A detailed chemistry model is necessary to simulate the effects of variations in fuel composition on soot emissions. In this work, we have developed a detailed chemistry model for the soot formation and oxidation chemistry, with a focus on the surface kinetics of the soot-particle. The model has been compared to a unique set of soot particle-size data measured in flames for several single-component fuels. Fuel components used in the experiments represent the chemical classes found in jet, gasoline, and diesel fuels, including n-heptane (representative of n-alkanes) and toluene (aromatic). Measurements were taken in burner-stabilized stagnation-flame (BSSF) experiments, which can be simulated well using the 1-dimensional BSSF flame model in CHEMKIN-PRO. Soot volume fraction and particle size distributions are modeled using the sectional method option for Particle Tracking, within CHEMKIN-PRO software. The well-characterized flow of the BSSF experiments allows the modeling to focus on the kinetics. Validated detailed reaction mechanisms for fuel combustion and PAH production, combined with the new soot surface-kinetics mechanism, were used in the simulations. Simulation results were compared to measurements for both particle size distributions and total soot volume fraction. Observed effects of fuel, temperature, pressure, equivalence ratio and residence time on the soot size distribution shape and soot quantity were reproduced by the model.
The chemistry in the soot surface model includes particle nucleation, growth through the HACA (hydrogen-abstraction/carbon-addition) and PAH-condensation (polycyclic aromatic hydrocarbons) pathways, as well as soot-oxidation pathways. In addition to soot chemistry, the physics of particle coagulation and aggregation were included in the model. The results demonstrate the ability of well-validated chemistry to predict both dramatic and subtle effects related to soot mass and soot particle size.