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出 处:《分子催化》2007年第6期579-584,共6页Journal of Molecular Catalysis(China)
基 金:山西省自然基金(20040402).
摘 要:以固载于微米级硅胶表面的聚4-乙烯吡啶-铜(Ⅱ)配合物(P4VP-Cu(Ⅱ)/SiO2)为催化剂,以分子氧为氧化剂,在常压下实施了将乙苯氧化为苯乙酮的催化氧化反应;用红外光谱、紫外光谱及液相色谱对产物的化学结构进行了表征;重点研究了催化剂的催化性能,以及各种条件(温度、催化剂性质、催化剂用量等)对催化氧化反应的影响;并分析了催化氧化反应的机理.研究结果表明,固载于硅胶表面的聚4-乙烯吡啶-Cu(Ⅱ)配合物能有效地活化分子氧,显著地催化氧化乙苯为苯乙酮的反应过程;该催化剂具有优良的催化活性与选择性,于130℃常压下通氧气反应10h,可使约60%的乙苯转化为苯乙酮,另一氧化产物α-甲基苄醇的含量则极少.另外,该催化剂具有较好的重复使用稳定性.In this work, the catalytic oxidation of ethylbenzene to acetophenone was performed using the complex of poly(4-vinyl pyridine) and Cu( Ⅱ ) as catalyst, which had been grafted on the surface of silica gel particles (i. e. catalyst P4VP-Cu( Ⅱ )/SiO2 ), and with molecular oxygen as oxidant under atmospheric pressure. The chemical structure of the product was characterized by UV, IR and liquid chromatography. The catalytic properties of the catalyst and the effects of various factors on the catalytic oxidation were studied, such as reaction temperature, reaction time, the used amount of the catalyst. The experiment results show that the catalyst P4VP-Cu( Ⅱ )/SiO2 has excellent catalytic activity and fine selectivity for transferring ethylbenzene into acetophenone, the product nearly is acetophenone, and the other product, α- methyl benzoic alcohol is few. As O2 was blown in the reaction system at 130 ℃ for 10 h under atmospheric pressure, the yield of acetophenone can get up to 60%. The experiment fact indicates that the catalyst P4VP-Cu( Ⅱ )/SiO2 ) can effectively activate dioxygen, and promote the oxidation of hydrocarbons.
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