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化学学报
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化学学报 ›› 2008, Vol. 66 ›› Issue (12): 1391-1398. 上一篇    下一篇

研究论文

新型WO3/TiO2纳米管催化剂的合成及其在环戊烯选择氧化反应中的 性能研究

杨新丽a,b 戴维林*,a 高瑞华a 沈晚晴a 范康年a   

  1. (a复旦大学化学系 上海市分子催化和功能材料重点实验室 上海 200433)
    (b河南工业大学化学化工学院 郑州 450052)
  • 投稿日期:2007-10-25 修回日期:2008-01-28 发布日期:2008-06-28
  • 通讯作者: 戴维林

Preparation of Novel WO3/TiO2 Nanotube Catalyst and Its Catalytic Performance for the Selective Oxidation of Cyclopentene

YANG, Xin-Li a,b DAI, Wei-Lin *,a GAO, Rui-Hua a
SHEN, Wan-Qing a FAN, Kang-Nian a   

  1. (a Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433)
    (b School of Chemistry & Chemical Engineering, Henan University of Technology, Henan 450052)
  • Received:2007-10-25 Revised:2008-01-28 Published:2008-06-28
  • Contact: DAI, Wei-Lin

PDF

857

被引次数

19

采用水热合成法以P25为原料制备了介孔TiO2纳米管, 并根据TEM和XPS表征结果对其形成机理进行了初步分析. 然后, 以制备出的介孔TiO2纳米管为载体, 钨酸铵为钨源, 采用传统浸渍方法制备了介孔WO3/TiO2纳米管催化剂. 利用N2吸附, TEM, XRD, XPS及Raman等手段对固载后的多相催化剂进行了表征, 并研究了催化剂在环戊烯选择氧化制备戊二醛反应中的催化性能. 结果表明, 在介孔20% WO3/TiO2纳米管催化下环戊烯的转化率达97.9%, 戊二醛的选择性高达69.3%. 钨物种以高度分散状态存在于催化剂中, 并与载体间存在着较强的相互作用, 使得钨的溶脱量很小, 脱落的钨对反应几乎没有影响. 另外, 催化剂具有较高的稳定性, 可以重复套用7次. 失活后的催化剂可通过简单焙烧的方式再生.

关键词: 介孔TiO2纳米管, WO3/TiO2纳米管催化剂, 环戊烯, 选择氧化, 过氧化氢, 戊二醛

Titania nanotubes were synthesized via a simple alkali hydrothermal treatment of P25 (Degussa) nanoparticles and the formation mechanism of TiO2 nanotubes was primarily analyzed based on the characterizations by TEM and XPS. Then, the novel WO3/TiO2 nanotube catalyst was prepared by an incipient wetness method using the TiO2 nanotube as the support and ammonium tungstate as the precursor, and was characterized by means of N2 adsorption, TEM, XRD, XPS and Raman spectroscopy. The catalytic performance of the as-prepared composite was investigated for the preparation of glutaraldehyde (GA) from the selective oxidation of cyclopentene (CPE). The 20 wt% catalyst showed 97.9% of CPE conversion and 69.3% of GA selectivity. It was found that the active tungsten species were highly dispersed and there was strong interaction between tungsten species and the titania nanotube support at tungsten oxide content ＜20 wt%. The leaching of the active sites was very small and had little effect on the catalytic performance. In addition, the WO3/TiO2 nanotube catalyst was very stable and could be reused for at least seven times. The deactivated catalyst could be regenerated by simple calcination.

Key words: mesoporous TiO2 nanotube, WO3/TiO2 nanotube catalyst, cyclopentene, selective oxidation, hydrogen peroxide, glutaraldehyde