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Complex reaction environments and competing reaction mechanisms in zeolite catalysis: insights from advanced molecular dynamics

(2015) CHEMISTRY-A EUROPEAN JOURNAL. 21(26). p.9385-9396
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Abstract
The methanol-to-olefin process is a showcase example of complex zeolite-catalyzed chemistry. At real operating conditions, many factors affect the reactivity, such as framework flexibility, adsorption of various guest molecules, and competitive reaction pathways. In this study, the strength of first principle molecular dynamics techniques to capture this complexity is shown by means of two case studies. Firstly, the adsorption behavior of methanol and water in H-SAPO-34 at 350 degrees C is investigated. Hereby an important degree of framework flexibility and proton mobility was observed. Secondly, the methylation of benzene by methanol through a competitive direct and stepwise pathway in the AFI topology was studied. Both case studies clearly show that a first-principle molecular dynamics approach enables unprecedented insights into zeolite-catalyzed reactions at the nanometer scale to be obtained.
Keywords
molecular dynamics, zeolites, olefins, heterogeneous catalysis, ab initio calculations, PROTON MOBILITY, IN-SITU, THERMAL-EXPANSION, PRODUCT SELECTIVITY, UV/VIS MICROSPECTROSCOPY, OLEFIN PROCESS, FREE-ENERGY, METHANOL-TO-HYDROCARBONS, X-RAY-DIFFRACTION, AB-INITIO

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Citation

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Chicago
De Wispelaere, Kristof, B Ensing, An Ghysels, EJ Meijer, and Veronique Van Speybroeck. 2015. “Complex Reaction Environments and Competing Reaction Mechanisms in Zeolite Catalysis: Insights from Advanced Molecular Dynamics.” Chemistry-a European Journal 21 (26): 9385–9396.
APA
De Wispelaere, K., Ensing, B., Ghysels, A., Meijer, E., & Van Speybroeck, V. (2015). Complex reaction environments and competing reaction mechanisms in zeolite catalysis: insights from advanced molecular dynamics. CHEMISTRY-A EUROPEAN JOURNAL, 21(26), 9385–9396.
Vancouver
1.
De Wispelaere K, Ensing B, Ghysels A, Meijer E, Van Speybroeck V. Complex reaction environments and competing reaction mechanisms in zeolite catalysis: insights from advanced molecular dynamics. CHEMISTRY-A EUROPEAN JOURNAL. 2015;21(26):9385–96.
MLA
De Wispelaere, Kristof, B Ensing, An Ghysels, et al. “Complex Reaction Environments and Competing Reaction Mechanisms in Zeolite Catalysis: Insights from Advanced Molecular Dynamics.” CHEMISTRY-A EUROPEAN JOURNAL 21.26 (2015): 9385–9396. Print.
@article{5991974,
  abstract     = {The methanol-to-olefin process is a showcase example of complex zeolite-catalyzed chemistry. At real operating conditions, many factors affect the reactivity, such as framework flexibility, adsorption of various guest molecules, and competitive reaction pathways. In this study, the strength of first principle molecular dynamics techniques to capture this complexity is shown by means of two case studies. Firstly, the adsorption behavior of methanol and water in H-SAPO-34 at 350 degrees C is investigated. Hereby an important degree of framework flexibility and proton mobility was observed. Secondly, the methylation of benzene by methanol through a competitive direct and stepwise pathway in the AFI topology was studied. Both case studies clearly show that a first-principle molecular dynamics approach enables unprecedented insights into zeolite-catalyzed reactions at the nanometer scale to be obtained.},
  author       = {De Wispelaere, Kristof and Ensing, B and Ghysels, An and Meijer, EJ and Van Speybroeck, Veronique},
  issn         = {0947-6539},
  journal      = {CHEMISTRY-A EUROPEAN JOURNAL},
  keyword      = {molecular dynamics,zeolites,olefins,heterogeneous catalysis,ab initio calculations,PROTON MOBILITY,IN-SITU,THERMAL-EXPANSION,PRODUCT SELECTIVITY,UV/VIS MICROSPECTROSCOPY,OLEFIN PROCESS,FREE-ENERGY,METHANOL-TO-HYDROCARBONS,X-RAY-DIFFRACTION,AB-INITIO},
  language     = {eng},
  number       = {26},
  pages        = {9385--9396},
  title        = {Complex reaction environments and competing reaction mechanisms in zeolite catalysis: insights from advanced molecular dynamics},
  url          = {http://dx.doi.org/10.1002/chem.201500473},
  volume       = {21},
  year         = {2015},
}

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