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Ab Initio Calculations of Intermediates of Oxygen Reduction on Low-Index Platinum Surfaces
Open accessAbstract
Properties of the oxygen molecule, atomic oxygen, and intermediate products of its reduction, OH, OOH, H 2 O 2 on (111), (100), and (110) Pt surfaces have been investigated using periodic density functional theory. The Pt surfaces are modeled as four-layer slabs. Adsorption energies and geometries, as well as the charge-transfer properties are calculated. Computed characteristics of the adsorbed oxygen reduction intermediates supply known tendencies of the low index Pt surface activities under different experimental conditions. Electric field dependencies of the properties of all species adsorbed on a Pt 9 ( 111 ) cluster have been also studied. Lowering the field causes an increase of the O-O bond length of O 2 ads , attracting the molecule to the Pt surface and increasing the charge transfer from Pt to 2π * orbitals of the oxygen molecule. The weakening of the O-O bond is evidenced by a decrease of the O-O stretching frequency. The charge-transfer from the Pt 9 cluster to the adsorbates is observed for all species. In our calculations hydrogen peroxide was unstable on all three low-index Pt surfaces and dissociated into two hydroxyls or a water molecule and atomic oxygen. The results of the calculations are discussed in the context of the mechanism of oxygen reduction. © 2004 The Electrochemical Society. All rights reserved.
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Cites
Oxygen Reduction on Carbon-Supported Pt−Ni and Pt−Co Alloy Catalysts
Paulus, U. A., Wokaun, A., Scherer, G. G., Schmidt, T. J., Stamenkovic, V., Radmilovic, V., Markovic, N. M., & Ross, P. N. (2002) · The Journal of Physical Chemistry B · doi:10.1021/jp013442l · Cited by 954
Cited by
Loynachan, C. N., Thomas, M. R., Gray, E. R., Richards, D. A., Kim, J., Miller, B. S., Brookes, J. C., Agarwal, S., Chudasama, V., McKendry, R. A., et al. (2018) · ACS Nano · doi:10.1021/acsnano.7b06229 · Cited by 403
Katsounaros, I., Schneider, W. B., Meier, J. C., Benedikt, U., Biedermann, P. U., Auer, A. A., & Mayrhofer, K. J. J. (2012) · Physical Chemistry Chemical Physics · doi:10.1039/c2cp40616k · Cited by 377
Theoretical Investigations of the Oxygen Reduction Reaction on Pt(111)
Keith, J. A., Jerkiewicz, G., & Jacob, T. (2010) · ChemPhysChem · doi:10.1002/cphc.201000286 · Cited by 233
Shah, A. A., Ralph, T. R., & Walsh, F. C. (2009) · Journal of The Electrochemical Society · doi:10.1149/1.3077573 · Cited by 149
How theory and simulation can drive fuel cell electrocatalysis
Eslamibidgoli, M. J., Huang, J., Kadyk, T., Malek, A., & Eikerling, M. (2016) · Nano Energy · doi:10.1016/j.nanoen.2016.06.004 · Cited by 83
Metadata
- Authors
- Panchenko, A., Koper, M. T. M., Shubina, T. E., Mitchell, S. J., & Roduner, E.
- Venue
- Journal of The Electrochemical Society
- Publisher
- The Electrochemical Society
- Published
- 2004
- Volume
- 151
- Issue
- 12
- Pages
- A2016
- ISSN
- 0013-4651 (ISSN-L)
- OpenAlex
- W2072873551
- Cited by
- 190
- References
- 1
- FWCI
- 6.78
- Type
- journal article
- Language
- en
- Open access
- bronze
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- Panchenko, A., Koper, M. T. M., Shubina, T. E., Mitchell, S. J., & Roduner, E. (2004). Ab Initio Calculations of Intermediates of Oxygen Reduction on Low-Index Platinum Surfaces. Journal of The Electrochemical Society. https://doi.org/10.1149/1.1809586
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