Fe loading of a carbon-supported Fe-N electrocatalyst and its effect on the oxygen reduction reaction

被引:61
作者
Zhang, Lei [1 ]
Lee, Kunchan [1 ]
Bezerra, Cicero W. B. [2 ]
Zhang, Jianlu [1 ]
Zhang, Jiujun [1 ]
机构
[1] Natl Res Council Canada, Inst Fuel Cell Innovat, Vancouver, BC V6T 1W5, Canada
[2] Univ Fed Maranhao, Dept Chem, BR-65080040 Sao Luis, MA, Brazil
关键词
Electrocatalyst; Oxygen reduction reaction (ORR); Iron (Fe)-nitrogen (N); 2,4,6-Tris(2-pyridyl)-1,3,5-triazine (TPTZ); Proton exchange membrane (PEM) fuel cell; ELECTROLYTE FUEL-CELLS; ACTIVE-SITES; CATALYSTS; IRON; PYROLYSIS; TEMPERATURE; SURFACE; O-2;
D O I
10.1016/j.electacta.2009.06.049
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
Carbon-supported non-noble metal catalysts with Fe as the metal and tripyridyl triazine (TPTZ) as the ligand (Fe-TPTZ/C) were synthesized using a simple chemical method. How the Fe loading in this Fe-TPTZ/C catalyst affected the ORR activity was investigated using several Fe loadings: 0.2, 0.4, 0.7, 2.7, 4.7, 5.8 and 7.8 wt%. The as-prepared catalysts were then heat-treated at 800 degrees C in an N-2 environment to obtain catalysts of Fe-N/C. Energy dispersive X-ray spectroscopy (EDX) was used to identify the Fe-N/C catalysts. These Fe-N/C catalysts showed significant ORR activity improvement over the as-prepared Fe-TPTZ/C catalysts. The kinetics of the ORR catalyzed by the catalysts with different Fe loadings was studied using the rotating disk electrode technique. It was observed that a 4.7 wt% Fe loading yielded the best catalytic ORR activity. Regarding the overall ORR electron transfer number, it was found that as the catalyst's Fe loading increased, the overall ORR electron transfer number changed from 2.9 to 3.9, suggesting that increasing the Fe loading could alter the ORR mechanism from a 2-electron to a 4-electron transfer dominated process. The Tafel method was also used to obtain one important kinetic parameter: the exchange current density. A fuel cell was assembled using a membrane electrode assembly with 4.7 wt% Fe loaded Fe-N/C as the cathode catalyst, and the cell was tested for both performance and durability, yielding a 1000-h lifetime. Crown Copyright (C) 2009 Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:6631 / 6636
页数:6
相关论文
共 15 条
[1]  
Bard A.J., 1980, ELECTROCHEMICAL METH
[2]   A class of non-precious metal composite catalysts for fuel cells [J].
Bashyam, Rajesh ;
Zelenay, Piotr .
NATURE, 2006, 443 (7107) :63-66
[3]   Novel carbon-supported Fe-N electrocatalysts synthesized through heat treatment of iron tripyridyl triazine complexes for the PEM fuel cell oxygen reduction reaction [J].
Bezerra, Cicero W. B. ;
Zhang, Lei ;
Lee, Kunchan ;
Liu, Hansan ;
Zhang, Jianlu ;
Shi, Zheng ;
Marques, Aldalea L. B. ;
Marques, Edmar P. ;
Wu, Shaohong ;
Zhang, Jiujun .
ELECTROCHIMICA ACTA, 2008, 53 (26) :7703-7710
[4]  
Dodelet J.-P., 2006, N4-Macrocyclic Metal Complexes. Ch 3: Oxygen Reduction in PEM Fuel Cell Conditions: Heat-Treated Non-Precious Metal-N4 Macrocycles and Beyond
[5]   Oxygen reduction catalysts for polymer electrolyte fuel cells from the pyrolysis of FeII acetate adsorbed 3,4,9,10-perylenetetracarboxylic dianhydride [J].
Faubert, G ;
Côté, R ;
Dodelet, JP ;
Lefèvre, M ;
Bertrand, P .
ELECTROCHIMICA ACTA, 1999, 44 (15) :2589-2603
[6]   Heat-treated Fe/N/C catalysts for O2 electroreduction:: Are active sites hosted in micropores? [J].
Jaouen, F ;
Lefèvre, M ;
Dodelet, JP ;
Cai, M .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (11) :5553-5558
[7]   IrxCo1-x (x=0.3-1.0) alloy electrocatalysts, catalytic activities, and methanol tolerance in oxygen reduction reaction [J].
Lee, Kunchan ;
Zhang, Lei ;
Zhang, Jiujun .
JOURNAL OF POWER SOURCES, 2007, 170 (02) :291-296
[8]   Molecular oxygen reduction in PEM fuel cells:: Evidence for the simultaneous presence of two active sites in Fe-based catalysts [J].
Lefèvre, M ;
Dodelet, JP ;
Bertrand, P .
JOURNAL OF PHYSICAL CHEMISTRY B, 2002, 106 (34) :8705-8713
[9]   Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells [J].
Lefevre, Michel ;
Proietti, Eric ;
Jaouen, Frederic ;
Dodelet, Jean-Pol .
SCIENCE, 2009, 324 (5923) :71-74
[10]   High-surface-area CoTMPP/C synthesized by ultrasonic spray pyrolysis for PEM fuel cell electrocatalysts [J].
Liu, Hansan ;
Song, Chaojie ;
Tang, Yuanhua ;
Zhang, Jianlu ;
Zhang, Jiujun .
ELECTROCHIMICA ACTA, 2007, 52 (13) :4532-4538