Synthesis Of Mesoporous MCM-41 Molecular Sieve Supported Palladium(0,Ⅱ) Complexes And BF₃·X Solid Acid Catalysts And Their Application Researches

Mesoporous MCM-41 molecular sieve possesses regular arrays of uniform channel and large internal surface area, the immobilization of inorganic or organic species onto its surface for application in catalysis is becoming widely recognized. In the present dissertation, we have reported the synthesis of various Palladium/BF₃·X -grafted mesoporous MCM-41 materials and their application as heterogeneous catalysts. The dissertation presents here the following main points:1. The immobilization of organic species onto mesoporous MCM-41 material was investigated. Various function groups(-NH₂-NHCH₂CH₂NH₂-SH -CN and -COOH) can be immobilized on the MCM-41 surface via reaction of the silanol groups with oxyalky-silane compounds .The results indicate that organically modified MCM-41 materials retain its hexagonally-packed porous structure during supporting organic species, but internal surface area and pore diameter of the materials decreased markedly.2. A number of new MCM-41 molecular sieve supported amine-palladium(0, II) complexes were prepared and their catalytic performances in the Heck arylation of alkenes were studied. It was found that the direct covalent binding to silica surfaces has been achieved by coordinative binding of the metal Pd center to supported amino ligands. Supported amine-palladium(0) and Pd(OAc)2 catalysts are highly active and stereoselective for the arylation of aryl iodides with styrene, acrylic acid and methyl acrylat at 70℃, and can be reused by washing without loss in activity.The effect of reduction conditions on catalytic properties of MCM-41 supported amine-palladium( II) complexes was studied. It was found that catalytic activities of supported amine-palladium( II) by reduction treatment would increased markedly. Catalytic activity increased with intensity of reducing agent, and the order of catalytic...