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Shaped Pt-Ni nanocrystals with an ultrathin Pt-enriched shell derived from one-pot hydrothermal synthesis as active electrocatalysts for oxygen reduction

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Abstract

Alloy nanocrystals (NCs) of Pt with 3d transition metals, especially Ni, are excellent catalysts for the oxygen reduction reaction (ORR). In this work, we, for the first time, demonstrated the water phase colloidal synthesis of Pt-M (M = Ni, Co and Fe) alloy NCs with tunable composition and morphology through a facile hydrothermal method. Pt-Ni alloy NCs synthesized with this method presented better ORR activity than commercial Pt/C catalysts. The X-ray energy dispersive spectra (EDS) mapping technique revealed that Pt-enriched shells existed on the as-synthesized Pt-Ni alloy NCs. About two atom thick layered Pt-enriched shells formed on Pt50Ni50 NCs and the thickness of the Pt-enriched shells increased as the Ni content increased. Furthermore, X-ray photoelectron spectroscopy analysis revealed that the oxidation level of the surface Pt atoms on the Pt-Ni alloy NCs decreased compared with monometallic Pt NCs, implying a decrease in the oxophilicity of the surface Pt atoms. Pt-Ni alloy NCs with lower oxophilicity of the surface Pt atoms give higher ORR activity. The most active alloy sample showed 13 times higher specific activity and six times higher mass activity at 0.9 V vs. a reversible hydrogen electrode when compared with commercial Pt/C. Pt-Ni alloy NCs also showed better durability than commercial Pt/C in long term ORR tests.

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Authors and Affiliations

  1. Beijing National Laboratory for Molecular Science, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China

    Jun Gu, Guangxu Lan, Yanshuang Xu, Wei Zhu & Yawen Zhang

  2. State Key Laboratory of Silicon Materials, Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province and School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China

    Yingying Jiang & Chuanhong Jin

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  1. Jun Gu
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  2. Guangxu Lan
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  3. Yingying Jiang
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  4. Yanshuang Xu
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Gu, J., Lan, G., Jiang, Y. et al. Shaped Pt-Ni nanocrystals with an ultrathin Pt-enriched shell derived from one-pot hydrothermal synthesis as active electrocatalysts for oxygen reduction. Nano Res. 8, 1480–1496 (2015). https://doi.org/10.1007/s12274-014-0632-7

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