TiO_x(x<2)表面修饰Ni/TiO_2-SiO_2催化顺酐液相选择加氢合成γ-丁内酯  

Selective Hydrogenation of Maleic Anhydride to γ-Butyrolactone over TiO_x (x < 2) Surface-Modified Ni/TiO_2-SiO_2 in Liquid Phase

作　　者：杨燕萍[1] 张因[1] 高春光[1] 赵永祥[1] 

机构地区：[1]山西大学化学化工学院,精细化学品教育部工程研究中心,山西太原030006

出　　处：《催化学报》2011年第11期1768-1774,共7页

基　　金：国家自然科学基金(21073114)~~

摘　　要：以TiO2-SiO2复合氧化物气凝胶为载体,制备了一系列Ni/TiO2-SiO2催化剂,并采用N2物理吸附-脱附、H2程序升温还原/脱附、X射线衍射及原位漫反射傅里叶变换红外光谱等技术对催化剂进行了表征,考察了载体中钛含量对催化剂结构、表面性质及其催化顺酐液相选择加氢合成γ-丁内酯反应性能的影响.结果表明,较小的Ni0晶粒有利于γ-丁内酯的生成.在催化剂活性组分的还原过程中,随着载体中钛含量的增加,越来越多的TiO2被还原为TiOx(x<2)物种.Ni0晶粒和TiOx物种的协同作用影响了催化剂的羰基加氢性能;当较小的Ni0晶粒匹配合适的TiOx物种时,催化剂表现出较高的羰基加氢活性.TiO2-SiO2 aerogel with different TiO2 content was prepared by the sol-gel method. Ni/TiO2-SiO2 catalyst samples were then prepared via impregnation and were applied to the selective hydrogenation of maleic anhydride （MA） to y-butyrolactone （GBL）. The catalyst samples were characterized by infrared spectroscopy, N2 adsorption-desorption, temperature-programmed reduction, X-ray diffraction, dif- fuse reflectance infrared Fourier transform spectroscopy, and H2 temperature-programmed adsorption-mass spectroscopy techniques. The characterization results indicated that smaller Ni0 species favored the formation of GBL. Meanwhile, TiOx （x 〈 2） species, produced by the partial reduction of TiO2, was generated during the reduction process. The formation of TiOx （x 〈 2） species effectively promoted the hydrogenation of C=O group. Therefore, the hydrogenation of carbonyl was affected by both the size ofNi0 and TiOx species. When the synergistic effect of small Ni0 and TiOx species existed, the catalyst showed higher hydrogenation activity for C=O group.

关 键 词：镍 氧化钛 氧化硅 负载型催化剂 顺酐 选择加氢 丁内酯 

分 类 号：TQ225.241[化学工程—有机化工]