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

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Wencong Zhang, Fan Li, Yi Li, Anran Song, Kun Yang, Dongchang Wu, Wen Shang, Zhenpeng Yao, Wenpei Gao, Tao Deng, Jianbo Wu
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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.

Abstract Image

表面置换在多组分核壳结构原子无序到有序相变中的作用
具有原子有序性的金属间相在催化剂中具有高度的活性和稳定性。然而,了解无序到有序相变的原子机制,尤其是多组分系统中的无序到有序相变,仍然具有挑战性。在此,我们利用原位电子显微镜和原位原子分辨率元素分析,研究了退火过程中 Pd@Pt-Co 立方纳米颗粒内部的原子扩散和相变。我们发现,最初向外扩散的钯部分取代了铂,在表面区域形成了(铂、钯)-钴三元体系,从而在 400 ℃ 的低温下实现了相变,随后有序相保持形状向内传播。在较高温度下,界面上过度的相互扩散改变了化学计量比,减弱了原子有序性,导致形态发生明显变化。计算表明,与铂钴合金相比,(铂,钯)钴体系中的钯替代物导致相变温度明显降低,从而降低了原子扩散的活化能。这些关于原子行为的见解对于未来多组分系统的设计至关重要。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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