Advanced search
1 file | 310.65 KB

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

(2011) CHEMCATCHEM. 3(1). p.208-212
Author
Organization
Project
HPC-UGent: the central High Performance Computing infrastructure of Ghent University
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.
Keywords
zeolites, kinetics, hydrocarbons, heterogeneous catalysis, density functional calculations, ACIDIC ZEOLITES, CATALYTIC CRACKING, DIMETHYL ETHER, HYDROCARBONS, ALKENES, METHYLATION, MECHANISMS, HSAPO-34, METHYLBENZENES, SELECTIVITY

Downloads

  • (...).pdf
    • full text
    • |
    • UGent only
    • |
    • PDF
    • |
    • 310.65 KB

Citation

Please use this url to cite or link to this publication:

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.
@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},
}

Altmetric
View in Altmetric
Web of Science
Times cited: