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Investigation of confinement effects on zeolite-catalyzed methylation reactions

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Abstract
Catalytic conversion of methanol to light olefins (MTO) over acidic zeolites is currently one of the most prominent alternatives to traditional crude oil cracking processes for the production of ethene and propene. The underlying reaction mechanisms have been under debate for decades, with current insight strongly supporting an indirect mechanism based on the hydrocarbon pool hypothesis: olefin formation is found to occur through repeated methylation and subsequent elimination and/or cracking reactions of organic co-catalysts inside the zeolite pores.[1] Depending on the characteristics of the zeolite material, the predominant hydrocarbon pool species vary from smaller alkenes to bulky polymethylbenzenes.[2] Theoretical studies showed that methylations are generally the rate-determining steps in the olefin producing catalytic cycles; therefore it is of utmost importance to gain an in-depth understanding of these reactions.[3,4] Quantum chemical calculations on extended cluster models that mimic the local environment of the active site were used in this work to model methylation reactions in a selection of zeolite frameworks. Activation barriers and rate constants are then mutually compared to assess the influence of confinement effects caused by different catalyst topologies. The balance between accuracy and computational efficiency signifies this approach as an important step toward routine study of reaction steps in heterogeneous catalysis.[5]

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Chicago
Van der Mynsbrugge, Jeroen, Kristof De Wispelaere, Jeroen De Ridder, Karen Hemelsoet, Michel Waroquier, and Veronique Van Speybroeck. 2011. “Investigation of Confinement Effects on Zeolite-catalyzed Methylation Reactions.” In Ninth Triennial Congress of the World Association of Theoretical and Computational Chemists, WATOC 2011, 60–60.
APA
Van der Mynsbrugge, J., De Wispelaere, K., De Ridder, J., Hemelsoet, K., Waroquier, M., & Van Speybroeck, V. (2011). Investigation of confinement effects on zeolite-catalyzed methylation reactions. Ninth triennial congress of the World Association of Theoretical and Computational Chemists, WATOC 2011 (pp. 60–60). Presented at the 9th Triennial congress of the World Association of Theoretical and Computational Chemists (WATOC 2011).
Vancouver
1.
Van der Mynsbrugge J, De Wispelaere K, De Ridder J, Hemelsoet K, Waroquier M, Van Speybroeck V. Investigation of confinement effects on zeolite-catalyzed methylation reactions. Ninth triennial congress of the World Association of Theoretical and Computational Chemists, WATOC 2011. 2011. p. 60–60.
MLA
Van der Mynsbrugge, Jeroen, Kristof De Wispelaere, Jeroen De Ridder, et al. “Investigation of Confinement Effects on Zeolite-catalyzed Methylation Reactions.” Ninth Triennial Congress of the World Association of Theoretical and Computational Chemists, WATOC 2011. 2011. 60–60. Print.
@inproceedings{1862333,
  abstract     = {Catalytic conversion of methanol to light olefins (MTO) over acidic zeolites is currently one of the most prominent alternatives to traditional crude oil cracking processes for the production of ethene and propene. The underlying reaction mechanisms have been under debate for decades, with current insight strongly supporting an indirect mechanism based on the hydrocarbon pool hypothesis: olefin formation is found to occur through repeated methylation and subsequent elimination and/or cracking reactions of organic co-catalysts inside the zeolite pores.[1] Depending on the characteristics of the zeolite material, the predominant hydrocarbon pool species vary from smaller alkenes to bulky polymethylbenzenes.[2] Theoretical studies showed that methylations are generally the rate-determining steps in the olefin producing catalytic cycles; therefore it is of utmost importance to gain an in-depth understanding of these reactions.[3,4] Quantum chemical calculations on extended cluster models that mimic the local environment of the active site were used in this work to model methylation reactions in a selection of zeolite frameworks. Activation barriers and rate constants are then mutually compared to assess the influence of confinement effects caused by different catalyst topologies. The balance between accuracy and computational efficiency signifies this approach as an important step toward routine study of reaction steps in heterogeneous catalysis.[5]},
  articleno    = {abstract OC 059},
  author       = {Van der Mynsbrugge, Jeroen and De Wispelaere, Kristof and De Ridder, Jeroen and Hemelsoet, Karen and Waroquier, Michel and Van Speybroeck, Veronique},
  booktitle    = {Ninth triennial congress of the World Association of Theoretical and Computational Chemists, WATOC 2011},
  language     = {eng},
  location     = {Santiago de Compostela, Spain},
  pages        = {abstract OC 059:60--abstract OC 059:60},
  title        = {Investigation of confinement effects on zeolite-catalyzed methylation reactions},
  year         = {2011},
}