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Title: Evidence for the Active Phase of Heterogeneous Catalysts through In Situ Reaction Product Imaging and Multiscale Modeling

We use multiscale modeling to analyze laser-induced fluorescence (LIF) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density functional theory-based kinetic Monte Carlo simulations of the active catalyst into fluid-dynamical simulations of the mass transport inside the reactor chamber, we calculate the reaction product concentration directly above the catalyst surface. Comparing corresponding data calculated for different surface models against the measured LIF signals, we can discriminate the one that predominantly actuates the experimentally measured catalytic activity. For the probed CO oxidation reaction conditions, the experimental activity is due to pristine Pd(100) possibly coexisting with other (oxidic) domains on the surface.
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Publication Date:
OSTI Identifier:
Report Number(s):
Journal ID: ISSN 2155-5435; arXiv:1506.05542
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Catalysis; Journal Volume: 5; Journal Issue: 8
American Chemical Society (ACS)
Research Org:
SLAC National Accelerator Laboratory (SLAC)
Sponsoring Org:
US DOE Office of Science (DOE SC)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY catalytic activity; density-functional theory; in-situ spectroscopy; laser-induced fluorescence; multiscale modeling; oxidation reaction over Pd(100)