Cargando…
Unraveling the Homologation Reaction Sequence of the Zeolite‐Catalyzed Ethanol‐to‐Hydrocarbons Process
Although industrialized, the mechanism for catalytic upgrading of bioethanol over solid‐acid catalysts (that is, the ethanol‐to‐hydrocarbons (ETH) reaction) has not yet been fully resolved. Moreover, mechanistic understanding of the ETH reaction relies heavily on its well‐known “sister‐reaction” the...
Autores principales: | , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2019
|
Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6519145/ https://www.ncbi.nlm.nih.gov/pubmed/30681254 http://dx.doi.org/10.1002/anie.201814268 |
_version_ | 1783418585612288000 |
---|---|
author | Chowdhury, Abhishek Dutta Lucini Paioni, Alessandra Whiting, Gareth T. Fu, Donglong Baldus, Marc Weckhuysen, Bert M. |
author_facet | Chowdhury, Abhishek Dutta Lucini Paioni, Alessandra Whiting, Gareth T. Fu, Donglong Baldus, Marc Weckhuysen, Bert M. |
author_sort | Chowdhury, Abhishek Dutta |
collection | PubMed |
description | Although industrialized, the mechanism for catalytic upgrading of bioethanol over solid‐acid catalysts (that is, the ethanol‐to‐hydrocarbons (ETH) reaction) has not yet been fully resolved. Moreover, mechanistic understanding of the ETH reaction relies heavily on its well‐known “sister‐reaction” the methanol‐to‐hydrocarbons (MTH) process. However, the MTH process possesses a C(1)‐entity reactant and cannot, therefore, shed any light on the homologation reaction sequence. The reaction and deactivation mechanism of the zeolite H‐ZSM‐5‐catalyzed ETH process was elucidated using a combination of complementary solid‐state NMR and operando UV/Vis diffuse reflectance spectroscopy, coupled with on‐line mass spectrometry. This approach establishes the existence of a homologation reaction sequence through analysis of the pattern of the identified reactive and deactivated species. Furthermore, and in contrast to the MTH process, the deficiency of any olefinic‐hydrocarbon pool species (that is, the olefin cycle) during the ETH process is also noted. |
format | Online Article Text |
id | pubmed-6519145 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
spelling | pubmed-65191452019-05-21 Unraveling the Homologation Reaction Sequence of the Zeolite‐Catalyzed Ethanol‐to‐Hydrocarbons Process Chowdhury, Abhishek Dutta Lucini Paioni, Alessandra Whiting, Gareth T. Fu, Donglong Baldus, Marc Weckhuysen, Bert M. Angew Chem Int Ed Engl Communications Although industrialized, the mechanism for catalytic upgrading of bioethanol over solid‐acid catalysts (that is, the ethanol‐to‐hydrocarbons (ETH) reaction) has not yet been fully resolved. Moreover, mechanistic understanding of the ETH reaction relies heavily on its well‐known “sister‐reaction” the methanol‐to‐hydrocarbons (MTH) process. However, the MTH process possesses a C(1)‐entity reactant and cannot, therefore, shed any light on the homologation reaction sequence. The reaction and deactivation mechanism of the zeolite H‐ZSM‐5‐catalyzed ETH process was elucidated using a combination of complementary solid‐state NMR and operando UV/Vis diffuse reflectance spectroscopy, coupled with on‐line mass spectrometry. This approach establishes the existence of a homologation reaction sequence through analysis of the pattern of the identified reactive and deactivated species. Furthermore, and in contrast to the MTH process, the deficiency of any olefinic‐hydrocarbon pool species (that is, the olefin cycle) during the ETH process is also noted. John Wiley and Sons Inc. 2019-02-14 2019-03-18 /pmc/articles/PMC6519145/ /pubmed/30681254 http://dx.doi.org/10.1002/anie.201814268 Text en © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the http://creativecommons.org/licenses/by-nc-nd/4.0/ License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non‐commercial and no modifications or adaptations are made. |
spellingShingle | Communications Chowdhury, Abhishek Dutta Lucini Paioni, Alessandra Whiting, Gareth T. Fu, Donglong Baldus, Marc Weckhuysen, Bert M. Unraveling the Homologation Reaction Sequence of the Zeolite‐Catalyzed Ethanol‐to‐Hydrocarbons Process |
title | Unraveling the Homologation Reaction Sequence of the Zeolite‐Catalyzed Ethanol‐to‐Hydrocarbons Process |
title_full | Unraveling the Homologation Reaction Sequence of the Zeolite‐Catalyzed Ethanol‐to‐Hydrocarbons Process |
title_fullStr | Unraveling the Homologation Reaction Sequence of the Zeolite‐Catalyzed Ethanol‐to‐Hydrocarbons Process |
title_full_unstemmed | Unraveling the Homologation Reaction Sequence of the Zeolite‐Catalyzed Ethanol‐to‐Hydrocarbons Process |
title_short | Unraveling the Homologation Reaction Sequence of the Zeolite‐Catalyzed Ethanol‐to‐Hydrocarbons Process |
title_sort | unraveling the homologation reaction sequence of the zeolite‐catalyzed ethanol‐to‐hydrocarbons process |
topic | Communications |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6519145/ https://www.ncbi.nlm.nih.gov/pubmed/30681254 http://dx.doi.org/10.1002/anie.201814268 |
work_keys_str_mv | AT chowdhuryabhishekdutta unravelingthehomologationreactionsequenceofthezeolitecatalyzedethanoltohydrocarbonsprocess AT lucinipaionialessandra unravelingthehomologationreactionsequenceofthezeolitecatalyzedethanoltohydrocarbonsprocess AT whitinggaretht unravelingthehomologationreactionsequenceofthezeolitecatalyzedethanoltohydrocarbonsprocess AT fudonglong unravelingthehomologationreactionsequenceofthezeolitecatalyzedethanoltohydrocarbonsprocess AT baldusmarc unravelingthehomologationreactionsequenceofthezeolitecatalyzedethanoltohydrocarbonsprocess AT weckhuysenbertm unravelingthehomologationreactionsequenceofthezeolitecatalyzedethanoltohydrocarbonsprocess |