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  Surface Chemistry of Perovskite-Type Electrodes during High Temperature CO2 Electrolysis Investigated by Operando Photoelectron Spectroscopy

Opitz, A. K., Nenning, A., Rameshan, C., Kubicek, M., Götsch, T., Blume, R., et al. (2017). Surface Chemistry of Perovskite-Type Electrodes during High Temperature CO2 Electrolysis Investigated by Operando Photoelectron Spectroscopy. ACS Applied Materials and Interfaces, 9(41), 35847-35860. doi:10.1021/acsami.7b10673.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-FCED-B Version Permalink: http://hdl.handle.net/21.11116/0000-0000-7615-4
Genre: Journal Article

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2017
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 Creators:
Opitz, Alexander K.1, Author
Nenning, Andreas1, Author
Rameshan, Christoph2, Author
Kubicek, Markus1, Author
Götsch, Thomas3, Author
Blume, Raoul4, Author              
Hävecker, Michael4, Author              
Knop-Gericke, Axel4, Author              
Rupprechter, Günther2, Author              
Klötzer, Bernhard3, Author
Fleig, Jürgen1, Author
Affiliations:
1Vienna University of Technology, Institute of Chemical Technologies and Analytics, Getreidemarkt 9/164-EC, 1060 Vienna, Austria, escidoc:persistent22              
2Vienna University of Technology, Institute of Materials Chemistry, escidoc:persistent22              
3University of Innsbruck, Institute of Physical Chemistry, Innrain 80-82, 6020 Innsbruck, Austria, escidoc:persistent22              
4Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, escidoc:24023              

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 Abstract: Any substantial move of energy sources from fossil fuels to renewable resources requires large scale storage of excess energy, for example via power to fuel processes. In this respect electrochemical reduction of CO2 may become very important, since it offers a method of sustainable CO production, which is a crucial prerequisite for synthesis of sustainable fuels. Carbon dioxide reduction in solid oxide electrolysis cells (SOECs) is particularly promising owing to the high operating temperature, which leads to both improved thermodynamics and fast kinetics. Additionally, compared to purely chemical CO formation on oxide catalysts, SOECs have the outstanding advantage that the catalytically active oxygen vacancies are continuously formed at the counter electrode, move to the working electrode where they reactivate the oxide surface without the need of a preceding chemical (e.g. by H2) or thermal reduction step. In the present work, the surface chemistry of (La,Sr)FeO3-δ and (La,Sr)CrO3-δ based perovskite-type electrodes was studied during electrochemical CO2 reduction by means of near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) at SOEC operating temperatures. These measurements revealed the formation of a carbonate intermediate, which develops on the oxide surface only upon cathodic polarization (i.e. under sufficiently reducing conditions). The amount of these adsorbates increases with increasing oxygen vacancy concentration of the electrode material, thus suggesting vacant oxygen lattice sites as the predominant adsorption sites for carbon dioxide. The correlation of carbonate coverage and cathodic polarization indicates that an additional electron transfer is required to form the carbonate radical and thus to activate CO2 on the oxide surface. The results also suggest that acceptor doped oxides with high electron concentration and high oxygen vacancy concentration may be particularly suited for CO2 reduction. In contrast to water splitting, the CO2 electrolysis reaction was not significantly affected by metallic particles, which were exsolved from the perovskite electrodes upon cathodic polarization. Carbon formation on the electrode surface was only observed under very strong cathodic conditions and the carbon could be easily removed by retracting the applied voltage without damaging the electrode, which is particularly promising from an application point of view.

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Language(s): eng - English
 Dates: 2017-07-202017-09-212017-09-212017-10-18
 Publication Status: Published in print
 Pages: 14
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acsami.7b10673
 Degree: -

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Title: ACS Applied Materials and Interfaces
  Abbreviation : ACS Appl. Mater. Interfaces
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 14 Volume / Issue: 9 (41) Sequence Number: - Start / End Page: 35847 - 35860 Identifier: ISSN: 1944-8244
CoNE: http://pubman.mpdl.mpg.de/cone/journals/resource/1944-8244