Double-oxygen-atom transfer in reactions of CemO 2m+ (m=2-6) with C2H2

Xun Lei Ding, Xiao Nan Wu, Yan Xia Zhao, Jia Bi Ma, Sheng Gui He*

*Corresponding author for this work

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Abstract

Cerium oxide cluster cations (CemOn+, m=2-16; n=2m, 2m±1 and 2m±2) are prepared by laser ablation and reacted with acetylene (C2H2) in a fast-flow reactor. A time-of-flight mass spectrometer is used to detect the cluster distribution before and after the reactions. Reactions of stoichiometric CemO 2m+ (m=2-6) with C2H2 produce CemO2m-2+ clusters, which indicates a "double-oxygen-atom transfer" reaction CemO 2m++C2H2→CemO 2m-2++(CHO)2 (ethanedial). A single-oxygen-atom transfer reaction channel is also identified as CemO 2m++C2H2→CemO 2m-1++C2H2O (at least for m=2 and 3). Density functional theory calculations are performed to study reaction mechanisms of Ce2O4++C2H 2, and the calculated results confirm that both the single- and double-oxygen-atom transfer channels are thermodynamically and kinetically favourable.

Original languageEnglish
Pages (from-to)2110-2117
Number of pages8
JournalChemPhysChem
Volume12
Issue number11
DOIs
Publication statusPublished - 1 Aug 2011
Externally publishedYes

Keywords

  • cerium
  • cluster compounds
  • density functional calculations
  • mass spectrometry
  • reaction mechanisms

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Ding, X. L., Wu, X. N., Zhao, Y. X., Ma, J. B., & He, S. G. (2011). Double-oxygen-atom transfer in reactions of CemO 2m+ (m=2-6) with C2H2. ChemPhysChem, 12(11), 2110-2117. https://doi.org/10.1002/cphc.201100216