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

Patricia Rubert-Nason, Manos Mavrikakis, Christos T. Maravelias, Lars C. Grabow, Lorenz T. Biegler

Research output: Contribution to journalArticlepeer-review

15 Scopus citations

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 languageEnglish (US)
Pages (from-to)1336-1346
Number of pages11
JournalAIChE Journal
Volume60
Issue number4
DOIs
StatePublished - Apr 2014
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Biotechnology
  • Environmental Engineering
  • Chemical Engineering(all)

Keywords

  • Density functional theory
  • Nonlinear programming
  • Parallel computing
  • Parameter estimation

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