The Preparation And Its Catalytic Performance Of Anchored Heterogenized Organometallic Complex Catalyst For Hydroformylation

In the thesis, Ph2PCH2CH2COOH was prepared from Ph3P in the usual Schlenk technique and characterized by MS, H-NMR and FI-IR spectra first. Then let it react with H2NCH2CH2CH2Si(OEt)3 to give the ligand with function group -Si(OEt)3, which reacts with [Rh (CO)2Cl]2 to give the correspondent homogeneous catalyst. Finally, the anchored heterogenized complex catalyst was obtained from the copolymerization of the above ligand with TEOS by sol-gel method.The factors affecting the properties of the catalysts in the preparation of the catalysts by the sol-gel method, which include pH, encapsulating temperature, drying temperature and Rh/P etc. were also investigated. The encapsulating conditions were optimized based on the results above. The catalyst was characterized by FI-IR spectra, XPS, TG-DTA and N2 absorption. The relationship between catalytic property and internal structure was revealed.The catalytic property of the catalyst for hydroformylation of 1-hexene was studied. The effects on the catalytic activity and selectivity of reaction temperature, time, pressure, quantities of catalyst and the kinds of solvent were observed. It was found that the conversion of 1-hexene can go up to 97.8%, the selectivity of aldehyde can be 99.9% and the n/i is 1.12, when the reaction was run at the optimal reaction conditions. Furthermore, the catalyst can be run for 8 times without obvious loss of activity. From the result of ICP and XPS, we can know that the catalyst only 12.68% losing of Rh mainly coming from the outer surface of the matrix. Therefore the losing of Rh was resolved partly, and the catalyst has the better recyclable property.Finally, the anchored heterogenized organometallic complex catalyst was applied to the hydroformylation of other olefins. It was found that conversion decreased as the order of 1-hexene >1-octylene > 1-dodecene > styrene. However the order of n/i of different olefms is styrene> 1-dodecene > 1-octylene > 1-hexene.