Oxygen dissociation at close-packed Pt terraces, Pt steps, and Ag-covered Pt steps studied with density functional theory
Апстракт
Using density functional theory we have characterized O(2) dissociation on flat and stepped Pt(111) surfaces. The reactivity of the steps is significantly higher than that of the flat terraces. Inclusion of Ag monoatomic chains along the Pt steps modifies the reactivity of the Pt steps towards that of the flat Pt terraces. Our investigations reveal the reaction energetics and the geometries for the molecular precursor states (MPS), transition states (TS) and final states of the dissociating oxygen. Both the MPS and TS geometries on stepped Pt involve oxygen species at the top of the step with no oxygen atoms diffusing onto the lower terrace. We further find that the Ag chains mainly modify the adsorption and reaction bond strengths while they leave the MPS and TS geometries essentially unchanged. The high reactivity of the Pt steps is explained in terms of the coordinative unsaturation of the Pt step atoms which cause a highlying valence 5d-electron system. (C) 2002 Elsevier Science B....V. All rights reserved.
Кључне речи:
platinum / silver / oxygen / density functional calculations / stepped single crystal surfaces / single crystal surfaces / surface chemical reactionИзвор:
Surface Science, 2002, 515, 1, 235-244
DOI: 10.1016/S0039-6028(02)01908-8
ISSN: 0039-6028
WoS: 000177735900027
Scopus: 2-s2.0-0036683369
Колекције
Институција/група
VinčaTY - JOUR AU - Šljivančanin, Željko AU - Hammer, B PY - 2002 UR - https://vinar.vin.bg.ac.rs/handle/123456789/2544 AB - Using density functional theory we have characterized O(2) dissociation on flat and stepped Pt(111) surfaces. The reactivity of the steps is significantly higher than that of the flat terraces. Inclusion of Ag monoatomic chains along the Pt steps modifies the reactivity of the Pt steps towards that of the flat Pt terraces. Our investigations reveal the reaction energetics and the geometries for the molecular precursor states (MPS), transition states (TS) and final states of the dissociating oxygen. Both the MPS and TS geometries on stepped Pt involve oxygen species at the top of the step with no oxygen atoms diffusing onto the lower terrace. We further find that the Ag chains mainly modify the adsorption and reaction bond strengths while they leave the MPS and TS geometries essentially unchanged. The high reactivity of the Pt steps is explained in terms of the coordinative unsaturation of the Pt step atoms which cause a highlying valence 5d-electron system. (C) 2002 Elsevier Science B.V. All rights reserved. T2 - Surface Science T1 - Oxygen dissociation at close-packed Pt terraces, Pt steps, and Ag-covered Pt steps studied with density functional theory VL - 515 IS - 1 SP - 235 EP - 244 DO - 10.1016/S0039-6028(02)01908-8 ER -
@article{ author = "Šljivančanin, Željko and Hammer, B", year = "2002", abstract = "Using density functional theory we have characterized O(2) dissociation on flat and stepped Pt(111) surfaces. The reactivity of the steps is significantly higher than that of the flat terraces. Inclusion of Ag monoatomic chains along the Pt steps modifies the reactivity of the Pt steps towards that of the flat Pt terraces. Our investigations reveal the reaction energetics and the geometries for the molecular precursor states (MPS), transition states (TS) and final states of the dissociating oxygen. Both the MPS and TS geometries on stepped Pt involve oxygen species at the top of the step with no oxygen atoms diffusing onto the lower terrace. We further find that the Ag chains mainly modify the adsorption and reaction bond strengths while they leave the MPS and TS geometries essentially unchanged. The high reactivity of the Pt steps is explained in terms of the coordinative unsaturation of the Pt step atoms which cause a highlying valence 5d-electron system. (C) 2002 Elsevier Science B.V. All rights reserved.", journal = "Surface Science", title = "Oxygen dissociation at close-packed Pt terraces, Pt steps, and Ag-covered Pt steps studied with density functional theory", volume = "515", number = "1", pages = "235-244", doi = "10.1016/S0039-6028(02)01908-8" }
Šljivančanin, Ž.,& Hammer, B.. (2002). Oxygen dissociation at close-packed Pt terraces, Pt steps, and Ag-covered Pt steps studied with density functional theory. in Surface Science, 515(1), 235-244. https://doi.org/10.1016/S0039-6028(02)01908-8
Šljivančanin Ž, Hammer B. Oxygen dissociation at close-packed Pt terraces, Pt steps, and Ag-covered Pt steps studied with density functional theory. in Surface Science. 2002;515(1):235-244. doi:10.1016/S0039-6028(02)01908-8 .
Šljivančanin, Željko, Hammer, B, "Oxygen dissociation at close-packed Pt terraces, Pt steps, and Ag-covered Pt steps studied with density functional theory" in Surface Science, 515, no. 1 (2002):235-244, https://doi.org/10.1016/S0039-6028(02)01908-8 . .