Microkinetic models, combined with experimentally measured reaction rates and orders, play a key role in elucidating detailed reaction mechanisms in heterogeneous catalysis and have typically been solved as systems of ordinary differential equations. In this work, we demonstrate a new approach to fitting those models to experimental data. For the specific example treated here, by reformulating a typical microkinetic model for a continuous stirred tank reactor to a system of nonlinear equations, we achieved a 1000-fold increase in solution speed. The reduced computational cost allows a more systematic search of the parameter space, leading to better fits to the available experimental data. We applied this approach to the problem of methanol synthesis by CO/CO2 hydrogenation over a supported-Cu catalyst, an important catalytic reaction with a large industrial interest and potential for large-scale CO2 chemical fixation.
Advanced Solution Methods for Microkinetic Models of Catalytic Reactions: A Methanol Synthesis Case Study.
Rubert-Nason P, M Mavrikakis, CT Maravelias, LC Grabow, and LT Biegler.2014."Advanced Solution Methods for Microkinetic Models of Catalytic Reactions: A Methanol Synthesis Case Study."AIChE Journal 60(4):13361346. doi:10.1002/aic.14322