纳米Ru-Mn/ZrO_2催化剂上苯选择加氢制环己烯  

Selective hydrogenation of benzene to cyclohexene over nanocomposite Ru-Mn/ZrO_2 catalysts

作　　者：孙海杰[1] 江厚兵[1] 李帅辉[1] 王红霞[1] 潘雅洁[1] 董英英[1] 刘寿长[1] 刘仲毅[1] 

机构地区：[1]郑州大学化学与分子工程学院,河南郑州450001

出　　处：《催化学报》2013年第4期684-694,共11页

基　　金：国家自然科学基金(21273205);国家科技型中小企业创新基金(10C26214104505);中国博士后科学基金(2012M511125);郑州大学优秀博士论文培育基金~~

摘　　要：采用共沉淀法制备了一系列不同Mn含量的纳米Ru-Mn催化剂,考察了纳米ZrO2作分散剂时它们催化苯选择加氢制环己烯的反应性能,并采用X射线衍射、透射电镜、N2物理吸附、X射线荧光、原子吸收光谱和俄歇电子能谱等手段对催化剂进行了表征.结果表明,Ru-Mn催化剂上Mn以Mn3O4存在于Ru的表面上.在加氢过程中,Mn3O4可以与浆液中ZnSO4发生化学反应生成一种难溶性的(Zn(OH)2)3(ZnSO4)(H2O)3盐.该盐易化学吸附在Ru催化剂表面上,从而在提高Ru催化剂上环己烯选择性起关键作用.当催化剂中Mn含量为5.4%时,环己烯收率为61.3%,同时具有良好的稳定性和重复使用性能.A series of Ru-Mn catalysts with different Mn contents were prepared by coprecipitation, and their catalytic performance, using nanoscale ZrO2 as a dispersant, for the selective hydrogenation of benzene to cyclohexene was investigated. The catalysts were characterized using X-ray diffraction, transmission electron microscopy, N2 physisorption, X-ray fluorescence, atomic absorption spectroscopy, and Auger electron spectroscopy. The results confirmed that the Mn existed as Mn3O4 on the Ru surface. The Mn3O4 reacted with ZnSO4 to form an insoluble [Zn(OH)2]3(ZnSO4)(H2O]3 salt, which was readily chemisorbed on the Ru surface. This chemisorbed salt played a key role in improving the cyclohexene selectivity over the Ru catalyst. The cyclohexene yield of 61.3% was obtained over the Ru-Mn catalyst with the optimum Mn content of 5.4%. This catalyst had good stability and excellent reusability.

关 键 词：苯 选择加氢 环己烯 钌 锰 二氧化锆 锌 

分 类 号：O643.32[理学—物理化学] O624.12[理学—化学]