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沸石负载的钒络合物催化剂对烷烃氧化反应的催化性能

Oxidation of Alkanes over Zeolite-Encapsulated Vanadium Picolinic Complexes

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【作者】 柏子龙方明芳陈绍洲

【Author】 BAI Zilong *, FANG Mingfang, CHEN Shaozhou (East China University of Science and Technology, Shanghai 200237, China)

【机构】 华东理工大学石油加工研究所华东理工大学石油加工研究所 上海200237上海200237上海200237

【摘要】 将钒氧吡啶甲基络合物VO(pic) 2 负载于Y及ZSM 5沸石分子筛中 ,制备出沸石负载的钒络合物催化剂 .用X射线衍射、电子自旋共振、红外光谱和元素分析等方法对催化剂进行了表征 .结果表明 ,VO(pic) 2 络合物确实负载于分子筛孔道内 ,负载后的络合物仍保持着原来的结构 .考察了催化剂对正己烷和环己烷氧化反应的催化性能 ,发现沸石分子筛负载的VO(pic) 2 络合物催化剂保留有络合物原有的催化性能 ,虽然催化活性有所下降 ,但显示出较好的形状选择性 .与未负载的络合物相比 ,NaY和ZSM 5沸石负载的VO(pic) 2 络合物催化剂对正己烷氧化反应的伯醇选择性分别提高了 2~ 3倍和 5~ 6倍

【Abstract】 The synthesis and catalytic properties of zeolite encapsulated vanadium picolinic complex catalysts have been studied. The catalysts were prepared by treating dehydrated zeolites with VOSO 4 to form VO 2+ zeolites, then reacting with molten picolinic acid. The formed zeolite encapsulated complexes were characterized by XRD, ESR, and FT IR spectroscopy. The results suggested that vanadium exists in the zeolite cavities in the form of VO(pic) 2 complex. The catalysts were used in the oxidation of n hexane and cyclohexane with CO(NH 2) 2·H 2O 2 as the oxidant. It was shown that the "ship in a bottle" catalysts retain the same catalytic activity as H[VO(O 2)(pic) 2]·H 2O in the homogeneous environment and exhibit good shape selectivity and regioselectivity in the oxidation of n hexane. The ratios of 1 hexanol to 2 hexanol and 1 hexanol to 3 hexanol are 1 39 and 2 04 respectively for VO(pic) 2 NaY, and 2 22 and 4 00 respectively for VO(pic) 2 ZSM 5.

【关键词】 沸石络合物正己烷环己烷氧化反应选择性
【Key words】 zeolitevanadium picolinic complexhexanecyclohexaneoxidationselectivity
【基金】 国家自然科学基金资助项目 ( 2 976 0 19)
  • 【文献出处】 催化学报 ,Chinese Journal of Catalysis , 编辑部邮箱 ,2002年01期
  • 【分类号】O643.3
  • 【被引频次】18
  • 【下载频次】246
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