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Operando X-ray Absorption Spectroscopy Study During Conditioning of Pt-Based Catalysts and Its Implications for CO Oxidation

  • Andreas M. Gänzler
    Andreas M. Gänzler
    Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), Engesserstr. 20, Karlsruhe 76131, Germany
  • Benjamin Betz
    Benjamin Betz
    Umicore AG & Co. KG, Rodenbacher Chaussee 4, Hanau 63457, Germany
  • Sina Baier-Stegmaier
    Sina Baier-Stegmaier
    Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), Engesserstr. 20, Karlsruhe 76131, Germany
    Department of Physics, Technical University of Denmark (DTU), Fysikvej 307, Kongens Lyngby 2800, Denmark
  • Stéphanie Belin
    Stéphanie Belin
    Synchrotron Soleil, L’Orme des Merisiers, BP48, Saint Aubin, Gif-sur Yvette CEDEX 91192, France
  • Valérie Briois
    Valérie Briois
    Synchrotron Soleil, L’Orme des Merisiers, BP48, Saint Aubin, Gif-sur Yvette CEDEX 91192, France
  • Martin Votsmeier
    Martin Votsmeier
    Umicore AG & Co. KG, Rodenbacher Chaussee 4, Hanau 63457, Germany
  • , and 
  • Maria Casapu*
    Maria Casapu
    Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), Engesserstr. 20, Karlsruhe 76131, Germany
    *Email: [email protected]
    More by Maria Casapu
Cite this: J. Phys. Chem. C 2020, 124, 37, 20090–20100
Publication Date (Web):August 18, 2020
https://doi.org/10.1021/acs.jpcc.0c04740
Copyright © 2020 American Chemical Society
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Abstract

The impact of catalyst pretreatment and its role in diesel oxidation catalysts was systematically studied by comparing the performance, CO adsorption characteristics, oxidation state, and local structure of Pt for Pt/CeO2-Al2O3 and Pt/Al2O3. The catalysts were characterized during oxidizing and reducing conditioning (conventional/reducing pulses) and the subsequent CO oxidation light-offs by operando X-ray absorption spectroscopy (XAS) and insitu diffuse reflectance infrared Fourier transform spectroscopy. The results indicate that a reducing pretreatment substantially enhances the CO oxidation activity of the ceria-based catalyst (70 °C lower light-off temperature). Operando XAS uncovered the highly dynamic nature of the Pt state in both catalysts. The oxidation state and particle size gradually change, and high CO oxidation activity was only observed after a partial reduction of the noble metal. Particularly, the oxidizing conditioning step resulted in a different noble metal response depending on the carrier material. Furthermore, pronounced differences were identified by correlating the Pt structure and catalytic activity: While for Pt/Al2O3, high activity was not observed when Pt was still covered by CO, high CO conversion (>80%) was encountered for Pt/CeO2-Al2O3 already at low temperatures, demonstrating the absence of a CO inhibition effect. The data underline the prominent role of the Pt–CeO2 interface to circumvent Pt self-poisoning by CO.

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  • Additional information on the experimental conditions for the catalytic tests, in situ DRIFT experiments, and operando XAS results (PDF)

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Cited By


This article is cited by 3 publications.

  1. Florian Maurer, Andreas Gänzler, Patrick Lott, Benjamin Betz, Martin Votsmeier, Stéphane Loridant, Philippe Vernoux, Vadim Murzin, Benjamin Bornmann, Ronald Frahm, Olaf Deutschmann, Maria Casapu, Jan-Dierk Grunwaldt. Spatiotemporal Investigation of the Temperature and Structure of a Pt/CeO2 Oxidation Catalyst for CO and Hydrocarbon Oxidation during Pulse Activation. Industrial & Engineering Chemistry Research 2021, 60 (18) , 6662-6675. https://doi.org/10.1021/acs.iecr.0c05798
  2. Xiaoqing Feng, Zilin Wang, Long Mu, Zhilin Chen, Jinhu Liang, Chao Xiao. The different evolution behaviors of carbonate-like species on Pt/CeO2 and Pt/Al2O3 by in situ DRIFTS-MS study. Catalysis Today 2021, 5 https://doi.org/10.1016/j.cattod.2021.11.009
  3. Paolo Dolcet, Florian Maurer, Maria Casapu, Jan-Dierk Grunwaldt. Insights into the Structural Dynamics of Pt/CeO2 Single-Site Catalysts during CO Oxidation. Catalysts 2021, 11 (5) , 617. https://doi.org/10.3390/catal11050617