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Wiley, Angewandte Chemie International Edition, 51(55), p. 15840-15845, 2016

DOI: 10.1002/anie.201608643

Wiley, Angewandte Chemie, 51(128), p. 16072-16077, 2016

DOI: 10.1002/ange.201608643

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

Journal article published in 2016 by Abhishek Dutta Chowdhury, Klaartje Houben ORCID, Gareth T. Whiting, Mohamed Mokhtar, Abdullah M. Asiri ORCID, Shaeel A. Al-Thabaiti, Suliman N. Basahel, Marc Baldus, Bert M. Weckhuysen
This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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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.