Pd/CMK-3的合成、表征及对甲酸的电催化氧化性能研究  

Synthesis,Characterization and Electrocatalytic Performance of Pd/CMK-3 for Formic Acid Oxidation

作　　者：还中科[1,2] 宗恩敏[1,2] 魏丹[1,2] 万海勤[1,2] 郑寿荣[1,2] 许昭怡[1,2] 

机构地区：[1]南京大学环境学院,污染控制与资源化研究国家重点实验室,南京210046 [2]江苏省机动车尾气污染控制重点实验室,南京210093

出　　处：《环境科学》2012年第10期3479-3483,共5页Environmental Science

基　　金：国家自然科学基金项目(21077050);江苏省自然科学基金项目(BK2010051;BK2010378);科技部国际科技合作项目(2010DFA91910);教育部长江学者和创新团队发展计划项目(IRT1019)

摘　　要：以中孔硅SBA-15为硬模板、蔗糖为炭源,合成了有序中孔炭CMK-3,并以此CMK-3为载体,采用络合还原法制备了负载量为20%的催化剂Pd/CMK-3.X射线衍射(XRD)和透射电镜(TEM)的结果表明,CMK-3孔结构高度有序,呈现二维六方结构,Pd/CMK-3和Pd/AC(活性炭)催化剂中Pd纳米颗粒分散均匀,平均粒径分别为4.2 nm和4.5 nm;拉曼光谱测试表明,CMK-3比活性炭的石墨化程度更高,导电性更强;N2吸附/脱附实验表明,CMK-3具有典型的中孔结构,CMK-3的最可几孔径为4.5 nm,显著大于活性炭的0.54 nm,CMK-3的BET比表面积为1 114 m2.g-1,大于活性炭的871 m2.g-1.在对甲酸电催化氧化的循环伏安(CV)和计时电流(CA)测试中,Pd/CMK-3的初始催化活性显著高于Pd/AC,而两者在100 s后的计时电流稳定性则基本相当.The synthesis of mesoporous carbons CMK-3 was implemented using SBA-15 samples as the hard templates and sucrose as the carbon source.Ordered mesoporous carbon CMK-3 supported palladium catalyst with a loading amount of 20%（Pd/CMK-3） was prepared by a complexing reduction method.XRD and TEM results showed that the p6mm hexagonal symmetric pore structures of CMK-3 were highly ordered and the Pd nanoparticles with the average size of 4.2 nm and 4.5 nm were well dispersed on CMK-3 and activated carbon（AC） surfaces respectively.Raman results revealed that CMK-3 presented higher graphitization and a higher electric conductivity than AC.The most probable pore size of CMK-3 was 4.5 nm,which is larger than that of AC（0.54 nm）.The BET surface area of CMK-3 was 1 114 m2·g-1,which was also larger than that of AC（871 m2·g-1）.The mesoporous structure of CMK-3 was also observed.The Pd/CMK-3 catalyst exhibited more excellent initial electrocatalytic activity for formic acid oxidation than Pd/AC by cyclic voltammetry（CV）.But the chronoamperometry（CA） demonstrated that the stability of the two catalysts were almost equal after 100 s polarization at 0.2 V（vs.SCE）.

关 键 词：有序中孔炭 络合还原法 Pd/CMK-3 电催化氧化 甲酸 

分 类 号：X703.1[环境科学与工程—环境工程]