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 language | English |
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Pages (from-to) | 1016-1020 |
Journal | Angewandte Chemie - International Edition |
Volume | 57 |
Issue number | 4 |
DOIs | |
Publication status | Published - 2018 |
Externally published | Yes |
Keywords
- dehydroaromatization
- hydrocarbons
- methane
- Mo/ZSM-5
- organocatalysis