Confined carbon mediating dehydroaromatization of methane over Mo/ZSM-5

N. Kosinov, A.S.G. Wijpkema, E. Uslamin, R. Rohling, F.J.A.G. Coumans, B. Mezari, A. Parastaev, A.S. Poryvaev, M.V. Fedin, E.A. Pidko, E.J.M. Hensen

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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.
Original languageEnglish
Pages (from-to)1028–1032
JournalAngewandte Chemie
Volume130
Issue number4
DOIs
Publication statusPublished - 22 Jan 2018

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