Cr掺杂对Cu-Ce复合催化剂催化甲醇水蒸气重整制氢的影响  

Effect of Cr doping on hydrogen production via methanol steam reforming over Cu-Ce composite catalysts

作　　者：王东哲 王丽宝 张磊[1] 庆绍军[2] 韩蛟[1] 张财顺 高志贤 冯旭浩 WANG Dong-zhe;WANG Li-bao;ZHANG Lei;QING Shao-jun;HAN Jiao;ZHANG Cai-shun;GAO Zhi-xian;FENG Xu-hao(College of Chemistry,Chemical Engineering and Environmental Engineering,Liaoning Shihua University,Fushun 113001,China;Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;No.3 Refinery of Fushun Petrochemical Company of CNPC,Fushun 113001,China)

机构地区：[1]辽宁石油化工大学化学化工与环境学部,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]中国石油天然气股份有限公司抚顺石化分公司石油三厂,辽宁抚顺113001

出　　处：《燃料化学学报》2020年第5期619-625,I0007,共8页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21376237);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);辽宁省自然科学基金指导计划项目(2019-ZD-0371)资助。

摘　　要：采用浸渍法制备了不同Cr含量的Cr/Cu-Ce催化剂,通过N2O滴定、H2-TPR和XPS等表征,对其结构、性质和催化性能进行了探究。结果表明,Cr助剂会改变Cu-Ce催化剂的铜比表面积、CuO还原温度以及氧空穴含量。其中,添加3%Cr的催化剂的Cu比表面积较大,CuO还原温度较低,氧空穴较多,进而表现出优良的催化性能。当反应温度为533 K,n(水)∶n(甲醇)=1.2∶1,甲醇和水的进料量为0.072 mL/min时,其催化效率达100%,重整气体组分中的CO体积分数为0.15%。与未掺杂Cr助剂的催化剂相比,其催化效率提高了10%,重整气体组分中的CO体积分数降低了0.34%。Cr/Cu-Ce catalyts with different Cr contents were prepared by impregnation method,and their structures,properties and catalytic performance were investigated using N2O titration,H2-TPR and XPS techniques.It is found that the Cr doping changs the specific surface area of copper,the reduction temperature of CuO and oxygen vacancies of the Cu-Ce catalysts.In addition,the catalyst with 3%Cr addition has larger Cu specific surface area,lower CuO reduction temperature and more oxygen vacancies,thus exhibits excellent catalytic performance.The catalytic efficiency reaches 100%and CO volume fraction in outlet gas is 0.15%when the reaction temperature is 533 K,n(water)∶n(methanol)is 1.2∶1 and the feeding rate of methanol and water is 0.072 mL/min.Compared with the un-doped Cr catalyst,the catalytic efficiency increases by 10%and the volume fraction of CO in the outlet gas decreases by 0.34%.

关 键 词：CR掺杂 氧空穴 Cu-Ce催化剂 还原温度 

分 类 号：O643[理学—物理化学]