State of the Surface of Polycrystalline Silver after Exposure to Activated Oxygen

Ашхотов, О. Г.; Khubezhov, Soslan A.; Ашхотова, И. Б.

doi:10.1134/s1063782619150028

Cited by 4 publications

(6 citation statements)

References 6 publications

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“…The calculated CBE gap of +0.85 eV is in very good agreement with the CBE gap between the low-coverage and high-coverage oxygen species in multiple XPS studies. 32,33,57 In these studies, the high-coverage peak at greater CBE was attributed to subsurface oxygen, which is congruent with our results. Finally, the CBEs of oxygen in the two subsurface regions remain similar to each other in the presence or absence of surface oxygen.…”

Section: Resultssupporting

confidence: 91%

“…This change suggests that surface oxygen has a considerable effect on the CBE of subsurface oxygen, resulting in significantly different electronic properties of atomic oxygen adsorbed to the two regions. The calculated CBE gap of +0.85 eV is in very good agreement with the CBE gap between the low-coverage and high-coverage oxygen species in multiple XPS studies. ,, In these studies, the high-coverage peak at greater CBE was attributed to subsurface oxygen, which is congruent with our results. Finally, the CBEs of oxygen in the two subsurface regions remain similar to each other in the presence or absence of surface oxygen.…”

Section: Results and Discussionsupporting

confidence: 89%

“…To this end, we have developed a lattice-gas adsorption model of atomic oxygen on Ag(111) that includes surface and subsurface sites and is fully parametrized using DFT. The application to O/Ag(111) was motivated by evidence from several experimental and ab initio computational studies that strongly indicate the formation of subsurface oxygen in Ag(111) and its participation in surface reconstruction, oxide formation, and oxidation catalysis. ,− To our knowledge, this is the first lattice-gas adsorption model that describes both surface and subsurface adsorption. In its present form, the model describes oxygen adsorption at the most strongly binding sites but can be extended to include all types of surface and subsurface sites on Ag(111).…”

Section: Introductionmentioning

confidence: 99%

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Insight into Subsurface Adsorption Derived from a Lattice-Gas Model and Monte Carlo Simulations

et al. 2022

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Theoretical gas-surface models that describe adsorption over a broad range of adsorbate concentrations can provide qualitative insight into chemical phenomena, such as subsurface adsorption, surface reconstruction, and industrial heterogeneous catalysis. However, most atomistic, quantum-mechanical models of gas-surface adsorption are limited to low adsorbate coverage due to the large computational cost of models built using many surface atoms and adsorbates. To investigate adsorption in the subsurface of a crystalline solid with increasing coverage, we present a lattice-gas adsorption model that includes surface and subsurface sites of the solid and is fully parametrized using density functional theory. We apply the model to study the competition between the surface and subsurface adsorption of atomic oxygen on the Ag(111) surface. Oxygen population distributions calculated using the model in combination with Monte Carlo simulations show the onset of subsurface adsorption above a total coverage of 0.375 monolayer and a greater accumulation of oxygen in the second than in the first subsurface at total coverages between 0.5 and 1 monolayer. Our simulations also show that oxygen atoms do not percolate into the bulk region of silver for total coverages of up to 1 monolayer, indicating that oxygen adsorbed in the subsurface is distinct from oxygen absorbed in the bulk in this coverage range. Computations of core–electron binding energies and projected density of states for the equilibrium oxygen distribution at 0.5 monolayer reveal qualitative differences in the oxygen–silver bonding at the surface and subsurface, suggesting that oxygen adsorbed in the two regions could play distinct roles in the surface chemistry.

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Section: Resultssupporting

confidence: 91%

Section: Results and Discussionsupporting

confidence: 89%

Section: Introductionmentioning

confidence: 99%

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Insight into Subsurface Adsorption Derived from a Lattice-Gas Model and Monte Carlo Simulations

et al. 2022

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“…The calculated CBE gap is in good agreement with the measured CBE gap between the adsorbed oxygen species at low and high coverages measured in multiple XPS studies in which the species at high coverage was attributed to subsurface oxygen. 27,29,40 Finally, the CBE of oxygen in the two subsurface regions remain similar to each other in the presence or absence of surface oxygen.…”

Section: Electronic and Bonding Properties Of Surface Oxygen And Subsurface Oxygenmentioning

confidence: 77%

“…10,[13][14][15][16][17][18][19][20][21][22][23][24][25] Evidence from several experimental studies strongly indicates that as the surface concentration of atomic oxygen increases, it percolates to the subsurface region, i.e., the region just below the surface of the metal. [26][27][28][29][30][31][32] Subsurface adsorption has been explored in many gas-surface systems, such as CO 2 /Cu(100) and Cu(111), H 2 /Ni(111), and O/Al(111). [33][34][35] Results suggest that subsurface adsorbates play an important role in surface reconstruction and catalysis, such as in the case of oxygen covered silver surfaces, but the exact nature of their participation is not yet completely understood.…”

Section: Introductionmentioning

confidence: 99%

Coverage-dependent adsorption model of atomic oxygen on Ag(111)

Mize

Isbill

Roy

2021

Preprint

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Theoretical gas-surface models that describe adsorption over a wide range of coverages can provide qualitative insight into chemical phenomena that occur at intermediate to high coverages, such as subsurface adsorption, surface reconstruction, and industrial heterogeneous catalysis. However, most atomistic, quantum-mechanical models of gas-surface adsorption are limited to low adsorbate coverage due to the large computational cost of models built using many surface atoms and adsorbates. To investigate adsorption in the subsurface of a crystalline solid at high coverage, we present a lattice-gas adsorption model that includes surface and subsurface sites of the solid, and is fully parametrized using density functional theory. We apply the model to study the coverage-dependent adsorption of atomic oxygen on the Ag(111) surface. Oxygen population distributions calculated using the model show the onset of subsurface adsorption at a total coverage of approximately 1/4 monolayer, the saturation of surface adsorption at a total coverage of approximately 1/3 monolayer, and a greater accumulation of oxygen in the second rather than the first subsurface at total coverages greater than 1/2 monolayer. Computation of core-electron binding energies and projected density of states of an oxygen distribution predicted by the model reveal qualitative differences in oxygen-silver bonding at the surface and subsurface, suggesting that oxygen adsorbed in the two regions could play distinct roles in surface chemistry.

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Structure and Reactivity of Active Oxygen Species on Silver Surfaces for Ethylene Epoxidation

Guo,

Dongfang,

Iannuzzi

et al. 2024

ACS Catal.

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State of the Surface of Polycrystalline Silver after Exposure to Activated Oxygen

Cited by 4 publications

References 6 publications

Insight into Subsurface Adsorption Derived from a Lattice-Gas Model and Monte Carlo Simulations

Insight into Subsurface Adsorption Derived from a Lattice-Gas Model and Monte Carlo Simulations

Coverage-dependent adsorption model of atomic oxygen on Ag(111)

Structure and Reactivity of Active Oxygen Species on Silver Surfaces for Ethylene Epoxidation

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