On the Origin of the Remarkably Variable Reactivities of [AlCeOx]+ (x=2-4) towards Methane as a Function of Oxygen Content
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- 作者：Dr. Shaodong Zhou ; Prof. Dr. Jilai Li ; Dr. Maria Schlangen and Prof. Dr. Helmut Schwarz
- 刊名：Angewandte Chemie International Edition
- 出版年：2017
- 出版时间：January 2, 2017
- 年：2017
- 卷：56
- 期：1
- 页码：413-416
- 全文大小：1806K
- ISSN：1521-3773
文摘
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.