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dc.contributor.author
Lustemberg, Pablo German
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Plessow, Philipp N.
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Wang, Yuemin
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Yang, Chengwu
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Nefedov, Alexei
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Studt, Felix
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Wöll, Christof
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Ganduglia Pirovano, Maria Veronica
dc.date.available
2021-10-18T17:05:38Z
dc.date.issued
2020-12
dc.identifier.citation
Lustemberg, Pablo German; Plessow, Philipp N.; Wang, Yuemin; Yang, Chengwu; Nefedov, Alexei; et al.; Vibrational Frequencies of Cerium-Oxide-Bound CO: A Challenge for Conventional DFT Methods; American Physical Society; Physical Review Letters; 125; 25; 12-2020; 1-7
dc.identifier.issn
0031-9007
dc.identifier.uri
http://hdl.handle.net/11336/144120
dc.description.abstract
In ceria-based catalysis, the shape of the catalyst particle, which determines the exposed crystal facets, profoundly affects its reactivity. The vibrational frequency of adsorbed carbon monoxide (CO) can be used as a sensitive probe to identify the exposed surface facets, provided reference data on well-defined single crystal surfaces together with a definitive theoretical assignment exist. We investigate the adsorption of CO on the CeO2(110) and (111) surfaces and show that the commonly applied DFT(PBE)+U method does not provide reliable CO vibrational frequencies by comparing with state-of-the-art infrared spectroscopy experiments for monocrystalline CeO2 surfaces. Good agreement requires the hybrid DFT approach with the HSE06 functional. The failure of conventional density-functional theory (DFT) is explained in terms of its inability to accurately describe the facet- A nd configuration-specific donation and backdonation effects that control the changes in the Câ"O bond length upon CO adsorption and the CO force constant. Our findings thus provide a theoretical basis for the detailed interpretation of experiments and open up the path to characterize more complex scenarios, including oxygen vacancies and metal adatoms.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
American Physical Society
dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
CO frequency shift
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PBE+U
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Hybrid calculation
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IRRAS spectra
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Otras Ciencias Químicas
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Ciencias Químicas
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CIENCIAS NATURALES Y EXACTAS
dc.title
Vibrational Frequencies of Cerium-Oxide-Bound CO: A Challenge for Conventional DFT Methods
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2021-09-06T21:00:48Z
dc.journal.volume
125
dc.journal.number
25
dc.journal.pagination
1-7
dc.journal.pais
Estados Unidos
dc.journal.ciudad
Washington D. C.
dc.description.fil
Fil: Lustemberg, Pablo German. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina. Consejo Superior de Investigaciones Científicas; España
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Fil: Plessow, Philipp N.. Karlsruher Institut fur Technologie; Alemania
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Fil: Wang, Yuemin. Karlsruher Institut fur Technologie; Alemania
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Fil: Yang, Chengwu. Karlsruher Institut fur Technologie; Alemania
dc.description.fil
Fil: Nefedov, Alexei. Karlsruher Institut fur Technologie; Alemania
dc.description.fil
Fil: Studt, Felix. Karlsruher Institut fur Technologie; Alemania
dc.description.fil
Fil: Wöll, Christof. Karlsruher Institut fur Technologie; Alemania
dc.description.fil
Fil: Ganduglia Pirovano, Maria Veronica. Karlsruher Institut fur Technologie; Alemania
dc.journal.title
Physical Review Letters
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1103/PhysRevLett.125.256101
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.125.256101
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://arxiv.org/abs/2011.06419
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