以Ce(NO_3)_3·6H_2O和ZrO(NO_3)_2·2H_2O为原料采用改进溶胶-凝胶法合成了纳米级铈锆固溶体,考察了不同铈锆摩尔比和温度条件对制备固溶体的粒度、晶型和还原性能的影响,获得了优化工艺条件.采用XRD、比表面积测定(BET)、扫描电子显微镜(SEM)、程序升温还原(TPR)进行表征.结果表明:此方法制备的固溶体均为立方萤石结构的铈锆固溶体复合氧化物,其比表面积可达92m~2/g;450℃焙烧制备的样品具有良好的还原活性.在常压固定床流动体系中进行乙醇水蒸气重整反应结果表明:当n(Ce):n(Zr)=3:1时,CeO_2-ZrO_2固溶体比CeO_2和其它比例的固溶体具有更高的催化活性和对氢气的选择性.ZrO_2的引入不但改进了CeO_2的热稳定性,而且提高了CeO_2的还原能力.
The nanosized CeO_2-ZrO_2 solid solutions were prepared by modified Sol-Gel method with Ce(NO_2)_3-6H_2O and ZrO(NO_3)_2·2H_2O as starting materials.The effects of different Ce/Zr molar ratio and calcination temperature on the particle size,crystal type and reducibility were studied to obtain optimal preparation condition. CeO_2-ZrO_2 solid solution was characterized by XRD,SEM and TPR measurements.Results show that the highest specific surface area of CeO_2-ZrO_2 solid solution is 92m~2/g while Ce/Zr molar ratio is 3:1.CeO_2-ZrO_2 solid solution prepared by modified Sol-Gel method is fluorite structured.TPR results show that CeO_2-ZrO_2 solid solution calcined at 450℃has good catalytic reducibility.Catalytic properties are estimated through a fix-bed reactor under atmospheric pressure.CeO_2-ZrO_2 solid solution with Ce/Zr molar ratio of 3:1 show higher catalytic activity and selectivity to ethanol steam reforming reaction than those of CeO_2 and other molar ratio CeO_2-ZrO_2 solid solution. Both reducibility and heat stability of CeO_2 can be improved with the addition of ZrO_2.