Computer generated microkinetics: a case study for methane dry reforming
1School of Engineering, Brown University,
Providence, RI-02912 – USA
2Department of Chemical Engineering, Northeastern University,
Boston, MA-02115, USA
Talk C5-02 CHE006 presented at the 10th International Conference on Chemical Kinetics, 24th May 2017, University of Illinois at Chicago, Chicago, IL, USA.
Accurate prediction of the reactivity and selectivity of catalytic materials under industrially relevant conditions requires a detailed list of elementary surface reactions, or a microkinetic mechanism. In this talk, we present recently developed software that can generate microkinetic mechanisms for heterogeneous catalysis automatically. For a given catalyst, the user provides the initial conditions (e.g. temperature, pressure, and gas-phase composition), and the computer automatically determines which reactions are important, obtains parameterizations of the thermodynamic properties and rate coefficients, and solves the governing equations – without subsequent human intervention.
The software is based upon the open-source software Reaction Mechanism Generator (Gao et al., 2016). We have added three new reaction families to RMG-Cat: adsorption, surface dissociation, and surface abstraction. The new code includes a novel method for predicting the thermodynamic properties of adsorbates, principally the temperature-dependent free energy.
As a proof-of-concept, RMG-Cat was tested on methane steam reforming, dry reforming, and partial oxidation on Ni (111). The results were compared to a literature mechanism (Delgado et al., 2015). Additionally, RMG-Cat successfully developed a mechanism for the catalytic combustion of methanol, even though methanol is not part of the Deutschmann mechanism.
