Depuis plusieurs années, les constructeurs automobiles suivent la voie du « downsizing » pour le développement des moteurs à allumage commandé. Ce procédé basé sur la réduction des cylindrées moteur combinée à la suralimentation a déjà fait ses preuves quant à son intérêt dans l’augmentation du rendement et la réduction des émissions polluantes des moteurs à essence. Les nouvelles conditions thermodynamiques, de turbulence et de dilution de ces moteurs engendrant de nouvelles possibilités de dilution dans les mélanges air/carburant, elles amènent également de nouvelles problématiques quant aux combustions anormales observées et l’apparition d’importantes variabilités cycliques. Ces travaux de thèse s’insèrent dans l’objectif de compréhension du comportement des flammes de prémélange d’isooctane/air en expansion dans des conditions représentatives d’un moteur « downsizé ». Leur étude a dans un premier temps été réalisée dans des conditions laminaires afin d’extraire les vitesses de flammes et longueurs de Markstein associées aux différents mélanges réactifs, et notamment sous forte dilution. Des corrélations ont alors été développées pour répondre aux besoins des modèles de simulation. Un nouveau dispositif de diagnostic optique a ensuite été employé pour améliorer la visualisation des flammes turbulentes en expansion. Une corrélation de coefficient correctif est ici développée pour remédier à la surestimation de vitesse engendrée par une visualisation Schlieren de ces flammes turbulentes. Une étude approfondie de l’influence des conditions thermodynamiques initiales, de la turbulence, ainsi que des caractéristiques diffusives du mélange air/carburant a par ailleurs été conduite afin d’isoler l’effet de chacun de ces paramètres sur le développement et la propagation de la flamme turbulente. Enfin l’effet d’une évolution simultanée des conditions thermodynamiques initiales similaire à celle d’une compression moteur a été étudié pour mieux appréhender les changements de comportement des flammes turbulentes dans des conditions plus représentatives du moteur à allumage commandé. / For several years, “downsizing” is used by car manufacturers to develop new spark ignition engines. This method based on the reduction of engine size combined with an increase of intake pressure (turbocharger) is well known to reduce pollutant emissions and increase efficiency. New thermodynamic, turbulent and dilution conditions could be used with these new engines but they can bring new issues like unusual combustion or cyclic variability. This thesis took place to improve the understanding of premixed expanding isooctane/air flames behavior under downsized engine-like conditions. As a first step, this work is conducted under laminar conditions to extract laminar burning velocities and Markstein lengths of the different mixtures, especially under high dilution. New correlations are then developed to answer the needs of numerical models. A new optical dispositive is then used to improve the visualization of turbulent expanding flames. A corrective coefficient correlation is proposed to avoid the overestimated values of turbulent burning speed generated by Schlieren visualization with such turbulent flames. A deep survey of starting conditions (temperature, pressure, turbulence, dissipative characteristics of air/fuel mixtures) influence is done to investigate the effect of each parameters on the development and the propagation of the turbulent flame. Finally, the effect of a coupled rise of initial temperature and pressure, similar to an engine compression, is studied to better understand the changes of flame behavior under more realistic spark-ignition engine conditions.

The arising environmental concerns make emission reduction from combustion devices one of the greatest challenges of the century. Modern dry low-NOx emission combustion systems often operate under lean premixed turbulent conditions. In order to design and operate these systems efficiently, it is necessary to have a thorough understanding of combustion process in these devices. In premixed combustion, flame speed determines the conversion rate of fuel. The flame speed under highly turbulent conditions is defined as turbulent flame speed. Turbulent flame speed depends on laminar flame speed, which is a property of the combustible mixture. The goal of this thesis is to estimate laminar flame speed and NOx emissions under certain conditions for specific industrial gas turbines. For this purpose, an in-house one-dimensional code, GENE-AC, is used. At first, a data validation is performed in order to select an optimized chemical reaction mechanism which can be used safely with the fuels of interest in gas turbines. Results show that GRI-Mech 3.0 performs well in most cases. This mechanism is selected for further simulations. Secondly, laminar flame speed is calculated using GRI-Mech 3.0 at SGT-800 conditions. Results show that at gas turbine conditions, increasing ambient temperature and fuel to air ratio enhances flame speed, mainly due to faster reaction rates. Moreover, laminar flame speed is highly affected by fuel composition. In particular, adding hydrogen to a fuel changes chemical processes significantly, because hydrogen is relatively light and highly diffusive. Calculations are conducted over a range of equivalence ratios and hydrogen fractions in methane at atmospheric as well as gas turbine operating conditions. Results reveal some trends for changes in laminar flame speed, depending on hydrogen content in the mixture. The final part of the thesis involves the development of a reactor network model for the SGT-700 combustor in order to predict NOx emissions. The network model is built in GENE-AC based on results from available computational fluid dynamics (CFD) simulations of the combustor. The model is developed for full load conditions with variable pilot fuel ratios. The NOx emissions are predicted using GRI-Mech 3.0 mechanism. A parametric study shows the dependency of NOx emissions on equivalence ratio and residence time. For SGT-700 running on natural gas, NOx emissions are fitted to measurement data by tuning equivalence ratio and residence time. The model is then tested for a range of ambient temperatures and fuel compositions. It is found that, although the model can correctly predict the trends of ambient temperature and fuel effects on NOx emissions, these effects are to some extent over-estimated. Using future engine tests and amending calibration can improve the results.

La vitesse de flamme adiabatique est un paramètre clé dans l'étude de la combustion d'hydrocarbures. Elle joue en effet un rôle essentiel dans le domaine de la combustion, dans la mesure où elle est utilisée pour valider des modèles numériques, pour construire des brûleurs, ou encore pour prédire d'éventuels retours de flamme ou souffles de la flamme. Le but de cette thèse a été d'étudier les vitesses de flammes laminaires d'un grand nombre d'hydrocarbures présents dans les gaz naturels, les essences et les gazoles. Ce travail comprend une partie expérimentale et une partie de modélisation. La partie expérimentale a permis d'enrichir les bases de données de la littérature pour différentes compositions de mélanges air/hydrocarbures. Les travaux ont été effectués sur un nouveau montage mis au point au LRGP (Laboratoire Réactions et Génie des Procédés) pour la mesure de vitesses de flammes laminaires par la méthode du flux de chaleur à l'aide d'un brûleur adiabatique à flamme plate. Cette méthode est basée sur l'équilibre des pertes thermiques nécessaires pour stabiliser la flamme par le flux de chaleur convectif allant de la surface du brûleur vers le front de flamme. Le brûleur est constitué d'une plaque perforée montée sur une chambre de mélange des gaz et la mesure de la distribution radiale de la température est réalisée grâce à une série de thermocouples. Ce montage a d'abord été utilisé à pression atmosphérique et plusieurs températures pour la mesure de vitesses de flammes de composés gazeux (alcanes, alcènes, méthane enrichi en hydrogène ou oxygène, gaz naturels, mélanges méthane-éthane et méthane-propane) et de composés liquides (alcanes, éthanol, essences commerciale et modèle additionnées ou non d'éthanol, alkylcyclohexanes, alkylbenzènes). Le montage a ensuite été placé dans une enceinte pour pouvoir travailler avec des pressions pouvant théoriquement aller jusqu'à 10 atm. Les vitesses de flammes de deux composés ont été étudiées à température ambiante et à haute pression : un composé gazeux, le méthane, jusqu'à une pression de 6 atm et un composé liquide, le n-pentane, jusqu'à une pression de 4 atm. Une étude de modélisation a complété ce travail par l'utilisation de modèles cinétiques détaillés pour la combustion des composés étudiés. Ces modèles ont été testés par la simulation des résultats expérimentaux précédemment obtenus, dans des conditions de richesse, température et pression variées / The laminar burning velocity is a key parameter in the combustion of hydrocarbons study. It plays an essential role in the combustion science area since it is used for the validation of numerical models, the design of burners or to predict potential flashback or blow off of the flame. The goal of the thesis was the study of laminar burning velocities of many hydrocarbons found in natural gases, gasolines or diesel fuels. This work includes an experimental part and a modeling part. The experimental part allowed the implementation of the literature database for different air/hydrocarbons mixtures. The experiments were performed with a new apparatus developed at LRGP (Laboratoire Réactions et Génie des Procédés) for the measurement of laminar burning velocities by the heat flux method thanks to a flat flame adiabatic burner. This method is based on balancing of the heat loss required for the flame stabilization by the convective heat flux from the burner surface to the flame front. The burner head is a thick perforated plate included in a plenum mixing chamber and the measurement of the radial distribution of the temperature is performed with a thermocouples series. This apparatus was first used at atmospheric pressure and several temperatures to measure laminar burning velocities of gaseous compounds (alkanes, alkenes, hydrogen-enriched or oxygen-enriched methane, natural gases, methane-ethane and methane-propane mixtures) and liquid compounds (alkanes, ethanol, commercial gasoline and model fuel with addition of ethanol or not, alkylcyclohexanes, alkylbenzènes). The apparatus was then placed in a chamber in order to work under pressures theoretically up to 10 atm. Laminar burning velocities of two compounds were studied at room temperature and high pressure : a gaseous compound, methane, for pressures up to 6 atm and a liquid compound, n-pentane, for pressures up to 4 atm. A modelling study completed this work by using detailed kinetic models for the combustion of studied compounds. These models were tested by the simulation of experimental results previously obtained, in various equivalence ratio, temperature and pressure conditions

Iso-octane, n-heptane, ethanol and their blends were tested in a constant volume combustion chamber to measure laminar burning velocities. The experimental apparatus was modified from the previous version to an automatically-controlled system. Accuracy and speed of data acquisition were improved by this modification. The laminar burning velocity analysis code was also improved for minimized error and fast calculation. A large database of laminar burning velocities at elevated temperatures and pressures was established using this improved experimental apparatus and analysis code. From this large database of laminar burning velocities, laminar flame speeds were extracted. Laminar flame speeds of iso-octane, n-heptane and blends were investigated and analysed to derive new correlations to predict laminar flame speeds of any blending ratio. Ethanol and ethanol blends with iso-octane and/or n-heptane were also examined to see the role of ethanol in the blends. Generally, the results for iso-octane and n-heptane agree with published data. Additionally, blends of iso-octane and n-heptane exhibited flame speeds that followed linear blending relationships. A new flame speed model was successfully applied to these fuels. Ethanol and ethanol blends with iso-octane and/or n-heptane exhibited a strongly non-linear blending relationship and the new flame speed model was not applied to these fuels. It was shown that the addition of ethanol into iso-octane and/or n-heptane accelerated the flame speeds. / text

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The work presented in this thesis was undertaken as part of the safety work package of the NATURALHY project which was an integrated project funded by the European Commission (EC) within the sixth framework programme. The purpose of the NATURALHY project was to investigate the feasibility of using existing natural gas infrastructure to assist a transition to a hydrogen based economy by transporting hydrogen from its place of production to its place of use as a mixture of natural gas and hydrogen. The hydrogen can then be extracted from the mixture for use in fuel cells or the mixture used directly in conventional combustion devices. The research presented in this thesis focused on predicting the consequences of explosions and fires involving natural gas and hydrogen mixtures, using engineering type mathematical models typical of those used by the gas industry for risk assessment purposes. The first part of the thesis concentrated on modifying existing models that had been developed to predict confined vented and unconfined vapour cloud explosions involving natural gas. Three geometries were studied: a confined vented enclosure, an unconfined cubical region of congestion and an unconfined high aspect ratio region of congestion. The modifications made to the models were aimed at accounting for the different characteristics of a natural gas/hydrogen mixture compared to natural gas. Experimental data for the laminar burning velocity of methane/hydrogen mixtures was obtained within the safety work package. For practical reasons, this experimental work was carried at an elevated temperature. Predictions from kinetic modelling were employed to convert this information for use in models predicting explosions at ambient temperature. For confined vented explosions a model developed by Shell (SCOPE) was used and modified by adding new laminar burning velocity and Markstein number data relevant to the gas compositions studied. For vapour cloud explosions in a cubical region of congestion, two models were used. The first model was developed by Shell (CAM2), and was applied using the new laminar burning velocity and other composition specific properties. The second model was based on a model provided by GL Services and was modified by generalising the flame speed model so that any natural gas/hydrogen mixture could be simulated. For vapour cloud explosions in an unconfined high aspect ratio region of congestion, a model from GL Services was used. Modifications were made to the modelling of flame speed so that it could be applied to different fuel compositions, equivalence ratios and the initial flame speed entering the congested region. Predictions from the modified explosion models were compared with large scale experimental data obtained within the safety work package. Generally, (apart from where continuously accelerating flames were produced), satisfactory agreement was achieved. This demonstrated that the modified models could be used, in many cases, for risk assessment purposes for explosions involving natural gas/hydrogen mixtures. The second part of thesis concentrated on predicting the incident thermal radiation from high pressure jet fires and pipelines fires involving natural gas/hydrogen mixtures. The approach taken was to modify existing models, developed for natural gas. For jet fires three models were used. Fuel specific input parameters were derived and the predictions of flame length and incident radiation compared with large scale experimental data. For pipeline fires a model was developed using a multi-point source approach for the radiation emitted by the fire and a correlation for flame length. Again predictions were compared with large scale experimental data. For both types of fire, satisfactory predictions of the flame length and incident radiation were obtained for natural gas and mixtures of natural gas and hydrogen containing approximately 25% hydrogen.

Turbulent premixed propane/air and methane/air flames were studied using planar Rayleigh scattering and particle image velocimetry on a stabilized Bunsen type burner. The fuel-air equivalence ratio was varied from Φ=0.7 to 1.0 for propane flames, and from Φ=0.6 to 1.0 for methane flames. The non-dimensional turbulence intensity, u'/SL (ratio of fluctuation velocity to laminar burning velocity), covered the range from 3 to 24, equivalent to conditions of corrugated flamelets and thin reaction zones regimes. Temperature gradients decreased with the increasing u'/SL and levelled off beyond u'/SL > 10 for both propane and methane flames. Flame front thickness increased slightly as u'/SL increased for both mixtures, although the thickness increase was more noticeable for propane flames, which meant the thermal flame front structure was being thickened. A zone of higher temperature was observed on the average temperature profile in the preheat zone of the flame front as well as some instantaneous temperature profiles at the highest u'/SL. Curvature probability density functions were similar to the Gaussian distribution at all u'/SL for both mixtures and for all the flame sections. The mean curvature values decreased as a function of u'/SL and approached zero. Flame front thickness was smaller when evaluated at flame front locations with zero curvature than that with curvature. Temperature gradients and FSD were larger when the flame curvature was zero. The combined thickness and FSD data suggest that the curvature effect is more dominant than that of the stretch by turbulent eddies during flame propagation. Integrated flame surface density for both propane and methane flames exhibited no dependance on u'/SL regardless of the FSD method used for evaluation. This observation implies that flame surface area may not be the dominant factor in increasing the turbulent burning velocity and the flamelet assumption may not be valid under the conditions studied. Dκ term, the product of diffusivity evaluated at conditions studied and the flame front curvature, was a magnitude smaller than or the same magnitude as the laminar burning velocity.

The laminar burning velocity is an important fundamental property of a fuel-air mixture at given conditions of temperature and pressure. Knowledge of burning velocities is required as an input for combustion models, including engine simulations, and the validation of chemical kinetic mechanisms. It is also important to understand the effect of stretch upon laminar flames, to correct for stretch and determine true (unstretched) laminar burning velocities, but also for modelling combustion where stretch rates are high, such as turbulent combustion models. A constant volume combustion vessel has been used in this work to determine burning velocities using two methods: a) flame speed measurements during the constant pressure period, and b) analysis of the pressure rise data. Consistency between these two techniques has been demonstrated for the first time. Flame front imaging and linear extrapolation of flame speed has been used to determine unstretched flame speeds at constant pressure and burned gas Markstein lengths. Measurement of the pressure rise during constant volume combustion has been used along with a numerical multi-zone combustion model to determine burning velocities for elevated temperatures and pressures as the unburned gas ahead of the spherically expanding flame front is compressed isentropically. This burning velocity data is correlated using a 14 term correlation to account for the effects of equivalence ratio, temperature, pressure and fraction of diluents. This correlation has been modified from an existing 12 term correlation to more accurately represent the dependence of burning velocity upon temperature and pressure. A number of fuels have been tested in the combustion vessel. Biogas (mixtures of CH₄ and CO₂) has been tested for a range of equivalence ratios (0.7–1.4), with initial temperatures of 298, 380 and 450 K, initial pressures of 1, 2 and 4 bar and CO₂ fractions of up to 40% by mole. Hydrous ethanol has been tested at the same conditions (apart from 298 K due to the need to vaporise the ethanol), and for fractions of water up to 40% by volume. Binary, ternary and quaternary blends of toluene, n-heptane, ethanol and iso-octane (THEO) have been tested for stoichiometric mixtures only, at 380 and 450 K, and 1, 2 and 4 bar, to represent surrogate gasoline blended with ethanol. For all fuels, correlation coefficients have been obtained to represent the burning velocities over wide ranging conditions. Common trends are seen, such as the reduction in burning velocity with pressure and increase with temperature. In the case of biogas, increasing CO₂ results in a decrease in burning velocity, a shift in peak burning velocity towards stoichiometric, a decrease in burned gas Markstein length and a delayed onset of cellularity. For hydrous ethanol the reduction in burning velocity as H₂O content is increased is more noticeably non-linear, and whilst the onset of cellularity is delayed, the effect on Markstein length is minor. Chemical kinetic simulations are performed to replicate the conditions for biogas mixtures using the GRI 3.0 mechanism and the FlameMaster package. For hydrous ethanol, simulations were performed by Carsten Olm at Eötvös Loránd University, using the OpenSMOKE 1D premixed flame solver. In both cases, good agreement with experimental results is seen. Tests have also been performed using a single cylinder optical engine to compare the results of the hydrous ethanol tests with early burn combustion, and a good comparison is seen. Results from tests on THEO fuels are compared with mixing rules developed in the literature to enable burning velocities of blends to be determined from knowledge of that of the pure components alone. A variety of rules are compared, and it is found that in most cases, the best approximation is found by using the rule in which the burning velocity of the blend is represented by weighting by the energy fraction of the individual components.