Journal
FUEL
Volume 300, Issue -, Pages -Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2021.120694
Keywords
Acidity; Shape selectivity; Beta; Butene; Mechanism; Oligomerization
Categories
Funding
- China National Funds for Distinguished Young Scientists [22025804]
- Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of Chinese Academy of Sciences [XDA 21000000]
- Synfuels China Technology Co., Ltd.
- Beijing Key Laboratory of Coal to Cleaning Liquid Fuels
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The study investigated the effect mechanisms of Bronsted acid sites and Lewis acid sites in zeolites on butene transformation, finding that BASs catalyze double bond activation and isomerization, while LASs act as weak acids through the formation of allyl species and alkoxyl groups.
The acidity and shape selectivity of zeolites are two important catalytic properties, and they have been extensively applied to the chemical and petrochemical industries. Here, we investigated the various effect mechanisms of Bronsted acid sites (BASs) from bridged hydroxyl groups in zeolite Beta and Lewis acid sites (LASs) from silanol nests in Si-Beta on butene transformation and their reaction pathways by diffuse-reflectance infrared Fourier-transform spectroscopy. BAS catalysis of butenes double bond activation and isomerization follows the classical carbenium ion mechanism, while catalysis by silanol nests as weak LASs due to hydrogen bond interaction is achieved by formation of allyl species and alkoxyl groups. Moreover, the oligomerization reactions of butene isomers are affected by the dynamic diameters and activation energies of the butene isomers and the synergy between acidity and shape selectivity of the zeolite. Oligomerization of n-butene and cis-2-butene is more likely to be affected by acids on the sample, while oligomerization of trans-2-butene and isobutene is influenced by the shape selectivity of the channel, in addition to the acidity on partly dealuminated zeolite Beta.
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