Effect of Different In2O3(111) Surface Terminations on CO2 Adsorption
(2023) In ACS Applied Materials and Interfaces 15(38). p.45367-45377- 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... (More)
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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- author
- organization
-
- LU Profile Area: Light and Materials
- Combustion Physics
- LTH Profile Area: The Energy Transition
- MAX IV, SMS
- MAX IV Laboratory
- LTH Profile Area: Nanoscience and Semiconductor Technology
- Chemical Engineering (M.Sc.Eng.)
- NanoLund: Centre for Nanoscience
- Division of Chemical Engineering
- LTH Profile Area: Photon Science and Technology
- Synchrotron Radiation Research
- publishing date
- 2023-09-27
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- CO adsorption, core-level shifts, density functional theory, heterogeneous catalysis, indium oxide, methanol synthesis, X-ray photoelectron spectroscopy
- in
- ACS Applied Materials and Interfaces
- volume
- 15
- issue
- 38
- pages
- 11 pages
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- pmid:37704018
- scopus:85172712712
- ISSN
- 1944-8244
- DOI
- 10.1021/acsami.3c07166
- language
- English
- LU publication?
- yes
- id
- d4c0f8bf-2f67-42ec-94e8-bba1a7d48448
- date added to LUP
- 2023-12-06 09:19:09
- date last changed
- 2024-04-19 03:50:46
@article{d4c0f8bf-2f67-42ec-94e8-bba1a7d48448, abstract = {{<p>In<sub>2</sub>O<sub>3</sub>-based catalysts have shown high activity and selectivity for CO<sub>2</sub> hydrogenation to methanol; however, the origin of the high performance of In<sub>2</sub>O<sub>3</sub> is still unclear. To elucidate the initial steps of CO<sub>2</sub> hydrogenation over In<sub>2</sub>O<sub>3</sub>, we have combined X-ray photoelectron spectroscopy and density functional theory calculations to study the adsorption of CO<sub>2</sub> on the In<sub>2</sub>O<sub>3</sub>(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 CO<sub>2</sub> adsorbs as a carbonate on all three surface terminations. We find that the adsorption of CO<sub>2</sub> is hindered by hydroxyl groups on the hydroxylated surface.</p>}}, author = {{Gericke, Sabrina M. and Kauppinen, Minttu M. and Wagner, Margareta and Riva, Michele and Franceschi, Giada and Posada-Borbón, Alvaro and Rämisch, Lisa and Pfaff, Sebastian and Rheinfrank, Erik and Imre, Alexander M. and Preobrajenski, Alexei B. and Appelfeller, Stephan and Blomberg, Sara and Merte, Lindsay R. and Zetterberg, Johan and Diebold, Ulrike and Grönbeck, Henrik and Lundgren, Edvin}}, issn = {{1944-8244}}, keywords = {{CO adsorption; core-level shifts; density functional theory; heterogeneous catalysis; indium oxide; methanol synthesis; X-ray photoelectron spectroscopy}}, language = {{eng}}, month = {{09}}, number = {{38}}, pages = {{45367--45377}}, publisher = {{The American Chemical Society (ACS)}}, series = {{ACS Applied Materials and Interfaces}}, title = {{Effect of Different In<sub>2</sub>O<sub>3</sub>(111) Surface Terminations on CO<sub>2</sub> Adsorption}}, url = {{http://dx.doi.org/10.1021/acsami.3c07166}}, doi = {{10.1021/acsami.3c07166}}, volume = {{15}}, year = {{2023}}, }