A new diagnostic technique for studying the turbulent mixing characteristics of supersonic mixing flowfields is developed and implemented in two Mach 3 mixing flowfields. The diagnostic utilizes simultaneous particle image velocimetry and quantitative planar laser-induced fluorescence of krypton gas to study the interaction between turbulent scalar and velocity fields. The fluorescence properties of krypton gas are determined; measurements of the pressure and temperature dependence of the collisional quenching rates and cross-sections are made for various mixtures with krypton. The gases tested in this fashion include helium, nitrogen, air, oxygen, and ethylene. Additional measurements are performed to measure the relative two-photon absorption cross-section for krypton gas. The non-dimensional quenching rates are found to follow a power-law dependence for temperature, while the pressure dependence of the total quenching rate is found to be linear. Two injection flowfields are studied for their general topology and kinematic characteristcs. The first injector model is a basic injector meant to serve as a baseline case; there are no hypermixing elements present in this model. The second model is an asymmetric, unswept hypermixing injector featuring 15 degree expansive ramps flanking a central block. These studies utilize particle image velocimetry in planar and stereoscopic configurations in various planes. Results for the mean flowfield show distinct differences between the two flowfields; the planar injector flowfield is shown to be highly two-dimensional and exhibits minimal coherent unsteady behavior. The hypermixing injector flowfield exhibits a highly three-dimensional wake, with a pair of stream-wise vortices driving both mean deviations in the flowfield and considerable vortical coupling in the span-wise direction. Simultaneous krypton PLIF and PIV are employed in the two mixing flowfields. An assay of the dependence of the krypton mole fraction calculations on the fluorescence signal is performed. The overall sensitivity and the resulting dynamic range of the calibration is dictated largely by the reference mole fraction. Additionally, several different theoretical models of the temperature dependence of the fluorescence signal are studied to assess their validity and influence over the PLIF calibration procedure. Finally, the technique is employed in the two mixing flowfields, and a brief analysis of the mean and unsteady behavior of the two is conducted. / text

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Doctor of Philosophy (PhD) / In recent times significant public attention has been drawn to the topic of combustion. This has been due to the fact that combustion is the underlying mechanism of several key challenges to modern society: climate change, energy security (finite reserves of fossil fuels) and air pollution. The further development of combustion science is undoubtedly necessary to find improved solutions to manage these combustion science related challenges in the near and long term future. Combustion is essentially an exothermic process, this exothermicity or heat release essentially occurs at small scales, by small scales it meant these scales are small relative to the fluid length scales, for example heat release layer thicknesses in flames are typically much less than the fluid integral length scales. As heat release occurs at small scales this means that in turbulent combustion the small scales of the turbulence (which can be of the order of the heat release layer thickness) can possibly interact and influence the heat release and thus chemistry of the flame reaction zone. Premixed combustion is a combustion mode where the fuel and oxidiser are completely premixed prior to the flame reaction zone, this mode of combustion has been shown to be a promising method to maximise combustion efficiency and minimise pollutant formation. The continued and further application of premixed combustion to practical applications is limited by the current understanding of turbulent premixed combustion, these limitations in understanding are linked to the specific flame phenomena that can significantly influence premixed combustion in a combustion device, examples of such phenomena are: flame flashback, flame extinction and fuel consumption rate – all phenomena that are influenced by the interaction of the small scales of turbulence and chemistry. It is the study and investigation of the interaction of turbulence and chemistry at the small scales (termed finite-rate chemistry) in turbulent premixed flames that is the aim of this thesis which is titled “Finite-rate chemistry effects in turbulent premixed combustion”. Two very closely related experimental burner geometries have been developed in this thesis: the Piloted Premixed Jet Burner (PPJB) and the Premixed Jet Burner (PJB). Both feature an axisymmetric geometry and exhibit a parabolic like flow field. The PPJB and PJB feature a small 4mm diameter central jet from which a high velocity lean-premixed methane-air mixture issues. Surrounding the central jet in the PPJB is a 23.5mm diameter pilot of stoichiometric methane-air products, the major difference between the PPJB and the PJB is that the PJB does not feature a stoichiometric pilot. The pilot in the PPJB provides a rich source of combustion intermediates and enthalpy which promotes initial ignition of the central jet mixture. Surrounding both the central jet and pilot is a large diameter hot coflow of combustion products. It is possible to set the temperature of the hot coflow to the adiabatic flame temperature of the central jet mixture to simulate straining and mixing against and with combustion products without introducing complexities such as quenching and dilution from cold air. By parametrically increasing the central jet velocity in the PPJB it is possible to show that there is a transition from a thin conical flame brush to a flame that exhibits extinction and re-ignition effects. The flames that exhibit extinction and re-ignition effects have a luminous region near the jet exit termed the initial ignition region. This is followed by a region of reduced luminosity further downstream termed the extinction region. Further downstream the flame luminosity increases this region is termed the re-ignition region. For the flames that exhibit extinction and re-ignition it is proposed that intense turbulent mixing and high scalar dissipation rates drives the initial extinction process after the influence of the pilot has ceased (x/D>10). Re-ignition is proposed to occur downstream where turbulent mixing and scalar dissipation rates have decreased allowing robust combustion to continue. As the PJB does not feature a pilot, the flame stabilisation structure is quite different to the PPJB. The flame structure in the PJB is essentially a lifted purely premixed flame, which is an experimental configuration that is also quite unique. A suite of laser diagnostic measurements has been parametrically applied to flames in the PPJB and PJB. Laser Doppler Velocimetry (LDV) has been utilised to measure the mean and fluctuating radial and axial components of velocity at a point, with relevant time and length scale information being extracted from these measurements. One of the most interesting results from the LDV measurements is that in the PPJB the pilot delays the generation of high turbulence intensities, for flames that exhibit extinction the rapid increase of turbulence intensity after the pilot corresponds to the start of the extinction region. Using the LDV derived turbulence characteristics and laminar flame properties and plotting these flames on a traditional turbulent regime diagram indicates that all of the flames examined should fall in the so call distributed reaction regime. Planar imaging experiments have been conducted for flames using the PPJB and PJB to investigate the spatial structure of the temperature and selected minor species fields. Results from two different simultaneous 2D Rayleigh and OH PLIF experiments and a simultaneous 2D Rayleigh, OH PLIF and CH2O PLIF experiment are reported. For all of the flames examined in the PPJB and PJB a general trend of decreasing conditional mean temperature gradient with increasing turbulence intensity is observed. This indicates that a trend of so called flame front thickening with increased turbulence levels occurs for the flames examined. It is proposed that the mechanism for this flame front thickening is due to eddies penetrating and embedding in the instantaneous flame front. In the extinction region it is found that the OH concentration is significantly reduced compared to the initial ignition region. In the re-ignition region it is found that the OH level increases again indicating that an increase in the local reaction rate is occurring. In laminar premixed flames CH2O occurs in a thin layer in the reaction zone, it is found for all of the flames examined that the CH2O layer is significantly thicker than the laminar flame. For the high velocity flames beyond x/D=15, CH2O no longer exist in a distinct layer but rather in a near uniform field for the intermediate temperature regions. Examination of the product of CH2O and OH reveals that the heat release in the initial ignition region is high and rapidly decreases in the extinction region, an increase in the heat release further downstream is observed corresponding to the re-ignition region. This finding corresponds well with the initial hypothesis of an extinction region followed by a re-ignition region that was based on the mean chemiluminescence images. Detailed simultaneous measurement of major and minor species has been conducted using the line Raman-Rayleigh-LIF technique with CO LIF and crossed plane-OH PLIF at Sandia National Laboratories. By measuring all major species it is also possible to define a mixture fraction for all three streams of the PPJB. Using these three mixture fractions it was found that the influence of the pilot in the PPJB decays very rapidly for all but the lowest velocity flames. It was also found that for the high velocity flames exhibiting extinction, a significant proportion of the coflow fluid is entrained into the central jet combustion process at both the extinction region and re-ignition regions. The product of CO and OH conditional on temperature is shown to be proportion to the net production rate of CO2 for certain temperature ranges. By examining the product of CO and OH the hypothesis of an initial ignition region followed by an extinction region then a re-ignition region for certain PPJB flames has been further validated complementing the [CH2O][OH] imaging results. Numerical modelling results using the transported composition probability density function (TPDF) method coupled to a conventional Reynolds averaged Naiver Stokes (RANS) solver are shown in this thesis to successfully predict the occurrence of finite-rate chemistry effects for the PM1 PPJB flame series. To calculate the scalar variance and the degree of finite-rate chemistry effects correctly, it is found that a value of the mixing constant ( ) of approximately 8.0 is required. This value of is much larger than the standard excepted range of 1.5-2.3 for that has been established for non-premixed combustion. By examining the results of the RANS turbulence model in a non-reacting variable density jet, it is shown that the primary limitation of the predictive capability of the TPDF-RANS method is the RANS turbulence model when applied to variable density flows.

This thesis assesses the extent to which jet precession can be used to control the mean and instantaneous particle distributions in particle-laden jet flows. Investigations were conducted, providing quantitative, planar measurements of instantaneous particle distributions in the first 10 nozzle diameters of a particle-laden co-annular nozzle with centrally located Precessing Jet (PJ). Equipment was specifically designed to conduct the investigations, a laser diagnostic technique developed and a methodology to quantify particle clusters was devised. The experimental facilities are scaled to simulate the near burner region of a typical rotary cement kiln. The laser diagnostic technique, called planar nephelometry, enables non-intrusive, quantitative, instantaneous, planar measurements of particle distributions without the need to identify individual particles. The methodology to quantify particle clusters is designed to enable statistical comparison of clusters without ambiguity. Measurements of the influence of particle mass loading and jet precession on the distribution of particles emerging from an particle-laden co-annular nozzle, with a centrally located PJ nozzle, are presented. These data include mean and standard deviation of the particle distributions and statistics on particle cluster characteristics. The results indicate that small amounts of momentum through the PJ nozzle causes an elongation of the jet, but larger amounts of momentum through the PJ nozzle will result in a wider mean particle distribution and greater mean centreline decay rate. An increase in jet precession also results in an increase in the fluctuations in the particle distributions. The transition is determined by the interplay of momentum of the particle-laden and precessing streams. The physical characteristics of identified particle clusters in the instantaneous planar flow field are also influenced by jet precession. An initial increase in the amount of jet precession results in an overall decrease in the average number of both small- and large-clusters. The size of small-clusters generally reduces with increasing jet precession, whereas large-clusters reach maximum sizes for an intermediate relative momentum of jet precession. Analogous to the influence of jet precession on the mean distribution of particles, increasing jet precession also results in a greater spread of small- and large-clusters. Results also indicate that increasing the mass flow rate of particles results in an elongation of the jet. However, these variations correspond to an increase in annular jet momentum, rather than an addition of secondary phase. The particle mass flow rate has a minor influence on the general characteristics of particle clusters. / http://proxy.library.adelaide.edu.au/login?url= http://library.adelaide.edu.au/cgi-bin/Pwebrecon.cgi?BBID=1370427 / Thesis (Ph.D.) -- University of Adelaide, School of Mechanical Engineering, 2009

Doctor of Philosophy (PhD) / In recent times significant public attention has been drawn to the topic of combustion. This has been due to the fact that combustion is the underlying mechanism of several key challenges to modern society: climate change, energy security (finite reserves of fossil fuels) and air pollution. The further development of combustion science is undoubtedly necessary to find improved solutions to manage these combustion science related challenges in the near and long term future. Combustion is essentially an exothermic process, this exothermicity or heat release essentially occurs at small scales, by small scales it meant these scales are small relative to the fluid length scales, for example heat release layer thicknesses in flames are typically much less than the fluid integral length scales. As heat release occurs at small scales this means that in turbulent combustion the small scales of the turbulence (which can be of the order of the heat release layer thickness) can possibly interact and influence the heat release and thus chemistry of the flame reaction zone. Premixed combustion is a combustion mode where the fuel and oxidiser are completely premixed prior to the flame reaction zone, this mode of combustion has been shown to be a promising method to maximise combustion efficiency and minimise pollutant formation. The continued and further application of premixed combustion to practical applications is limited by the current understanding of turbulent premixed combustion, these limitations in understanding are linked to the specific flame phenomena that can significantly influence premixed combustion in a combustion device, examples of such phenomena are: flame flashback, flame extinction and fuel consumption rate – all phenomena that are influenced by the interaction of the small scales of turbulence and chemistry. It is the study and investigation of the interaction of turbulence and chemistry at the small scales (termed finite-rate chemistry) in turbulent premixed flames that is the aim of this thesis which is titled “Finite-rate chemistry effects in turbulent premixed combustion”. Two very closely related experimental burner geometries have been developed in this thesis: the Piloted Premixed Jet Burner (PPJB) and the Premixed Jet Burner (PJB). Both feature an axisymmetric geometry and exhibit a parabolic like flow field. The PPJB and PJB feature a small 4mm diameter central jet from which a high velocity lean-premixed methane-air mixture issues. Surrounding the central jet in the PPJB is a 23.5mm diameter pilot of stoichiometric methane-air products, the major difference between the PPJB and the PJB is that the PJB does not feature a stoichiometric pilot. The pilot in the PPJB provides a rich source of combustion intermediates and enthalpy which promotes initial ignition of the central jet mixture. Surrounding both the central jet and pilot is a large diameter hot coflow of combustion products. It is possible to set the temperature of the hot coflow to the adiabatic flame temperature of the central jet mixture to simulate straining and mixing against and with combustion products without introducing complexities such as quenching and dilution from cold air. By parametrically increasing the central jet velocity in the PPJB it is possible to show that there is a transition from a thin conical flame brush to a flame that exhibits extinction and re-ignition effects. The flames that exhibit extinction and re-ignition effects have a luminous region near the jet exit termed the initial ignition region. This is followed by a region of reduced luminosity further downstream termed the extinction region. Further downstream the flame luminosity increases this region is termed the re-ignition region. For the flames that exhibit extinction and re-ignition it is proposed that intense turbulent mixing and high scalar dissipation rates drives the initial extinction process after the influence of the pilot has ceased (x/D>10). Re-ignition is proposed to occur downstream where turbulent mixing and scalar dissipation rates have decreased allowing robust combustion to continue. As the PJB does not feature a pilot, the flame stabilisation structure is quite different to the PPJB. The flame structure in the PJB is essentially a lifted purely premixed flame, which is an experimental configuration that is also quite unique. A suite of laser diagnostic measurements has been parametrically applied to flames in the PPJB and PJB. Laser Doppler Velocimetry (LDV) has been utilised to measure the mean and fluctuating radial and axial components of velocity at a point, with relevant time and length scale information being extracted from these measurements. One of the most interesting results from the LDV measurements is that in the PPJB the pilot delays the generation of high turbulence intensities, for flames that exhibit extinction the rapid increase of turbulence intensity after the pilot corresponds to the start of the extinction region. Using the LDV derived turbulence characteristics and laminar flame properties and plotting these flames on a traditional turbulent regime diagram indicates that all of the flames examined should fall in the so call distributed reaction regime. Planar imaging experiments have been conducted for flames using the PPJB and PJB to investigate the spatial structure of the temperature and selected minor species fields. Results from two different simultaneous 2D Rayleigh and OH PLIF experiments and a simultaneous 2D Rayleigh, OH PLIF and CH2O PLIF experiment are reported. For all of the flames examined in the PPJB and PJB a general trend of decreasing conditional mean temperature gradient with increasing turbulence intensity is observed. This indicates that a trend of so called flame front thickening with increased turbulence levels occurs for the flames examined. It is proposed that the mechanism for this flame front thickening is due to eddies penetrating and embedding in the instantaneous flame front. In the extinction region it is found that the OH concentration is significantly reduced compared to the initial ignition region. In the re-ignition region it is found that the OH level increases again indicating that an increase in the local reaction rate is occurring. In laminar premixed flames CH2O occurs in a thin layer in the reaction zone, it is found for all of the flames examined that the CH2O layer is significantly thicker than the laminar flame. For the high velocity flames beyond x/D=15, CH2O no longer exist in a distinct layer but rather in a near uniform field for the intermediate temperature regions. Examination of the product of CH2O and OH reveals that the heat release in the initial ignition region is high and rapidly decreases in the extinction region, an increase in the heat release further downstream is observed corresponding to the re-ignition region. This finding corresponds well with the initial hypothesis of an extinction region followed by a re-ignition region that was based on the mean chemiluminescence images. Detailed simultaneous measurement of major and minor species has been conducted using the line Raman-Rayleigh-LIF technique with CO LIF and crossed plane-OH PLIF at Sandia National Laboratories. By measuring all major species it is also possible to define a mixture fraction for all three streams of the PPJB. Using these three mixture fractions it was found that the influence of the pilot in the PPJB decays very rapidly for all but the lowest velocity flames. It was also found that for the high velocity flames exhibiting extinction, a significant proportion of the coflow fluid is entrained into the central jet combustion process at both the extinction region and re-ignition regions. The product of CO and OH conditional on temperature is shown to be proportion to the net production rate of CO2 for certain temperature ranges. By examining the product of CO and OH the hypothesis of an initial ignition region followed by an extinction region then a re-ignition region for certain PPJB flames has been further validated complementing the [CH2O][OH] imaging results. Numerical modelling results using the transported composition probability density function (TPDF) method coupled to a conventional Reynolds averaged Naiver Stokes (RANS) solver are shown in this thesis to successfully predict the occurrence of finite-rate chemistry effects for the PM1 PPJB flame series. To calculate the scalar variance and the degree of finite-rate chemistry effects correctly, it is found that a value of the mixing constant ( ) of approximately 8.0 is required. This value of is much larger than the standard excepted range of 1.5-2.3 for that has been established for non-premixed combustion. By examining the results of the RANS turbulence model in a non-reacting variable density jet, it is shown that the primary limitation of the predictive capability of the TPDF-RANS method is the RANS turbulence model when applied to variable density flows.

<div>Recent interest in tailoring energetic materials designed to combat biological weapons agents (BWAs) has resulted in significant effort to produce and test these munitions. These energetic materials may contain agent defeat additives that enhance the capability of a munition to destroy BWAs through chemical methods in addition to heat. However, quantifying levels of agent and biocidal species and their interaction is difficult, and efforts have primarily focused on either ex-situ culturing of exposed bioagent simulants or in situ laser absorption measurements. These experiments are valuable for exploring long term agent defeat and line of sight averaged defeat. What these experiments do not provide, however, is in-situ, spatio-temporally resolved imaging in the reaction zone. To address this gap, this work develops the use of in-situ, high speed, two-dimensional optical diagnostics of fireballs and biological weapons agents simulants (BWA-S).</div><div> </div><div> Planar laser induced fluorescence (PLIF) and laser scattering have been conducted in situ. PLIF of both iodine vapor and BWA-S has demonstrated the ability to qualitatively observe species concentration in fireballs. The application of simultaneous techniques provides imaging of multiple parameters, which is invaluable to the further study of BWA-S and agent defeat interactions. These studies also provide the framework for future work in moving towards quantitative measurements, including the development of absorption and fluorescence models.</div>

Emissions of soot and polycyclic aromatic hydrocarbons (PAHs) from incomplete burning of hydrocarbon fuels pose a great threat to the environment and human health. To reduce such emissions, a comprehensive understanding of their evolution process is essential. In this work, a series of research studies were conducted to evaluate sooting tendencies and to experimentally and theoretically develop PAH mechanisms. The sooting tendencies of oxygenated fuels were quantitively investigated in counterflow diffusion flames. Sooting limits are described by critical fuel and oxygen mole fractions, measured with a laser scattering technique. The addition of dimethyl ether displays non-monotonic behavior on sooting tendencies at elevated pressures, which is attributed to the chemical effect from kinetic simulations. The tendency of incipient soot formation of other oxygenated fuels (e.g., alcohol, acid, ether, ketone, and carbonate ester) was also assessed, using a similar approach. As the precursor of soot, PAH measurement using laser induced fluoresecnce was implemented to track the evolution processes from PAHs to incipient soot. Developing a PAH mechanism is essential to the understanding of soot formation; however, PAH formation and its growth process are not well understood. Based on previous research, PAHs with 5-membered rings are abundant in flames. Therefore, the growth of PAHs with 5-membered rings was investigated, using acenaphthylene (A2R5) as the example. The density functional theory (DFT) and the transition state theory (TST) were adopted to calculate potential energy surfaces and reaction rate coefficients. The existence of 5-membered rings appreciably impacts PAH production by facilitating the formation of planar PAHs with C2H substitution, thereby improving existing PAH mechanisms. In PAH mechanisms, the thermochemistry properties are not all calculated, but are hypothesized to be equal to those of a similar structure. The simulation accuracy of the hypothesis is explored here by discussing the sensitivity of the thermochemistry parameters in flame simulations. The group additivity method utilizing THERM codes is used to calculate thermochemistry properties. PAH loading affects the sensitivity of thermochemistry properties to both flame temperature and product yields. These results show that either accurate thermochemistry properties, or reverse reaction rates should be provided in the mechanism to improve simulation accuracy.