Platinum-monolayer electrocatalysts Palladium interlayer on IrCo alloy core improves activity in oxygen-reduction reaction

被引:41
作者
Gong, Kuanping [1 ]
Chen, Wei-Fu [1 ]
Sasaki, Kotaro [1 ]
Su, Dong [1 ]
Vukmirovic, Miomir B. [1 ]
Zhou, Weiping [1 ]
Izzo, Elise L. [2 ]
Perez-Acosta, Carmen [2 ]
Hirunsit, Pussana [3 ]
Balbuena, Perla B. [3 ]
Adzic, Radoslav R. [1 ]
机构
[1] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
[2] UTC Power Corp, S Windsor, CT USA
[3] Texas A&M Univ, Dept Chem Engn, College Stn, TX 77843 USA
关键词
Electrocatalysts; Iridium; Platinum; Palladium; Oxygen reduction; INITIO MOLECULAR-DYNAMICS; TRANSITION; IRIDIUM; METALS;
D O I
10.1016/j.jelechem.2010.04.011
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
We describe the synthesis and electrocatalytic properties of a new low-Pt electrocatalyst consisting of an IrCo core a Pd interlayer and a surface Pt monolayer emphasizing the interlayer s role in improving electrocatalytic activity for the oxygen reduction reaction on Pt in HClO4 solution We prepared the IrCo alloys by decomposing at 800 C hexacyanometalate KCoIr(cN)(6) adsorbed on the carbon surfaces The synthesis of Ir3Co/C involved heating a mix of metal salts and carbon in hydrogen at 500 degrees C Thereafter we placed a palladium and/or platinum monolayer on them via the galvanic displacement of an underpotentially deposited copper monolayer The electrocatalysts were characterized using structural- and electrochemical techniques For Pt-ML/Pd-ML/IrCo/C we observed a Pt mass activity of 1 18 A/mg((Pt)) and the platinum group-metals mass of 0 16 A/mg((Pt Pd Ir)) In comparison without a Pd interlayer le Pt-ML/IrCo/C the activities of 0 15 A/mg(pt) and 0 036 A/mg((Pt Pd Ir)) were considerably lower We consider that the palladium interlayer plays an essential role in achieving high catalytic activity by adjusting the electronic interaction of the platinum monolayer with the IrCo core so that it accelerates the kinetics of adsorption and desorption of the intermediates of oxygen reduction A similar trend was observed for Pt-ML/Pd-ML, and Pt-ML deposited on Ir3Co/C alloy core We used density functional theory to interpret the observed phenomena (C) 2010 Elsevier B V All rights reserved
引用
收藏
页码:232 / 237
页数:6
相关论文
共 30 条
[1]   Platinum monolayer fuel cell electrocatalysts [J].
Adzic, R. R. ;
Zhang, J. ;
Sasaki, K. ;
Vukmirovic, M. B. ;
Shao, M. ;
Wang, J. X. ;
Nilekar, A. U. ;
Mavrikakis, M. ;
Valerio, J. A. ;
Uribe, F. .
TOPICS IN CATALYSIS, 2007, 46 (3-4) :249-262
[2]   Formation of carbon supported PtRu alloys: an XRD analysis [J].
Antolini, E ;
Cardellini, F .
JOURNAL OF ALLOYS AND COMPOUNDS, 2001, 315 (1-2) :118-122
[3]  
Azaroff L.V., 1974, X-ray diffraction
[4]   Pd-Ti and Pd-Co-Au electrocatalysts as a replacement for platinum for oxygen reduction in proton exchange membrane fuel cells [J].
Fernández, JL ;
Raghuveer, V ;
Manthiram, A ;
Bard, AJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (38) :13100-13101
[5]   Polymer-assisted synthesis of manganese dioxide/carbon nanotube nanocomposite with excellent electrocatalytic activity toward reduction of oxygen [J].
Gong, Kuanping ;
Yu, Ping ;
Su, Lei ;
Xiong, Shaoxiang ;
Mao, Lanqun .
JOURNAL OF PHYSICAL CHEMISTRY C, 2007, 111 (05) :1882-1887
[6]   Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction [J].
Gong, Kuanping ;
Du, Feng ;
Xia, Zhenhai ;
Durstock, Michael ;
Dai, Liming .
SCIENCE, 2009, 323 (5915) :760-764
[7]  
Greeley J, 2009, NAT CHEM, V1, P552, DOI [10.1038/nchem.367, 10.1038/NCHEM.367]
[8]   Regular alumina-supported nanoparticles of iridium, rhodium and platinum under hydrogen reduction: structure, morphology and activity in the neopentane conversion [J].
Hayek, K ;
Goller, H ;
Penner, S ;
Rupprechter, G ;
Zimmermann, C .
CATALYSIS LETTERS, 2004, 92 (1-2) :1-9
[9]   IMAGE-CONTRAST AND LOCALIZED SIGNAL SELECTION TECHNIQUES [J].
HOWIE, A .
JOURNAL OF MICROSCOPY-OXFORD, 1979, 117 (SEP) :11-23
[10]  
IGLESIAS FJV, 2007, J POWER SOURCES, V171, P448