Solid-state NMR study of the stability of MOR framework aluminum

Chinese Journal of Structural Chemistry(2024)

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摘要
MOR zeolite has been effectively utilized for dimethyl ether (DME) carbonylation reaction due to its unique pore structure and acidity. During industrial production, the transformation of ammonium type MOR zeolite (NH4-MOR) into proton type MOR zeolite (H-MOR) causes inevitable dealumination. Therefore, understanding the influencing factors and dynamic evolution mechanism of zeolite dealumination is crucial. In this work, the stability of framework aluminum was studied by XRD, FTIR, 29Si, 27Al, 1H MAS NMR, and DME carbonylation performance evaluation. These results indicated that extra-framework cation Na+ and NH4+ could better preserve the aluminum structure of the MOR zeolite framework compared to H+, primarily due to the different ‘attraction’ of the framework to water. Furthermore, the impact of water on the zeolite framework aluminum at high temperature was studied by manipulation the humidity of the calcination atmosphere, revealing the formation of extra-framework six-coordinated aluminum (Al (VI)-EF) and the mechanism of water influence on the zeolite framework aluminum.
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关键词
H-MOR,Solid-state NMR,H2O,Framework aluminum stability,Dealumination
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