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  Evolution of Oxygen–Metal Electron Transfer and Metal Electronic States During Manganese Oxide Catalyzed Water Oxidation Revealed with In Situ Soft X-Ray Spectroscopy

Tesch, M., Bonke, S., Jones, T., Shaker, M., Xiao, J., Skorupska, K., et al. (2019). Evolution of Oxygen–Metal Electron Transfer and Metal Electronic States During Manganese Oxide Catalyzed Water Oxidation Revealed with In Situ Soft X-Ray Spectroscopy. Angewandte Chemie, 131(11), 3464-3470. doi:10.1002/ange.201810825.

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 Creators:
Tesch, Marc1, 2, Author
Bonke, Shannon3, 4, 5, Author
Jones, Travis6, Author              
Shaker, Maryam1, 7, Author
Xiao, Jie1, Author
Skorupska, Katarzyna2, 6, Author              
Mom, Rik6, Author              
Melder, Jens8, Author
Kurz, Philipp8, Author
Knop-Gericke, Axel6, Author              
Schlögl, Robert2, 6, Author              
Hocking, Rosalie9, Author
Simonov, Alexandr Nikolaevich3, Author
Affiliations:
1Institut Methoden der Materialentwicklung, Helmholtz Zentrum Berlin für Materialien und Energie, Albert-Einstein-Straße 15, 12489 Berlin (Germany), ou_persistent22              
2Abteilung Heterogene Reaktionen, Max-Planck-Institut für Chemische Energiekonversion, Stiftstraße 34–36, 45470 Mülheim an der Ruhr (Germany), ou_persistent22              
3School of Chemistry and the ARC Centre of Excellence for Electromaterials Science, Monash University, Victoria 3800 (Australia), ou_persistent22              
4Institut Nanospektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Kekulestraße 5, 12489 Berlin (Germany, ou_persistent22              
5EPR Research Group, Max-Planck-Institut für Chemische Energiekonversion, Stiftstraße 34-36, 45470 Mülheim an der Ruhr (Germany), ou_persistent22              
6Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
7Freie Universität Berlin, Fachbereich Physik, Arnimallee 14, 14159 Berlin (Germany), ou_persistent22              
8Institut für Anorganische und Analytische Chemie and Freiburger Materialforschungszentrum, Albert-Ludwigs-Universität Freiburg, Albertstraße 21, 79104 Freiburg (Germany), ou_persistent22              
9Department of Chemistry and Biotechnology, Swinburne University of Technology, John Street, Hawthorn, Victoria 3122 (Australia), ou_persistent22              

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 Abstract: Manganese oxide (MnOx) electrocatalysts are examined herein by in situ soft X‐ray absorption spectroscopy (XAS) and resonant inelastic X‐ray scattering (RIXS) during the oxidation of water buffered by borate (pH 9.2) at potentials from 0.75 to 2.25 V vs. the reversible hydrogen electrode. Correlation of L‐edge XAS data with previous mechanistic studies indicates MnIV is the highest oxidation state involved in the catalytic mechanism. MnOx is transformed into birnessite at 1.45 V and does not undergo further structural phase changes. At potentials beyond this transformation, RIXS spectra show progressive enhancement of charge transfer transitions from oxygen to manganese. Theoretical analysis of these data indicates increased hybridization of the Mn−O orbitals and withdrawal of electron density from the O ligand shell. In situ XAS experiments at the O K‐edge provide complementary evidence for such a transition. This step is crucial for the formation of O2 from water.

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Language(s): eng - English
 Dates: 2018-09-202018-12-272018-12-272019-03-11
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/ange.201810825
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Title: Angewandte Chemie
  Abbreviation : Angew. Chem.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 7 Volume / Issue: 131 (11) Sequence Number: - Start / End Page: 3464 - 3470 Identifier: ISSN: 0044-8249
CoNE: https://pure.mpg.de/cone/journals/resource/954926979058_1