Frozen thermal fluctuations in adsorbate-induced step restructuring

Zhang, Xueqing; Offermans, W. K.; Santen, Rutger A. van; Jansen, Apj Tonek; Scheibe, A.; Lins, U.; Imbihl, R.

doi:10.1103/physrevb.82.113401

Cited by 4 publications

(2 citation statements)

References 27 publications

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“…They also presented a model of first-principles atomistic thermodynamics for oxidation catalysis . A DFT coupled thermodynamic model, studying the H 2 -induced reconstruction of supported Pt clusters, was presented by Sautet et al By using kinetic Monte Carlo (kMC), coupled with DFT, we reported the ammonia coverage dependent meandering of Pt(111) …”

Section: Introductionmentioning

confidence: 99%

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Carbon-Induced Surface Transformations of Cobalt

2014

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A reactive force field has been developed that is used in molecular dynamics (MD) studies of the surface transformation of the cobalt (0001) surface induced by an overlayer of adsorbed carbon atoms. Significant surface reconstruction is observed with movement of the Co atoms upward and part of the C atoms to positions below the surface. In a particular C ad atom coverage regime step edge type surface sites are formed, which can dissociate adsorbed CO with a low activation energy barrier. A driving force for the surface transformation is the preference of C adatoms to adsorb in 5- or 6-fold coordinated sites and the increasing strain in the surface because of the changes in surface metal atom–metal atom bond distances with the increasing surface overlayer concentration. The process is found to depend on the nanosize dimension of the surface covered with carbon. When this surface is an overlayer on top of a vacant Co surface, it can reduce stress by displacement of the Co atoms to unoccupied surface positions and the popping up process of Co atom does not occur. This explains why small nanoparticles will not reconstruct by popping up of Co atoms and do not create CO dissociation active sites even when covered with a substantial overlayer of C atoms.

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Section: Introductionmentioning

confidence: 99%

“…There have been important advances in the theory of surface reconstruction. ,,− By coupling first principles with statistical mechanics, Reuter et al computed the surface kinetics of CO oxidation catalysis at RuO 2 (110). They also presented a model of first-principles atomistic thermodynamics for oxidation catalysis .…”

Section: Introductionmentioning

confidence: 99%

Carbon-Induced Surface Transformations of Cobalt

2014

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Jansen

2012

An Introduction to Kinetic Monte Carlo Simulations of Surface Reactions

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A DFT study of H-dissolution into the bulk of a crystalline Ni(111) surface: a chemical identifier for the reaction kinetics

Shirazi

Bogaerts

Neyts

2017

Phys. Chem. Chem. Phys.

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In this study, we investigated the diffusion of H-atoms to the subsurface and their further diffusion into the bulk of a Ni(111) crystal by means of density functional theory calculations in the context of thermal and plasma-assisted catalysis. The H-atoms at the surface can originate from the dissociative adsorption of H 2 or CH 4 molecules, determining the surface H-coverage. When a threshold H-coverage is passed, corresponding to 1.00 ML for the crystalline Ni(111) surface, the surface-bound H-atoms start to diffuse to the subsurface. A similar threshold coverage is observed for the interstitial H-coverage. Once the interstitial sites are filled up with a coverage above 1.00 ML of H, dissolution of interstitial H-atoms to the layer below the interstitial sites will be initiated. Hence, by applying a high pressure or inducing a reactive plasma and high temperature, increasing the H-flux to the surface, a large amount of hydrogen can diffuse in a crystalline metal like Ni and can be absorbed. The formation of metal hydride may modify the entire reaction kinetics of the system. Equivalently, the H-atoms in the bulk can easily go back to the surface and release a large amount of heat. In a plasma process, H-atoms are formed in the plasma, and therefore the energy barrier for dissociative adsorption is dismissed, thus allowing achievement of the threshold coverage without applying a high pressure as in a thermal process. As a result, depending on the crystal plane and type of metal, a large number of H-atoms can be dissolved (absorbed) in the metal catalyst, explaining the high efficiency of plasma-assisted catalytic reactions. Here, the mechanism of H-dissolution is established as a chemical identifier for the investigation of the reaction kinetics of a chemical process.

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Frozen thermal fluctuations in adsorbate-induced step restructuring

Cited by 4 publications

References 27 publications

Carbon-Induced Surface Transformations of Cobalt

Carbon-Induced Surface Transformations of Cobalt

Examples

A DFT study of H-dissolution into the bulk of a crystalline Ni(111) surface: a chemical identifier for the reaction kinetics

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