Maximizing the Catalytic Performance of Pd@Aux Pd1-x Nanocubes in H2 O2 Production by Reducing Shell Thickness to Increase Compositional Stability

Yu Zhang; Zhiheng Lyu; Zitao Chen; Shangqian Zhu; Yifeng Shi; Ruhui Chen; Minghao Xie; Yao Yao; Miaofang Chi; Minhua Shao; Younan Xia

doi:10.1002/anie.202105137

Maximizing the Catalytic Performance of Pd@Au_x Pd_1-x Nanocubes in H₂ O₂ Production by Reducing Shell Thickness to Increase Compositional Stability

Angew Chem Int Ed Engl. 2021 Sep 1;60(36):19643-19647. doi: 10.1002/anie.202105137. Epub 2021 Jul 26.

Authors

Yu Zhang^{1

2}, Zhiheng Lyu³, Zitao Chen¹, Shangqian Zhu², Yifeng Shi³, Ruhui Chen³, Minghao Xie³, Yao Yao², Miaofang Chi⁴, Minhua Shao^{2

5}, Younan Xia^{1

3}

Affiliations

¹ The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, GA, 30332, USA.
² Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.
³ School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
⁴ Center for Nanophase Materials Science, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
⁵ Energy Institute, Hong Kong Branch of the Southern Marine Science and Engineering, Guangdong Laboratory, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.

PMID: 34128305
DOI: 10.1002/anie.202105137

Abstract

We report a simple route based upon seed-mediated growth to the synthesis of Pd@Au_x Pd_1-x (0.8≤x≤1) core-shell nanocubes. Benefiting from the well-defined {100} facets and an optimal Au/Pd ratio for the surface, the nanocubes bearing a shell made of Au_0.95 Pd_0.05 work as an efficient electrocatalyst toward H₂ O₂ production, with high selectivity of 93-100 % in the low-overpotential region of 0.4-0.7 V. When the Au_0.95 Pd_0.05 alloy is confined to a shell of only three atomic layers in thickness, the electrocatalyst is able to maintain its surface structure and elemental composition, endowing continuous and stable production of H₂ O₂ during oxygen reduction at a high rate of 1.62 mol g_(Pd+Au) ^-1 h^-1 . This work demonstrates a versatile route to the rational development of active and durable electrocatalysts based upon alloy nanocrystals.

Keywords: alloys; electrocatalysts; noble metals; shell; surface stability.

Abstract

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