Parameter estimation by Density Functional Theory for a lattice-gas model of Br and Cl chemisorption on Ag (100)

Juwono, Tjipto; Hamad, Ibrahim Abou; Rikvold, Per Arne; Wang, Sanwu

doi:10.1016/j.jelechem.2011.04.029

Cited by 10 publications

(2 citation statements)

References 25 publications

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“…Adsorbate–adsorbate interactions on electrode surfaces have been determined in the past by comparison of lattice gas models with experimental adsorption isotherms . For example, this approach provided interaction parameters for Cl and Br on Ag(100), which were in agreement with the results of DFT calculations for various discrete coverages. , Here, the isotherms for Br could be fully explained by long-range electrostatic repulsion, whereas for Cl additional short-range attractive interactions were necessary. More direct experimental data were again obtained from atomic-scale in situ Video-STM observations of S ad , Pb ad , and CH 3 S ad on Cu(100) and Ag(100) surfaces, embedded in a c (2 × 2) lattice of coadsorbed halide. ,,, By a quantitative analysis of local adsorbate configurations in the videos, the effective interactions between these adsorbates as well as the diffusion barriers in the neighborhood of another adsorbate could be determined.…”

Section: Adsorbate Dynamics On Electrode Surfacesmentioning

confidence: 99%

Toward an Atomic-Scale Understanding of Electrochemical Interface Structure and Dynamics

2019

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For the knowledged-based development of electrochemical processes, a better fundamental understanding of the interfaces between electrodes and electrolytes is necessary. This requires insight into the interface structure and dynamics on the atomic-scale, including that of the liquid electrolyte in the near-surface region, i.e., in the inner and outer part of the electrochemical double layer. This perspective describes current studies of simple and well-defined electrochemical interfaces by first-principles electronic structure calculations and in situ structure-sensitive methods. It is shown that these experimental and theoretical studies are now approaching a level, where they can operate on the same footing, making direct comparison of the obtained results feasible. Using selected examples, progress in clarifying the structure and dynamics of the double layer, of adsorbed species on electrode surfaces, and of initial steps in electrochemical phase formation processes is discussed.

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Section: Adsorbate Dynamics On Electrode Surfacesmentioning

confidence: 99%

Toward an Atomic-Scale Understanding of Electrochemical Interface Structure and Dynamics

2019

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“…This quadratic dependence has previously been observed in lattice gas model Hamiltonians that include pair-wise interactions between adsorbed species. 38 Depending upon the adsorbate/ surface pair, several physical mechanisms have been shown in literature to be responsible for pairwise inter-adsorbate interactions. We consider four mechanisms here.…”

Section: Mechanisms Responsible For Inter-adsorbate Interactionsmentioning

confidence: 99%

Quantifying the origin of inter-adsorbate interactions on reactive surfaces for catalyst screening and design

Krishnamoorthy

Yildiz

2015

Phys. Chem. Chem. Phys.

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The adsorption energy of reactant molecules and reaction intermediates is one of the key descriptors of catalytic activity of surfaces and is commonly used as a metric in screening materials for design of heterogeneous catalysts. The efficacy of such screening schemes depends on the accuracy of calculated adsorption energies under reaction conditions. These adsorption energies can depend strongly on interactions between adsorbed molecules in the adlayer. However, these interactions are typically not accounted for in screening procedures that use DFT-based zero-coverage adsorption energies. Identifying the physical mechanisms behind these interactions is essential to model realistic catalyst surfaces under reaction conditions and to understand the dependence of adsorption energies on reaction parameters like surface strain and composition. This article describes a method to quantitatively resolve the observed inter-adsorbate interactions into various direct adsorbate-adsorbate interactions (i.e. Coulombic and steric) and surface-mediated interactions (i.e. adsorbate-induced surface relaxation and change in electronic structure) by combining density functional theory and cluster-expansion calculations of coverage-dependent adsorption energies. The approach is implemented on a model catalyst surface of FeS2(100) reacting with H2S molecules. We find that the adsorption energy of H2S molecules can be affected by over 0.55 eV by the repulsive inter-adsorbate interactions caused primarily by the adsorbate-induced changes to the electronic structure of the FeS2 surface. These interactions also show a strong monotonic dependence on surface strain, being three times stronger on compressively strained surfaces than on surfaces under tensile strain. The large magnitude of inter-adsorbate interactions as well as their strong dependence on lattice strain demonstrate the need for using coverage-dependent adsorption energies for more accurate screening, for example for strained catalytic systems like core-shell and overlayer structures.

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Multilayer adsorption of C 2 H 4 and CF 4 on graphite: Grand Canonical Monte Carlo simulation

Abdelatif

Drir

2016

Chemical Physics

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Parameter estimation by Density Functional Theory for a lattice-gas model of Br and Cl chemisorption on Ag (100)

Abstract: false2016-03-16T23:02:09

Cited by 10 publications

References 25 publications

Toward an Atomic-Scale Understanding of Electrochemical Interface Structure and Dynamics

Toward an Atomic-Scale Understanding of Electrochemical Interface Structure and Dynamics

Quantifying the origin of inter-adsorbate interactions on reactive surfaces for catalyst screening and design

Multilayer adsorption of C 2 H 4 and CF 4 on graphite: Grand Canonical Monte Carlo simulation

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