Computer-Generated Kinetics for Coupled Heterogeneous/Homogeneous Systems: A Case Study in Catalytic Combustion of Methane on Platinum

The
automatic microkinetic mechanism generator for heterogeneous
catalysis, RMG-Cat, has been extensively updated. Density functional
theory calculations were performed for 69 adsorbates on Pt(111), and
the resulting thermodynamic properties were added to RMG-Cat. The
thermo database is significantly more accurate; it includes nitrogen-containing
adsorbates for the first time as well as better capabilities for predicting
the thermochemistry of novel adsorbates. Additionally, RMG-Cat can
now simultaneously pursue a mechanism expansion both on the surface
and in the gas phase. This heterogeneous/homogeneously coupled capability
is tested on the catalytic combustion of methane on platinum. The
results confirm that under some conditions the catalyst is capable
of inducing thermal ignition in the gas phase.