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P/Rh比对PPh₃-Rh/SiO₂催化剂上丙烯氢甲酰化反应的影响

Influence of Phosphine Concentration on Propylene Hydroformylation over the PPh₃-Rh/SiO₂ Catalyst

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【Author】 YAN Li1,2,DING Yunjie1,2,,LIU Jia1,2,ZHU Hejun1,2,LIN Liwu1,2 1Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China 2Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China

【机构】中国科学院大连化学物理研究所；中国科学院大连化学物理研究所洁净能源国家实验室；

【摘要】研究了P/Rh比对PPh3-Rh/SiO2催化剂上丙烯氢甲酰化反应性能的影响.结果表明,当P/Rh比为15时,丙烯氢甲酰化反应性能最好,丙烯转化率为25.9%,产物丁醛正异比为14,转换频率为241h-1.PPh3-Rh/SiO2催化剂的固体31P核磁共振结果表明,在合成气气氛下,物理吸附的PPh3能够溢流到Rh/SiO2表面形成化学吸附的PPh3,从而促进了具有氢甲酰化活性的铑膦络合物的形成.Wilkinson催化平衡理论也很好地解释了本实验结果.更多还原

【Abstract】 The effect of triphenyl phosphine concentration in the novel PPh3-Rh/SiO2 catalyst for propylene hydroformylation was studied and found an optimum P/Rh ratio of 15,a butyraldehyde n/i ratio of 14,a butyraldehyde TOF of 241 h-1,and high catalytic stability for PPh3-Rh/SiO2.Solid-state 31P NMR shows that in an atmosphere of syngas the physically adsorbed PPh3 migrates onto the surface of Rh/SiO2 where it chemically adsorbs and then promotes the in situ formation of carbonyl phosphine complexes.更多还原