水热合成温度对CuO/CeO_(2)催化甲醇水蒸气重整制氢性能的影响  

Effects of hydrothermal reaction temperatures on the performance of CuO/CeO_(2) catalyst for hydrogen production from steam reforming methanol

作　　者：冯旭 林宇 张财顺 韩蛟 庆绍军[2] 张磊[1] 高志贤 官国清 FENG Xu;LIN Yu;ZHANG Cai-shun;HAN Jiao;QING Shao-jun;ZHANG Lei;GAO Zhi-xian;GUAN Guo-qing(Liaoning Petrochemical University,School of Petrochemical Engineering,Fushun 113001,China;Shanxi Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;Energy Conversion Engineering Laboratory,Institute of Regional Innovation,Hirosaki University,Matsubara 030-0813,Japan)

机构地区：[1]辽宁石油化工大学石油化工学院,辽宁抚顺113001 [2]中国科学院山西煤炭化学研究所,山西太原030001 [3]国立弘前大学区域创新研究所能量转换工程实验室,青森松原030-0813

出　　处：《燃料化学学报》2022年第7期832-840,共9页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21673270);辽宁省教育厅科学研究经费项目(L2019038);辽宁省自然科学基金面上项目(2019-MS-221)资助。

摘　　要：以Ce(NO_(3))_(3)·6H_(2)O为铈源,尿素为沉淀剂,采用水热法制备纳米CeO_(2)载体,并通过改变水热合成温度来控制CeO_(2)载体的微观结构,再通过等体积浸渍法制得CuO/CeO_(2)催化材料,并将其应用在甲醇水蒸气重整制氢反应(MSR)中进行性能评价。通过低温N2吸附-脱附、XRD、H_(2)-TPR、XPS等表征,探究了不同水热合成温度对纳米CeO_(2)载体的微观结构、CuO/CeO_(2)催化材料结构和甲醇水蒸气重整制氢反应性能的影响。结果表明,在水热合成温度为180℃条件下制备的纳米CeO_(2)载体具有立方萤石结构,且负载CuO后制备的CuO/CeO_(2)催化材料中表相CuO的还原温度较低、Cu-Ce间的相互作用较强、催化材料表面氧空穴较多,因此,表现出较好的催化活性。当反应温度为280℃,水醇物质的量比(W/M)为1.2,甲醇水蒸气气体空速(GHSV)为800 h^(−1)时,甲醇转化率可达到91.0%,重整气中CO摩尔分数为1.29%。Using cerium nitrate as the source material and urea as the precipitant,nanometer CeO_(2)carrier was prepared by hydrothermal method,and the microstructure of CeO_(2)carrier was controlled by changing the hydrothermal reaction temperature.Then the CuO/CeO_(2)catalytic material was prepared by loading CuO on the CeO_(2)carrier and evaluated in methanol steam reforming for hydrogen production.Based on the characterization data of low temperature nitrogen adsorption,XRD,H_(2)-TPR and XPS,the effects of hydrothermal reaction temperature on the microstructure of CeO_(2),the structure of CuO/CeO_(2)catalytic material and the performance of methanol steam reforming were investigated.The results show that the nanometer CeO_(2)support prepared at 180℃has a cubic fluorite structure.After loading CuO onto the CeO_(2),the obtained CuO/CeO_(2)catalyst exhibits better catalytic activity due to its stronger Cu-Ce interaction,lower reduction temperature of Cu species in the surface,and more oxygen vacancies on the surface of the catalyst.When the reaction temperature is 280℃,the molar ratio of water to alcohol(W/M)is 1.2,and the space velocity of methanol vapor gas(GHSV)is 800 h^(−1),the methanol conversion rate can reach 91.0%,the mole fraction of CO in reforming gas is 1.29%.

关 键 词：水热温度 氧化铈 尿素 催化剂 

分 类 号：O643[理学—物理化学]