期刊
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
卷 343, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2023.123528
关键词
CO 2-assisted propane aromatization; Ga-MFI zeolite; Cu modification; Br onsted/Lewis acid ratio; Aromatics selectivity
This study fabricates a Cu/Ga-MFI catalyst with well-dispersed framework Ga species and achieves high selectivity for aromatics production. The Ga atoms in the MFI framework create a moderate acid strength, while the introduced Cu provides an appropriate acid distribution, enhancing the synergy between metal-related species and the zeolite. Additionally, DFT simulation results suggest that the acid sites in Ga-MFI are more preferable for propane dehydrogenation. Furthermore, CO2 can inhibit coke formation, endowing Cu/Ga-MFI catalyst with excellent anti-coking ability and regeneration stability.
The acidity and Ga-species status in the zeolite play a crucial role in the CO2-assisted propane dehydroaromatization (CO2-PDA). In this work, a copper modified Ga-MFI zeolite (Cu/Ga-MFI) with well dispersed framework Ga species was fabricated. A remarkable aromatics selectivity of 73% at propane conversion of 93.6% was achieved on Cu/Ga-MFI catalyst. The Ga atoms in MFI framework can create a moderate acid strength, while the introduced Cu provide an appropriate Bronsted/Lewis acid distribution, enhancing the synergy between metal related species and the zeolite. Besides, DFT results indicate that the acid sites in Ga-MFI are more preferable for the dehydrogenation of propane instead of the C-C cleavage. Moreover, CO2 can inhibit coke formation through reverse Boudouard and reverse water gas shift reaction, which endows Cu/Ga-MFI catalyst with superior anti coking ability and regeneration stability. This work provides a novel approach for designing catalysts with high activity, aromatics selectivity, and stability for CO2-PDA reactions.
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