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

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

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23000h-1,而相应均相催化剂体系的TOF仅为3060h-1.

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 arrangement 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.