一氧化碳和乙醇酸甲酯对草酸二甲酯加氢制备乙二醇Cu/SiO_2催化剂的影响  

Effects of CO and methyl glycolate on hydrogenation of dimethyl oxalate to ethyl glycol over Cu/SiO_2 catalysts

作　　者：张素华[1] 张博[1] 惠胜国[1] 李伟[1] 

机构地区：[1]华东理工大学化学工程国家重点实验室,上海200237

出　　处：《天然气化工—C1化学与化工》2012年第3期5-9,13,共6页Natural Gas Chemical Industry

摘　　要：研究了CO和乙醇酸甲酯(MG)对草酸二甲酯(DMO)加氢反应的影响。气相中的CO对催化活性影响较大,系统中通入一定CO后,乙二醇(EG)收率从95.6%下降至25.4%;CO对该过程影响可逆,停止进料液,用H2吹扫20h后,催化剂活性可恢复至未通CO时水平。MG浓度、进料方式及反应温度均对反应过程有较大影响。195℃较低温度时,MG预吸附对反应影响更大,MG预吸附7 h,反应35 h后,乙二醇(EG)收率仅为23.7%。MG在催化剂表面较难脱附,系统中MG浓度较高时,会生成多聚物,堵塞催化剂孔道,会导致催化剂失活。Effects of CO and methyl glycolate （MG） on hydrogenation of dimethyl oxalate to ethyl glycolover Cu/SiO2 catalysts were studied. CO in the gas phase had great influence on the catalytic activity, and the yieldof ethylene glycol （EG） decreased from 95.6 % to 25.4 % after CO was introduced to the reaction system. The effect of CO was reversible, and the activity of the catalyst could be recovered to the same extent as before CO being introduced after feeding was stopped and the system was purged by Hz for 20 hours. The catalytic activity was also affected by MG concentration, feeding way and reaction temperature. Comparing with higher temperature （200℃）, at lower temperature （195℃） catalytic activity decreased more sharply after MG pre-adsorption. The yield of EG decreased to 23.7% at 35 hours time on stream when the catalyst was pre-adsorbed with MG methanol solution （wm-=20%） for 7 hours before reaction. MG desorption from the catalyst surface was very difficult, and the polymer might be formed which could block the pores of catalyst and result in the deactivation of catalyst when the catalyst worked at high concentration of MG for a long time.

关 键 词：一氧化碳 乙醇酸甲酯 CU/SIO2催化剂 失活 草酸二甲酯 加氢 乙二醇 

分 类 号：O643[理学—物理化学]