RESEARCH ARTICLE
The effect of hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios on its pore structure and catalytic performance
. Laboratory of Living Materials at the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China.. State Key Laboratory of Silicate Material for Architectures, Wuhan University of Technology, Wuhan 430070, China.. Laboratory of Inorganic Materials Chemistry (CMI), University of Namur, B-5000 Namur, Belgium.. Nanostructure Research Centre (NRC), Wuhan University of Technology, Wuhan 430070, China.. Clare Hall, University of Cambridge, Cambridge, CB3 9AL, UK
Received: 2020-04-22
Accepted: 2020-07-13
Available online: 2020-07-13
Abstract
Hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios (Hier-ZSM-5- , where = 50, 100, 150 and 200) were synthesized using an ordered mesoporous carbon-silica composite as hard template. Hier-ZSM-5- exhibits improved mass transport properties, excellent mechanical and hydrothermal stability, and higher catalytic activity than commercial bulk zeolites in the benzyl alcohol self-etherification reaction. Results show that a decrease in the Si/Al ratio in hierarchical single-crystal ZSM-5 zeolites leads to a significant increase in the acidity and the density of micropores, which increases the final catalytic conversion. The effect of porous hierarchy on the diffusion of active sites and the final catalytic activity was also studied by comparing the catalytic conversion after selectively designed poisoned acid sites. These poisoned Hier-ZSM-5- shows much higher catalytic conversion than the poisoned commercial ZSM-5 zeolite, which indicates that the numerous intracrystalline mesopores significantly reduce the diffusion path of the reactant, leading to the faster diffusion inside the zeolite to contact with the acid sites in the micropores predominating in ZSM-5 zeolites. This study can be extended to develop a series of hierarchical single-crystal zeolites with expected catalytic performance.
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