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

作　　者：柏子龙[1] 方明芳[1] 陈绍洲[1] 

机构地区：[1]华东理工大学石油加工研究所,上海200237

出　　处：《催化学报》2002年第1期29-32,共4页

基　　金：国家自然科学基金资助项目 ( 2 976 0 19)

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～The synthesis and catalytic properties of zeolite-encapsulated vanadium picolinic complex catalysts have been studied. The catalysts were prepared by treating dehydrated zeolites with VOSO4 to form VO2+ 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(NH2)(2).H2O2 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)].H2O 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 钒络合物 正己烷 环己烷 氧化反应 选择性 烷烃 负载型催化剂 催化性能 

分 类 号：O643.3[理学—物理化学]