催化学报

催化学报 ›› 2010, Vol. 31 ›› Issue (8): 933-937.DOI: 10.1016/S1872-2067(09)60090-5

• 研究快讯 • 上一篇    下一篇

NaY 分子筛超笼内离子液体和金属配合物自组装制备溶剂分子和金属配合物一体化催化剂

马昱博 1,2, 何昱德 1, 张庆华 1, 石峰 1, 马祥元 1, 卢六斤 1, 邓友全 1   

  1. 1中国科学院兰州化学物理研究所绿色化学与催化中心, 甘肃兰州 730000 2中国科学院研究生院, 北京 100049
  • 收稿日期:2010-03-14 出版日期:2010-08-30 发布日期:2013-12-26

Self-Assembly of Ionic Liquids and Metal Complexes in Super-Cages of NaY: Integration of Free Catalysts and Solvent Molecules into Confined Catalytic Sites

MA Yubo1,2, HE Yude1, ZHANG Qinghua1, SHI Feng1,*, MA Xiangyuan1, LU Liujin1, DENG Youquan1,*   

  1. 1Center for Green Chemistry and Catalysis, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, Gansu, China 2Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2010-03-14 Online:2010-08-30 Published:2013-12-26

PDF

1167

被引次数

5

摘要： 采用自组装-瓶中造船法在 NaY 分子筛超笼内, 将溴化 1-癸基-3-甲基咪唑离子液体和邻菲罗啉钯组合成一体化催化剂, 并用于苯胺羰化反应. 结果表明, 相对于以离子液体为溶剂, 邻菲罗啉钯配合物/NaY 分子筛为催化剂的体系, 该一体化催化剂在离子液体和邻菲罗啉钯配合物用量显著降低的条件下, TOF 可达 23 000 h?1, 而相应均相催化剂体系的 TOF 仅为 3 060 h-1.

关键词: 活性位, 离子液体, 金属配合物, 羰化, 苯胺, 苯胺基甲酸甲酯, 转化频率

Abstract: The integration of a free metal complex, Pd(phen)2+, and a room temperature ionic liquid (IL) solvent molecule, 1-decyl-3-methyl imidazolium bromide, into a complete catalytically active site and confined in a NaY zeolite super-cage with an appropriate spatial arrange-ment was investigated. This integration was achieved through a molecular self-assembly method. A preliminary test of this catalyst system for the carbonylation of aniline to methyl phenyl carbamate indicated that far higher catalytic activity could be achieved (TOF increased from 3 000 to 23 000 h–1) with far lower amounts of the IL solvent and the Pd complex in comparison with a simple mixture of Pd(phen)Cl2/IL/NaY as the catalyst. This new system can also be applied to other areas of catalysis.

Key words: active site, ionic liquid, metal complex, carbonylation, aniline, phenyl methyl carbamate, turn over frequency