Influence of Topology and Chemical Composition of MTT and MFI Zeolites on Catalytic Properties in the Isomerization Reaction of Ethylene Oxide to Acetaldehyde

被引:4
|
作者
Piryutko, L., V [1 ]
Lazareva, S., V [1 ]
Chernyayskii, V. S. [1 ]
Kharitonov, A. S. [1 ]
Noskov, A. S. [1 ]
机构
[1] Russian Acad Sci, Boreskov Inst Catalysis, Siberian Branch, Novosibirsk 630090, Russia
关键词
zeolites; ZSM-23; ZSM-5; acid sites; isomerization; ethylene oxide; acetaldehyde; MECHANISM; KINETICS; ZSM-5;
D O I
10.1134/S0965544119070144
中图分类号
O62 [有机化学];
学科分类号
070303 ; 081704 ;
摘要
It has been shown by the example of zeolites with the MTT (Al-ZSM-23 and Fe-ZSM-23) and MFI (Al-ZSM-5 and Fe-ZSM-5) structures that mesoporous zeolites are efficient catalysts for the gas-phase isomerization of ethylene oxide to acetaldehyde. At 300-400 degrees C and complete conversion of ethylene oxide, the selectivity of its conversion to acetaldehyde (S-AA) reaches at least 90%. The key factors determining the selectivity and stability of the catalyst are the topology of the zeolite and its acid properties. Unidimensional zeolites with the MTT structure demonstrate higher S-AA in comparison with the samples with the three-dimensional MFI structure. Decreasing the strength of Bronsted acid sites by replacing Al by Fe in the zeolites of both structural types also leads to a growth in S-AA. The samples are arranged in following order of decreasing S-AA: Fe-ZSM-23 > Fe-ZSM-5 = ZSM-23 > ZSM-5. The main byproduct of the reaction is crotonic aldehyde, the formation of which is promoted by strong Bronsted acid sites. The crotonic aldehyde selectivity over aluminosilicate samples is above 6%.
引用
收藏
页码:726 / 732
页数:7
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