Automatic Mechanism Generation Involving Kinetics of Surface Reactions with Bidentate Adsorbates

14 September 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


New features have been added to the open-source Reaction Mechanism Generator (RMG) that enhance its ability to handle multidentate adsorbates. New reaction families and improved thermophysical estimation routines have been added, based upon ab-initio data from 26 reactions involving CxOyHz bidentate adsorbates with two heavy atoms on Pt(111). Non-oxidative dehydrogenation of ethane over Pt(111) is used as a case study to demonstrate the effectiveness of these new features. RMG not only discovered the pathways from prior literature, but it also uncovered new elementary steps involving abstraction reactions. Various mono- and bimetallic catalysts for this process were screened using linear scaling relations within RMG, where a unique mechanism is generated for each catalyst. These results are consistent with prior literature trends, but they add additional insight into the rate determining steps across the periodic table. With these additions, RMG can now explore more intricate reaction mechanisms of heterogeneously catalyzed processes for the conversion of larger molecules, which will be particularly important in fuel synthesis.


Heterogeneous catalysis
Mechanism generation
Microkinetic modeling

Supplementary materials

Supporting Information
Details on transition state theory and BEP relations, electronic structure results, and additional simulation results


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