水热合成时间对Cu/Ce-Zr催化水气变换反应性能的影响  

Effect of hydrothermal synthesis time on the performance of Cu/Ce-Zr catalysts for catalytic water-gas shift reaction

作　　者：康玉姝 王丽宝 李永志 白金[1] 张财顺 刘道胜[1] 张磊[1] 高志贤 KANG Yu-shu;WANG Li-bao;LI Yong-zhi;BAI Jin;ZHANG Cai-shun;LIU Dao-sheng;ZHANG Lei;GAO Zhi-xian(School of Petrochemical Engineering,Liaoning Petrochemical University,Fushun 113001,China;Chemical Operation Department,Sinopec Shijiazhuang Refining and Chemical Company,Shijiazhuang 050099,China;Shenyang Ecological and Environmental Affairs Service Economic Development Zone sub-center,Shenyang 110000,China)

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]中国石化石家庄炼化公司化工运行部,河北石家庄050099 [3]沈阳市生态环境事务服务经济开发区分中心,辽宁沈阳110000

出　　处：《燃料化学学报（中英文）》2023年第6期776-782,共7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(L2019012)资助。

摘　　要：以硝酸盐为铈、锆原料,以柠檬酸代替碱类沉淀剂,固定n(Zr∶Ce)为2∶8,采用水热法合成Ce-Zr氧化物载体,再通过浸渍法制备Cu/Ce-Zr催化剂。通过XRD、BET、H2-TPR、XPS等手段对载体和催化剂进行表征,研究水热时间对催化剂结构、性质和水气变换反应性能的影响。结果表明,催化活性主要与Cu比表面积、CuO的还原温度以及催化剂表面氧空位含量有关。其中,Cu/Ce-Zr-12催化剂的Cu比表面积较大、CuO的还原温度较低,催化剂表面的氧空位数量较多,表现出较好的催化活性。在320℃、水气比(W∶M)为2,体积空速GHSV=6600 h−1的反应条件下,CO转化率为96.9%,与热力学平衡值97.1%接近。Ce-Zr oxide support was hydrothermally synthesized from metal nitrates of cerium and zirconium as the raw materials using citric acid instead of alkali precipitant,and then Cu/Ce-Zr catalyst was prepared by the impregnation method.The support and catalyst samples were characterized by XRD,BET,H2-TPR,XPS techniques,and the effects of different hydrothermal time on the structure,properties and performance in water-gas shift reaction were investigated.The results show that the catalyst activity is mainly related to the Cu specific surface area,reduction temperature of CuO and the number of oxygen vacancies on the catalyst surface.Among them,the Cu/Ce-Zr catalyst with hydrothermal time of 12 h has a large Cu specific surface area,a lower reduction temperature of CuO,and a large number of oxygen vacancies,so it shows a good catalytic activity.When the reaction temperature is 320℃,the molar ratio of water to gas(W/M)is 2,and the gas space velocity GHSV=6600 h−1,the CO conversion rate is 96.9%,which is close to the thermodynamic equilibrium value of 97.1%.

关 键 词：水热法 水热时间 水气变换 CeO_(2)-ZrO_(2)固溶体 

分 类 号：O643[理学—物理化学]