Oxygen reduction reaction on a Pt/carbon fuel cell catalyst in the presence of trace quantities of ammonium ions: An RRDE study

被引:31
作者
Lopes, Thiago [1 ,2 ]
Chlistunoff, Jerzy [1 ]
Sansinena, Jose-Maria [1 ]
Garzon, Fernando H. [1 ]
机构
[1] Los Alamos Natl Lab, Los Alamos, NM 87545 USA
[2] Univ Sao Paulo, Inst Quim Sao Carlos, BR-13560970 Sao Carlos, SP, Brazil
关键词
ORR kinetics; Ammonia; Contaminant; PEMFCs; PERCHLORIC-ACID; PLATINUM; PT(111); CHARGE;
D O I
10.1016/j.ijhydene.2011.12.040
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
The effect of trace quantities of ammonia on oxygen reduction reaction (ORR) on carbon-supported platinum catalysts in perchloric acid solutions is assessed using rotating ring disk electrode (RRDE) technique. The study demonstrates that ammonia has detrimental effects on ORR. The most significant effect takes place in the potential region above 0.7 V vs RHE. The effect is explained by the electrochemical oxidation of ammonia, which blocks Pt active sites and increases the formation of H2O2. This leads to losses in the disk currents and increments in the ring currents. The apparent losses in ORR currents may occur in two ways, namely, through the blocking of the active sites for ORR as well as by generating a small anodic current, which is believed to have a lower contribution. In addition, a detrimental effect of sodium cations in the potential range below 0.75 V vs RHE was demonstrated. This effect is most likely due to the co-adsorption of sodium cations and perchlorate anions on the Pt surface. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:5202 / 5207
页数:6
相关论文
共 28 条
[1]  
Adzic R, 1998, FRONT ELECT, P197
[2]   Potential of zero total charge of palladium modified Pt(111) electrodes in perchloric acid solutions [J].
Alvarez, B ;
Climent, V ;
Rodes, A ;
Feliu, JM .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2001, 3 (16) :3269-3276
[3]  
ANGERSTEINKOZLOWSKA H, 1979, J ELECTROANAL CHEM, V100, P417, DOI 10.1016/0368-1874(79)85127-8
[4]  
[Anonymous], US FREEDOMCAR FUEL S
[5]  
Bard AJ., 2001, ELECTROCHEMICAL METH, P473
[6]   POTENTIALS OF ZERO TOTAL AND ZERO FREE CHARGE OF PLATINUM GROUP METALS [J].
FRUMKIN, AN ;
PETRII, OA .
ELECTROCHIMICA ACTA, 1975, 20 (05) :347-359
[7]   The Impact of Impurities On Long Term PEMFC Performance [J].
Garzon, Fernando H. ;
Lopes, Thiago ;
Rockward, Tommy ;
Sansinena, Jose-Maria ;
Kienitz, Brian ;
Mukundan, Rangachary ;
Springer, Thomas .
PROTON EXCHANGE MEMBRANE FUEL CELLS 9, 2009, 25 (01) :1575-1583
[8]   Effect of ammonia on the performance of polymer electrolyte membrane fuel cells [J].
Halseid, R ;
Vie, PJS ;
Tunold, R .
JOURNAL OF POWER SOURCES, 2006, 154 (02) :343-350
[9]   Oxygen reduction on platinum in aqueous sulphuric acid in the presence of ammonium [J].
Halseid, R ;
Bystron, T ;
Tunold, R .
ELECTROCHIMICA ACTA, 2006, 51 (13) :2737-2742
[10]   Influence of ammonium on conductivity and water content of Nafion 117 membranes [J].
Halseid, R ;
Vie, PJS ;
Tunold, R .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2004, 151 (03) :A381-A388