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  The rise of electrochemical NAPXPS operated in the soft X-ray regime exemplified by the oxygen evolution reaction on IrOx electrocatalysts

Velasco Vélez, J., Bernsmeier, D., Jones, T., Zeller, P., Carbonio, E., Chuang, C.-H., et al. (2022). The rise of electrochemical NAPXPS operated in the soft X-ray regime exemplified by the oxygen evolution reaction on IrOx electrocatalysts. Faraday Discussions. doi:10.1039/d1fd00114k.

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Velasco Vélez, Juan1, 2, Author              
Bernsmeier, Denis3, Author
Jones, Travis2, Author              
Zeller, Patrick2, 4, Author              
Carbonio, Emilia4, Author
Chuang, Cheng-Hao5, Author
Falling, Lorenz2, 6, Author              
Streibel, Verena2, Author              
Mom, Rik2, 7, Author              
Hammud, Adnan2, Author              
Hävecker, Michael1, 2, Author              
Arrigo, Rosa8, Author
Stotz, Eugen2, Author              
Lunkenbein, Thomas2, Author              
Knop-Gericke, Axel1, 2, Author              
Krähnert, Ralph3, Author
Schlögl, Robert1, 2, Author              
Affiliations:
1Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, 45470 Mülheim an der Ruhr, Germany , ou_persistent22              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
3Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, Germany , ou_persistent22              
4Helmholtz-Zentrum Berlin für Materialien und Energie, BESSY II, 12489 Berlin, Germany, ou_persistent22              
5Department of Physics, Tamkang University, New Taipei City 25137, Taiwan , ou_persistent22              
6Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA , ou_persistent22              
7Leiden Institute of Chemistry, Leiden University, Einsteinweg 55, 2333 CC Leiden, The Netherlands , ou_persistent22              
8School of Science, Engineering and Environment, University of Salford, Manchester, UK , ou_persistent22              

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 Abstract: Photoelectron spectroscopy offers detailed information about the electronic structure and chemical composition of surfaces, owing to the short distance that the photoelectrons can escape from a dense medium. Unfortunately, photoelectron based spectroscopies are not directly compatible with the liquids required to investigate electrochemical processes, especially in the soft X-ray regime. To overcome this issue, different approaches based on photoelectron spectroscopy have been developed in our group over the last few years. The performance and the degree of information provided by these approaches are compared with those of the well established bulk sensitive spectroscopic approach of total fluorescence yield detection, where the surface information gained from this approach is enhanced using samples with large surface to bulk ratios. The operation of these approaches is exemplified and compared using the oxygen evolution reaction on IrOx catalysts. We found that all the approaches, if properly applied, provide similar information about surface oxygen speciation. However, using resonant photoemission spectroscopy, we were able to prove that speciation is more involved and complex than previously thought during the oxygen evolution reaction on IrOx based electrocatalysts. We found that the electrified solid–liquid interface is composed of different oxygen species, where the terminal oxygen atoms on iridium are the active species, yielding the formation of peroxo species and, finally, dioxygen as the reaction product. Thus, the oxygen–oxygen bond formation is dominated by peroxo species formation along the reaction pathway. Furthermore, the methodologies discussed here open up opportunities to investigate electrified solid–liquid interfaces in a multitude of electrochemical processes with unprecedented speciation capabilities, which are not accessible by one-dimensional X-ray spectroscopies.

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Language(s): eng - English
 Dates: 2021-12-052022-02-082022-02-08
 Publication Status: Published online
 Pages: 23
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/d1fd00114k
 Degree: -

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Title: Faraday Discussions
  Abbreviation : Faraday Discuss.
Source Genre: Journal
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Publ. Info: London : Royal Society of Chemistry
Pages: 23 Volume / Issue: - Sequence Number: - Start / End Page: - Identifier: ISSN: 1359-6640
CoNE: https://pure.mpg.de/cone/journals/resource/954925269326