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

Autor: Anna Liutkova, Hao Zhang, Jérôme F. M. Simons, Brahim Mezari, Marta Mirolo, Gustavo A. Garcia, Emiel J. M. Hensen, Nikolay Kosinov
Přispěvatelé: Inorganic Materials & Catalysis, EIRES Chem. for Sustainable Energy Systems
Jazyk: angličtina
Rok vydání: 2023
Předmět:
Zdroj: ACS Catalysis, 13(6), 3471-3484. American Chemical Society
ISSN: 2155-5435
Popis: 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.
Databáze: OpenAIRE