Octahedral gold-silver nanoframes with rich crystalline defects for efficient methanol oxidation manifesting a CO-promoting effect

Likun Xiong, Zhongti Sun, Xiang Zhang, Liang Zhao, Peng Huang, Xiwen Chen, Huidong Jin, Hao Sun, Yuebin Lian, Zhao Deng (), Mark H. Rümmerli, Wanjian Yin (), Duo Zhang, Shuao Wang and Yang Peng ()
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Likun Xiong: Soochow University
Zhongti Sun: Soochow University
Xiang Zhang: Soochow University
Liang Zhao: Soochow University
Peng Huang: Soochow University
Xiwen Chen: Soochow University
Huidong Jin: Soochow University
Hao Sun: Soochow University
Yuebin Lian: Soochow University
Zhao Deng: Soochow University
Mark H. Rümmerli: Soochow University
Wanjian Yin: Soochow University
Duo Zhang: Soochow University
Shuao Wang: Soochow University
Yang Peng: Soochow University

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract Three-dimensional bimetallic nanoframes with high spatial diffusivity and surface heterogeneity possess remarkable catalytic activities owing to their highly exposed active surfaces and tunable electronic structure. Here we report a general one-pot strategy to prepare ultrathin octahedral Au3Ag nanoframes, with the formation mechanism explicitly elucidated through well-monitored temporal nanostructure evolution. Rich crystalline defects lead to lowered atomic coordination and varied electronic states of the metal atoms as evidenced by extensive structural characterizations. When used for electrocatalytic methanol oxidation, the Au3Ag nanoframes demonstrate superior performance with a high specific activity of 3.38 mA cm−2, 3.9 times that of the commercial Pt/C. More intriguingly, the kinetics of methanol oxidation on the Au3Ag nanoframes is counter-intuitively promoted by carbon monoxide. The enhancement is ascribed to the altered reaction pathway and enhanced OH− co-adsorption on the defect-rich surfaces, which can be well understood from the d-band model and comprehensive density functional theory simulations.

Date: 2019
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DOI: 10.1038/s41467-019-11766-w

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