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作 者:李源[1,2] 张香平[1] 王蕾[1] 李春山[1] 刘龙[1,2] 张天龙[1] 张锁江[1]
机构地区:[1]中国科学院过程工程研究所多相复杂系统国家重点实验室,北京100190 [2]中国科学院研究生院,北京100049
出 处:《过程工程学报》2010年第4期781-787,共7页The Chinese Journal of Process Engineering
基 金:国家杰出青年科学基金资助项目(编号:20625618);中国科学院知识创新工程前瞻性基金资助项目(编号:082702);中国科学院知识创新工程重要方向基金资助项目(编号:KGCX2-YW-321);国家重点基础研究发展规划(973)基金资助项目(编号:2009CB219907)
摘 要:采用并流共沉淀法制备了不同Cu:(Mg+Zn)及Mg:Zn摩尔比的铜基催化剂Cu/MgO/ZnO,用于低温液相甲醇的合成,并对比了Cu/ZnO及Cu/MgO催化剂,分析了催化剂中载体MgO的作用.结果表明,MgO的引入有利于催化剂中Cu^+的生成并均匀分散在载体中,可提高催化剂的催化活性.以合成气CO+H_2为原料,在443K和5.0MPa条件下,采用液体石蜡作溶剂,考察了催化剂的催化性能.结果表明,Cu/MgO/ZnO催化剂的活性优于Cu/ZnO和Cu/MgO催化剂,且当Cu:Mg:Zn=2:1:1时催化性能最好,此时合成气中CO的转化率为63.56%,甲醇的选择性为99.09%,时空收率为5.413mol/(kg.h).分析了Cu/MgO催化剂在高温反应条件下的失活现象,认为铜烧结是其失活的主要原因.A series of Cu/MgO/ZnO catalysts with different Cu:(Mg+Zn) and Mg:Zn molar ratios were prepared by conventional co-precipitation method,which are used for low-temperature methanol synthesis.And Cu/ZnO and Cu/MgO catalysts were prepared as well.Comparison was made among them by characterization.Addition of MgO to Cu/ZnO catalyst could introduce more dispersed Cu~+ sites,therefore the catalytic activity was promoted.At 443 K and 5.0 MPa,the activities of prepared catalysts were tested in a slurry reactor using liquid paraffin as solvent.The results indicated that the activity of Cu/MgO/ZnO catalyst was superior to that of Cu/ZnO and Cu/MgO,and when Cu:Mg:Zn=2:1:1,the catalyst had the highest activity:the conversion rate of CO was as high as 63.56%,and the selectivity and space time yield of methanol reached 99.09% and 5.413 mol/(kg·h) respectively.The deactivation phenomenon of Cu/MgO/ZnO catalyst was observed under high reaction temperature,and the characterization results indicated that it was due to the sintering of Cu particles.
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