Confined Carbon Mediating Dehydroaromatization of Methane over Mo/ZSM-5

Nikolay Kosinov*, Alexandra S.G. Wijpkema, Evgeny Uslamin, Roderigh Rohling, Ferdy J.A.G. Coumans, Brahim Mezari, Alexander Parastaev, Evgeny A. Pidko, Emiel J.M. Hensen, More Authors

*Corresponding author for this work

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68 Citations (Scopus)

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)1016-1020
JournalAngewandte Chemie - International Edition
Volume57
Issue number4
DOIs
Publication statusPublished - 2018
Externally publishedYes

Keywords

  • dehydroaromatization
  • hydrocarbons
  • methane
  • Mo/ZSM-5
  • organocatalysis

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