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A Functionally Stable Manganese Oxide Oxygen Evolution Catalyst in Acid
Abstract
First-row metals have been a target for the development of oxygen evolution reaction (OER) catalysts because they comprise noncritical elements. We now report a comprehensive electrochemical characterization of manganese oxide (MnOx) over a wide pH range, and establish MnOx as a functionally stable OER catalyst owing to self-healing, is derived from MnOx redeposition that offsets catalyst dissolution during turnover. To study this process in detail, the oxygen evolution mechanism of MnOx was investigated electrokinetically over a pH range spanning acidic, neutral, and alkaline conditions. In the alkaline pH regime, a ∼60 mV/decade Tafel slope and inverse first-order dependence on proton concentration were observed, whereas the OER acidic pH regime exhibited a quasi-infinite Tafel slope and zeroth-order dependence on proton concentration. The results reflect two competing mechanisms: a one-electron one-proton PCET pathway that is dominant under alkaline conditions and a Mn(3+) disproportionation process, which predominates under acidic conditions. Reconciling the rate laws of these two OER pathways with that of MnOx electrodeposition elucidates the self-healing characteristics of these catalyst films. The intersection of the kinetic profile of deposition and that of water oxidation as a function of pH defines the region of kinetic stability for MnOx and importantly establishes that a non-noble metal oxide OER catalyst may be operated in acid by exploiting a self-healing process.
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Metadata
- Authors
- Huynh, M., Bediako, D. K., & Nocera, D. G.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-04-11
- Volume
- 136
- Issue
- 16
- Pages
- 6002-6010
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2321284911
- Cited by
- 585
- References
- 54
- FWCI
- 17.36
- Type
- journal article
- Language
- en
- Open access
- closed
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