Isothermal solidification for high-entropy alloy synthesis

Qiubo Zhang, Max C. Gallant, Yi Chen, Zhigang Song, Yang Liu, Qi Zheng, Linfeng Chen, Karen. C. Bustillo, Yu Huang, Kristin A. Persson and Haimei Zheng ()
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Qiubo Zhang: Lawrence Berkeley National Laboratory
Max C. Gallant: Lawrence Berkeley National Laboratory
Yi Chen: Lawrence Berkeley National Laboratory
Zhigang Song: Lawrence Berkeley National Laboratory
Yang Liu: University of California, Los Angeles
Qi Zheng: Lawrence Berkeley National Laboratory
Linfeng Chen: Lawrence Berkeley National Laboratory
Karen. C. Bustillo: Lawrence Berkeley National Laboratory
Yu Huang: University of California, Los Angeles
Kristin A. Persson: Lawrence Berkeley National Laboratory
Haimei Zheng: Lawrence Berkeley National Laboratory

Nature, 2025, vol. 646, issue 8084, 323-330

Abstract: Abstract Kinetically trapping the high-temperature states through rapid cooling solidification is widely used for the synthesis of high-entropy alloys (HEAs), especially those with intrinsically immiscible elemental combinations1–4. However, strategies need to be developed to overcome the fundamental limitations of rapid cooling solidification in controlling the crystallinity, structure and morphology of HEAs. Here we introduce an isothermal solidification strategy for the synthesis of HEAs by rapidly altering the metal alloy composition through liquid–liquid interface reactions at low temperatures, for example, from 25 °C to 80 °C. We use gallium (Ga)-based metal as the sacrificial reagent and mixing medium. By directing the reactions to the interfaces between the Ga-based liquid metal and an aqueous metal ion solution, the foreign metal ions can be reduced at the interfaces and incorporated into the liquid metal quickly. HEAs with various crystallinity (single crystal, mesocrystal, polycrystal and amorphous), morphology (zero, two and three dimensions) and compositions can be achieved through the isothermal solidification. Ga can be completely consumed, resulting in Ga-free HEAs. If desired, Ga can be one of the metal elements in the final products. In situ liquid phase transmission electron microscopy (TEM) studies and theoretical analysis show the isothermal solidification mechanisms. Our direct observations show the enhanced mixing of liquid metal elements and the solidification process with fluctuating nucleation dynamics. The isothermal solidification marks a powerful strategy for HEA synthesis through an unexplored pathway of kinetically trapping the high-entropy states.

Date: 2025
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DOI: 10.1038/s41586-025-09530-w

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