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  Surface Electron-Hole Rich Species Active in the Electrocatalytic Water Oxidation

Velasco Vélez, J., Carbonio, E., Chuang, C.-H., Hsu, C.-J., Lee, J.-F., Arrigo, R., et al. (2021). Surface Electron-Hole Rich Species Active in the Electrocatalytic Water Oxidation. Journal of the American Chemical Society, 143(32), 12524-12534. doi:10.1021/jacs.1c01655.

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 Creators:
Velasco Vélez, Juan1, 2, Author              
Carbonio, Emilia2, 3, Author              
Chuang, Cheng-Hao4, Author
Hsu, Cheng-Jhih4, Author
Lee, Jyh-Fu5, Author
Arrigo, Rosa6, Author
Hävecker, Michael1, 2, Author              
Wang, Ruizhi7, Author
Plodinec, Milivoj2, 8, Author              
Wang, Feng Ryan9, Author
Centeno, Alba10, Author
Zurutuza, Amaia10, Author
Falling, Lorenz2, Author              
Mom, Rik2, Author              
Hofmann, Stephan7, Author
Schlögl, Robert1, 2, Author              
Knop-Gericke, Axel1, 2, Author              
Jones, Travis2, Author              
Affiliations:
1Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Mülheim an der Ruhr 45470, Germany, ou_persistent22              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
3Helmholtz-Center Berlin for Materials and Energy, BESSY II, Berlin 12489, Germany, ou_persistent22              
4Department of Physics, Tamkang University, New Taipei City 25137, Taiwan, ou_persistent22              
5National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan, ou_persistent22              
6School of Sciences, University of Salford, Environment and Life, Cockcroft building, M5 4WT, Manchester, U.K., ou_persistent22              
7Department of Engineering, University of Cambridge, Cambridge CB3 0FA, U.K., ou_persistent22              
8Rudjer Boskovic Institute, Bijenicka 54, HR-10000 Zagreb, Croatia, ou_persistent22              
9Department of Chemical Engineering, University College London, Torrington Placa, London WC1E7JE, U.K., ou_persistent22              
10Graphenea, San Sebastian 20018, Spain, ou_persistent22              

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 Abstract: Iridium and ruthenium and their oxides/hydroxides are the best candidates for the oxygen evolution reaction under harsh acidic conditions owing to the low overpotentials observed for Ru- and Ir-based anodes and the high corrosion resistance of Ir-oxides. Herein, by means of cutting edge operando surface and bulk sensitive X-ray spectroscopy techniques, specifically designed electrode nanofabrication and ab initio DFT calculations, we were able to reveal the electronic structure of the active IrOx centers (i.e., oxidation state) during electrocatalytic oxidation of water in the surface and bulk of high-performance Ir-based catalysts. We found the oxygen evolution reaction is controlled by the formation of empty Ir 5d states in the surface ascribed to the formation of formally IrV species leading to the appearance of electron-deficient oxygen species bound to single iridium atoms (μ1-O and μ1-OH) that are responsible for water activation and oxidation. Oxygen bound to three iridium centers (μ3-O) remains the dominant species in the bulk but do not participate directly in the electrocatalytic reaction, suggesting bulk oxidation is limited. In addition a high coverage of a μ1-OO (peroxo) species during the OER is excluded. Moreover, we provide the first photoelectron spectroscopic evidence in bulk electrolyte that the higher surface-to-bulk ratio in thinner electrodes enhances the material usage involving the precipitation of a significant part of the electrode surface and near-surface active species.

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Language(s): eng - English
 Dates: 2021-02-102021-08-062021-08-18
 Publication Status: Published in print
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.1c01655
 Degree: -

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Title: Journal of the American Chemical Society
  Other : JACS
  Abbreviation : J. Am. Chem. Soc.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 11 Volume / Issue: 143 (32) Sequence Number: - Start / End Page: 12524 - 12534 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870