Este trabalho analisa os efeitos da transferência de calor por radiação térmica em uma chama laminar resultante da combustão de metano com ar. No processo, são resolvidas as equações da continuidade, da quantidade de movimento, da conservação das espécies químicas e da energia. Ainda é utilizado um modelo de formação de fuligem a duas equações e o modelo de combustão de Arrhenius considerando um mecanismo com 112 reações químicas. Para avaliar os efeitos da radiação térmica, o divergente do fluxo radiante é calculado considerando quatro modelos diferentes para os gases: o modelo do gás cinza, a soma ponderada de gases cinzas, e os métodos SLW e CW. Nessa modelagem, é considerado um meio participante composto por monóxido de carbono, dióxido de carbono, vapor d’água e fuligem. No modelo do gás cinza e da soma ponderada de gases cinzas, o coeficiente de absorção da mistura é obtido por correlações que consideram a temperatura local e a concentração do meio. Nos modelos SLW e CW, o coeficiente de absorção é calculado baseado no banco de dados HITEMP. Assim, primeiramente os resultados do divergente do fluxo radiante são confrontados com os diferentes modelos considerando campos pré-estabelecidos de temperatura e concentrações da mistura de gases com a presença de fuligem e, em seguida, é feita uma análise da influência da radiação considerando uma chama difusa oriunda do processo de combustão de metano com ar. Apesar de o meio analisado ser opticamente fino, situação em que os efeitos da absorção são muito baixos, os resultados encontrados para o divergente do fluxo radiante com os modelos de radiação usados na pesquisa mostraram uma diferença média de aproximadamente 20% entre os modelos, chegando a uma diferença máxima local de mais de 50% quando foi considerado o modelo WSGG. Por outro lado, nas situações em que é considerado todo o processo de combustão, a diferença maior ocorre na comparação de casos em que a radiação térmica é negligenciada com os casos em que a radiação é considerada. Os efeitos causados entre os diferentes modelos de radiação no campo de temperaturas e concentrações dos gases foram pequenos. Assim, é observado que, mesmo em meios opticamente finos, a modelagem da radiação térmica é necessária, pois causa diferenças significativas nos resultados e que nesse tipo de meio não é necessário o uso de modelos mais sofisticados de radiação, pois os efeitos da absorção dos gases é muito pequeno. / This work analyses the effects of thermal radiation heat transfer on methane-air laminar diffusion flames. The analysis is based on the solution of the equations of continuity, fluid motion, species mass-fraction and enthalpy. The soot formation is accounted with a twoequation model while a chemistry mecanism with 112 reactions is used for the combustion of methane. To evaluate the effects of thermal radiation, the divergence of the radiative heat flux is calculated based on four different gas models: the gray gas, the weighted sum of gray gases, the SLW and the CW model. In the modeling, it is considered a participating media composed of carbon monoxide, carbon dioxide, water vapor and soot. Both in the gray gas model and in the weighted sum of gray gases model, the absorption coefficient of the mixture is obtained by correlations that depend on the local temperature and concentration of the medium. On the other hand, in the SLW and CW models, the absorption coefficient is calculated based on the HITEMP spectral database. Thus, the results of the divergence of the radiative heat flux are compared with the different gas models based on a temperature and concentration fields previously obtained, and then, the four gas models used are considered in the entire combustion process to verify the influence of the radiation heat transfer. The results obtained for the divergence of the radiative heat flux considering the four different radiation models used showed an avereged difference of 20%, with a maximum local difference of more than 50%, when the WSGG model was considered. On the other hand, in situations where the whole combustion process is considered, the major difference occurs when is compared the results obtained with a radiation model and the ones where it is neglected. The effects observed with the different radiation models in the temperature field and the gas concentrations were small. Thus is observed that, even in optically thin media, the thermal radiation gas modeling is necessary, and in this particular kind of media, the use of sofisticated gas models are not necessary, because the absorption effect fo the gases are small when compared with their emission.

Les enjeux écologiques liés au réchauffement climatique, et plus généralement la lutte contre la pollution, ont occasionné une révolution sans précédent dans le domaine des transports. De nombreuses recherches portant sur l’identification de voies d’amélioration du rendement mécanique des moteurs à combustion interne ont été menées au cours de ces dernières décennies. Dans les moteurs Diesel, le contact Segments-Piston-Chemise (SPC) représente à lui seul près de 40 % des pertes d’énergie par frottement mécanique totales du moteur. Ce travail de thèse s’inscrit dans le cadre général de la lubrification des moteurs Diesel en présence de suies et s’intéresse plus particulièrement au poste SPC pour des contacts Diamond-Like Carbon (DLC) lubrifiés. Ce travail de thèse s’appuie sur des outils de tribométrie originaux pour reproduire les cinématiques particulières des contacts impliqués au niveau de la segmentation. Cette thèse s’attache à identifier l’influence d’un lubrifiant vieilli en fonctionnement sur les mécanismes de lubrification et les mécanismes de frottement associés de couches minces dures de type DLC, en balayant l’ensemble des régimes de lubrification pour des conditions stationnaires et transitoires. Les revêtements DLC développés dans le cadre de ce travail de thèse ont permis de diminuer significativement le frottement limite en conditions stationnaires et transitoires. La déstructuration du lubrifiant via la formation d’agrégats, générés par le passage des suies, ou par une annulation temporaire de la vitesse d’entraînement représentative des cinématiques de contact observées en zone SPC, sont gouvernés par le triptyque, lubrifiant, surface et cinématique de contact. Enfin, l’analyse de la réponse tribologique de l’interface lubrifiée en conditions stationnaires et transitoires permet à la modélisation théorique du frottement lors d’un cycle complet de glissement à vitesses variables. / Ecological issues related to global warming, and more generally the reduction of pollution, have lead to a major revolution in the field of transport. Considerable research work has been carried out during the past decades in order to improve the mechanical efficiency of internal combustion engines. In Diesel engines, almost 40 % of total engine energy losses due to mechanical friction occur in the Piston rings-Piston-Cylinder contact (PPC). The overall framework of this PhD thesis is Diesel engine lubrication in presence of soot and this work focuses more particularly on Diamond-Like Carbon (DLC) lubricated contacts for PPC region. Unique tribometry tools are used to reproduce the particular contact kinematics involved in the piston assembly. This thesis aims to identify the influence of an aged lubricant on the lubrication and friction mechanisms of DLC hard coatings for all lubrication regimes in steady-state and transient conditions. DLC coatings developed during this thesis significantly reduce the boundary friction in steady-state and transient conditions. The lubricant destructuring due to aggregate formation, generated by the passage of soot, or by a temporary vanishing of the entrainment speed, are governed by the triplet, lubricant, surface and contact kinematics. Finally, the analysis of the tribological response of the lubricated interface in steady-state and transient conditions leads to the theoretical modeling of the friction during a complete cycle of sliding at variable velocities.

Les suies se présentent sous la forme de fines particules carbonées de diamètres compris entre quelques dizaines de nanomètres à quelques micromètres. Dans l’atmosphère, elles entraînent des enjeux climatiques, de par leurs propriétés radiatives, mais aussi des enjeux sanitaires, du fait de leur faible taille : elles pénètrent facilement dans le système respiratoire et même, pour les plus fines, dans le système sanguin. L’objectif est de parfaire les connaissances sur les propriétés physiques des suies produites par différents systèmes de combustion. C’est dans le but de mieux comprendre l’influence des systèmes de combustion, faisant intervenir des temps de séjours différents, des propriétés de turbulence, d’oxydation et de pression distinctes que nous avons choisi d’étudier trois types de combustion spécifiques : d’une part, des flammes de diffusion laminaires à pression atmosphérique, initiées dans un brûleur développé au cours de ces travaux ; d’autre part, une flamme de diffusion laminaire sous atmosphère pressurisée (3 à 5 bars) ; enfin, une flamme turbulente produite par une chambre tubulaire, elle aussi sous atmosphère pressurisée (1.2 à 3 bar). Un autre enjeu de ce travail était d’approfondir les informations relatives à la combustion de carburants liquides, à savoir le kérosène et le diester. Les travaux effectués visent à déterminer les caractéristiques morphologiques (dimension fractale, diamètre des monomères...) et l’indice complexe m* des suies issues des différents systèmes de combustion. La technique employée pour la mesure de l’indice complexe de réfraction des suies, repose sur l’analyse d’une partie des fumées produites par les flammes. Ces fumées sont acheminées dans un banc d’analyse permettant la mesure de signaux d’extinction et de diffusion, ainsi que de distributions de taille des suies. Par ailleurs, des analyses de clichés obtenus par microscope en transmission d’électrons (TEM) permettent l’obtention d’informations sur la morphologie des agrégats de suies. L’utilisation de la théorie de la diffusion de la lumière pour des agrégats fractals dans la limite de Rayleigh (RDG-FA) permet d’estimer à partir de ces données deux fonctions de l’indice complexe E(m) et F(m), et ainsi de retrouver m*. / Soot are carbonaceous fine particles, which diameters are ranged from a few nanometres to a few micrometers. They have an impact on climate, due to their radiative properties, as well as on health, due to their small size. That’s why particulate matter is an important concern. In order to gain a better understanding of the influence of the combustion devices, which implies specific residence time and also specific turbulence, oxidation and pressure properties, we studied three specific kinds of combustion : first, laminar diffusion flames at atmospheric pressure ; then, a laminar diffusion flame a high pressures (3 to 5 bar) ; finally, a turbulent flame produced in a combustor at high pressures (1,2 to 3 bar). Another objective of this work was to improve the knowledge about soot produced by the combustion of liquid fuels, namely kerosene and biofuel. We studied morphological properties (fractal dimension, primary particle size…) and the refractive index m* of soot produced by these combustion systems. The technique employed to characterize the soot refractive index is based on the analysis of a part of smokes produced by flames. These are transported towards two optical cells, so that extinction and scattering coefficients can be measured, in addition to soot size distributions. Furthermore, a morphological characterization of the aggregates is conducted, using transmission electron microscopy (TEM) photographs. Rayleigh-Debye-Gans theory for fractal aggregates is used to determine two functions of the refractive index E(m) and F(m), so that m* can be deduced.

Microgravité éthylène laminaires couche limite flammes de diffusion générés par un brûleur poreux plat et caractérisées par les vitesses d'injection de carburant de 3 et 4 mm / s et une vitesse d'oxydation de 250 mm / s ont été simulées en utilisant un modèle de rayonnement précis, un mécanisme cinétique complète et un modèle de suie constitué de lancement par suite de la collision de deux molécules de pyrène, l'évolution de la surface hétérogène et oxydation suivant l'abstraction d'un atome d'hydrogène addition d'acétylène (HACA) mécanisme, la coagulation à particules de suie, et la condensation de la surface de l'HTAP. La distance d'écartement et la production de suie sont améliorées lorsque la vitesse du carburant augmente. H et des radicaux OH, responsables de la de-hydrogénation des sites dans le processus HACA, et le pyrène, de l'espèce pour la création de la suie et des processus de condensation HAP, se trouvent à être situé dans une région qui suit la distance stand-off. La suie est ensuite produite dans cette région et est transporté à l'intérieur de la couche limite par convection et thermophorèse. Perte radiatif est sensiblement plus élevé dans ces flammes que dans flammes de diffusion de gravité normales dues à beaucoup plus longues durées de séjour. Calculs effectués par négliger le rayonnement de la suie et en utilisant l'approximation optiquement mince (OTA) a révélé que la suie domine le transfert de chaleur par rayonnement dans ces flammes et que l'utilisation de l'OTA donne lieu à des écarts significatifs dans la fraction du volume température et la suie. / Microgravity ethylene laminar boundary layer diffusion flames generated by a flat porous burner and characterized by the fuel injection velocities of 3 and 4 mm/s and an oxidizer velocity of 250 mm/s have been simulated by using an accurate radiation model, a comprehensive kinetic mechanism, and a soot model consisting of inception as a result of the collision of two pyrene molecules, heterogeneous surface growth and oxidation following the hydrogen abstraction acetylene addition (HACA) mechanism, soot particle coagulation, and PAH surface condensation. Model predictions are in reasonable agreement with the experimental data in terms of the stand-off distance and soot volume fraction. The stand-off distance and soot production are enhanced as the fuel velocity increases. H and OH radicals, responsible of the de-hydrogenation of sites in the HACA process, and pyrene, of the species for soot inception and PAH condensation processes, are found to be located in a region that follows the stand-off distance. Soot is then produced in this region and is transported inside the boundary layer by convection and thermophoresis. Radiative loss is substantially higher in these flames than in normal gravity diffusion flames owing to much longer residence times. Calculations carried out by neglecting soot radiation and by using the optically-thin approximation (OTA) revealed that soot dominates the radiative heat transfer in these flames and that the use of OTA gives rise to significant discrepancies in temperature and soot volume fraction.

It is estimated that around three billion people globally rely on traditional usage of biomass to cover their daily energy needs, which causes health and social inequality problems and contributes to global warming. Thus, the study of particle emissions from cookstoves provides important information that can help improve global welfare.   This study aims to (a) evaluate a new laboratory setup for measurement of particle emissions from cookstoves and (b) use this setup to compare the particle emissions from three cookstove appliances that cover the whole spectra of used technologies, namely a 3-stone fire, an improved cookstove and a gasifier stove. Emissions of total suspended particles (TSP), fine particles (≤ 2500 nm) and other emission components such as carbon dioxide were measured. Results from this study show that the new laboratory setup is appropriate to measure and investigate fine particle emissions from cookstoves as well as cookstove efficiency. Further, it also shows that the 3-stone fire was the cookstove with the highest emission factor of all, followed by the rocket stove and the gasifier stove respectively. The analysis of the data obtained from the transient particle measurement provided some information on the particle size and the soot and salt contained in the overall emitted particles. Finally, some suggestions such as continuous measurements of background particle and CO2 levels are recommended. Additionally, further research ideas are also proposed.

La réduction des émissions polluantes des foyers aéronautiques est un enjeu majeur pour les motoristes. Afin de les accompagner dans cette tâche, il est nécessaire de développer des outils de simulation numérique permettant de prédire avec précision les émissions d'espèces chimiques en sortie du foyer. Pour cela, une description détaillée des réactions chimiques est nécessaire. Celle-ci est néanmoins incompatible avec la simulation des foyers industriels, compte tenu des puissances de calcul actuelles. C'est pourquoi il est nécessaire de recourir à des méthodes de réduction de la chimie qui préservent la capacité de prédire la concentration des polluants. La démarche consistant à tabuler la chimie nous a semblé appropriée pour aborder ces problèmes et son développement a fait l'objet de cette thèse. Un premier travail a été effectué afin de sélectionner dans la littérature les modèles permettant de traiter des écoulements réactifs turbulents diphasiques avec une approche de chimie tabulée. Par rapport à l’existant, des améliorations ont été apportées à la génération des tables chimiques, afin de prendre en compte l'effet du temps de résidence des gaz brûlés dans le foyer sur la formation des oxydes d'azote. Le couplage de la méthode avec un modèle de formation des suies a également été réalisé. La chimie tabulée permet d’avoir accès à la concentration des précurseurs de suie et des espèces oxydantes, quantités sur lesquelles s’appuie le modèle de formation des suies. Le modèle de chimie tabulée développé dans le cadre de cette thèse a été appliqué à la simulation d'une configuration représentative des foyers aéronautiques. Les concentrations d'oxydes d'azote, de particules de suie, mais aussi de monoxyde de carbone et d'hydrocarbures imbrûlés prédites par les calculs ont été comparées aux résultats expérimentaux. Un bon accord avec l'expérience est observé concernant la topologie du champ de suie et l'allure des profils de concentration de polluants en sortie. Néanmoins, les niveaux de concentration obtenus par les simulations diffèrent des résultats expérimentaux. Cela est imputable notamment à une erreur de prédiction du champ de température qui n'est pas due à l'approche de chimie-tabulée puisque une erreur similaire a été observée avec un autre modèle de combustion. / The reduction of pollutant emissions of aeronautical combustion chambers is a major issue for engine manufacturers. In order to support them in this task, it is necessary to develop numerical simulation tools able to predict accurately chemical species emissions at the chamber outlet. To achieve this, a detailed description of the chemical reactions is necessary. Nevertheless, considering the current computer capabilities, this description is not presently affordable. This is why the use of chemistry reduction methods preserving the capability to predict pollutants species is necessary. The method of tabulated chemistry is a good candidate to tackle these problems and therefore is used as the basis of model developments achieved in the framework of this PhD thesis. A preliminary work has been made to select in the literature tabulated chemistry methods applying to turbulent reactive two-phase flows. The technique to create the chemical tables has been improved in order to take into account the effect of the residence time of the burnt gases on nitrogen oxides formation. The coupling of the method with a soot model has also been achieved. The tabulated chemistry gives access to the concentration of soot precursors and oxidizers, quantities which are required by the model used for the soot prediction. The developed tabulated chemistry model has been applied to the simulation of a configuration representative of aeronautical combustors. The concentration of nitrogen oxides, soot particles, carbon monoxide and unburnt hydrocarbons predicted by the numerical simulations have been compared to experimental results. The topology of the soot volume fraction field and the shape of pollutant concentrations profiles at the outlet agree quite well with the experiments. Nevertheless, concentration levels obtained from the simulations differ from the experimental results. This can be imputed to the error in the prediction of the temperature field that is independent of the combustion model, since a similar error was observed with another combustion model.

Black carbon (BC) is the light-absorbing component of soot, a combustion-generated aerosol that warms the climate by absorbing solar radiation. Its impacts on climate depend on its microphysical properties, which are modified by atmospheric processes including condensation, coagulation and wet removal. State of the art climate models consider soot in a concentric core/shell configuration, with a BC core coated by nonrefractory material such as organics or sulphate. Within this model, thicker coatings enhance visible light absorption, but also wet removal efficiency, and these have opposing effects on the total amount of light absorbed over BC’s lifetime. How well the core/shell model can calculate Mass Absorption Coefficient (MAC, the ratio of absorption to BC mass) is uncertain, as real soot forms more complex (often fractal) shapes, and detailed optical models using these morphologies predict the core/shell model may under- or over-estimate MAC depending on the precise properties of the particles. Few reliable measurements of variations in ambient MAC are available, as most older measurement techniques suffer from systematic uncertainties. In this work, a Single Particle Soot Photometer (SP2) and PhotoAcoustic Soot Spectrometer (PASS) were used to measure BC mass concentration and absorption, and these instruments do not suffer from such uncertainties. The SP2 was also used to report core size and coating thickness distributions that are required to test state of the art climate models. Firstly, a method was developed to minimise bias in the measured coating thicknesses related to the limited detection range of the SP2. The sensitivity of this technique to the assumed density and refractive index of the BC core was also explored, and the most appropriate parameters to use with ambient measurements were determined. Core and shell distributions were measured in Pasadena, California under a range of different photochemical ages. These were then used to calculate MAC, which was compared to that measured using the SP2 and PASS. The measured and modelled MAC agreed within 10% at 532 nm, though this was dependent on the assumed refractive index of the BC core. Overall MAC increased by 15 –25% in around one third of a day of photochemical ageing. This is quite modest compared to some climate models, but not compared to the previous best estimate, which predicted MAC may increase by a factor of ~1.5 over BC’s lifetime. Core and coating distributions were also measured in Canadian boreal biomass burning plumes. A case study was presented comparing the properties of BC in three plumes, one of which had passed through a precipitating cloud. It was demonstrated that larger and more coated BC-containing particles were removed more efficiently, in agreement with previous thermodynamic theory. By calculating MAC using the measured core/shell distributions and comparing to measured scattering, it was demonstrated that the MAC and single-scattering albedo in the plumes were likely not significantly affected by the wet removal, as greater differences were observed between the two plumes not affected by precipitation.

Dans les installations nucléaires, les particules en suspension sont le vecteur d’une grande partie de la contamination radiologique. Pour cette raison, l'IRSN (Institut de Radioprotection et de Sûreté Nucléaire) étudie les filtres THE (Très Haute Efficacité) plissés qui sont l'un des dispositifs permettant assurer la sécurité de l'exploitation nucléaire. Pour éviter les rejets dans l'environnement, la compréhension du comportement des filtres en particulier dans la situation accidentelle doit être aussi exhaustive que possible. L'accident le plus probable et le plus pénalisant pour les dispositifs de confinement est l’incendie qui conduit à une production massive de particules de suie. Dans ce cas, le colmatage des filtres est un problème qui doit être pris en compte. Jusqu'à présent, une corrélation empirique a été développée pour prédire l'augmentation de perte de charge. Toutefois, le caractère empirique de cette corrélation ne permet pas son utilisation dans toutes les situations. Une compréhension phénoménologique et un modèle de colmatage est alors nécessaire. Le travail de thèse qui suit vise à lier l'évolution de la perte de charge à des observations physiques pour chaque étape du colmatage. Pour ce faire, l'étude a été divisée en deux parties. La première se focalise sur le comportement du filtre plan en mesurant la pénétration de particules à l'intérieur du medium et la porosité du dépôt formé sur sa surface. La deuxième partie consiste en une expérience à petite échelle basée sur un seul pli. L'accumulation de particules à l'intérieur du pli a été directement observée, de plus, la déformation du pli ainsi que les écoulements d'air dans le pli (en utilisant une méthode de PIV) ont été mesurés. Au cours de ces expériences, la perte de charge a été mesurée et les paramètres mesurés ont été liés à l'évolution de la perte de charge. La finalité est de construire un modèle analytique simple afin de prédire l'évolution de la perte de charge des filtres en fonction de la masse déposée, des caractéristiques de l'aérosol et des conditions aérauliques. La principale perspective ouverte par ces résultats est la validation des modèles numériques complets pour surmonter les limites expérimentales. Le prolongement logique de ce travail sera l'étude du comportement d'un filtre colmaté soumis à des contraintes de température, d’humidité et aux agressions chimiques de produits de combustion / In nuclear facilities, airborne particles are the vector of most of the radiological contamination. For this reason, pleated HEPA filters are one of the containment devices which are actively studied by the IRSN (Institut de Radioprotection et de Sûreté Nucléaire) to ensure the safety of nuclear exploitation. To avoid contamination of the environment, the understanding of the behavior of the filters especially in accidental situation has to be as exhaustive as possible. The most probable accident and the most penalizing for the containment devices is fire which leads to a massive soot particle production. In this case, the clogging of the filters is a problematic which has to be taken into account. Up to now, an empirical correlation has been developed to predict the pressure drop increase. The empirical nature of this correlation doesn’t allow its use in all situations. A phenomenological understanding and model of the clogging is then necessary. The following PhD work aims to reduce the pressure drop evolution to physical observations for each step of the clogging in order to model it on the most physical basis as possible. To do so, the study has been divided in two parts. The first one focusing on the behavior of flat filter by measuring the penetration of particles inside the medium and the porosity of the deposit formed on its surface. In the second part a small scale experiment based on a single pleat has been developed. Accumulation of the particles inside the pleat has been directly observed, deformation of the pleat as well as airflow in the pleat (using a PIV method) has been measured. During these experiments, pressure drop has been monitored and the measured parameters have been linked to the pressure drop evolution. Finality is to build a simple analytical model to predict the pressure drop evolution of the filters as a function of the deposited mass, the aerosol characteristics and the ventilation conditions. The main perspective opened by these results is the validation of complete numerical models to overcome the experimental limits. The logical extension of this work will be the study of the interaction of a clogged filter with temperature, air moisture and chemical aggression

Les suies de combustion sont principalement connues pour leur caractère nocif, dans le cas des feux de forêt, de fumées de cheminées ou d'émissions polluantes d'un tuyau d'échappement. Cependant, le noir de carbone, un produit industriel de combustion d'hydrocarbures largement utilisé dans notre vie quotidienne. La surface d'une particule de suies ou de noir de carbon joue un rôle important tant au niveau de son utilisation que de son effet nocif. Il est donc important de connaître la masse, le volume ainsi que la morphologie des suies. En particulier, la surface des particules est un paramètre important pour prédire leur utilisation ainsi que leur effet nocif. Les suies sont généralement des agrégats présentant une structure fractale constituée d'éléments de forme sphérique, appelés particules primaires. Il est possible de connaître la surface des agrégats à partir de la distribution en taille de particules primaires (PPSD-Primary particules size distribution). Compte tenu de l'intérêt grandissant pour la surface des particules et leurs évolutions, il est aujourd’hui nécessaire d'étendre les modèles numériques pour la prévision de la PPSD. De plus, comme la taille des la particules primaires influence les processus chimiques et les processus de collision, la prise en compte de ce paramètre peut améliorer les prévisions des modèles. Les flammes multidimensionnelles laminaires, comme les flammes de diffusion, sont moins complexes que les flammes rencontrées dans les systèmes de combustion industriels. Cependant, les processus de formation de suies sont analogues dans les deux cas, ce qui rend l'étude de ces flammes intéressante. Afin d'obtenir une description détaillée des processus chimiques ayant lieu dans ces flammes tout en maintenant le coût de calcul à un niveau abordable, l'utilisation de modèles sectionnels discrets chimiques (CDSchemical discret sectional methods) est un choix approprié. Le développement de modèles CDS est au coeur de cette thèse. D'abord, une stratégie numérique pour déterminer la taille des particules primaires est présentée dans le contexte des modéles CDS. Elle repose sur la résolution d'une équation de transport pour la densité en nombre de particules primaires pour chaque section d'agrégats considérée. Pour valider la taille des particules primaires déterminée numériquement, les résultats doivent être comparés avec des données expérimentales obtenues via la technique d'Incandescence Induite par Laser résolue temporellement (TiRe-LII). Cette comparaison, dite inverse, est affectée par les incertitudes expérimentales et les hypothèses sous-jacentes au post-traitement du signal TiRe-LII pour obtenir la PSD. Pour améliorer la stratégie de validation, une nouvelle approche, dite directe, est proposée pour la validation de la PPSD à partir des données obtenues par TiRe-LII. Elle est basée sur la reconstruction numérique de l'évolution temporelle du signal d'incandescence à partir des résultats numériques et de sa comparaison avec le signal mesuré. L'efficacité de l'approche proposée est démontrée a priori en évaluant l'erreur potentiellement évitée par la nouvelle stratégie. Le modèle proposé pour le suivi des particules primaires est ensuite validé en utilisant à la fois les approches ’directe’ et ’inverse’ sur les flammes cibles issues de l'International Sooting FlameWorkshop (ISF): une flamme pré-mélangée éthylèneair et une flamme de diffusion coflow avec deux dilutions différentes. Le caractère général du modèle est discuté en effectuant une étude de sensibilité des résultats aux paramètres du modèle même. Enfin, le modèle est utilisé pour comprendre l'effet de la dilution du combustible sur la taille des particules primaires dans les flammes de diffusion en examinant les corrélations possibles entre phase gazeuse et phase solide ainsi que l'évolution temporelle des particules le long de leur trajectoires. / An image appearing when the phrase soot is heard is the smoke emitted by an exhaust pipe. The imperfect combustion of hydrocarbon fuels is a source of this harmful pollutant. The industrially controlled combustion of hydrocarbons can provide the carbon black, an industrial product widely used in our everyday life. For both its utilization and its harming effect, the surface of these combustion generated particles plays an important role, therefore, it is of interest to possess information on the particle morphology beside its mass or volume. Soot particles were found, at various conditions, to have a fractal-like structure built up from spherical shape building blocks, socalled primary particles. This increased interest in the particle surface and its evolution gives the motivation to extend numerical models to provide related information, i.e. particle surface or primary particle size. Furthermore, as the primary particle size influences the chemical and collisional processes, accounting for this parameter can improve the model predictions. The requirements for numerical models are various depending on the purpose of the simulation. Multidimensional laminar flames, like a laminar coflow diffusion flame, are less complex than flames of industrial combustion systems. However, the soot formation processes are analogous in the two cases, therefore, the investigation of these flames are of interest. In order to obtain a detailed description of the chemical processes, while keeping the computational cost in these flames at an affordable level, using chemical discrete sectional models is a suitable choice. As in their current version, these models do not provide information on the primary particle size their development in this direction is of interest. Guided by the above motivation, a numerical strategy to determine the primary particle size is presented in the context of the chemical sectional models. The proposed strategy is based on solving the transport equation of the primary particle number density for each considered aggregate section. In order to validate numerical primary particle size, the comparison to experimental data is required. Due to its numerous advantages, the Time-Resolved Laser-Induced Incandescence (TiRe-LII) technique is a nowadays popular experimental method. However, the comparison of the numerically and the experimentally obtained primary particle size may be charged with uncertainties introduced by the additional measurements or assumptions of the numerous parameters required to derive primary particle size from the detected signal. In order to improve the validation strategy, an additional approach for primary particle size distribution validation with TiRe-LII is proposed. This is based on the reconstruction of the temporal evolution of incandescence from the numerical results and its comparison with the measured signal. The effectiveness of this ’forward’ method is demonstrated a priori by quantifying the errors potentially avoided by the new strategy. The validity of the proposed primary particle tracking model is tested by both the traditional ’inverse’ and the ’forward’ method on target flames of the International Sooting Flame (ISF) Workshop. In particular a laminar premixed ethylene flame is considered first. Then, two laminar coflow ethylene flames with different dilutions are put under the scope. The sensitivity to the model parameters, such as accounting for the surface rounding and the choice of smallest aggregating particle size, is explored in both the premixed flame and in the coflow flame with highest ethylene content. To understand the effect of the fuel stream dilution on the primary particle size in the coflow flame, first, the flame-flow interaction and the effect of the dilution on the flame structure is investigated. [...]

The effects of elevated pressure and high heating rates on coal pyrolysis and gasification were investigated. A high-pressure flat-flame burner (HPFFB) was designed and built to conduct these studies. The HPFFB was designed to provide an environment with laminar, dispersed entrained flow, with particle heating rates of ~10^5 K/s, pressures of up to 15 atm, and gas temperatures of up to 2000 K. Residence times were varied from 30 to 700 ms in this study. Pyrolysis experiments were conducted at particle heating rates of ~10^5 K/s and maximum gas temperatures of ~1700 K at pressures of 1 to 15 atm. A new coal swelling correlation was developed that predicts the effects of heating rate, pressure, and coal rank on the swelling ratio at heating rates above ~10^4 K/s. A coal swelling rank index system based on 13C-NMR chemical structural parameters was devised. The empirical swelling model requires user inputs of the coal ultimate and proximate analyses and the use of a transient particle energy balance to predict the maximum particle heating rate. The swelling model was used to explain differences in previously reported bituminous coal swelling ratios that were measured in facilities with different heating rates. Char gasification studies by CO2 were conducted on a subbituminous coal and 4 bituminous coals in the HPFFB. Pressures of 5, 10, and 15 atmospheres were used with gas compositions of 20, 40, and 90 mole % CO2. Gas conditions with peak temperatures of 1700 K to 2000 K were used, which resulted in char particle temperatures of 1000 K to 1800 K. Three gasification models were developed to fit and analyze the gasification data. A simple 1st-order model was used to show that the measured gasification rates were far below the film-diffusion limit. The other two models, designated CCK and CCKN, were based on three versions of the CBK models. CCKN used an nth-order kinetic mechanism and CCK used a semi-global Langmuir-Hinshelwood kinetic mechanism. The two CCK models fit the HPFFB gasification data better than the 1st-order model. The fits of the gasification data with CCK and CCKN were comparable to each other. The fit of the data in CCK suggests that Knudsen diffusion may have influenced the gasification rates in the HPFFB experiments. The gasification rate parameters in each of the three models were correlated with coal rank. 13C-NMR parameters were used to estimate a structural parameter of the coal char. Char-CO2 gasification rate coefficients correlated better with this NMR-based char structure index than it did with the carbon and oxygen content of the parent coal.