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Research Article | Open Access

Architecting high-entropy yolk–shell chalcogenide nanoarchitectures toward high-performance energy storage

Yana Luo1,§Chunyan Zhang2,§Mengfei Su2Feifan Zhen2Shengfa Li2Chen Wang2Feng Gao1 ( )Qingyi Lu2 ( )
Jiangsu Key Laboratory of Artificial Functional Materials, Collaborative Innovation Center of Advanced Microstructures, Department of Materials Science and Engineering, College of Engineering and Applied Sciences, Nanjing University, Nanjing 210023, China
State Key Laboratory of Coordination Chemistry, Coordination Chemistry Institute, Collaborative Innovation Center of Advanced Microstructures, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China

§ Yana Luo and Chunyan Zhang contributed equally to this work.

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Abstract

High-entropy sulfides/selenides are expected to be promising anode materials for lithium-ion batteries due to their unique advantages, such as improved electrical conductivity, component adjustability and structural stability. However, the complexity of their preparation makes the morphology/structure regulation of the high-entropy sulfides/selenides more challenging, thus hindering their application in energy storage. In this paper, high-entropy sulfides/selenides with a special yolk–shell structure is designed through a high-entropy precursor vulcanization/selenization strategy. The high-entropy precursors with yolk–shell structure are first prepared by a simple low-temperature solvothermal method, which are transformed to yolk–shell structured high-entropy sulfide ((CrMnFeCoNi)S2) and selenide ((CrMnFeCoNi)Se2) by an upstream gas method. Not only do the high-entropy sulfide has a weak short-range order, increasing the ion diffusion channel, but the yolk–shell structure also provides many benefits for lithium-ion batteries, such as enhancing the stability, increasing the ion diffusion rate, and easing the volume expansion. The (CrMnFeCoNi)S2 electrode exhibits impressive high specific capacity and long cycle life (1375.8 mAh·g−1 after 1250 cycles at 1 A·g−1), and excellent rate capability (1310.6 mAh·g−1 at 2 A·g−1). This research opens a new window of opportunity for developing the next generation of high-entropy compound electrodes for lithium-ion batteries.

Graphical Abstract

This study presents yolk–shell structured high-entropy sulfides/selenides ((CrMnFeCoNi)S2/Se2) synthesized via a precursor-driven strategy, where the synergistic combination of entropy-stabilized composition and hierarchical architecture enables exceptional lithium storage performance, achieving ultrahigh capacity retention (1375.8 mAh·g−1 after 1250 cycles) and outstanding rate capability through enhanced ion kinetics and structural resilience. The innovative integration of high-entropy engineering with yolk–shell morphology effectively addresses challenges in conductivity and volume expansion, paving the way for advanced battery electrode design.

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Nano Research
Article number: 94907510

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Cite this article:
Luo Y, Zhang C, Su M, et al. Architecting high-entropy yolk–shell chalcogenide nanoarchitectures toward high-performance energy storage. Nano Research, 2025, 18(6): 94907510. https://doi.org/10.26599/NR.2025.94907510
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Received: 08 March 2025
Revised: 21 April 2025
Accepted: 24 April 2025
Published: 01 June 2025
© The Author(s) 2025. Published by Tsinghua University Press.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).