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  The electronic structure of iridium and its oxides

Pfeifer, V., Jones, T., Velasco Vélez, J., Massué, C., Arrigo, R., Teschner, D., et al. (2016). The electronic structure of iridium and its oxides. Surface and Interface Analysis, 48(5), 261-273. doi:10.1002/sia.5895.

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Pfeifer, Verena1, 2, Author              
Jones, Travis1, Author              
Velasco Vélez, Juan1, 3, Author              
Massué, Cyriac1, 3, Author              
Arrigo, Rosa1, 4, Author              
Teschner, Detre1, Author              
Girgsdies, Frank1, Author              
Scherzer, Michael1, 3, Author              
Greiner, Mark1, Author              
Allan, Jasmin1, Author              
Hashagen, Maike1, Author              
Weinberg, Gisela1, 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              
2Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Elektronenspeicherring BESSY II, Albert-Einstein-Str. 15, 12489 Berlin, Germany, ou_persistent22              
3Max-Planck-Institut für Chemische Energiekonversion, Stiftstr. 34-36, 45470 Mülheim a. d. Ruhr, Germany, ou_persistent22              
4Diamond Light Source Ltd., Harwell Science and Innovation Campus, Didcot, Oxfordshire, OX11 0DE UK, ou_persistent22              
5Istituto Officina dei Materiali (CNR-IOM), c/o SISSA – Scuola Internazionale Superiore di Studi Avanzati, Via Bonomea 267, 34136 Trieste, Italy, ou_persistent22              

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 Abstract: Iridium-based materials are among the most active and stable electrocatalysts for the oxygen evolution reaction. Amorphous iridium oxide structures are found to be more active than their crystalline counterparts. Herein, we combine synchrotron-based X-ray photoemission and absorption spectroscopies with theoretical calculations to investigate the electronic structure of Ir metal, rutile-type IrO2, and an amorphous IrOx. Theory and experiment show that while the Ir 4f line shape of Ir metal is well described by a simple Doniach–Šunjić function, the peculiar line shape of rutile-type IrO2 requires the addition of a shake-up satellite 1 eV above the main line. In the catalytically more active amorphous IrOx, we find that additional intensity appears in the Ir 4f spectrum at higher binding energy when compared with rutile-type IrO2 along with a pre-edge feature in the O K-edge. We identify these additional features as electronic defects in the anionic and cationic frameworks, namely, formally OI− and IrIII, which may explain the increased activity of amorphous IrOx electrocatalysts. We corroborate our findings by in situ X-ray diffraction as well as in situ X-ray photoemission and absorption spectroscopies.

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Language(s): eng - English
 Dates: 2015-10-292015-12-282016-05
 Publication Status: Published in print
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 Rev. Type: Peer
 Identifiers: DOI: 10.1002/sia.5895
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Title: Surface and Interface Analysis
Source Genre: Journal
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Publ. Info: New York, NY : John Wiley & Sons
Pages: 13 Volume / Issue: 48 (5) Sequence Number: - Start / End Page: 261 - 273 Identifier: ISSN: 0142-2421
CoNE: https://pure.mpg.de/cone/journals/resource/954925471358