Time-Resolved, In Situ DRIFTS/EDE/MS Studies on Alumina-Supported Rhodium Catalysts: Effects of Ceriation and Zirconiation on Rhodium-CO Interactions

Anna B. Kroner, Mark A. Newton*, Moniek Tromp, Otello M. Roscioni, Andrea E. Russell, Andrew J. Dent, Carmelo Prestipino, John Evans

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

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Abstract

The effects of ceria and zirconia on the structure-function properties of supported rhodium catalysts (1.6 and 4 wt% Rh/gamma-Al2O3 ) during CO exposure are described. Ceria and zirconia are introduced through two preparation methods: 1) ceria is deposited on gamma-Al2O3 from [Ce(acac)(3)] and rhodium metal is subsequently added, and 2) through the controlled surface modification (CSM) technique, which involves the decomposition of [M(acac)(x)] (M=Ce, x=3; M=Zr, x=4) on Rh/gamma-Al2O3 . The structure-function correlations of ceria and/or zirconia-doped rhodium catalysts are investigated by diffuse reflectance infrared Fourier-transform spectroscopy/energy-dispersive extended X-ray absorption spectroscopy/mass spectrometry (DRIFTS/EDE/MS) under time-resolved, in situ conditions. CeOx and ZrO2 facilitate the protection of Rh particles against extensive oxidation in air and CO. Larger Rh core particles of ceriated and zirconiated Rh catalysts prepared by CSM are observed and compared with Rh/gamma-Al2O3 samples, whereas supported Rh particles are easily disrupted by CO forming mononuclear Rh geminal dicarbonyl species. DRIFTS results indicate that, through the interaction of CO with ceriated Rh particles, a significantly larger amount of linear CO species form; this suggests the predominance of a metallic Rh phase.

Original languageEnglish
Pages (from-to)3049-3059
Number of pages11
JournalChemphyschem
Volume15
Issue number14
DOIs
Publication statusPublished - 6-Oct-2014
Externally publishedYes

Keywords

  • CEO2-ZRO2 SOLID-SOLUTIONS
  • CARBON-MONOXIDE
  • RH CATALYSTS
  • INFRARED-SPECTROSCOPY
  • CHEMISORBED CO
  • SURFACE
  • OXIDATION
  • REDUCTION
  • PARTICLES
  • NO

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