On the dynamic nature of Mo sites for methane dehydroaromatization

Ina Vollmer, Bart van der Linden, Samy Ould-Chikh, Antonio Aguilar-Tapia, Irina Yarulina, Edy Abou-Hamad, Yuri G. Sneider, Alma I. Olivos Suarez, Jean-Louis Hazemann, Freek Kapteijn, Jorge Gascon

Research output: Contribution to journalArticlepeer-review

37 Scopus citations

Abstract

The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-MoC nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane (CH). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites.
Original languageEnglish (US)
Pages (from-to)4801-4807
Number of pages7
JournalChemical Science
Volume9
Issue number21
DOIs
StatePublished - 2018

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