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Full theoretical cycle for both Ethene and Propene formation during Methanol-to-Olefin conversion in H-ZSM-5

David Lesthaeghe UGent, Jeroen Van der Mynsbrugge UGent, Matthias Vandichel UGent, Michel Waroquier UGent and Veronique Van Speybroeck UGent (2011) CHEMCATCHEM. 3(1). p.208-212
abstract
The methanol-to-olefin (MTO) process, catalyzed by acidic zeolites such as H-ZSM-5, provides an increasingly important alternative to the production of light olefins from crude oil. However, the various mechanistic proposals for methanol-to-olefin conversion have been strongly disputed for the past several decades. This work provides theoretical evidence that the experimentally suggested 'alkene cycle', part of a co-catalytic hydrocarbon pool, offers a viable path to the production of both propene and ethene, in stark contrast to the often-proposed direct mechanisms. This specific proposal hinges on repeated methylation reactions of alkenes, starting from propene, which occur easily within the zeolite environment. Subsequent cracking steps regenerate the original propene molecule, while also forming new propene and ethene molecules as primary products. Because the host framework stabilizes intermediate carbenium ions, isomerization and de-protonation reactions are extremely fast. Combined with earlier joint experimental and theoretical work on polymethylbenzenes as active hydrocarbon pool species, it is clear that, in zeolite H-ZSM-5, multiple parallel and interlinked routes operate on a competitive basis.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
zeolites, kinetics, hydrocarbons, heterogeneous catalysis, density functional calculations, ACIDIC ZEOLITES, CATALYTIC CRACKING, DIMETHYL ETHER, HYDROCARBONS, ALKENES, METHYLATION, MECHANISMS, HSAPO-34, METHYLBENZENES, SELECTIVITY
journal title
CHEMCATCHEM
ChemCatChem
volume
3
issue
1
pages
208 - 212
Web of Science type
Article
Web of Science id
000285888500026
JCR category
CHEMISTRY, PHYSICAL
JCR impact factor
5.207 (2011)
JCR rank
24/129 (2011)
JCR quartile
1 (2011)
ISSN
1867-3880
DOI
10.1002/cctc.201000286
project
HPC-UGent: the central High Performance Computing infrastructure of Ghent University
language
English
UGent publication?
yes
classification
A1
copyright statement
I have transferred the copyright for this publication to the publisher
id
1154842
handle
http://hdl.handle.net/1854/LU-1154842
date created
2011-02-18 08:53:42
date last changed
2013-09-17 10:46:27
@article{1154842,
  abstract     = {The methanol-to-olefin (MTO) process, catalyzed by acidic zeolites such as H-ZSM-5, provides an increasingly important alternative to the production of light olefins from crude oil. However, the various mechanistic proposals for methanol-to-olefin conversion have been strongly disputed for the past several decades. This work provides theoretical evidence that the experimentally suggested 'alkene cycle', part of a co-catalytic hydrocarbon pool, offers a viable path to the production of both propene and ethene, in stark contrast to the often-proposed direct mechanisms. This specific proposal hinges on repeated methylation reactions of alkenes, starting from propene, which occur easily within the zeolite environment. Subsequent cracking steps regenerate the original propene molecule, while also forming new propene and ethene molecules as primary products. Because the host framework stabilizes intermediate carbenium ions, isomerization and de-protonation reactions are extremely fast. Combined with earlier joint experimental and theoretical work on polymethylbenzenes as active hydrocarbon pool species, it is clear that, in zeolite H-ZSM-5, multiple parallel and interlinked routes operate on a competitive basis.},
  author       = {Lesthaeghe, David and Van der Mynsbrugge, Jeroen and Vandichel, Matthias and Waroquier, Michel and Van Speybroeck, Veronique},
  issn         = {1867-3880},
  journal      = {CHEMCATCHEM},
  keyword      = {zeolites,kinetics,hydrocarbons,heterogeneous catalysis,density functional calculations,ACIDIC ZEOLITES,CATALYTIC CRACKING,DIMETHYL ETHER,HYDROCARBONS,ALKENES,METHYLATION,MECHANISMS,HSAPO-34,METHYLBENZENES,SELECTIVITY},
  language     = {eng},
  number       = {1},
  pages        = {208--212},
  title        = {Full theoretical cycle for both Ethene and Propene formation during Methanol-to-Olefin conversion in H-ZSM-5},
  url          = {http://dx.doi.org/10.1002/cctc.201000286},
  volume       = {3},
  year         = {2011},
}

Chicago
Lesthaeghe, David, Jeroen Van der Mynsbrugge, Matthias Vandichel, Michel Waroquier, and Veronique Van Speybroeck. 2011. “Full Theoretical Cycle for Both Ethene and Propene Formation During Methanol-to-Olefin Conversion in H-ZSM-5.” Chemcatchem 3 (1): 208–212.
APA
Lesthaeghe, David, Van der Mynsbrugge, J., Vandichel, M., Waroquier, M., & Van Speybroeck, V. (2011). Full theoretical cycle for both Ethene and Propene formation during Methanol-to-Olefin conversion in H-ZSM-5. CHEMCATCHEM, 3(1), 208–212.
Vancouver
1.
Lesthaeghe D, Van der Mynsbrugge J, Vandichel M, Waroquier M, Van Speybroeck V. Full theoretical cycle for both Ethene and Propene formation during Methanol-to-Olefin conversion in H-ZSM-5. CHEMCATCHEM. 2011;3(1):208–12.
MLA
Lesthaeghe, David, Jeroen Van der Mynsbrugge, Matthias Vandichel, et al. “Full Theoretical Cycle for Both Ethene and Propene Formation During Methanol-to-Olefin Conversion in H-ZSM-5.” CHEMCATCHEM 3.1 (2011): 208–212. Print.