摘要
用等体积浸渍法制备了一系列不同镍负载量的负载型Ni/TiO2催化剂,并将其应用于邻氯硝基苯加氢制邻氯苯胺的反应.采用N2吸附、X射线衍射、程序升温还原、透射电镜、H2化学吸附及间歇加压釜式反应器活性评价等方法,考察了镍负载量对Ni/TiO2催化剂的物化性质及邻氯硝基苯加氢反应性能的影响.结果表明,随着镍负载量的增加,Ni/TiO2催化剂上邻氯硝基苯的转化率逐渐提高;当镍负载量超过30%时,催化剂的活性和选择性不再明显变化.当催化剂中镍负载量高于20%时,在温度343K、氢压1·0MPa和催化剂/邻氯硝基苯质量比1/10的条件下反应210min后,邻氯硝基苯的转化率和邻氯苯胺的选择性均高于99%,催化剂具有良好的应用前景.分析表明,影响Ni/TiO2催化剂性能的主要因素为催化剂表面镍晶粒的活性表面积以及载体TiO2与金属镍之间的强相互作用.
A series of titania-supported nickel catalysts with different Ni loadings (10 % - 40 % ) were prepared by the incipient impregnation method and applied in the hydrogenation of o-chloronitrobenzene to o-chloroaniline. The effects of nickel loading on the physico-chemical properties of the Ni/TiO2 catalysts were studied by nitrogen adsorption-desorption, X-ray diffraction, temperature-programmed reduction, transmission electron microscopy, and He chemisorption. The catalyst performance for the hydrogenation was evaluated in an autoclave reactor. The results showed that the o-chloronitrobenzene conversion increased with increasing Ni loading of the Ni/TiO2 catalysts. When the Ni loading was higher than 30 %, no remarkable difference in catalyst performance was observed. For the catalysts with Ni loadings higher than 20 % under the reaction conditions of temperature 343 K, hydrogen pressure 1.0 MPa, and catalyst to o-chloronitrobenzene mass ratio of 1/10, both the o- chloronitrobenzene conversion and the selectivity for o-chloroaniline exceeded 99 % within 210 min. Hence, Ni/ TiO2 is a promising catalyst for the synthesis of o-chloroaniline. The characterization results suggested that Ni surface area and the strong metal-support interaction were important factors affecting the catalyst performance, whereas there was no distinct relation between the specific surface area and catalytic performance of the catalyst.
出处
《催化学报》
SCIE
CAS
CSCD
北大核心
2006年第7期579-584,共6页
关键词
镍
二氧化钛
负载型催化剂
邻氯硝基苯
催化加氢
邻氯苯胺
nickel
titania
supported catalyst
o-chloronitrobenzene
catalytic hydrogenation
o-chloroaniline