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Issue 3, 2017
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In situ observation of reactive oxygen species forming on oxygen-evolving iridium surfaces

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Abstract

Water splitting performed in acidic media relies on the exceptional performance of iridium-based materials to catalyze the oxygen evolution reaction (OER). In the present work, we use in situ X-ray photoemission and absorption spectroscopy to resolve the long-standing debate about surface species present in iridium-based catalysts during the OER. We find that the surface of an initially metallic iridium model electrode converts into a mixed-valent, conductive iridium oxide matrix during the OER, which contains OII− and electrophilic OI− species. We observe a positive correlation between the OI− concentration and the evolved oxygen, suggesting that these electrophilic oxygen sites may be involved in catalyzing the OER. We can understand this observation by analogy with photosystem II; their electrophilicity renders the OI− species active in O–O bond formation, i.e. the likely potential- and rate-determining step of the OER. The ability of amorphous iridium oxyhydroxides to easily host such reactive, electrophilic species can explain their superior performance when compared to plain iridium metal or crystalline rutile-type IrO2.

Graphical abstract: In situ observation of reactive oxygen species forming on oxygen-evolving iridium surfaces

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Supplementary files

Article information


Submitted
16 Oct 2016
Accepted
30 Nov 2016
First published
01 Dec 2016

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2017,8, 2143-2149
Article type
Edge Article

In situ observation of reactive oxygen species forming on oxygen-evolving iridium surfaces

V. Pfeifer, T. E. Jones, J. J. Velasco Vélez, R. Arrigo, S. Piccinin, M. Hävecker, A. Knop-Gericke and R. Schlögl, Chem. Sci., 2017, 8, 2143 DOI: 10.1039/C6SC04622C

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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