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Uncovering The Role of Oxygen in Ni-Fe(OxHy) Electrocatalysts using In situ Soft X-ray Absorption Spectroscopy during the Oxygen Evolution Reaction
Open accessAbstract
In-situ X-ray absorption spectroscopy (XAS) at the oxygen K-edge was used to investigate the role of oxygen during the oxygen evolution reaction (OER) in an electrodeposited Ni-Fe(O x H y) electrocatalyst in alkaline pH. We show the rise of a pre-peak feature at 529 eV in the O K-edge spectra, correlated to the appearance of a shoulder at the Ni L 3-edge and formation of oxidized Ni 3+/4+-O. Then, for the first time, we track the spectral changes in a dynamic fashion in both the soft and hard X-ray regimes during cyclic voltammetry (in situ CV-XAS) to obtain a fine-tuned resolution of the potential-related changes. The pre-peak feature at the O K-edge likely signifies formation of an electron deficient oxygen site. The electrophilic oxygen species appears and disappears reversibly in correlation with the Ni 2+ ↔ Ni 3+/4+ process, and persists during OER catalysis as long the metal is oxidized. Our study provides new insight into OER electrocatalysis: Before onset of the O-O bond formation step, the catalytic oxyhydroxide has accumulated electron deficiencies by both, oxidation of transition metal ions and formation of partially oxidized oxygen sites.
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Cites
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
Man, I. C., Su, H., Calle‐Vallejo, F., Hansen, H. A., Martínez, J. I., Inoglu, N. G., Kitchin, J., Jaramillo, T. F., Nørskov, J. K., & Rossmeisl, J. (2011) · ChemCatChem · doi:10.1002/cctc.201000397 · Cited by 4,769
Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis
Hong, W. T., Risch, M., Stoerzinger, K. A., Grimaud, A., Suntivich, J., & Shao-Horn, Y. (2015) · Energy & Environmental Science · doi:10.1039/c4ee03869j · Cited by 2,089
The 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
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Cited by
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
Zhao, Y., Adiyeri Saseendran, D. P., Huang, C., Triana, C. A., Marks, W. R., Chen, H., Zhao, H., & Patzke, G. R. (2023) · Chemical Reviews · doi:10.1021/acs.chemrev.2c00515 · Cited by 802
Yu, M., Budiyanto, E., & Tüysüz, H. (2022) · Angewandte Chemie International Edition · doi:10.1002/anie.202103824 · Cited by 771
Ferreira de Araújo, J., Dionigi, F., Merzdorf, T., Oh, H., & Strasser, P. (2021) · Angewandte Chemie International Edition · doi:10.1002/anie.202101698 · Cited by 155
Aerogel-derived nickel-iron oxide catalysts for oxygen evolution reaction in alkaline media
Osmieri, L., Yu, H., Hermann, R. P., Kreider, M. E., Meyer, H. M., Kropf, A. J., Park, J. H., Alia, S. M., Cullen, D. A., Myers, D. J., et al. (2024) · Applied Catalysis B: Environment and Energy · doi:10.1016/j.apcatb.2024.123843 · Cited by 34
Metadata
- Authors
- Drevon, D., Görlin, M., Chernev, P., Xi, L., Dau, H., & Lange, K. M.
- Venue
- Scientific Reports
- Published
- 2019-02-06
- Volume
- 9
- Issue
- 1
- Pages
- 1532-1532
- ISSN
- 2045-2322 (ISSN-L)
- OpenAlex
- W2917602402
- Cited by
- 190
- References
- 3
- FWCI
- 4.12
- Type
- journal article
- Language
- en
- Open access
- gold
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- Drevon, D., Görlin, M., Chernev, P., Xi, L., Dau, H., & Lange, K. M. (2019). Uncovering The Role of Oxygen in Ni-Fe(OxHy) Electrocatalysts using In situ Soft X-ray Absorption Spectroscopy during the Oxygen Evolution Reaction. Scientific Reports. https://doi.org/10.1038/s41598-018-37307-x
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