铜锰盐前驱体对铜锰催化剂变换反应性能的影响  

Influence of Copper-Manganese Salt Precursors on Catalytic Performance of Copper-Manganese Catalysts for Water-Gas Shift Reaction

作　　者：何润霞[1] 智科端[1] 王斌[1] 武芳[1] 姜浩强[1] 刘全生[1] 

机构地区：[1]内蒙古工业大学化工学院内蒙古工业催化重点实验室,呼和浩特010051

出　　处：《分子催化》2015年第6期534-544,共11页Journal of Molecular Catalysis(China)

基　　金：国家自然科学基金项目(21266017;21566028;21566029);内蒙古科技计划项目(20101502);内蒙古自然科学基金项目(2015BS0206;2014MS0220)资助~~

摘　　要：以铜锰硝酸、铜锰硫酸、铜锰醋酸和铜锰氯化盐为前驱体,采用共沉淀法制备了铜锰催化剂,利用XRD、TPR、STPR（表面氧化程序升温还原）、TPD和XPS等对样品进行了表征,并考察了其水煤气变换反应催化性能.结果表明,所制备的催化剂主晶相均为尖晶石结构的Cu1.5Mn1.5O4金属固溶体,经变换反应后均被还原分解为Cu和Mn O,其中以铜锰醋酸盐制备得到的样品出现了较为明显的Mn CO3特征衍射峰.铜锰醋酸盐制备的样品因单质铜和氧化锰协同效应良好,可显著增加对CO2的吸附能力,提高其表面铜的分散性,具有良好的热稳定性和低温变换反应活性.以铜锰硝酸盐制备的样品在400~450℃维持了较高的热稳定性及催化活性,但在300℃以下CO转化率明显下降,而以铜锰硫酸盐及铜锰氯化盐制备的样品在200~450℃测试温区内催化性能较差.Copper-manganese catalysts were prepared using different Copper manganese salt precursors,copper manganese nitrate,copper manganese sulfate,copper manganese acetate and copper manganese chloride by co-precipitation method. The samples were characterized by X-ray diffraction（ XRD）,temperature-programmed reduction（ TPR）,temperature-programmed reduction of oxidized surfaces（ STPR）,temperature-programmed desorption（ TPD）,X-ray photoelectron spectrometer（ XPS）,and tested for water gas shift（ WGS） reaction. The results show the main crystalline phase of samples prepared as starting materials was a Cu1. 5Mn1. 5O4 spinel structure. After WGS reaction,the main crystalline phases were transformed into Cu and Mn O. The sample prepared with acetate as starting materials showed the most obvious Mn CO3 characteristic diffraction peaks,the Cu and Mn O showed better synergistic effects in it,which increased the adsorption of CO2 and improved the dispersion of Cu on the catalyst surface,meanwhile,it showed the best thermal stability and the highest low temperature catalytic activity. Sample prepared with nitrate as starting materials maintained high thermal stability and catalytic performance from 400 to450 ℃,but the CO conversion decreased below 300 ℃. The catalytic performance of sample prepared with sulfate and chloride as starting materials was poor,ranging from 200 to 450 ℃.

关 键 词：铜锰催化剂 铜锰盐前驱体 变换反应 催化性能 

分 类 号：TQ426.6[化学工程] O643.32[理学—物理化学]