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

Pfeifer, V., Jones, T., Velasco Vélez, J., Arrigo, R., Piccinin, S., Hävecker, M., et al. (2017). In situ observation of reactive oxygen species forming on oxygen-evolving iridium surfaces. Chemical Science, 8(3), 2143-2149. doi:10.1039/C6SC04622C.

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This journal is © The Royal Society of Chemistry 2017

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Pfeifer, Verena1, 2, Author           
Jones, Travis1, Author           
Velasco Vélez, Juan1, 3, Author           
Arrigo, Rosa4, Author
Piccinin, Simone5, Author
Hävecker, Michael1, 3, Author           
Knop-Gericke, Axel1, Author           
Schlögl, Robert1, 3, Author           
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Catalysis for Energy, Group EM-GKAT, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Elektronenspeicherring BESSY II, Albert-Einstein-Str. 15, Berlin, Germany, ou_persistent22              
3Department of Heterogeneous Reactions, Max-Planck-Institut für Chemische Energiekonversion, Stiftstr. 34-36, Mülheim a. d. Ruhr, Germany, ou_persistent22              
4Diamond Light Source Ltd., Harwell Science & Innovation Campus, Didcot, UK, ou_persistent22              
5Consiglio Nazionale delle Ricerche – Istituto Officina dei Materiali, c/o SISSA, Via Bonomea 265, Trieste, Italy, ou_persistent22              

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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.

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 Dates: 2016-10-162016-11-302016-12-012017-03-01
 Publication Status: Issued
 Pages: 7
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/C6SC04622C
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Title: Chemical Science
  Other : Chem. Sci.
Source Genre: Journal
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Publ. Info: Cambridge, UK : Royal Society of Chemistry
Pages: 7 Volume / Issue: 8 (3) Sequence Number: - Start / End Page: 2143 - 2149 Identifier: ISSN: 2041-6520
CoNE: https://pure.mpg.de/cone/journals/resource/2041-6520