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Pt-Se纳米空球修饰玻碳电极上甲酸的电催化氧化
引用本文:颜亮亮,江庆宁,刘德宇,钟艳,温飞鹏,邓小聪,钟起玲,任斌,田中群.Pt-Se纳米空球修饰玻碳电极上甲酸的电催化氧化[J].物理化学学报,2010,26(9):2337-2342.
作者姓名:颜亮亮  江庆宁  刘德宇  钟艳  温飞鹏  邓小聪  钟起玲  任斌  田中群
作者单位:1. College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, P. R. China; 2. State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China
基金项目:国家自然科学基金,厦门大学固体表面物理化学国家重点实验室基金 
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/GCPtHN/GCPt/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.

关 键 词:电催化  Pt-Se  纳米空球  (Pt-Se)HN/GC  电极  甲酸  氧化  
收稿时间:2010-03-11
修稿时间:2010-06-30

Electrocatalytic Oxidation of Formic Acid on Pt-Se Hollow Nanosphere Modified Glassy Carbon Electrodes
YAN Liang-Liang,JIANG Qing-Ning,LIU De-Yu,ZHONG Yan,WEN Fei-Peng,DENG Xiao-Cong,ZHONG Qi-Ling,REN Bin,TIAN Zhong-Qun.Electrocatalytic Oxidation of Formic Acid on Pt-Se Hollow Nanosphere Modified Glassy Carbon Electrodes[J].Acta Physico-Chimica Sinica,2010,26(9):2337-2342.
Authors:YAN Liang-Liang  JIANG Qing-Ning  LIU De-Yu  ZHONG Yan  WEN Fei-Peng  DENG Xiao-Cong  ZHONG Qi-Ling  REN Bin  TIAN Zhong-Qun
Institution:1. College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, P. R. China; 2. State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China
Abstract: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 hollownanospheres ((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/GCand commercial Pt/C/GCelectrodes 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 seleniumcontent showed optimal electrocatalytic activity for the oxidation of formic acid.
Keywords:Electrocatalysis  Pt-Se hollow nanosphere  HN/GC electrode'  ')  (Pt-Se)HN/GC electrode" target="_blank">">(Pt-Se)HN/GC electrode  Formic acid  Oxidation
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