Confined Carbon Mediating Dehydroaromatization of Methane over Mo/ZSM‐5 |
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| Authors: | Dr Nikolay Kosinov Alexandra S G Wijpkema Evgeny Uslamin Roderigh Rohling Ferdy J A G Coumans Brahim Mezari Alexander Parastaev Artem S Poryvaev Dr Matvey V Fedin Dr Evgeny A Pidko Prof Emiel J M Hensen |
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| Institution: | 1. Laboratory of Inorganic Materials Chemistry, Eindhoven University of Technology, Eindhoven, The Netherlands;2. International Tomography Center SB RAS and, Novosibirsk State University, Novosibirsk, Russia |
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| Abstract: | Non‐oxidative dehydroaromatization of methane (MDA) is a promising catalytic process for direct valorization of natural gas to liquid hydrocarbons. The application of this reaction in practical technology is hindered by a lack of understanding about the mechanism and nature of the active sites in benchmark zeolite‐based Mo/ZSM‐5 catalysts, which precludes the solution of problems such as rapid catalyst deactivation. By applying spectroscopy and microscopy, it is shown that the active centers in Mo/ZSM‐5 are partially reduced single‐atom Mo sites stabilized by the zeolite framework. By combining a pulse reaction technique with isotope labeling of methane, MDA is shown to be governed by a hydrocarbon pool mechanism in which benzene is derived from secondary reactions of confined polyaromatic carbon species with the initial products of methane activation. |
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| Keywords: | organocatalysis dehydroaromatization hydrocarbons methane Mo/ZSM-5 |
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