Pt-Se纳米空球修饰玻碳电极上甲酸的电催化氧化  

Electrocatalytic Oxidation of Formic Acid on Pt-Se Hollow Nanosphere Modified Glassy Carbon Electrodes

作　　者：颜亮亮[1] 江庆宁[2] 刘德宇[2] 钟艳[1] 温飞鹏[1] 邓小聪[1] 钟起玲[1] 任斌[2] 田中群[2] 

机构地区：[1]江西师范大学化学化工学院,南昌330022 [2]厦门大学化学化工学院化学系 固体表面物理化学国家重点实验室,福建厦门361005

出　　处：《物理化学学报》2010年第9期2337-2342,共6页Acta Physico-Chimica Sinica

基　　金：国家自然科学基金(20663002);厦门大学固体表面物理化学国家重点实验室基金(200511)资助项目~~

摘　　要：以无定形硒溶胶为模板制备了不同硒覆盖度(θSe)(θSe=0.49,0.39,0.06,0)的Pt-Se和Pt纳米空球(分别记为(Pt-Se)HN和PtHN),发展了利用亚硫酸盐彻底除去核壳纳米粒子上Se的方法.对获得的纳米空球进行了形貌和结构的表征,结果表明所制备的(Pt-Se)HN粒径均匀,分散性好,球壳呈多孔结构.以其作为电催化剂制备了(Pt-Se)HN修饰的玻碳(GC)电极((Pt-Se)HN/GC),利用常规电化学方法比较该电极与PtHN/GC和商用碳载铂(Pt/C)修饰GC(Pt/C/GC)电极对甲酸的催化氧化作用,发现对甲酸氧化的活性顺序为(Pt-Se)HN/GC>PtHN/GC>Pt/C/GC.三种电极催化甲酸氧化的机理有所不同:前者更倾向于通过弱吸附中间体直接氧化成CO2的单途径机理进行,后两者则通过强吸附和弱吸附中间体的双途径机理进行.在一定Se覆盖度条件下,(Pt-Se)HN/GC对甲酸的氧化有助催化作用.Platinum-selenium and platinum hollow nanospheres（denoted as（Pt-Se）HN and PtHN,respectively） with different coverages of Se（θSe）（θSe=0.49,0.39,0.06,0） were prepared using amorphous Se colloids as a sacrificial template.Sulfite was used to completely remove Se from the core-shell nanoparticles.The morphology and structure of the nanoparticles were characterized using various methods,which revealed a hollow structure with a very uniform size distribution and a porous structure on the shell.Assembly of Pt-Se hollow nanospheres（（Pt-Se）HN） on a glassy carbon（GC） electrode produced a（Pt-Se）HN/GC electrode.The electrocatalytic activity of the electrode for the oxidation of formic acid was compared with the PtHN/GC and commercial Pt/C/GC electrodes by cyclic voltammetry and chronoamperometry.The activity followed the order：（Pt-Se）HN/GC PtHN/GC Pt/C/GC.The electrooxidation of formic acid on（Pt-Se）HN/C,PtHN/C,and Pt/C catalysts follows different mechanisms：the former tends to directly oxidize formic acid to CO2 via weakly adsorbed intermediates,and the latter two via both weakly and strongly adsorbed intermediates.（Pt-Se）HN with a suitable selenium content showed optimal electrocatalytic activity for the oxidation of formic acid.

关 键 词：电催化 Pt-Se纳米空球 (Pt-Se)HN/GC电极 甲酸 氧化 

分 类 号：O646.54[理学—物理化学]