1. Complex reaction environments and competing reaction mechanisms in zeolite catalysis: insights from advanced molecular dynamics
- Author
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Veronique Van Speybroeck, Evert Jan Meijer, An Ghysels, Kristof De Wispelaere, Bernd Ensing, and Molecular Simulations (HIMS, FNWI)
- Subjects
Reaction mechanism ,OLEFIN PROCESS ,zeolites ,PROTON MOBILITY ,Heterogeneous catalysis ,Catalysis ,UV/VIS MICROSPECTROSCOPY ,Molecular dynamics ,Adsorption ,X-RAY-DIFFRACTION ,Computational chemistry ,Reactivity (chemistry) ,METHANOL-TO-HYDROCARBONS ,Topology (chemistry) ,PRODUCT SELECTIVITY ,Flexibility (engineering) ,AB-INITIO ,Chemistry ,ab initio calculations ,IN-SITU ,Organic Chemistry ,General Chemistry ,FREE-ENERGY ,molecular dynamics ,heterogeneous catalysis ,olefins ,THERMAL-EXPANSION - 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.
- Published
- 2015