Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 21, Pages 6916-6920Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201900565
Keywords
CO oxidation; CO2 chemisorption; site specificity; surface dynamics
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Funding
- U.S. National Science Foundation [CHE-1462109, CHE-1665077]
- Alexander-von-Humboldt Foundation
- Deutsche Forschungsgemeinschaft (DFG)
- Ministerium fur Wissenschaft und Kultur (MWK) Niedersachsen
- Volkswagenstiftung [INST 186/952-1]
- National Natural Science Foundation of China [21603200]
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The post-transition-state dynamics in CO oxidation on Pt surfaces are investigated using DFT-based abinitio molecular dynamics simulations. While the initial CO2 formed on a terrace site on Pt(111) desorbs directly, it is temporarily trapped in a chemisorption well on a Pt(332) step site. These two reaction channels thus produce CO2 with hyperthermal and thermal velocities with drastically different angular distributions, in agreement with recent experiments (Nature, 2018, 558, 280-283). The chemisorbed CO2 is formed by electron transfer from the metal to the adsorbate, resulting in a bent geometry. While chemisorbed CO2 on Pt(111) is unstable, it is stable by 0.2eV on a Pt(332) step site. This helps explain why newly formed CO2 produced at step sites desorbs with far lower translational energies than those formed at terraces. This work shows that steps and other defects could be potentially important in finding optimal conditions for the chemical activation and dissociation of CO2.
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