Nitrogen-modified carbon-based catalysts for oxygen reduction reaction in polymer electrolyte membrane fuel cells

被引:395
作者
Subramanian, Nalini P. [1 ]
Li, Xuguang [1 ]
Nallathambi, Vijayadurda [1 ]
Kumaraguru, Swaminatha P. [1 ]
Colon-Mercado, Hector [1 ]
Wu, Gang [1 ]
Lee, Jong-Won [1 ]
Popov, Branko N. [1 ]
机构
[1] Univ S Carolina, Dept Chem Engn, Ctr Electrochem Engn, Columbia, SC 29208 USA
关键词
Carbon-based catalyst; Nitrogen modification; Oxygen reduction; PEM fuel cell; FE-BASED CATALYSTS; CO-BASED CATALYSTS; HIGH-AREA CARBON; FUNCTIONAL-GROUPS; O-2; REDUCTION; ELECTROCATALYSTS; ADSORPTION; CHLORIDE; PHASE; BLACK;
D O I
10.1016/j.jpowsour.2008.11.087
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
Nitrogen-modified carbon-based catalysts for oxygen reduction were synthesized by modifying carbon black with nitrogen-containing organic precursors. The electrocatalytic properties of catalysts were studied as a function of surface pre-treatments, nitrogen and oxygen concentrations, and heat-treatment temperatures. On the optimum catalyst, the onset potential for oxygen reduction is approximately 0.76V (NHE) and the amount of hydrogen peroxide produced at 0.5V (NHE) is approximately 3% under our experimental conditions. The characterization studies indicated that pyridinic and graphitic (quaternary) nitrogens may act as active sites of catalysts for oxygen reduction reaction. In particular, pyridinic nitrogen, which possesses one lone pair of electrons in addition to the one electron donated to the conjugated pi bond, facilitates the reductive oxygen adsorption. (C) 2008 Elsevier B.V. All rights reserved.
引用
收藏
页码:38 / 44
页数:7
相关论文
共 52 条
[1]  
Adzic R, 1998, FRONT ELECT, P197
[2]   ELECTROCATALYSIS OF OXYGEN REDUCTION PROCESS ON METAL-CHELATES IN ACID ELECTROLYTE [J].
BAGOTZKY, VS ;
TARASEVICH, MR ;
RADYUSHKINA, KA ;
LEVINA, OA ;
ANDRUSYOVA, SI .
JOURNAL OF POWER SOURCES, 1978, 2 (03) :233-240
[3]   A class of non-precious metal composite catalysts for fuel cells [J].
Bashyam, Rajesh ;
Zelenay, Piotr .
NATURE, 2006, 443 (7107) :63-66
[4]   SOME ASPECTS OF THE SURFACE-CHEMISTRY OF CARBON-BLACKS AND OTHER CARBONS [J].
BOEHM, HP .
CARBON, 1994, 32 (05) :759-769
[5]   Origin of the large N is binding energy in X-ray photoelectron spectra of calcined carbonaceous materials [J].
Casanovas, J ;
Ricart, JM ;
Rubio, J ;
Illas, F ;
JimenezMateos, JM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (34) :8071-8076
[6]   Acid/base-treated activated carbons: Characterization of functional groups and metal adsorptive properties [J].
Chen, JP ;
Wu, SN .
LANGMUIR, 2004, 20 (06) :2233-2242
[7]   Influence of nitrogen-containing precursors on the electrocatalytic activity of heat-treated Fe(OH)2 on carbon black for O2 reduction [J].
Cote, R ;
Lalande, G ;
Guay, D ;
Dodelet, JP ;
Denes, G .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1998, 145 (07) :2411-2418
[8]  
EASTON EB, 2006, ECS T, V3, P241
[9]   Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs [J].
Gasteiger, HA ;
Kocha, SS ;
Sompalli, B ;
Wagner, FT .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 56 (1-2) :9-35
[10]   Heat-treated iron(III) tetramethoxyphenyl porphyrin chloride supported on high-area carbon as an electrocatalyst for oxygen reduction: Part III. Detection of hydrogen-peroxide during oxygen reduction [J].
Gojkovic, SL ;
Gupta, S ;
Savinell, RF .
ELECTROCHIMICA ACTA, 1999, 45 (06) :889-897