Surface evolution of a Pt–Pd–Au electrocatalyst for stable oxygen reduction

Jian Li, Hui-Ming Yin, Xi-Bo Li, Eiji Okunishi, Yong-Li Shen, Jia He, Zhen-Kun Tang, Wen-Xin Wang, Emrah Yücelen, Chao Li, Yue Gong, Lin Gu, Shu Miao, Li-Min Liu (), Jun Luo () and Yi Ding ()
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Jian Li: Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, School of Materials Science and Engineering, Tianjin University of Technology
Hui-Ming Yin: Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, School of Materials Science and Engineering, Tianjin University of Technology
Xi-Bo Li: Beijing Computational Science Research Center
Eiji Okunishi: JEOL Ltd.
Yong-Li Shen: Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, School of Materials Science and Engineering, Tianjin University of Technology
Jia He: Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, School of Materials Science and Engineering, Tianjin University of Technology
Zhen-Kun Tang: Beijing Computational Science Research Center
Wen-Xin Wang: Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, School of Materials Science and Engineering, Tianjin University of Technology
Emrah Yücelen: NanoPort Europe, FEI Company BV
Chao Li: Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, School of Materials Science and Engineering, Tianjin University of Technology
Yue Gong: Institute of Physics, Chinese Academy of Sciences
Lin Gu: Institute of Physics, Chinese Academy of Sciences
Shu Miao: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Li-Min Liu: Beijing Computational Science Research Center
Jun Luo: Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, School of Materials Science and Engineering, Tianjin University of Technology
Yi Ding: Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, School of Materials Science and Engineering, Tianjin University of Technology

Nature Energy, 2017, vol. 2, issue 8, 1-9

Abstract: Abstract Core–shell nanocatalysts have demonstrated potential as highly active low-Pt fuel cell cathodes for the oxygen reduction reaction (ORR); however, challenges remain in optimizing their surface and interfacial structures, which often exhibit undesirable structural degradation and poor durability. Here, we construct an unsupported nanoporous catalyst with a Pt–Pd shell of sub-nanometre thickness on Au, which demonstrates an initial ORR activity of 1.140 A mgPt−1 at 0.9 V. The activity increases to 1.471 A mgPt−1 after 30,000 potential cycles and is stable over a further 70,000 cycles. Using aberration-corrected scanning transmission electron microscopy and atomically resolved elemental mapping, the origin of the activity change is revealed to be an atomic-scale evolution of the shell from an initial Pt–Pd alloy into a bilayer structure with a Pt-rich trimetallic surface, and finally into a uniform and stable Pt–Pd–Au alloy. This Pt–Pd–Au alloy possesses a suitable configuration for ORR, giving a relatively low free energy change for the final water formation from adsorbed OH intermediate during the reaction.

Date: 2017
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DOI: 10.1038/nenergy.2017.111

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