Confined carbon mediates non-oxidative dehydroaromatization of methane over molybdenum ZSM-5 zeolite

Autors: Пидько Е.А., 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.J.M. Hensen

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.

DOI:10.1002/anie.201711098

Read Full Here:

https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.201711098