锂离子电池低温电解液的研究进展

doi:10.19799/j.cnki.2095-4239.2022.0650

摘要/Abstract

摘要：

锂离子电池在低温条件下运行时，电池的电化学性能已经不能达到最佳状态，存在容量迅速恶化的问题，这限制了其在极寒地区以及航空、国防军事等特殊领域的应用。因此，提高电池的低温性能成为研究热点之一。本文通过对相关文献的探讨，综述了改善锂离子电池低温性能的策略，着重介绍了电导率较高的新型锂盐、由低熔点和高介电常数组成的混合溶剂以及有助于形成稳定SEI膜的成膜添加剂对电池低温性能的影响，重点分析了上述因素对于锂离子电池低温性能的影响机制。综合分析表明，Li⁺的溶剂化结构与去溶剂化过程在电极界面上的行为直接决定了电池的低温性能。本文强调了从电解液的溶剂化结构入手来设计低温电解液的重要性，为未来低温锂离子电池开发提供了新思路。

关键词: 锂离子电池, 低温, 电解液, 锂盐, 溶剂, 添加剂

Abstract:

When lithium-ion battery operates at low temperature, their electrochemical performance cannot reach the optimal state, and their capacity deteriorates rapidly, which limits their application in extremely cold regions, aviation, national defense and military, and other fields. Therefore, improving the low-temperature performance of batteries has become an interesting field of research, and this study discusses the relevant strategies in the literature. The effects and mechanism of factors, including new lithium salts with high conductivity, mixed solvents with low melting point and high dielectric constant, and film-forming additives that facilitate stable solid electrolyte interface (SEI) films, on the low-temperature performance of lithium-ion batteries, are emphatically studied. The comprehensive analysis shows that the solvation structure of Li⁺ and the behavior of the desolvation at the electrode interface directly determine the low-temperature performance of the battery. The importance of designing low-temperature electrolytes using the solvation structure of electrolytes was emphasized. It provides a novel idea for developing low-temperature lithium-ion batteries in the future.

Key words: lithiumion battery, low temperature, electrolyte, lithium salt, solvent, additive

中图分类号:

TM 911

封迈, 陈楠, 陈人杰. 锂离子电池低温电解液的研究进展[J]. 储能科学与技术, 2023, 12(3): 792-807.

Mai FENG, Nan CHEN, Renjie CHEN. Research progress of low-temperature electrolyte for lithium-ion battery[J]. Energy Storage Science and Technology, 2023, 12(3): 792-807.

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Lithium salt	Characteristics	Usage and dosage	Stability on AI	Stability on Cu
LiPF₆	1.空气中分解，放出PF₅，产生白色烟雾； 2.在有机溶剂中分解温度80 ℃； 3.对水敏感，副反应产物HF，破坏SEI	1. 1.2 mol/L电解液电导率最高； 2. 1 mol/L以上利于长循环寿命	好	好
LiBF₄	1.对水分不敏感； 2.分解温度390 ℃，热稳定性好； 3.溶剂中分解温度大于100 ℃； 4.离子电导率低，常用作添加剂	1.高温优于LiBOB，低温性能较好； 2.使用量0.5%以内	好	好
LiBOB	1.溶解度低； 2.离子电导率低于LiPF₆； 3.吸湿性； 4.成膜性能优异，参与SEI膜形成； 5.分解温度302 ℃，热稳定性好	1.提升锰酸锂循环并抑制膨胀； 2.负极成膜稳定，可以在PC溶剂中使用，拓宽电池温度适用范围； 3.使用量1%以内	好	好
LiODFB	1.分解温度240 ℃，不会在高温条件下与溶剂反应； 2.电导率介于LiBF₄和LiBOB之间； 3.负极成膜稳定，阻抗小	1.高压体系使用较多，与其他添加剂组合使用更好； 2.影响电解液酸度测试； 3.使用量1%以内	好	好
LiTFSI	1.较高的电化学稳定性和电导率； 2.分解温度370 ℃，热稳定性好； 3.对于电压要求不高的电池有优势	1.高低温性能、安全性能及容量方面，都超过了LiClO₄电解液； 2.使用量1.5%以内	差	好
LiFSI	1.具有较优异的电导率； 2.分解温度308 ℃，热稳定性好； 2.低温性能好，在低于-20 ℃时，有着明显的优势； 3.可以抑制软包电池胀气	1.提升倍率； 2.提升低温性能； 3.使用量1.5%以内	差	好

Solvent	Melting point/℃	Permittivity(F/M)	Viscosity/(mPa·s)
乙酸丙酯(PA)	-95	6.00	0.55
乙酸乙酯(EA)	-84	6.02	0.55
丙酸乙酯(EP)	-74	—	0.90(15 ℃)
乙酸甲酯(MA)	-98	6.7	0.37
碳酸甲乙酯(EMC)	-55	2.40	0.65
碳酸丙烯酯(PC)	-49	64.92	2.53
碳酸二乙酯(DEC)	-43	2.82	0.75
碳酸二甲酯(DMC)	2～4	3.12	0.59
碳酸乙烯酯(EC)	35～38	89.60	1.85(40 ℃)

Number	Sample name	Electrolyte composition
1#	BA0%+EC0%	Base(DMC∶EMC=3∶5)+1 mol/L LPF
2#	BA16%+EC10%	Base+16%BA+10%EC+1 mol/L LPF
3#	0.1 mol/L LBF	Base+16%BA+10%EC+0.1 mol/L LBF+0.9 mol/L LPF
4#	0.2 mol/L LBF	Base+16%BA+10%EC+0.2 mol/L LBF+0.8 mol/L LPF
5#	0.3 mol/L LBF	Base+16%BA+10%EC+0.3 mol/L LBF+0.7 mol/L LPF

Electrolyte	Cathode	Test temperature/℃	Current density	Cycling	Capacity /(mAh/g)	Reference
LiPF₆+80%EC/DMC(30∶70)+2%FEC+20%MA	NCM532	20	0.5 C	100	202	[38]
1 mol/L LiPF₆+0.05 mol/L CsPF₆+EC/PC/EMC(1∶1∶8)	Gr\|\|NCM111	-40	0.2 C	400	40	[37]
1.2 mol/L LiTFSI/AN/FM	NCM622	-20	0.2 C	100	130	[24]
1 mol/L LiDFOB/FEC/IZ	C	-10	0.1 C	20	155	[41]
BE+MA+1%TMSP+1%PCS	MCMB\|\|LiNi_0.5Mn_1.5O₄	-5	0.3 C	200	102	[20]
1.28 mol/L LiFSI+FEMC/FEC-D2	NCA	-20	1/3 C	400	150	[18]
BA16%+EC10%+0.3 mol/L LBF	NCM811	-20	0.1 C	10	150	[56]
1 mol/L LiFSI-LiNO₃/DME	NCM811	-91	5 C	700	86	[40]

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