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  Role of Nanoscale Inhomogeneities in Co2FeO4 Catalysts during the Oxygen Evolution Reaction

Haase, F., Rabe, A., Schmidt, F., Herzog, A., Jeon, H., Frandsen, W., et al. (2022). Role of Nanoscale Inhomogeneities in Co2FeO4 Catalysts during the Oxygen Evolution Reaction. Journal of the American Chemical Society, 144(27), 12007-12019. doi:10.1021/jacs.2c00850.

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 Creators:
Haase, Felix1, Author           
Rabe, Anna2, 3, Author
Schmidt, Franz4, 5, Author           
Herzog, Antonia1, Author           
Jeon, Hyosang1, Author           
Frandsen, Wiebke1, Author           
Narangoda, Praveen Vidusha5, Author
Spanos, Ioannis5, Author
Ortega, Klaus Friedel2, Author
Timoshenko, Janis1, Author           
Lunkenbein, Thomas4, Author           
Behrens, Malte2, 3, Author
Bergmann, Arno1, Author           
Schlögl, Robert4, 5, Author           
Roldan Cuenya, Beatriz1, Author           
Affiliations:
1Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
2Inorganic Chemistry and Center for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen, 7 Universitätsstr. , Essen, 45141, Germany , ou_persistent22              
3Inorganic Chemistry, Christian Albrechts University, 2 Max-Eyth-Straße, Kiel, 24118, Germany , ou_persistent22              
4Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
5Max Planck Institute for Chemical Energy Conversion, 34-36 Stiftstrasse, Mülheim an der Ruhr, 45470, Germany, ou_persistent22              

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 Abstract: Spinel-type catalysts are promising anode materials for the alkaline oxygen evolution reaction (OER), exhibiting low overpotentials and providing long-term stability. In this study, we compared two structurally equal Co2FeO4 spinels with nominally identical stoichiometry and substantially different OER activities. In particular, one of the samples, characterized by a metastable precatalyst state, was found to quickly achieve its steady-state optimum operation, while the other, which was initially closer to the ideal crystallographic spinel structure, never reached such a state and required 168 mV higher potential to achieve 1 mA/cm2. In addition, the enhanced OER activity was accompanied by a larger resistance to corrosion. More specifically, using various ex situ, quasi in situ, and operando methods, we could identify a correlation between the catalytic activity and compositional inhomogeneities resulting in an X-ray amorphous Co2+-rich minority phase linking the crystalline spinel domains in the as-prepared state. Operando X-ray absorption spectroscopy revealed that these Co-rich domains transform during OER to structurally different Co3+-rich domains. These domains appear to be crucial for enhancing OER kinetics while exhibiting distinctly different redox properties. Our work emphasizes the necessity of the operando methodology to gain fundamental insight into the activity-determining properties of OER catalysts and presents a promising catalyst concept in which a stable, crystalline structure hosts the disordered and active catalyst phase.

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Language(s): eng - English
 Dates: 2022-01-222022-062022-06-292022-07-13
 Publication Status: Published in print
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.2c00850
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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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: 13 Volume / Issue: 144 (27) Sequence Number: - Start / End Page: 12007 - 12019 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870