Synthesis and catalytic performance of hierarchical MCM-22 zeolite aggregates with the assistance of carbon particles and fluoride ions

doi:10.1016/S1872-2067(12)60711-6

Abstract

Abstract:

Hierarchical MCM-22 zeolite aggregates (MCM-22-FC) were prepared by one-pot hydrothermal synthesis with the assistance of carbon particles and fluoride ions. The effects of carbon particles and fluoride ions on the morphology and catalytic properties of the MCM-22 zeolite were investigated. The hierarchical MCM-22-FC zeolite aggregates were constructed by intergrown and stacked thin MCM-22 lamellas and possessed macro-/mesopores and inherent micropores. The MCM-22-FC zeolite was modified to form the Mo/MCM-22-FC catalyst, which exhibited an improved benzene yield and aromatic selectivity as well as catalyst life in the methane dehydroaromatization (MDA) reaction. Based on NH₃-TPD and pyridine-Fourier transform infrared spectroscopy measurements together with thermogravimetric analysis, we found that the improved MDA catalytic performance of Mo/MCM-22-FC resulted from the formation of more active MoC_x or MoO_xC_y species that evolved from increased amounts of Brönsted acids with the assistance of fluoride ions. This promoted the diffusion of large molecule products because of the thin MCM-22 lamellas. Less excess Brönsted acid sites were retained in the Mo/HMCM-22-FC catalyst because the formation of active centers inhibited the formation of coke, which contributed to its improved aromatic selectivity.

Key words: Methane dehydroaromatization, MCM-22 zeolite, Hierarchical pore, Fluoride route, Catalytic performance

Jianhua Yang, Jun Chu, Jinqu Wang, Dehong Yin, Jinming Lu, Yan Zhang. Synthesis and catalytic performance of hierarchical MCM-22 zeolite aggregates with the assistance of carbon particles and fluoride ions[J]. Chinese Journal of Catalysis, 2014, 35(1): 49-57.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(12)60711-6

https://www.cjcatal.com/EN/Y2014/V35/I1/49

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