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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

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 co...

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Autores principales: Chowdhury, Abhishek Dutta, Houben, Klaartje, Whiting, Gareth T., Mokhtar, Mohamed, Asiri, Abdullah M., Al‐Thabaiti, Shaeel A., Basahel, Suliman N., Baldus, Marc, Weckhuysen, Bert M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2016
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5214583/
https://www.ncbi.nlm.nih.gov/pubmed/27805783
http://dx.doi.org/10.1002/anie.201608643
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author Chowdhury, Abhishek Dutta
Houben, Klaartje
Whiting, Gareth T.
Mokhtar, Mohamed
Asiri, Abdullah M.
Al‐Thabaiti, Shaeel A.
Basahel, Suliman N.
Baldus, Marc
Weckhuysen, Bert M.
author_facet Chowdhury, Abhishek Dutta
Houben, Klaartje
Whiting, Gareth T.
Mokhtar, Mohamed
Asiri, Abdullah M.
Al‐Thabaiti, Shaeel A.
Basahel, Suliman N.
Baldus, Marc
Weckhuysen, Bert M.
author_sort Chowdhury, Abhishek Dutta
collection PubMed
description 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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spelling pubmed-52145832017-01-18 Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate Chowdhury, Abhishek Dutta Houben, Klaartje Whiting, Gareth T. Mokhtar, Mohamed Asiri, Abdullah M. Al‐Thabaiti, Shaeel A. Basahel, Suliman N. Baldus, Marc Weckhuysen, Bert M. Angew Chem Int Ed Engl Communications 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. John Wiley and Sons Inc. 2016-11-02 2016-12-19 /pmc/articles/PMC5214583/ /pubmed/27805783 http://dx.doi.org/10.1002/anie.201608643 Text en © 2016 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution‐NonCommercial (http://creativecommons.org/licenses/by-nc/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.
spellingShingle Communications
Chowdhury, Abhishek Dutta
Houben, Klaartje
Whiting, Gareth T.
Mokhtar, Mohamed
Asiri, Abdullah M.
Al‐Thabaiti, Shaeel A.
Basahel, Suliman N.
Baldus, Marc
Weckhuysen, Bert M.
Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate
title Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate
title_full Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate
title_fullStr Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate
title_full_unstemmed Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate
title_short Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate
title_sort initial carbon–carbon bond formation during the early stages of the methanol‐to‐olefin process proven by zeolite‐trapped acetate and methyl acetate
topic Communications
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5214583/
https://www.ncbi.nlm.nih.gov/pubmed/27805783
http://dx.doi.org/10.1002/anie.201608643
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