Дисертації з теми "Sooty flame"

This study addresses the influence of elevated pressures, fuel type, fuel flow rate and co-flow air on the flame structure and flickering behaviour of laminar oscillating diffusion flames. Photomultipliers, high speed photography and schlieren, accompanied with digital image processing techniques have been used to study the flame dynamics. Furthermore, the effects of pressure on the flame geometry and two-dimensional soot temperature distribution in a laminar stable diffusion flame have been investigated, utilising narrow band photography and two-colour pyrometry technique in the near infra-red region. This study provides a broad dataset on the diffusion (sooty) flame properties under pressures from atmospheric to 16 bar for three gaseous hydrocarbon fuels (methane, ethylene and propane) in a co-flow burner facility.It has been observed that the flame properties are very sensitive to the fuel type and flow rate at elevated pressures. The cross-sectional area of the stable flame shows an average inverse dependence on pressure to the power of n, where n was found to be 0.8±0.2 for ethylene flame, 0.5±0.1 for methane flame and 0.6±0.1 for propane flame. The height of a flame increases firstly with pressure and then decreases with further increase of pressure. It is observed that the region of stable combustion was markedly reduced as pressure was increased. An ethylene flame flickers with at least three dominant modes, each with corresponding harmonics at elevated pressures. In contrast, methane flames flicker with one dominant frequency and as many as six harmonic modes at elevated pressures. The increase in fuel flow rate was observed to increase the magnitude of oscillation. The flickering frequency, however, remains almost constant at each pressure. The dominant flickering frequency of a methane diffusion flame shows a power-law dependence on chamber pressure.It has been observed that the flame dynamics and stability are also strongly affected by the co-flow air velocity. When the co-flow velocity reached a certain value, the buoyancy driven flame oscillation was completely suppressed. The schlieren imaging has revealed that the co-flow of air is able to push the initiation point of outer toroidal vortices beyond the visible flame to create a very stable flame. The oscillation frequency was observed to increase linearly with the air co-flow rate. The soot temperature results obtained by applying the two-colour method in the near infra-red region shows that in diffusion flames the overall temperatures decrease with increasing pressure. It is shown that the rate of temperature drop is greater for a pressure increase at lower pressures in comparison with higher pressures.

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

Thesis (M.S.)--Worcester Polytechnic Institute.
Keywords: soot formation; FDS; flame radiation; soot oxidation; field modeling; diffusion flames; soot. Includes bibliographical references (p. 14-15).

Le rayonnement joue un rôle fondamental dans les problèmes d'incendie puisque c'est le mode dominant de transfert de chaleur entre la flamme et le milieu environnant. Il contrôle la pyrolyse, et donc la puissance de flamme, et la vitesse de croissance de l'incendie. Étudier les flammes de diffusion contrôlées par les forces de flottabilité est une première étape pour comprendre et de prédire les incendies. Le principal objectif de ce travail est de modéliser le transfert radiatif et les processus de production/destruction de la suie dans ce type de flammes. Premièrement, différents modèles de propriétés radiatives des gaz ont été comparés dans des configurations tests. Il est apparu que le modèle FSCK couplé avec le schéma de mélange de Modest et Riazzi est le meilleur compromis entre précision et temps de calcul, ce modèle étant un bon candidat pour être implémenté dans des codes CFD traitant des problèmes d'incendie. Dans un second temps, un modèle de formation/oxydation des suies semi-détaillé, considérant l'acétylène et le benzène comme précurseurs, a été validé dans des flammes de diffusion laminaires de type coflow sur une large gamme d'hydrocarbures (C1-C3) et pour différentes conditions. Ensuite, le FSCK et le modèle de formation/destruction ont été appliqués pour simuler des feux de nappe de méthane et de propane aux échelles du laboratoire et intermédiaire. Les structures de flamme prédites ainsi que les flux radiatif transférés au milieu environnant ont montré un bon accord avec les résultats expérimentaux disponibles. Finalement, les interactions entre le rayonnement et la turbulence ont été quantifiées
The radiative heat transfer plays an important role in fire problems since it is the dominant mode of heat transfer between flames and surroundings. It controls the pyrolysis, and therefore the heat release rate, and the growth rate of the fire. In the present work a numerical study of buoyant diffusion flames is carried out, with the main objective of modelling the thermal radiative transfer and the soot formation/destruction processes. In a first step, different radiative property models were tested in benchmark configurations. It was found that the FSCK coupled with the Modest and Riazzi mixing scheme was the best compromise in terms of accuracy and computational requirements, and was a good candidate to be implemented in CFD codes dealing with fire problems. In a second step, a semi-empirical soot model, considering acetylene and benzene as precursor species for soot nucleation, was validated in laminar coflow diffusion flames over a wide range of hydrocarbons (C1-C3) and conditions. In addition, the optically-thin approximation was found to produce large discrepancies in the upper part of these small laminar flames. Reliable predictions of soot volume fractions require the use of an advanced radiation model. Then the FSCK and the semi-empirical soot model were applied to simulate laboratory-scale and intermediate-scale pool fires of methane and propane. Predicted flame structures as well as the radiant heat flux transferred to the surroundings were found to be in good agreement with the available experimental data. Finally, the interaction between radiation and turbulence was quantified

An experimental study of sooting characteristics of laminar underventillated ethylene non-premixed flames in hot vitiated environments was performed using a modified Wolfhard-Parker co-flowing slot burner. The burner could be operated in "single mode" with a cold air/oxygen mixture as the oxidizer for the non-premixed flame or in varying degrees of "dual mode" where the products of lean premixed hydrogen/air/oxygen flames were used as the oxidizer for the non-premixed flame. Premixed flame stoichiometries of 0.3 and 0.5 were considered for the dual mode cases. Dual mode operation of the burner was intended to simulate the conditions of fuel rich pockets of gas burning in the wake of previously burned fuel/air mixture as typically found in real nonpremixed combustion devices. Dual mode operation introduced competing thermal and chemical effects on soot chemistry. Experimental conditions were chosen to match peak nonpremixed flame temperatures among the cases by varying oxidizer inert (N2) concentration to minimize the dual mode thermal effect. In addition the molecular oxygen (post premixed flame for dual mode cases) and ethylene fuel flow rates were held constant to maintain the same overall equivalence ratio from case to case. Thermocouple thermometry utilizing a rapid insertion technique and radiation corrections yielded the gas temperature field. Soot volume fractions were measured simultaneously with temperature using Thermocouple Particle Densitometry (TPD). Soot volume fraction, particle size and particle number density fields were measured using laser light scattering and extinction. Gas velocities were measured using Particle Imaging Velocimetry (PIV) on the non-premixed flame centerline by seeding the ethylene flow and calculated in the oxidizer flow stream. Porous sinters in the oxidizer slots prevented oxidizer particle seeding required for PIV measurements. In general as the degree of dual mode operation was increased (i.e. increasing stoichiometry of the premixed flames) soot volume fractions decreased, particle sizes increased and soot particle number densities decreased. This trend is suspected to be result of water vapor elevating OH concentrations near the flame front in dual mode operation reducing soot particle nucleation early in the flame by oxidizing soot precursors. The larger particle sizes measured at later stages of dual mode flames are suspected to be the result of lower competition for surface growth species for the lower particle number densities in those flames. Integrated soot volume fraction and particle number fluxes at various heights in the flame decreased with increasing degree of dual mode operation.
Master of Science

Thesis (S.M.)--Massachusetts Institute of Technology, Dept. of Mechanical Engineering, 1999.
Includes bibliographical references (leaves 81-85).
In-flame soot particle size and concentration analysis techniques were developed for high concentrations of ultra-fine soot particles (particle diameters<< 1000 nm) using a Scanning Mobility Particle Sizer (SMPS). The SMPS particle size results were compared to results obtained by thermo phoretic sampling and Transmission Electron Microscopy (TEM). SMPS particle concentration results were compared to mass measurements obtained by filter collection and gravimetric techniques. The SMPS analysis techniques were then used to investigate soot oxidation in fuel rich flames. Soot sampling techniques for polycyclic aromatic hydrocarbon (PAH) analysis were also developed and used to obtain P AH information on soot generated from methane/oxygen premixed flames. The SMPS analysis was performed for SMPS inlet flowrates of 1 lpm and 2 lpm while keeping a constant ratio of inlet to sheath air flowrate of 1 : 10. The 2 lpm flowrate results gave much smaller particle diameters compared to the 1 lpm flowrate results. The shift in particle diameters was around 6 nm. This shift can not be explained by diffusion losses alone because, in some cases, an increase in mean particle diameter is accompanied by an increase in number concentration. The cause of this shift is unknown at this point, but the problem seems to reside in the SMPS instrument itself. The SMPS manufacturer has recently confirmed the shift when sampling polydispersed aerosols. Comparison of the SMPS results with mass measurements is very good for the 1 lpm case, but not for the 2 lpm case. Conversely, comparison of the SMPS results with TEM measurements is very good for the 2 lpm case, but not good for the 1 lpm case. Therefore, the true particle distribution has not been determined conclusively from this analysis. More investigation into the diameter shift phenomenon needs to be done before mass and TEM comparisons can be conclusive. Oxidation was studied in fuel rich ethylene/air/nitrogen flames using a Jet-stirred Reactor/Plugflow Reactor (JSR/PFR) system with oxygen injection at the beginning of the PFR section. An initial amount of oxygen injection was found to increase soot particle size and number concentration most likely due to the increased temperature resulting from the oxygen and combustion products reacting. Further increasing the amount of oxygen injection reduced soot particle number concentration, and eventually decreased the particle mean diameter. P AH analysis of methane/oxygen flame-generated soot revealed that cyclopenta[cd]pyrene, a know mutagen, was the most abundant species aside form pyrene. Cyclopenta[cd]pyrene concentration relative to pyrene increased significantly with soot flame residence time. Other known mutagens were detected in the soot samples including benzo[a]pyrene and some oxy-PAH.
by Stephen William Lasher.
S.M.

Combustion-generated carbon black nano particles, or soot, have both positive and negative effects depending on the application. From a positive point of view, it is used as a reinforcing agent in tires, black pigment in inks, and surface coatings. From a negative point of view, it affects performance and durability of many combustion systems, it is a major contributor of global warming, and it is linked to respiratory illness and cancer. Laser-Induced Incandescence (LII) was used in this study to measure soot volume fractions in four steady and twenty-eight pulsed ethylene diffusion flames burning at atmospheric pressure. A laminar coflow diffusion burner combined with a very-high-speed solenoid valve and control circuit provided unsteady flows by forcing the fuel flow with frequencies between 10 Hz and 200 Hz. Periodic flame oscillations were captured by two-dimensional phase-locked LII images and broadband luminosity images for eight phases (0°- 360°) covering each period. A comparison between the steady and pulsed flames and the effect of the pulsation frequency on soot volume fraction in the flame region and the post flame region are presented. The most significant effect of pulsing frequency was observed at 10 Hz. At this frequency, the flame with the lowest mean flow rate had 1.77 times enhancement in peak soot volume fraction and 1.2 times enhancement in total soot volume fraction; whereas the flame with the highest mean flow rate had no significant change in the peak soot volume fraction and 1.4 times reduction in the total soot volume fraction. A correlation (ƒv Reˉ1 = a+b· Str) for the total soot volume fraction in the flame region for the unsteady laminar ethylene flames was obtained for the pulsation frequency between 10 Hz and 200 Hz, and the Reynolds number between 37 and 55. The soot primary particle size in steady and unsteady flames was measured using the Time-Resolved Laser-Induced Incandescence (TIRE-LII) and the double-exponential fit method. At maximum frequency (200 Hz), the soot particles were smaller in size by 15% compared to the steady case in the flame with the highest mean flow rate.

Le contrôle de la production des particules de suies est aujourd'hui un enjeu industriel majeur en raison de leur impact néfaste tant sur le climat que sur la santé humaine et de leur forte contribution aux transferts radiatifs. Pour mieux comprendre et contrôler la production de ces polluants dans les foyers industriels, il est primordial d’améliorer nos connaissances à ce sujet dans un brûleur turbulent. L’objectif de cette thèse est donc de mettre en place des diagnostics optiques pour l’étude des flammes suitées turbulentes et pour caractérise la production de suies dans une nouvelle configuration de combustion prémélangée,confinée, swirlée turbulente académique tout en se rapprochant des configurations industrielles. Une première configuration expérimentale laminaire est donc considérée afin de valider la mise en place de la technique d’Incandescence Induite par Laser (LII) pour mesurer la fraction volumique de suies fv. Il s’agit d’un brûleur conçu à l’université de Yale qui permet la stabilisation d’une flamme laminaire de diffusion éthylène/air. Ce brûleur a été largement étudié dans la littérature nous permettant ainsi de comparer nos mesures aux résultats de différentes équipes internationales. La calibration du signal LII avec la technique MAE (Modulated Absorption Emission) a été effectuée via une collaboration avec l’UPMC, permettant de mesurer quantitativement fv et de comparer les techniques MAE et LII. Le brûleur a ensuite été équipé d’un haut-parleur afin de moduler l’écoulement et de pouvoir étudier les effets d’une perturbation contrôlée sur la production de suies, se rapprochant ainsi des phénomènes instationnaires caractéristiques des écoulements turbulents. Enfin, les effets d’élargissement de la nappe laser sur les résultats de la LII sont examinés afin de pouvoir appliquer ce diagnostic optique dans une configuration turbulente innovante caractérisée par de grandes dimensions. Ce brûleur (EM2Soot) a été développé pour mesurer la production de suies dans une flamme turbulente swirlée riche confinée prémélangée. Il permet de quantifier indépendamment les effets de la richesse, de la puissance et de l’environnement thermique sur la production de suies. Un point de fonctionnement représentatif a alors été étudié et, en parallèle avec la LII, les techniques de vélocimétrie par images de particules (PIV), et de mesure de température des parois par phosphorescence induite par laser (LIP) ont été employées afin de caractériser l’effet de la turbulence sur la production des suies et d’établir une base de données pour la validation de futures simulations numériques. Enfin, la géométrie du brûleur a été modifiée permettant une stabilisation différente de la flamme (en forme d’un V). Un nouveau point de fonctionnement a alors été étudié afin de mettre en évidence le rôle de la géométrie de l’injecteur sur la stabilisation de la flamme et, par conséquent, la production totale de suies
The control of soot particles production represents today a major industrial issue because of their harmful impact on both the climate and the human health and their strong contribution to the radiative transfers. To better understand and control the production of these polluting emissions, it is essential to improve our knowledge on this subject in a turbulent burner. The objective of this Ph.D. is to set up optical diagnostics for the study of turbulent flames and to experimentally characterize soot production in a new academic turbulent premixed combustion configuration while approaching industrial configurations, generally confined and swirled flows. For this, a laminar experimental configuration is first considered to validate the implementation of the Laser Induced Incandescence (LII) technique to measure the soot volume fraction fv. This burner designed at Yale University allows the stabilization of a laminar ethylene/air diffusion flame. This burner has been widely studied in the literature, so that it is possible to compare the quality of our measurements with the results of different international teams. Through collaborations with the UPMC, we calibrated the LII signal with the MAE (Modulated Absorption Emission) technique, making it possible to quantitatively measure fv and to compare the MAE and LII techniques. Finally, the burner was equipped with a loudspeaker to modulate the flow and to study the effects of a controlled perturbation on the soot production, thus approaching the unsteady phenomena characteristics of turbulent flows. Finally, the effects of the enlargement of the laser sheet on LII results were also investigated in order to be able to apply this diagnostic technique in an innovative large turbulent configuration. This experimental configuration, called EM2Soot, was developed to measure the production of soot in a turbulent swirled rich confined premixed ethylene/air flame. This burner makes it possible to independently quantify the effects of the equivalence ratio, the total flame power and the thermal environment on the total soot production. A representative operating point was then characterized, in parallel with LII measurements, Particle Image Velocimetry (PIV) and Laser Induced Phosphorescence (LIP) techniques have been employed in order to characterize the effect of the turbulence on soot production and to establish a database for the validation of future numerical simulations. Finally, the geometry of the burner has been modified allowing a different stabilization of the flame (V flame shape). A new operating point is then studied in order to highlight the role of the injector geometry on the stabilization of the flame and, consequently, on the total soot production

En las últimas décadas ha avanzado mucho la comprensión científica sobre el proceso de combustión de los chorros diesel de inyección directa gracias al desarrollo de todo tipo de técnicas e instalaciones ópticas. Además, se han desarrollado y mejorado una gran cantidad de modelos de Dinámica de Fluidos Computacional (CFD), los cuales se usan para el desarrollo de motores altamente eficientes y con bajas emisiones. Sin embargo, debido a la complejidad de los procesos físicos y químicos involucrados en este proceso de combustión, así como a las limitaciones significativas de los experimentos, aún hay muchas cuestiones sin responder: ¿Cómo afecta la combustión a la dinámica del chorro? ¿Cómo cuantificar de forma efectiva la cantidad de hollín y la temperatura del mismo en la llama? ¿Cómo afecta el flujo del aire y las inyecciones partidas al desarrollo del chorro y a la formación de hollín en condiciones no quiescente? Para ayudar a resolver las preguntas planteadas, el objetivo de este trabajo se pone en investigar al dinámica del chorro y la formación de hollín de los chorros Diesel de inyección directa en condiciones quiescentes y no quiescentes por medio de diferentes técnicas ópticas. El trabajo se ha dividido en dos bloques principales. El primero está centrado en el estudio de las modificaciones inducidas por la combustión en la dinámica del chorro, así como la caracterización de la formación de hollín en la llama, todo ello en condiciones quiescentes. Dichas condiciones son proporcionadas por una maqueta de flujo continuo a alta presión y temperatura. La expansión radial y axial del chorro reactivo se ha investigado usando n-dodecano, n-heptano y una mezcla binaria de combustibles primarios de referencia (80% n-heptano y 20% iso-octano en masa), basándose en una base de datos existente medida mediante visualización de schlieren. Se ha estudiado tanto el papel de las condiciones de operación como las propiedades del combustible. A continuación se ha desarrollado por primera vez una técnica combinada de extinción-radiación, aplicada a la medida de hollín en llamas diesel. Gracias a esta técnica, tanto la fracción volumétrica de hollín como la temperatura se obtuvieron simultáneamente considerando los efectos de la autoabsorción en la radiación. Todo este trabajo se ha desarrollado dentro del marco de actividades de la Engine Combustion Network (ECN). El segundo bloque corresponde a la caracterización de la dinámica del chorro y de la formación de hollín en condiciones no quiescentes, que ocurren en la cámara de combustión de un motor monocilíndrico de dos tiempos con accesos ópticos. En esta parte, se ha llevado a cabo en primer lugar la visualización del chorro para una inyección única en condiciones no-reactivas y reactivas. Se han aplicado la visualización simultánea de schlieren y de la quimioluminiscencia del radical OH* para obtener la penetración del chorro y la longitud de despegue de la llama, mientras que la visualización de la extinción de ombroscopía difusa (DBI) se ha aplicado para cuantificar la formaciónde hollín. Los resultados se han comparado con los de la base de datos de la Engine Combustion Network antes mencionados, para estudiar los efectos del movimiento del aire inducido por el movimiento del pistón sobre el desarrollo del chorro y del hollín. Finalmente, se han usado diferentes estrategias de inyección partida para estudiar cómo la primera inyección afecta a los procesos de mezcla y a formación de hollín de la segunda, al cambiar el tiempo de separación entre ambos eventos de inyección o la cantidad inyectada en el primer pulso.
In recent decades, the scientific understanding of the combustion process of direct injection diesel spray has progressed a lot, thanks to the development of all kinds of optical facilities and techniques. In addition, a large amount of efficient and accurate Computational Fluid Dynamics (CFD) models, which are used for the design of highly efficient, low emission engines has been developed and improved. However, because of the complexity of the physical and chemical process involved in this combustion process, as well as significant experimental limitations and uncertainties, there are still a lot of remaining questions: How does combustion affect spray dynamics? How can in-flame soot amount and soot temperature be quantified effectively? How do the airflow and split-injection affect spray development and soot formation under non-quiescent conditions? To help solve these raised questions, the objective of this work is set to investigate the spray dynamics and soot formation process of direct injection diesel sprays under both quiescent and non-quiescent conditions by means of different optical techniques. The work has been divided into two main blocks. The first one is focused on the study of combustion-induced modifications in spray dynamics, as well as the characterization of in-flame soot formation under quiescent conditions. The quiescent conditions are provided by a kind of high-temperature high-pressure constant flow vessel. The radial and axial reacting spray expansion were investigated using n-dodecane, n-heptane and one binary blend of Primary Reference Fuels (80% n-heptane and 20% iso-octane in mass) based on an existing database from Schlieren imaging technique. Both operating conditions and fuel properties on this combustion-induced expansion were studied. Next, a combined extinction-radiation technique was first developed and applied in diesel spray soot measurement. Thanks to this technique, both the in-flame soot volume fraction and temperature were obtained simultaneously by considering the self-absorption effect on radiation. All this work has been carried out within the framework of activities of the engine combustion network (ECN). The second block corresponds to the characterization of spray dynamics and soot formation under non-quiescent conditions, which occur within the combustion chamber of a single-cylinder two-stroke optical engine. In this part, the spray visualization for single-injection under both non-reacting and reacting operating conditions was conducted first. Schlieren and OH * chemiluminescence were simultaneously applied to obtain the spray tip penetration and flame lift-off length, while the Diffuse Back Illumination (DBI) extinction imaging was applied to quantify the instantaneous soot formation. Results were compared with Engine Combustion Network database mentioned above to study the airflow effects induced by piston movement on spray and soot development. Finally, different split-injection strategies were used to study how the first injection affects the mixing and soot formation processes of the second one, by changing the dwell time between both injection events or the first injection quantity.
En les últimes dècades ha avançat molt la comprensió científica sobre el procés de combustió dels dolls dièsel d'injecció directa gràcies al desenvolupament de tot tipus de tècniques i instal·lacions òptiques. A més, s'han desenvolupat i millorat una gran quantitat de models de Dinàmica de Fluids Computacional (CFD), els quals s'usen per al desenvolupament de motors altament eficients i amb baixes emissions. No obstant açò, a causa de la complexitat dels processos físics i químics involucrats en aquest procés de combustió, així com de les limitacions significatives dels experiments, encara hi ha moltes qüestions sense respondre: Com afecta la combustió a la dinàmica del doll? Com quantificar de forma efectiva la quantitat de sutge i la temperatura del mateix en la flama? Com afecta el flux de l'aire i les injeccions partides al desenvolupament del doll i a la formació de sutge en condicions no quiescents? Per a ajudar a resoldre les preguntes plantejades, l'objectiu d'aquest treball es posa a investigar al dinàmica del doll i la formació de sutge dels dolls Dièsel d'injecció directa en condicions quiescents i no quiescents per mitjançant diferents tècniques òptiques. El treball s'ha dividit en dos blocs principals. El primer està centrat en l'estudi de les modificacions induïdes per la combustió en la dinàmica del doll, així com la caracterització de la formació de sutge en la flama, tot açò en condicions quiescents. Aquestes condicions són proporcionades per una maqueta de flux continu a alta pressió i temperatura. L'expansió radial i axial del doll reactiu s'ha investigat usant n-dodecà, n-heptà i una mescla binària de combustibles primaris de referència (80% n-heptà i 20% iso-octà en massa), basant-se en una base de dades existent mesura mitjançant visualització de schlieren. S'ha estudiat tant el paper de les condicions d'operació com les propietats del combustible. A continuació s'ha desenvolupat per primera vegada una tècnica combinada d'extinció-radiació, aplicada a la mesura de sutge en flames dièsel. Gràcies a aquesta tècnica, tant la fracció volumètrica de sutge com la temperatura es van obtenir simultàniament considerant els efectes de l'autoabsorció en la radiació. Tot aquest treball s'ha desenvolupat dins del marc d'activitats de la Engine Combustion Network (ECN). El segon bloc correspon a la caracterització de la dinàmica del doll i de la formació de sutge en condicions no quiescents, que ocorren en la cambra de combustió d'un motor monocilíndric de dos temps amb accessos òptics. En aquesta part, s'ha dut a terme en primer lloc la visualització del doll per a una injecció única en condicions no-reactives i reactives. S'han aplicat la visualització simultània de schlieren i de la quimioluminescència del radical OH* per a obtenir la penetració del doll i la longitud d'enlairament de la flama, mentre que la visualització de l'extinció d'ombroscopia difusa (DBI) s'ha aplicat per a quantificar la formaciónde sutge. Els resultats s'han comparat amb els de la base de dades de la Engine Combustion Network abans esmentats, per a estudiar els efectes del moviment de l'aire induït pel moviment del pistó sobre el desenvolupament del doll i del sutge. Finalment, s'han usat diferents estratègies d'injecció partida per a estudiar com la primera injecció afecta als processos de mescla i a formació de sutge de la segona, en canviar el temps de separació entre tots dos esdeveniments d'injecció o la quantitat injectada en el primer pols.
Xuan, T. (2017). Optical investigations on Diesel spray dynamics and in-flame soot formation [Tesis doctoral no publicada]. Universitat Politècnica de València. https://doi.org/10.4995/Thesis/10251/94626
TESIS

Chaque année, une quantité de 107tonnes de suie est produite à l'échelle mondiale. Le carbone-suie dans l'atmosphère a des effets graves sur le changement climatique et la santé humaine. Les impacts dépendent de nombreux facteurs comme les composés organiques adsorbés, le vieillissement et les processus de mélange. Par conséquent, afin de réduire la quantité de suie émise, outre l'examen des facteurs mentionnés, les études de la cinétique de formation, de la structure et des propriétés optiques des suies sont également essentielles. Il existe plusieurs méthodes optiques dans les études sur la suie. La spectroscopie Raman occupe un rôle particulier puisqu'elle est un outil puissant pour l'étude structurale des matériaux carbonés grâce à sa sensibilité aux structures à l’échelle moléculaire. Dans ce travail, des sections Raman différentielles de suies et quelques autres particules carbonées ont été mesurées pour progresser vers la spectroscopie Raman quantitative de ces particules. Les suies produites par des flammes d'éthylène pré-mélangées à basse pression ont été étudiées par mesure Raman ex-situ sur des films déposés et des mesures Raman in-situ (enligne) dans la phase gazeuse. La combinaison de la spectroscopie Raman de suies échantillonnées sur substrat avec les spectroscopies infrarouge et optique et la microscopie électronique en transmission a permis de progresser sur l'interprétation des spectres Raman de suie. Les mesures en phase gazeuse, obtenues pour la première fois, fournissent de nouvelles informations sur la naissance des suies et leurs structures dans les flammes à basse pression avec, par exemple, la détection d'une grande quantité d'atomes de carbones hybridés sp lors de la formation et de la croissance des premières suies. Ces étude s’ouvrent la voie à la détection et à l'analyse des suies directement en phase gazeuse et à leur détection quantitative dans l’atmosphère au travers de leurs spectres Raman
Every year, an amount of 107 tons of soot is produced on the world scale. Soot, as part of atmospheric black carbon, has serious impacts on climate change and human health. The impacts depend on many factors including adsorbed compounds, aging and mixing processes. Therefore in order to reduce the soot amount, besides considering these mentioned factors, the study of formation kinetics, structure and optical properties is also essential. There are several methods applied in soot investigations. Raman spectroscopy plays a particular role as it is a powerful tool for structural investigation of the carbon-based materials because it is sensitive to molecular structures. In this work, differential Raman cross sections of soot and some other carbonaceous particles were measured to progress toward quantitative Raman spectroscopy. Soot particles produced by premixed ethylene flames at a low pressure were investigated by ex-situ Raman measurement on deposited films and in-situ(online) Raman measurement in the gas phase. Combination of the Raman spectroscopy of soot sampled on substrates with infrared and optical spectroscopy and transmission electron microscopy allowed progressing on the interpretation of soot Raman spectra. The online gas phase measurements provided a novel view on soot birth and structures in low pressure flames with, for instance, the detection of a large amount of sp hybrized carbon atoms during nascent soot growth. These studies pave the way to soot detection and analysis directly and quantitatively in the atmosphere

The present work focuses on a computational study of a simplified soot model to predict soot production and destruction in methane/oxidizer (O2 and N2) and ethylene/air flames using a one-dimensional laminar opposed diffusion flame setup. Two different detailed reaction mechanisms (361 reactions and 61 species for methane/oxidizer flame and 527 reactions and 99 species for ethylene/air flame) are used to validate the simplified soot model in each flame. The effects of strain rate and oxygen content on the soot production and destruction are studied, and the soot related properties such as soot volume fraction, particle number density and particle diameter are compared with published results. The results show reasonable agreement with data and that the soot volume fraction decreases with higher strain rate and lower oxygen content. The simplified soot model has also been used with two reduced reaction mechanisms (12-step, 16-species for methane flame and 20-species for ethylene flame) since such reduced mechanisms are computationally more efficient for practical application. The profiles of the physical properties and the major species are in excellent agreement with the results using the detailed reaction mechanisms. However, minor hydrocarbon-species such as acetylene (C2H2) that is the primary pyrolysis species in the simplified soot model is significantly over predicted and this, in turn, results in an over-prediction of soot production. Finally, the reduced reaction mechanism is modified to get more accurate prediction of the minor hydrocarbon-species. The modified reduced reaction mechanism shows that the soot prediction can be improved by improving the predictions of the key minor species.

Le travail présenté dans ce mémoire concerne l'étude, à la fois expérimentale et numérique, des processus de formation et d'oxydation des particules de suie dans des flammes laminaires de diffusion. Les travaux expérimentaux ont été réalisés dans deux flammes de diffusion, éthylène-air et éthylène-oxygène. Afin de mieux appréhender les processus d'oxydation des suies, une analyse plus complète a été menée dans la flamme éthylène-oxygène. Les mesures ont été effectuées au moyen de différentes techniques optiques. La fraction volumique de suie, le diamètre et le nombre de particules ont été déterminés par la méthode extinction-diffusion. Les diamètres ainsi déduits ont été comparés aux valeurs obtenues par P. C. S. (spectroscopie par corrélation de photons). La température a été mesurée par pyrométrie à deux couleurs. La fluorescence induite par laser a été utilisée afin de déterminer la concentration du radical OH, ainsi que le coefficient d'extinction des suies dans l'ultraviolet. L'ensemble de ces résultats a permis une analyse des processus de formation et d'oxydation des suies ainsi que la détermination, dans la flamme suroxygénée, de l'efficacité de collision du radical OH. L'étude numérique a été menée à l'aide d'un code de calcul simulant des flammes de diffusion à contre-courant. Un mécanisme réactionnel détaillé a été utilisé pour prédire la phase gazeuse. Des modèles simplifiés de formation et d'oxydation des suies ont été implantés dans le code. Les modèles d'oxydation étudiés ont permis de mettre en évidence la prédominance du rôle du radical OH sur celui de la molécule d'oxygène lors de l'oxydation des particules de suie.

Ce travail concerne l'étude de la formation des suies dans les flammes d'hydrocarbure et l'influence de la turbulence sur celle-ci. Trois flammes d'éthylène, turbulentes, non prémélangées, de débit massique identique mais de vitesse débitante différente (uo=30 m/s, 6,3 m/s et 0,05 m/s) ont été étudiées expérimentalement. Les champs dynamiques ont été obtenus par anémométrie Doppler laser à deux dimensions. La construction de sondes optiques a permis la mesure instantanée et simultanée de la fraction volumique des suies et de la température. Les valeurs moyennes ont été comparées aux mesures obtenues en utilisant une méthode d'inversion optique et les valeurs fluctuantes aux mesures obtenues en utilisant une technique de corrélations de faisceaux croisés. Tous ces résultats permettent de compléter la bibliothèque de données expérimentales indispensables à la validation des modèles. La finalité de ce travail a été de créer un code de calcul permettant la simulation des flammes de diffusion turbulentes. La comparaison des modèles de formation des suies de Moss et de Lindstedt, insérés dans le code de calcul, montre que le second modèle donne un meilleur accord avec l'expérience lorsque l'on utilise une bibliothèque de relations entre la température d'équilibre et la fraction de mélange (variation de cette relation par rayonnement)

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. [...]

A novel nonintrusive soot diagnostics methodology was developed, validated and applied for in-situ determination of temperature, volume fraction and refractive index of soot aggregates formed inside flames by using near-infrared emission spectrometry. Research was conducted in three main parts, first one addressing development and validation of a comprehensive "
direct"
model for simulation of line-of-sight radiative emission from axisymmetric sooty flames by coupling sub-models for radiative transfer, radiative properties and optical constants. Radiative property estimation for soot agglomerates was investigated by experimentally validating discrete dipole approximation against microwave measurements and using it as reference to assess applicability of simpler Rayleigh-Debye-Gans approximation for fractal aggregates (RDG-FA). Comparisons between predictions of two methods for soot-like model aggregates demonstrated that radiative property predictions of RDG-FA are acceptably accurate for relatively small soot aggregates encountered in small-scale flames. Part two concerns experimental investigation of an axisymmetric ethylene/air diffusion flame by Fourier Transform Near-Infrared spectroscopy. Measurement of line-of-sight emission intensity spectra was performed along with analyses on calibration, noise, uncertainty and reproducibility. A noise characterization approach was introduced to account for spatial fluctuations which were found to dominate over spectral noise. Final part focuses on development, evaluation and application of an inversion methodology that inputs spectral emission intensity measurements from optically thin flames, removes noise, identifies soot refractive index from spectral gradients and retrieves soot temperature and volume fraction fields by tomographic reconstruction. Validation with simulated data and favorable application to measurements indicate that proposed methodology is a promising option for nonintrusive soot diagnostics in flames.

A novel nonintrusive soot diagnostics methodology was developed, validated and applied for in-situ determination of temperature, volume fraction and refractive index of soot aggregates formed inside flames by using near-infrared emission spectrometry. Research was conducted in three main parts, first one addressing development and validation of a comprehensive direct model for simulation of line-of-sight radiative emission from axisymmetric sooty flames by coupling sub-models for radiative transfer, radiative properties and optical constants. Radiative property for soot agglomerates was investigated by experimentally validating DDA method against microwave measurements and using it as a reference to assess applicability of simpler RDG-FA approximation. Part two concerns experimental investigation of an axisymmetric ethylene/air diffusion flame by Fourier Transform Near-Infrared spectroscopy. Measurement of line-of-sight emission intensity spectra was performed along with analyses on calibration, noise, uncertainty and reproducibility. Final part focuses on development, evaluation and application of an inversion methodology that inputs spectral emission intensity measurements from optically thin flames, removes noise, identifies soot refractive index from spectral gradients and retrieves soot temperature and volume fraction fields by tomographic reconstruction. Validation with simulated data and favourable application to measurements indicate that proposed methodology is a promising option for nonintrusive soot diagnostics in flames
Une méthodologie originale de diagnostique des suies a été développée, validée et mise en œuvre pour la détermination in-situ de la température, la fraction volumique et l'indice de réfraction des agrégats de suie formés dans les flammes, en utilisant la spectrométrie d'émission dans le proche infrarouge. Les travaux ont été conduits en trois parties. La première a concerné le développement et la validation d'un modèle direct complet de simulation de l'émission radiative des flammes sur une ligne de visée. Les propriétés radiatives des agrégats de suie ont été étudiées en validant expérimentalement la méthode DDA avec des mesures micro-ondes et en l'utilisant ensuite pour évaluer l'applicabilité de l'approximation RDG-FA. La deuxième partie a impliqué l'analyse expérimentale de l'émission radiative de flammes de diffusion éthylène/air en mettant en œuvre la spectrométrie à Transformée de Fourier dans le Proche Infra-Rouge. La mesure des flux de rayonnement émis sur une ligne de visée a été réalisée en conjonction avec une analyse de l'étalonnage, du bruit, des incertitudes et de la reproductibilité. La dernière partie a consisté en le développement, l'évaluation et l'application d'une méthodologie d'inversion qui a pour données d'entrée les spectres d'émission de flammes optiquement minces, élimine le bruit, identifie l'indice de réfraction des suies à partir des gradients spectraux et fournit la température et la fraction volumique par reconstruction tomographique. La validation avec des données simulées et une application aux spectres mesurés indiquent que la méthodologie proposée est prometteuse pour le diagnostic non intrusif des suies dans les flammes

Soot and radiation play an important role when designing practical combustion devices, and great efforts have been put into developing models which describe soot formation and oxidation. The Eddy Dissipation Concept (EDC) has proven to describe turbulent combustion well, and has the flexibility to describe chemical kinetics in a detailed manner. The aim of this work is to study how the EDC handles soot models based on a detailed representation of the gas-phase chemical kinetics.

Two versions of a semi-empirical soot model is used in conjunction with the EDC. Concentrations of various intermediate species are used as input to the soot models.

The implementation of the new soot models is discussed in relation to the previous implementation of a less detailed soot model. To assure that the interaction between soot and the gas-phase species is represented correctly, the soot models are implemented with a two-way coupling of soot and gas-phase kinetics.

Soot is a good radiator. In a sooting flame a substantial amount of energy will be transferred to the surroundings by thermal radiation. This transfer of energy will alter the temperature field of the flame and the change in temperature will affect the kinetics of soot and gas-phase chemistry. To simulate sooting flames correctly, it was therefore necessary to include a radiation model.

To validate the coupled models of turbulence, combustion, soot, and radiation two different turbulent flames were simulated. One turbulent jet flame of methane and one turbulent jet flame of ethylene. For both flames the computed results were compared with measured values.

Several aspects of the simulations are studied and discussed, such as the effect of the two-way coupling of soot and gas-phase kinetics on both soot yield and gas-phase composition, and the importance of a suitable radiation model.

The two-way coupling of soot and gas phase kinetics is shown to have a positive effect on the computed soot volume fractions, and the results are considered to be encouraging. The work has demonstrated that the EDC has the capacity to handle different types of chemical reaction mechanisms, such as mechanisms for gas-phase combustion and soot kinetics, without modification.

The aim of this study is to advance the present capability for modelling soot production and thermal radiation from turbulent jet diffusion flames. Turbulent methane / air jet diffusion flames at atmospheric and elevated pressure are studied experimentally to provide data for subsequent model development and validation. Methane is only lightly sooting at atmospheric pressure whereas at elevated pressure the soot yield increases greatly. This allows the creation of an optically thick, highly radiating flame within a laboratory scale rig. Essential flame properties needed for model validation are measured at 1 and 3 atm. These are mean mixture fraction, mean temperature, mean soot volume fraction, and mean and instantaneous spectrally resolved radiation intensity. These two flames are modelled using the parabolic CFD code GENMIX. The combustion / turbulence interaction is modelled using the conserved scalar / laminar flamelet approach. The chemistry of methane combustion is modelled using a detailed chemistry laminar flame code. The combustion model accommodates the non-adiabatic nature of the flames through the use of multiple flamelets for each scalar. The flamelets are differentiated by the amount of radiative heat loss that is included. Flamelet selection is carried out through the solution of a balance equation for enthalpy, which includes a source term for the radiative heat loss. A new soot model has been developed and calibrated by application to a laminar flame calculation. Within the turbulent flame calculations the soot production is fully coupled to the radiative loss. This is achieved through the use of multiple flamelets for the soot source terms and the inclusion of the radiative loss from the soot (as well as the gases) in the enthalpy source. Spectral radiative emission from the flames has been modelled using the RADCAL code. Mean flame properties from the GENMIX calculations are used as an input to RADCAL.

O objetivo desta tese é o estudo de formação de fuligem em chamas laminares de difusão. Para o modelo de formação de fuligem é escolhido um modelo semi-empírico de duas equações para prever a fração mássica de fuligem e o número de partículas de fuligem. O modelo descreve os processos de nucleação, de crescimento superficial e de oxidação das partículas. Para o modelo de radiação, a perda de calor por radiação térmica (gás e fuligem) é modelada considerando o modelo de gás cinza no limite de chama opticamente fina (OTA - Optically Thin Approximation). São avaliados diferentes modelos de cálculo das propriedades de transporte (detalhado e simplificado). Em relação à cinética química, tanto modelos detalhados quanto reduzidos são utilizados. No presente estudo, é explorada a técnica automática de redução conhecida como Flamelet Generated Manifold (FGM), sendo que esta técnica é capaz de resolver cinética química detalhada com tempos computacionais reduzidos. Para verificar o modelo de formação de fuligem foram realizados uma variedade de experimentos numéricos, desde chamas laminares unidimensionais adiabáticas de etileno em configuração tipo jatos opostos (counterflow) até chamas laminares bidimensionais com perda de calor de etileno em configuração tipo jato (coflow). Para testar a limitação do modelo os acoplamentos de massa e energia entre a fase sólida e a fase gasosa são investigados e quantificados para as chamas contra-corrente Os resultados mostraram que os termos de radiação da fase gasosa e sólida são os termos de maior importancia para as chamas estudas. Os termos de acoplamento adicionais (massa e propriedade termodinâmicas) são geralmente termos de efeitos de segunda ordem, mas a importância destes termos aumenta conforme a quantidade de fuligem aumenta. Como uma recomendação geral o acoplamento com todos os termos deve ser levado em conta somente quando a fração mássica de fuligem, YS, for igual ou superior a 0.008. Na sequência a formação de fuligem foi estudada em chamas bi-dimensionais de etileno em configuração jato laminar usando cinética química detalhada e explorando os efeitos de diferentes modelos de cálculo de propriedades de transporte. Foi encontrado novamente que os termos de radiação da fase gasosa e sólida são os termos de maior importância e uma primeira aproximação para resolver a chama bidimensional de jato laminar de etileno pode ser feita usando o modelo de transporte simplificado. Finalmente, o modelo de fuligem é implementado com a técnica de redução FGM e diferentes formas de armazenar as informações sobre o modelo de fuligem nas tabelas termoquímicas (manifold) são testadas A melhor opção testada neste trabalho é a de resolver todos os flamelets com as fases sólida e gasosa acopladas e armazenar as taxas de reação da fuligem por área de partícula no manifold. Nas simulações bidimensionais estas taxas são então recuperadas para resolver as equações adicionais de formação de fuligem. Os resultados mostraram uma boa concordância qualitativa entre as predições do FGM e da solução detalhada, mas a grande quantidade de fuligem no sistema ainda introduz alguns desafios para a obtenção de bons resultados quantitativos. Entretanto, este trabalho demonstrou o grande potencial do método FGM em predizer a formação de fuligem em chamas multidimensionais de difusão de etileno em tempos computacionais reduzidos.
The objective of this thesis is to study soot formation in laminar diffusion flames. For soot modeling, a semi-empirical two equation model is chosen for predicting soot mass fraction and number density. The model describes particle nucleation, surface growth and oxidation. For flame radiation, the radiant heat losses (gas and soot) is modelled by using the grey-gas approximation with Optically Thin Approximation (OTA). Different transport models (detailed or simplified) are evaluated. For the chemical kinetics, detailed and reduced approaches are employed. In the present work, the automatic reduction technique known as Flamelet Generated Manifold (FGM) is being explored. This reduction technique is able to deal with detailed kinetic mechanisms with reduced computational times. To assess the soot formation a variety of numerical experiments were done, from one-dimensional ethylene counterflow adiabatic flames to two-dimensional coflow ethylene flames with heat loss. In order to assess modeling limitations the mass and energy coupling between soot solid particles and gas-phase species are investigated and quantified for counterflow flames. It is found that the gas and soot radiation terms are of primary importance for flame simulations. The additional coupling terms (mass and thermodynamic properties) are generally a second order effect, but their importance increase as the soot amount increases As a general recommendation the full coupling should be taken into account only when the soot mass fraction, YS, is equal to or larger than 0.008. Then the simulation of soot is applied to two-dimensional ethylene co-flow flames with detailed chemical kinetics and explores the effect of different transport models on soot predictions. It is found that the gas and soot radiation terms are also of primary importance for flame simulations and that a first attempt to solve the two-dimensional ethylene co-flow flame can be done using a simplified transport model. Finally an implementation of the soot model with the FGM reduction technique is done and different forms for storing soot information in the manifold is explored. The best option tested in this work is to solve all flamelets with soot and gas-phase species in a coupled manner, and to store the soot rates in terms of specific surface area in the manifold. In the two-dimensional simulations, these soot rates are then retrieved to solve the additional equations for soot modeling. The results showed a good qualitative agreement between FGM solution and the detailed solution, but the high amount of soot in the system still imposes some challenges to obtain good quantitative results. Nevertheless, it was demonstrated the great potential of the method for predicting soot formation in multidimensional ethylene diffusion flames with reduced computational time.

Soot volume fraction (f_sv) is measured quantitatively in a laminar diffusion flame at elevated pressures up to 25 atmospheres as a function of fuel type in order to gain a better understanding of the effects of pressure on the soot formation process. Methane and ethylene are used as fuels; methane is chosen since it is the simplest hydrocarbon while ethylene represents a larger hydrocarbon with a higher propensity to soot. Soot continues to be of interest because it is a sensitive indicator of the interactions between combustion chemistry and fluid mechanics and a known pollutant. To examine the effects of increased pressure on soot formation, Laser Induced Incandescence (LII) is used to obtain the desired temporally and spatially resolved, instantaneous f_sv measurements as the pressure is incrementally increased up to 25 atmospheres. The effects of pressure on the physical characteristics of the flame are also observed. A laser light extinction method that accounts for signal trapping and laser attenuation is used for calibration that results in quantitative results. The local peak f_sv is found to scale with pressure as p^1.2 for methane and p^1.7 for ethylene.

L'application de la diffusion quasiélastique de la lumière a permis la caractérisation de particules de suies, générées dans des flammes CH4O2 et C2H6O2. Les hypothèses utilisées pour la modélisation des interactions lumière-particule et particule-écoulement sont mises en évidence

The objective of this thesis is to develop and validate a model of soot formation which is capable of being applied to a computational fluid dynamic (CFD) simulation of gas turbine combustion. The work follows previous research by Moss and Co-workers (Moss et al.1987, Syed 1990, Stewart et al.1991) The concept of the study is to generate a detailed set of experimental data in turbulent flames of kerosine in which the complicating factors of gas turbine combustion - that is 3D geometry and droplet combustion - are removed. This allows more confidence in the computational simulation of the flames and therefore more insight into the soot formation process. There are two components to the work: the experimental and theoretical studies. The first involves the compilation of an experimental dataset of key variables in ethylene and vaporised kerosine jet flames at elevated pressure, the second with the simulation of two of the experimentally studied flames using CFD methods. The main achievement of the study is the generation of a formidable and detailed experimental database for flames at a variety of pressures and conditions. The unexpected finding is the extremely large conversion of carbon to soot found in the flames even at low pressure. This results in high radiant heat losses and measurement difficulties. From the data, it is possible to assess the pressure dependence of soot growth in kerosine flames. Although, at the higher pressures, high soot levels created uncertainties in the measurements, in absolute terms growth rate is shown to be independent of pressure up to 6atm pressure. Above this it increases significantly. The soot model of Moss et al.1988 - originally developed in laminar e~hylene flames - was shown to give excellent agreement in turbulent situations. However, owing to the large radiant heat loss and soot levels, its application to the kerosine flames was more problematic since the assumptions that soot is a perturbation to the gaseous field and that temperature may be accurately described by a single perturbed flamelet were no longer valid. Further models to deal with such situations are proposed and tested. Aside from the obvious relevance of this study to the field of gas turbine combustion, the large radiant heat loss and high soot levels observed in the flames studied here imply a further significance for the study of fire hazards. That a laboratory scale flame maybe made to behave in a similar manner to a much larger pool fire flame is a very useful finding.

The entire world is concerned about running out of petroleum in the future, since 90% of all primary energy currently produced is derived from petroleum. Concern also exists about emissions and their impact on the environment, which are a byproduct of the petroleum combustion process. Renewable biofuels are currently seen as good alternatives, which may address both concerns. One of the most promising biofuels, to be used in the world transportation sector on ground and in air, is farnesane (C15H32). Farnesane is a hydrocarbon produced by adding Hydrogen to farnesene, which is extracted from yeast-fermented sugar cane. Among the air pollutants emitted by any combustion process, particulates are most harmful to the environment. Particulates whose size is lower than 100 nm are known as soot. Soot emission also represents a loss of useful energy, negatively affecting the efficiency of any combustion process. This work provides a comparison of the soot emissions of wick-fed diffusion flames from mixtures, in different proportions (0, 5, 10, 20, 50, 75 and 100%), of aviation kerosine (also known as aviation turbine fuel or simply jet fuel) with farnesane, using Laser Induced Incandescence (LII) technique, to evaluate the effects of farnesane in aviation kerosine combustion. Furthermore, a mapping of Polycyclic Aromatic Hydrocarbons (PAH) formation for each blend is provided, since PAH is considered to be the main soot precursor. The results demonstrate that the maximum concentration of soot is located 11 mm above the burner and that the addition of farnesane to kerosine inhibits PAH formation, which causes soot concentration to decrease. Regarding soot particle diameter, they present low axial variation for fuel blends with low quantities of farnesane. Soot particle size decreases at fuel blends with higher proportions of farnesane, and for all fuel blends the smallest soot particle sizes are observed at 11 mm above burner, which is the same height as the highest soot volume fraction.

Une étude expérimentale a été réalisée avec le but principal de caractériser la production de suie pour différents indices d’oxygène (OI) dans des flammes de diffusion normale (NDF) et inverse (IDF). Pour les IDFs, une augmentation de l’OI augmente la formation de suie mais n’affectent pas les processus d’oxydation, ce qui conduit à une augmentation de la fraction volumique de la suie et de la fraction rayonnée. Une analyse dimensionnelle basée sur le point de fumée (SP) a permis d’unifier les comportements pour les NDFs générées par la combustion de l’éthylène, du propane et du butane en termes de hauteur de flamme, de fraction volumique de suie et de fraction rayonnée au SP. Dans une deuxième étape, une étude numérique a été réalisée avec pour objectif principal d’évaluer les capacités de la méthode sectionnelle (SM) et trois méthodes des moments (MOM) à prédire la structure morphologique des particules de suie. A cette fin, les MOMs ont été implémentées dans un code` parallèle existant pour la simulation des flammes de diffusion laminaires axisymétriques. Les résultats ont montré que la SM est capable de reproduire les données expérimentales disponibles, tandis que les MOMs ne sont pas en mesure de prédire tous les détails de la morphologie des particules de suie avec le même niveau de précision. Une analyse des principales différences entre la SM et les MOM a été réalisée. La principale raison des différences observées entre les MOMs et la SM est liée à l’impossibilité des MOMs à satisfaire l’hypothèse de conservation du nombre densité de particules primaires et du nombre de particules primaires par agrégat pendant les processus de croissance surfacique de la suie
An experimental study was performed with the main objective of characterizing soot production for different oxygen indices (OIs) in normal (NDFs) and inverse (IDFs) diffusion flames. Specific absorption-emission based methods were developed, implemented and validated to measure soot volume fraction and temperature. It was found that for IDFs, an increase on the OI produces an enhancement of soot formation but does not affect oxidation processes, leading to an increase on soot volume fraction and radiant fraction. In addition, a scaling analysis based on the smoke point (SP) resulted on a unified behavior for ethylene, propane and butane fueled NDFs in terms of flame height, soot volume fraction and radiant fraction at SP. In a second step, a numerical study was performed with the main objective of evaluating the predictive capabilities of the sectional method (SM) and three methods of moments (MOMs) for the resolution of the population balance equation (PBE) for soot particle size distribution (PSD). For this purpose, the MOMs were added to an existing parallel code for simulating laminar axisymmetric diffusion flames. The SM was able to reproduce the available experimental data whereas the MOMs were not able to predict details of soot morphology with the same level of accuracy. An analysis on the main differences between the SM and MOMs was performed. The main issue identified for the MOMs was the inability to satisfy the assumption of conservation of number density of primary particles and number of primary particles per aggregate during soot surface processes

Dans la première partie de cette thèse de doctorat une méthodologie est présentée qui permet de prédire les niveaux de suies produits dans des flammes laminaires monodimensionnelles, ou un modèle semi-empirique de suies est utilisé en combinaison avec une chimie complexe et un solveur radiatif détaillé. La méthodologie est appliquée au calcul de suies dans une série de flammes de diffusion à contre-courant d'éthylène/air. Plusieurs modèles d'oxydation de suies sont testés et les constantes du modèle sont ajustées afin de retrouver un meilleur accord avec les expériences. L'effet des pertes thermiques radiatives sur la formation de suies et la structure des flammes est évalué. Finalement, la performance du modèle de suies est évalué sur des flammes prémélangées monodimensionnelles, ou une expression alternative du terme de croissance de surface est proposée pour reproduire les résultats expérimentaux. Dans la deuxième partie de cette thèse, des outils de Simulation aux Grandes Échelles (SGE) et d'analyse acoustique sont appliqués à la prédiction des oscillations de cycle limite (OCL) d'une instabilité thermo-acoustique qui apparaît dans un brûleur académique partiellement prémélangé de méthane/air à pression atmosphérique. La SGE prédit bien l'apparition et le développement des OCL est un bon accord est trouvé entre simulations et expériences en termes d'amplitude et fréquence des OCL. La simulation permet de révéler certains aspects clés responsables du comportement instable de la flamme. Ensuite, une analyse préliminaire de la quantification des incertitudes est fait, ou l'effet des paramètres tels que l'impédance des entrées, le degré de raffinement du maillage ou les pertes thermiques sur les caractéristiques des OCL est évalué. Aussi, la SGE prédit bien la dépendance de la stabilité de la flamme du point d'opération et de la géométrie du brûleur
In the first part of the present PhD. thesis a methodology is presented that allows to predict the soot produced in one-dimensional academic flames, where a semi-empirical soot model is used in combination with a complex chemistry and a detailed radiation solver. The methodology is applied to the computation of soot in a set of ethylene/air counterflow diffusion flames. Several oxidation models are tested and the constants of the model were adjusted to retrieve the experimental results. Also, the effect of radiative losses on soot formation and the flame structure is evaluated. Finally, the performance of the soot model is evaluated on 1D premixed flames, where an alternative expression for the surface growth term is proposed to better reproduce the experimental findings. In the second part of the thesis, Large-Eddy Simulation (LES) and acoustic analysis tools are applied to the prediction of limit cycle oscillations (LCO) of a thermo-acoustic instability appearing in a partially premixed methane/air academic burner operating at atmospheric pressure. The LES captures well the appearance and development of the LCO and a good agreement is found between simulations and experiments in terms of amplitude and frequency of the LCO. Some light is shed on the mechanisms leading to the existence of such instability. Then, a preliminar uncertainty quantification (UQ) analysis is performed, where the effect on the features of the LCO of several computational parameters such as the inlets impedances, mesh refinement or heat losses is assessed. Also, the LES captures well the flame stability behaviour dependence on the operating point and the burner geometry

PONTIFÍCIA UNIVERSIDADE CATÓLICA DO RIO DE JANEIRO
CONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICO
O presente trabalho apresenta um estudo experimental da distribuição da fuligem e de hidrocarbonetos aromáticos policíclicos (PAH) em chamas laminares não pré-misturadas de etileno e ar, mediante o uso de técnicas de diagnóstico espectroscópico, num queimador tipo co-flow. Para este fim são aplicadas as técnicas de fluorescência induzida por plano laser e incandescência induzida por plano laser, com excitação no espectro ultravioleta. Bandas espectrais de detecção centradas em 340, 400, 450, 500, 550 nm são empregadas para caracterizar diferentes PAH, aproveitado o fenômeno do deslocamento do espectros de fluorescência para o infravermelho, conforme se incrementa sua massa molecular. A técnica de extinção laser é utilizada para calibrar os resultados de incandescência e obter a fração volumétrica de fuligem. A radiação espontânea emitida pela fuligem é utilizada para medir a temperatura pela técnica de termometria em duas cores. A comparação dos resultados obtidos com uma detecção simultânea (0 ns) e atrasada (50 ns) com respeito ao pulso laser permite discriminar entre as regiões onde estão presentes PAHs e fuligem ou apenas fuligem. Os resultados mostram que na região mais fria, perto da entrada de combustível, apenas existem PAH. Seguindo esta região, numa zona de altura intermediária e mais quente, tanto a fuligem como o PAHs coexistem até a o ponto de máxima fração volumétrica integrada de fuligem. O deslocamento no sentido vertical da distribuição de fluorescência é observado com o aumento do comprimento de onda de detecção, o que é consistente com o crescimento do tamanho de PAH e sua progressiva transformação em fuligem. A distribuição de PAH e da fuligem é investigada como função da vazão de combustível. A fração volumétrica de fuligem apresenta uma distribuição clássica, cujo valor se incrementa com a vazão de combustível, enquanto que a temperatura medida diminui.
This work presents an experimental study of soot and polycyclic aromatic hydrocarbons (PAH) distribution in axisymmetric ethylene-air non-premixe laminar flames using spectroscopic diagnostic in a co-flow target burner. For this purpose, are applied laser-induced fluorescence and laser-induced incandescence techniques with UV excitation. Spectral detection bands centered at 340, 400, 450, 500, 550 nm are employed to characterize PAH, using the infrared fluorescence spectra displacement phenomenon with the molecular mass increase. The incandescence is captured at 400 nm and the laser extinction technique is used to calibrate the signal, and, thus to obtain the soot volume fraction at the reaction zone. The soot spontaneous emitted radiation is used to measure the temperature by the two-color pyrometry technique. The comparison between results with prompt (0 ns) and delayed (50 ns) detection, with respect to the laser pulse, allows to discriminate the regions between soot precursors (PAH) and soot. The results show that, in the colder region, near the fuel inlet, PAH exist only. Following this region, in an intermediate warmer zone, both soot and PAH appear to coexist until the point of maximum integral soot volumetric fraction. A vertical displacement of the fluorescence distribution with increasing detection wavelength is observed, which is consistent with PAH size growth and with its progressive transformation into soot. PAH and soot distribution are investigated as a function of the fuel flow rate. The soot volumetric fraction exhibits a classical distribution, whose value increases with the fuel flow rate, whereas the measured temperature decreases, exhibiting a singular behavior in the region where the soot is formed.

The concurrent spreading of a boundary layer type diffusion flame is studied. The impossibility of obtaining a low velocity laminar flow without any perturbation induced by buoyancy has lead to the development of an experimental apparatus for use in micro-gravity facilities. Based on previous experimental observations, an original numerical approach has been developed showing, first the dominating role of the radiative heat transfer on the structure of the flame and second the major role of the soot on the extinction phenomenon at the flame trailing edge. The influence of the forced flow velocity, the fuel injection velocity and oxygen concentration on the geometry of the flame has been examined by imaging of CH* and OH* radicals spontaneous emission. Laser-Induced Incandescence (LII) is used to determine the soot field concentration in the flame. The soot formation has been studied by Laser Induced Fluorescence (LIF) of Polycyclic Aromatic Hydrocarbons (PAHs). The interaction between the reaction zone and the field of soot formation/oxidation is taken into account to analyze the flame length. These results can be used as the experimental input data for a future complete validation of numerical model simulating the soot formation and oxidation in this kind of flame.

The mechanisms governing the formation and destruction of soot in turbulent combustion are intimately coupled to thermal radiation due to the strong dependence of sooting processes and radiative loss on temperature. Detailed computational fluid dynamics (CFD) predictions of the radiative and soot output from turbulent non-premixed flames are normally performed by parabolic algorithms. However, the modelling of combustion systems, such as furnaces and unwanted enclosure fires, often require a fully elliptic description of the flow field and its related physical phenomena. Thus, this thesis investigates the intimate coupling between radiative energy exchange and the mechanisms governing soot formation and destruction within a three-dimensional, general curvilinear CFD code. Thermal radiation is modelled by the discrete transfer radiation model (DTRM). Special emphasis is given to approximate solutions to the radiative transfer equation encompassing various models for the radiative properties of gases and soot. A new algorithm is presented, entitled the differential total absorptivity (DTA) solution, which, unlike alternative solutions, incorporates the source temperature dependence of absorption. Additionally, a weighted sum of gray gases (WSGG) solution is described which includes the treatment of gray boundaries. Whilst the DTA solution is particularly recommended for systems comprising large temperature differences, the WSGG solution is deemed most appropriate for numerical simulation of lower temperature diffusion flames, due to its significant time advantage. The coupling between radiative loss and soot concentration is investigated via a multiple laminar flamelet concept applied within the CFD simulation of confined turbulent diffusion flames burning methane in air at 1 and 3 atm. Flamelet families are employed relating individual sooting mechanisms to the level of radiative loss, which is evaluated by the DTRM formulated for emitting-absorbing mixtures of soot, C02 and H20. Combustion heat release is described by an eddy break-up concept linked to the k-c turbulence model, whilst temperature is evaluated from the solved enthalpy field. Detailed comparisons between prediction and experiment for the critical properties of mixture fraction, temperature and soot volume fraction demonstrate the effectiveness of this novel, coupled strategy within an elliptic flow field calculation.

In this thesis, a discretised Population Balance Equation (PBE) model is coupled with a detailed in-house Computational Fluid Dynamics code to study soot formation in axisymmetric diffusion flames with comprehensive gas-phase chemistries for C2H4 and CH4 fuels. The main aim of this study is to predict the complete Particle Size Distribution (PSD) of soot particles in turbulent non-premixed flames via a transported Probability Density Function approach. The PSD is obtained from the solution of the PBE without any prior assumption on its shape, using volume or diameter to describe the size of soot particles. However, due to a great number of uncertainties that appear from the turbulence interactions with chemistry, radiation and particle formation, the main objective is divided into smaller tasks where these complexities are avoided. Initially, the performance of the PBE is assessed under several numerical methods on an initial distribution-convection test, 0D reactors and 1D flamelet framework. The PBE has been originally discretised via a collocation type finite element method, and in the present work Finite Volume (FV) methods are used. The PBE with Total Variation Diminishing (TVD) scheme demonstrates better performance. The FV-TVD PBE with suitable soot kinetics is employed in 2D laminar flames where overall good agreement is achieved for the velocity, temperature, mole fraction of C2H2 and OH species and the mean properties of PSD (i.e. total number density and soot volume fraction). However, the temperature and soot volume fraction profiles on the turbulent flames do not exhibit similar accuracy as the laminar flames and there is still room for improvement. The evolution of the PSD is computed for both flames in the entire flame region exhibiting weak bimodal distribution in some points. The performance of complex coupled phenomena in PBE modelling via soot kinetics, detailed chemistry, radiation and turbulence interactions is explored.

Soot particles formed and emitted from (e.g.) direct-injected diesel engines are dangerous to human health and legislative measures used to reduce emis- sions pose a technical challenge for manufacturers. Models of soot formation and oxidation may therefore be useful tools for developing engines and con- trol strategies. In the present work, a sectional soot model able to reproduce the soot particle size distribution (PSD) is applied to laminar premixed and diffusion flames as well as a reactor system. The soot PSDs in laminar premixed stagnation flow flames were found to be sensitive to the coagula- tion collision efficiency and a novel model was developed. The soot model under-predicted soot volume fraction levels when applied to a set of laminar ethylene and propane counter-flow diffusion flames and a sensitivity anal- ysis suggested further assessment of the formation of poly-cyclic aromatic hydrocarbons (PAH) was needed. The chemical reaction mechanism was subsequently assessed using species measurements from a laminar premixed benzene flame and selected parts of the reaction mechanism reviewed. Rea- sonable agreement was obtained, including for formation of PAHs. However, non-existing or insufficient oxidation paths of some PAH species, including pyrene, may contribute to over-predictions by the soot model during non- sooting conditions. Formation of PAHs in a laminar ethylene counter-flow diffusion flame was investigated next. The agreement between calculations and measurements was found to be reasonable for major, minor and single ring aromatic species. However, the calculated concentrations of all PAH species are under-predicted. The under-prediction of pyrene is comparable to the under-prediction of the soot volume fraction in some of the diffusion flames previously investigated, making the uncertainty of the PAH chem- istry a possible explanation. Future soot modelling research should therefore focus on investigating the PAH chemistry for different types of flames and fuels.

Cette thèse consiste en l'étude expérimentale et numérique des processus de formation des particules de suie au sein des flammes laminaires non-pré-mélangées et partiellement prémélangées sous l'influence d'un champ magnétique ou d'une stimulation acoustique. Dans une premiére étape, la capacité du code CIAO à prédire la fraction volumique de suie dans une flamme axisymétrique est étudiée. Par la suite, deux flammes subissant une stimulation acoustique ont été étudiées. Les résultats peuvent être utilisés pour améliorer les modèles de suie futurs, en particulier concernant les différentes échelles temporelles de la chimie en phase gazeuse, et la formation d'hydrocarbures polyaromatiques (PAH) et de suie couplée avec des flux transitoires. Pour étudier la formation des particules de suie sous l'influence de gradients de champ magnétique, un brûleur de type Santoro est utilisé. Les techniques de mesure utilisées dans le cadre de cette thèse sont l'imagerie directe à haute cadence, la technique Background Oriented Schlieren (BOS) et la méthode d'Absorption/Emission Modulée (MAE). Une augmentation de la fraction volumique de suie intégrée a été mise en évidence lorsque le gradient de champ magnétique est ascendant. Une analyse de stabilité linéaire locale appliquée à l'écoulement non-visqueux est présentée pour une flamme sous l'influence de la perturbation magnétique envisagée. Le gradient de champ magnétique provoque alors une réduction du taux d'amplification. De fait, l'étude est complété par l'identification d'un domaine où les flammes qui oscillent naturellement peuvent être stabilisées et contrôlées par des gradients de champ magnétique
In this thesis light is shed on the soot formation processes in laminar coflow flames influenced by magnetic field gradients and acoustic forcing. Both influences have been assessed experimentally and numerically. First, the CIAO in-house code's ability to predict soot volume fraction fields in a steady coflow flame is studied. Then, two acoustically forced cases were studied. These findings are used to improve future soot models, especially, concerning the different time scales of gas phase chemistry and the formation of polycyclic aromatic hydrocarbons (PAH) and soot coupled with unsteady flows. To investigate soot formation under magnetic field gradients, a Santoro type burner is used. The measurement techniques applied in the course of this thesis are high-speed luminosity measurements, Background Oriented Schlieren (BOS) and one- and two-color Modulated Absorption/Emission (MAE) techniques. The magnetic field impact on soot formation was first studied experimentally in steady laminar flames. A scaling of soot production similar to the increased integrated soot volume fraction with increased oxygen content in the coflow was documented. A local inviscid stability analysis is presented for an ethylene coflow flame to investigate the flame's response to small perturbations of the mean velocity, temperature, fuel, and oxygen massfraction under magnetic field exposure. The magnetic field is found to reduce the perturbations' growth rate. The magnetic field study is completed by identifying a domain where naturally oscillating flames can be stabilized and controlled by magnetic field gradients

Les suies et les hydrocarbures polyaromatiques, qui sont émis à l’échappement des moteurs Diesel, constituent une part importante de la pollution urbaine. Depuis plusieurs années, de nombreuses recherches ont permis de progresser dans le domaine de la cinétique de la combustion des hydrocarbures qui est maintenant relativement bien connue. Il reste néanmoins des zones d’ombre concernant la formation des composés aromatiques (benzène, toluène,…) et des hydrocarbures aromatiques polycycliques (HAP) dont la formation provient d’espèces composées de deux à six atomes de carbone et qui mènent directement ou indirectement à la formation des suies.L’allène, le propyne, le butadiène et le cyclopentène sont des produits intermédiaires importants de la combustion dans les moteurs. Dans ce contexte, ce travail de thèse a permis de mieux comprendre les voies réactionnelles importantes dans la formation du benzène et du toluène. Le chapitre I de ce mémoire présente une revue bibliographique des travaux antérieurs sur l’oxydation du méthane, de l’allène, de propyne, de 1,3-butadiène et du cyclopentène. Le chapitre II présente une description détaillée du montage expérimental utilisé durant cette étude afin d’étudier la structure de la flamme laminaire de prémélange. Les chapitres III, IV et V présentent les résultats expérimentaux obtenus en flamme laminaire de prémélange, ainsi qu’une comparaison avec des simulations effectuées à l’aide de mécanismes réactionnels élaborés durant ce travail de thèse
Soots and polyaromatic hydrocarbons (PAH), which are present in the exhaust gas of diesel engines, represent a large part of the urban pollution. Many efforts have then been focused on reducing the emissions of these compounds. The formation of soot precursors and PAH in combustion involves small unsaturadted hydrocarbons the chemistry of which is still very uncertain. Allene, propyne, 1,3-butadiene and cyclopentene are intermediate products in the combustion in cars engines. This work has led to a better understanding of several important paths in the formation of benzene and toluene. The chapter I of this report presents a bibliographic review of former work on the oxidation of methane, allene, propyne, 1,3-butadiene and cyclopentene. Chapter II gives a detailed description of the experimental set up used during this work to study the structure of the premixed flat laminar flames. Chapters III, IV and V present our experimental results obtained in laminar premixed flat flames and also the comparison with simulations

La propagation d’un incendie dans un espace clos s’explique par l’inflammation de matières combustibles. Un cas important est celui de la propagation d’une flamme sur une paroi verticale. En effet si la flamme progresse dans le même sens que l’écoulement (cas co-courant), la croissance est rapide. Dans ce cas, l’émission des vapeurs combustibles (pyrolyse) et le dégagement de la chaleur apportée par la combustion sont couplés par les flux convectés et rayonnés à la paroi. Ces flammes de paroi verticale sont pilotées par les forces de flottabilité, et se caractérisent par un régime de basse vitesse et avec une forte production de suie. Bien que de nombreux travaux aient été consacrés à l’étude des flammes de paroi verticale [1-3], peu d’entre eux ont été dédiés à l’étude de l’écoulement dans la couche limite proche de la paroi et à l’étude des zones de production de suie, lesquels sont des données nécessaires pour la validation des codes de calcul. Pour cela, des mesures simultanées de vitesse par PIV et de concentration de suie par LII ont été réalisées sur un brûleur gaz en configuration paroi-verticale. Dans un premier temps, ces mesures ont permis l’analyse de la forme, de la taille et de la concentration des zones de formation de suies (poches de suie) à différentes hauteurs dans la flamme. Ensuite, les champs 2D de vitesses moyennes (horizontales et verticales) ont été étudiés, ainsi que leurs fluctuations (densités de probabilité et écart-type). Une description de la couche limite réactive, à l’aide d’une échelle caractéristique obtenue avec des mesures de vitesse plus résolues spatialement (PIV « zoomé »), a également été réalisée. Finalement, les mesures de LII et PIV couplées ont permis d’étudier l’influence du champ de vitesse sur la distribution des suies dans la flamme, ainsi que le transport et le flux turbulent de la fraction volumique de suie dans la couche limite réactive
The fire growth and spread on a confined space depends on the inflammation and combustion of combustible materials. An important case is the fire propagation on a vertical wall configuration, in which the pyrolysis gas and the total heat flux released by the flame are coupled by convective and radiative heat flux from the flame to the wall. This kind of flame is piloted by the buoyancy forces, and is characterized by a low velocity regime and a strong generation of soot particles. Although numerous works have been devoted on the study of vertical wall flames, few have been carried out on the analysis of the flame within the reactive boundary layer and the study of the zones of production of soot particles, which is data necessary for fire simulation codes validation. In this aim, simultaneous measurements of velocity by Particle Image Velocity (PIV) and of soot volume fraction by planar laser induced incandescence (LII) have been carried out on vertical wall fire generated by a vertical porous burner fed with a CH4/C2H4 mixture. First, the characteristics of soot sheet (shape, size, thickness, and peak concentration) have been studied at different heights into the flame, as well as the average and RMS soot volume fraction fields. Then, average and RMS fields of velocity and their probability density function have been analyzed. A description of the reactive boundary layer, through the definition of a characteristic velocity scale in the near-wall zone (viscous sub-layer), has been carried out by using a « PIV Zoom » set-up. Finally, simultaneous LII/PIV measurements have been carried out in order to study the influence of the aerodynamics of the flow on the soot volume fraction distribution, as well as the transport and turbulent flux of soot into the reactive boundary layer