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Abstract
A series of perfectly stirred reactor (PSR) calculations has been performed that allow the comparison of numerical predictions for sooting trends in PSRs with those observed in experiments. A detailed chemical kinetics model for soot production is employed that has been extensively tested for laminar flames. The chemical kinetics model is used without any adjustments. The PSR code Aurora that is a CHEMKIN III application has been modified considerably to incorporate the method of moments. Gas-phase and surface reactions are rigorously coupled in the model. Predicted sooting characteristics are consistent with behavior observed experimentally for premixed laminar flames and well-stirred reactors. Specifically, soot volume fraction exhibited the same qualitative behavior with equivalence ratio, temperature, and pressure as observed for flames. Concentration profile shapes were consistent with profile shapes measured for flames as well. The model also predicts soot threshold values and the relationship of soot volume fraction with temperature and equivalence ratio that has been observed experimentally for well-stirred reactors. Under the conditions of the present investigation, soot formation dynamics was dominated by nucleation. The temperature dependence of surface reaction rates revealed the importance of the HACA mechanism (H-abstraction-C2H2 addition reaction sequence) in surface growth. Under PSR conditions, coupling the gasphase and surface chemistry is significant with the degree of coupling increasing with pressure.
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