CoPdx oxygen reduction electrocatalysts for polymer electrolyte membrane and direct methanol fuel cells

被引:79
作者
Mustain, William E.
Kepler, Keith
Prakash, Jai [1 ]
机构
[1] IIT, Ctr Electrochem Sci & Engn, Dept Chem & Environm Engn, Chicago, IL 60616 USA
[2] Farasis Energy Inc, Hayward, CA 94545 USA
关键词
oxygen reduction; PEM fuel cell; palladium; methanol; stability;
D O I
10.1016/j.electacta.2006.08.020
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
The electrochemical activity of carbon-supported cobalt-palladium alloy electrocatalysts of various compositions have been investigated for the oxygen reduction reaction in a 5 cm(2) single cell polymer electrolyte membrane fuel cell. The polarization experiments have been conducted at various temperatures between 30 and 60 degrees C and the reduction performance compared with data from a commercial Pt catalyst under identical conditions. Investigation of the catalytic activity of the CoPdx PEMFC system with varying composition reveals that a nominal cobalt-palladium atomic ratio of 1:3, CoPd3, exhibits the best performance of all studied catalysts, exhibiting a catalytic activity comparable to the commercial Pt catalyst. The ORR on CoPd3 has a low activation energy, 52 kJ/mol, and a Tafel slope of approximately 60 mV/decade, indicating that the rate-determining step is a chemical step following the first electron transfer step and may involve the breaking of the oxygen bond. The CoPd3 catalyst also exhibits excellent chemical stability, with the open circuit cell voltage decreasing by only 3% and the observed current decreasing by only 10% at 0.8 V over 25 It. The CoPd3 catalyst also exhibits superior tolerance to methanol crossover poisoning than Pt. (c) 2006 Elsevier Ltd. All rights reserved.
引用
收藏
页码:2102 / 2108
页数:7
相关论文
共 43 条
[1]   Catalytic effect of platinum on oxygen reduction -: An ab initio model including electrode potential dependence [J].
Anderson, AB ;
Albu, TV .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2000, 147 (11) :4229-4238
[2]   Activation energies for oxygen reduction on platinum alloys: Theory and experiment [J].
Anderson, AB ;
Roques, J ;
Mukerjee, S ;
Murthi, VS ;
Markovic, NM ;
Stamenkovic, V .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (03) :1198-1203
[3]   Theoretical analysis of oxygen adsorption on Pt-based clusters alloyed with Co, Ni, or Cr embedded in a Pt matrix [J].
Balbuena, PB ;
Altomare, D ;
Agapito, L ;
Seminario, JM .
JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (49) :13671-13680
[4]   Capacitance limits of high surface area activated carbons for double layer capacitors [J].
Barbieri, O ;
Hahn, M ;
Herzog, A ;
Kötz, R .
CARBON, 2005, 43 (06) :1303-1310
[5]   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
[6]   Anode materials for low-temperature fuel cells: A density functional theory study [J].
Christoffersen, E ;
Liu, P ;
Ruban, A ;
Skriver, HL ;
Norskov, JK .
JOURNAL OF CATALYSIS, 2001, 199 (01) :123-131
[7]   Kinetics of oxygen reduction on an epitaxial film of palladium on Pt(111) [J].
Climent, V ;
Markovic, NM ;
Ross, PN .
JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (14) :3116-3120
[8]   ELECTRODE CATALYSIS OF THE 4-ELECTRON REDUCTION OF OXYGEN TO WATER BY DICOBALT FACE-TO-FACE PORPHYRINS [J].
COLLMAN, JP ;
DENISEVICH, P ;
KONAI, Y ;
MARROCCO, M ;
KOVAL, C ;
ANSON, FC .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1980, 102 (19) :6027-6036
[9]   Stability of platinum based alloy cathode catalysts in PEM fuel cells [J].
Colón-Mercado, HR ;
Popov, BN .
JOURNAL OF POWER SOURCES, 2006, 155 (02) :253-263
[10]   ELECTRODE KINETICS OF OXYGEN REDUCTION ON OXIDE-FREE PLATINUM ELECTRODES [J].
DAMJANOVIC, A ;
BRUSIC, V .
ELECTROCHIMICA ACTA, 1967, 12 (06) :615-+