催化学报 ›› 2014, Vol. 35 ›› Issue (9): 1456-1464.DOI: 10.1016/S1872-2067(14)60068-1

• 论文 • 上一篇    下一篇

编织芳基网络聚合物负载Rh催化剂上高碳烯烃氢甲酰化反应性能

姜淼a,c, 丁云杰a,b, 严丽a, 宋宪根a, 林荣和a   

  1. a 中国科学院大连化学物理研究所洁净能源国家实验室(筹), 辽宁大连116023;
    b 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连116023;
    c 中国科学院大学, 北京100049
  • 收稿日期:2014-01-23 修回日期:2014-02-26 出版日期:2014-08-19 发布日期:2014-08-22
  • 通讯作者: 丁云杰

Rh catalysts supported on knitting aryl network polymers for the hydroformylation of higher olefins

Miao Jianga,c, Yunjie Dinga,b, Li Yana, Xiangen Songa, Ronghe Lina   

  1. a Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
    b State Key Laboratory for Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
    c University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2014-01-23 Revised:2014-02-26 Online:2014-08-19 Published:2014-08-22

摘要:

考察了编织芳基网络聚合物(KAPs)负载的Rh催化剂(Rh/KAPs)在高碳烯烃氢甲酰化反应中的催化性能. 结果表明,三苯基膦-苯基底KAPs负载Rh催化剂(Rh/KAPs-1)具有优异的高碳烯烃氢甲酰化反应活性,产物醛收率显著高于Rh/SiO2催化剂. 傅里叶变换红外光谱、热重、氮气吸附-脱附、X射线衍射、透射电子显微镜、13C核磁共振和31P核磁共振结果显示,Rh/KAPs-1催化剂具有优异的热稳定性及大的比表面积和多级孔道结构,Rh颗粒处于高度分散状态,并可在反应过程中形成均相催化活性物种.

关键词: 三苯基膦, 编织芳基网络聚合物, 铑, 多相催化剂, 高碳烯烃氢甲酰化

Abstract:

Rh catalysts supported on knitting aryl network polymers (Rh/KAPs) were prepared for the hydroformylation of higher olefins. Rh catalysts supported on triphenylphosphine-benzene-base polymers (Rh/KAPs-1) showed higher activity for the higher olefins than Rh/SiO2 catalysts. Fourier transform infrared spectroscopy, thermogravimetry, N2 adsorption-desorption, X-ray diffraction, transmission electron microscopy, 13C NMR, and 31P NMR showed that the Rh/KAPs-1 catalysts have high thermal stability, high surface area, hierarchical porosity, highly dispersed Rh nanoparticles, and in situ formed homogeneous active species during the reaction.

Key words: Triphenylphosphine, Knitting aryl network polymer, Rhodium, Heterogeneous catalyst, Hydroformylation of higher olefins