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《Chinese Journal of Catalysis》 2003-03
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Study of Mo-Based Catalysts for Dehydro-aromatization of Methane

YE Fei 1, YU Lin 1*, SONG Yibing 1, SUN Changyong 1, FANG Yiwen 1, HAO Zhifeng 1, LIN Weiming 2, XU Yide 3, LIN Liwu 3(1 Department of Chemistry, Shantou University, Shantou 515063, Guangdong, China;2 Department of Chemical Engineering, South China University of Technology, Guangzhou 510641,Guangdong, China; 3 State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, The Chinese Academy of Sciences, Dalian 116023, Liaoning, China)  
Methane dehydro-aromatization over Mo/HZSM-5 catalyst has been widely studied in recent years. One of the main problems for the industrial application is the short lifetime of the catalyst owing to the serious carbon deposit on the catalyst surface. The addition of CO or CO_2 in feed as well as the steaming-dealumination and the silanization of the support was used to enhance the stability of the catalyst. In order to effectively suppress the formation of carbon deposit, we designed an easy and special route to prepare the Mo/HZSM-5(t) catalyst, in which HZSM-5 was precisely pretreated by calcination in air at 400 ℃ for 4 h , then re-calcination in N_2 at 500 ℃ for 4 h (precise pretreatment of support) before impregnation with ammonium molybdate. The precise pretreatment was found to be able to significantly improve the activity and the stability of the catalyst. On Mo/HZSM-5(t), the methane conversion and benzene yield even remained at 8.8% and 5.3% respectively after 30 h. Addition of promoter Fe leads to a significant increase in methane conversion and the selectivity for benzene, and methane conversion and benzene yield increase by 18% and 52% respectively, compared with Mo/HZSM-5(t). Through XRD and TPO characterization, it is concluded that Mo and Fe species are highly dispersed on the surface of the support or migrate into the channels of the support. The precise pretreatment of support and the addition of Fe restrain carbon deposit, hence the catalysts with high stability can be obtained.
【Fund】: 国家自然科学基金 ( 2 0 14 30 0 4);; 广东省自然科学基金 ( 0 115 73)资助项目
【CateGory Index】: O643.3
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