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Electrochemical water splitting by gold: evidence for an oxide decomposition mechanism
Abstract
In this paper we study through a multiplicity of experimental and theoretical techniques the electrochemical evolution of oxygen on gold, the metal on which water splitting was initially discovered more than two centuries ago. The evidence obtained with a combination of in situ surface-enhanced Raman spectroscopy, online electrochemical mass spectrometry and density functional theory calculations suggests the existence of several mechanisms for the evolution of O2 on Au electrodes, depending on the electrode potential. Significantly, at approximately 2.0 V vs. RHE the first O2 that is evolved consists of two oxygens from the surface oxide, suggesting an oxide decomposition or oxide disproportionation step. At somewhat higher potentials, O2 is formed by a combination of oxygen from the oxide lattice and oxygen provided by water. The oxide decomposition step implies a more three-dimensional mechanism for oxygen evolution than suggested in previous mechanisms, which involve only surface-adsorbed intermediates.
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Cites
Special points for Brillouin-zone integrations
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Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
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Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
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Self-citationThe Mechanism of Water Oxidation: From Electrolysis via Homogeneous to Biological Catalysis
Dau, H., Limberg, C., Reier, T., Risch, M., Roggan, S., & Strasser, P. (2010) · ChemCatChem · doi:10.1002/cctc.201000126 · Cited by 1,783
Cited by
A review on fundamentals for designing oxygen evolution electrocatalysts
Song, J., Wei, C., Huang, Z.-F., Liu, C., Zeng, L., Wang, X., & Xu, Z. J. (2020) · Chemical Society Reviews · doi:10.1039/c9cs00607a · Cited by 2,936
Chatenet, M., Pollet, B. G., Dekel, D. R., Dionigi, F., Deseure, J., Millet, P., Braatz, R. D., Bazant, M. Z., Eikerling, M., Staffell, I., et al. (2022) · Chemical Society Reviews · doi:10.1039/d0cs01079k · Cited by 2,025
Reier, T., Nong, H. N., Teschner, D., Schlögl, R., & Strasser, P. (2017) · Advanced Energy Materials · doi:10.1002/aenm.201601275 · Cited by 1,253
Moysiadou, A., Lee, S., Hsu, C.-S., Chen, H. M., & Hu, X. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.0c04867 · Cited by 987
Trześniewski, B. J., Diaz-Morales, O., Vermaas, D. A., Longo, A., Bras, W., Koper, M. T. M., & Smith, W. A. (2015) · Journal of the American Chemical Society · doi:10.1021/jacs.5b06814 · Cited by 697
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Metadata
- Authors
- Diaz-Morales, O., Calle-Vallejo, F., de Munck, C., & Koper, M. T. M.
- Venue
- Chemical Science
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2013
- Volume
- 4
- Issue
- 6
- Pages
- 2334
- ISSN
- 2041-6520 (ISSN-L)
- 2041-6539
- OpenAlex
- W2096162182
- Cited by
- 285
- References
- 4
- FWCI
- 6.01
- Type
- journal article
- Language
- en
- Open access
- closed
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