Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction

Xue Wang, Sang-Il Choi, Luke T. Roling, Ming Luo, Cheng Ma, Lei Zhang, Miaofang Chi, Jingyue Liu, Zhaoxiong Xie, Jeffrey A. Herron, Manos Mavrikakis () and Younan Xia ()
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Xue Wang: Georgia Institute of Technology and Emory University
Sang-Il Choi: Georgia Institute of Technology and Emory University
Luke T. Roling: University of Wisconsin-Madison
Ming Luo: Georgia Institute of Technology and Emory University
Cheng Ma: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Lei Zhang: Georgia Institute of Technology and Emory University
Miaofang Chi: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Jingyue Liu: Arizona State University
Zhaoxiong Xie: State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, Xiamen University
Jeffrey A. Herron: University of Wisconsin-Madison
Manos Mavrikakis: University of Wisconsin-Madison
Younan Xia: Georgia Institute of Technology and Emory University

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: Abstract Conformal deposition of platinum as ultrathin shells on facet-controlled palladium nanocrystals offers a great opportunity to enhance the catalytic performance while reducing its loading. Here we report such a system based on palladium icosahedra. Owing to lateral confinement imposed by twin boundaries and thus vertical relaxation only, the platinum overlayers evolve into a corrugated structure under compressive strain. For the core-shell nanocrystals with an average of 2.7 platinum overlayers, their specific and platinum mass activities towards oxygen reduction are enhanced by eight- and sevenfold, respectively, relative to a commercial catalyst. Density functional theory calculations indicate that the enhancement can be attributed to the weakened binding of hydroxyl to the compressed platinum surface supported on palladium. After 10,000 testing cycles, the mass activity of the core-shell nanocrystals is still four times higher than the commercial catalyst. These results demonstrate an effective approach to the development of electrocatalysts with greatly enhanced activity and durability.

Date: 2015
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DOI: 10.1038/ncomms8594

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