Structure sensitivity in oxide catalysis: First-principles kinetic Monte Carlo simulations for CO oxidation at RuO2(111)
Abstract
We present a density-functional theory based kinetic Monte Carlo study of CO oxidation at the (111) facet of RuO2. We compare the detailed insight into elementary processes, steady-state surface coverages, and catalytic activity to equivalent published simulation data for the frequently studied RuO2(110) facet. Qualitative differences are identified in virtually every aspect ranging from binding energetics over lateral interactions to the interplay of elementary processes at the different active sites. Nevertheless, particularly at technologically relevant elevated temperatures, near-ambient pressures and near-stoichiometric feeds both facets exhibit almost identical catalytic activity. As a result, these findings challenge the traditional definition of structure sensitivity based on macroscopically observable turnover frequencies and prompt scrutiny of the applicability of structure sensitivity classifications developed for metals to oxide catalysis.
- Authors:
-
[1];
- Technische Univ. Munchen, Garching (Germany)
- Technische Univ. Munchen, Garching (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1263412
- Report Number(s):
- SLAC-PUB-16626
Journal ID: ISSN 0021-9606; JCPSA6; arXiv:1508.03697
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 143; Journal Issue: 20; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS AND COMPUTING; MATSCI; adsorption; surface reactions; surface oxidation; catalysis; atom surface interactions
Citation Formats
Wang, Tongyu, and Reuter, Karsten. Structure sensitivity in oxide catalysis: First-principles kinetic Monte Carlo simulations for CO oxidation at RuO2(111). United States: N. p., 2015.
Web. doi:10.1063/1.4936354.
Wang, Tongyu, & Reuter, Karsten. Structure sensitivity in oxide catalysis: First-principles kinetic Monte Carlo simulations for CO oxidation at RuO2(111). United States. https://doi.org/10.1063/1.4936354
Wang, Tongyu, and Reuter, Karsten. Tue .
"Structure sensitivity in oxide catalysis: First-principles kinetic Monte Carlo simulations for CO oxidation at RuO2(111)". United States. https://doi.org/10.1063/1.4936354. https://www.osti.gov/servlets/purl/1263412.
@article{osti_1263412,
title = {Structure sensitivity in oxide catalysis: First-principles kinetic Monte Carlo simulations for CO oxidation at RuO2(111)},
author = {Wang, Tongyu and Reuter, Karsten},
abstractNote = {We present a density-functional theory based kinetic Monte Carlo study of CO oxidation at the (111) facet of RuO2. We compare the detailed insight into elementary processes, steady-state surface coverages, and catalytic activity to equivalent published simulation data for the frequently studied RuO2(110) facet. Qualitative differences are identified in virtually every aspect ranging from binding energetics over lateral interactions to the interplay of elementary processes at the different active sites. Nevertheless, particularly at technologically relevant elevated temperatures, near-ambient pressures and near-stoichiometric feeds both facets exhibit almost identical catalytic activity. As a result, these findings challenge the traditional definition of structure sensitivity based on macroscopically observable turnover frequencies and prompt scrutiny of the applicability of structure sensitivity classifications developed for metals to oxide catalysis.},
doi = {10.1063/1.4936354},
journal = {Journal of Chemical Physics},
number = 20,
volume = 143,
place = {United States},
year = {Tue Nov 24 00:00:00 EST 2015},
month = {Tue Nov 24 00:00:00 EST 2015}
}
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