锂离子电池预锂化技术研究进展及工程化应用展望

doi:10.19799/j.cnki.2095-4239.2024.1196

摘要/Abstract

摘要：

锂离子电池因其高能量密度和长循环寿命成为广泛使用的储能器件之一。然而，在初始循环过程中，固体电解质界面的形成以及一些不可逆副反应的发生需要消耗部分活性锂，导致初始库仑效率降低，整体电化学性能不佳。因此，需要开发出一种补锂策略来改善这一问题，而预锂化技术被认为是当前解决这一问题的最有效策略之一。本文通过调研相关文献，首先从固体电解质界面膜的形成以及不可逆反应的发生两个角度出发阐明了锂离子电池初始容量损失机理。其次，重点对现有的各种预锂化策略进行了系统分类和总结，对于负极预锂化技术，主要介绍了化学预锂化、负极富锂添加剂以及电化学预锂化等策略；对于正极预锂化技术，主要介绍了过锂化正极材料以及正极预锂化添加剂两种策略。最后，本文还探讨了预锂化技术当前所面临的瓶颈，并为各种预锂化策略提出了后续的改进建议，展望了预锂化技术在大规模实际应用中的潜力，旨在为锂离子电池先进预锂化技术的开发及应用提供有价值的参考。

关键词: 预锂化技术, 固态电解质界面膜，库仑效率, 高能量密度, 锂离子电池

Abstract:

Lithium-ion batteries are widely used energy storage devices owing to their high energy density and long cycle life. However, the formation of the solid electrolyte interface and irreversible side reactions during the initial cycling process consume active lithium, resulting in low initial coulombic efficiency and poor overall electrochemical performance. To address this issue, a lithium replenishment strategy is needed, with prelithiation technology being one of the most effective solutions. This study explores the initial capacity loss mechanism of lithium-ion batteries by examining the formation of the solid electrolyte interfacial film and irreversible reactions based on relevant literature. It then systematically classifies and summarizes various existing prelithiation strategies. For anode prelithiation technology, it introduces chemical prelithiation, anode lithium-rich additives, and electrochemical prelithiation strategies. For cathode prelithiation technology, it discusses the strategies of over-lithiation of cathode materials and anode prelithiation additives. In addition, this study highlights the challenges facing prelithiation technology and proposes improvements for various strategies. Finally, it explores the potential of prelithiation technology for large-scale practical applications, aiming to provide valuable insights for developing and applying advanced prelithiation technology in lithium-ion batteries.

Key words: prelithiation technology, solid electrolyte interface, initial Coulombic efficiency, high energy density, lithium-ion batteries

中图分类号:

TM 911

许陈程, 王湛, 李爽, 蒋江民, 鞠治成. 锂离子电池预锂化技术研究进展及工程化应用展望[J]. 储能科学与技术, 2025, 14(3): 930-946.

Chencheng XU, Zhan WANG, Shuang LI, Jiangmin JIANG, Zhicheng JU. Research progress and engineering application prospects of prelithiation technology for lithium-ion batteries[J]. Energy Storage Science and Technology, 2025, 14(3): 930-946.

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预锂化体系	电池体系	预锂化后ICE/%	容量保持率/%	参考文献
Li-Ph/2-MeTHF	石墨\|\|Li	102	94.89(200圈)	[24]
Li-BP/2-MeTHF	石墨\|\|Li	98.81	102.8(200圈)	[30]
4 BP/2-MeTHF	SiO/C\|\|Li	100.6	—	[33]
Li-FBp-MeTHF	SiO₂\|\|Li	101.7	75.4(300圈)	[34]
4,4′-DMBP-Li/DME(HFPN)	μSiO\|\|Li	99.57	90.67(350圈)	[35]
4,4′-DMBP-Li/THF(SbF₃)	SiO _x \|\|Li(Ni_0.8Co_0.1Mn_0.1)O₂	86.0	86.6(100圈)	[36]
金属锂直接接触	SiO _x \|\|NCM622	87.0	74 (200圈)	[42]
卷对卷机械法	Na₃V₂(PO₄)₂F₃(NVPF)\|\|Na-Sn合金	75.0	—	[40]
卷对卷机械法	LFP\|\|Li _x Sn	94.0	94.5 (200圈)	[41]
SLMP	Si-CNT\|\|Li	79	—	[44]
锂合金化合物Li _x Si-Li₂O	Si\|\|Li、石墨\|\|Li	94～100	—	[59]
复合材料Li _x Ge/Li₂O	石墨\|\|Li	100.6	—	[61]
外部短路	NCA\|\|c-SiO _x	85.34	61(100圈)	[64]
垂直预掺杂	石墨\|\|Li	接近100	—	[65]

预锂化体系	容量/(mAh/g)	电池体系	预锂化后容量提升/%	参考文献
LFO	867	7%LFO@LiCoO₂\|\|HC	14	[71]
LCO@LFO	736.6	NCM with 5% LCO@LFO)\|\|石墨	8.8	[72]
Li₂S/KB/PVP	1053	Li₂S/KB/PVP\|\|石墨	16.7	[79]
Li₃P@rGO	1547.61	LiFePO₄(2.5%Li₃P@rGO)\|\|石墨	10.2	[80]
M/Li₂O(M=Co，Ni，Fe)	800	LiFePO₄with 4.8% Co/Li₂O\|\|石墨	11	[81]
Li₁₊_x Ni_0.5Mn_1.5O₄	220.5	Li₁₊_x Ni_0.5Mn_1.5O₄\|\|石墨	4	[82]
CS-LiCoO₂	155	CS-LiCoO₂/石墨-SiO	11	[83]
LR-Ni65	220	LR-Ni65\|\|Si/石墨	11.5	[84]

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