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The role of surface substitution in the atomic disorder-to-order phase transition in multi-component core–shell structures

Author

Listed:
  • Wencong Zhang

    (Shanghai Jiao Tong University
    Shanghai Jiao Tong University)

  • Fan Li

    (Shanghai Jiao Tong University)

  • Yi Li

    (Shanghai Jiao Tong University
    Shanghai Jiao Tong University)

  • Anran Song

    (Shanghai Jiao Tong University
    Shanghai Jiao Tong University)

  • Kun Yang

    (Shanghai Jiao Tong University
    Shanghai Jiao Tong University)

  • Dongchang Wu

    (Thermo Fisher Scientific)

  • Wen Shang

    (Shanghai Jiao Tong University)

  • Zhenpeng Yao

    (Shanghai Jiao Tong University
    Shanghai Jiao Tong University
    Shanghai Jiao Tong University)

  • Wenpei Gao

    (Shanghai Jiao Tong University
    Shanghai Jiao Tong University
    Shanghai Jiao Tong University)

  • Tao Deng

    (Shanghai Jiao Tong University)

  • Jianbo Wu

    (Shanghai Jiao Tong University
    Shanghai Jiao Tong University
    Shanghai Jiao Tong University)

Abstract

Intermetallic phases with atomic ordering are highly active and stable in catalysts. However, understanding the atomistic mechanisms of disorder-to-order phase transition, particularly in multi-component systems, remains challenging. Here, we investigate the atom diffusion and phase transition within Pd@Pt-Co cubic nanoparticles during annealing, using in-situ electron microscopy and ex-situ atomic resolution element analysis. We reveal that initial outward diffusing Pd partially substitutes Pt, forming a (Pt, Pd)-Co ternary system in the surface region, enabling the phase transition at a low temperature of 400 °C, followed by shape-preserved inward propagation of the ordered phase. At higher temperatures, excessive interdiffusion across the interface changes the stoichiometric ratio, diminishing the atomic ordering, leading to obvious change in morphology. Calculations indicate that the Pd-substitute in (Pt, Pd)-Co system leads to a significantly lower phase transition temperature compared to that of Pt-Co alloy and thus a lower activation energy for atomic diffusion. These insights into atomistic behavior are crucial for future design of multi-component systems.

Suggested Citation

  • Wencong Zhang & Fan Li & Yi Li & Anran Song & Kun Yang & Dongchang Wu & Wen Shang & Zhenpeng Yao & Wenpei Gao & Tao Deng & Jianbo Wu, 2024. "The role of surface substitution in the atomic disorder-to-order phase transition in multi-component core–shell structures," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54104-5
    DOI: 10.1038/s41467-024-54104-5
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    References listed on IDEAS

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    1. Hao Shan & Wenpei Gao & Yalin Xiong & Fenglei Shi & Yucong Yan & Yanling Ma & Wen Shang & Peng Tao & Chengyi Song & Tao Deng & Hui Zhang & Deren Yang & Xiaoqing Pan & Jianbo Wu, 2018. "Nanoscale kinetics of asymmetrical corrosion in core-shell nanoparticles," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    2. Tian-Wei Song & Cong Xu & Zhu-Tao Sheng & Hui-Kun Yan & Lei Tong & Jun Liu & Wei-Jie Zeng & Lu-Jie Zuo & Peng Yin & Ming Zuo & Sheng-Qi Chu & Ping Chen & Hai-Wei Liang, 2022. "Small molecule-assisted synthesis of carbon supported platinum intermetallic fuel cell catalysts," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Sheng Dai & Yuan You & Shuyi Zhang & Wei Cai & Mingjie Xu & Lin Xie & Ruqian Wu & George W. Graham & Xiaoqing Pan, 2017. "In situ atomic-scale observation of oxygen-driven core-shell formation in Pt3Co nanoparticles," Nature Communications, Nature, vol. 8(1), pages 1-8, December.
    4. Wei-Jie Zeng & Chang Wang & Qiang-Qiang Yan & Peng Yin & Lei Tong & Hai-Wei Liang, 2022. "Phase diagrams guide synthesis of highly ordered intermetallic electrocatalysts: separating alloying and ordering stages," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    5. Miaofang Chi & Chao Wang & Yinkai Lei & Guofeng Wang & Dongguo Li & Karren L. More & Andrew Lupini & Lawrence F. Allard & Nenad M. Markovic & Vojislav R. Stamenkovic, 2015. "Surface faceting and elemental diffusion behaviour at atomic scale for alloy nanoparticles during in situ annealing," Nature Communications, Nature, vol. 6(1), pages 1-9, December.
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