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Molecular dynamics kinetic study on the zeolite-catalyzed benzene methylation in ZSM-5

(2013) ACS CATALYSIS. 3(11). p.2556-2567
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Abstract
The methylation of arenes is a key step in the production of hydrocarbons from methanol over acidic zeolites. We performed ab initio static and molecular dynamics free energy simulations of benzene methylation in H-ZSM-S to determine the factors that influence the reaction kinetics. Special emphasis is given to the effect of the surrounding methanol molecules on the methylation kinetics. It is found that for higher methanol loadings, methylation may also occur from a protonated methanol cluster, indicating that the exact location of the Bronsted acid site is not essential for the zeolite-catalyzed methylation reaction. However, methylations from a protonated methanol cluster exhibit higher free energy barriers than a methylation from a single methanol molecule. Finally, comparison with a pure methanol solvent reaction environment indicates that the main role of the zeolite during the methylation of benzene is to provide the acidic proton and to create a polar environment for the reaction. The metadynamics approach, which is specifically designed to sample rare events, allows exploring new reaction pathways, which take into account the flexibility of the framework and additional guest molecules in the pores and channels of the zeoli
Keywords
ZSM-5, methylation, methanol to olefins, benzene, methanol clusters, metadynamics, TO-OLEFIN PROCESS, DIMETHYL ETHER, REACTION-MECHANISM, CO-REACTION, AB-INITIO, HYDROCARBON FORMATION, PRODUCT SELECTIVITY, SHAPE-SELECTIVITY, ACIDIC ZEOLITES, LIGHT ALKENES

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MLA
Moors, Samuel, Kristof De Wispelaere, Jeroen Van der Mynsbrugge, et al. “Molecular Dynamics Kinetic Study on the Zeolite-catalyzed Benzene Methylation in ZSM-5.” ACS CATALYSIS 3.11 (2013): 2556–2567. Print.
APA
Moors, Samuel, De Wispelaere, K., Van der Mynsbrugge, J., Waroquier, M., & Van Speybroeck, V. (2013). Molecular dynamics kinetic study on the zeolite-catalyzed benzene methylation in ZSM-5. ACS CATALYSIS, 3(11), 2556–2567.
Chicago author-date
Moors, Samuel, Kristof De Wispelaere, Jeroen Van der Mynsbrugge, Michel Waroquier, and Veronique Van Speybroeck. 2013. “Molecular Dynamics Kinetic Study on the Zeolite-catalyzed Benzene Methylation in ZSM-5.” Acs Catalysis 3 (11): 2556–2567.
Chicago author-date (all authors)
Moors, Samuel, Kristof De Wispelaere, Jeroen Van der Mynsbrugge, Michel Waroquier, and Veronique Van Speybroeck. 2013. “Molecular Dynamics Kinetic Study on the Zeolite-catalyzed Benzene Methylation in ZSM-5.” Acs Catalysis 3 (11): 2556–2567.
Vancouver
1.
Moors S, De Wispelaere K, Van der Mynsbrugge J, Waroquier M, Van Speybroeck V. Molecular dynamics kinetic study on the zeolite-catalyzed benzene methylation in ZSM-5. ACS CATALYSIS. 2013;3(11):2556–67.
IEEE
[1]
S. Moors, K. De Wispelaere, J. Van der Mynsbrugge, M. Waroquier, and V. Van Speybroeck, “Molecular dynamics kinetic study on the zeolite-catalyzed benzene methylation in ZSM-5,” ACS CATALYSIS, vol. 3, no. 11, pp. 2556–2567, 2013.
@article{4227484,
  abstract     = {The methylation of arenes is a key step in the production of hydrocarbons from methanol over acidic zeolites. We performed ab initio static and molecular dynamics free energy simulations of benzene methylation in H-ZSM-S to determine the factors that influence the reaction kinetics. Special emphasis is given to the effect of the surrounding methanol molecules on the methylation kinetics. It is found that for higher methanol loadings, methylation may also occur from a protonated methanol cluster, indicating that the exact location of the Bronsted acid site is not essential for the zeolite-catalyzed methylation reaction. However, methylations from a protonated methanol cluster exhibit higher free energy barriers than a methylation from a single methanol molecule. Finally, comparison with a pure methanol solvent reaction environment indicates that the main role of the zeolite during the methylation of benzene is to provide the acidic proton and to create a polar environment for the reaction. The metadynamics approach, which is specifically designed to sample rare events, allows exploring new reaction pathways, which take into account the flexibility of the framework and additional guest molecules in the pores and channels of the zeoli},
  author       = {Moors, Samuel and De Wispelaere, Kristof and Van der Mynsbrugge, Jeroen and Waroquier, Michel and Van Speybroeck, Veronique},
  issn         = {2155-5435},
  journal      = {ACS CATALYSIS},
  keywords     = {ZSM-5,methylation,methanol to olefins,benzene,methanol clusters,metadynamics,TO-OLEFIN PROCESS,DIMETHYL ETHER,REACTION-MECHANISM,CO-REACTION,AB-INITIO,HYDROCARBON FORMATION,PRODUCT SELECTIVITY,SHAPE-SELECTIVITY,ACIDIC ZEOLITES,LIGHT ALKENES},
  language     = {eng},
  number       = {11},
  pages        = {2556--2567},
  title        = {Molecular dynamics kinetic study on the zeolite-catalyzed benzene methylation in ZSM-5},
  url          = {http://dx.doi.org/10.1021/cs400706e},
  volume       = {3},
  year         = {2013},
}

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