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Tuning the Pt/CeO2 Interface by in Situ Variation of the Pt Particle Size

  • Andreas M. Gänzler
    Andreas M. Gänzler
    Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), Engesserstraße 20, 76131 Karlsruhe, Germany
  • Maria Casapu
    Maria Casapu
    Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), Engesserstraße 20, 76131 Karlsruhe, Germany
    More by Maria Casapu
  • Florian Maurer
    Florian Maurer
    Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), Engesserstraße 20, 76131 Karlsruhe, Germany
  • Heike Störmer
    Heike Störmer
    Laboratory for Electron Microscopy, Karlsruhe Institute of Technology (KIT), Engesserstraße 7, 76131 Karlsruhe, Germany
  • Dagmar Gerthsen
    Dagmar Gerthsen
    Laboratory for Electron Microscopy, Karlsruhe Institute of Technology (KIT), Engesserstraße 7, 76131 Karlsruhe, Germany
  • Géraldine Ferré
    Géraldine Ferré
    Université de Lyon, Institut de Recherches sur la Catalyse et l’Environnement de Lyon (IRCELYON), UMR 5256, CNRS, Université Claude Bernard Lyon 1, 2 avenue A. Einstein, 69626 Villeurbanne, France
  • Philippe Vernoux
    Philippe Vernoux
    Université de Lyon, Institut de Recherches sur la Catalyse et l’Environnement de Lyon (IRCELYON), UMR 5256, CNRS, Université Claude Bernard Lyon 1, 2 avenue A. Einstein, 69626 Villeurbanne, France
  • Benjamin Bornmann
    Benjamin Bornmann
    Department of Physics, University of Wuppertal, Gaußstraße 20, 42119 Wuppertal, Germany
  • Ronald Frahm
    Ronald Frahm
    Department of Physics, University of Wuppertal, Gaußstraße 20, 42119 Wuppertal, Germany
    More by Ronald Frahm
  • Vadim Murzin
    Vadim Murzin
    Deutsches Elektronen-Synchrotron (DESY), Notkestraße 85, 22607 Hamburg, Germany
    More by Vadim Murzin
  • Maarten Nachtegaal
    Maarten Nachtegaal
    Paul Scherrer Institute (PSI), PSI Aarebrücke, 5232 Villigen, Switzerland
  • Martin Votsmeier
    Martin Votsmeier
    Umicore AG & Co. KG, Rodenbacher Chaussee 4, 63457 Hanau, Germany
  • , and 
  • Jan-Dierk Grunwaldt*
    Jan-Dierk Grunwaldt
    Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), Engesserstraße 20, 76131 Karlsruhe, Germany
    *E-mail for J.-D.G.: [email protected]
Cite this: ACS Catal. 2018, 8, 6, 4800–4811
Publication Date (Web):April 12, 2018
https://doi.org/10.1021/acscatal.8b00330
Copyright © 2018 American Chemical Society

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    Abstract

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    Pt-CeO2-Al2O3 catalysts play an important role in diesel oxidation and three-way catalysis. In this study, the fast structural dynamics of both platinum and ceria in a 1 wt %Pt/5 wt %CeO2-Al2O3 catalyst prepared by flame spray pyrolysis have been systematically investigated under reducing and oxidizing conditions to elucidate the role of the Pt–CeO2 interface for CO oxidation and fast oxygen storage/release of ceria. The catalyst showed enhanced catalytic activity, particularly after application of a reducing/oxidizing conditioning step at 250 °C, with a pronounced dependence on the reducing agent (C3H6 < H2 < CO). In situ time-resolved X-ray absorption spectroscopy (XAS) at the Ce L3-edge unraveled a dependence of the reduction extent of ceria during temperature-programmed reduction on the noble metal constituent and the applied reducing agent. Dynamic reducing/oxidizing cycling (2% H2 ↔ 10% O2 or 2% CO ↔ 10% O2) at various temperatures (150, 250, and 350 °C) showed that the reducibility of ceria increased at higher temperature and by using a more strongly reducing reaction mixture. This coincides with the trend in catalytic activity. Time-resolved XAS data recorded at the Pt L3-edge and Ce L3-edge during redox cycling revealed a close relationship between the Pt oxidation state and the ceria redox response. The formation of reduced Pt particles was found to induce variations in ceria reducibility under transient conditions and was identified as a decisive prerequisite for ceria reduction at low temperatures. Variations in the extent of ceria reduction during the reducing/oxidizing cycles indicate an evolution of the Pt–ceria interface from an inactive state toward an optimal activated state due to reduction and slight sintering of the noble metal particles. Further growth of Pt particles leads to a decrease in ceria reduction rate due to the smaller Pt–CeO2 interface perimeter. A schematic model illustrating the role of Pt for ceria reducibility is developed and the optimal Pt particle size derived. The results are relevant for various applications, particularly for catalysts operated at low temperature under highly dynamic reaction conditions such as exhaust gas catalysts.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.8b00330.

    • Further Ce L3 XANES data obtained during TPR experiments and redox cycling, Pt L3 XANES data obtained during TPR, evaluation of apparent activation energy for ceria reduction, and estimation of optimal Pt particle size for ceria reduction (PDF)

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