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

Wencong Zhang, Fan Li, Yi Li, Anran Song, Kun Yang, Dongchang Wu, Wen Shang, Zhenpeng Yao (), Wenpei Gao (), Tao Deng and Jianbo Wu ()
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Wencong Zhang: Shanghai Jiao Tong University
Fan Li: Shanghai Jiao Tong University
Yi Li: Shanghai Jiao Tong University
Anran Song: Shanghai Jiao Tong University
Kun Yang: Shanghai Jiao Tong University
Dongchang Wu: Thermo Fisher Scientific
Wen Shang: Shanghai Jiao Tong University
Zhenpeng Yao: Shanghai Jiao Tong University
Wenpei Gao: Shanghai Jiao Tong University
Tao Deng: Shanghai Jiao Tong University
Jianbo Wu: Shanghai Jiao Tong University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-54104-5

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