An investigation of possible mechanisms of the water-gas shift reaction over a ZrO2-supported Pt catalyst

Daniele Tibiletti, Frederic Meunier, Alexandre Goguet, D. Reid, Robbie Burch, M. Boaro, M. Vicario, A. Trovarelli

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95 Citations (Scopus)

Abstract

The present work investigates the reactivity of the surface species observable by in situ DRIFTS formed over a Pt/ZrO2 during the water-gas shift (WGS) reaction. A DRIFTS cell/mass spectrometer system was operated at the chemical steady state during isotopic transients to yield information about the true nature (i.e., main reaction intermediate or spectators) of adsorbates. Only carbonyl and formate species were observed by DRIFTS under reaction conditions; the surface coverage of carbonate species was negligible. Isotopic transient kinetic analyses revealed that formates exchanged uniformly according to a first-order law, suggesting that most formates observed by DRIFTS were of the same reactivity. In addition, the time scale of the exchange of the reaction product CO2 was significantly shorter than that of the surface formates. Therefore, a formate route based on the formates as detected by DRIFTS can be ruled out as the main reaction pathway in the present case. The number of precursors of the reaction product CO2 was smaller than the number of surface Pt atoms, suggesting that carbonyl species or some \
Original languageEnglish
Pages (from-to)183-191
Number of pages9
JournalJournal of Catalysis
Volume244
Issue number2
DOIs
Publication statusPublished - 10 Dec 2006

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology

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