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Investigation of the methanol conversion over high Si Beta zeolites and the reaction mechanism for high propene selectivity

Abstract

Large pore high Si Beta (Si/Al = 130-340) were synthesized by a HF-assisted method and their catalytic performance for the methanol to propene conversnion was explored. It is demonstrated that Beta zeolites with low acid density faciliate the achievment of high propene selectivity and high propene/ethene ratio. The HF dosage in the synthesis has great influence on the Al distribution in the framework as evidenced by the 27Al MAS NMR and 27Al MQ MAS NMR, which may influence the acidity and microstructure of acid sites and leads to distinct catalytic lifespan. A HF/SiO2 ratio of 0.45 is found to facilitate the synthesis of high Si Beta enriched with Al atoms located at T9 sites, which helps the catalyst to show the longest lifetime with propene selectivity of 49.7-58.3 % at 550 oC and WHSV = 2 h-1. With the aid of the 12C/13C-methanol switch experiments, the olefins-based mechanism is elucidated to dominate in the reaction and contributes to the formation of ethene, propene and higher olefins. Moreover, two phenol compounds are identified in the coke species, which have not been observed before and are found to be detrimental to the reaction.

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Publication details

The article was received on 01 Sep 2017, accepted on 08 Nov 2017 and first published on 09 Nov 2017


Article type: Paper
DOI: 10.1039/C7CY01804E
Citation: Catal. Sci. Technol., 2017, Accepted Manuscript
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    Investigation of the methanol conversion over high Si Beta zeolites and the reaction mechanism for high propene selectivity

    X. zhao, L. Wang, J. Li, S. Xu, W. Zhang, Y. Wei, X. Guo, P. Tian and Z. Liu, Catal. Sci. Technol., 2017, Accepted Manuscript , DOI: 10.1039/C7CY01804E

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