化工学报 ›› 2005, Vol. 56 ›› Issue (11): 2114-2118.

• 催化、动力学与反应器 • 上一篇    下一篇

氧化镧助剂对镍/二氧化硅催化剂结构和加氢性能的影响

刘迎新;陈吉祥;张继炎;何菲   

  1. 天津大学化工学院催化科学与工程系;天津大学绿色合成与转化教育部重点实验室,天津 300072
  • 出版日期:2005-11-25 发布日期:2005-11-25

Effect of La2O3 promoter on structure and hydrogenation performance of Ni/SiO2 catalyst

LIU Yingxin;CHEN Jixiang;ZHANG Jiyan;HE Fei   

  • Online:2005-11-25 Published:2005-11-25

摘要: 采用等体积浸渍法制备了La2O3改性的Ni/SiO2催化剂,考察了La2O3的引入方法对Ni/SiO2催化剂催化间二硝基苯加氢制间苯二胺反应性能的影响,并采用XRD、TPR和XPS等表征技术对催化剂的物化性质进行了研究.结果表明,La2O3的添加顺序对Ni/SiO2催化剂的物化性质和加氢性能影响非常明显.当镧以先于镍浸渍方式引入时,将大大削弱载体与镍物种之间的相互作用,镍晶粒度变小,分散度增加,催化剂的活性显著提高,间二硝基苯转化率和间苯二胺收率分别达到97.1%和93.5%.在以镍和镧共浸方式制备的催化剂中,La2O3的存在也使Ni/SiO2催化剂的反应性能有所改善,但效果没有镧先于镍浸渍方式突出.当以先浸镍后浸镧的方式加入助剂时,催化剂中的镍晶粒增大,分散性变差,催化剂的活性大幅度下降.

关键词: 氧化镧助剂, 镍/二氧化硅催化剂, 间二硝基苯, 加氢, 间苯二胺

Abstract: A series of silica supported nickel catalysts promoted by lanthanumozide were prepared by using the incipient wetness co-impregnation and sequential impregnation methods.The effect of La2O3 introducing method on the activity and selectivity of Ni/SiO2 catalyst for m-dinitrobenzene hydrogenation to m-phenylenediamine was studied,and the physical and chemical properties of the catalysts were investigated by the techniques of X-ray diffraction (XRD), temperature-programmed reduction (TPR), and X-ray photoelectron spectroscopy (XPS).The results showed that the addition sequence of La promoter played a substantial role in determining the catalytic hydrogenation properties of the nickel-based catalysts.When stepwise incipient impregnation method was used and La component was firstly impregnated on support before nickel component, the interaction between nickel and support was obviously weakened, the particle size of nickel crystallites was significantly reduced, and the nickel species were well dispersed, thus the activity of catalyst was apparently improved.In hydrogenation of m-dinitrobenzene under the conditions of hydrogen pressure 2.6 MPa, temperature 373 K and reaction time for 1 h, the conversion of m-dinitrobenzene and the yield of m-phenylenediamine on the above catalyst were up to 97.1% and 93.5%, respectively.The sample prepared by the La-Ni co-impregnation method also positively affected the catalytic performance of catalyst, but not as good as the former.When La component was impregnated after nickel component, however, the particle size of nickel crystallites increased apparently, thus resulting in dramatic decrease of catalyst activity.

Key words: 氧化镧助剂, 镍/二氧化硅催化剂, 间二硝基苯, 加氢, 间苯二胺