Jump to main content
Jump to site search

Issue 9, 2014
Previous Article Next Article

Ageing induced improvement of methane oxidation activity of Pd/YFeO3

Author affiliations

Abstract

The ageing characteristics of flame-made 2 wt% Pd supported on YFeO3 were analysed in comparison with a Pd/Al2O3–CeO2–ZrO2 three-way catalyst (TWC) with respect to structural changes and catalytic performance for methane oxidation under stoichiometric reaction conditions. Thermal treatment under lean conditions (air, 900 °C) resulted in slight decrease in the methane oxidation activity of the TWC. In marked contrast, YFeO3-supported Pd catalysts exhibit an increase in activity after such treatment. Activity enhancement is even higher when the treatment was performed under stoichiometric conditions (air–fuel equivalence ratio, λ = 1, 900 °C). To explain this observation, in-depth characterization (BET, STEM, OSCC, XAS, and CO chemisorption) of fresh and aged catalysts was performed. Both thermal and stoichiometric ageing cause a severe sintering of the support particles and the phase transformation from hexagonal to orthorhombic YFeO3. Despite the absence of a mixed Pd–YFeO3 phase, the growth of Pd particles appears to be limited under the λ = 1 atmosphere. In contrast to thermally aged catalysts where large PdO particles are formed, well-defined metallic Pd nanoparticles of 10–20 nm are present after stoichiometric ageing along with higher methane oxidation activity. Although it is tempting to conclude that metallic Pd is active for methane oxidation under the given conditions, reversible and periodic partial oxidation of the large metallic particles is observed in modulation excitation high energy X-ray diffraction (HXRD) experiments designed to simulate the oscillating redox conditions experienced during operation. These results indicate that large Pd particles exhibit improved methane oxidation activity but equally confirm that activity under stoichiometric conditions is the result of a delicate equilibrium dictated by the bulk-Pd/surface-PdO pair.

Graphical abstract: Ageing induced improvement of methane oxidation activity of Pd/YFeO3

Back to tab navigation

Publication details

The article was received on 07 Mar 2014, accepted on 10 Apr 2014 and first published on 10 Apr 2014


Article type: Paper
DOI: 10.1039/C4CY00289J
Citation: Catal. Sci. Technol., 2014,4, 2919-2931
  • Open access: Creative Commons BY license
  •   Request permissions

    Ageing induced improvement of methane oxidation activity of Pd/YFeO3

    Y. Lu, S. Keav, V. Marchionni, G. L. Chiarello, A. Pappacena, M. Di Michiel, M. A. Newton, A. Weidenkaff and D. Ferri, Catal. Sci. Technol., 2014, 4, 2919
    DOI: 10.1039/C4CY00289J

    This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material.

    Reproduced material should be attributed as follows:

    • For reproduction of material from NJC:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
    • For reproduction of material from PCCP:
      [Original citation] - Published by the PCCP Owner Societies.
    • For reproduction of material from PPS:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
    • For reproduction of material from all other RSC journals:
      [Original citation] - Published by The Royal Society of Chemistry.

    Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.

Search articles by author

Spotlight

Advertisements