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

作     者：Jiaxin Wu Chenxiao Wang Xianliang Meng Haichen Liu Ruizhi Chu Guoguang Wu Weisong Li Xiaofeng Jiang Deguang Yang Jiaxin Wu;Chenxiao Wang;Xianliang Meng;Haichen Liu;Ruizhi Chu;Guoguang Wu;Weisong Li;Xiaofeng Jiang;Deguang Yang

作者机构：School of Chemical Engineering and TechnologyChina University of Mining&TechnologyXuzhou 221116China Key Laboratory of Coal Processing and Efficient Utilization of Ministry of EducationXuzhou 221116China 

出 版 物：《Chinese Journal of Chemical Engineering》 (中国化学工程学报（英文版）)

年 卷 期：2023年第56卷第4期

页      面：314-324页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：supported by the National Natural Science Foundation of China (51974312, 51974308) the National Key Research & Development Program of China (2019YFE0100100) 

主　　题：Composite zeolite film Methanol to aromatics Anti-carbon deposition Si/Al ratio Hydrocarbon pool circulation mechanism 

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 synthesized 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 mesoporous 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-toluenexylene 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 behavior 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 methylbenzene 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.