有机官能团化介孔分子筛固载铑膦配合物的制备及其对己烯-1氢甲酰化的催化性能  

Preparation of Organo-Functionalized Mesoporous Zeolites Supported Phosphine-Rhodium Complex and Their Catalytic Performance for Hexene-1 Hydroformylation

作　　者：杨勇[1] 彭庆蓉[1] 袁友珠[1] 

机构地区：[1]厦门大学化学系固体表面物理化学国家重点实验室,福建厦门361005

出　　处：《催化学报》2004年第5期421-425,共5页

基　　金：国家自然科学基金 (2 0 0 2 3 0 0 1;2 0 0 2 10 0 2 );国家重点基础研究发展规划 (G2 0 0 0 0 480 0 8)资助项目

摘　　要：制备了表面有机官能团化的MCM 4 1和MCM 4 8介孔分子筛以及SiO2 等载体固载铑膦配合物催化剂 ,考察了所制备催化剂对液相己烯 1氢甲酰化的催化性能 ,并用X射线衍射、BET、红外光谱和原子吸收光谱等技术对载体和催化剂的组成和结构进行了表征 .结果表明 ,固载化铑膦配合物对烯烃氢甲酰化的催化性能与有机官能团的种类及载体的结构有关 ;固载于含胺基和腈基有机官能团化介孔分子筛载体的铑膦配合物表现出较高的催化活性和稳定性 .Organo-functionalized mesoporous zeolites MCM-41 and MCM-48, and amorphous SiO 2 were used as supports to prepare heterogenized phosphine-rhodium complex via anchoring for the hydrofomylation of hexene-1. The supports and the catalysts were characterized by means of XRD, BET, FT-IR and AAS. The MCM-41 and MCM-48 were functionalized with silanes containing (mono-, di-, tri-) amino-, mercapto- and nitrile- groups, respectively, without destruction of the mesoporous structure of the zeolites. The catalytic performance of the catalysts was related to the structure of organo-groups and also to the structural features of the supports. Higher catalytic activity and selectivity for n-C 6H 13CHO were obtained in the case of the catalysts using the mesoporous zeolites functionalized with amino- and nitrile-silanes as supports. No significant decrease in the catalytic performance of the phosphine-rhodium complex immobilized on the amino-functionalized mesoporous zeolites used repeatedly for 6 times was observed.

关 键 词：介孔分子筛 二氧化硅 有机官能团化 膦 铑配合物 己烯 氢甲酰化 庚醛 

分 类 号：O643[理学—物理化学]