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  Reactive oxygen species in iridium-based OER catalysts

Pfeifer, V., Jones, T., Wrabetz, S., Massué, C., Velasco Vélez, J., Arrigo, R., et al. (2016). Reactive oxygen species in iridium-based OER catalysts. Chemical Science, 7(11), 6791-6795. doi:10.1039/C6SC01860B.

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2016
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This journal is © The Royal Society of Chemistry

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Pfeifer, Verena1, 2, Author              
Jones, Travis1, Author              
Wrabetz, Sabine1, Author              
Massué, Cyriac1, 3, Author              
Velasco Vélez, Juan1, 3, Author              
Arrigo, Rosa 4, Author
Scherzer, Michael1, 3, Author              
Piccinin, Simone 5, 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, 12489, Berlin, Germany, ou_persistent22              
3MPI for Chemical Energy Conversion, ou_persistent22              
4Diamond Light Source Ltd., Harwell Science & Innovation Campus, Didcot, Oxfordshire OX 11 0DE, Great Britain, ou_persistent22              
5Consiglio Nazionale delle Ricerche – Instituto Officina dei Materiali, c/o SISSA, Via Bonomea 267, 34136, Trieste, Italy, ou_persistent22              

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 Abstract: Tremendous effort has been devoted towards elucidating the fundamental reasons for the higher activity of hydrated amorphous IrIII/IV oxyhydroxides (IrOx) in the oxygen evolution reaction (OER) in comparison with their crystalline counterpart, rutile-type IrO2, by focusing on the metal oxidation state. Here we demonstrate that, through an analogy to photosystem II, the nature of this reactive species is not solely a property of the metal but is intimately tied to the electronic structure of oxygen. We use a combination of synchrotron-based X-ray photoemission and absorption spectroscopies, ab initio calculations, and microcalorimetry to show that holes in the O2p states in amorphous IrOx give rise to a weakly bound oxygen that is extremely susceptible to nucleophilic attack, reacting stoichiometrically with CO already at room temperature. As such, we expect this species to play the critical role of the electrophilic oxygen involved in O-O bond formation in the electrocatalytic OER on IrOx. We propose that the dynamic nature of the Ir framework in amorphous IrOx imparts the flexibility in Ir oxidation state required for the formation of this active electrophilic oxygen.

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 Dates: 2016-04-282016-07-182016-07-19
 Publication Status: Published online
 Pages: 5
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 Rev. Type: Peer
 Identifiers: DOI: 10.1039/C6SC01860B
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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: 5 Volume / Issue: 7 (11) Sequence Number: - Start / End Page: 6791 - 6795 Identifier: ISSN: 2041-6520
CoNE: https://pure.mpg.de/cone/journals/resource/2041-6520