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
[21]   O2 reduction in PEM fuel cells:: Activity and active site structural information for catalysts obtained by the pyrolysis at high temperature of Fe precursors [J].
Lefèvre, M ;
Dodelet, JP ;
Bertrand, P .
JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (47) :11238-11247
[22]   Development of method for synthesis of Pt-Co cathode catalysts for PEM fuel cells [J].
Li, Xuguang ;
Colon-Mercado, Hector R. ;
Wu, Gang ;
Lee, Jong-Won ;
Popov, Branko N. .
ELECTROCHEMICAL AND SOLID STATE LETTERS, 2007, 10 (11) :B201-B205
[23]   Development of ruthenium-based bimetallic electrocatalysts for oxygen reduction reaction [J].
Liu, Lingyun ;
Lee, Jong-Won ;
Popov, Branko N. .
JOURNAL OF POWER SOURCES, 2006, 162 (02) :1099-1103
[24]   Development of ruthenium-based catalysts for oxygen reduction reaction [J].
Liu, Lingyun ;
Kim, Hansung ;
Lee, Jong-Won ;
Popov, Branko N. .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2007, 154 (02) :A123-A128
[25]   Influence of nitrogen doping on oxygen reduction electrocatalysis at carbon nanofiber electrodes [J].
Maldonado, S ;
Stevenson, KJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (10) :4707-4716
[26]   Electroreduction of oxygen on Co-based catalysts:: determination of the parameters affecting the two-electron transfer reaction in an acid medium [J].
Marcotte, S ;
Villers, D ;
Guillet, N ;
Roué, L ;
Dodelet, JP .
ELECTROCHIMICA ACTA, 2004, 50 (01) :179-188
[27]  
Markovic N.M., 2002, Surface Science Reports, V286, P1
[28]   Electrocatalysts by design: from the tailored surface to a commercial catalyst [J].
Markovic, NM ;
Ross, PN .
ELECTROCHIMICA ACTA, 2000, 45 (25-26) :4101-4115
[29]   Characterization of the iron phase in CNx-based oxygen reduction reaction catalysts [J].
Matter, Paul H. ;
Wang, Eugenia ;
Millet, Jean-Marc M. ;
Ozkan, Umit S. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2007, 111 (03) :1444-1450
[30]   Non-metal catalysts for dioxygen reduction in an acidic electrolyte [J].
Matter, Paul H. ;
Ozkan, Umit S. .
CATALYSIS LETTERS, 2006, 109 (3-4) :115-123