Effects of Alloyed and Oxide Phases on Methanol Oxidation of Pt-Ru/C Nanocatalysts of the Same Particle Size

被引:53
作者
Godoi, Denis R. M. [1 ]
Perez, Joelma [1 ]
Villullas, H. Mercedes [1 ]
机构
[1] Univ Estadual Paulista, UNESP, Inst Quim, Dept Quim Fis, BR-14801970 Araraquara, Brazil
基金
巴西圣保罗研究基金会;
关键词
RAY ABSORPTION-SPECTROSCOPY; TEMPERATURE FUEL-CELLS; ANODE ELECTROCATALYSTS; CARBON-MONOXIDE; CATALYSTS; RUTHENIUM; ELECTROOXIDATION; ELECTRODE; PLATINUM; SN;
D O I
10.1021/jp8108804
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In this work, methanol oxidation was studied on carbon-supported Pt-Ru nanocatalysts, where the amounts of alloyed and oxide phases were modified by heat treatments in different atmospheres. Because particle growth was avoided using, mild temperature conditions, the study reported here was conducted in the absence of particle size effects. All samples were characterized by X-ray diffraction and transmission electron microscopy. The general electrochemical behavior of the nanocatalysts was evaluated by cyclic voltammetry, and the electrocatalytic activity for the oxidation of methanol was studied in 0.5 mol L-1 methanol acid solutions by linear potential sweeps and chronoamperometry. The results obtained clearly evidence that the presence of oxide species is necessary to enhance the electrocatalytic activity for methanol oxidation. Oxidation of adsorbed CO was also measured. Both reactions, methanol and adsorbed CO oxidation, were found to be very sensitive to the surface changes produced by the heat treatments. Interestingly, the best catalyst for methanol oxidation was not found to be the most efficient for the oxidation of adsorbed CO. Electrocatalytic activities correlate well with oxidation states and electronic properties analyzed by X-ray photoelectron spectroscopy and in situ dispersive X-ray absorption spectroscopy.
引用
收藏
页码:8518 / 8525
页数:8
相关论文
共 46 条
[1]  
[Anonymous], 1992, Handbook of X-Ray Photoelectron Spectroscopy: A Reference Book of Standard Spectra for Identification and Interpretation of XPS Data 1992
[2]   Formation of carbon-supported PtM alloys for low temperature fuel cells: a review [J].
Antolini, E .
MATERIALS CHEMISTRY AND PHYSICS, 2003, 78 (03) :563-573
[3]   Physical and morphological characteristics and electrochemical behaviour in PEM fuel cells of PtRu/C catalysts [J].
Antolini, E ;
Giorgi, L ;
Cardellini, F ;
Passalacqua, E .
JOURNAL OF SOLID STATE ELECTROCHEMISTRY, 2001, 5 (02) :131-140
[4]   New mechanistic aspects of methanol oxidation [J].
Batista, EA ;
Malpass, GRP ;
Motheo, AJ ;
Iwasita, T .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2004, 571 (02) :273-282
[5]   New insight into the pathways of methanol oxidation [J].
Batista, EA ;
Malpass, GRP ;
Motheo, AJ ;
Iwasita, T .
ELECTROCHEMISTRY COMMUNICATIONS, 2003, 5 (10) :843-846
[6]   THE STRUCTURE AND ACTIVITY OF PT-CO ALLOYS AS OXYGEN REDUCTION ELECTROCATALYSTS [J].
BEARD, BC ;
ROSS, PN .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1990, 137 (11) :3368-3374
[7]   Dependence of CH3OH oxidation activity for a wide range of PtRu alloys -: Detailed analysis and new views [J].
Bock, C ;
MacDougall, B ;
LePage, Y .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2004, 151 (08) :A1269-A1278
[8]   Methanol oxidation on Pt/Ru, Pt/Ni, and Pt/Ru/Ni anode electrocatalysts at different temperatures for DMFCs [J].
Choi, JH ;
Park, KW ;
Kwon, BK ;
Sung, YE .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2003, 150 (07) :A973-A978
[9]  
Cullity B. D., 1978, ELEMENTS XRAY DIFFRA
[10]   The electro-oxidation of carbon monoxide on ruthenium modified Pt(111) [J].
Davies, JC ;
Hayden, BE ;
Pegg, DJ ;
Rendall, ME .
SURFACE SCIENCE, 2002, 496 (1-2) :110-120