Gas-phase reaction of CeV2O7+ with C2H4: activation of C-C and C-H bonds

Chemphyschem. 2014 Dec 15;15(18):4117-25. doi: 10.1002/cphc.201402347. Epub 2014 Sep 11.

Abstract

The reactivity of metal oxide clusters toward hydrocarbon molecules can be changed, tuned, or controlled by doping. Cerium-doped vanadium cluster cations CeV2O7(+) are generated by laser ablation, mass-selected by a quadrupole mass filter, and then reacted with C2H4 in a linear ion trap reactor. The reaction is characterized by a reflectron time-of-flight mass spectrometer. Three types of reaction channels are observed: 1) single oxygen-atom transfer , 2) double oxygen-atom transfer , and 3) C=C bond cleavage. This study provides the first bimetallic oxide cluster ion, CeV2O7(+), which gives rise to C=C bond cleavage of ethene. Neither Ce(x)O(y)(±) nor V(x)O(y)(±) alone possess the necessary topological and electronic properties to bring about such a reaction.

Keywords: cluster compounds; density functional calculations; gas-phase reactions; mass spectrometry; reaction mechanisms.