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%.
作者
冯旭
林宇
张财顺
韩蛟
庆绍军
张磊
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)
出处
《燃料化学学报》
EI
CAS
CSCD
北大核心
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。
关键词
水热温度
氧化铈
尿素
催化剂
hydrothermal temperatures
ceria
urea
catalyst
