Suppression of the Aromatic Cycle in Methanol-to-Olefins Reaction over ZSM-5 by Post-Synthetic Modification Using Calcium
Publication date
2016-10-06
Authors
Yarulina, Irina
Bailleul, Simon
Pustovarenko, Alexey
Ruiz Martinez, Javier
Wispelaere, Kristof De
Hajek, Julianna
Weckhuysen, Bert M.
Houben, Klaartje
Baldus, Marc
Van Speybroeck, Veronique
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Document Type
Article
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taverne
Abstract
Incorporation of Ca in ZSM-5 results in a twofold increase of propylene selectivity (53 %), a total light-olefin selectivity of 90 %, and a nine times longer catalyst lifetime (throughput 792 gMeOH gcatalyst −1) in the methanol-to-olefins (MTO) reaction. Analysis of the product distribution and theoretical calculations reveal that post-synthetic modification with Ca2+ leads to the formation of CaOCaOH+ that strongly weaken the acid strength of the zeolite. As a result, the rate of hydride transfer and oligomerization reactions on these sites is greatly reduced, resulting in the suppression of the aromatic cycle. Our results further highlight the importance of acid strength on product selectivity and zeolite lifetime in MTO chemistry.
Keywords
acidity, alkenes, calcium, density functional calculations, zeolites, Taverne, Catalysis, Physical and Theoretical Chemistry, Organic Chemistry, Inorganic Chemistry
Citation
Yarulina, I, Bailleul, S, Pustovarenko, A, Martinez, J R, Wispelaere, K D, Hajek, J, Weckhuysen, B M, Houben, K, Baldus, M, Van Speybroeck, V, Kapteijn, F & Gascon, J 2016, 'Suppression of the Aromatic Cycle in Methanol-to-Olefins Reaction over ZSM-5 by Post-Synthetic Modification Using Calcium', ChemCatChem, vol. 8, no. 19, pp. 3057-3063. https://doi.org/10.1002/cctc.201600650