催化学报

催化学报 ›› 2011, Vol. 32 ›› Issue (2): 362-367.DOI: 10.3724/SP.J.1088.2011.00937

• 研究论文 • 上一篇    下一篇

无第二模板剂法合成多级结构 ZSM-5 分子筛微球及其在甲烷无氧芳构化反应中的应用

杨建华, 于素霞, 胡慧晔, 初乃波, 鲁金明, 殷德宏, 王金渠   

  1. 大连理工大学精细化工国家重点实验室, 吸附与无机膜研究所, 辽宁大连 116012
  • 收稿日期:2010-09-27 修回日期:2010-11-19 出版日期:2011-01-26 发布日期:2014-06-25

Synthesis of Hierarchical HZSM-5 Microspheres without Second Template and Their Application in Methane Dehydroaromatization

YANG Jianhua, YU Suxia, HU Huiye, CHU Naibo, LU Jinming, YIN Dehong, WANG Jinqu   

  1. Institute of Adsorption and Inorganic Membrane, State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116012, Liaoning, China
  • Received:2010-09-27 Revised:2010-11-19 Online:2011-01-26 Published:2014-06-25

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1167

被引次数

28

摘要： 在无第二模板剂的条件下, 采用简单的水热晶化法, 通过控制条件合成出具有多级结构的 ZSM-5 (ZSM-5-HW) 分子筛, 并运用 X 射线衍射、红外光谱、扫描电镜和 N2 吸附-脱附等技术对合成的分子筛进行了表征. 结果表明, 所得样品是由棒状晶体组装而成的具有介孔结构的分子筛微球. 用等体积浸渍法制备了 Mo/HZSM-5-HW 催化剂并用于 CH4 无氧芳构化反应, 表现出较高的催化活性和稳定性. 在实验条件下, CH4 初始转化率为 18.5%, 而苯收率最高可达 9.5%; 反应 24 h 后, 两者仍然分别保持在 10.2% 和 5.5% 左右.

关键词: 多级结构, ZSM-5 分子筛, 第二模板剂, 甲烷, 无氧芳构化

Abstract: Hierarchical ZSM-5(ZSM-5-HW) microspheres were synthesized by controlling the hydrothermal conditions without any secondary template. The ZSM-5-HW microspheres with a diameter range of 10–15 μm were constructed by many rod-shaped crystals. N2 adsorption at –196 oC revealed that the ZSM-5-HW zeolite is of both micropore and mesopore structure. The hierarchical Mo/HZSM-5-HW catalyst exhibited higher catalytic activity and stability in methane dehydroaromatization. The initial CH4 conversion and the highest benzene yield were 18.5% and 9.5%, respectively, which are better than that of the conventional Mo/HZSM-5 catalyst. The CH4 conversion and benzene yield was kept at 10.2% and 5.5%, respectively, after running the reaction for 24 h.

Key words: hierarchical structure, ZSM-5 zeolite, secondary template, methane, dehydroaromatization