Highly Stable Pt/Ordered Graphitic Mesoporous Carbon Electrocatalysts for Oxygen Reduction

被引:89
作者
Gupta, Gaurav [1 ]
Slanac, Daniel A. [1 ]
Kumar, Pavan [1 ]
Wiggins-Camacho, Jaclyn D. [1 ]
Kim, Jeongnam [2 ]
Ryoo, Ryong [2 ]
Stevenson, Keith J. [1 ]
Johnston, Keith P. [1 ]
机构
[1] Univ Texas Austin, Austin, TX 78712 USA
[2] Korea Adv Inst Sci & Technol, Taejon 305701, South Korea
基金
美国国家科学基金会;
关键词
MEMBRANE FUEL-CELLS; PT/C CATALYTIC CATHODE; PLATINUM NANOPARTICLES; DURABILITY ENHANCEMENT; SURFACE MODIFICATION; SUPPORT MATERIAL; SILICA; NANOCRYSTALS; PERFORMANCE; NANOTUBES;
D O I
10.1021/jp907015j
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
In this manuscript, we have synthesized a stable fuel cell catalyst composed of presynthesized Pt nanocrystals (<4 nm) on graphitic mesoporous carbon. The catalyst shows negligible loss in mass activity and active surface area after an accelerated durability test (1000 cycles, 0.5-1.2 V), whereas the commercial Pt on amorphous carbon loses similar to 70% in activity and area. Strong Pt graphite interactions, resulting from metal/support orbital overlap (pi-backbonding) coupled with partial charge transfer, as shown by XPS, and a low coverage of weakly bound ligands on the Pt surface facilitated high dispersion and loadings up to 20 wt %. The high oxidation resistance of the graphitized carbon, along with the strong Pt-C interactions, helped to maintain electrical contact between the metal and carbon while mitigating Pt dissolution, ripening, and coalescence. The ability to disperse well-defined metal nanoparticles onto graphitic mesoporous carbon offers the potential for creating highly stable and active catalysts.
引用
收藏
页码:10796 / 10805
页数:10
相关论文
共 55 条
[1]   Formation, microstructural characteristics and stability of carbon supported platinum catalysts for low temperature fuel cells [J].
Antolini, E .
JOURNAL OF MATERIALS SCIENCE, 2003, 38 (14) :2995-3005
[2]   Physical and morphological characteristics and electrochemical behaviour in PEM fuel cells of PtRu/C catalysts [J].
Antolini, E ;
Giorgi, L ;
Cardellini, F ;
Passalacqua, E .
JOURNAL OF SOLID STATE ELECTROCHEMISTRY, 2001, 5 (02) :131-140
[3]   Thermal stability in air of Pt/C catalysts and PEM fuel cell catalyst layers [J].
Baturina, OA ;
Aubuchon, SR ;
Wynne, KJ .
CHEMISTRY OF MATERIALS, 2006, 18 (06) :1498-1504
[4]  
Chen Z., 2007, ECS T, V11, P1289, DOI [10.1149/1.2781042, DOI 10.1149/1.2781042]
[5]   Platinum nanoclusters studded in the microporous nanowalls of ordered mesoporous carbon [J].
Choi, WC ;
Woo, SI ;
Jeon, MK ;
Sohn, JM ;
Kim, MR ;
Jeon, HJ .
ADVANCED MATERIALS, 2005, 17 (04) :446-+
[6]   HEAT-TREATED CARBON-BLACKS AS SUPPORTS FOR PLATINUM CATALYSTS [J].
COLOMA, F ;
SEPULVEDAESCRIBANO, A ;
RODRIGUEZREINOSO, F .
JOURNAL OF CATALYSIS, 1995, 154 (02) :299-305
[7]   Structural and electronic properties of Ptn (n=3, 7, 13) clusters on metallic single wall carbon nanotube [J].
Cuong, Nguyen Thanh ;
Chi, Dam Hieu ;
Kim, Yong-Tae ;
Mitani, Tadaoki .
PHYSICA STATUS SOLIDI B-BASIC SOLID STATE PHYSICS, 2006, 243 (13) :3472-3475
[8]   Surface chemistry of ordered mesoporous carbons [J].
Darmstadt, H ;
Roy, C ;
Kaliaguine, S ;
Choi, SJ ;
Ryoo, R .
CARBON, 2002, 40 (14) :2673-2683
[9]   Platinum and platinum-ruthenium nanoparticles supported on ordered mesoporous carbon and their electrocatalytic performance for fuel cell reactions [J].
Ding, J ;
Chan, KY ;
Ren, JW ;
Xiao, FS .
ELECTROCHIMICA ACTA, 2005, 50 (15) :3131-3141
[10]   Surface modification of small platinum nanoclusters with alkylamine and alkylthiol: An XPS study on the influence of organic ligands on the Pt 4f binding energies of small platinum nanoclusters [J].
Fu, XY ;
Wang, Y ;
Wu, NZ ;
Gui, LL ;
Tang, YQ .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2001, 243 (02) :326-330