物理化学学报 >> 2003, Vol. 19 >> Issue (05): 450-454.doi: 10.3866/PKU.WHXB20030515

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镍基催化剂的制备、表征及选择加氢性能

赵永祥;秦晓琴;侯希才;徐贤伦;刘滇生   

  1. 山西大学化学化工学院,太原 030006;中国科学院兰州化学物理研究所, 羰基合成与选择氧化国家重点实验室, 兰州 730000
  • 收稿日期:2002-08-05 修回日期:2002-10-16 发布日期:2003-05-15
  • 通讯作者: 刘滇生 E-mail:dsliu@mail.sxu.edu.cn

Preparation,Characterization and Properties of Selective Hydrogenation on Ni-based Catalysts

Zhao Yong-Xiang;Qin Xiao-Qin;Hou Xi-Cai;Xu Xian-Lun;Liu Dian-Sheng   

  1. School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006;State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000
  • Received:2002-08-05 Revised:2002-10-16 Published:2003-05-15
  • Contact: Liu Dian-Sheng E-mail:dsliu@mail.sxu.edu.cn

摘要: 研究了溶胶-凝胶-超临界流体干燥法(sol-gel-SCFD)和浸渍法(IM)制备的SiO2负载镍催化剂的顺酐液相加氢性能,并用XRD、TPR、IR等手段对催化剂的体相和表面结构进行了表征.结果表明: 1) Sol-Gel-SCFD法制备的催化剂其体相和表面结构与镍含量有关,当镍含量 < 30%(质量分数)时,NiO主要以簇团形式存在;随镍含量增高到50%,过量的NiO以微晶态存在并覆盖部分NiO簇团.顺酐(MA)加氢产物有丁二酸酐(SA)和γ-丁内酯(γ-BL),它们的选择性随镍含量增加呈规律性变化;在镍含量为30%的催化剂上γ-BL选择性呈现最大值. 2) IM法制备的催化剂其体相和表面结构与镍含量无关,当镍含量在6%~30%范围内变化时,NiO都以结晶态存在,MA加氢产物为SA; NiO与SiO2的相互作用随镍含量增加而减弱,SA的选择性不变.

关键词: 溶胶-凝胶-超临界流体干燥法, 浸渍法, 镍基催化剂, 催化加氢

Abstract: Nickel catalysts with SiO2 as the support were prepared by impregnation (IM) and sol-gel-supercritical fluid drying (Sol-Gel-SCFD) methods. The catalyst were tested with hydrogenation of maleic anhydride (MA) and characterized by XRD, TPR and IR techniques. The preparation methods and nickel content determine the catalysts final structure, activity and selectivity. The NiO forms and interaction with SiO2 are important factors affecting the activity and selectivity. For catalyst prepared by Sol-Gel-SCFD method, the NiO form is related to the Ni content, and the hydrogenation products of MA are succinic anhydride (SA) and γ-butyrolactone (γ-BL).But for catalyst prepared by IM method, the form of NiO is independent on the Ni content, and the MA hydrogenation product is SA only.

Key words: Sol-gel-supercritical fluid drying, Impregnation, Nibased catalysts,  Catalytic hydrogenation