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

作　　者：郑海涛[1] 褚洪岭 楼辉[1] 侯昭胤[1] 费金华[1] 李影辉[3] 肖海成[3] 杨玉和[3] 郑小明[1] 

机构地区：[1]浙江大学催化研究所,浙江杭州310028 [2]哈尔滨工程大学化工学院,黑龙江哈尔滨150001 [3]大庆石化公司研究院,黑龙江大庆163714

出　　处：《催化学报》2005年第1期49-54,共6页

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 )

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 .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 similar to 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 degreesC 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 (CH4)-C-13 in the presence of propane, in which significant C-13 enrichment in C6H6+, C7H8+ and C8H10+ fragments was found.

关 键 词：甲烷 丙烷 无氧芳构化 铜 锌 HZSM-5 负载型催化剂 

分 类 号：O643[理学—物理化学]