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Atomic-scale insights into surface species of electrocatalysts in three dimensions

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Li,  Tong
Atom Probe Tomography, Microstructure Physics and Alloy Design, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;
Institute for Materials & ZGH, Ruhr-Universität Bochum, Germany;

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Kasian,  Olga
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Cherevko,  Serhiy
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;
Helmholtz-Institute Erlangen-Nuremberg for Renewable Energy (IEK-11), Forschungszentrum Jülich, Egerlandstrasse 3, 91058 Erlangen, Germany;

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Zhang,  Siyuan
Nanoanalytics and Interfaces, Independent Max Planck Research Groups, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Geiger,  Simon
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Scheu,  Christina
Nanoanalytics and Interfaces, Independent Max Planck Research Groups, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Raabe,  Dierk
Microstructure Physics and Alloy Design, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Gault,  Baptiste
Atom Probe Tomography, Microstructure Physics and Alloy Design, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Mayrhofer,  Karl Johann Jakob
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;
Department of Chemical and Biological Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg, 91058 Erlangen, Germany;

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Citation

Li, T., Kasian, O., Cherevko, S., Zhang, S., Geiger, S., Scheu, C., et al. (2018). Atomic-scale insights into surface species of electrocatalysts in three dimensions. Nature Catalysis, 1(4), 300-305. doi:10.1038/s41929-018-0043-3.


Cite as: http://hdl.handle.net/21.11116/0000-0001-E81F-8
Abstract
The topmost atomic layers of electrocatalysts determine the mechanism and kinetics of reactions in many important industrial processes, such as water splitting, chlor-electrolysis or fuel cells. Optimizing the performance of electrocatalysts requires a detailed understanding of surface-state changes during the catalytic process, ideally at the atomic scale. Here, we use atom probe tomography to reveal the three-dimensional structure of the first few atomic layers of electrochemically grown iridium oxide, an efficient electrocatalyst for the oxygen evolution reaction. We unveil the formation of confined, non-stoichiometric Ir-O species during oxygen evolution. These species gradually transform to IrO2, providing improved stability but also a decrease in activity. Additionally, electrochemical growth of oxide in deuterated solutions allowed us to trace hydroxy-groups and water molecules present in the regions of the oxide layer that are favourable for the oxygen evolution and iridium dissolution reactions. Overall, we demonstrate how tomography with near-atomic resolution advances the understanding of complex relationships between surface structure, surface state and function in electrocatalysis. © 2018 The Author(s).