Methanol oxidation reaction on Ti/RuO2(x)Pt(1-x) electrodes prepared by the polymeric precursor method

被引:26
作者
Freitas, R. G.
Marchesi, L. R.
Oliveira, R. T. S.
Mattos-Costa, F. I.
Pereira, E. C.
Bulhoes, L. O. S.
Santos, M. C.
机构
[1] Univ Fed ABC, Ctr Ciencias Nat & Humanas, Lab Eletroquim & Mat Nanoestruct, LEMN,CCNH, BR-09210170 Bairro Bangu, Santo Andrei, Brazil
[2] Univ Fed Sao Carlos, Dept Quim, Ctr Multidisciplinar Para Desenvolvimento Mat Cer, Lab Interdisciplinar Eletroquim & Ceram, BR-13560905 Sao Carlos, SP, Brazil
[3] Univ Sao Paulo, Inst Quim, Grp Mat Eletroquim & Metodos Eletroanaltt, BR-13566590 Sao Carlos, SP, Brazil
[4] UNICEP, Ctr Univ Cent Paulista, CENIP, BR-13563470 Sao Carlos, SP, Brazil
基金
巴西圣保罗研究基金会;
关键词
methanol oxidation reaction; electrocatalysis; Pt nanoparticles; polymeric precursor method;
D O I
10.1016/j.jpowsour.2007.06.046
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, ruthenium oxide films containing platinum nanoparticles were prepared using the polymeric precursor method on Ti substrates with several molar ratios. This paper aims at presenting the characterization of the Pt content effect in the methanol electrochemical oxidation reaction. The films were physically characterized using X-ray diffraction and both Pt and RuO2 (rutile) phases were observed. The mean crystallite sizes were 6 nm for Pt and 25 nm for RuO2. The X-ray photoelectronic results indicated that on the electrodes surfaces, depending on the substrate, there was RuO2, Ru metal and Pt metal. Besides, it was not observed the formation of PtRu alloys. The atomic force microscopy images of the films showed highly rough surfaces. A decrease in the roughness mean square values is observed as the Pt content increases. These last results are similar to electroactive surface area values calculated by redox-couple (K4FeCN6/K3FeCN6). There was an increase in the globular size observed on the electrode surface and lower particle dispersion as the Pt content is increased from 12.5 to 75 mol%. Regarding the eletrode electrocatalytical behavior for methanol oxidation, it was observed that the onset oxidation overpotential is displaced towards more negative values as Pt content is decreased. Besides, an increase has been shown in the current density for methanol oxidation of 600% using a Ti/RuO2-Pt (87.5:12.5) electrode compared to polycrystalline Pt. (C) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:373 / 380
页数:8
相关论文
共 35 条
[1]   INNER AND OUTER ACTIVE SURFACE OF RUO2 ELECTRODES [J].
ARDIZZONE, S ;
FREGONARA, G ;
TRASATTI, S .
ELECTROCHIMICA ACTA, 1990, 35 (01) :263-267
[2]  
Briggs D., 1993, PRACTICAL SURFACE AN, V1
[3]   ELECTROOXIDATION OF METHANOL AND RELATED COMPOUNDS AT RUTHENIUM DIOXIDE-COATED ELECTRODES [J].
BURKE, LD ;
MURPHY, OJ .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1979, 101 (03) :351-361
[4]   The influence of PtRu atomic composition on the yields of ethanol oxidation: A study by in situ FTIR spectroscopy [J].
Camara, GA ;
de Lima, RB ;
Iwasita, T .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2005, 585 (01) :128-131
[5]   Synthesis of hydrous ruthenium oxide supported platinum catalysts for direct methanol fuel cells [J].
Chen, ZG ;
Qiu, XP ;
Lu, B ;
Zhang, SC ;
Zhu, WT ;
Chen, LQ .
ELECTROCHEMISTRY COMMUNICATIONS, 2005, 7 (06) :593-596
[6]  
Cullity B.D., 1967, ELEMENTS XRAY DIFFRA, P262
[7]   Electro-oxidation of ethanol on Pt, Rh, and PtRh electrodes. A study using DEMS and in-situ FTIR techniques [J].
de Souza, JPI ;
Queiroz, SL ;
Bergamaski, K ;
Gonzalez, ER ;
Nart, FC .
JOURNAL OF PHYSICAL CHEMISTRY B, 2002, 106 (38) :9825-9830
[8]   ELECTROCHEMICAL OXIDATION AND REDUCTION OF RUO2-TI ELECTRODE SURFACE [J].
DOBLHOFER, K ;
METIKOS, M ;
OGUMI, Z ;
GERISCHER, H .
BERICHTE DER BUNSEN-GESELLSCHAFT-PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1978, 82 (10) :1046-1050
[9]   On the structure effects of bimetallic PtRu electrocatalysts towards methanol oxidation [J].
Dubau, L ;
Hahn, F ;
Coutanceau, C ;
Léger, JM ;
Lamy, C .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2003, 554 :407-415
[10]   Methanol and ethanol electroxidation using Pt electrodes prepared by the polymeric precursor method [J].
Freitas, R. G. ;
Santos, M. C. ;
Oliveira, R. T. S. ;
Bulhoes, L. O. S. ;
Pereira, E. C. .
JOURNAL OF POWER SOURCES, 2006, 158 (01) :164-168