钙钛矿型BaZrO_3负载钌催化剂氨合成和性能研究  

Ru-Based Catalysts Supported on Perovskite Type BaZrO_3 for Ammonia Synthesis

作　　者：王自庆[1] 林建新王 榕魏 可镁 

机构地区：[1]福州大学化肥催化剂国家工程研究中心,福州350002

出　　处：《无机化学学报》2013年第3期493-499,共7页Chinese Journal of Inorganic Chemistry

基　　金：中国石油科技创新基金(No.2010D-5006-0502);国家科技支撑计划(2007BAE08B02)资助项目

摘　　要：采用柠檬酸络合法制备了钙钛矿型BaZrO3纳米材料,负载Ru以后用于催化氨合成反应,研究了BaZrO3前驱体焙烧温度对载体结构和Ru/BaZrO3催化剂氨合成反应性能的影响。以X射线衍射(XRD)、CO2程序升温脱附(CO2-TPD)、N2物理吸附、扫描电镜(SEM)和H2程序升温还原技术(H2-TPR)等方法对载体材料和催化剂进行了表征。结果表明,随着焙烧温度的升高,材料的比表面积和孔容均不断降低,但是有利于BaZrO3的生成。在750℃条件下焙烧得到的催化剂表现出最高的氨合成活性。在425℃,5 MPa,空速为10 000 h-1条件下,出口氨浓度可以达到9.12%,这可能是由于载体与活性金属间的强相互作用和载体的强电子传导综合作用所致。The BaZrO3 material was synthesized by the citric acid method. A series of Ru/BaZrO3 catalyst samples were prepared using the above BaZrO3 calcined at different temperatures as the support. The support materials and catalyst samples were characterized by X-ray diffraction （XRD）, H2 temperature programmed reduction （H2-TPR）, CO2 temperature programmed desorption （CO2-TPD）, N2 adsorption-desorption isotherms and scanning electron microscopy （SEM）. The results show that the catalytic performance is greatly influenced by the calcination temperature of the BaZrO3 support. The highest catalytic activity for ammonia synthesis is obtained on the Ru-based catalyst with the support calcined at 750 ℃. The ammonia concentration of RBZ-750 can achieve to 9.12% under the condition of 425 ℃, 5 MPa and 10 000 h^-1. The strong mental-support interaction and electron conductivity of the support may be the key factors for the high activity at low reaction temperature.

关 键 词：锆酸钡 焙烧温度 钌 氨合成 金属-载体强相互作用 

分 类 号：O614.821[理学—无机化学] O614.333[理学—化学]