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Electrochemical Water Oxidation with Cobalt-Based Electrocatalysts from pH 0–14: The Thermodynamic Basis for Catalyst Structure, Stability, and Activity
Open accessAbstract
Building upon recent study of cobalt-oxide electrocatalysts in fluoride-buffered electrolyte at pH 3.4, we have undertaken a mechanistic investigation of cobalt-catalyzed water oxidation in aqueous buffering electrolytes from pH 0-14. This work includes electrokinetic studies, cyclic voltammetric analysis, and electron paramagnetic resonance (EPR) spectroscopic studies. The results illuminate a set of interrelated mechanisms for electrochemical water oxidation in alkaline, neutral, and acidic media with electrodeposited Co-oxide catalyst films (CoO(x)(cf)s) as well as for a homogeneous Co-catalyzed electrochemical water oxidation reaction. Analysis of the pH dependence of quasi-reversible features in cyclic voltammograms of the CoO(x)(cf)s provides the basis for a Pourbaix diagram that closely resembles a Pourbaix diagram derived from thermodynamic free energies of formation for a family of Co-based layered materials. Below pH 3, a shift from heterogeneous catalysis producing O(2) to homogeneous catalysis yielding H(2)O(2) is observed. Collectively, the results reported here provide a foundation for understanding the structure, stability, and catalytic activity of aqueous cobalt electrocatalysts for water oxidation.
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Cites
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
Proton-coupled electron transfer
Huynh, M. H. V., & Meyer, T. J. (2007) · Chemical Reviews · doi:10.1021/cr0500030 · Cited by 1,659
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Earth-abundant catalysts for electrochemical and photoelectrochemical water splitting
Roger, I., Shipman, M. A., & Symes, M. D. (2017) · Nature Reviews Chemistry · doi:10.1038/s41570-016-0003 · Cited by 3,503
Recent Progress in Cobalt‐Based Heterogeneous Catalysts for Electrochemical Water Splitting
Wang, J., Cui, W., Liu, Q., Xing, Z., Asiri, A. M., & Sun, X. (2016) · Advanced Materials · doi:10.1002/adma.201502696 · Cited by 2,446
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
Xiao, Z., Huang, Y.-C., Dong, C.-L., Xie, C., Liu, Z., Du, S., Chen, W., Yan, D., Tao, L., Shu, Z., et al. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.0c00257 · Cited by 1,445
Bao, J., Zhang, X., Fan, B., Zhang, J., Zhou, M., Yang, W., Hu, X., Wang, H., Pan, B., & Xie, Y. (2015) · Angewandte Chemie International Edition · doi:10.1002/anie.201502226 · Cited by 1,428
Metadata
- Authors
- Gerken, J. B., McAlpin, J. G., Chen, J. Y. C., Rigsby, M. L., Casey, W. H., Britt, R. D., & Stahl, S. S.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2011-08-19
- Volume
- 133
- Issue
- 36
- Pages
- 14431-14442
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W1985778735
- Cited by
- 814
- References
- 2
- FWCI
- 18.39
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- Gerken, J. B., McAlpin, J. G., Chen, J. Y. C., Rigsby, M. L., Casey, W. H., Britt, R. D., & Stahl, S. S. (2011). Electrochemical Water Oxidation with Cobalt-Based Electrocatalysts from pH 0–14: The Thermodynamic Basis for Catalyst Structure, Stability, and Activity. Journal of the American Chemical Society. https://doi.org/10.1021/ja205647m
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