A Covalently Immobilized Triphenylphosphine Rhodium Complex: Synthesis, Characterization, and Application in Catalytic Olefin Hydrogenation
A Covalently Immobilized Triphenylphosphine Rhodium Complex: Synthesis, Characterization, and Application in Catalytic Olefin Hydrogenation
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DOI：
10.1002/cctc.201000133
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发表时间：
2010-11
期刊：
影响因子：
4.5
通讯作者：
Lei Wang;Ming-jun Jia;S. Shylesh;Thomas Philippi;A. Seifert;S. Ernst;A. Singh;W. Thiel
中科院分区：
文献类型：
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作者：
Lei Wang;Ming-jun Jia;S. Shylesh;Thomas Philippi;A. Seifert;S. Ernst;A. Singh;W. Thiel
将三甲氧基硅烷官能化的三苯基膦配位到铑（I）上，并将所得铑络合物共价结合到介孔SBA-15载体上。研究了该杂化材料对2-环己烯-1-酮加氢反应的催化活性，并与相应的均相催化剂进行了比较。根据31 P-MAS NMR数据，催化活性物质对氧化是稳定的;在暴露于空气超过两个月后，没有检测到结构变化。对所使用的催化剂的透射电子显微镜（TEM）测量证实，铑物质也对还原成金属是稳定的，因为可以排除在催化期间铑纳米颗粒的形成。循环体系的动力学曲线证实，这种杂化催化剂显示出优异的活性，选择性，稳定性和可重复使用性，并在加氢反应中是真正的非均相。
A trimethoxysilane functionalized triphenylphosphine was coordinated to rhodium(I) and the resulting rhodium complex was covalently bound to a mesoporous SBA‐15 support. The catalytic activity of this hybrid material was studied for the hydrogenation of 2‐cyclohexen‐1‐one and compared with the corresponding homogeneous catalyst. According to the 31P‐MAS NMR data, the catalytically active species was stable against oxidation; no structural change could be detected after exposing it to air for more than two months. Transmission electron microscopy (TEM) measurements on the used catalyst confirmed that the rhodium species was also stable against reduction to the metal because the formation of rhodium nanoparticles during the catalysis could be excluded. The kinetic curves of the recycled system confirmed that this hybrid catalyst shows excellent activity, selectivity, stability, and reusability, and is truly heterogeneous in the hydrogenation reaction.