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Insight into the formation and reactivity of framework-bound methoxide species in H-ZSM-5 from static and dynamic molecular simulations

(2014) CHEMCATCHEM. 6(7). p.1906-1918
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Abstract
Framework-bound methoxides occur as intermediates in the stepwise mechanism for zeolite-catalyzed methylation reactions. Herein, the formation of methoxides from methanol or dimethyl ether in H-ZSM-5 is investigated by a combination of static and dynamic simulations, with particular focus on the effect of additional water and methanol molecules on the mechanism and kinetics. Metadynamics simulations allow partitioning the reaction path into distinct phases. Proton transfer from the zeolite to the reactants is found to be the rate-limiting phase in the methoxide formation. Additional methanol molecules only assist the proton transfer in the methoxide formation from methanol, whereas the reaction from dimethyl ether does not benefit from methanol assistance. Once formed, methoxides are found to be as reactive toward alkene methylation as methanol and dimethyl ether.
Keywords
METHANOL, AB-INITIO, N-ALKANES, ZEOLITES

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Citation

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Chicago
Van der Mynsbrugge, Jeroen, Samuel Moors, Kristof De Wispelaere, and Veronique Van Speybroeck. 2014. “Insight into the Formation and Reactivity of Framework-bound Methoxide Species in H-ZSM-5 from Static and Dynamic Molecular Simulations.” Chemcatchem 6 (7): 1906–1918.
APA
Van der Mynsbrugge, J., Moors, S., De Wispelaere, K., & Van Speybroeck, V. (2014). Insight into the formation and reactivity of framework-bound methoxide species in H-ZSM-5 from static and dynamic molecular simulations. CHEMCATCHEM, 6(7), 1906–1918.
Vancouver
1.
Van der Mynsbrugge J, Moors S, De Wispelaere K, Van Speybroeck V. Insight into the formation and reactivity of framework-bound methoxide species in H-ZSM-5 from static and dynamic molecular simulations. CHEMCATCHEM. 2014;6(7):1906–18.
MLA
Van der Mynsbrugge, Jeroen, Samuel Moors, Kristof De Wispelaere, et al. “Insight into the Formation and Reactivity of Framework-bound Methoxide Species in H-ZSM-5 from Static and Dynamic Molecular Simulations.” CHEMCATCHEM 6.7 (2014): 1906–1918. Print.
@article{5712431,
  abstract     = {Framework-bound methoxides occur as intermediates in the stepwise mechanism for zeolite-catalyzed methylation reactions. Herein, the formation of methoxides from methanol or dimethyl ether in H-ZSM-5 is investigated by a combination of static and dynamic simulations, with particular focus on the effect of additional water and methanol molecules on the mechanism and kinetics. Metadynamics simulations allow partitioning the reaction path into distinct phases. Proton transfer from the zeolite to the reactants is found to be the rate-limiting phase in the methoxide formation. Additional methanol molecules only assist the proton transfer in the methoxide formation from methanol, whereas the reaction from dimethyl ether does not benefit from methanol assistance. Once formed, methoxides are found to be as reactive toward alkene methylation as methanol and dimethyl ether.},
  author       = {Van der Mynsbrugge, Jeroen and Moors, Samuel and De Wispelaere, Kristof and Van Speybroeck, Veronique},
  issn         = {1867-3880},
  journal      = {CHEMCATCHEM},
  language     = {eng},
  number       = {7},
  pages        = {1906--1918},
  title        = {Insight into the formation and reactivity of framework-bound methoxide species in H-ZSM-5 from static and dynamic molecular simulations},
  url          = {http://dx.doi.org/10.1002/cctc.201402146},
  volume       = {6},
  year         = {2014},
}

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