Unraveling the Nature of Sites Active toward Hydrogen Peroxide Reduction in 
Fe–N–C Catalysts

Choi, Chang Hyuck; Choi, Won Seok; Kasian, Olga; Mechler, Anna Katharina; Sougrati, Moulay Tahar; Brüller, Sebastian; Strickland, Kara; Jia, Qingying; Mukerjee, Sanjeev; Mayrhofer, Karl J. J.; Jaouen, Frédéric

doi:10.1002/anie.201704356

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Unraveling the Nature of Sites Active toward Hydrogen Peroxide Reduction in Fe–N–C Catalysts

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Choi, Chang Hyuck
School of Materials Science and Engineering, Gwangju Institute of Science and Technology, Gwangju, South Korea;
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Choi, Won Seok
Microstructure Physics and Alloy Design, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;
Graduate Institute of Ferrous Technology, Pohang University of Science and Technology, Pohang, South Korea;

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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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Strickland, Kara
Department of Chemistry and Chemical Biology, Northeastern University, Boston, MA, USA;
Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Mayrhofer, Karl J. J.
Helmholtz-Institute Erlangen-Nuremberg for Renewable Energy (IEK-11), Forschungszentrum Jülich, Egerlandstrasse 3, 91058 Erlangen, Germany;
Department of Chemical and Biological Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg, 91058 Erlangen, Germany ;
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Citation

Choi, C. H., Choi, W. S., Kasian, O., Mechler, A. K., Sougrati, M. T., Brüller, S., et al. (2017). Unraveling the Nature of Sites Active toward Hydrogen Peroxide Reduction in Fe–N–C Catalysts. Angewandte Chemie International Edition, 56(30), 8809-8812. doi:10.1002/anie.201704356.

Cite as: https://hdl.handle.net/11858/00-001M-0000-002D-C5D9-0

Abstract

Fe-N-C catalysts with high O-2 reduction performance are crucial for displacing Pt in low-temperature fuel cells. However, insufficient understanding of which reaction steps are catalyzed by what sites limits their progress. The nature of sites were investigated that are active toward H2O2 reduction, a key intermediate during indirect O-2 reduction and a source of deactivation in fuel cells. Catalysts comprising different relative contents of FeNxCy moieties and Fe particles encapsulated in N-doped carbon layers (0-100%) show that both types of sites are active, although moderately, toward H2O2 reduction. In contrast, N-doped carbons free of Fe and Fe particles exposed to the electrolyte are inactive. When catalyzing the ORR, FeNxCy moieties are more selective than Fe particles encapsulated in N-doped carbon. These novel insights offer rational approaches for more selective and therefore more durable Fe-N-C catalysts.