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The soot properties of round, nonbuoyant, laminar jet diffusion flames are described, based on experiments at microgravity carried out on orbit during three flights of the Space Shuttle Columbia, (Flights STS-83, 94 and 107). Experimental conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K and ambient pressures of 35-100 kPa. Measurements included soot volume fraction distributions using deconvoluted laser extinction imaging, and soot temperature distributions using deconvoluted multiline emission imaging. Flowfield modeling based on the work of Spalding is presented. The present work explores whether soot properties of these flames are universal functions of mixture fraction, i.e., whether they satisfy soot state relationships. Measurements are presented, including radiative emissions and distributions of soot temperature and soot volume fraction. It is shown that most of the volume of these flames is bounded by the dividing streamline and thus should follow residence time state relationships. Most streamlines from the fuel supply to the surroundings are found to exhibit nearly the same maximum soot volume fraction and temperature. The radiation intensity along internal streamlines also is found to have relatively uniform values. Finally, soot state relationships were observed, i.e., soot volume fraction was found to correlate with estimated mixture fraction for each fuel/pressure selection. These results support the existence of soot property state relationships for steady nonbuoyant laminar diffusion flames, and thus in a large class of practical turbulent diffusion flames through the application of the laminar flamelet concept.

Processes of soot formation and oxidation must be understood in order to achieve reliable computational combustion calculations for nonpremixed (diffusion) flames involving hydrocarbon fuels. Motivated by this observation, the present investigation extended earlier work on soot formation and oxidation in laminar jet ethylene/air and methane/oxygen premixed and acetylene-nitrogen/air diffusion flames at atmospheric pressure in this laboratory, emphasizing soot surface growth and early soot surface oxidation in laminar diffusion flames fueled with a variety of hydrocarbons at pressures in the range 0.1 - 1.0 atm.

The present experimental study of soot processes in hydrocarbon-fueled laminar nonbuoyant and nonpremixed (diffusion) flames at microgravity within a spacecraft was motivated by the relevance of soot to the performance of power and propulsion systems, to the hazards of unwanted fires, and to the emission of combustion-generated pollutants. Soot processes in turbulent flames are of greatest practical interest, however, direct study of turbulent flames is not tractable because the unsteadiness and distortion of turbulent flames limit available residence times and spatial resolution within regions where soot processes are important. Thus, laminar diffusion flames are generally used to provide more tractable model flame systems to study processes relevant to turbulent diffusion flames, justified by the known similarities of gas-phase processes in laminar and turbulent diffusion flames, based on the widely-accepted laminar flamelet concept of turbulent flames. Unfortunately, laminar diffusion flames at normal gravity are affected by buoyancy due to their relatively small flow velocities and, as discussed next, they do not have the same utility for simulating the soot processes as they do for simulating the gas phase processes of turbulent flames.

Soot surface oxidation was studied experimentally in laminar hydrocarbon/air diffusion flames at atmospheric pressure. Measurements were carried out along the axes of round fuel jets burning in coflowing dry air considering acetylene-nitrogen, ethylene, propyiene-nitrogen, propane and acetylene-benzene-nitrogen in the fuel stream. Measurements were limited to the initial stages of soot oxidation (carbon consumption less than 70%) where soot oxidation occurs at the surface of primary soot particles. The following properties were measured as a function of distance above the burner exit: soot concentrations by deconvoluted laser extinction, soot temperatures by deconvoluted multiline emission, soot structure by thermophoretic sampling and analysis using Transmission Electron Microscopy (TEM), concentrations of major stable gas species (N2, H2O, H2, O2, CO, CO2, CH4, C2H2, C2H6, C3H6, C3H8, and C6H6) by sampling and gas chromatography, concentrations of some radical species (H, OH, O) by deconvoluted Li/LiOH atomic absorption and flow velocities by laser velocimetry. For present test conditions, it was found that soot surface oxidation rates were not affected by fuel type, that direct rates of soot surface oxidation by O2 estimated from Nagle and Strickland-Constable (1962) were small compared to observed soot surface oxidation rates because soot surface oxidation was completed near the flame sheet where O2 concentrations were less than 3% by volume, and that soot surface oxidation rates were described by the OH soot surface oxidation mechanism with a collision efficiency of 0.14 and an uncertainty (95% confidence) of +/- 0.04 when allowing for direct soot surface oxidation by O2, which is in reasonably good agreement with earlier observations of soot surface oxidation rates in both premixed and diffusion flames at atmospheric pressure.

The structure and soot surface growth properties of round laminar jet diffusion flames were studied experimentally. Measurements were made along the axes of ethylene-, propylene-propane- and acetylene-benzene-fueled flames burning in coflowing air at atmospheric pressure with the reactants at normal temperature. The measurements included soot structure, soot concentrations, soot temperatures, major gas species concentrations, some radial species (H, OH and 0) concentrations, and gas velocities. These measurements yielded the local flame properties that are thought to affect soot surface growth as well as local soot surface growth rates. When present results were combined with similar earlier observations of acetylene-fueled laminar jet diffusion flames, the results suggested that soot surface growth involved decomposition of the original fuel to form acetylene and H, which were the main reactants for soot surface growth, and that the main effect of the parent fuel on soot surface growth involved its yield of acetylene and H for present test conditions. Thus, as the distance increased along the axes of the flames, soot formation (which was dominated by soot surface growth) began near the cool core of the flow once acetylene and H appeared together and ended near the flame sheet when acetylene disappeared. Species mainly responsible for soot oxidation - OH and 02 were present throughout the soot formation region so that soot surface growth and oxidation proceeded at the same time. Present measurements of soot surface growth rates (corrected for soot surface oxidation) in laminar jet diffusion flames were consistent with earlier measurements of soot surface growth rates in laminar premixed flames and exhibited good agreement with existing Hydrogen-Abstraction/Carbon-Addition (HACA) soot surface growth mechanisms in the literature with steric factors in these mechanisms having values on the order of unity, as anticipated.

This is the final report of a research program considering the structure and the soot surface reaction properties of laminar nonpremixed (diffusion) flames. The study was limited to ground-based measurements of buoyant laminar jet diffusion flames at pressures of 0.1-1.0 atm. The motivation for the research is that soot formation in flames is a major unresolved problem of combustion science that influences the pollutant emissions, durability and performance of power and propulsion systems, as well as the potential for developing computational combustion. The investigation was divided into two phases considering the structure of laminar soot-containing diffusion flames and the soot surface reaction properties (soot surface growth and oxidation) of these flames, in turn. The first phase of the research addressed flame and soot structure properties of buoyant laminar jet diffusion flames at various pressures. The measurements showed that H, OH and O radical concentrations were generally in superequilibrium concentrations at atmospheric pressure but tended toward subequilibrium concentrations as pressures decreased. The measurements indicated that the original fuel decomposed into more robust compounds at elevated temperatures, such as acetylene (unless the original fuel was acetylene) and H, which are the major reactants for soot surface growth, and that the main effect of the parent fuel on soot surface growth involved its yield of acetylene and H for present test conditions. The second phase of the research addressed soot surface reaction properties, e.g., soot surface growth and surface oxidation. It was found that soot surface growth rates in both laminar premixed and diffusion flames were in good agreement, that these rates were relatively independent of fuel type, and that these rates could be correlated by the Hydrogen-Abstraction/Carbon-Addition (HACA) mechanisms of Colket and Hall (1994), Frenklach et al. (1990,1994), and Kazakov et al. (1995). It was also found that soot surface oxidation rates were relatively independent of fuel type, were not correlated with O2, CO2, H2O and O collision rates but were correlated with the collision rates of OH with a collision efficiency of 0.14, in agreement with the early measurements in premixed flames of Neoh et al. (1980), after allowing for oxidation by O2 via the classical rate expression of Nagle and Strickland-Constable (1962).

This is the final report of a research program considering interactions between flow and soot properties within laminar diffusion flames. Laminar diffusion flames were considered because they provide model flame systems that are far more tractable for theoretical and experimental studies than more practical turbulent diffusion flames. In particular, understanding the transport and chemical reaction processes of laminar flames is a necessary precursor to understanding these processes in practical turbulent flames and many aspects of laminar diffusion flames have direct relevance to turbulent diffusion flames through application of the widely recognized laminar flamelet concept of turbulent diffusion flames. The investigation was divided into three phases, considering the shapes of nonbuoyant round laminar jet diffusion flames in still air, the shapes of nonbuoyant round laminar jet diffusion flames in coflowing air, and the hydrodynamic suppression of soot formation in laminar diffusion flames.

The shapes (flame-sheet and luminous-flame boundaries) or steady weakly buoyant round hydrocarbon-fueled laminar-jet diffusion flames in still and coflowing air were studied both experimentally and theoretically. Flame-sheet shapes were measured from photographs using a CH optical filter to distinguish flame-sheet boundaries in the presence of blue CO2 and OH emissions and yellow continuum radiation from soot. Present experimental conditions included acetylene-, methane-, propane-, and ethylene-fueled flames having initial reactant temperatures of 300 K. ambient pressures of 4-50 kPa, jet-exit Reynolds numbers of 3-54, initial air/fuel velocity ratios of 0-9, and luminous flame lengths of 5-55 mm; earlier measurements for propylene- and 1,3-butadiene-fueled flames for similar conditions were considered as well. Nonbuoyant flames in still air were observed at microgravity conditions; essentially nonbuoyant flames in coflowing air were observed at small pressures to control effects of buoyancy. Predictions of luminous flame boundaries from soot luminosity were limited to laminar smoke-point conditions, whereas predictions of flame-sheet boundaries ranged from soot-free to smoke-point conditions. Flame-shape predictions were based on simplified analyses using the boundary-layer approximations along with empirical parameters to distinguish flame-sheet and luminous-flame (at the laminar smoke point) boundaries. The comparison between measurements and predictions was remarkably good and showed that both flame-sheet and luminous-flame lengths are primarily controlled by fuel flow rates with lengths in coflowing air approaching 2/3 of the lengths in still air as coflowing air velocities are increased. Finally, luminous flame lengths at laminar smoke-point conditions were roughly twice as long as flame-sheet lengths at comparable conditions because of the presence of luminous soot particles in the fuel-lean region of the flames.

The structure of the soot growth region of laminar premixed methane/oxygen flames (fuel-equivalence ratios of 1.60-2.77) was studied both experimentally and computationally. Measurements were carried out in flames stabilized on a flat flame burner operated at standard temperature and pressure, and included velocities by laser velocimetry, soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, major gas species concentrations by sampling and gas chromatography, and hydrogen atom concentrations by the Li/LiOH technique in conjunction with atomic absorption to find the proportion of free lithium in the flames. The measured concentrations of major gas species were in reasonably good agreement with predictions based on the detailed mechanisms of Leung and Lindstedt, and Frenklach and coworkers. The measurements also confirmed predictions of both these mechanisms that H-atom concentrations are in local thermodynamic equilibrium throughout the soot growth region even through the concentrations of major gas species are not. Thus, present findings support recent evaluations of the hydrogen-abstraction/carbon-addition (HACA) soot growth mechanism in similar flames, where the approximation that H-atom concentrations were in local thermodynamic equilibrium was adopted, based on predictions using the two mechanisms, due to the absence of direct H-atom concentration measurements.

The structure and soot surface growth properties of round laminar jet diffusion flames were studied experimentally. Measurements were made along the axes of ethylene-, propylene-propane- and acetylene-benzene-fueled flames burning in coflowing air at atmospheric pressure with the reactants at normal temperature. The measurements included soot structure, soot concentrations, soot temperatures, major gas species concentrations, some radial species (H, OH and O) concentrations, and gas velocities. These measurements yielded the local flame properties that are thought to affect soot surface growth as well as local soot surface growth rates. When present results were combined with similar earlier observations of acetylene-fueled laminar jet diffusion flames, the results suggested that soot surface growth involved decomposition of the original fuel to form acetylene and H, which were the main reactants for soot surface growth, and that the main effect of the parent fuel on soot surface growth involved its yield of acetylene and H for present test conditions. Thus, as the distance increased along the axes of the flames, soot formation (which was dominated by soot surface growth) began near the cool core of the flow once acetylene and H appeared together and ended near the flame sheet when acetylene disappeared. Species mainly responsible for soot oxidation - OH and O2 were present throughout the soot formation region so that soot surface growth and oxidation proceeded at the same time. Present measurements of soot surface growth rates (corrected for soot surface oxidation) in laminar jet diffusion flames were consistent with earlier measurements of soot surface growth rates in laminar premixed flames and exhibited good agreement with existing Hydrogen-Abstraction/Carbon-Addition (HACA) soot surface growth mechanisms in the literature with steric factors in these mechanisms having values on the order of unity, as anticipated.

The shapes (flame-sheet and luminous-flame boundaries) of steady nonbuoyant round hydrocarbon-fueled laminar-jet diffusion flames in still and coflowing air were studied both experimentally and theoretically. Flame-sheet shapes were measured from photographs using a CH optical filter to distinguish flame-sheet boundaries in the presence of blue CO2 and OH emissions and yellow continuum radiation from soot. Present experimental conditions included acetylene-, methane-, propane-, and ethylene-fueled flames having initial reactant temperatures of 300 K, ambient pressures of 4-50 kPa, jet exit Reynolds number of 3-54, initial air/fuel velocity ratios of 0-9 and luminous flame lengths of 5-55 mm; earlier measurements for propylene- and 1,3-butadiene-fueled flames for similar conditions were considered as well. Nonbuoyant flames in still air were observed at micro-gravity conditions; essentially nonbuoyant flames in coflowing air were observed at small pressures to control effects of buoyancy. Predictions of luminous flame boundaries from soot luminosity were limited to laminar smokepoint conditions, whereas predictions of flame-sheet boundaries ranged from soot-free to smokepoint conditions. Flame-shape predictions were based on simplified analyses using the boundary layer approximations along with empirical parameters to distinguish flame-sheet and luminous flame (at the laminar smoke point) boundaries. The comparison between measurements and predictions was remarkably good and showed that both flame-sheet and luminous-flame lengths are primarily controlled by fuel flow rates with lengths in coflowing air approaching 2/3 lengths in still air as coflowing air velocities are increased. Finally, luminous flame lengths at laminar smoke-point conditions were roughly twice as long as flame-sheet lengths at comparable conditions due to the presence of luminous soot particles in the fuel-lean region of the flames.

Recent past studies of soot reaction processes in laminar premixed and nonpremixed flames generally have used the intrusive technique of thermophoretic sampling and analysis by transmission electron microscopy (TEM) to observe soot structure and obtain important fundamental information about soot particle properties, such as soot primary particle diameters, the rate of change of soot primary particle diameter as a function of time (or rate of soot surface growth or oxidation), the amount of soot particle reactive surface area per unit volume, the number of primary soot particles per unit volume, and the rate of formation of primary soot particles (or the rate of soot primary particle nucleation). Given the soot volume per unit volume of the flame (or the soot volume fraction), all these properties are readily found from a measurement of the soot primary particle diameter (which usually is nearly a constant for each location within a laminar flame). This approach is not possible within freely propagating flames, however, because soot properties at given positions in such flames vary relatively rapidly as a function of time in the soot formation and oxidation regions compared to the relatively lengthy sampling times needed to accumulate adequate soot samples and to minimize effects of soot collected on the sampling grid as it moves to and from the sampling position through other portions of the flame. Thus, nonintrusive optical methods must be used to find the soot primary particle diameters needed to define the soot surface reaction properties mentioned earlier. Unfortunately, approximate nonintrusive methods used during early studies of soot reaction properties in flames, found from laser scattering and absorption measurements analyzed assuming either Rayleigh scattering or Mie scattering from polydisperse effective soot particles having the same mass of soot as individual soot aggregates, have not been found to be an effective way to estimate the soot surface reaction area per unit volume. Thus, alternative nonintrusive optical methods of finding these properties must be sought, which was the objective of this phase of the investigation. The alternative method used here involves use of the Rayleigh-Debye-Gans-Polydisperse-Fractal-Aggregate (RDG-PFA) scattering approximation for soot aggregates in flames. Thus, the development of this method will be discussed next before describing its evaluation as a means of nonintrusively measuring soot primary particle diameters in soot-containing flames.

The structure and soot properties of round, soot-emitting, nonbuoyant, laminar jet diffusion flames are described, based on long-duration (175-230-s) experiments at microgravity carried out on orbit in the Space Shuttle Columbia. Experimental conditions included ethylene-fueled flames burning in still air at nominal pressures of 50 and 100 kPa and an ambient temperature of 300 K with luminous flame lengths of 49-64 mm Measurements included luminous flame shapes using color video imaging soot concentration (volume fraction) distributions using deconvoluted laser extinction imaging, soot temperature distributions using deconvoluted multiline emission imaging, gas temperature distributions at fuel-lean (plume) conditions using thermocouple probes, soot structure distributions using thermophoretic sampling and analysis by transmission electron microscopy, and flame radiation using a radiometer.The present flames were larger, and emitted soot more readily, than comparable flames observed during ground-based microgravity experiments due to closer approach to steady conditions resulting from the longer test times and the reduced gravitational disturbances of the space-based experiments.

Flame structure and soot formation were studied within soot-containing laminar premixed methanefoxygen flames at atmospheric pressure. The following measurements were made: soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, soot structure by thermophoretic sampling and transmission electron microscope (TEM), major gas species concentrations by sampling and gas chromatography, and gas velocities by laser velocimetry. Present measurements of gas species concentrations were in reasonably good agreement with earlier measurements due to Ramer et al. as well as predictions based on the detailed mechanisms of Frenklach and co-workers and Leung and Lindstedt; the predictions also suggest that H atom concentrations are in local thermodynamic equilibrium throughout the soot formation region. Using this information, it was found that measured soot surface growth rates could be correlated successfully by predictions based on the hydrogenabstraction/carbon-addition (HACA) mechanisms of both Frenklach and co-workers and Colket and Hall, extending an earlier assessment of these mechanisms for premixed ethylene/air flames to conditions having larger H/C ratios and acetylene concentrations. Measured primary soot particle nucleation rates were somewhat lower than the earlier observations for laminar premixed ethylene/air flames and were significantly lower than corresponding rates in laminar diffusion flames, for reasons that still must be explained.

Soot oxidation was studied experimentally in laminar hydrocarbon/air diffusion flames at atmospheric pressure. Measurements were carried out along the axes of round jets burning in coflowing air considering acetylene, ethylene, propylene and propane as fuels. Measurements were limited to the initial stages of soot oxidation (carbon consumption less than 70%) where soot oxidation mainly occurs at the surface of primary soot particles. The following properties were measured as a function of distance above the burner exit: soot concentrations by deconvoluted laser extinction, soot temperatures by deconvoluted multiline emission, soot structure by thermophoretic sampling and analysis using Transmission Electron Microscopy (TEM), concentrations of stable major gas species (N2, H2O, H2, O2, CO, CO2, CH4, C2H2,C2H4, C2H6, C3H6, and C3H8) by sampling and gas chromatography, concentrations of some radical species (H, OH, O) by the deconvoluted Li/LiOH atomic absorption technique and flow velocities by laser velocimetry. It was found that soot surface oxidation rates are not particularly affected by fuel type for laminar diffusion flames and are described reasonably well by the OH surface oxidation mechanism with a collision efficiency of 0.10, (standard deviation of 0.07) with no significant effect of fuel type in this behavior; these findings are in good agreement with the classical laminar premixed flame measurements of Neoh et al. Finally, direct rates of surface oxidation by O2 were small compared to OH oxidation for present conditions, based on estimated O2 oxidation rates due to Nagle and Strickland-Constable (1962), because soot oxidation was completed near the flame sheet where O2 concentrations were less than 1.2% by volume.

Soot formation was studied within laminar premixed ethylene/air flames (C/O ratios of 0.78-0.98) stabilized on a flat-flame burner operating at atmospheric pressure. Measurements included soot volume fractions by both laser extinction and gravimetric methods, temperatures by multiline emission, soot structure by thermophoretic sampling and transmission electron microscopy, major gas species concentrations by sampling and gas chromatography, concentrations of condensable hydrocarbons by gravimetric sampling. and velocities by laser velocimetry. These data were used to find soot surface growth rates and primary soot particle nucleation rates along the axes of the flames. Present measurements of soot surface growth rates were correlated successfully by predictions based on typical hydrogen-abstraction/carbon-addition (HACA) mechanisms of Frenklach and co-workers and Colket and Hall. These results suavest that reduced soot surface growth rates with increasing residence time seen in the present and other similar flames were mainly caused by reduced rates of surface activation due to reduced H atom concentrations as temperatures decrease as a result of radiative heat losses. Primary soot particle nucleation rates exhibited variations with temperature and acetylene concentrations that were similar to recent observations for diffusion flames; however, nucleation rates in the premixed flames were significantly lower than in, the diffusion flames for reasons that still must be explained. Finally, predictions of yields of major gas species based on mechanisms from both Frenklach and co-workers and Leung and Lindstedt were in good agreement with present measurements and suggest that H atom concentrations (relevant to HACA mechanisms) approximate estimates based on local thermodynamic equilibrium in the present flames.

Extinction and scattering properties at wavelengths of 250-5200 nm were studied for soot emitted from buoyant turbulent diffusion flames in the long residence time regime where soot properties are independent of position in the overfire region and characteristic flame residence times. Flames burning in still air and fueled with gas (acetylene, ethylene, propane, and propylene) and liquid (benzene, toluene, cyclohexane, and n-heptane) hydrocarbon fuels were considered Measured scattering patterns and ratios of total scattering/absorption cross sections were in good agreement with predictions based on the Rayleigh-Debye-Gans (RDG) scattering approximation in the visible. Measured depolarization ratios were roughly correlated by primary particle size parameter, suggesting potential for completing RDG methodology needed to make soot scattering predictions as well as providing a nonintrusive way to measure primary soot particle diameters. Measurements of dimensionless extinction coefficients were in good agreement with earlier measurements for similar soot populations and were independent of fuel type and wavelength except for reduced values as the near ultraviolet was approached. The ratios of the scattering/absorption refractive index functions were independent of fuel type within experimental uncertainties and were in good agreement with earlier measurements. The refractive index function for absorption was similarly independent of fuel type but was larger than earlier reflectometry measurements in the infrared. Ratios of total scattering/absorption cross sections were relatively large in the visible and near infrared, with maximum values as large as 0.9 and with values as large as 0.2 at 2000 nm, suggesting greater potential for scattering from soot particles to affect flame radiation properties than previously thought.

Recent measurements and predictions of the properties of homogeneous (gaseous) laminar and turbulent non-premixed (diffusion) flames are discussed, emphasizing results from both ground- and space-based studies at microgravity conditions. Initial considerations show that effects of buoyancy not only complicate the interpretation of observations of diffusion flames but at times mislead when such results are applied to the non-buoyant diffusion flame conditions of greatest practical interest. This behavior motivates consideration of experiments where effects of buoyancy are minimized; therefore, methods of controlling the intrusion of buoyancy during observations of non-premixed flames are described, considering approaches suitable for both normal laboratory conditions as well as classical microgravity techniques. Studies of laminar flames at low-gravity and microgravity conditions are emphasized in view of the computational tractability of such flames for developing methods of predicting flame structure as well as the relevance of such flames to more practical turbulent flames by exploiting laminar flamelet concepts.

The flame structure and soot-formation (soot nucleation and growth) properties of axisymmetric laminar coflowing jet diffusion flames were studied experimentally. Test conditions involved acetylene-nitrogen jets burning in coflowing air at atmospheric pressure. Measurements were limited to the axes of the flames and included soot concentrations, soot temperatures, soot structure, major gas species concentrations, radical species (H, OH, and O) concentrations, and gas velocities. The results show that as distance increases along the axes of the flames, detectable soot formation begins when significant H concentrations are present, and ends when acetylene concentrations become small. Species potentially associated with soot oxidation--O2, CO2, H2O, O, and OH-are present throughout the soot-formation region so that soot formation and oxidation proceed at the same time. Strong rates of soot growth compared to soot nucleation early in the soot-formation process, combined with increased rates of soot nucleation and oxidation as soot formation proceeds, causes primary soot particle diameters to reach a maximum relatively early in the soot-formation process. Aggregation of primary soot particles proceeds, however, until the final stages of soot oxidation. Present measurements of soot growth (corrected for soot oxidation) in laminar diffusion flames were consistent with earlier measurements of soot growth in laminar premixed flames and exhibited encouraging agreement with existing hydrogen-abstraction/carbon-addition (HACA) soot growth mechanisms in the literature that were developed based on measurements within laminar premixed flames. Measured primary soot particle nucleation rates in the present laminar diffusion flames also were consistent with corresponding rates measured in laminar premixed flames and yielded a crude correlation in terms of acetylene and H concentrations and the temperature.

It is well known that microgravity conditions, by eliminating buoyant flow, enable many combustion phenomena to be observed that are not possible to observe at normal gravity. One example is the spherical diffusion flame surrounding a porous spherical burner. The present paper demonstrates that by superimposing a spherical electrical field on such a flame, the flame remains spherical so that we can study the interaction between the electric field and flame in a one-dimensional fashion. Flames are susceptible to electric fields that are much weaker than the breakdown field of the flame gases owing to the presence of ions generated in the high temperature flame reaction zone. These ions and the electric current of the moving ions, in turn, significantly change the distribution of the electric field. Thus, to understand the interplay between the electric field and the flame is challenging. Numerous experimental studies of the effect of electric fields on flames have been reported. Unfortunately, they were all involved in complex geometries of both the flow field and the electric field, which hinders detailed study of the phenomena. In a one-dimensional domain, however, the electric field, the flow field, the thermal field and the chemical species field are all co-linear. Thus the problem is greatly simplified and becomes more tractable.

Soot formation within hydrocarbon-fueled flames is an important unresolved problem of combustion science for several reasons: soot emissions are responsible for more deaths than any other combustion-generated pollutant, thermal loads due to continuum radiation from soot limit the durability of combustors, thermal radiation from soot is mainly responsible for the growth and spread of unwanted fires, carbon monoxide emissions associated with soot emissions are responsible for most fire deaths, and limited understanding of soot processes in flames is a major impediment to the development of computational combustion. Motivated by these observations, soot processes within laminar premixed and nonpremixed (diffusion) flames are being studied during this investigation. The study is limited to laminar flames due to their experimental and computational tractability, noting the relevance of these results to practical flames through laminar flamelet concepts. Nonbuoyant flames are emphasized because buoyancy affects soot processes in laminar diffusion flames whereas effects of buoyancy are small for most practical flames. This study involves both ground- and space-based experiments, however, the following discussion will be limited to ground-based experiments because no space-based experiments were carried out during the report period. The objective of this work was to complete measurements in both premixed and nonpremixed flames in order to gain a better understanding of the structure of the soot-containing region and processes of soot nucleation and surface growth in these environments, with the latter information to be used to develop reliable ways of predicting soot properties in practical flames. The present discussion is brief, more details about the portions of the investigation considered here can be found in refs. 8-13.

Laminar nonpremixed (diffusion) flames are of interest because they provide model flame systems that are far more tractable for analysis and experiments than practical turbulent flames. In addition, many properties of laminar diffusion flames are directly relevant to turbulent diffusion flames using laminar flamelet concepts. Finally, laminar diffusion flame shapes have been of interest since the classical study of Burke and Schumann because they involve a simple nonintrusive measurement that is convenient for evaluating flame shape predictions. Motivated by these observations, the shapes of round hydrocarbon-fueled laminar jet diffusion flames were considered, emphasizing conditions where effects of buoyancy are small because most practical flames are not buoyant. Earlier studies of shapes of hydrocarbon-fueled nonbuoyant laminar jet diffusion flames considered combustion in still air and have shown that flames at the laminar smoke point are roughly twice as long as corresponding soot-free (blue) flames and have developed simple ways to estimate their shapes. Corresponding studies of hydrocarbon-fueled weakly-buoyant laminar jet diffusion flames in coflowing air have also been reported. These studies were limited to soot-containing flames at laminar smoke point conditions and also developed simple ways to estimate their shapes but the behavior of corresponding soot-free flames has not been addressed. This is unfortunate because ways of selecting flame flow properties to reduce soot concentrations are of great interest; in addition, soot-free flames are fundamentally important because they are much more computationally tractable than corresponding soot-containing flames. Thus, the objectives of the present investigation were to observe the shapes of weakly-buoyant laminar jet diffusion flames at both soot-free and smoke point conditions and to use the results to evaluate simplified flame shape models. The present discussion is brief.

Soot is an important unsolved problem of combustion science because it is present in most hydrocarbon-fueled flames and current understanding of the reactive and physical properties of soot in flame environments is limited. This lack of understanding affects progress toward developing reliable predictions of flame radiation properties, reliable predictions of flame pollutant emission properties and reliable methods of computational combustion, among others. Motivated by these observations, the present investigation extended past studies of soot formation in this laboratory, to consider soot oxidation in laminar diffusion flames using similar methods. Early work showed that O2 was responsible for soot oxidation in high temperature O2-rich environments. Subsequent work in high temperature flame environments having small O2 concentrations, however, showed that soot oxidation rates substantially exceeded estimates based on the classical O2 oxidation rates of Nagle and Strickland-Constable and suggests that radicals such as O and OH might be strong contributors to soot oxidation for such conditions. Neoh et al. subsequently made observations in premixed flames, supported by later work, that showed that OH was responsible for soot oxidation at these conditions with a very reasonable collision efficiency of 0.13. Subsequent studies in diffusion flames, however, were not in agreement with the premixed flame studies: they agreed that OH played a dominant role in soot oxidation in flames, but found collision efficiencies that varied with flame conditions and were not in good agreement with each other or with Neoh et al. One explanation for these discrepancies is that optical scattering and extinction properties were used to infer soot structure properties for the studies that have not been very successful for representing the optical properties of soot. Whatever the source of the problem, however, these differences among observations of soot oxidation in premixed and diffusion flames clearly must be resolved. Motivated by these findings, the present study undertook measurements of soot and flame properties within the soot oxidation region of some typical laminar diffusion flames and exploited the new measurements to identify soot oxidation mechanisms for these conditions. Present considerations were limited to the early stages of soot oxidation (carbon consumption less than 70%) where reactions at the surface of primary soot particles dominate the process, rather than the later stages when particle porosity and internal particle oxidation become important as discussed by Neoh et al.

The shapes (luminous flame boundaries) of round luminous nonbuoyant soot-containing hydrocarbon/air laminar jet diffusion flames at microgravity were found from color video images obtained on orbit in the Space Shuttle Columbia. Test conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K ambient pressures of 35-130 kPa, initial jet diameters of 1.6 and 2.7 mm, and jet exit Reynolds numbers of 45-170. Present test times were 100-200 s and yielded steady axisymmetric flames that were close to the laminar smoke point (including flames both emitting and not emitting soot) with luminous flame lengths of 15-63 mm. The present soot-containing flames had larger luminous flame lengths than earlier ground-based observations having similar burner configurations: 40% larger than the luminous flame lengths of soot-containing low gravity flames observed using an aircraft (KC-135) facility due to reduced effects of accelerative disturbances and unsteadiness; roughly twice as large as the luminous flame lengths of soot-containing normal gravity flames due to the absence of effects of buoyant mixing and roughly twice as large as the luminous flame lengths of soot-free low gravity flames observed using drop tower facilities due to the presence of soot luminosity and possible reduced effects of unsteadiness, Simplified expressions to estimate the luminous flame boundaries of round nonbuoyant laminar jet diffusion flames were obtained from the classical analysis of Spalding; this approach provided successful correlations of flame shapes for both soot-free and soot-containing flames, except when the soot-containing flames were in the opened-tip configuration that is reached at fuel flow rates near and greater than the laminar smoke point fuel flow rate.

Soot oxidation was studied experimentally in laminar hydrocarbon/air diffusion flames at atmospheric pressure. Measurements were carried out along the axes of round jets burning in coflowing air considering acetylene, ethylene, proplyene and propane as fuels. Measurements were limited to the initial stages of soot oxidation (carbon consumption less than 70%) where soot oxidation mainly occurs at the surface of primary soot particles. The following properties were measured as a function of distance above the burner exit: soot concentrations by deconvoluted laser extinction, soot temperatures by deconvoluted multiline emission, soot structure by thermophoretic sampling and analysis using Transmission Electron Microscopy (TEM), concentrations of stable major gas species (N2, H2O, H2, 02, CO, CO2, CH4, C2H2, C2H4, C2H6, C3H6, and C3H8) by sampling and gas chromatography, concentrations of some radical species (H, OH, O) by the deconvoluted Li/LiOH atomic absorption technique and flow velocities by laser velocimetry. It was found that soot surface oxidation rates are not particularly affected by fuel type for laminar diffusion flames and are described reasonably well by the OH surface oxidation mechanism with a collision efficiency of 0.10, (standard deviation of 0.07) with no significant effect of fuel type in this behavior; these findings are in good agreement with the classical laminar premixed flame measurements of Neoh et al. Finally, direct rates of surface oxidation by O2 were small compared to OH oxidation for present conditions, based on estimated O2 oxidation rates due to Nagle and Strickland-Constable, because soot oxidation was completed near the flame sheet where O2 concentrations were less than 1.2% by volume.

The flame structure and soot-formation (soot nucleation and growth) properties of axisymmetric laminar coflowing jet diffusion flames were studied experimentally. Test conditions involved acetylene-nitrogen jets burning in coflowing air at atmospheric pressure. Measurements were limited to the axes of the flames and included soot concentrations, soot temperatures, soot structure, major gas species concentrations, radical species (H, OH, and O) concentrations, and gas velocities. The results show that as distance increases along the axes of the flames, detectable soot formation begins when significant H concentrations are present, and ends when acetylene concentrations become small. Species potentially associated with soot oxidation-O2, CO2, H2O, O, and OH-are present throughout the soot-formation region so that soot formation and oxidation proceed at the same time. Strong rates of soot growth compared to soot nucleation early in the soot-formation process, combined with increased rates of soot nucleation and oxidation as soot formation proceeds, causes primary soot particle diameters to reach a maximum relatively early in the soot-formation process. Aggregation of primary soot particles proceeds, however, until the final stages of soot oxidation. Present measurements of soot growth (corrected for soot oxidation) in laminar diffusion flames were consistent with earlier measurements of soot growth in laminar premixed flames and exhibited encouraging agreement with existing hydrogen-abstraction/carbon-addition (HACA) soot growth mechanisms in the literature that were developed based on measurements within laminar premixed flames. Measured primary soot particle nucleation rates in the present laminar diffusion flames also were consistent with corresponding rates measured in laminar premixed flames and yielded a crude correlation in terms of acetylene and H concentrations and the temperature.

The structure and state relationships of laminar soot-free (permanently-blue) diffusion flames at various strain rates were studied experimentally using an opposed-jet configuration, motivated by the importance of soot-free hydrocarbon-fueled diffusion flames for many practical applications. Measurements of gas velocities, temperatures and compositions were carried out along the stagnation stream line. Flame conditions studied included propylene- and 1,3-butadiene-fueled opposed-jet diffusion flames having a stoichiometric mixture fractions of 0.7 and strain rates of 60-240/s at normal temperature and pressure. It was found that oxygen leakage to fuel-rich conditions and carbon monoxide leakage to fuel-lean conditions both increased as strain rates increased. Furthermore, increased strain rates caused increased fuel concentrations near the flame sheet decreased peak gas temperatures, and decreased concentrations of carbon dioxide and water vapor throughout the flames. State relationships for major gas species and gas temperatures for these flames were found to exist over broad ranges of strain rates. In addition, current measurements, as well as previous measurements and predictions of ethylene-fueled permanently-blue diffusion flames, all having a stoichiometric mixture fraction of 0.7, were combined to establish generalized state relationships for permanently-blue diffusion flames for this stoichiometric mixture fraction. The combined measurements and predictions support relatively universal generalized state relationships for N2, CO2, H2O and fuel over a broad range of strain rates and fuel types. State relationships for O2 in the fuel-rich region, and for CO in the fuel-lean region, however, are functions of strain rate and fuel type. State relationships for H2 and temperature exhibit less universality, mainly due to the increased experimental uncertainties for these variables. The existence of state relationships for soot-free hydrocarbon-fueled diffusion flames provides potential for significant computational simplifications for modeling purposes in many instances, allowing for effects of finite-rate chemistry while avoiding time-consuming computations of Arrhenius expressions.

The laminar smoke-point properties of non-buoyant round laminar jet diffusion flames were studied emphasizing results from long-duration (100-230 s) experiments at microgravity carried out in orbit aboard the space shuttle Columbia. Experimental conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K, pressures of 35-130 kPa, jet exit diameters of 1.6 and 2.7 mm, jet exit velocities of 170-690 mm/s, jet exit Reynolds numbers of 46-172, characteristic flame residence times of 40-302 ms, and luminous flame lengths of 15-63 mm. Contrary to the normal-gravity laminar smoke point, in microgravity, the onset of laminar smoke-point conditions involved two flame configurations: closed-tip flames with soot emissions along the flame axis and open-tip flames with soot emissions from an annular ring about the flame axis. Open-tip flames were observed at large characteristic flame residence times with the onset of soot emissions associated with radiative quenching near the flame tip: nevertheless, unified correlations of laminar smoke-point properties were obtained that included both flame configurations. Flame lengths at laminar smoke-point conditions were well correlated in terms of a corrected fuel flow rate suggested by a simplified analysis of flame shape. The present steady and non-buoyant flames emitted soot more readily than non-buoyant flames in earlier tests using ground-based microgravity facilities and than buoyant flames at normal gravity, as a result of reduced effects of unsteadiness, flame disturbances, and buoyant motion. For example, present measurements of laminar smoke-point flame lengths at comparable conditions were up to 2.3 times shorter than ground-based microgravity measurements and up to 6.4 times shorter than buoyant flame measurements. Finally, present laminar smoke-point flame lengths were roughly inversely proportional to pressure to a degree that is a somewhat smaller than observed during earlier tests both at microgravity (using ground-based facilities) and at normal gravity.

The structure of the soot growth region of laminar premixed methane/oxygen flames (fuel-equivalence ratios of 1.60 - 2.77) was studied both experimentally and computationally. Measurements were carried out in flames stabilized on a flat flame burner operated at standard temperature and pressure, and included velocities by laser velocimetry, soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, major gas species concentrations by sampling and gas chromatography, and hydrogen atom concentrations by the Li/LiOH technique in conjunction with atomic absorption to find the proportion of free lithium in the flames. The measured concentrations of major gas species were in reasonably good agreement with predictions based on the detailed mechanisms of Leung and Lindstedt, and Frenklach and coworkers. The measurements also confirmed predictions of both these mechanisms that H-atom concentrations are in local thermodynamic equilibrium throughout the soot growth region even through the concentrations of major gas species are not. Thus, present findings support recent evaluations of the hydrogen-abstraction/carbon-addition (HACA) soot growth mechanism in similar flames, where the approximation that H-atom concentrations were in local thermodynamic equilibrium was adopted, based on predictions using the two mechanisms, due to the absence of direct H-atom concentration measurements.

Ground-based studies of soot processes in laminar flames proceeded in two phases, considering laminar premixed flames and laminar diffusion flames, in turn. The test arrangement for laminar premixed flames involved round flat flame burners directed vertically upward at atmospheric pressure. The test arrangement for laminar jet diffusion flames involved a round fuel port directed vertically upward with various hydrocarbon fuels burning at atmospheric pressure in air. In both cases, coflow was used to prevent flame oscillations and measurements were limited to the flame axes. The measurements were sufficient to resolve soot nucleation, growth and oxidation rates, as well as the properties of the environment needed to evaluate mechanisms of these processes. The experimental methods used were also designed to maintain capabilities for experimental methods used in corresponding space-based experiments. This section of the report will be limited to consideration of flame structure for both premixed and diffusion flames.

The structure and state relationships of laminar soot-free (permanently blue) ethylene-fueled diffusion flames at various strain rates were studied both experimentally and computationally using an opposed-jet configuration. Measurements of gas velocities, temperatures, and compositions were carried out along the stagnation stream line. Corresponding predictions of flame structure were obtained, based on numerical simulations using several contemporary reaction mechanisms for methane oxidation. Flame conditions studied included ethylene-fueled opposed-jet diffusion flames having stoichiometric mixture fractions of 0.7 with measurements involving strain rates of 60-240/s and predictions involving strain rates of 0-1140/s at normal temperature and pressure. It was found that measured major gas species concentrations and temperature distributions were in reasonably good agreement with predictions using mechanisms due to GRI-Mech and Peters and that effects of preferential diffusion significantly influence flame structure even when reactant mass diffusivities are similar. Oxygen leakage to fuel-rich conditions and carbon monoxide leakage to fuel-lean conditions both increased as strain rates increased. Furthermore, increased strain rates caused increased fuel concentrations near the flame sheet, decreased peak gas temperatures, and decreased concentrations of carbon dioxide and water vapor throughout the flames. State relationships for major gas species and gas temperatures were found to exist over a broad range of strain rates, providing potential for significant computational simplifications for modeling purposes in some instances.

Laminar diffusion flames are of interest because they provide model flame systems that are far more tractable for analysis and experiments than more practical turbulent diffusion flames. Certainly, understanding flame processes within laminar diffusion flames must precede understanding these processes in more complex turbulent diffusion flames. In addition, many properties of laminar diffusion flames are directly relevant to turbulent diffusion flames using laminar flamelet concepts. Laminar jet diffusion flame shapes (luminous flame boundaries) have been of particular interest since the classical study of Burke and Schumann because they are a simple nonintrusive measurement that is convenient for evaluating flame structure predictions. Thus, consideration of laminar flame shapes is undertaken in the following, emphasizing conditions where effects of gravity are small, due to the importance of such conditions to practical applications. Another class of interesting properties of laminar diffusion flames are their laminar soot and smoke point properties (i.e., the flame length, fuel flow rate, characteristic residence time, etc., at the onset of soot appearance in the flame (the soot point) and the onset of soot emissions from the flame (the smoke point)). These are useful observable soot properties of nonpremixed flames because they provide a convenient means to rate several aspects of flame sooting properties: the relative propensity of various fuels to produce soot in flames; the relative effects of fuel structure, fuel dilution, flame temperature and ambient pressure on the soot appearance and emission properties of flames; the relative levels of continuum radiation from soot in flames; and effects of the intrusion of gravity (or buoyant motion) on emissions of soot from flames. An important motivation to define conditions for soot emissions is that observations of laminar jet diffusion flames in critical environments, e.g., space shuttle and space station facilities, cannot involve soot emitting flames in order to ensure that test chamber windows used for experimental observations are not blocked by soot deposits, thereby compromising unusually valuable experimental results. Another important motivation to define conditions where soot is present in diffusion flames is that flame chemistry, transport and radiation properties are vastly simplified when soot is absent, making such flames far more tractable for detailed numerical simulations than corresponding soot-containing flames. Motivated by these observations, the objectives of this phase of the investigation were as follows: (1) Observe flame-sheet shapes (the location of the reaction zone near phi=1) of nonluminous (soot free) laminar jet diffusion flames in both still and coflowing air and use these results to develop simplified models of flame-sheet shapes for these conditions; (2) Observe luminous flame boundaries of luminous (soot-containing) laminar jet diffusion flames in both still and coflowing air and use these results to develop simplified models of luminous flame boundaries for these conditions. In order to fix ideas here, maximum luminous flame boundaries at the laminar smoke point conditions were sought, i.e., luminous flame boundaries at the laminar smoke point; (3) Observe effects of coflow on laminar soot- and smoke-point conditions because coflow has been proposed as a means to control soot emissions and minimize the presence of soot in diffusion flames.

The shapes (flame-sheet and luminous-flame boundaries) of steady nonbuoyant round hydrocarbon-fueled laminar-jet diffusion flames in still and coflowing air were studied both experimentally and theoretically. Flame-sheet shapes were measured from photographs using a CH optical filter to distinguish flame-sheet boundaries in the presence of blue C02 and OH emissions and yellow continuum radiation from soot. Present experimental conditions included acetylene-, methane-, propane-, and ethylene-fueled flames having initial reactant temperatures of 300 K, ambient pressures of 4-50 kPa, jet exit Reynolds number of 3-54, initial air/fuel velocity ratios of 0-9 and luminous flame lengths of 5-55 mm; earlier measurements for propylene- and 1,3-butadiene-fueled flames for similar conditions were considered as well. Nonbuoyant flames in still air were observed at micro-gravity conditions; essentially nonbuoyant flames in coflowing air were observed at small pressures to control effects of buoyancy. Predictions of luminous flame boundaries from soot luminosity were limited to laminar smoke-point conditions, whereas predictions of flame-sheet boundaries ranged from soot-free to smoke-point conditions. Flame-shape predictions were based on simplified analyses using the boundary layer approximations along with empirical parameters to distinguish flame-sheet and luminous-flame (at the laminar smoke point) boundaries. The comparison between measurements and predictions was remarkably good and showed that both flame-sheet and luminous-flame lengths are primarily controlled by fuel flow rates with lengths in coflowing air approaching 2/3 lengths in still air as coflowing air velocities are increased. Finally, luminous flame lengths at laminar smoke-point conditions were roughly twice as long as flame-sheet lengths at comparable conditions due to the presence of luminous soot particles in the fuel-lean region of the flames.

The shapes (luminous flame boundaries) of steady nonbuoyant round luminous hydrocarbon-fueled laminar-jet diffusion flames in coflowing air were studied both experimentally and theoretically. Flame shapes were measured from photographs of flames burning at low pressures in order to minimize the effects of buoyancy. Test conditions involved acetylene-, propylene. and 1,3-butadiene-fueled flames having initial reactant temperatures of 300 K, ambient pressures of 19-50 kPa, jet-exit Reynolds numbers of 18-121, and initial air/fuel velocity ratios of 0.22-32.45 to yield luminous flame lengths of 21-198 mm. The present flames were close to the laminar smoke point but were not soot emitting. Simple expressions to estimate the shapes of nonbuoyant laminar-jet diffusion flames in coflow were found by extending an earlier analysis of Mahalingam et al. These formulas provided a good correlation of present measurements except near the burner exit where self-similar approximations used in the simplified analysis are no longer appropriate.

The structure and soot properties of round, soot-emitting, nonbuoyant, laminar jet diffusion flames are described, based on long-duration (175-230/s) experiments at microgravity carried out on orbit In the Space Shuttle Columbia. Experiments] conditions included ethylene-fueled flames burning in still air at nominal pressures of 50 and 100 kPa and an ambient temperature of 300 K with luminous Annie lengths of 49-64 mm. Measurements included luminous flame shapes using color video imaging, soot concentration (volume fraction) distributions using deconvoluted laser extinction imaging, soot temperature distributions using deconvoluted multiline emission imaging, gas temperature distributions at fuel-lean (plume) conditions using thermocouple probes, not structure distributions using thermophoretic sampling and analysis by transmission electron microscopy, and flame radiation using a radiometer. The present flames were larger, and emitted soot men readily, than comparable observed during ground-based microgravity experiments due to closer approach to steady conditions resulting from the longer test times and the reduced gravitational disturbances of the space-based experiments.

Three major soot reaction processes are needed to predict soot properties in flame environments: soot growth, or the formation of soot on soot nuclei and soot particles; soot oxidation, or the reaction of soot with oxidizing species to yield the combustion products of soot oxidation; and soot nucleation, or the formation of soot nuclei from soot precursors having large molecular weights (generally thought to be large and particularly stable PAH molecules in flame environments, called stabilomers). These processes are addressed in the following, considering soot growth, oxidation and nucleation, in turn, by exploiting the soot and flame structure results for premixed and diffusion flames already discussed in Section 2.

The structure of the soot growth region of laminar premixed methane/oxygen flames (fuel-equivalence ratios of 1.60-2.77) was studied both experimentally and computationally. Measurements were carried out in flames stabilized on a flat flame burner operated at standard temperature and pressure, and included velocities by laser velocimetry, soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, major gas species concentrations by sampling and gas chromatography, and hydrogen atom concentrations by the Li/LiOH technique in conjunction with atomic absorption to find the proportion of free lithium in the flames. The measured concentrations of major gas species were in reasonably good agreement with predictions based on the detailed mechanisms of Leung and Lindstedt, and Frenklach and coworkers. The measurements also confirmed predictions of both these mechanisms that H-atom concentrations are in local thermodynamic equilibrium throughout the soot growth region even through the concentrations of major gas species are not. Thus, present findings support recent evaluations of the hydrogen-abstraction/carbon-addition (HACA) soot growth mechanism in similar flames, where the approximation that H-atom concentrations were in local thermodynamic equilibrium was adopted, based on predictions using the two mechanisms, due to the absence of direct H-atom concentration measurements.

Effects of flow (hydrodynamic) properties on limiting conditions for soot-free laminar non-premixed hydrocarbon/air flames (called laminar soot-point conditions) were studied, emphasizing non-buoyant laminar coflowing jet diffusion flames. Effects of air/fuel-stream velocity ratios were of particular interest; therefore, the experiments were carried out at reduced pressures to minimize effects of flow acceleration due to the intrusion of buoyancy. Test conditions included reactant temperatures of 300 K; ambient pressures of 3.7-49 8 kPa; methane-, acetylene-, ethylene-, propane-, and methane-fueled flames burning in coflowing air with fuel-port diameters of 1.7, 3.2, and 6.4 mm, fuel jet Reynolds numbers of 18-121; air coflow velocities of 0-6 m/s; and air/fuel-stream velocity ratios of 0.003-70. Measurements included laminar soot-point flame lengths, laminar soot-point fuel flow rates, and laminar liftoff conditions. The measurements show that laminar soot-point flame lengths and fuel flow rates can be increased, broadening the range of fuel flow rates where the flames remain soot free, by increasing air/fuel-stream velocity ratios. The mechanism of this effect involves the magnitude and direction of flow velocities relative to the flame sheet where increased air/fuel-stream velocity ratios cause progressive reduction of flame residence times in the fuel-rich soot-formation region. The range of soot-free conditions is limited by both liftoff, particularly at low pressures, and the intrusion of effects of buoyancy on effective air/fuel-stream velocity ratios, particularly at high pressures. Effective correlations of laminar soot- and smoke-point flame lengths were also found in terms of a corrected fuel flow rate parameter, based on simplified analysis of laminar jet diffusion flame structure. The results show that laminar smoke-point flame lengths in coflowing air environments are roughly twice as long as soot-free (blue) flames under comparable conditions due to the presence of luminous soot particles under fuel-lean conditions when smoke-point conditions are approached. This is very similar to earlier findings concerning differences between laminar smoke- and sootpoint flame lengths in still environments.

The laminar smoke-point properties of non-buoyant round laminar jet diffusion flames were studied emphasizing results from long-duration (100-230 s) experiments at microgravity carried out in orbit aboard the space shuttle Columbia. Experimental conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K, pressures of 35-130 kPa, jet exit diameters of 1.6 and 2.7 mm, jet exit velocities of 170-690 mm/s, jet exit Reynolds numbers of 46-172, characteristic flame residence times of 40-302 ms, and luminous flame lengths of 15-63 mm. Contrary to the normal-gravity laminar smoke point, in microgravity the onset of laminar smoke-point conditions involved two flame configurations: closed-tip flames with soot emissions along the flame axis and open-tip flames with soot emissions from an annular ring about the flame axis. Open-tip flames were observed at large characteristic flame residence times with the onset of soot emissions associated with radiative quenching near the flame tip: nevertheless, unified correlations of laminar smoke-point properties were obtained that included both flame configurations. Flame lengths at laminar smoke-point conditions were well correlated in terms of a corrected fuel flow rate suggested by a simplified analysis of flame shape. The present steady and nonbuoyant flames emitted soot more readily than non-buoyant flames in earlier tests using ground-based microgravity facilities and than buoyant flames at normal gravity, as a result of reduced effects of unsteadiness, flame disturbances, and buoyant motion. For example, present measurements of laminar smokepoint flame lengths at comparable conditions were up to 2.3 times shorter than ground-based microgravity measurements and up to 6.4 times shorter than buoyant flame measurements. Finally, present laminar smoke-point flame lengths were roughly inversely proportional to pressure to a degree that is a somewhat smaller than observed during earlier tests both at microgravity (using ground-based facilities) and at normal gravity

Soot formation within hydrocarbon-fueled flames is an important unresolved problem of combustion science for several reasons: soot emissions are responsible for more deaths than any other combustion pollutant, thermal loads due to continuum radiation from soot limit the durability of combustors, thermal radiation from soot is mainly responsible for the growth and spread of unwanted fires, carbon monoxide associated with soot emissions is responsible for most fire deaths, and limited understanding of soot processes is a major impediment to the development of computational combustion. Thus, soot processes within laminar nonpremixed (diffusion) flames are being studied, emphasizing space-based experiments at microgravity. The study is limited to laminar flames due to their experimental and computational tractability, noting the relevance of these results to practical flames through laminar flamelet concepts. The microgravity environment is emphasized because buoyancy affects soot processes in laminar diffusion flames whereas effects of buoyancy are small for most practical flames. Results discussed here were obtained from experiments carried out on two flights of the Space Shuttle Columbia. After a brief discussion of experimental methods, results found thus far are described, including soot concentration measurements, laminar flame shapes, laminar smoke points and flame structure. The present discussion is brief.

Nonpremixed (diffusion) flames are attractive for practical applications because they avoid the stability, autoignition, flashback, etc. problems of premixed flames. Unfortunately, soot formation in practical hydrocarbon-fueled diffusion flames reduces their attractiveness due to widely-recognized public health and combustor durability problems of soot emissions. For example, more deaths are attributed to the emission of soot (15,000-60,000 deaths annually in the U.S. alone) than any other combustion-generated pollutant. In addition, continuum radiation from soot-containing flames is the principle heat load to combustor components and is mainly responsible for engine durability problems of aircraft and gas turbine engines. As a result, there is considerable interest in controlling both soot concentrations within flames and soot emissions from flames. Thus, the objective of the present investigation is to study ways to control soot formation in diffusion flames by manipulating the mixing process between the fuel and oxidant streams. In order to prevent the intrusion of gravity from masking flow properties that reduce soot formation in practical flames (where effects of gravity are small), methods developed during past work will be exploited to minimize effects of buoyant motion.

Soot processes within hydrocarbon-fueled flames affect emissions of pollutant soot, thermal loads on combustors, hazards of unwanted fires and capabilities for computational combustion. In view of these observations, the present study is considering processes of soot formation in both burner-stabilized and freely-propagating laminar premixed flames. These flames are being studied in order to simplify the interpretation of measurements and to enhance computational tractability compared to the diffusion flame environments of greatest interest for soot processes. In addition, earlier studies of soot formation in laminar premixed flames used approximations of soot optical and structure properties that have not been effective during recent evaluations, as well as questionable estimates of flow residence times). The objective of present work was to exploit methods of avoiding these difficulties developed for laminar diffusion flames to study soot growth in laminar premixed flames. The following description of these studies is brief.

The shapes (luminous flame boundaries) of round luminous nonbuoyant soot-containing hydrocarbon/air laminar jet diffusion flames at microgravity were found from color video images obtained on orbit in the Space Shuttle Columbia. Test conditions included ethylene- and propane-fueled flames burning in still air at an ambient temperature of 300 K, ambient pressures of 35-130 kPa, initial jet diameters of 1.6 and 2.7 mm, and jet exit Reynolds numbers of 45-170. Present test times were 100-200 s and yielded steady axisymmetric flames that were close to the laminar smoke point (including flames both emitting and not emitting soot) with luminous flame lengths of 15-63 mm. The present soot-containing flames had larger luminous flame lengths than earlier ground-based observations having similar burner configurations: 40% larger than the luminous flame lengths of soot-containing low gravity flames observed using an aircraft (KC-135) facility due to reduced effects of accelerative disturbances and unsteadiness; roughly twice as large as the luminous flame lengths of soot-containing normal gravity flames due to the absence of effects of buoyant mixing and roughly twice as large as the luminous flame lengths of soot-free low gravity flames observed using drop tower facilities due to the presence of soot luminosity and possible reduced effects of unsteadiness. Simplified expressions to estimate the luminous flame boundaries of round nonbuoyant laminar jet diffusion flames were obtained from the classical analysis of Spalding (1979); this approach provided Successful Correlations of flame shapes for both soot-free and soot-containing flames, except when the soot-containing flames were in the opened-tip configuration that is reached at fuel flow rates near and greater than the laminar smoke point fuel flow rate.

Laminar diffusion flames are of interest as model flame systems that are more tractable for analysis and experiments than practical turbulent diffusion flames. Certainly understanding laminar flames must precede understanding more complex turbulent flames while man'y laminar diffusion flame properties are directly relevant to turbulent diffusion flames using laminar flamelet concepts. Laminar diffusion flame shapes have been of interest since the classical study of Burke and Schumann because they involve a simple nonintrusive measurement that is convenient for evaluating flame structure predictions. Motivated by these observations, the shapes of laminar flames were considered during the present investigation. The present study was limited to nonbuoyant flames because most practical flames are not buoyant. Effects of buoyancy were minimized by observing flames having large flow velocities at small pressures. Present methods were based on the study of the shapes of nonbu,3yant round laminar jet diffusion flames of Lin et al. where it was found that a simple analysis due to Spalding yielded good predictions of the flame shapes reported by Urban et al. and Sunderland et al.

Soot is a dominant feature of hydrocarbon/air flames, affecting their reaction mechanisms and structure. As a result, soot processes affect capabilities for computational combustion as well as predictions of flame radiation and pollution emissions. Motivated by these observations, the present investigation extended past work on soot growth in laminar premixed flames, seeking to evaluate model predictions of flame structure. Xu et al. report direct measurements of soot residence times, soot concentrations, soot structure, gas temperatures and gas compositions for premixed flames similar to those studied by Harris and Weiner and Ramer et al. respectively. It was found that predictions of major stable gas species concentrations based on mechanisms of Leung and Lindstedt and Frenklach and coworkers, were in good agreement with the measurements. The results were also used to evaluate the hydrogen-abstraction/carbon-addition (HACA) soot growth mechanisms of Frenklach and coworkers and Colket and Hall. It was found that these mechanisms were effective using quite reasonable correlations for the steric factors appearing in the theories. The successful evaluation of the HACA mechanism of soot growth in Refs. 1 and 2 is encouraging but one aspect of this evaluation is a concern. In particular, H-atom concentrations play a crucial role in the HACA mechanism and it was necessary to estimate these concentrations because they were not measured directly. These estimates were made assuming local thermodynamic equilibrium between H, and H based on measured temperatures and H2 concentrations and the equilibrium constant data of Kee et al.. This approach was justified by the flame structure predictions; nevertheless, direct evaluation of equilibrium estimates of H-atom concentrations in the soot growth regions of laminar premixed flames is needed to provide more convincing proof of this behavior. Thus, the objective of the present investigation was to complete new measurements of the structure of the soot growth region of laminar premixed flames and to use these results to evaluate whether H and H2 are in thermodynamic equilibrium and to extend the earlier evaluation of predictions of concentrations of major gas species.

Flame structure and soot formation were studied within soot-containing laminar premixed mc1hane/oxygen flames at atmospheric pressure. The following measurements were made: soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, soot structure by thermophoretic sampling and transmission electron microscope (TEM), major gas species concentrations by sampling and gas chromatography, and gas velocities by laser velocimetry. Present measurements of gas species concentrations were in reasonably good agreement with earlier measurements due to Ramer et al. as well as predictions based on the detailed mechanisms of Frenklach and co-workers and Leung and Lindstedt: the predictions also suggest that H atom concentrations are in local thermodynamic equilibrium throughout the soot formation region. Using this information, it was found that measured soot surface growth rates could be correlated successfully by predictions based on the hydrogen-abstraction/carbon-addition (HACA) mechanisms of both Frenklach and co-workers and Colket and Hall, extending an earlier assessment of these mechanisms for premixed ethylene/air flames to conditions having larger H/C ratios and acetylene concentrations. Measured primary soot particle nucleation rates were somewhat lower than the earlier observations for laminar premixed ethylene/air flames and were significantly lower than corresponding rates in laminar diffusion flames. for reasons that still must be explained.

Soot processes within hydrocarbon-fueled flames affect particle emissions from combustion processes, thermal loads of combustor components, hazards of unwanted fires, and capabilities for computational combustion. Thus, soot processes within laminar nonpremixed (diffusion) and premixed flames are being studied, using both space-based (flight) experiments at MicroGravity (MG) and supporting ground-based experiments at Normal Gravity (NG). The study is limited to laminar flames due to their experimental and computational tractability, noting the relevance of these results to practical turbulent flames based on laminar flamelet concepts. Unfortunately, buoyancy affects soot processes in laminar diffusion flames while effects of buoyancy are small for most practical flames; therefore, present observations of laminar diffusion flames involve either particular flame conditions where effects of buoyancy are small during ground-based experiments at ng or truly nonbuoyant flames during planned flight experiments at mg. Laminar premixed flames are also being considered during ground-based experiments at ng because soot processes are easier to interpret and less affected by buoyancy in laminar premixed flames than in laminar diffusion flames.

Soot formation within hydrocarbon-fueled flames is an important unresolved problem of combustion science. Thus, the present study is considering soot formation in freely-propagating laminar premixed flames, exploiting the microgravity environment to simplify measurements at the high-pressure conditions of interest for many practical applications. The findings of the investigation are relevant to reducing emissions of soot and continuum radiation from combustion processes, to improving terrestrial and spacecraft fire safety, and to developing methods of computational combustion, among others. Laminar premixed flames are attractive for studying soot formation because they are simple one-dimensional flows that are computationally tractable for detailed numerical simulations. Nevertheless, studying soot-containing burner-stabilized laminar premixed flames is problematical: spatial resolution and residence times are limited at the pressures of interest for practical applications, flame structure is sensitive to minor burner construction details so that experimental reproducibility is not very good, consistent burner behavior over the lengthy test programs needed to measure soot formation properties is hard to achieve, and burners have poor durability. Fortunately, many of these problems are mitigated for soot-containing, freely-propagating laminar premixed flames. The present investigation seeks to extend work in this laboratory for various soot processes in flames by observing soot formation in freely-propagating laminar premixed flames. Measurements are being made at both Normal Gravity (NG) and MicroGravity (MG), using a short-drop free-fall facility to provide MG conditions.

Effects of flow (hydrodynamic properties on the presence of soot in hydrocarbon-fueled laminar opposed-jet diffusion flames were studied experimentally at atmospheric pressure, emphasizing effects of velocities normal to the Rom sheet. These velocities were varied for conditions corresponding to combustion in air by transferring nitrogen from the oxidizer stream to the fuel stream which increases the stoichiometric mixture fraction of the flame and causes the stagnation plane of the flow to shift toward the fuel-rich side of the flame sheet. Fuels considered included acetylene, ethylene, ethane, propylene, propane, and 1-3 butadiene. Present measurements consisted of the critical strain rates for the flames to contain soot (the soot extinction limit) and for the flames to extinguish (the flame extinction limit) It was found that increasing the stoichiometric mixture fraction causes a progressive reduction of the critical strain rates for both flame and soot extinction; however, their ratio increases, and even becomes unbounded in most instances to yield a permanently-blue-flame regime. The results suggest that soot formation in nonpremixed flames can be controlled by varying velocities normal to the flame sheet. Nevertheless, definitive conclusions along these lines require evaluation of effects of corresponding variations of fuel and oxygen concentrations on soot formation when velocities normal to the flame sheet are changed by varying stoichiometric mixture fractions for laminar opposed-jet diffusion flames.

Soot processes within hydrocarbon fueled flames are important because they affect the durability and performance of propulsion systems, the hazards of unwanted fires, the pollutant and particulate emissions from combustion processes, and the potential for developing computational combustion. Motivated by these observations, the present investigation is studying soot processes in laminar diffusion and premixed flames in order to better understand the soot and thermal radiation emissions of luminous flames. Laminar flames are being studied due to their experimental and computational tractability, noting the relevance of such results to practical turbulent flames through the laminar flamelet concept. Weakly-buoyant and nonbuoyant laminar diffusion flames are being considered because buoyancy affects soot processes in flames while most practical flames involve negligible effects of buoyancy. Thus, low-pressure weakly-buoyant flames are being observed during ground-based experiments while near atmospheric pressure nonbuoyant flames will be observed during space flight experiments at microgravity. Finally, premixed laminar flames also are being considered in order to observe some aspects of soot formation for simpler flame conditions than diffusion flames. The main emphasis of current work has been on measurements of soot nucleation and growth in laminar diffusion and premixed flames.