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  • Title: Active Ensembles in Methane Dehydroaromatization over Molybdenum/ZSM-5 Zeolite Identified by 2D 1 H-95 Mo Magic Angle Spinning Nuclear Magnetic Resonance Correlation Spectroscopy.
    Author: Gao W, Wang Q, Qi G, Liang J, Wang C, Xu J, Deng F.
    Journal: Angew Chem Int Ed Engl; 2023 Aug 01; 62(31):e202306133. PubMed ID: 37261941.
    Abstract:
    Methane dehydroaromatization (MDA) over Mo-modified zeolite is a potential catalytic route for converting natural gas into valuable aromatics. However, the active species in this reaction are highly complex, involving diverse Mo species, acidic sites of zeolite, and organic molecules. Herein, we apply 1D 95 Mo NMR and 2D 1 H-95 Mo heteronuclear correlation solid-state NMR spectroscopy to directly observe the active ensembles in the confined channels of Mo/ZSM-5 zeolite during the MDA reaction. We monitor the evolution of the spatial correlations of Mo species with the Brønsted acid sites and organic products (olefins and aromatics) in the zeolite channels. We identified two kinds of MoOx Cy species, with the more carbidic one (MoOx Cy -II) exhibiting higher activity for methane activation and benzene formation. The strong spatial interactions between the active Mo species and the organic species in the Mo/ZSM-5 pores are related to the MDA activity.
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