Cross-Laboratory Experimental Study of Non-Noble-Metal Electrocatalysts for the Oxygen Reduction Reaction

被引:648
作者
Jaouen, Frederic [1 ]
Herranz, Juan [1 ]
Lefevre, Michel [1 ]
Dodelet, Jean-Pol [1 ]
Kramm, Ulrike I. [2 ]
Herrmann, Iris [2 ]
Bogdanoff, Peter [2 ]
Maruyama, Jun [3 ]
Nagaoka, Toru [4 ]
Garsuch, Arnd [5 ]
Dahn, Jeff R. [5 ]
Olson, Tim [6 ]
Pylypenko, Svitlana [6 ]
Atanassov, Plamen [6 ]
Ustinov, Eugene A. [7 ]
机构
[1] Inst Natl Rech Sci Energie Mat & Telecommun, Varennes, PQ J3X 1S2, Canada
[2] Helmholtz Zentrum Berlin GmbH, D-14109 Berlin, Germany
[3] Osaka Municipal Tech Res Inst, Environm Technol Res Div, Joto Ku, Osaka 5368553, Japan
[4] Osaka Municipal Tech Res Inst, Proc Technol Res Div, Joto Ku, Osaka 5368553, Japan
[5] Dalhousie Univ, Dept Phys & Atmospher Sci, Halifax, NS B3H 3J5, Canada
[6] Univ New Mexico, Dept Chem & Nucl Engn, Albuquerque, NM 87131 USA
[7] AF Ioffe Phys Tech Inst, St Petersburg 194021, Russia
基金
俄罗斯基础研究基金会; 加拿大自然科学与工程研究理事会;
关键词
non-platinum group metal; catalyst; oxygen electroreduction; fuel cell; polymer electrolyte; DENSITY-FUNCTIONAL THEORY; FE-BASED ELECTROCATALYSTS; ELECTROLYTE FUEL-CELLS; PORE-SIZE DISTRIBUTION; HEAT-TREATMENT AFFECT; HIGH-AREA CARBON; O-2; REDUCTION; PLATINUM MONOLAYER; TETRAMETHOXYPHENYL PORPHYRIN; NONNOBLE ELECTROCATALYSTS;
D O I
10.1021/am900219g
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Nine non-noble-metal catalysts (NNMCs) from five different laboratories were investigated for the catalysis of O-2 electroreduction in an acidic medium. The catalyst precursors were synthesized by wet impregnation, planetary ball milling, a foaming-agent technique, or a templating method. All catalyst precursors were subjected to one or more heat treatments at 700-1050 degrees C in an inert or reactive atmosphere. These catalysts underwent an identical set of electrochemical characterizations, including rotating-disk-electrode and polymer-electrolyte membrane fuel cell (PEMFC) tests and voltammetry under N-2. Ex situ characterization was comprised of X-ray photoelectron spectroscopy, neutron activation analysis, scanning electron microscopy, and N2 adsorption and its analysis with an advanced model for carbonaceous powders. In PEMFC, several NNMCs display mass activities of 10-20 A g(-1) at 0.8 V versus a reversible hydrogen electrode, and one shows 80 A g(-1). The latter value corresponds to a volumetric activity of 19 A cm(-3) under reference conditions and represents one-seventh of the target defined by the U.S. Department of Energy for 2010 (130 A cm(-3)). The activity of all NNMCs is mainly governed by the microporous surface area, and active sites seem to be hosted in pore sizes of 5-15 angstrom. The nitrogen and metal (iron or cobalt) seem to be present in sufficient amounts in the NNMCs and do not limit activity. The paper discusses probable directions for synthesizing more active NNMCs. This could be achieved through multiple pyrolysis steps, ball-milling steps, and control of the powder morphology by the addition of foaming agents and/or sulfur.
引用
收藏
页码:1623 / 1639
页数:17
相关论文
共 129 条
[91]   A NEW ANALYSIS METHOD FOR THE DETERMINATION OF THE PORE-SIZE DISTRIBUTION OF POROUS CARBONS FROM NITROGEN ADSORPTION MEASUREMENTS [J].
SEATON, NA ;
WALTON, JPRB ;
QUIRKE, N .
CARBON, 1989, 27 (06) :853-861
[92]   Electroreduction of O-2 to H2O at unusually positive potentials catalyzed by the simplest of the cobalt porphyrins [J].
Shi, C ;
Steiger, B ;
Yuasa, M ;
Anson, FC .
INORGANIC CHEMISTRY, 1997, 36 (20) :4294-4295
[93]   In situ TEM studies of metal-carbon reactions [J].
Sinclair, R ;
Itoh, T ;
Chin, R .
MICROSCOPY AND MICROANALYSIS, 2002, 8 (04) :288-304
[94]   Effect of preparation conditions of sol-gel-derived Co-N-C-based catalysts on ORR activity in acidic solutions [J].
Sirk, A. H. C. ;
Campbell, S. A. ;
Birss, V. I. .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2008, 155 (06) :B592-B601
[95]   Temperature dependence of oxygen reduction catalyzed by cobalt fluoro-phthalocyanine adsorbed on a graphite electrode [J].
Song, C. ;
Zhang, L. ;
Zhang, J. ;
Wilkinson, D. P. ;
Baker, R. .
FUEL CELLS, 2007, 7 (01) :9-15
[96]   Comparison of the behavior of several cobalt porphyrins as electrocatalysts for the reduction of O2 at graphite electrodes [J].
Song, EH ;
Shi, CN ;
Anson, FC .
LANGMUIR, 1998, 14 (15) :4315-4321
[97]   Studies on Co-based catalysts supported on modified carbon substrates for PEMFC cathodes [J].
Subramanian, Nalini P. ;
Kumaraguru, Swaminatha P. ;
Colon-Mercado, Hector ;
Kim, Hansung ;
Popov, Branko N. ;
Black, Timothy ;
Chen, Donna A. .
JOURNAL OF POWER SOURCES, 2006, 157 (01) :56-63
[98]  
Sun G.Q., 2001, J APPL ELECTROCHEM, V31, P1025, DOI DOI 10.1023/A:1003413226041
[99]   A methodology for investigating new nonprecious metal catalysts for PEM fuel cells [J].
Susac, D. ;
Sode, A. ;
Zhu, L. ;
Wong, P. C. ;
Teo, M. ;
Bizzotto, D. ;
Mitchell, K. A. R. ;
Parsons, R. R. ;
Campbell, S. A. .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (22) :10762-10770
[100]   PYROPOLYMERS OF N-4 COMPLEXES - STRUCTURE AND ELECTROCATALYTIC PROPERTIES [J].
TARASEVICH, MR ;
RADYUSKINA, KA .
MATERIALS CHEMISTRY AND PHYSICS, 1989, 22 (3-4) :477-502