期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 51, 页码 15840-15845出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201608643
关键词
methanol-to-olefin reaction; operando spectroscopy; reaction mechanisms; solid-state NMR spectroscopy; zeolites
资金
- European Research Council (ERC) [321140]
- NWO (Middelgroot program) [700.58.102]
- Deanship of Scientific Research (DSR) of King Abdulaziz University [T-002-431]
Methanol-to-olefin (MTO) catalysis is a very active field of research because there is a wide variety of sometimes conflicting mechanistic proposals. An example is the ongoing discussion on the initial C-C bond formation from methanol during the induction period of the MTO process. By employing a combination of solid-state NMR spectroscopy with UV/Vis diffuse reflectance spectroscopy and mass spectrometry on an active H-SAPO-34 catalyst, we provide spectroscopic evidence for the formation of surface acetate and methyl acetate, as well as dimethoxymethane during the MTO process. As a consequence, new insights in the formation of the first C-C bond are provided, suggesting a direct mechanism may be operative, at least in the early stages of the MTO reaction.
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