Samenvatting
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.
Originele taal-2 | Engels |
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Pagina's (van-tot) | 1028–1032 |
Tijdschrift | Angewandte Chemie |
Volume | 130 |
Nummer van het tijdschrift | 4 |
DOI's | |
Status | Gepubliceerd - 22 jan. 2018 |