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Title

Tuning the Reactivities of the Heteronuclear [Al<sub>n</sub>V<sub>3−n</sub>O<sub>7−n</sub>]<sup> </sup> (n=1, 2) Cluster Oxides towards Methane by Varying the Composition of the Metal Centers.

Authors

Zhou, Shaodong; Sun, Xiaoyan; Yue, Lei; Schlangen, Maria; Schwarz, Helmut

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. The reactivity of cluster oxides [AlnV3−nO7−n] (n=1, 2) towards methane was tuned by varying the composition of the metal centers. 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. Mechanistic aspects are revealed and the crucial roles of the metal centers are discussed.

Subjects

METHANE; ALUMINUM oxide; VANADIUM oxide; FORMALDEHYDE; CHEMISORPTION; OXIDATION

Publication

Chemistry - A European Journal, 2019, Vol 25, Issue 12, p2967

ISSN

0947-6539

Publication type

Academic Journal

DOI

10.1002/chem.201805908

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