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

Keywords: diffusion flame, high pressure, soot formation.

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 fou