de N2O sur ces mêmes catalyseurs". Lyon 1, 1992. http://www.theses.fr/1992LYO10247.
Guérin, Frédéric. "ÉMISSION DE GAZ A EFFET DE SERRE (CO2, CH4) PAR UNE RETENUE DE BARRAGE HYDROÉLECTRIQUE EN ZONE TROPICALE (PETIT-SAUT, GUYANE FRANÇAISE) :EXPÉRIMENTATION ET MODÉLISATION". Phd thesis, Université Paul Sabatier - Toulouse III, 2006. http://tel.archives-ouvertes.fr/tel-00079947.
Sur 10 ans, les émissions atmosphériques se sont avérées très significatives, notamment les trois premières années ayant suivies la mise en eau, puis décroissent au cours du temps. Tandis que 50% des émissions de CO2 ont lieu à la surface du lac, les émissions de CH4 sont principalement localisées en aval des turbines.
Les émissions atmosphériques résultent de la dégradation de la MO (sol et biomasse issus de la forêt tropicale) immergée lors de la mise en eau et leur diminution au cours du temps découle de l'épuisement du stock de MO. Au terme de 10 ans, 20% du stock de carbone a été minéralisé et émis vers l'atmosphère sous forme de CO2 et de CH4. L'oxydation aérobie du CH4 transforme plus de 95% du CH4 diffusant depuis l'hypolimnion en CO2 dans la colonne d'eau du lac et 40% du CH4 entrant dans la rivière à l'aval. A l'échelle du barrage ce processus est responsable de l'oxydation de 90% du CH4 produit et de 30% des émissions totales de CO2. Le CH4 et le CO2 qui atteignent les eaux de surface du barrage sont émis vers l'atmosphère par flux diffusifs. L'étude de ce processus de transfert gazeux à l'interface air-eau montre que, en milieu tropical, les flux diffusifs sont accélérés par les fortes températures et les phénomènes pluvieux.
Le modèle est basé sur le modèle hydrodynamique SYMPHONIE 2D et les modules biogéochimiques développés dans le cadre de cette étude à partir des données cinétiques des processus étudiés. Les profils verticaux simulés de température, d'oxygène, de CO2 et de CH4 sont bien reproduits. Ce modèle pose les bases d'un outil opérationnel de modélisation pour la retenue de Petit Saut ainsi que pour d'autres réservoirs en milieu tropical.
Guérin, Frédéric. "Emission de gaz à effet de serre (CO2,CH4) par une retenue de barrage hydroélectrique en zone tropicale (Petit-saut, Guyane française) : expérimentation et modélisation". Toulouse 3, 2006. https://tel.archives-ouvertes.fr/tel-00079947.
The emissions of carbon dioxide (CO2) and methane (CH4) and the carbon cycle in the Petit-Saut reservoir and in the Sinnamary River (French Guiana) were studied with an aim of developing a coupled physical/biogeochemical model. The development of this model required the study of three processes controlling these emissions: (i) CO2 and CH4 production during the mineralization in anoxic condition of organic matter (OM) from soils and plants, (ii) aerobic CH4 oxidation in the water column of the lake and (iii) the processes involved in gas exchange at the air-water interface. Over 10 years, atmospheric emissions were shown to be very significant, in particular the first three years having followed the reservoir impoundment and then decreased with time. While 50% of the CO2 emissions take place at the surface of the lake, the emissions of CH4 are mainly localized downstream from the turbines. The atmospheric emissions result from the degradation of OM (soil and biomass originating from the tropical forest) flooded during impoundment and their reduction with time rises from the exhaustion of the OM stock. 10 years after impoundement, 20% of the carbon stock were mineralized and emitted to the atmosphere in the form of CO2 and of CH4. Aerobic CH4 oxidation transforms more than 95% of the CH4 diffusing upward from the hypolimnion into CO2 in the water column of the lake and 40% of the CH4 entering the river downstream of the dam. In the whole Petit Saut system, this process is responsible for the oxidation of 90% of the produced CH4 and 30% of the total CO2 emissions. The CH4 and CO2 which reach the water surface of the reservoir and of the river downstream of the dam are emitted to the atmosphere by diffusive flux. The study of this process of gas transfer to the interface air-water shows that, in tropical environment, diffusive fluxes are enhanced by the elevated temperatures and the rainy phenomena. The model is based on the hydrodynamic model SYMPHONY 2D and the biogeochemical model developed during this study starting from the kinetic data of the studied processes. The simulated vertical profiles of temperature, oxygen, CO2 and CH4 are well reproduced. This model poses the bases of an operational tool of modeling for the Petit-Saut reservoir like for other reservoirs in tropical environments
Awada, Hawraà. "Synthèse sélective de γ-amino acides cyclobutaniques : préparation de nouveaux organogélateurs peptidiques". Thesis, Paris 11, 2014. http://www.theses.fr/2014PA112365/document.
The γ-aminobutyric acid (GABA) is the major inhibitory neurotransmitter in the central nervous system (CNS). In order to obtain new enantiomerically pure cyclobutanic derivative of GABA, the cis-3,4CB-GABA, two efficient synthetic strategies have been established. Both synthetic routes employed a photocycloaddition [2 +2] protocol, which provided the cyclobutanic ring. The first route involved the homolgation of the cis-2-aminocyclobutanecarboxylic acid (cis-ACBC), whereas the second route is a multi-step synthesis using caprolactam as starting material.On the other hand, the (1R,2S)-cis-GABA-2,3CB was synthetized, and a series of N- and C-protected oligomers of di, tri, and tetrapeptides of this amino acid were prepared. These oligomers were characterized by NMR (1D and 2D) techniques, IR, and X-ray. The analyses have shown that there are no non-covalent interactions (hydrogen bonds) between the residues of each oligomers. However, the gelation property of these oligomers in various organic solvents was demonstrated. Solutions and gels formed from these peptides were analyzed by scanning electron microscopy, and the obtained images showed a fibrous organization of the di- and tetrapeptide, while the tripeptide showed no regular intermolecular assembly
Hue, Vincent. "Modélisations photochimiques saisonnières des stratosphères de Jupiter et Saturne". Thesis, Bordeaux, 2015. http://www.theses.fr/2015BORD0155/document.
One of the goals of this thesis is to interpret the observations of the main hydrocarbons(C2H2 and C2H6) from Cassini (NASA/ESA) on Jupiter and Saturn. The one-dimensional photochemical models are insufficient to explain these spatially resolved observations. I have developed the first two-dimensional (altitude-latitude) seasonal photochemical model for the giant planets, which predicts their chemical composition.Without meridional transport, Saturn’s chemical composition follows the insolation variations. The C2H2 and C2H6 abundances measured by Cassini (Guerlet et al., 2009)are reproduced from the equator up to mid-latitudes, at pressures higher than 0.1mbar.At higher latitudes, the disagreements suggest either a stratospheric circulation cell orthe signature of ion-neutral chemistry. For the first time, I have coupled our seasonal photochemical model with the seasonal radiative model of Greathouse et al. (2008). I predict that the seasonal temperature peak is shifted half a season earlier, with respect to previous models, at high latitudes in the higher stratosphere.Jupiter shows weak seasonal variations of chemical composition, only controlled by its orbital eccentricity. The observed meridional distributions of C2H2 and C2H6 show opposition trends (Nixon et al., 2010). C2H6 observed distribution is reproduced when Isuppose a combination of meridional diffusion and stratospheric circulation, while causingat the same time a stronger agreement with the C2H2 observations. Accounting for theion-neutral chemistry might preferentially affect C2H2 and potentially play a key role on hydrocarbon abundances in Jupiter’s stratosphere
Sayes, Morgane. "Développement d'une réaction d'amidation utilisant le diphénylsilane en tant qu'agent de couplage et d'une réaction de borocyclopropanation photochimique". Thèse, 2019. http://hdl.handle.net/1866/23405.
This manuscript describes the work carried out in Pr. Charette’s laboratory between 2015 and 2019. It can be divided into two different topics: the development of new amidation strategies and the development of new cyclopropanation methodologies. Amide synthesis is still a challenge for the scientific community nowadays. Indeed, the development of simple, robust, atom economical and environmental friendly procedures remain one of the research priority in organic chemistry. To contribute to this field, an amide synthesis methodology has been developed by using diphenylsilane as a coupling reagent. The latter is commercially available, stable and cheap. Moreover, only a siloxane and dihydrogen are generated during the reaction. The developed methodology has also been applied to the synthesis of a series of di- and tripeptides. The cyclopropane moiety has been increasingly used in pharmaceuticals. Indeed, this moiety can influence different crucial parameters in the development of bioactive molecules. The development of new cyclopropanation methodologies is therefore a relevant field. Borocyclopropane synthesis is of particular interest: as a matter of fact, these compounds can create structural diversity via boronate functionalization. In order to obtain a user-friendly, robust and greener chemical process, a photochemical approach using continuous flow technology has been favored. A photoredox borocyclopropanation of styrenes has been developed; the latter is carried out under UV-A irradiation with xanthone as a photosensitizer. Mechanistic studies have supported that this transformation proceeds according to two concurrent photoredox catalytic cycles. Finally, a new diiodo reagent bearing a pinacol boronate group and a trimethylsilyl group has been developed to access gem-disubstituted cyclopropanes. The bases of a UV-visible photochemical process using this new reagent have then been established. Thereby, the first example of a gem-borocyclopropyl silane derived from styrene has been synthesized.