Ru/ZrO_2催化剂在苯部分加氢反应中的粒径效应

来源 :中国科学:化学 | 被引量 : 0次 | 上传用户:bobypig_31
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采用多元醇还原法将2.4~5.4 nm范围内粒径均一、尺寸可控的Ru纳米粒子负载在ZrO2上,研究了Ru的粒径对Ru/ZrO2催化剂上苯部分加氢性能的影响.采用紫外-可见吸收光谱(UV-Vis)、N2物理吸附、H2化学吸附、H2-程序升温脱附(H2-TPD)、粉末X射线衍射(XRD)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)等手段对催化剂进行了系统的表征.研究表明,用于还原的醇的种类及添加剂乙酸钠的浓度对Ru粒径有显著影响.在苯部分加氢反应中,Ru/ZrO2催化剂有明显的粒径效应.随着Ru粒径的增大,苯的转换频率(TOF)提高,环己烯初始选择性(S0)则呈火山型变化趋势,选择性最高时的Ru粒径为4.4 nm.1,2-丙二醇还原得到的Ru/ZrO2催化剂上S0及环己烯得率最高,分别可达82%和39%.结合催化剂的表征和加氢结果,讨论了Ru粒径影响苯部分加氢活性和选择性的原因. Ru-ZrO2 catalyst was used to study the effect of Ru on the hydrogenation of benzene over Ru / ZrO2 catalyst by using polyol reduction method to uniformize the size of Ru nanoparticles on the ZrO2 in the range of 2.4-5.4 nm. - UV-Vis, N2 physisorption, H2 chemisorption, H2-TPD, XRD, TEM and X-ray photoelectron spectroscopy (XPS) were used to characterize the catalysts. The results showed that the type of alcohol used for reduction and the concentration of sodium acetate as additive had a significant effect on the particle size of Ru. In the partial hydrogenation of benzene, Ru / ZrO2 catalyst had Obvious particle size effect.With the increase of Ru particle size, benzene conversion frequency (TOF) increased, the initial selectivity of cyclohexene (S0) showed a volcanic trend, the highest selectivity of Ru particle size of 4.4 The highest yields of S0 and cyclohexene on the Ru / ZrO2 catalyst obtained from the reduction of 1, 2-propanediol were 82% and 39%, respectively.With the characterization of the catalyst and hydrogenation results, the effect of Ru particle size on the benzene fraction Hydrogenation activity and selectivity reasons.
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