Initial oxidation of Cu(100) studied by X-ray photo-electron spectroscopy and density functional theory calculations

Posada-Borbón, Alvaro; Hagman, Benjamin; Schaëfer, Andreas; Zhang, Chu; Shipilin, Mikhail; Hellman, Anders; Gustafson, Johan; Grönbeck, Henrik

doi:10.1016/j.susc.2018.04.015

Cited by 18 publications

(22 citation statements)

References 37 publications

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“…Although the atomic structure of these two surface reconstructions has been determined from post-mortem analyses using atomically resolved probes such as scanning tunneling microscopy imaging of the reconstructed surfaces formed by dosing a small amount of oxygen in UHV conditions and at elevated temperature and then cooling to the room temperature for characterization, the mechanism and kinetics of the oxygen chemisorption-induced reconstruction process are not addressed based on the post-mortem tools. A recent study using AP-XPS monitored the transition from p (2 × 2) to MR reconstruction . Here, we mainly focus on the kinetic aspect of the oxygen chemisorption process.…”

Section: Resultsmentioning

confidence: 99%

“…For the initial oxygen exposure (1 min), O 1s can be deconvoluted into two peaks at BE = 529.3 and 529.9 eV, which can be assigned to the oxygen in the p(2 × 2) and MR reconstruction, respectively. 13 Upon the increased oxygen surface coverage from the oxygen exposure at this oxygen pressure, the MR peak intensity increases concomitantly with the decrease in the p(2 × 2) peak intensity. The correlated evolution in the intensity of the two peaks suggests that the p(2 × 2) reconstruction serves as a precursor to the MR reconstruction.…”

Section: Progressive Oxidation Stages From Oxygenmentioning

confidence: 91%

“…A recent study using AP-XPS monitored the transition from p(2 × 2) to MR reconstruction. 13 Here, we mainly focus on the kinetic aspect of the oxygen chemisorption process. 2) 45 × °O MR reconstruction that has the maximum oxygen surface coverage of 0.5 ML prior to the onset of the bulk oxide formation.…”

Section: Progressive Oxidation Stages From Oxygenmentioning

confidence: 99%

“…Therefore, this saturated O 1s intensity corresponds to the fully developed R (2 22) 45 × °O MR reconstruction that has the maximum oxygen surface coverage of 0.5 ML prior to the onset of the bulk oxide formation.Figure2bshows more detail about the O 1s spectra from the oxygen exposure at pO 2 = 1 × 10 −7 Torr. For the initial oxygen exposure (1 min), O 1s can be deconvoluted into two peaks at BE = 529.3 and 529.9 eV, which can be assigned to the oxygen in the p(2 × 2) and MR reconstruction, respectively 13. Upon the increased oxygen surface coverage from the oxygen exposure at this oxygen pressure, the MR peak intensity…”

mentioning

confidence: 99%

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Insight into the Phase Transformation Pathways of Copper Oxidation: From Oxygen Chemisorption on the Clean Surface to Multilayer Bulk Oxide Growth

Wang

Zhu

et al. 2018

J. Phys. Chem. C

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We have employed ambient-pressure X-ray photoelectron spectroscopy to monitor the full pathway of copper oxidation from the initial stages of oxygen chemisorption on the clean surface to oxide nucleation and growth and then to growing continuous oxide layer. By increasing oxygen pressure in a stepwise way from pO 2 = 10 −7 to 1 Torr at T = 350 °C, we show that the oxidation of Cu(100) takes place by dissociative chemisorption of oxygen to first form the p(2 × 2) phase at pO 2 = 1 × 10 −7 Torr, which then transforms to the R (2 22) 45 × °missing-row reconstruction with a higher oxygen coverage and upon increasing pO 2 from 1 × 10 −6 to 1 × 10 −3 Torr. After reaching pO 2 = 1 × 10 −2 Torr, nucleation and growth of Cu 2 O islands occurs by consuming the R (2 22) 45 × °regions. Increasing pO 2 to 0.1 Torr results in the continued Cu 2 O growth with increased surface roughness. The surface is quickly covered with a CuO layer upon increasing pO 2 to 1 Torr, at which the surface oxidation occurs via the CuO/Cu 2 O bilayer growth. The measurements delineate the range of pO 2 required for the crossover between the different stages of the surface oxidation and may have practical importance by tuning the oxidation conditions that allow for controlling the oxide phase and atomic structure of the surface.

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Section: Resultsmentioning

confidence: 99%

Section: Progressive Oxidation Stages From Oxygenmentioning

confidence: 91%

Section: Progressive Oxidation Stages From Oxygenmentioning

confidence: 99%

mentioning

confidence: 99%

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Insight into the Phase Transformation Pathways of Copper Oxidation: From Oxygen Chemisorption on the Clean Surface to Multilayer Bulk Oxide Growth

Wang

Zhu

et al. 2018

J. Phys. Chem. C

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“…kinetic Monte Carlo -KMC) and macro scale (e.g. computational fluid dynamics -CFD) is gaining importance, particularly when considering the engineering and intensification of unconventional feedstock processing, as well as the design of emerging catalysis routes (Hagman et al, 2018;Kattel et al, 2017;Maestri and Cuoci, 2013;Posada-Borbón et al, 2018;Wu and Yang, 2017). In order to do so, it is mandatory that we understand the reacting system on the atomic scale.…”

Section: Introductionmentioning

confidence: 99%

Multiscale modelling of CO2 reduction to methanol over industrial Cu/ZnO/Al2O3 heterogeneous catalyst: Linking ab initio surface reaction kinetics with reactor fluid dynamics

Pavlišič

Huš

Prašnikar

et al. 2020

Journal of Cleaner Production

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There has been a growing trend to couple different levels of modelling, such as going from first-principle calculations to the meso (e.g. kinetic Monte Carlo-KMC) and macro scale (e.g. computational fluid dynamics-CFD). In the current investigation, we put forward a CFD study of CO 2 hydrogenation to methanol for heterogeneous reacting flows in reactors with complex shape geometries, coupled with first-principle calculations (density functional theory (DFT)). KMC operation simulations were also performed to obtain insight into the uppermost layer conditions during the reaction. With computational fluid dynamics, the focus was placed on the non-uniform catalytic reduction of carbon dioxide to formate, which we treated with a detailed mean-field first-principle microkinetic model, analysed, and corroborated with experiments. The results showed a good consistent agreement with experimental data. The formulated methodological approach paves the way towards full virtual multiscale system descriptions of industrial processing units, encompassing all conventional stages, from catalyst design to the optimisation of mass transfer parameters. Such a bridging is outlined for carbon capture and utilisation.

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Core level photoemission line shape selection: Atomic adsorbates on iron

Acres

Hussain

Walczak

et al. 2020

Surface & Interface Analysis

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Robust fitting of core level photoemission spectra is often central to reliable interpretation of X-ray photoelectron spectroscopy (XPS) data. One key element is employment of the correct line shape function for each spectral component. In this study, we consider this topic, focusing on XPS data from atomic adsorbates, namely O and S, on Fe(110). The potential of employing density functional theory (DFT) for generating adsorbate projected electronic density of states (PDOS) to support line shape selection is explored. O 1s core level XPS spectra, acquired from various ordered overlayers of chemisorbed O, all display an equivalent asymmetric line shape. Previous work suggests that this asymmetry is a result of finite O PDOS in the vicinity of the Fermi level, allowing O 1s photoexcitation to induce a weighted continuum of final states through electron-hole pair excitation. This origin is corroborated by O DFT-PDOS generated for an optimised 5 layer Fe(110)(2x2)-O slab.

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Initial oxidation of Cu(100) studied by X-ray photo-electron spectroscopy and density functional theory calculations

Cited by 18 publications

References 37 publications

Insight into the Phase Transformation Pathways of Copper Oxidation: From Oxygen Chemisorption on the Clean Surface to Multilayer Bulk Oxide Growth

Insight into the Phase Transformation Pathways of Copper Oxidation: From Oxygen Chemisorption on the Clean Surface to Multilayer Bulk Oxide Growth

Multiscale modelling of CO2 reduction to methanol over industrial Cu/ZnO/Al2O3 heterogeneous catalyst: Linking ab initio surface reaction kinetics with reactor fluid dynamics

Core level photoemission line shape selection: Atomic adsorbates on iron

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