A study of polymer electrolyte fuel cell performance at high voltages. Dependence on cathode catalyst layer composition and on voltage conditioning

被引:89
作者
Uribe, FA [1 ]
Zawodzinski, TA [1 ]
机构
[1] Los Alamos Natl Lab, Los Alamos, NM 87545 USA
关键词
fuel cell; ORR; cathode catalyst; voltage pulsing;
D O I
10.1016/S0013-4686(02)00350-X
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
We report polymer electrolyte fuel cell (PEFC) performances at high cell voltages ( > 0.7 V). We have tested various carbon supported Pt-M alloys (M: Cr, Ni, Rh, Sn) as cathode catalysts and compared performances with Pt/C. Pt-Ni and Pt-Cr provided the best results. Fuel cell performance at high constant voltages ( > 0.8 V) decreases rapidly with time. Within 1 h currents may drop to one half of their original value. Experiments strongly suggest that, at these voltages, there is an inherent Pt activity loss for oxygen reduction reaction (ORR) due to adsorption of oxygenated species from water. We also demonstrate that OH- species (from water oxidation), which block Pt active sites, adsorb at more positive voltages on Pt-M than on Pt surfaces. Thus, we conclude that the Pt surfaces of these alloys are more active for the ORR because of slower OH- species adsorption at high cell voltages. We have also found that short time cell voltage excursions from 0.8 to 0.5 V or lower at regular intervals, completely recovers the loss of performance. Consistent with our other results, pulsing to lower voltages reactivates the Pt surface by electrodesorption of OH- or other anions. Published by Elsevier Science Ltd.
引用
收藏
页码:3799 / 3806
页数:8
相关论文
共 16 条
[1]  
HAGEDORN C, UNPUB
[2]  
Markovic NM, 1999, INTERFACIAL ELECTROCHEMISTRY, P821
[3]   ROLE OF STRUCTURAL AND ELECTRONIC-PROPERTIES OF PT AND PT ALLOYS ON ELECTROCATALYSIS OF OXYGEN REDUCTION - AN IN-SITU XANES AND EXAFS INVESTIGATION [J].
MUKERJEE, S ;
SRINIVASAN, S ;
SORIAGA, MP ;
MCBREEN, J .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1995, 142 (05) :1409-1422
[4]   TEMPERATURE-DEPENDENCE OF THE ELECTRODE-KINETICS OF OXYGEN REDUCTION AT THE PLATINUM NAFION(R) INTERFACE - A MICROELECTRODE INVESTIGATION [J].
PARTHASARATHY, A ;
SRINIVASAN, S ;
APPLEBY, AJ ;
MARTIN, CR .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1992, 139 (09) :2530-2537
[5]   Oxygen reduction on a high-surface area Pt/Vulcan carbon catalyst: a thin-film rotating ring-disk electrode study [J].
Paulus, UA ;
Schmidt, TJ ;
Gasteiger, HA ;
Behm, RJ .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2001, 495 (02) :134-145
[6]   Characterization of polymer electrolyte fuel cells using AC impedance spectroscopy [J].
Springer, TE ;
Zawodzinski, TA ;
Wilson, MS ;
Gottesfeld, S .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1996, 143 (02) :587-599
[7]  
TARASEVICH MR, 1983, COMPR TREAT, V7, pCH6
[8]   Enhancement of the electroreduction of oxygen on Pt alloys with Fe, Ni, and Co [J].
Toda, T ;
Igarashi, H ;
Uchida, H ;
Watanabe, M .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1999, 146 (10) :3750-3756
[9]   Role of electronic property of Pt and Pt alloys on electrocatalytic reduction of oxygen [J].
Toda, T ;
Igarashi, H ;
Watanabe, M .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1998, 145 (12) :4185-4188
[10]   Enhancement of the electrocatalytic O2 reduction on Pt-Fe alloys [J].
Toda, T ;
Igarashi, H ;
Watanabe, M .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1999, 460 (1-2) :258-262