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Mo/HZSM-5催化剂上甲烷芳构化反应行为的改善—催化剂制备因素及反应物添加剂的考察

Improvement of Methane Dehydroaromatization Performance over Mo/HZSM-5 Catalyst-Effects of Catalyst Preparation Methods and Reactant Additives

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【作者】 陈会英李永刚陈为申文杰徐奕德包信和

【Author】 CHEN Hui-ying~(1,2), LI Yong-gang~(1,2), CHEN Wei~(1,2), SHEN Wen-jie~1, XU Yi-de~1, BAO Xin-he~1(1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, The Chinese Academy of Sciences, Dalian 116023, China;2. Graduate School of The Chinese Academy of Sciences, Beijing 100039, China)

【机构】 中国科学院大连化学物理研究所催化基础国家重点实验室中国科学院大连化学物理研究所催化基础国家重点实验室 辽宁大连116023中国科学院研究生院北京100039辽宁大连116023辽宁大连116023

【摘要】 考察了6Mo/HZSM-5催化剂的不同制备因素对其甲烷芳构化反应性能的影响,包括甲烷气氛下以不同的程序升温速率(从600℃到700℃)预还原催化剂,及采用热溶液(70~80℃)浸渍制备催化剂等方法.在t=700℃,P=0.1MPa,SV=1500mL/(g-cat·h)的反应条件下,发现适当的程序升温速率预还原和热溶液浸渍制备等方法可以改善6Mo/HZSM-5催化剂的甲烷芳构化反应性能,提高催化剂的反应活性及稳定性.同时还考察了1.5%二甲醚作为反应物添加剂在不同反应温度、不同Mo担载量的HZSM-5催化剂上的甲烷芳构化反应性能,并与CO2,H2O的反应结果进行了对比.实验结果表明,在P=0.1MPa,SV=1500mL/(g-cat·h)的反应条件下,较高的反应温度及适量增加催化剂Mo担载量有利于进一步改善1.5%二甲醚/甲烷共进料情况下的芳构化反应行为;反应6h后催化剂的TEM照片显示,二甲醚与甲烷共进料改变了催化剂上积碳的形貌.

【Abstract】 Methane aromatization performance of different 6Mo/HZSM\|5 catalysts, which were prepared by changing the conditions of preparation, was investigated under the reaction conditions of t=700 ℃, P=0.1 MPa, SV=1 500 mL/(g-cat·h). It was found that the catalysts prepared by reducing Mo/HZSM-5 in CH4 stream at a slower heating rate from 600 ℃ to 700 ℃ or by impregnating HZSM-5 power in hot (NH4)6Mo7O24 solution (70 80 ℃) had a better catalytic activity and stability. The effects of 1.5% dimethyl ether (DME) as reactant additive to CH4 feed were also investigated over Mo/HZSM-5 catalysts with different Mo loadings and at different temperatures. The results showed that higher reaction temperatures and higher Mo loadings were in favor of the aromatization of 1.5%DME/CH4 co-feed under the reaction conditions of P=0.1 MPa and SV=1 500 mL/(g-cat·h). The TEM images of 6Mo/HZSM-5 catalysts coked for 6 h showed that the appearance of the coke was changed by 1.5%DME/CH4 co-feed. The effects of 1.5% H2O and 2.5% CO2 co-reactants were also investigated and compared.

【关键词】 Mo/HZSM-5甲烷芳构化二甲醚CO2H2O
【Key words】 Mo/HZSM-5Methane aromatizationDimethyl ether (DME)CO2H2O
【基金】 国家重点基础研究发展规划(973计划)资助项目(G1999022406);BP-China“面向未来”清洁能源研究计划资助项目.
  • 【文献出处】 分子催化 ,Journal of Molecular Catalysis , 编辑部邮箱 ,2005年02期
  • 【分类号】O643.3
  • 【被引频次】4
  • 【下载频次】226
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