Density functional theory study of the adsorption of oxygen atoms on gold (111), (100) and (211) surfaces

Daigle, April D.; BelBruno, Joseph J.

doi:10.1016/j.susc.2011.04.025

Cited by 11 publications

(15 citation statements)

References 25 publications

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“…The most favorable adsorption sites (see Figure 1b for atomic oxygen on both Au(211) and AgAu(211) (θ Ag = 6/9 ML)) are located near the step, consistent with previous theoretical studies. 33,42 O has nearly the same adsorption energy in the bridge site on the step (site d), the fcc hollow near the step (site e), and the hcp hollow near the step (site c). O adsorbs more strongly on AgAu(211) than Au(211) (see Figure 1b), but the trends in site preference are similar.…”

Section: ■ Resultsmentioning

confidence: 99%

“…In previous theoretical studies, the adsorption of O has been studied on flat Au(111) and Au(100) surfaces, − as well as stepped Au(211), but a detailed study on the adsorption and diffusion of oxidation intermediates on AgAu surfaces is lacking. Because flat, low-index surfaces are less active for O 2 dissociation, we focus on the (211) surface, which combines the features of (111) surface terraces and (100) surface steps.…”

Section: Introductionmentioning

confidence: 99%

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Density Functional Theory Investigation of Oxidation Intermediates on Gold and Gold–Silver Surfaces

Şensoy

Montemore

2020

J. Phys. Chem. C

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Gold and gold−silver alloys can be active and selective oxidation catalysts. Previous work has suggested that O 2 dissociation occurs at bimetallic step sites on gold−silver alloys, but the site responsible for the rest of the reaction steps has not been studied. As a first step in gaining insight into this issue, we investigated the adsorption of oxygen and other oxidation intermediates on the ( 111) and ( 211) facets of gold−silver alloys using density functional theory. Oxygen and silver coverage effects were analyzed, and different model structures were compared. We also examined the energy barriers for the diffusion of atomic oxygen to gain insight into O migration and spillover. On (111) surfaces, O adsorption is much stronger at low O coverage (less than 0.22 ML), while on (211) surfaces O is strongly bound at both high and low O coverage. O diffusion across the step is faster than diffusion along the step. Ag stabilizes O, both when directly bound to it and when in an adjacent site. Ag also reduces repulsive O−O interactions at low O coverage. Our calculated reaction barriers for O-assisted CH 3 O dehydrogenation suggest that reaction is faster on steps than on terraces. Overall, our findings suggest that spillover of O from Ag-rich steps to Au-rich terraces does not occur and that oxidation reactions on gold−silver alloys occur on step sites. More specifically, oxidation likely occurs either on Ag-rich step sites or on Au-rich step sites that are adjacent to Ag-rich step sites.

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Section: ■ Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Density Functional Theory Investigation of Oxidation Intermediates on Gold and Gold–Silver Surfaces

Şensoy

Montemore

2020

J. Phys. Chem. C

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“…Research on crystal surfaces at the nano and molecular scale is of great interest. [1][2][3][4][5][6] From a molecular perspective, molecules on the surface are unique. The same crystal may have different facets and molecules on the non-symmetric facets are arranged in different ways.…”

Section: Introductionmentioning

confidence: 99%

Nanocrystal formation and polymorphism of glycine

Yang

Myerson

2015

CrystEngComm

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“…The gold-sulfur atom distances are within the customary range cited for such bonds. 45,46 Methylamine, methanethiol and methanol adsorb through the heteroatom end in the ontop site and show a preference for the ontop site over the hollow and bridge sites by 0.3 eV, 0.2 eV and 0.1 eV, respectively. Methanethiol has the greatest tilt, adsorbing with the methyl group more parallel to the surface than either methylamine or methanol; methanol has the smallest adsorption energy and the greatest distance from the gold surface.…”

Section: Discussionmentioning

confidence: 99%

“…Atomic nitrogen has previously been found to have the strongest preference for hollow sites over bridge and ontop sites among nitrogen, oxygen and sulfur atoms, and, from nudged elastic band calculations, the greatest barriers to diffusion on gold surfaces. 45,46 Along with stronger adsorption, methylamine binds more closely to the (111) ontop site than methanol or methanethiol. Methanethiol, which has the greater height above the surface, also has the greatest tilt, bringing the alkyl chain in closer…”

Section: Adsorption Of Alkylamines On Au(111)mentioning

confidence: 99%

Impact of surface steps and oxygen pre-coverage on the adsorption of methylamine on gold

Lewoczko

BelBruno

2013

Phys. Chem. Chem. Phys.

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Using density functional theory calculations, we report on the adsorption of methylamine on gold and compare its adsorption to a selection of alkylamines, methanol and methanethiol. On the (111) surface, the amines, thiol and alcohol bind in the ontop site with a preference over hollow and bridge sites of 0.3 eV, 0.2 eV and 0.1 eV for methylamine, methanethiol and methanol, respectively. The effect of steps is considered on the (211) surface of gold and we find that methylamine adsorbs 0.2 eV more strongly in the step ontop site of the surface than on the (111) surface. For oxygen atom pre-coverages of 0.04-0.25 ML on the (111) surface, we find cooperative adsorption of amines and oxygen atoms. The energetic costs of adsorbate tilt from the surface normal and of rotation about the gold-heteroatom bond are compared among the studied surfaces and conditions.

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Density functional theory study of the adsorption of oxygen atoms on gold (111), (100) and (211) surfaces

Cited by 11 publications

References 25 publications

Density Functional Theory Investigation of Oxidation Intermediates on Gold and Gold–Silver Surfaces

Density Functional Theory Investigation of Oxidation Intermediates on Gold and Gold–Silver Surfaces

Nanocrystal formation and polymorphism of glycine

Impact of surface steps and oxygen pre-coverage on the adsorption of methylamine on gold

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