title: Complex Reaction Environments and Competing Reaction Mechanisms in Zeolite Catalysis: Insights from Advanced Molecular Dynamics.
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 °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.
authors.affiliation: Center for Molecular Modeling (CMM), Ghent University, Technologiepark 903, 9052 Zwijnaarde (Belgium).|Amsterdam Center for Multiscale Modeling and van 't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam (The Netherlands).
authors.forename: Kristof
authors.initials: K
authors.lastname: De Wispelaere
authors.affiliation: Amsterdam Center for Multiscale Modeling and van 't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam (The Netherlands). b.ensing@uva.nl.
authors.forename: Bernd
authors.initials: B
authors.lastname: Ensing
authors.affiliation: Center for Molecular Modeling (CMM), Ghent University, Technologiepark 903, 9052 Zwijnaarde (Belgium).
authors.forename: An
authors.initials: A
authors.lastname: Ghysels
authors.affiliation: Amsterdam Center for Multiscale Modeling and van 't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam (The Netherlands).
authors.forename: Evert Jan
authors.initials: EJ
authors.lastname: Meijer
authors.affiliation: Center for Molecular Modeling (CMM), Ghent University, Technologiepark 903, 9052 Zwijnaarde (Belgium). veronique.vanspeybroeck@ugent.be.
authors.forename: Veronique
authors.initials: V
authors.lastname: Van Speybroeck
keywords: ab initio calculations; heterogeneous catalysis; molecular dynamics; olefins; zeolites