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Tuning the Reactivities of the Heteronuclear [AlnV3−nO7−n]+ (n=1, 2) Cluster Oxides towards Methane by Varying the Composition of the Metal Centers |
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| Authors: | Prof Dr Shaodong Zhou Dr Xiaoyan Sun Dr Lei Yue Dr Maria Schlangen Prof Dr Helmut Schwarz |
| Institution: | 1. Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, 310027 Hangzhou, P. R. China;2. Institut für Chemie, Technische Universität Berlin, Straße des 17. Juni 135, 10623 Berlin, Germany |
| Abstract: | The thermal gas-phase reactions of Al2VO5]+ and AlV2O6]+ 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. Al2VO5]+ could break only one C−H bond to liberate CH3, whereas AlV2O6]+ 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. |
| Keywords: | cluster compounds gas-phase reaction methane activation quantum chemical calculations vanadium |