Ni-La/Ce_xZr_(1-x)O_2催化剂制备及其甲烷部分氧化/CH_4-CO_2重整耦合制合成气反应性能  

The Preparation and Performance of Ni-La/Ce_xZr_(1-x)O_2 Catalysts for Coupled Methane Partial Oxidation/CH_4-CO_2 Reforming to Syngas

作　　者：师少飞[1,2] 王玉琪[1,2] 马进成[1,2] 郑岚[1,2] 姚瑞清[1,2] 周立发 

机构地区：[1]西北大学化工学院,陕西西安710069, [2]陕西省能源化工研究院,陕西西安710069

出　　处：《分子催化》2013年第6期539-547,共9页Journal of Molecular Catalysis(China)

基　　金：国家自然科学基金项目(No.21276209);陕西省重大科技创新项目(2012ZKC03-1);陕西省教育厅专项科研计划项目(12JK0588)

摘　　要：通过共沉淀法制备铈锆固溶体作为载体,采用等体积、分步浸渍的方法制备了一系列10%Ni-3%La/Ce x Zr1-x O2(x=0、0.16、0.5、0.75、1)催化剂,并将其应用到甲烷部分氧化和甲烷二氧化碳重整耦合制合成气的反应中.对不同Ce/Zr比的催化剂性能展开研究,采用BET、XRD、H2-TPR、SEM、TG-DSC手段对载体及催化剂进行了表征.结果表明,铈锆固溶体的形成不仅提高了催化剂表面活性组分的分散度,使催化剂表面NiO晶粒尺寸从26.5 nm减到13.7 nm;而且能够加强活性组分与载体之间的相互作用,提高催化剂的热稳定性能;随着Ce/Zr比的增加,催化剂的转化率、选择性及稳定性随之增高,其顺序为:Ni-La/Ce0.75Zr0.25O2>Ni-La/Ce0.5Zr0.5O2>NiLa/Ce0.16Zr0.84O2.CexZr1-xO2 supports were prepared by coprecipitation methed. 10% Ni-3% La catalysts supported on CexZr1-xO2 were produced by an fractional wetness impregnation method and applied in syngas production, using coupled methane partial oxidation and CH4/CO2 reforming. The series of 10% Ni-3% La/CexZr1-xO2（x=O, O. 16, 0.5, 0.75, 1 ）catalysts were characterized by X-ray diffraction, H2 temperature-programmed reduction, scanning electron microscope etc. Experimental results show that Ce/Zr solid solution can improve the dispersion of active components on catalyst surface, reduce the NiO crystalline size from 26.5 nm to 13.5 nm. Moreover, it can strengthen the interaction between active metal and supports, boost the thermal stability of the catalysts. The conversion, selectivity and stability of the catalysts were enhanced with the increase of Ce/Zr ratio as follows, Ni La/Ceo.75Zr0.25O2〉Ni La/Ce0.5 Zr0.5O2〉Ni La/Ceo. 16 Zr0.84O2.

关 键 词：铈锆固溶体 甲烷部分氧化 甲烷二氧化碳重整 镍-镧催化剂 催化性能 

分 类 号：O643.32[理学—物理化学]