Suppression of the Aromatic Cycle in Methanol-to-Olefins Reaction over ZSM-5 by Post-Synthetic Modification Using Calcium

Irina Yarulina, Simon Bailleul, Alexey Pustovarenko, Javier Ruiz Martinez, Kristof De Wispelaere, Julianna Hajek, Bert M. Weckhuysen, Klaartje Houben, Marc Baldus, Veronique Van Speybroeck, Freek Kapteijn, Jorge Gascon Sabate*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

36 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)3057-3063
Number of pages7
JournalChemCatChem
Volume8
Issue number19
DOIs
StatePublished - Oct 6 2016
Externally publishedYes

Keywords

  • acidity
  • alkenes
  • calcium
  • density functional calculations
  • zeolites

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry
  • Organic Chemistry
  • Inorganic Chemistry

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