Advanced solution methods for microkinetic models of catalytic reactions: A methanol synthesis case study

作者：Rubert Nason Patricia; Mavrikakis Manos^*; Maravelias Christos T; Grabow Lars C; Biegler Lorenz T

来源：AICHE Journal, 2014, 60(4): 1336-1346.

DOI：10.1002/aic.14322

• nonlinear programming
• parallel computing
• density functional theory
• parameter estimation

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.

• 出版日期2014-4