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  Operando Structure–Activity–Stability Relationship of Iridium Oxides during the Oxygen Evolution Reaction

Mom, R., Falling, L., Kasian, O., Algara-Siller, G., Teschner, D., Crabtree, R. H., et al. (2022). Operando Structure–Activity–Stability Relationship of Iridium Oxides during the Oxygen Evolution Reaction. ACS Catalysis, 12(9), 5174-5184. doi:10.1021/acscatal.1c05951.

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 Creators:
Mom, Rik1, 2, Author              
Falling, Lorenz1, Author              
Kasian, Olga3, 4, Author
Algara-Siller, Gerardo1, Author              
Teschner, Detre1, 5, Author              
Crabtree, Robert H.6, Author
Knop-Gericke, Axel1, 5, Author              
Mayrhofer, Karl J. J.7, 8, Author
Velasco Vélez, Juan1, Author              
Jones, Travis1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Leiden Institute of Chemistry, Leiden University, 2300 RA Leiden, The Netherlands, ou_persistent22              
3Helmholtz-Zentrum Berlin GmbH, Helmholtz Institute Erlangen-Nürnberg, 14109 Berlin, Germany , ou_persistent22              
4Max Planck Institute for Iron Research, 40237 Düsseldorf, Germany, ou_persistent22              
5Max Planck Institute for Chemical Energy Conversion, 45413 Mülheim an der Ruhr, Germany, ou_persistent22              
6Department of Chemistry and Energy Sciences Institute, Yale University, New Haven, Connecticut 06520, United States, ou_persistent22              
7Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Forschungszentrum Jülich GmbH, 91058 Erlangen, Germany, ou_persistent22              
8Friedrich-Alexander- Universität Erlangen-Nürnberg, 91058 Erlangen, Germany, ou_persistent22              

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 Abstract: Creating active and stable electrodes is an essential step toward efficient and durable electrolyzers. To achieve this goal, understanding what aspects of the electrode structure dictate activity and catalyst dissolution is key. Here, we investigate these aspects by studying trends in the activity, stability, and operando structure of iridium oxides during the oxygen evolution reaction. Using operando X-ray photoelectron and X-ray absorption spectroscopy, we determined the near-surface structure of oxides ranging from amorphous to crystalline during the reaction. We show that applying oxygen evolution potentials universally yields deprotonated μ2-O moieties and a μ1-O/μ1-OH mixture, with universal deprotonation energetics but in different amounts. This quantitative difference mainly results from variations in deprotonation depth: surface deprotonation for crystalline IrO2 versus near-surface deprotonation for semicrystalline and amorphous IrOx. We argue that both surface deprotonation and subsurface deprotonation modify the barrier for the oxygen evolution and Ir dissolution reactions, thus playing an important role in catalyst performance.

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Language(s): eng - English
 Dates: 2022-03-082021-12-242022-05-06
 Publication Status: Published online
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.1c05951
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: 11 Volume / Issue: 12 (9) Sequence Number: - Start / End Page: 5174 - 5184 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435