Institut für Chemie, Technische Universität Berlin, Strasse des 17. Juni 135, 10623, Berlin, Germany.
Institute of Theoretical Chemistry, Jilin University, Changchun, 130023, P.R. China.
Angew Chem Int Ed Engl. 2017 Jan 2;56(1):413-416. doi: 10.1002/anie.201610424. Epub 2016 Dec 2.
The thermal gas-phase reactions of the closed-shell heteronuclear metal-oxide clusters [AlCeO ] (x=2-4) with methane have been explored by FT-ICR mass spectrometry and high-level quantum-chemical calculation. Whereas [AlCeO ] and [AlCeO ] are inert towards methane under ambient conditions, [AlCeO ] spontaneously abstracts one hydrogen atom from methane. Mechanistic aspects have been addressed to reveal the reasons for the rather distinct reactivities of the [AlCeO ] /CH couples, and the electronic origins of the unprecedented single hydrogen-atom abstraction from methane by closed-shell [AlCeO ] are discussed.
采用傅里叶变换离子回旋共振质谱和高精度量子化学计算研究了闭壳层异核金属氧化物簇[AlCeO]（x=2-4）与甲烷的气相热反应。虽然[AlCeO]和[AlCeO]在环境条件下对甲烷惰性，但[AlCeO]会自发地从甲烷中提取一个氢原子。研究了反应机理，以揭示[AlCeO]/CH 对不同反应活性的原因，并讨论了闭壳层[AlCeO]前所未有地从甲烷中提取单个氢原子的电子起源。
