Abstract
Reliable prediction of char conversion, heat release, and particle temperature during heterogeneous char oxidation relies upon quantitative calculation of the CO2/CO production ratio. This ratio depends strongly on the surface temperature, but also on the local partial pressure of oxygen and thus becomes more important in simulations of oxy-fuel or pressurized combustion systems. Existing semi-empirical intrinsic kinetic models of char combustion have been calibrated against the temperature-dependence of the CO2/CO production ratio, but have neglected the effect of the local oxygen concentration. In this study we employ steady-state analysis to demonstrate the limitations of the existing 3-step semi-global kinetics models and to show the necessity of using a 5-step model to adequately capture the temperature- and oxygen-dependence of the CO2/CO production ratio. A suitable 5-step heterogeneous reaction mechanism is developed and its rate parameters fit to match CO2/CO production data, global reaction orders, and activation energies reported in the literature. The model predictions are interrogated for a broad range of conditions characteristic of pressurized, oxy-fuel, and conventional high-temperature char combustion, for which essentially no experimental information on the CO2/CO production ratio is available. The results suggest that the CO2/CO production ratio may be considerably lower than that estimated with existing power-law correlations for oxygen partial pressures less than 10kPa and surface temperatures higher than 1600K. To assist with implementation of the mechanistic CO2/CO production ratio results, an analytical procedure for calculating the CO2/CO production ratio is presented.
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