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)(PPh3)3 Complex for Isobutene Hydroformylation
作者：许俊强(四川大学 化工学院，四川 成都 610065)；储伟(四川大学 化工学院，四川 成都 610065)；罗仕忠(四川大学 化工学院，四川 成都 610065)
Author：(School of Chem. Eng., Sichuan Univ., Chengdu 610065, China)；(School of Chem. Eng., Sichuan Univ., Chengdu 610065, China)；(School of Chem. Eng., Sichuan Univ., Chengdu 610065, China)
收稿日期：2006-12-20 年卷（期）页码：2007,39(5):70-74
期刊名称：工程科学与技术
Journal Name：Advanced Engineering Sciences
关键字：介孔分子筛Si-MCM-41; 铑膦络合物; 异丁烯; 氢甲酰化; 异戊醛
Key words：mesoporous Si-MCM-41 materials;HRh(CO)(PPh3)3;isobutene;hydroformylation;isovaleraldehyde
基金项目：四川大学科技创新基金资助项目(2005CF07);国家自然科学基金资助项目(205903603)
中文摘要
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。
英文摘要
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.
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