期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 38, 页码 16741-16746出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202007283
关键词
bifunctional catalysts; methane dehydroaromatization; reaction mechanisms; solid-state NMR spectroscopy; zeolites
资金
- King Abdullah University of Science and Technology (KAUST)
- IAS, Wuhan University
- TOP-PUNT grant from Netherlands Organization of Scientific Research (NWO) [718.015.001]
Methane dehydroaromatization (MDA) is among the most challenging processes in catalysis science owing to the inherent harsh reaction conditions and fast catalyst deactivation. To improve this process, understanding the mechanism of the initial C-C bond formation is essential. However, consensus about the actual reaction mechanism is still to be achieved. In this work, using advanced magic-angle spinning (MAS) solid-state NMR spectroscopy, we study in detail the early stages of the reaction over a well-dispersed Mo/H-ZSM-5 catalyst. Simultaneous detection of acetylene (i.e., presumably the direct C-C bond-forming product from methane), methylidene, allenes, acetal, and surface-formate species, along with the typical olefinic/aromatic species, allow us to conclude the existence of at least two independent C-H activation pathways. Moreover, this study emphasizes the significance of mobility-dependent host-guest chemistry between an inorganic zeolite and its trapped organic species during heterogeneous catalysis.
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