Cette thèse est une contribution à l’étude des flammes de méthane turbulentes non prémélangées en rotation, dites swirlées, avec ou sans enrichissement en oxygène de l’oxydant. L’étude se focalise sur la stabilité de la flamme, les émissions polluantes et la dynamique du jet en non réactif et réactif. Notre dispositif expérimental se compose d’un brûleur à swirler coaxial avec injection radiale de méthane au voisinage de la sortie du brûleur. Ce dernier est confiné dans une chambre de combustion. La teneur en oxygène dans l’oxydant, le nombre de swirl géométrique et la richesse globale à l’injection sont les principaux paramètres qui peuvent être précisément contrôlés. La stabilité de la flamme est caractérisée par chimiluminescence OH*. Les émissions polluantes sont mesurées par des analyseurs en ligne via un prélèvement dans les gaz brûlés. La dynamique du jet est caractérisée principalement par PIV stéréoscopique dans un plan longitudinal et plusieurs plans transverses. La diffusion du méthane dans le jet swirlé est abordée qualitativement par fluorescence induite par laser de l’acétone dans un plan. À ce jour, peu de travaux portent sur la caractérisation notamment dynamique de ces flammes swirlées avec enrichissement en O2. La mise en rotation du jet est à l’origine d’une zone de recirculation centrale qui favorise la stabilisation de la flamme en régime pauvre et à grand nombre de Reynolds. L’étude des émissions polluantes montre que les régimes de combustion à l’air pour lesquels la flamme est liftée stable sont aussi ceux qui produisent du CO et du CH4 résiduel en des quantités non négligeables. L’enrichissement en oxygène permet alors de convertir les imbrûlés et ce pour de faibles enrichissements tout en améliorant la stabilité de flamme via une diminution de la hauteur d’accrochage et des fluctuations associées comme le confirment de précédentes études. L’augmentation des NOx par la voie thermique a été quantifiée pour des enrichissements en oxygène inférieurs à 30 % vol. L’étude systématique en non réactif et réactif apporte des détails sur la topologie tridimensionnelle du jet swirlé suivant les paramètres de l’étude. L’étude de la décroissance des vitesses et de la décroissance du nombre de swirl dans la direction de l’écoulement permetde mettre en évidence l’effet de la flamme sur le jet swirlé. Un couplage entre l’évolution du taux d’entraînement par la recirculation externe et les émissions polluantes est mis en évidence pour expliquer l’évolution des NOx suivant la richesse globale à l’injection. Nous avons proposé une modélisation des écoulements swirlés qui repose sur les écoulements à vorticité hélicoïdale afin d’identifier les caractéristiques principales des structures hélicoïdales au sein de l’écoulement. / This thesis is a contribution to the study of turbulent non-premixed swirling methane flames with or without oxygen addition in the oxidizer. The study deals with the flame stability, the pollutant emissions and the jet dynamic behaviour in non-reacting and reacting conditions. The burner, operating in a combustion chamber, consists of two concentric tubes with a swirler placed in an annular arrangement, which supplied the oxidant flow (air or oxygen-enriched air). The central pipe delivers fuel (methane) radially just below the burner exit plane. The oxygen content in the oxidizer, the geometric swirl number and the global equivalence ratio are the main parameters, which can be precisely set. OH* chemiluminescence imaging is used to characterize flame stability. Multi-gas analyzers are used to measure pollutant emissions in the exhaust gas. The flow is characterized using stereoscopic PIV measurements in different longitudinal and transverse planes. A qualitative study dealing with the methane diffusion imaging is also conducted by use of acetone planar laser-induced fluorescence. Up to now only few studies have examined the dynamic behavior of this type of swirled flames with oxygen addition. Introducing swirl allows creating a central recirculation zone which favors lean flame stabilization at higher Reynolds numbers. The mapping of the combustion regimes combined with the pollutant emission results show that the stable lifted flames are related to high CO and residual CH4 emission levels in the exhaust gas. Oxygen addition, even by a few percent, allows improving CO and unburned hydrocarbons conversion and increasing flame stability at the same time via a decrease of liftoff heights and the related fluctuations. The NOx emissions increase via the thermal pathway with increasing the oxygen-enrichment rate up to 30 % vol. A comparative study in non-reacting and reacting conditions is conducted to give insight into the tridimensional flow field topology varying the above-mentioned parameters. Mean streamwise velocity and swirl number decay rates show the flame effects on the flow dynamics. A coupling mechanism between the entrainment rate of the surroundings via the external recirculation and the pollutant emissions is proposed to explain the NOx emission trend with the global equivalence ratio. A model is also proposed based on the helical vortices to identify the main features of helix structures in the jet in non-reacting and reacting conditions.

<p dir="ltr">Interest in using detonation-based combustion cycles for use propulsion and power generation has gained considerable attention in the last 10 years or so. The rotating detonation engine (RDE), in particular, has garnered the most attention as a possible replacement for current generation combustion systems. RDEs are continuous flow devices that typically operate in a non-premixed fashion. Reactants are injected into an annular combustion chamber that is usually several millimeters wide. One or more detonation waves propagate azimuthally around the annulus, consuming the reactants. The products then expand out of the combustor where it can produce thrust or be passed into a turbine. The detonation wave front in RDEs travel at speeds between 1-3 km/s which poses additional complexity beyond traditional combustors. There are large gaps in the research community for RDEs that use one or more liquid based propellants. Questions regarding liquid breakup, atomization, breakup, recovery all remain unanswered both experimentally and numerically. This work seeks to understand these fundamental physical phenomena that drive these devices by applying advanced, high-speed laser and other optical diagnostics. </p><p dir="ltr"> A 120 mm nominal diameter rotating detonation combustor that operates on non-premixed hydrogen-air was modified to remove a hydrogen orifice and was replaced with a single liquid fuel injector. This simple, yet important, modification enables the study of a one-way coupling between a liquid fuel jet and a detonation wave at relevant spatio-temporal scales. Planar laser-induced fluorescence was performed at rates up to 1 MHz to quantify the quasi-steady jet dynamics and the recovery behavior of the single liquid jet. Long-duration PLIF imaging lasting 30-40 detonation periods at 300 kHz was also performed for statistical significance. A diesel liquid-in-crossflow injector was observed to breakup or be removed from the PLIF plane within only a few microseconds. After the detonation wave passes through the spray there is a significant dwell period can last between 20-40% of the detonation period before the new fuel is issued into the channel. The quasi-steady liquid jet trajectory was also compared to a jet-in-crossflow from literature and there is decent agreement in the jet near-field. </p><p dir="ltr"> The same hardware scheme with a different liquid fuel injector was tested in conjunction with an alternative imagine scheme. The first technique was able to capture details in the radial-axial plane but could not resolve any motion in the azimuthal direction. A volume-based illumination scheme was used for LIF to image a liquid fuel jet in the azimuthal-axial plane. For this experiment the location of the liquid fuel jet was moved into a different position and as a result experiences significantly different behavior than the jet in crossflow. The breakup and evaporation process takes place over a much longer period of time and there is no pause of liquid fuel injection. Similarly, LIF was performed at 300 kHz for 30 detonation cycles to enable sadistically quantification and phase averaging. Filtered OH* and CH* chemiluminescence imaging was also performed over the same field of view as the LIF imaging. Estimation of the velocity field was calculated using optical flow from the Jet-A LIF images. The velocity results agree well with the recovery analysis from the PLIF measurements.</p><p dir="ltr"> Using the same liquid fuel injection scheme, Jet-A droplet diameter and velocity was measured <i>in-situ</i> during a hot-fire experiment using phase Doppler interferometry (PDI). Although a point technique, PDI was used to measure thousands of droplets during a single test at multiple locations and with multiple conditions. As a means of comparison, cold flow experiments were performed with water in the exit plume. Droplet diameters were measured between 1-20 µs in both cases. PDI results were compared with the optical flow results and there is agreement in median velocities and some differences in the minimum and maximum velocity values. Possible sources of error in the diameter measurement are discussed as well.</p>

Este projeto nasceu inserido num contexto de crescentes pesquisas em direção à construção de um cabedal de conhecimento acerca das ciências ambientais que tratam e estudam a dinâmica dos reservatórios de carbono e suas contribuições para o Efeito Estufa. Extrapolações de novos mapas digitalizados de solos sugerem que os espodossolos hidromórficos da Amazônia podem estar com uma contagem de carbono subestimada em até 12,3 Pg de C e trabalhos anteriores mostram que o carbono imobilizado neste perfil pode sofrer mineralização devido ao corte na rede de drenagem ou rebaixamento do nível freático, podendo assim contribuir em grande parte para o aumento de emissão dos Gases do Efeito Estufa. Nesta circunstância, coube a este trabalho, caracterizar espectroscopicamente, a matéria orgânica estocada em profundidade em 9 perfis de solo da região de São Gabriel da Cachoeira - AM, na floresta amazônica. Foram analisadas 127 amostras em quantidade de carbono e por fluorescência induzida por laser (FIL). A partir destas análises preliminares, foi possível selecionar 12 amostras de 2 perfis para análise mais detalhada através da extração das substâncias húmicas. Foram realizadas análises para obtenção da textura destes perfis, análise dos ácidos húmicos como relação C/N, espectroscopia de infravermelho com transformada de Fourier (FTIR), RMN de 13C no estado sólido, fluorescências bidimensional e tridimensional com aplicação do método estatístico análise dos fatores paralelos (PARAFAC) e também análise dos ácidos fúlvicos como carbono orgânico total (TOC), espectroscopia na região do ultra-violeta e visível e fluorescência 3D associada ao PARAFAC. Em geral, as amostras se dividiram em 3 grupos diferentes, onde a matéria orgânica em superfície se mostrou lábil e recente, a matéria orgânica nos horizontes B húmicos se mostraram com características recalcitrantes e a matéria orgânica contida nos horizontes onde existia água livre (lençol freático), se mostraram com características diferentes, indicando não serem tão jovens quanto as em superfície, porém mais jovens do que a armazenada no Bh, devido a uma possível migração por movimentos laterais do lençol freático. A correlação entre os resultados mostrou que a textura do solo é importante para o acúmulo da matéria orgânica e conseqüentemente sua humificação. Os resultados de fluorescência corroboraram a interpretação dos dados de RMN, FTIR e textura, apontando que o Perfil 4 (mais próximo ao rio) por ter C2 maior nos horizontes intermediários, contém maior quantidade de exsudatos microbianos frescos. Para o Perfil 5, que é uma mancha de Espodossolo dentro de um Latossolo e encontra-se mais longe do rio, os fluoróforos mais representativos são oriundos de anéis aromáticos mais antigos e conseqüentemente mais humificados, devido às maiores intensidades de C1 e C3. Vale ressaltar que esta interpretação se alinha com os resultados de datação do 14C desta região. Foi notório que a humificação ocorre a partir do começo do horizonte Bh e que seu acúmulo pode ocorrer tanto nos horizontes intermediários (Bh) quanto mais os profundos (úmidos). Dessa forma, pode-se concluir que uma drenagem excessiva das bordas dos rios nesta região que acumula carbono em profundidade, poderá expor a MO guardada e estocada a longo tempo, contribuindo para o aumento da temperatura global e por conseguinte catalisando um desequilíbrio no clima da sua maior reguladora no mundo: a Floresta Amazônica. / This project was born inserted in a context of increasing research towards building knowledge about environmental science that treat and study the dynamics of carbon reservoirs and their contribution to the greenhouse. Extrapolation of new digital soil maps suggests that Amazonian hydromorphic Spodosols may be with a carbon accounting underestimated by up to 12.3 Pg of C and previous work show that the carbon fixed in this profile may suffer mineralization due to the cut in the drainage network or lowering of the water level and can contribute largely to the increased emission of greenhouse gas. In this circumstance, it was instructed to this work, the spectroscopic characterization, of the stored organic matter in depth at 9 soil profiles of São Gabriel da Cachoeira - AM, in the Amazon rainforest. 127 samples were analyzed for amount of carbon and laser-induced fluorescence (LIF). From these preliminary analyzes, it was possible to select 12 samples of 2 profiles for humic substances extraction and further detailed analysis. Analyzes were conducted to obtain the texture of these profiles, analysis of humic acids as C/N ratio, Fourier Transform Infrared Spectroscopy (FTIR), solid state 13C NMR, two and three dimensional fluorescence with applying of the Parallel factors analysis (PARAFAC) statistical method and also fulvic acid analysis as Total Organic Carbon (TOC), ultra-violet and visible region spectroscopy and 3D fluorescence associated with PARAFAC. In general, the samples were divided into 3 different groups, wherein the surface organic matter evinced labile and recent. The B humic horizons organic matter proved recalcitrant characteristics and organic matter contained in horizons which had free water (groundwater), showed different characteristic, indicating they are not so young as the surface, but younger than stored in Bh, because of possible migration by lateral movements of the water table. The correlation between the results showed that soil texture is important for the accumulation of organic matter and therefore its humification. The fluorescence results confirmed the interpretation of the NMR, FTIR and texture datas, indicating that the profile 4 (closest to the river), presenting major C2 in intermediate horizons, contains larger amount of fresh microbial exudates. To profile 5, which is a Spodosol spot within a Ferrasol and is thither from the river, the most representative fluorophores came from older aromatic rings and therefore is more humified, due to higher intensities C1 and C3. It is noteworthy that this interpretation is in accord with the results of 14C dating of samples from this region. It was clear that the humification occurs from the beginning of the Bh horizon and their accumulation can occur both in the intermediate horizons (Bh) and in deeper (wet). Thus, it can be concluded that excessive drainage of the edges of rivers in this region that collects carbon in depth, may expose the OM stored for long time, contributing to increase the overall temperature and therefore catalyzing an imbalance in the climate of the biggest regulatory of it in the world: the Amazon rainforest.

Este projeto nasceu inserido num contexto de crescentes pesquisas em direção à construção de um cabedal de conhecimento acerca das ciências ambientais que tratam e estudam a dinâmica dos reservatórios de carbono e suas contribuições para o Efeito Estufa. Extrapolações de novos mapas digitalizados de solos sugerem que os espodossolos hidromórficos da Amazônia podem estar com uma contagem de carbono subestimada em até 12,3 Pg de C e trabalhos anteriores mostram que o carbono imobilizado neste perfil pode sofrer mineralização devido ao corte na rede de drenagem ou rebaixamento do nível freático, podendo assim contribuir em grande parte para o aumento de emissão dos Gases do Efeito Estufa. Nesta circunstância, coube a este trabalho, caracterizar espectroscopicamente, a matéria orgânica estocada em profundidade em 9 perfis de solo da região de São Gabriel da Cachoeira - AM, na floresta amazônica. Foram analisadas 127 amostras em quantidade de carbono e por fluorescência induzida por laser (FIL). A partir destas análises preliminares, foi possível selecionar 12 amostras de 2 perfis para análise mais detalhada através da extração das substâncias húmicas. Foram realizadas análises para obtenção da textura destes perfis, análise dos ácidos húmicos como relação C/N, espectroscopia de infravermelho com transformada de Fourier (FTIR), RMN de 13C no estado sólido, fluorescências bidimensional e tridimensional com aplicação do método estatístico análise dos fatores paralelos (PARAFAC) e também análise dos ácidos fúlvicos como carbono orgânico total (TOC), espectroscopia na região do ultra-violeta e visível e fluorescência 3D associada ao PARAFAC. Em geral, as amostras se dividiram em 3 grupos diferentes, onde a matéria orgânica em superfície se mostrou lábil e recente, a matéria orgânica nos horizontes B húmicos se mostraram com características recalcitrantes e a matéria orgânica contida nos horizontes onde existia água livre (lençol freático), se mostraram com características diferentes, indicando não serem tão jovens quanto as em superfície, porém mais jovens do que a armazenada no Bh, devido a uma possível migração por movimentos laterais do lençol freático. A correlação entre os resultados mostrou que a textura do solo é importante para o acúmulo da matéria orgânica e conseqüentemente sua humificação. Os resultados de fluorescência corroboraram a interpretação dos dados de RMN, FTIR e textura, apontando que o Perfil 4 (mais próximo ao rio) por ter C2 maior nos horizontes intermediários, contém maior quantidade de exsudatos microbianos frescos. Para o Perfil 5, que é uma mancha de Espodossolo dentro de um Latossolo e encontra-se mais longe do rio, os fluoróforos mais representativos são oriundos de anéis aromáticos mais antigos e conseqüentemente mais humificados, devido às maiores intensidades de C1 e C3. Vale ressaltar que esta interpretação se alinha com os resultados de datação do 14C desta região. Foi notório que a humificação ocorre a partir do começo do horizonte Bh e que seu acúmulo pode ocorrer tanto nos horizontes intermediários (Bh) quanto mais os profundos (úmidos). Dessa forma, pode-se concluir que uma drenagem excessiva das bordas dos rios nesta região que acumula carbono em profundidade, poderá expor a MO guardada e estocada a longo tempo, contribuindo para o aumento da temperatura global e por conseguinte catalisando um desequilíbrio no clima da sua maior reguladora no mundo: a Floresta Amazônica. / This project was born inserted in a context of increasing research towards building knowledge about environmental science that treat and study the dynamics of carbon reservoirs and their contribution to the greenhouse. Extrapolation of new digital soil maps suggests that Amazonian hydromorphic Spodosols may be with a carbon accounting underestimated by up to 12.3 Pg of C and previous work show that the carbon fixed in this profile may suffer mineralization due to the cut in the drainage network or lowering of the water level and can contribute largely to the increased emission of greenhouse gas. In this circumstance, it was instructed to this work, the spectroscopic characterization, of the stored organic matter in depth at 9 soil profiles of São Gabriel da Cachoeira - AM, in the Amazon rainforest. 127 samples were analyzed for amount of carbon and laser-induced fluorescence (LIF). From these preliminary analyzes, it was possible to select 12 samples of 2 profiles for humic substances extraction and further detailed analysis. Analyzes were conducted to obtain the texture of these profiles, analysis of humic acids as C/N ratio, Fourier Transform Infrared Spectroscopy (FTIR), solid state 13C NMR, two and three dimensional fluorescence with applying of the Parallel factors analysis (PARAFAC) statistical method and also fulvic acid analysis as Total Organic Carbon (TOC), ultra-violet and visible region spectroscopy and 3D fluorescence associated with PARAFAC. In general, the samples were divided into 3 different groups, wherein the surface organic matter evinced labile and recent. The B humic horizons organic matter proved recalcitrant characteristics and organic matter contained in horizons which had free water (groundwater), showed different characteristic, indicating they are not so young as the surface, but younger than stored in Bh, because of possible migration by lateral movements of the water table. The correlation between the results showed that soil texture is important for the accumulation of organic matter and therefore its humification. The fluorescence results confirmed the interpretation of the NMR, FTIR and texture datas, indicating that the profile 4 (closest to the river), presenting major C2 in intermediate horizons, contains larger amount of fresh microbial exudates. To profile 5, which is a Spodosol spot within a Ferrasol and is thither from the river, the most representative fluorophores came from older aromatic rings and therefore is more humified, due to higher intensities C1 and C3. It is noteworthy that this interpretation is in accord with the results of 14C dating of samples from this region. It was clear that the humification occurs from the beginning of the Bh horizon and their accumulation can occur both in the intermediate horizons (Bh) and in deeper (wet). Thus, it can be concluded that excessive drainage of the edges of rivers in this region that collects carbon in depth, may expose the OM stored for long time, contributing to increase the overall temperature and therefore catalyzing an imbalance in the climate of the biggest regulatory of it in the world: the Amazon rainforest.