Simulation of automotive NH3 oxidation catalysts based on pre-computed rate data from mechanistic surface kinetics

This paper demonstrates how pre-computed rate data can be used to enable the numerically efficient implementation of mechanistic kinetics in a reactor model for an automotive ammonia slip catalyst. In a pre-processing step the source terms for the gas species are mapped as a function of gas composition and temperature. From this map (80,000 data points), a spline interpolation function is constructed. The spline function approximates the numerical steady state solution of the kinetic model with an average error of less than 1%. Application of the rate mapping procedure results in a speedup of about two orders of magnitude. The spline approximation is implemented in a 2-dimensional model of a monolith reactor channel that includes diffusion in the washcoat layer. Depending on the channel diameter and the washcoat thickness, diffusion limitations in the open channel and in the washcoat can have a significant influence on the NH3 conversion. Surprisingly, the selectivity for the products N2, N2O and NO is not sensitive to diffusion effects in the gas phase or in the washcoat.