| 1. |
- Gericke, Sabrina M., et al.
(author)
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Effect of Different In 2 O 3 (111) Surface Terminations on CO 2 Adsorption
- 2023
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In: ACS Applied Materials & Interfaces. - 1944-8252 .- 1944-8244. ; 15:38, s. 45367-45377
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Journal article (peer-reviewed)abstract
- In2O3-based catalysts have shown high activity and selectivity for CO2 hydrogenation to methanol; however, the origin of the high performance of In2O3 is still unclear. To elucidate the initial steps of CO2 hydrogenation over In2O3, we have combined X-ray photoelectron spectroscopy and density functional theory calculations to study the adsorption of CO2 on the In2O3(111) crystalline surface with different terminations, namely, the stoichiometric, reduced, and hydroxylated surface. The combined approach confirms that the reduction of the surface results in the formation of In adatoms and that water dissociates on the surface at room temperature. A comparison of the experimental spectra and the computed core-level shifts (using methanol and formic acid as benchmark molecules) suggests that CO2 adsorbs as a carbonate on all three surface terminations. We find that the adsorption of CO2 is hindered by hydroxyl groups on the hydroxylated surface.
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| 2. |
- Gericke, Sabrina M., et al.
(author)
-
Effect of Different In2O3(111) Surface Terminations on CO2 Adsorption
- 2023
-
In: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 15:38, s. 45367-45377
-
Journal article (peer-reviewed)abstract
- In2O3-based catalysts have shown high activity and selectivity for CO2 hydrogenation to methanol; however, the origin of the high performance of In2O3 is still unclear. To elucidate the initial steps of CO2 hydrogenation over In2O3, we have combined X-ray photoelectron spectroscopy and density functional theory calculations to study the adsorption of CO2 on the In2O3(111) crystalline surface with different terminations, namely, the stoichiometric, reduced, and hydroxylated surface. The combined approach confirms that the reduction of the surface results in the formation of In adatoms and that water dissociates on the surface at room temperature. A comparison of the experimental spectra and the computed core-level shifts (using methanol and formic acid as benchmark molecules) suggests that CO2 adsorbs as a carbonate on all three surface terminations. We find that the adsorption of CO2 is hindered by hydroxyl groups on the hydroxylated surface.
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| 3. |
- Harlow, Gary S., et al.
(author)
-
HAT : a high-energy surface X-ray diffraction analysis toolkit
- 2023
-
In: Journal of Applied Crystallography. - 0021-8898. ; 56, s. 312-321
-
Journal article (peer-reviewed)abstract
- This work introduces the high-energy surface X-ray diffraction analysis toolkit (HAT), an open-source cross-platform software package written in Python to allow the extraction and processing of high-energy surface X-ray diffraction (HESXRD) data sets. Thousands of large-area detector images are collected in a single HESXRD scan, corresponding to billions of pixels and hence reciprocal space positions. HAT is an optimized reciprocal space binner that implements a graphical user interface to allow the easy and interactive exploration of HESXRD data sets. Regions of reciprocal space can be selected with movable and resizable masks in multiple views and are projected onto different axes to allow the creation of reciprocal space maps and the extraction of crystal truncation rods. Current and future versions of HAT can be downloaded and used free of charge.
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| 4. |
- Larsson, Alfred, et al.
(author)
-
Operando Surface Optical Reflectance Microscopy Study of Corrosion Film Growth on a Ni-Cr-Mo Alloy During Anodic Polarization
- 2023
-
In: Journal of Physical Chemistry C. - 1932-7447. ; 127:44, s. 21871-21877
-
Journal article (peer-reviewed)abstract
- The solid-liquid interface, where corrosion reactions occur, is notoriously difficult to study in operando conditions. Few experimental techniques can provide surface sensitivity and spatial and temporal resolution and are compatible with liquid environments. 2-Dimensional surface optical reflectance (2D-SOR) is an emerging optical technique providing microscopic information with high temporal resolution. It complements methods such as ambient pressure X-ray photoelectron spectroscopy or inductively coupled plasma-mass spectrometry, which provides valuable chemical information from the surface and the dissolving species but lacks spatial resolution. Here, we show how 2D-SOR can be used to measure the formation and growth of corrosion products in operando through oscillations in the reflected signal caused by constructive and destructive interference of the light in the film of growing corrosion products. The total thickness of the corrosion product film obtained with 2D-SOR agrees well with that measured using scanning electron microscopy ex situ. 2D-SOR has proved to be an excellent and valuable tool for monitoring the corrosion process with spatial resolution in operating conditions.
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| 5. |
- Larsson, Alfred, et al.
(author)
-
Operando Surface Optical Reflectance Microscopy Study of Corrosion Film Growth on a Ni-Cr-Mo Alloy During Anodic Polarization
- 2023
-
In: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 127:44, s. 21871-21877
-
Journal article (peer-reviewed)abstract
- The solid-liquid interface, where corrosion reactions occur, is notoriously difficult to study in operando conditions. Few experimental techniques can provide surface sensitivity and spatial and temporal resolution and are compatible with liquid environments. 2-Dimensional surface optical reflectance (2D-SOR) is an emerging optical technique providing microscopic information with high temporal resolution. It complements methods such as ambient pressure X-ray photoelectron spectroscopy or inductively coupled plasma-mass spectrometry, which provides valuable chemical information from the surface and the dissolving species but lacks spatial resolution. Here, we show how 2D-SOR can be used to measure the formation and growth of corrosion products in operando through oscillations in the reflected signal caused by constructive and destructive interference of the light in the film of growing corrosion products. The total thickness of the corrosion product film obtained with 2D-SOR agrees well with that measured using scanning electron microscopy ex situ. 2D-SOR has proved to be an excellent and valuable tool for monitoring the corrosion process with spatial resolution in operating conditions.
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| 6. |
- Mehar, Vikram, et al.
(author)
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Formation of Epitaxial PdO(100) During the Oxidation of Pd(100)
- 2023
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In: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 14:38, s. 8493-8499
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Journal article (other academic/artistic)abstract
- The catalytic oxidation of CO and CH4 can be strongly influenced by the structures of oxide phases that form on metallic catalysts during reaction. Here, we show that an epitaxial PdO(100) structure forms at temperatures above 600 K during the oxidation of Pd(100) by gaseous O atoms as well as exposure to O2-rich mixtures at millibar partial pressures. The oxidation of Pd(100) by gaseous O atoms preferentially generates an epitaxial, multilayer PdO(101) structure at 500 K, but initiating Pd(100) oxidation above 600 K causes an epitaxial PdO(100) structure to grow concurrently with PdO(101) and produces a thicker and rougher oxide. We present evidence that this change in the oxidation behavior is caused by a temperature-induced change in the stability of small PdO domains that initiate oxidation. Our discovery of the epitaxial PdO(100) structure may be significant for developing relationships among oxide structure, catalytic activity, and reaction conditions for applications of oxidation catalysis.
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