Abstract
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.
Original language | English (US) |
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Pages (from-to) | 1336-1346 |
Number of pages | 11 |
Journal | AIChE Journal |
Volume | 60 |
Issue number | 4 |
DOIs | |
State | Published - Apr 2014 |
Externally published | Yes |
All Science Journal Classification (ASJC) codes
- Biotechnology
- Environmental Engineering
- General Chemical Engineering
Keywords
- Density functional theory
- Nonlinear programming
- Parallel computing
- Parameter estimation