Detailed modeling of PAH and soot formation in a laminar premixed benzene/oxygen/argon low-pressure flame

Abstract

Combustion-generated polycyclic aromatic hydrocarbons (PAH) and soot particles are of significant environmental concern whereas controlled combustion is of increasing interest for the synthesis of carbonaceous nanostructures such as fullerenic material. Improved understanding of chemical and physical processes involved in PAH and soot formation is required to correlate operating conditions with emission characteristics. A detailed kinetic model describing the formation and consumption of PAH and soot in fuel-rich hydrocarbon combustion has been developed. Using a sectional approach, large PAH and carbonaceous particles with diameters of up to ≈70 nm are defined as classes (BINs) covering given mass ranges. Numbers of carbon and hydrogen atoms corresponding to their average masses are assigned to each BIN, accounting for a decrease in H/C ratios with increasing particle size. The model has been successfully tested for a rich premixed benzene/oxygen/argon flame ( ϕ = 2.4, 10% argon, v = 25 cm s −1, 5.33 kPa). Model predictions are compared with published experimental data including mole fraction profiles of individual PAH and concentration as well as number density profiles of soot. Reactions of PAH radicals with PAH and between PAH radicals were found to be the dominant pathway to soot nuclei. Surface growth contributes ≈75% to the final particle mass, and reaction of acetylene with particle radicals is the major growth pathway. Surface growth reactions are involved in PAH depletion in the postflame zone. Particle coagulation involving BINs and BIN radicals significantly contributes to the formation of progressively larger particles whereas oxidation by OH plays a non-negligible role in their depletion.