Enhanced Electrocatalytic Performance of Processed, Ultrathin, Supported Pd-Pt Core-Shell Nanowire Catalysts for the Oxygen Reduction Reaction

被引:422
作者
Koenigsmann, Christopher [1 ]
Santulli, Alexander C. [1 ]
Gong, Kuanping [2 ]
Vukmirovic, Miomir B. [2 ]
Zhou, Wei-ping [2 ]
Sutter, Eli [3 ]
Wong, Stanislaus S. [1 ,4 ]
Adzic, Radoslav R. [2 ]
机构
[1] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA
[2] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
[3] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA
[4] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA
关键词
PLATINUM-MONOLAYER ELECTROCATALYSTS; O-2; REDUCTION; DURABILITY ENHANCEMENT; NANOPARTICLES; CARBON; METAL; STABILITY; NANOTUBES; PALLADIUM; SURFACES;
D O I
10.1021/ja111130t
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We report on the synthesis, characterization, and electrochemical performance of novel, ultrathin Pt monolayer shell-Pd nanowire core catalysts. Initially, ultrathin Pd nanowires with diameters of 2.0 +/- 0.5 nm were generated, and a method has been developed to achieve highly uniform distributions of these catalysts onto the Vulcan XC-72 carbon support. As-prepared wires are activated by the use of two distinctive treatment protocols followed by selective CO adsorption in order to selectively remove undesirable organic residues. Subsequently, the desired nanowire core-Pt monolayer shell motif was reliably achieved by Cu underpotential deposition followed by galvanic displacement of the Cu adatoms. The surface area and mass activity of the acid and ozone-treated nanowires were assessed, and the ozone-treated nanowires were found to maintain outstanding area and mass specific activities of 0.77 mA/cm(2) and 1.83 A/mg(pt), respectively, which were significantly enhanced as compared with conventional commercial Pt nanoparticles, core-shell nanoparticles, and acid-treated nanowires. The ozone-treated nanowires also maintained excellent electrochemical durability under accelerated half-cell testing, and it was found that the area-specific activity increased by similar to 1.5 fold after a simulated catalyst lifetime.
引用
收藏
页码:9783 / 9795
页数:13
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