期刊
ACS CATALYSIS
卷 13, 期 6, 页码 3471-3484出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.3c00059
关键词
methanol-to-hydrocarbons; step-response kinetic experiment s; operando spectroscopy; hydrocarbon pool; confinement; zeolite; Ca; ZSM-5
The presence of Ca2+ in zeolite catalysts modifies the local environment inside micropores, resulting in enhanced propylene selectivity in the methanol-to-hydrocarbons (MTH) process. Ca/ZSM-5 exhibits strong adsorption of water, hydrocarbons, and oxygenates, which occupy up to 10% of the micropores during the MTH reaction. This change in effective pore geometry affects the formation of hydrocarbon pool components and directs the MTH reaction towards the olefin cycle.
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.
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