High density adsorbed oxygen on Rh(111) and enhanced routes to metallic oxidation using atomic oxygen

Gibson, K. D.; Viste, M.; Sanchez, Errol; Sibener, S. J.

doi:10.1063/1.477877

Cited by 43 publications

(56 citation statements)

References 27 publications

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“…The 'oval' protrusions are observed in the Cu(110)-c(6Â2)-8O phase [48] and the 'honeycomb' protrusions composed of the 'dumbbells' are observed from the Cu(111)-O surface at higher temperature [49]. All the (Ag, Cu, Ni, Pt)(110) [53,54] and Ru(0001)-O surfaces [55,56]. STM studies should be able to reveal inherently common features caused by oxygen adsorption from all these many specific forms.…”

Section: Alternation Of Atomic Valenciesmentioning

confidence: 92%

“…The former presents zigzag strips, while the latter gives a regular array of depressions and protrusions. One may attribute such a difference to the Á values in Figs [53]. Common to all other O-chemisorbed systems, the first layer spacing expands and the second contracts.…”

Section: à2mentioning

confidence: 99%

“…Logan et al [351] obtained a set of TDS data from the O-Rh(111) surface in the temperature range of 850-1050 K, higher than those reported by Peterlinz and Sibener who used lower oxygen doses. Using the time-of-flight spectroscopy, Gibson et al [53,193] found that the velocity distribution of the desorbed oxygen follows approximately the MaxwellBoltzmann description. They relate such characteristics to a 'hot' desorption, that is, the temperature of the desorbing gas is higher than the surface temperature.…”

Section: Identity Similaritymentioning

confidence: 99%

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Oxidation electronics: bond–band–barrier correlation and its applications

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Section: Alternation Of Atomic Valenciesmentioning

confidence: 92%

Section: à2mentioning

confidence: 99%

Section: Identity Similaritymentioning

confidence: 99%

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Oxidation electronics: bond–band–barrier correlation and its applications

Sun

2003

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219

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“…The first of these steps, i.e. the chemisorption of oxygen on Rh single crystal surfaces, has been the subject of intensive experimental and theoretical research, [7][8][9][10] but only few experimental studies have addressed the ensuing formation of sub-surface oxygen, [11][12][13][14][15][16][17] . In one of these studies it could recently be shown 16 that exposure of the Rh(111) surface to O 2 at moderatly elevated temperatures (∼ 470 K) leads to the formation of sub-surface oxygen species, and there is evidence that at least ∼ 0.9 monolayer (ML) of O is adsorbed on the surface before sub-surface sites are occupied.…”

Section: Introductionmentioning

confidence: 99%

Stability of subsurface oxygen at Rh(111)

2002

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Using density-functional theory (DFT) we investigate the incorporation of oxygen directly below the Rh(111) surface. We show that oxygen incorporation will only commence after nearly completion of a dense O adlayer (θtot ≈ 1.0 monolayer) with O in the fcc on-surface sites. The experimentally suggested octahedral sub-surface site occupancy, inducing a site-switch of the onsurface species from fcc to hcp sites, is indeed found to be a rather low energy structure. Our results indicate that at even higher coverages oxygen incorporation is followed by oxygen agglomeration in two-dimensional sub-surface islands directly below the first metal layer. Inside these islands, the metastable hcp/octahedral (on-surface/sub-surface) site combination will undergo a barrierless displacement, introducing a stacking fault of the first metal layer with respect to the underlying substrate and leading to a stable fcc/tetrahedral site occupation. We suggest that these elementary steps, namely, oxygen incorporation, aggregation into sub-surface islands and destabilization of the metal surface may be more general and precede the formation of a surface oxide at close-packed late transition metal surfaces.

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“…oxygen incorporation will only start after completion of a full O(1 × 1) overlayer, in nice agreement with experimental findings. 26,27 Close to Θ = 1 ML the energy differences are very small in the case of Rh though. Hence, a fi-…”

Section: B Oxygen Accommodation Below the Top Metal Layermentioning

confidence: 99%

Nanometer and Subnanometer Thin Oxide Films at Surfaces of Late Transition Metals

Reuter

2007

Nanocatalysis

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If metal surfaces are exposed to sufficiently oxygen-rich environments, oxides start to form. Important steps in this process are the dissociative adsorption of oxygen at the surface, the incorporation of O atoms into the surface, the formation of a thin oxidic overlayer and the growth of the once formed oxide film. For the oxidation process of late transition metals (TM), recent experimental and theoretical studies provided a quite intriguing atomic-scale insight: The formed initial oxidic overlayers are not merely few atomic-layer thin versions of the known bulk oxides, but can exhibit structural and electronic properties that are quite distinct to the surfaces of both the corresponding bulk metals and bulk oxides. If such nanometer or even sub-nanometer surface oxide films are stabilized in applications, new functionalities not scalable from the known bulk materials could correspondingly arise. This can be particularly important for oxidation catalysis, where technologically relevant gas phase conditions are typically quite oxygen-rich. In such environments surface oxides may even form naturally in the induction period, and actuate then the reactive steady-state behavior that has traditionally been ascribed to the metal substrates. Corresponding aspects are reviewed by focusing on recent progress in the modeling and understanding of the oxidation behavior of late TMs, using particularly the late 4d series from Ru to Ag to discuss trends.

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High density adsorbed oxygen on Rh(111) and enhanced routes to metallic oxidation using atomic oxygen

Abstract: Physical and chemical properties of high density atomic oxygen overlayers under ultrahigh vacuum conditions: (1×1)-O/Rh (111)

Cited by 43 publications

References 27 publications

Oxidation electronics: bond–band–barrier correlation and its applications

Oxidation electronics: bond–band–barrier correlation and its applications

Stability of subsurface oxygen at Rh(111)

Nanometer and Subnanometer Thin Oxide Films at Surfaces of Late Transition Metals

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