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金属卟啉-磷酸铜杂化材料的制备及其在烯烃环氧化反应中的应用
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摘要
环氧化物是一类用途广泛的化学品,可经选择性开环反应,高效地转化为一系列重要的目标产物,在化学化工领域有着广泛的应用。~([1])金属卟啉模拟酶催化烯烃环氧化因其反应条件温和、产物选择性高等优点而受到广泛关注,但其活性和循环使用稳定性还有待提高。我们通过有机-无机杂化的方法~([2])制备了具有精细结构的金属卟啉-无机基底杂化催化剂。该催化剂呈微米花球结构,金属卟啉固载量约为2%。将其用于环己烯环氧化反应,在室温和常压鼓泡的条件下,可获得96%的环己烯转化率和95%的氧化环己烯选择性。该催化剂重复使用三次,催化性能保持稳定。进一步与浸渍法制备的金属卟啉/无机基底催化剂进行对比,证明了有机-无机杂化方法制备的催化剂中金属卟啉与无机基底间存在较强的相互作用。
Epoxides are a kind of useful chemicals that can be converted into a series of important products through ring opening reaction. Epoxidation of olefins catalyzed by metalloporphyrins has been widely concerned for its mild reaction conditions and high selectivity. However, it is urgent to improve the catalytic performance, including activity and stability. The catalysts of metalloporphyrins-inorgnic substrates with nano/micro flower structure were prepared with orgnic-inorgnic hybrid method, and showed excellent catalytic activity(96% cyclohexene conversion, 95% cyclohexene oxide selectivity) and stability even after three runs. Further experimental studies proved there was strong interaction between metalloporphyrin and inorganic substrates.
引文
[1]Yan W.;Ramanathan A.;Ghanta M.;Subramaniam B.Catal Sci Technol 2014,4:4433.
    [2]Ge J.;Lei J.;Zare R.N.Nat Nanotechnol 2012,7:428.

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