Ca Cations Impact the Local Environment inside HZSM-5 Pores during the Methanol-to-Hydrocarbons Reaction

Anna Liutkova, Hao Zhang, Jérôme F.M. Simons, Brahim Mezari, Marta Mirolo, Gustavo A. Garcia, Emiel J.M. Hensen (Corresponding author), Nikolay Kosinov (Corresponding author)

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

20 Citaten (Scopus)
82 Downloads (Pure)

Samenvatting

The methanol-to-hydrocarbons (MTH) process is an industrially relevant method to produce valuable light olefins such as propylene. One of the ways to enhance propylene selectivity is to modify zeolite catalysts with alkaline earth cations. The underlying mechanistic aspects of this type of promotion are not well understood. Here, we study the interaction of Ca2+ with reaction intermediates and products formed during the MTH reaction. Using transient kinetic and spectroscopic tools, we find strong indications that the selectivity differences between Ca/ZSM-5 and HZSM-5 are related to the different local environment inside the pores due to the presence of Ca2+. In particular, Ca/ZSM-5 strongly retains water, hydrocarbons, and oxygenates, which occupy as much as 10% of the micropores during the ongoing MTH reaction. This change in the effective pore geometry affects the formation of hydrocarbon pool components and in this way directs the MTH reaction toward the olefin cycle.
Originele taal-2Engels
Pagina's (van-tot)3471-3484
Aantal pagina's14
TijdschriftACS Catalysis
Volume13
Nummer van het tijdschrift6
DOI's
StatusGepubliceerd - 17 mrt. 2023

Financiering

FinanciersFinanciernummer
Netherlands Center for Multiscale Catalytic Energy Conversion
European Union’s Horizon Europe research and innovation programme
H2020 Marie Skłodowska-Curie Actions801359
European Synchrotron Radiation FacilityCH6231, CH6391
Ministerie van OCW
Nederlandse Organisatie voor Wetenschappelijk Onderzoek

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