Initial Carbon-Carbon Bond Formation during the Early Stages of the Methanol-to-Olefin Process Proven by Zeolite-Trapped Acetate and Methyl Acetate

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2016-12-19

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Chowdhury, Abhishek DuttaISNI 000000050599307X
Houben, KISNI 000000039586206X
Whiting, G.T.ISNI 0000000427335898
Mokhtar, Mohamed
Asiri, Abdullah M
Al-Thabaiti, Shaeel A
Basahel, Suliman N
Baldus, MarcISNI 0000000139673796
Weckhuysen, B.M.ORCID 0000-0001-5245-1426ISNI 0000000110540180

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Abstract

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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Chowdhury, A D, Houben, K, Whiting, G T, Mokhtar, M, Asiri, A M, Al-Thabaiti, S A, Basahel, S N, Baldus, M & Weckhuysen, B M 2016, 'Initial Carbon-Carbon Bond Formation during the Early Stages of the Methanol-to-Olefin Process Proven by Zeolite-Trapped Acetate and Methyl Acetate', Angewandte Chemie-International Edition, vol. 55, no. 51, pp. 15840-15845. https://doi.org/10.1002/anie.201608643