Advanced solution methods for microkinetic models of catalytic reactions: A methanol synthesis case study. Issue 4 (31st December 2013)

• Record Type: Journal Article
• Authors: Rubert‐Nason, Patricia; Mavrikakis, Manos; Maravelias, Christos T.; Grabow, Lars C.; Biegler, Lorenz T.
• Is Part Of: AIChE journal. Volume 60:Issue 4(2014:Apr.)
• Page Start: 1336
• Page End: 1346
• Publication Date: 2013-12-31
• Subjects: Chemical engineering -- Periodicals; Génie chimique -- Périodiques; 660.28
• DOI: 10.1002/aic.14322
• Languages: English
• ISSNs: 0001-1541

Abstract

<abstract abstract-type="main"> <title> <x xml:space="preserve">Abstract</x> </title> <p>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. © 2013 American Institute of Chemical Engineers <italic>AIChE J</italic>, 60: 1336–1346, 2014</p> </abstract>