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Oxidation State and Dielectric Properties of Ceria-Based Catalysts by Complementary Microwave Cavity Perturbation and X-Ray Absorption Spectroscopy Measurements

  • C. Steiner
  • A. M. Gänzler
  • M. Zehentbauer
  • G. Hagen
  • M. Casapu
  • S. Müller
  • J.-D. Grunwaldt
  • R. Moos
Original Paper
  • 15 Downloads

Abstract

The three-way catalytic converter (TWC) has become an integral part of the modern exhaust gas aftertreatment for gasoline engines. Some years ago, radio frequency technology has been successfully tested for monitoring and controlling ceria based TWC oxygen storage by contactless measuring the dielectric catalyst properties inside a cavity resonator. Applying the cavity perturbation method, we present results on CeO2, the oxygen storage component of three-way catalysts, and on differently prepared Pt–ceria model catalysts and combine it with in situ X-ray absorption spectroscopic (XAS) measurements conducted at the Ce L3-edge. The dielectric properties of the oxidized and reduced Pt–ceria and pure ceria powders were determined at 1.2 GHz between 250 and 550 °C. As the experiments show, the reduction of the material changes both, the polarization and the occurring dielectric losses. The complementary in situ XAS measurements, which allow monitoring variations in the redox state of ceria, gave a precise evaluation of the ceria reduction and oxidation. In addition, a substantial improvement of the low-temperature reducibility of ceria in the presence of Pt was demonstrated by both measurement techniques, in agreement with earlier studies. Furthermore, time resolved XAS data obtained during reducing/oxidizing cycles at 250 °C and 350 °C unraveled the faster and more pronounced reduction of ceria at higher temperature. Both methods proved to be valuable methods to provide insight into the oxygen storage and release process of ceria based materials, and capable to discriminate the impact of the noble metal or the ceria surface area in great detail, even under dynamic conditions, which is highly relevant for studying the function of state-of-the art three-way catalysis and giving input for OSC modeling studies.

Keywords

Ceria Oxygen storage capacity (OSC) Three-way catalyst (TWC) Exhaust gas aftertreatment Cavity perturbation Microwave X-ray absorption spectroscopy 

Notes

Acknowledgements

J.-D. Grunwaldt thanks the German Federal Ministry for Economic Affairs and Energy (BMWi: 19U15014B) for financial support of the ORCA project within the DEUFRAKO program as well as the Ministry for Science, Research and Art of Baden-Württemberg for funding for MEMO-SENS-CAT. Ralf Moos acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG Grant MO 1060/29-1). The group of Prof. M. Türk (ITTK, KIT) is acknowledged for the support provided to SM during the preparation of the SFRD catalyst. The SLS is acknowledged for providing beamtime. We thank the following people for their support: Angela Beilmann (BET, KIT), Florian Maurer, Abhijeet Gaur, Dmitry Doronkin (beamtime support, ITCP, KIT), Heike Störmer and Radian Popescu (electron microscopy, LEM, KIT) and Thomas Bergfeldt (elemental analysis, IAM, KIT), as well as Maarten Nachtegaal, Olga Safonova and Urs Vogelsang (SuperXAS beamline, SLS, PSI). Additionally, we also thank Ingo Horn (Institute for Mineralogy, Leibniz University Hannover) for the support on LA-ICP-MS.

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Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2018

Authors and Affiliations

  • C. Steiner
    • 1
  • A. M. Gänzler
    • 2
  • M. Zehentbauer
    • 1
  • G. Hagen
    • 1
  • M. Casapu
    • 1
  • S. Müller
    • 2
  • J.-D. Grunwaldt
    • 2
  • R. Moos
    • 1
  1. 1.Department of Functional Materials, Bayreuth Engine Research Center (BERC)University of BayreuthBayreuthGermany
  2. 2.Institute for Chemical Technology and Polymer ChemistryKarlsruhe Institute of Technology (KIT)KarlsruheGermany

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