The function of ruthenium oxides in Pt-Ru catalysts for methanol electro-oxidation at low temperatures

被引:42
作者
Lasch, K [1 ]
Jörissen, L [1 ]
Friedrich, KA [1 ]
Garche, J [1 ]
机构
[1] Ctr Solar Energy & Hydrogen Res Baden Wurttemberg, Div 3, D-89081 Ulm, Germany
关键词
anode catalysts; electro-oxidation; hydrous ruthenium oxides; methanol;
D O I
10.1007/s10008-003-0442-4
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
The electrocatalytic activities of different binary Pt-Ru(ox) catalysts have been investigated in half-cell experiments by cyclic voltammetry and stationary current-potential measurements. The materials have been prepared using a modification of the Adams method. X-ray analytical methods (X-ray diffraction, XRD, and energy dispersive X-ray spectroscopy, EDX) as well as thermogravimetric analysis (TGA) have been used to characterize the composition and the catalysts' content of the crystalline phases, and their surface areas have been determined by the BET method. It is found that the composition of the catalyst is strongly influenced by the synthesis temperature, which is varied between 400 and 600 degreesC. In contrast, the particle size of the metallic phases of the catalysts is not significantly affected for synthesis temperatures below 600 degreesC, as investigated by transmission electron microscopy. Synthesis temperatures of greater than or equal to500 degreesC favor the formation of crystalline RuO2 phases, whereas at synthesis temperatures below 500 degreesC the presence of metallic alloy and of hydrous oxides was derived by the combined XRD and EDX measurements. The stationary current-potential curves show a correlation with the different synthesis temperatures. It can be concluded that both the presence of an alloyed metallic Pt-Ru phase as well as the presence of amorphous hydrated Ru oxides are favorable for the electrocatalytic oxidation of methanol.
引用
收藏
页码:619 / 625
页数:7
相关论文
共 26 条
[1]   Platinum oxide as a catalyst in the reduction of organic compounds III Preparation and properties of the oxide of platinum obtained by the fusion of ceiloroplatinic acid with sodium nitrate [J].
Adams, R ;
Shriner, RL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1923, 45 :2171-2179
[2]   DIFFERENTIAL THERMAL ANALYSIS AND THERMOGRAVIMETRIC ANALYSIS OF FISSION PRODUCT OXIDES AND NITRATES TO 1500DEGREES C [J].
CAMPBELL, PF ;
ORTNER, MH ;
ANDERSON, CJ .
ANALYTICAL CHEMISTRY, 1961, 33 (01) :58-&
[3]   Methanol electro-oxidation on unsupported Pt-Ru alloys at different temperatures [J].
Chu, D ;
Gilman, S .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1996, 143 (05) :1685-1690
[4]   ON THE ROLE OF RU AND SN AS PROMOTERS OF METHANOL ELECTROOXIDATION OVER PT [J].
FRELINK, T ;
VISSCHER, W ;
VANVEEN, JAR .
SURFACE SCIENCE, 1995, 335 (1-3) :353-360
[5]   TEMPERATURE-DEPENDENT METHANOL ELECTROOXIDATION ON WELL-CHARACTERIZED PT-RU ALLOYS [J].
GASTEIGER, HA ;
MARKOVIC, N ;
ROSS, PN ;
CAIRNS, EJ .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1994, 141 (07) :1795-1803
[6]   LEIS AND AES ON SPUTTERED AND ANNEALED POLYCRYSTALLINE PT-RU BULK ALLOYS [J].
GASTEIGER, HA ;
ROSS, PN ;
CAIRNS, EJ .
SURFACE SCIENCE, 1993, 293 (1-2) :67-80
[7]   METHANOL OXIDATION ON UNSUPPORTED AND CARBON SUPPORTED PT + RU ANODES [J].
GOODENOUGH, JB ;
HAMNETT, A ;
KENNEDY, BJ ;
MANOHARAN, R ;
WEEKS, SA .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1988, 240 (1-2) :133-145
[8]  
HAGANS PL, 1997, P ELECTROCHEMICAL SO, V9713
[9]   Mechanism and electrocatalysis in the direct methanol fuel cell [J].
Hamnett, A .
CATALYSIS TODAY, 1997, 38 (04) :445-457
[10]  
Hogarth M. P., 1996, PLATIN MET REV, V40, P150, DOI DOI 10.1149/1.1837166