Interaction of oxygen with a Ru(OO1) surface

Surnev, L.; Rangelov, G.; Bliznakov, G.

doi:10.1016/0039-6028(85)90430-3

Cited by 98 publications

(48 citation statements)

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“…(1)] and is calculated here using transfer matrix techniques. Regarding the sticking coefficient, we note that dissociation is not activated initially, but at (local) coverages of u * 0.5, it is hindered by an energy barrier [6,12]. Under these circumstances, to obtain the coverage and temperature dependence of the sticking coefficient ab initio would be a significant undertaking.…”

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confidence: 99%

“…On doing this, we present a consistent first-principles-based approach for calculation of the thermodynamic and kinetic properties of an adsorbate, such as heats of adsorption, temperature programmed desorption (TPD) spectra, and the surface phase diagram. We have chosen the system of oxygen at Ru(0001) for which detailed structural [4][5][6][7][8][9], thermodynamic [10], and kinetic data [11,12] exist. We will show that, with the present approach, a realistic description of these physical properties is indeed feasible.…”

mentioning

confidence: 99%

“…Under these circumstances, to obtain the coverage and temperature dependence of the sticking coefficient ab initio would be a significant undertaking. Therefore we use an analytic expression which well approximates the measured behavior in the temperature regime of desorption [12]: The sticking coefficient drops approximately as ͑2͞3 2 u͒ 2 and for coverages above 2͞3 it remains very small up to a monolayer. The actual equation we use is S dis ͑u͒ S 0 exp͓2͑u͞s͒ 2 ͔, with S 0 0.27 and s 0.3.…”

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First-Principles Theory of Surface Thermodynamics and Kinetics

et al. 1999

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Understanding the complex behavior of particles at surfaces requires detailed knowledge of both macroscopic and microscopic processes that take place; also certain phenomena depend critically on temperature and gas pressure. To link these processes we combine state-of-the-art microscopic, and macroscopic phenomenological, theories. We apply our theory to the O͞Ru(0001) system and calculate thermal desorption spectra, heat of adsorption, and the surface phase diagram. The agreement with experiment provides validity for our approach which thus identifies the way for a predictive simulation of surface thermodynamics and kinetics. PACS numbers: 68.45.Da, 82.65.Dp, 82.65.My The study of the physical and chemical processes that take place at gas-surface interfaces have long been an area of intense research. This interest is both fundamental as well as driven by the possible discovery of important technological applications, e.g., in the field of heterogeneous catalysis, corrosion, etc. [1,2]. With respect to the field of the theory of adsorption of gases on solid surfaces, advancement in recent years has developed in two distinct, albeit complimentary, directions: (i) electronic structure calculations, at best done by density-functional theory (DFT), to determine the geometries, energetics, and vibrational properties of adsorbate covered surfaces, and (ii) phenomenological models, both for the thermodynamics and the kinetics [3] of the adsorbate. If one can assume that the geometry of the solid surface does not change dramatically and that adsorption occurs at well defined sites, one frequently employs a lattice gas model. A number of parameters enter this type of model, such as the binding energies and vibrational frequencies of a single adparticle in the various adsorption sites, and their mutual lateral interactions with adparticles in close-by sites. Traditionally, these parameters are adjusted in the theory in order to fit a variety of experimental data such as phase diagrams, heats of adsorption, infrared spectra, and thermal desorption data, etc. Such an approach, while useful, is clearly not necessarily predictive in nature, nor the parameters unique, and may not capture the physics of the microscopic processes that are behind the "best-fit" adjusted "effective" parameters.In this Letter, with the aim to improve upon this approach, we combine state-of-the-art procedures of (i) microscopic theories, i.e., DFT electronic structure calculations and (ii) macroscopic phenomenological approaches, i.e., lattice gas and rate equations, and Monte Carlo schemes. On doing this, we present a consistent first-principles-based approach for calculation of the thermodynamic and kinetic properties of an adsorbate, such as heats of adsorption, temperature programmed desorption (TPD) spectra, and the surface phase diagram. We have chosen the system of oxygen at Ru(0001) for which detailed structural [4-9], thermodynamic [10], and kinetic data [11,12] exist. We will show that, with the present approach, a realistic description...

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First-Principles Theory of Surface Thermodynamics and Kinetics

et al. 1999

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“…Particularly the sharp drop after reaching a coverage of about 0.5 ML at Ru(0001) and Rh(111) leads to an apparent uptake saturation, when employing low gas exposures as typical for many early ultra-high vacuum (UHV) surface science studies. 12,13,14 DFT calculations predicted, however, that much higher coverages should still be possible 15,16,17 , and Fig. 2 shows such data for some selected adsorbate configurations spanning the whole coverage range up to 1 ML 18 .…”

Section: A Formation Of Adlayersmentioning

confidence: 97%

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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“…For the direct process, the dissociation occurs just on the first initial collision of the gas molecule with the surface. Although it is the most common dissociative chemisorption process of gases such as H2 and N2 on metal surfaces, 212 O2 chemisorption on Ru undergoes via a precursor-mediated mechanism, 216 the indirect process. For the indirect process, the dissociation is preceded by the formation of a surface precursor that either diffuses freely across the surface to find a favorable dissociation site, or its mobility is limited to the place where the precursor is initially formed.…”

Section: Introductionmentioning

confidence: 99%

Growth and thermal oxidation of Ru and ZrO2 thin films as oxidation protective layers

Ribera¹

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Interaction of oxygen with a Ru(OO1) surface

Cited by 98 publications

References 15 publications

First-Principles Theory of Surface Thermodynamics and Kinetics

First-Principles Theory of Surface Thermodynamics and Kinetics

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

Growth and thermal oxidation of Ru and ZrO2 thin films as oxidation protective layers

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