摘要
近年来,具有丰富活性中心的二维合金高效电催化剂的合成引起人们极大关注.本工作以十六烷基三甲基溴化铵和六羰基钼为结构导向剂合成出三金属钯-银-铜纳米片组装体.用高角度环形暗场扫描透射电子显微镜、透射电子显微镜和X射线衍射仪对三金属PdAgCu纳米片组装体的形貌和结构进行了表征.结果表明三金属Pd6Ag3Cu2纳米片组装体电催化性能优异,且对乙二醇氧化反应(5696 mA mgPd^(-1))和乙醇氧化反应(4374 mA mgPd^(-1))具有良好的催化稳定性.电催化活性的增强可归因于应变效应、配体效应及双功能效应的协同作用.本文系统研究了三金属电催化剂对C2醇的电催化机理,发现较高的羟基和C2醇浓度有利于乙二醇氧化反应和乙醇氧化反应.
The synthesis of two-dimensional(2D)alloyed efficient electrocatalysts with several active sites has attracted considerable attention in recent years.In this work,trimetallic palladium-silver-copper(PdAgCu)nanosheet assemblies(NS As)are synthesized in the presence of cetyltrimethylammonium bromide and molybdenum hexacarbonyl as the structure-directing agents.The morphologies and structures of the trimetallic PdAgCu NS As are identified by high-angle annular dark-field scanning transmission electron microscopy,transmission electron microscopy,and X-ray diffraction.The trimetallic Pd6Ag3Cu2NS A has high electrocatalytic performance with outstanding long-term stabilities for ethylene glycol oxidation reaction(EGOR=5696 mA mgPd^(-1))and ethanol oxidation reaction(EOR=4374 mA mgPd^(-1)).The enhanced electrocatalytic activities can be attributed to the synergistic effects,including strain,ligand,and bifunctional effects.Furthermore,the electrocatalytic mechanisms of the trimetallic electrocatalysts toward C2alcohols are determined,and high concentrations of OH-and C2alcohols favor EGOR and EOR.
作者
李泽
劳显焯
杨立康
傅爱萍
郭培志
Ze Li;Xianzhuo Lao;Likang Yang;Aiping Fu;Peizhi Guo(Institute of Materials for Energy and Environment,College of Materials Science and Engineering,Qingdao University,Qingdao 266071,China;College of Chemistry and Chemical Engineering,Qingdao University,Qingdao 266071,China)
基金
supported by the National Natural Science Foundation of China(22172084 and 21773133)
the World-Class Discipline Program of Shandong Province,China。
