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作 者:田龙[1,4] 龙艳 宋术岩 王成[1,3] TIAN Long;LONG Yan;SONG Shuyan;WANG Cheng(State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Science,Changchun 130022,China;College of Chemistry and Materials Science,Sichuan Normal University,Chengdu 610068,China;Institute for New Energy Materials&Low-Carbon Technologies,Tianjin University of Technology,Tianjin 300384,China;University of Chinese Academy of Sciences,Beijing 100049,China)
机构地区:[1]中国科学院长春应用化学研究所,稀土资源利用国家重点实验室,长春130022 [2]四川师范大学化学与材料科学学院,成都610068 [3]天津理工大学新能源材料与低碳技术研究院,天津300384 [4]中国科学院大学,北京100049
出 处:《高等学校化学学报》2019年第12期2549-2555,共7页Chemical Journal of Chinese Universities
基 金:国家重点研发计划项目(批准号:2017YFA0700104);国家自然科学基金(批准号:21571170);天津市自然科学基金(批准号:17JCZDJC000)资助~~
摘 要:通过构建CeO2与过渡金属氧化物的复合材料提高了CeO2的高温热稳定性并改善其催化活性.利用溶剂热法合成了不同组成的三维花状结构Mn/CuO-CeO2多元复合纳米材料.XRD分析结果表明,复合材料是以萤石相CeO2结构为主体的固溶体;SEM照片显示花状结构微球由无数纳米片组装而成,而每个纳米片的结构单元为尺寸约10nm的纳米颗粒.复合材料中CuO和MnOx的高分散性使各组分之间产生强的相互作用,所以催化剂的催化活性按照CeO2<CuO-CeO2<x Mn/CuO-CeO2的顺序依次升高.随着Mn掺杂量的增加,复合材料的催化活性先升高后降低,在nCe∶nCu∶nMn=25∶5∶2时催化剂表现出最佳催化性能:在CO氧化反应中,173℃时即能实现CO的完全转化,并且具有很好的催化稳定性.The unique properties make CeO2 play important roles in many catalytic reactions.However,CeO2 alone as a catalyst is fairly unfavorable due to its low catalytic activity and poor stability for hightemperature reactions.Therefore,in this work,we constructed the composite of CeO2 and transition metal oxides for the purpose of increasing the stability and improving the catalytic performance of CeO2.We synthesized the Mn/CuO-CeO2 composite nanomaterials with different components and three-dimensional flower-like structures via solvent thermal method.The XRD patterns confirmed that the synthesis formed solid solutions affording the single phase of fluorite-type CeO2.And the SEM images showed the composites have flowerlike structures which were assembled by numerous nanocrystals and the structural unit of each nanocrystal was nanoparticles with a size of about 10 nm.The catalytic activity of the catalyst increases successively in the order of CeO2<CuO-CeO2<xMn/CuO-CeO2 mainly associated with the strong interaction between constituents owing to the highly dispersed copper and manganese species.And with the increase of Mn doping,the catalytic activity of the composite increases first and then decreases.When nCe∶nCu∶nMn=25∶5∶2,the catalyst exhibited the best catalytic performance:the complete transformation of CO can be achieved at 173℃ in CO oxidation test,and it showed good stability.
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