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Cu-Zn/HZS M-5催化剂上甲烷与丙烷的共活化

Activation of Methane Using Propane as Co-reactant over Cu-Zn/HZSM-5 Catalyst

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【作者】 郑海涛褚洪岭楼辉侯昭胤费金华李影辉肖海成杨玉和郑小明

【Author】 ZHENG Haitao 1, ZHU Hongling 2, LOU Hui 1, HOU Zhaoyin 1, FEI Jinhua 1, LI Yinghui 3, XIAO Haicheng 3, YANG Yuhe 3, ZHENG Xiaoming 1* (1 Institute of Catalysis, Zhejiang University, Hangzhou 310028, Zhejiang, China; 2 School of Chemical Engineering, Harbin Engineering University, Harbin 150001, Heilongjiang, China; 3 Research Institute of Daqing Petrochemical Company, Daqing 163714, Heilongjiang, China)

【机构】 浙江大学催化研究所哈尔滨工程大学化工学院大庆石化公司研究院浙江大学催化研究所 浙江杭州310028黑龙江哈尔滨150001浙江杭州310028黑龙江大庆163714浙江杭州310028

【摘要】 研究了xCu 6 %Zn/HZSM 5 (x =0~ 0 9% )系列催化剂对甲烷和丙烷混合气体无氧芳构化反应的催化性能 .结果表明 ,在此系列催化剂上 ,丙烷促进了甲烷的活化 ,使之参与到芳烃的形成过程中 .在 6 0 0℃和甲烷 /丙烷摩尔比为 1 0的条件下 ,0 7%Cu 6 %Zn/HZSM 5催化剂表现出最佳活性 ,甲烷转化率达到 36 % ,芳烃选择性达到 85 7% .这说明在Zn/HZSM 5中添加第二组分Cu有助于提高催化剂的活性和稳定性 .考察了反应时间和甲烷 /丙烷摩尔比对甲烷和丙烷转化率及产物分布的影响 .13 CH4同位素示踪实验发现13 C进入到了C6H+ 6,C7H+ 8和C8H+ 10 碎片中 ,这进一步证实甲烷参与了芳烃的形成 .

【Abstract】 The catalytic conversion of methane into higher hydrocarbons in the absence of oxygen using propane as a co-reactant over the xCu-6%Zn/HZSM-5 (x=0~0.9%) catalyst was investigated. It was found that methane could be activated and transferred into higher hydrocarbons and aromatics with a methane conversion of 36% and an aromatics selectivity of 85.7% at 600 ℃ and methane/propane molar ratio of 1.0. The effects of methane/propane molar ratio on the methane and propane conversion and product distribution were studied in details. There was a positive relationship between the methane activation and aromatics production. Incorporation of methane into aromatics was confirmed by mass spectral analysis of aromatics products in the aromatization of isotope-labeled 13 CH 4 in the presence of propane, in which significant 13 C enrichment in C 6H + 6, C 7H + 8 and C 8H + 10 fragments was found.

【关键词】 甲烷丙烷无氧芳构化HZSM-5负载型催化剂
【Key words】 methanepropanenon-oxidative aromatizationcopperzincHZSM-5supported catalyst
【基金】 国家自然科学基金资助项目 (2 0 3 43 0 0 2 ) ;浙江省自然科学基金资助项目 (990 3 )
  • 【文献出处】 催化学报 ,Chinese Journal of Catalysis , 编辑部邮箱 ,2005年01期
  • 【分类号】O643
  • 【被引频次】16
  • 【下载频次】238
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