The Unique Gas-Phase Chemistry of the [AuO]+/CH4 Couple: Selective Oxygen-Atom Transfer to, Rather than Hydrogen-Atom Abstraction from, Methane

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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：2016
• 出版时间：August 26, 2016
• 年：2016
• 卷：55
• 期：36
• 页码：10877-10880
• 全文大小：1534K
• ISSN：1521-3773

文摘

The thermal reaction of [AuO]⁺ with methane has been explored using FT-ICR mass spectrometry complemented by high-level quantum chemical calculations. In contrast to the previously studied congener [CuO]⁺, and to [AgO]⁺, [AuO]⁺ reacts with CH₄ exclusively via oxygen-atom transfer to form CH₃OH, and a novel mechanistic scenario for this selective oxidation process has been revealed. Also, the origin of the inertness of the [AgO]⁺/CH₄ couple has been addressed computationally.