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

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

Journal Article (2016)

Author(s)

Irina Yarulina (TU Delft - Applied Sciences)

Simon Bailleul (Universiteit Gent)

A. Pustovarenko (TU Delft - Applied Sciences)

Javier Ruiz Martinez (Universiteit Utrecht)

Kristof De Wispelaere (Universiteit Gent)

Julianna Hajek (Universiteit Gent)

Bert M. Weckhuysen (Universiteit Utrecht)

Klaartje Houben (Universiteit Utrecht)

Marc Baldus (Universiteit Utrecht)

Veronique Van Speybroeck (Universiteit Gent)

Freek Kapteijn (TU Delft - Applied Sciences)

Jorge Gascon (TU Delft - Applied Sciences)

Research Group

ChemE/Catalysis Engineering

Calcium Zeolites Acidity Alkenes Density functional calculations

DOI related publication

https://doi.org/10.1002/cctc.201600650 Final published version

To reference this document use

https://resolver.tudelft.nl/uuid:a997e333-ace5-485f-970e-c01b9950f454

More Info

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Publication Year

2016

Language

English

Research Group

ChemE/Catalysis Engineering

Journal title

ChemCatChem

Issue number

19

Volume number

8

Pages (from-to)

3057-3063

Downloads counter

229

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 g_MeOH g_catalyst ⁻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.