非Mo基高温耐硫甲烷化催化剂研究

摘要

制备非Mo基的CeO2-ZrO2催化剂,在固定床反应器于650℃,3MPa,GHSV=5000h-1,V (H2)/V (CO)=1.0且含有体积分数为0.6％的H2S的合成气中考察催化剂制备方法、成分比例和热稳定添加剂(La、Mg、Y)对其高温耐硫甲烷化性能的影响.采用N2物理吸附、H2程序升温还原、X射线衍射对催化剂进行了表征.结果表明,共沉淀法制备的催化剂(CeO2-ZrO2)比浸渍法制备的催化剂(CeO2/ZrO2)的高温甲烷化活性高,稳定性好.XRD表征发现,共沉淀法制备的CeO2-ZrO2催化剂能形成类合金.共沉淀过程中添加La助剂有利于提高催化剂的热稳定性.%The non-Mo-based catalysts--modified CeO2-ZrO2 were prepared,and the effects of preparation methods,proportions of components and thermal stability additives (La,Mg,Y) on the performances of the catalysts for high temperature sulfur-resistant methanationin were investigated in a fixed-bed reactor under the reaction conditions of 650℃,3MPa,GHSV of 5000h1 and the syngas with the H2/CO volume ratio of 1.0 and containing H2S of 0.6％ by volume.The results indicate that the catalysts prepared by co-precipitation (CeO2-ZrO2) have better activity and stability than the catalysts prepared by impregnation (CeO2/ZrO2) during the methanation reaction at high temperature.XRD results show that the co-precipitated CeO2-ZrO2 catalysts can form metal alloy.In the process of co-precipitation adding La additive can improve the thermal stability of the catalyst.