Electrooxidation of small organic molecules on mesoporous on precious metal catalysts I:CO and methanol on platinum

被引:81
作者
Jiang, JH [1 ]
Kucernak, A [1 ]
机构
[1] Univ London Imperial Coll Sci Technol & Med, Dept Chem, London SW7 2AZ, England
来源
JOURNAL OF ELECTROANALYTICAL CHEMISTRY | 2002年 / 533卷 / 1-2期
基金
英国工程与自然科学研究理事会;
关键词
nanostructure; electrocatalysis; mesoporous platinum; carbon monoxide; methanol;
D O I
10.1016/S0022-0728(02)01083-5
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
Nanostructured platinum prepared by the chemical reduction of hexachloroplatinic acid dissolved in aqueous domains of the liquid crystalline phases of oligoethylene oxide surfactants has been examined as an innovative model electrocatalyst. Owing to its high specific surface area and periodic mesoporous nanostructure, electrooxidation of both carbon monoxide and methanol has been investigated using cyclic voltammetry and chronoamperometry as a probe of the electrocatalytic properties of this material. The oxidation of CO adsorbed on the new type of platinum is determined by the rate of an adsorption and nucleation-growth controlled phase transformation occurring inside the CO adlayer. This mechanism appears to be different from the traditional Langmuir-Hinshelwood model for CO oxidation. The methanol electrooxidation reaction appears to proceed mainly through a direct pathway with CO as the final product and the potentiostatic current attains a steady-state value even at low potentials ( < 0.5 V). These results are very important since the nanostructured platinum shows a much lower poisoning rate at potentials relevant to fuel cell operation. Enhanced electrocatalytic durability to the methanol oxidation reaction is obtained on this new type of platinum in comparison to one high surface area platinum from Johnson-Matthey plc. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:153 / 165
页数:13
相关论文
共 81 条
[51]   Temperature-dependent hydrogen electrochemistry on platinum low-index single-crystal surfaces in acid solutions [J].
Markovic, NM ;
Grgur, BN ;
Ross, PN .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (27) :5405-5413
[52]   Electrooxidation of CO and H2/CO mixtures on Pt(111) in acid solutions [J].
Markovic, NM ;
Grgur, BN ;
Lucas, CA ;
Ross, PN .
JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (03) :487-495
[53]   INVESTIGATION OF MECHANISM OF OXIDATION OF CARBON-MONOXIDE ADSORBED ONTO A SMOOTH PT ELECTRODE IN AQUEOUS ACID [J].
MCCALLUM, C ;
PLETCHER, D .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1976, 70 (03) :277-290
[54]   CO oxidation on smooth and high area Pt, Pt-Ru and Pt-Sn electrodes [J].
Morimoto, Y ;
Yeager, EB .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1998, 441 (1-2) :77-81
[55]   Electrocatalytic oxidation of carbon monoxide at lower potentials on platinum-based alloys incorporated in polyaniline [J].
Napporn, WT ;
Leger, JM ;
Lamy, C .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1996, 408 (1-2) :141-147
[56]   Electro-oxidation of C1 molecules at Pt-based catalysts highly dispersed into a polymer matrix: Effect of the method of preparation [J].
Napporn, WT ;
Laborde, H ;
Leger, JM ;
Lamy, C .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1996, 404 (01) :153-159
[57]   LINEAR SWEEP VOLTAMMETRIC APPROACH FOR THE STUDY OF MONOLAYER FORMATION - DISTINCT FEATURES OF ADSORPTION, NUCLEATION GROWTH COLLISION AND COMBINED MODELS [J].
NOEL, M ;
CHANDRASEKARAN, S ;
BASHA, CA .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1987, 225 (1-2) :93-109
[58]  
Noel M., 1990, Cyclic Voltammetry and the frontiers of Electrochemistry
[59]   Monte Carlo simulation of CO adlayers electrooxidation on Pt(111) [J].
Orts, JM ;
Louis, E ;
Sander, LM ;
Feliu, JM ;
Aldaz, A ;
Clavilier, J .
SURFACE SCIENCE, 1998, 416 (03) :371-383
[60]   ELECTROCHEMICAL-BEHAVIOR OF CO LAYERS FORMED BY SOLUTION DOSING AT OPEN CIRCUIT ON PT(111) - VOLTAMMETRIC DETERMINATION OF CO COVERAGES AT FULL HYDROGEN ADSORPTION BLOCKING IN VARIOUS ACID-MEDIA [J].
ORTS, JM ;
FERNANDEZVEGA, A ;
FELIU, JM ;
ALDAZ, A ;
CLAVILIER, J .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1992, 327 (1-2) :261-278