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

Katrin Blondal; Jelena Jelic; Emily Mazeau; Felix Studt; Richard H. West; C. Franklin Goldsmith

doi:10.1021/acs.iecr.9b01464

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

Katrin Blondal, Jelena Jelic, Emily Mazeau, Felix Studt, Richard H. West, C. Franklin Goldsmith

Research output: Contribution to journal › Article › peer-review

28 Scopus citations

Abstract

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.

Original language	English
Pages (from-to)	17682-17691
Number of pages	10
Journal	Industrial and Engineering Chemistry Research
Volume	58
Issue number	38
DOIs	https://doi.org/10.1021/acs.iecr.9b01464
State	Published - Sep 25 2019
Externally published	Yes

Funding

We gratefully acknowledge support from the U.S. Department of Energy, through the Computational Chemical Sciences program within the Basic Energy Science division, with Dr. Mark Pedersen as the program manager. J.J. and F.S. acknowledge support from the state of Baden-Wüttemberg through bwHPC (bwunicluster and JUSTUS, RV bw17D011).

Funders	Funder number
U.S. Department of Energy
state of Baden-Wüttemberg

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10.1021/acs.iecr.9b01464

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

abstract = "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.",

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AU - Studt, Felix

AU - West, Richard H.

AU - Goldsmith, C. Franklin

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AB - 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.

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

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