异丁烯氢甲酰化用介孔MCM-41分子筛负载铑磷络合物催化剂的研究

Study on Preparation of Mesoporous MCM-41 Zeolite Supported HRh(CO)(PPh_3)_3 Complex for Isobutene Hydroformylation

采用水热合成法制备Si-MCM-41介孔分子筛,并在其上担载HRh(CO)(PPh3)3络合物合成负载型催化剂,考察了该载体Si-MCM-41分子筛的制备条件对异丁烯氢甲酰化反应的影响。实验结果表明分子筛的制备条件中pH值,原料配比,晶化温度对反应性能的影响最显著,在pH=10,n(Si)∶n(CTAB)=1∶0.2和晶化温度为120℃的条件下制备的Si-MCM-41载体对异丁烯氢甲酰化制异戊醛的选择性达最优。采用低温液氮吸附脱附分析(BET)和X射线衍射分析(XRD)技术对载体Si-MCM-41和负载型HRh(CO)(PPh3)3-MCM-41催化剂进行表征,结果表明载体在负载络合物后仍然保持了较好的介孔特征,其较均匀的孔径分布表现出对反应产物较好的择形催化性能。

The mesoporous molecular sieves Si -MCM -41 was synthesized by hydrothermal method, and the catalysts supported the HRh（CO） （PPh3 ）3 on the Si -MCM -41 material were prepared. The proper parameters of the Si -MCM -41carrier synthesis were investigated. The isobutene Hydroformylation was studied as a model reaction. The results indicated that the optimum process of Si - MCM - 41carrier were selected： n （Si）： n （CTAB） = 1： 0. 2, pH = 10, crystallizing temperature = 120 ℃, the selectivity of isovaleraldehyde was the best. The good mesopore -structure order of Si - MCM - 41 and HRh （CO） （ PPh3 ） 3 - MCM - 41 were proved by BET data and XRD spectra. The uniform pore diameter distribution was beneficial for the selectivity of isovaleraldehyde for isobutene Hydroformylation reaction.