This thesis is concerned with investigations on two related issues of turbulent jet diffusion flame, namely (a) stabilization at liftoff and (b) autoignition in a turbulent jet diffusion flame. The approach of Conditional Moment Closure (CMC) has been taken. Fully elliptic first order CMC equations are solved with detailed chemistry to simulate lifted H2/N2 flame in vitiated coflow. The same approach is further used to simulate transient autoignition process in inhomogeneous mixing layers. In Chapter 1, difficulties involved in numerical simulation of turbulent combustion problems are explained. Different numerical tools used to simulate turbulent combustion are briefly discussed. Previous experimental, theoretical and numerical studies of lifted jet diffusion flames and autoignition are reviewed. Various research issues related to objectives of the thesis are discussed. In Chapter 2, the first order CMC transport equations for the reacting flows are presented. Various closure models that are required for solving the governing equations are given. Calculation of mean reaction rate term for detailed chemistry is given with special focus on the reaction rates for pressure dependent reactions. In Chapter 3, starting with the laminar flow code, further extension is carried to include kε turbulence model and PDF model. The code is validated at each stage of inclusion of different model. In this chapter, the code is first validated for the test problem of constant density, 2D, axisymmetric turbulent jet. Further, validation of PDF model is carried out by simulating the problem of nonreacting jet of cold air issuing into a vitiated coflow. The results are compared with the published data from experiments as well as numerical simulations. It is shown that the results compare well with the data. In Chapter 4, numerical results of lifted jet diffusion flame are presented. Detailed chemistry is modelled using Mueller mechanism for H2/O2 system with 9 species and 21 reversible reactions. Simulations are carried out for different jet velocities and coflow stream temperatures. The predicted liftoff generally agrees with experimental data, as well as joint PDF results. Profiles of mean scalar fluxes in the mixture fraction space, for different coflow temperatures reveal that (1) Inside the flamezone, the chemical term balances the molecular diffusion term, and hence the structure is of a diffusion flamelet for both cases. (2) In the preflame zone, the structure depends on the coflow temperature: for low coflow temperatures, the chemical term being small, the advective term balances the axial diffusion term. However, for the high coflow temperature case, the chemical term is large and balances the advective term, the axial diffusion term being small. It is concluded that, liftoff is controlled (a) by turbulent premixed flame propagation for low cofflow temperature while (b) by autoignition for high coflow temperature. In Chapter 5, the numerical results of autoignition in inhomogeneous mixing layer are presented. The configuration consists of a fuel jet issued into hot air for which transient simulations are performed. It is found that the constants assumed in various modelling terms can severely influence the results, particularly the flame temperature. Hence, modifications to these constants are suggested to obtain improved predictions. Preliminary work is carried out to predict autoignition lengths (which may be defined by Tign × Ujet incase of jet- and coflowvelocities being equal) by varying the coflow temperature. The autoignition lengths show a reasonable agreement with the experimental data and LES results. In Chapter 6, main conclusions of this thesis are summarized. Possible future studies on this problem are suggested.

This thesis describes the application of the first-order Conditional Moment Closure (CMC) to the autoignition of high-pressure fuel jets, and to piloted and lifted turbulent jet flames using classical and advanced CMC submodels. A Doubly-Conditional Moment Closure (DCMC) formulation is further proposed. In the first study, CMC is applied to investigate the impact of C₂H₆, H₂ and N₂ additives on the autoignition of high-pressure CH₄ jets injected into lower pressure heated air. A wide range of pre-combustion air temperatures is considered and detailed chemical kinetics are employed. It is demonstrated that the addition of C₂H₆ and H₂ does not change the main CH₄ oxidisation pathways. The decomposition of these additives provides additional ignition-promoting radicals, and therefore leads to shorter ignition delays. N₂ additives do not alter the CH₄ oxidisation pathways, however, they reduce the amount of CH₄ available for reaction, causing delayed ignition. It is further shown that ignition always occurs in lean mixtures and at low scalar dissipation rates. The second study is concerned with the modelling of a piloted CH₄/air turbulent jet flame. A detailed assessment of several Probability Density Function (PDF), Conditional Scalar Dissipation Rate (CSDR) and Conditional Velocity (CV) submodels is first performed. The results of two β-PDF-based implementations are then presented. The two realisations differ by the modelling of the CSDR. Homogeneous (inconsistent) and inhomogeneous (consistent) closures are considered. It is shown that the levels of all reactive scalars, including minor intermediates and radicals, are better predicted when the effects of inhomogeneity are included in the modelling of the CSDR. The two following studies are focused on the consistent modelling of a lifted H₂/N₂ turbulent jet flame issuing into a vitiated coflow. Two approaches are followed to model the PDF. In the first, a presumed β-distribution is assumed, whereas in the second, the Presumed Mapping Function (PMF) approach is employed. Fully consistent CV and CSDR closures based on the β-PDF and the PMF-PDF are employed. The homogeneous versions of the CSDR closures are also considered in order to assess the effect of the spurious sources which stem from the inconsistent modelling of mixing. The flame response is analysed over a narrow range of coflow temperatures (Tc). The stabilisation mechanism is determined from the analysis of the transport budgets in mixture fraction and physical spaces, and the history of radical build-up ahead of the stabilisation height. The β-PDF realisations indicate that the flame is stabilised by autoignition irrespective of the value of Tc. On the other hand, the PMF realisations reveal that the stabilisation mechanism is susceptible to Tc. Autoignition remains the controlling stabilisation mechanism for sufficiently high Tc. However, as Tc is decreased, stabilisation is achieved by means of premixed flame propagation. The analysis of the spurious sources reveals that their effect is small but non-negligible, most notably within the flame zone. Further, the assessment of several H₂ oxidation mechanisms show that the flame is very sensitive to chemical kinetics. In the last study, a DCMC method is proposed for the treatment of fluctuations in non-premixed and partially premixed turbulent combustion. The classical CMC theory is extended by introducing a normalised Progress Variable (PV) as a second conditioning variable beside the mixture fraction. The unburnt and burnt states involved in the normalisation of the PV are specified such that they are mixture fraction-dependent. A transport equation for the normalised PV is first obtained. The doubly-conditional species, enthalpy and temperature transport equations are then derived using the decomposition approach and the primary closure hypothesis is applied. Submodels for the doubly-conditioned unclosed terms which arise from the derivation of DCMC are proposed. As a preliminary analysis, the governing equations are simplified for homogeneous turbulence and a parametric assessment is performed by varying the strain rate levels in mixture fraction and PV spaces.

This thesis describes the application of the first-order Conditional Moment Closure (CMC) to the autoignition of high-pressure fuel jets, and to piloted and lifted turbulent jet flames using classical and advanced CMC submodels. A Doubly-Conditional Moment Closure (DCMC) formulation is further proposed. In the first study, CMC is applied to investigate the impact of C₂H₆, H₂ and N₂ additives on the autoignition of high-pressure CH₄ jets injected into lower pressure heated air. A wide range of pre-combustion air temperatures is considered and detailed chemical kinetics are employed. It is demonstrated that the addition of C₂H₆ and H₂ does not change the main CH₄ oxidisation pathways. The decomposition of these additives provides additional ignition-promoting radicals, and therefore leads to shorter ignition delays. N₂ additives do not alter the CH₄ oxidisation pathways, however, they reduce the amount of CH₄ available for reaction, causing delayed ignition. It is further shown that ignition always occurs in lean mixtures and at low scalar dissipation rates. The second study is concerned with the modelling of a piloted CH₄/air turbulent jet flame. A detailed assessment of several Probability Density Function (PDF), Conditional Scalar Dissipation Rate (CSDR) and Conditional Velocity (CV) submodels is first performed. The results of two β-PDF-based implementations are then presented. The two realisations differ by the modelling of the CSDR. Homogeneous (inconsistent) and inhomogeneous (consistent) closures are considered. It is shown that the levels of all reactive scalars, including minor intermediates and radicals, are better predicted when the effects of inhomogeneity are included in the modelling of the CSDR. The two following studies are focused on the consistent modelling of a lifted H₂/N₂ turbulent jet flame issuing into a vitiated coflow. Two approaches are followed to model the PDF. In the first, a presumed β-distribution is assumed, whereas in the second, the Presumed Mapping Function (PMF) approach is employed. Fully consistent CV and CSDR closures based on the β-PDF and the PMF-PDF are employed. The homogeneous versions of the CSDR closures are also considered in order to assess the effect of the spurious sources which stem from the inconsistent modelling of mixing. The flame response is analysed over a narrow range of coflow temperatures (Tc). The stabilisation mechanism is determined from the analysis of the transport budgets in mixture fraction and physical spaces, and the history of radical build-up ahead of the stabilisation height. The β-PDF realisations indicate that the flame is stabilised by autoignition irrespective of the value of Tc. On the other hand, the PMF realisations reveal that the stabilisation mechanism is susceptible to Tc. Autoignition remains the controlling stabilisation mechanism for sufficiently high Tc. However, as Tc is decreased, stabilisation is achieved by means of premixed flame propagation. The analysis of the spurious sources reveals that their effect is small but non-negligible, most notably within the flame zone. Further, the assessment of several H₂ oxidation mechanisms show that the flame is very sensitive to chemical kinetics. In the last study, a DCMC method is proposed for the treatment of fluctuations in non-premixed and partially premixed turbulent combustion. The classical CMC theory is extended by introducing a normalised Progress Variable (PV) as a second conditioning variable beside the mixture fraction. The unburnt and burnt states involved in the normalisation of the PV are specified such that they are mixture fraction-dependent. A transport equation for the normalised PV is first obtained. The doubly-conditional species, enthalpy and temperature transport equations are then derived using the decomposition approach and the primary closure hypothesis is applied. Submodels for the doubly-conditioned unclosed terms which arise from the derivation of DCMC are proposed. As a preliminary analysis, the governing equations are simplified for homogeneous turbulence and a parametric assessment is performed by varying the strain rate levels in mixture fraction and PV spaces.

Autoignition characteristics of pre-vaporized iso-octane, primary reference fuels, gasolines, and dimethyl ether (DME) have been investigated experimentally in a coflow with elevated temperature of air. With the coflow air at relatively low initial temperatures below autoignition temperature Tauto, an external ignition source was required to stabilize the flame. Non-autoignited lifted flames had tribrachial edge structures and their liftoff heights correlated well with the jet velocity scaled by the stoichiometric laminar burning velocity, indicating the importance of the edge propagation speed on flame stabilization balanced with local flow velocity. At high initial temperatures over Tauto, the autoignited flames were stabilized without requiring an external ignition source. The autoignited lifted flames exhibited either tribrachial edge structures or Mild combustion behaviors depending on the level of fuel dilution. For the iso-octane and n-heptane fuels, two distinct transition behaviors were observed in the autoignition regime from a nozzle-attached flame to a lifted tribrachial-edge flame and then a sudden transition to lifted Mild combustion as the jet velocity increased at a certain fuel dilution level. The liftoff data of the autoignited flames with tribrachial edges were analyzed based on calculated ignition delay times for the pre-vaporized fuels. Analysis of the experimental data suggested that ignition delay time may be much less sensitive to initial temperature under atmospheric pressure conditions as compared with predictions. For the gasoline fuels for advanced combustion engines (FACEs), and primary reference fuels (PRFs), autoignited liftoff data were correlated with Research Octane Number and Cetane Number. For the DME fuel, planar laser-induced fluorescence (PLIF) of formaldehyde (CH2O) and CH* chemiluminescence were visualized qualitatively. In the autoignition regime for both tribrachial structure and mild combustion, formaldehyde were found mainly between the fuel nozzle and the lifted flame edge. On the other hand, they were formed just prior to the flame edge for the non-autoignited lifted flames. The effect of fuel pyrolysis and partial oxidation were found to be important in explaining autoignited liftoff heights, especially in the Mild combustion regime. Flame structures of autoignited flames were investigated numerically for syngas (CO/H2) and methane fuels. The simulations of syngas fuel accounting for the differential diffusion have been performed by adopting several kinetic mechanisms to test the models ability in predicting the flame behaviors observed previously. The results agreed well with the observed nozzle-attached flame characteristics in case of non-autoignited flames. For autoignited lifted flames in high temperature regime, a unique autoignition behavior can be predicted having HO2 and H2O2 radicals in a broad region between the nozzle and stabilized lifted flame edge. Autoignition characteristics of laminar nonpremixed methane jet flames in high- temperature coflow air were studied numerically. Several flame configurations were investigated by varying the initial temperature and fuel mole fraction. Characteristics of chemical kinetics structures for autoignited lifted flames were discussed based on the kinetic structures of homogeneous autoignition and flame propagation of premixed mixtures. Results showed that for autoignited lifted flame with tribrachial structure, a transition from autoignition to flame propagation modes occurs for reasonably stoichiometric mixtures. Characteristics of Mild combustion can be treated as an autoignited lean premixed lifted flame. Transition behavior from Mild combustion to a nozzle-attached flame was also investigated by increasing the fuel mole fraction.

Detailed investigation of the vaporization of an isolated of ethanol and 1-propanol droplet was carried out in this experimental study. The experimental set-up consists of a heated chamber with a cross quartz fibers configuration as droplet support. An alcohol droplet is located at the intersection of the cross quartz fibre with a controlled initial diameter (300-600µm). Ambient temperature is varied from 298 to 973K at atmospheric pressure. The quasi-steady theory has been used to compare and to explain all experimental results. The real impact of the water concentration on the vaporization rate of an ethanol droplet is also examined, where two 'quasi-steady' periods are observed on the d2-curves, clearly showing that the vaporization of an ethanol droplet is accompanied by the simultaneous condensation of water vapour on the droplet surface and thus the temporal evolution of the droplet squared diameter exhibits an unsteady behavior. The histories of the instantaneous vaporization rates of both 1-propanol and ethanol droplets confirm this phenomenon. The autoignition experimental study of ethanol, 1-propanol and blends of ethanol and water have been carried out in a rapid compression machine at a compressed pressure of 30bar over a temperature range of 750-860K for stoichiometric mixture of fuel and air. The ignition delay times recorded show a significant decrease with increasing temperature. 1-propanol is more reactive than ethanol, which results in shorter ignition delay times. However, water addition to ethanol increases the reactivity of the mixture and results in a shorter ignition delay times than 1-propanol