Pt-supported nanocrystalline ceria-zirconia doped with La, Pr or Gd: Factors controlling syngas generation in partial oxidation/autothermal reforming of methane or oxygenates

V. A. Sadykov, N. V. Mezentseva, G. M. Alikina, A. I. Lukashevich, Yu V. Borchert, T. G. Kuznetsova, V. P. Ivanov, S. N. Trukhan, E. A. Paukshtis, V. S. Muzykantov, V. L. Kuznetsov, V. A. Rogov, J. R.H. Ross, E. Kemnitz, C. Mirodatos

Research output: Chapter in Book/Report/Conference proceedingConference contributionpeer-review

Abstract

Nanocrystalline CeO2-ZrO2 (Ce:Zr 1:1) samples doped with La, Pr or Gd cations (containing up to 30 at.%) were prepared via the Pechini route. Pt (1.4 wt.%) was supported via impregnation with H 2PtCl6 solution followed by drying and calcination. The samples' surface features were studied by SIMS and FTIRS of adsorbed CO. The oxygen mobility was characterized by the dynamic oxygen isotope exchange and H2 TPR. Catalytic activity was studied in the flow installation using diluted feeds (0.7% CH4 +0.5% O2 or 1% C 3H6O + 0.5% O2 +0.5% H2O in He). In the selective oxidation of methane (POM), the catalytic activity correlates with Pt dispersion controlled by the oxidized sample's ability to stabilize Pt 2+ cations as precursors of small reactive Pt clusters formed under reaction conditions. This is favoured by a larger doping cation (La) and a developed network of nanodomain boundaries. At comparable Pt dispersion, the highest performance was demonstrated by a La-doped system, which correlates with the highest surface/near-surface oxygen mobility controlled by the strength of Ce-O bonds in the surface layer. In the autothermal reforming of acetone, the activity trends differ from those in POM because of the more prominent role of the oxygen mobility required to prevent surface coking. doped zirconia-ceria, surface features, Pt dispersion, oxygen mobility, selective oxidation of methane, FTIRS, SIMS, Dynamic oxygen isotope exchange, H2 TPR.

Original languageEnglish
Title of host publicationDoped Nanopowders
Subtitle of host publicationSynthesis, Characterisation Applications - Proceedings of Symposium C European Materials Research Society Fall Meeting
PublisherTrans Tech Publications Ltd
Pages239-248
Number of pages10
ISBN (Print)9783908451389
DOIs
Publication statusPublished - 2007
EventSymposium C of the European Materials Research Society, Fall Meeting 2006 - Warsaw, Poland
Duration: 4 Sep 20068 Sep 2006

Publication series

NameSolid State Phenomena
Volume128
ISSN (Print)1012-0394

Conference

ConferenceSymposium C of the European Materials Research Society, Fall Meeting 2006
Country/TerritoryPoland
CityWarsaw
Period4/09/068/09/06

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