Enhancement of catalytic and anti-carbon deposition performance of SAPO-34/ZSM-5/quartz films in MTA reaction by Si/Al ratio regulation

Chinese Journal of Chemical Engineering(2022)

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摘要
In order to further improve the catalytic performance of zeolite catalyst for methanol to aromatics (MTA) technology, the double-tier SAPO-34/ZSM-5/quartz composite zeolite films were successfully synthe-sized via hydrothermal crystallization. The Si/Al ratio of SAPO-34 film was used as the only variable to study this material. The composite zeolite material with 0.6Si/Al ratio of SAPO-34 has the largest meso-porous specific surface area and the most suitable acid distribution. The catalytic performance for the MTA process showed that 0.6-SAPO-34/ZSM-5/quartz film has as high as 50.3% benzene-toluene-xylene selectivity and 670 min lifetime. The MTA reaction is carried out through the path we designed to effectively avoid the hydrocarbon pool circulation of ZSM-5 zeolite, so as to improve the aromatics selectivity and inhibit the occurrence of deep side reactions to a great extent. The coke deposition behav-ior was monitored by thermogravimetric analysis and gas chromatograph/mass spectrometer, it is found that with the increase of Si/Al ratio, the active intermediates changed from low-substituted methylben-zene to high-substituted methylbenzene, which led to the rapid deactivation of the catalyst. This work provides a possibility to employ the synergy effect of composite zeolite film synthesizing anti-carbon deposition catalyst in MTA reaction.(c) 2022 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.
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关键词
Composite zeolite film,Methanol to aromatics,Anti-carbon deposition,Si,Al ratio,Hydrocarbon pool circulation mechanism
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