Abstract
The thermal gas-phase reactions of the closed-shell heteronuclear metal-oxide clusters [AlCeOx ]+ (x=2-4) with methane have been explored by FT-ICR mass spectrometry and high-level quantum-chemical calculation. Whereas [AlCeO2 ]+ and [AlCeO4 ]+ are inert towards methane under ambient conditions, [AlCeO3 ]+ spontaneously abstracts one hydrogen atom from methane. Mechanistic aspects have been addressed to reveal the reasons for the rather distinct reactivities of the [AlCeOx ]+ /CH4 couples, and the electronic origins of the unprecedented single hydrogen-atom abstraction from methane by closed-shell [AlCeO3 ]+ are discussed.
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