Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, 310027, Hangzhou, P. R. China.
Institut für Chemie, Technische Universität Berlin, Straße des 17. Juni 135, 10623, Berlin, Germany.
Chemistry. 2019 Feb 26;25(12):2967-2971. doi: 10.1002/chem.201805908. Epub 2019 Feb 7.
The thermal gas-phase reactions of [Al VO ] and [AlV O ] with methane have been explored by using Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry complemented by high-level quantum chemical calculations. Both cluster ions chemisorbed methane as the major reaction channels at room temperature. [Al VO ] could break only one C-H bond to liberate CH , whereas [AlV O ] exhibited higher oxidizing ability such that it brings about the selective generation of formaldehyde. Mechanistic aspects are revealed and the crucial roles of the metal centers are discussed.
采用傅里叶变换离子回旋共振（FT-ICR）质谱仪结合高精度量子化学计算，研究了[AlVO]和[AlVO]与甲烷的气相热反应。在室温下，两种团簇离子均通过化学吸附甲烷作为主要反应通道。[AlVO]仅能断裂一个 C-H 键生成 CH，而[AlVO]则表现出更高的氧化能力，能够选择性地生成甲醛。揭示了反应的机理，并讨论了金属中心的关键作用。
