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Active Ensembles in Methane Dehydroaromatization over Molybdenum/ZSM-5 Zeolite Identified by 2D 1H-95Mo Magic Angle Spinning Nuclear Magnetic Resonance Correlation Spectroscopy

 Date:2023/6/12 15:28:47 Views:Times


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 95Mo NMR and 2D 1H-95Mo 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 identify two kinds of MoOxCy species, with the more carbidic one (MoOxCy-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.



中国科学院精密测量科学与技术创新研究院 (中国科学院武汉物理与数学研究所) 邓风课题组
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