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Amorphous Sb/C composite with isotropic expansion property as an ultra-stable and high-rate anode for lithium-ion batteries

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Abstract

Antimony (Sb) is an intriguing anode material for Li-ion batteries (LIBs) owing to its high theoretical capacity of 660 mAh·g−1 and appropriate working potential of ~ 0.8 V (vs. Li+/Li). However, just like all alloying materials, the Sb anode suffers from huge volume expansion (230%) during repeated insertion/extraction of Li+ ions, resulting in structural deterioration and rapid capacity decay. In this work, a novel amorphous Sb/C composite with atomically dispersed Sb particles in carbon matrix is prepared via a straightforward high-energy ball milling approach. The intimate intermixing of amorphous Sb with C provides homogeneous element distribution and isotropic volume expansion during cycling, resulting in persistent structural stability. Meanwhile, the disordered structure of amorphous material shortens the diffusion distance of lithium ions/electrons, promoting fast reaction kinetics and rate capability. Benefiting from the aforementioned effects, the amorphous Sb/C exhibits a high reversible capacity of 537.4 mAh·g−1 at 0.1 A·g−1 and retains 201.0 mAh·g−1 at an ultrahigh current rate of 10.0 A·g−1. Even after 1500 deep cycles at 2.0 A·g−1, the amorphous Sb/C electrode still maintains 86.3% of its initial capacity, which outperforms all existing Sb-based anodes reported so far. Post-mortem analysis further reveals a greatly reduced volume variation of merely 34.6% for the amorphous Sb/C electrode, much lower than that of 223.1% for crystalline Sb materials. This study presents a new approach to stabilizing Sb-based alloy anodes and contributes to the construction of high-performance amorphous anode materials for LIBs, enabling advanced energy storage.

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摘要

锑 (Sb) 基负极具有660 mAh·g−1的高理论容量和约0.8 V (相对于Li+/Li) 的工作电位, 是一种极具发展潜力的锂离子电池负极材料。然而, Sb负极在嵌脱锂程中会遭受巨大的体积膨胀 (230%), 导致结构稳定性恶化和容量迅速下降, 阻碍了其实际应用。在本工作中, 我们采用简单的高能球磨法首次制备了一种新型无定形Sb/C复合材料。在该复合物中, 非晶态的Sb颗粒均匀分散在碳主体框架中, 这一原子尺度的元素均匀分布使得嵌锂过程产生各向同性的体积膨胀, 从而缓解了结构应力, 并有助于维持长循环过程的结构稳定性。此外, 无定形纳米结构缩短了锂离子/电子的扩散通道, 促进了快速锂化反应动力学和高倍率性能。得益于此, 无定形Sb/C复合材料在0.1 A·g−1电流密度下表现出537.4 mAh·g−1的高可逆容量, 并在10 A·g−1的超高电流下仍能保持201 mAh·g−1的容量。即使在2.0 A·g−1下深度循环1500次后, 该材料仍能保持其初始容量的86.3%, 远超迄今报道的所有Sb基负极。对长循环后电极的形貌深入分析显示, 无定形Sb/C电极的体积膨胀率仅为34.6%, 远低于传统纳米晶态Sb/C负极223.1%的体积膨胀。总的来说, 本工作提出了一种制备超长循环寿命、超高倍率Sb基合金负极的新方法, 并将有助于高性能锂离子电池的开发。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22279093 and 22075216), the Natural Science Foundation of Hubei Province, China (No. 2022CFB096), and the Fundamental Research Funds for Central University (Nos. 2042022gf0005 and 2042021kf0194). The authors would like to thank Prof. Burak Ülgüt at Bilkent University for his assistance with EIS analysis and Dr. Shaobo Mo from the Core Facility of Wuhan University for the support of TEM tests.

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  1. Hubei Key Laboratory of Electrochemical Power Sources, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, China

    Ze-Zhou Yang, Yu-Qing Ou, Zhi-Kang Su, Heng-Jiang Cong, Xin-Ping Ai & Jiang-Feng Qian

  2. Institute of Technological Sciences, Wuhan University, Wuhan, 430072, China

    Cheng-Yi Zhang & Yan Zhao

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  4. Zhi-Kang Su
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  5. Yan Zhao
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  6. Heng-Jiang Cong
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  8. Jiang-Feng Qian
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Correspondence to Yan Zhao or Jiang-Feng Qian.

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Ze-Zhou Yang and Cheng-Yi Zhang have contributed equally to this work.

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Yang, ZZ., Zhang, CY., Ou, YQ. et al. Amorphous Sb/C composite with isotropic expansion property as an ultra-stable and high-rate anode for lithium-ion batteries. Rare Met. 43, 2039–2052 (2024). https://doi.org/10.1007/s12598-023-02548-x

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