催化学报

催化学报 ›› 2008, Vol. 29 ›› Issue (1): 52-56.

• 研究论文 • 上一篇    下一篇

镍基催化剂上苯酐选择性加氢合成苯酞

刘迎新1,魏作君2,傅杰1,高颖1,严巍1   

  1. 1 浙江工业大学药学院, 绿色化学合成技术国家重点实验室培育基地, 浙江杭州 310032; 2 浙江大学材料与化学工程学院化学工程与生物工程系, 浙江杭州 310027
  • 收稿日期:2008-01-25 出版日期:2008-01-25 发布日期:2011-12-25

Selective Hydrogenation of Phthalic Anhydride to Phthalide over Supported Nickel Catalysts

LIU Yingxin1*, WEI Zuojun2, FU Jie1, GAO Ying1, YAN Wei1   

  1. 1 College of Pharmaceutical Science, State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, China; 2 Department of Chemical and Biochemical Engineering, College of Materials Science and Chemical Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China
  • Received:2008-01-25 Online:2008-01-25 Published:2011-12-25

PDF

1326

被引次数

21

摘要： 分别以SiO2, TiO2,γ-Al2O3, TiO2-SiO2和TiO2-Al2O3为载体,以硝酸镍为镍源,采用等体积浸渍法制备了一系列镍基催化剂,并将其用于苯酐选择性加氢合成苯酞反应. 结果表明,以TiO2-SiO2为载体制备的镍催化剂上Ni0活性组分分散度较高,催化剂表现出较高的活性和苯酞选择性. 在此基础上,采用溶胶-凝胶法制备出了一系列Ni/TiO2-SiO2催化剂,考察了催化剂制备中各因素(包括溶剂、焙烧温度、还原温度和镍前驱体类型等)对其催化苯酐加氢反应性能的影响. 结果表明,将镍前驱体溶于不同溶剂制备的催化剂性能差异很大,其中以水为溶剂制备的催化剂活性较高,且性能优于等体积浸渍法制备的相应催化剂. 焙烧温度和还原温度过高会导致活性组分镍晶粒度变大,致使催化剂活性明显降低. 镍源对Ni/TiO2-SiO2催化剂的性能影响较大,以硫酸镍为镍源制备的催化剂几乎无活性,而以氯化镍和硝酸镍为镍源制备的催化剂表现出较高的催化活性和选择性,其中以氯化镍制备的催化剂性能略高于硝酸镍,苯酐转化率为100%, 苯酞选择性为88.5%.

关键词: 溶胶-凝胶法, 镍, 二氧化钛, 二氧化硅, 苯酐, 加氢, 苯酞

Abstract: The selective hydrogenation of phthalic anhydride to phthalide in liquid phase was studied with nickel catalysts supported on SiO2, TiO2,γ-Al2O3, TiO2-SiO2, and TiO2-Al2O3 carriers prepared by the incipient wetness impregnation method, using nickel nitrate as the nickel precursor. The results showed that the nickel catalyst supported on TiO2-SiO2 with well-dispersed active nickel species exhibited the highest activity and selectivity for phthalide. Then, a series of Ni/TiO2-SiO2 catalysts were prepared by sol-gel method through changing the preparation conditions. The sol-gel Ni/TiO2-SiO2 catalyst using water as the solvent had much better catalytic performance than the one using alcohol as solvent and the one prepared by the impregnation method. Improperly high calcination temperature and reduction temperature caused sintering of nickel species and reduced the catalytic activity. In addition, the nickel precursors obviously affected the performance of the catalysts. The catalyst prepared from nickel chloride showed higher activity and selectivity than the catalysts prepared from nickel sulfate and nickel nitrate. Over this catalyst, the conversion of phthalic anhydride was 100%, and the selectivity for phthalide was 88.5%.

Key words: sol-gel method, nickel, titania, silica, phthalic anhydride, hydrogenation, phthalide