dc.creator | Lustemberg, Pablo German | |
dc.creator | Plessow, Philipp N. | |
dc.creator | Wang, Yuemin | |
dc.creator | Yang, Chengwu | |
dc.creator | Nefedov, Alexei | |
dc.creator | Studt, Felix | |
dc.creator | Wöll, Christof | |
dc.creator | Ganduglia Pirovano, Maria Veronica | |
dc.date.accessioned | 2021-10-18T17:05:38Z | |
dc.date.accessioned | 2022-10-15T07:10:44Z | |
dc.date.available | 2021-10-18T17:05:38Z | |
dc.date.available | 2022-10-15T07:10:44Z | |
dc.date.created | 2021-10-18T17:05:38Z | |
dc.date.issued | 2020-12 | |
dc.identifier | 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 | 0031-9007 | |
dc.identifier | http://hdl.handle.net/11336/144120 | |
dc.identifier | CONICET Digital | |
dc.identifier | CONICET | |
dc.identifier.uri | https://repositorioslatinoamericanos.uchile.cl/handle/2250/4358973 | |
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.language | eng | |
dc.publisher | American Physical Society | |
dc.relation | info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1103/PhysRevLett.125.256101 | |
dc.relation | info:eu-repo/semantics/altIdentifier/url/https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.125.256101 | |
dc.relation | info:eu-repo/semantics/altIdentifier/url/https://arxiv.org/abs/2011.06419 | |
dc.rights | https://creativecommons.org/licenses/by-nc-sa/2.5/ar/ | |
dc.rights | info:eu-repo/semantics/openAccess | |
dc.subject | CO frequency shift | |
dc.subject | PBE+U | |
dc.subject | Hybrid calculation | |
dc.subject | IRRAS spectra | |
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 | |