Operando XAS Study of the Surface Oxidation State on a Monolayer IrOx on RuOx and Ru Oxide Based Nanoparticles for Oxygen Evolution in Acidic Media
Abstract
Here in this paper we present surface sensitive operando XAS L-edge measurements on IrOx/RuO2 thin films as well as mass-selected RuOx and Ru nanoparticles. We observed shifts of the white line XAS peak toward higher energies with applied electrochemical potential. Apart from the case of the metallic Ru nanoparticles, the observed potential dependencies were purely core-level shifts caused by a change in oxidation state, which indicates no structural changes. These findings can be explained by different binding energies of oxygenated species on the surface of IrOx and RuOx. Simulated XAS spectra show that the average Ir oxidation state change is strongly affected by the coverage of atomic O. The observed shifts in oxidation state suggest that the surface has a high coverage of O at potentials just below the potential where oxygen evolution is exergonic in free energy. In conclusion, this observation is consistent with the notion that the metal–oxygen bond is stronger than ideal.
- Authors:
-
- Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics
- Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; Univ. of Copenhagen (Denmark). Dept. of Chemistry; Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering
- Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering
- Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; Imperial College, London (United Kingdom). Dept. of Materials
- Univ. of Copenhagen (Denmark). Dept. of Chemistry
- Stockholm Univ. (Sweden). Fysikum
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); European Union (EU); Villum Foundation; Danish Ministry of Higher Education and Science; Danish Council for Independent Research
- OSTI Identifier:
- 1471512
- Grant/Contract Number:
- 9455; AC02-76SF00515; 607417
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 2; Journal ID: ISSN 1520-6106
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Pedersen, Anders F., Escudero-Escribano, Maria, Sebok, Bela, Bodin, Anders, Paoli, Elisa, Frydendal, Rasmus, Friebel, Daniel, Stephens, Ifan E. L., Rossmeisl, Jan, Chorkendorff, Ib, and Nilsson, Anders. Operando XAS Study of the Surface Oxidation State on a Monolayer IrOx on RuOx and Ru Oxide Based Nanoparticles for Oxygen Evolution in Acidic Media. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcb.7b06982.
Pedersen, Anders F., Escudero-Escribano, Maria, Sebok, Bela, Bodin, Anders, Paoli, Elisa, Frydendal, Rasmus, Friebel, Daniel, Stephens, Ifan E. L., Rossmeisl, Jan, Chorkendorff, Ib, & Nilsson, Anders. Operando XAS Study of the Surface Oxidation State on a Monolayer IrOx on RuOx and Ru Oxide Based Nanoparticles for Oxygen Evolution in Acidic Media. United States. https://doi.org/10.1021/acs.jpcb.7b06982
Pedersen, Anders F., Escudero-Escribano, Maria, Sebok, Bela, Bodin, Anders, Paoli, Elisa, Frydendal, Rasmus, Friebel, Daniel, Stephens, Ifan E. L., Rossmeisl, Jan, Chorkendorff, Ib, and Nilsson, Anders. Fri .
"Operando XAS Study of the Surface Oxidation State on a Monolayer IrOx on RuOx and Ru Oxide Based Nanoparticles for Oxygen Evolution in Acidic Media". United States. https://doi.org/10.1021/acs.jpcb.7b06982. https://www.osti.gov/servlets/purl/1471512.
@article{osti_1471512,
title = {Operando XAS Study of the Surface Oxidation State on a Monolayer IrOx on RuOx and Ru Oxide Based Nanoparticles for Oxygen Evolution in Acidic Media},
author = {Pedersen, Anders F. and Escudero-Escribano, Maria and Sebok, Bela and Bodin, Anders and Paoli, Elisa and Frydendal, Rasmus and Friebel, Daniel and Stephens, Ifan E. L. and Rossmeisl, Jan and Chorkendorff, Ib and Nilsson, Anders},
abstractNote = {Here in this paper we present surface sensitive operando XAS L-edge measurements on IrOx/RuO2 thin films as well as mass-selected RuOx and Ru nanoparticles. We observed shifts of the white line XAS peak toward higher energies with applied electrochemical potential. Apart from the case of the metallic Ru nanoparticles, the observed potential dependencies were purely core-level shifts caused by a change in oxidation state, which indicates no structural changes. These findings can be explained by different binding energies of oxygenated species on the surface of IrOx and RuOx. Simulated XAS spectra show that the average Ir oxidation state change is strongly affected by the coverage of atomic O. The observed shifts in oxidation state suggest that the surface has a high coverage of O at potentials just below the potential where oxygen evolution is exergonic in free energy. In conclusion, this observation is consistent with the notion that the metal–oxygen bond is stronger than ideal.},
doi = {10.1021/acs.jpcb.7b06982},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 2,
volume = 122,
place = {United States},
year = {Fri Oct 13 00:00:00 EDT 2017},
month = {Fri Oct 13 00:00:00 EDT 2017}
}
Web of Science
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