腈类化合物在高电压电解液中的研究进展

doi:10.19799/j.cnki.2095-4239.2024.1123

摘要/Abstract

摘要：

提高工作电压是提升锂离子电池能量密度的有效途径，但由此引发的电解液氧化分解、过渡金属离子溶出以及正极材料结构破坏等问题，严重制约了其实际应用。因此，开发具有优异电化学稳定性的电解液成为研究的热点。腈类化合物由于高介电常数和优良的氧化稳定性，被视为高电压体系中优化电解液的理想选择。本文回顾了腈类化合物作为溶剂和添加剂的作用机理及性能特点，针对腈类溶剂与石墨及锂金属不相容的问题，讨论了高浓度电解液、弱溶剂化电解液、含氟腈类电解液及共晶电解质等4种优化策略，并总结了各策略的实际应用前景及商业化过程中面临的局限性，明确指出添加剂是当前最有效的应用方式。此外，通过介绍含硅、硼、硫等元素的化学基团修饰的新型腈类添加剂，探究了不同官能团的作用机制及其应用潜力。最后，本文阐述了腈类化合物在开发与应用中面临的机遇与挑战，展望了通过合成工艺的优化与新型添加剂的开发，获得低黏度、高纯度、界面稳定性更强的多官能团腈类化合物，并探讨其在高电压电解液，尤其是在钴酸锂电池电解液中的应用前景。

关键词: 锂离子电池, 电解液, 腈类化合物, 固体电解质界面膜

Abstract:

Increasing the working voltage is an effective strategy to enhance the energy density of lithium-ion batteries. However, issues such as electrolyte oxidation, transition metal ion dissolution, and structural degradation of cathode materials pose significant challenges, severely limiting their practical application. Consequently, the development of electrolytes with superior electrochemical stability has become a key research focus. Nitrile compounds, owing to their high dielectric constant and excellent oxidative stability, are regarded as ideal candidates for optimizing electrolytes in high-voltage systems. This review examines the functional mechanisms and performance characteristics of nitrile compounds as solvents and additives. To overcome the incompatibility of nitrile solvents with graphite and lithium metal, four optimization strategies are presented: high-concentration electrolytes, weakly solvated electrolytes, fluorinated nitrile electrolytes, and eutectic electrolytes. The review explores the practical applications and commercialization challenges associated with each strategy, emphasizing that additives currently represent the most effective approach. Furthermore, novel nitrile additives modified with chemical groups containing silicon, boron, or sulfur are introduced, and the mechanisms and potential applications of these functional groups are analyzed. Finally, the review summarizes the opportunities and challenges in the development and application of nitrile compounds. It anticipates that process optimization and the development of new additives will enable the synthesis of multifunctional nitrile compounds with low viscosity, high purity, and enhanced interface stability, and discusses their potential applications in high-voltage electrolytes, particularly for lithium cobalt oxide battery systems.

Key words: lithium-ion batteries, electrolyte, nitrile compound, solid-electrolyte interphase film

中图分类号:

TM 911

李南, 马静, 黄挺秀, 沈毅星, 沈旻, 江依义, 洪涛, 马国强, 马紫峰. 腈类化合物在高电压电解液中的研究进展[J]. 储能科学与技术, 2025, 14(3): 997-1009.

Nan LI, Jing MA, Tingxiu HUANG, Yixing SHEN, Min SHEN, Yiyi JIANG, Tao HONG, Guoqiang MA, Zifeng MA. Research progress on nitrile compounds in high potential electrolytes[J]. Energy Storage Science and Technology, 2025, 14(3): 997-1009.

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电池体系	电解液（如无特殊说明均指质量比）	电压/V	容量保持率/%	参考文献
LiNi_0.6Mn_0.2Co_0.2O₂/ silicon–graphite	1.0 mol/L LiPF₆-EC∶DEC(1∶1，体积比)，5% FEC，2% VC，1.0% TEOSCN	2.5~4.35	75.95(0.5C,364cycles,45 ℃)	[60]
Li/Li₄Ti₅O₁₂	1.15 mol/L LiPF₆-EC∶EMC∶DMC (1∶1∶1)， 2.0% OS3	1.0~2.5	80.00(1.0C, 150cycles, 25 ℃)	[61]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC∶DMC(1∶1∶1，体积比)，0.5% 4-TB	3.0~4.5	86.69(1.0C,100cycles, 25 ℃)	[54]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC∶DEC(1∶1∶1，体积比)，2.0%TCEB	2.75~4.5	78.20(1.0C,200cycles,25 ℃)	[64]
LiNi_1/3Co_1/3Mn_1/3O₂/ graphite Li/LiMn₂O₄	1.0 mol/L LiPF₆-EC∶DMC∶EMC(1∶1∶1)，0.2% SDPN; 1.0 mol/L LiPF₆-EC∶DMC∶EMC(1∶1∶1)，0.5% SDPN	3.0~4.6; 3.0~4.3	77.30(0.2C,100cycles, 25 ℃) 70.30(1.0C,200cycles, 55 ℃)	[69] [70]
Li/LiCoO₂ Li/graphite	1.0 mol/L LiPF₆-EC∶EMC(3∶7)，1.0% PSPN	3.0~4.4; 0.01~3.0	74.81(0.5C,200cycles, 25 ℃) 92.58(0.5C,200cycles, 25℃)	[71]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶EMC(3∶7)，1.0%苯磺酰基乙腈(PSPAN)	3.0~4.4	91.84(1.0C, 100cycles, 25 ℃)	[72]
Li/LiCoO₂	1.0 mol/L LiPF₆-EC∶DEC∶EMC(3∶2∶5)，2.0% 4-苯甲腈三甲基硼酸酯(LBTB)	3.0~4.4	73.21(1.0C,300cycles, 25 ℃)	[73]
Li/LiFePO₄ Graphite/ LiNi_0.6Co_0.2Mn_0.2O₂	1.0 mol/L LiPF₆-EC∶DMC∶DEC(1∶1∶1，体积比)，1.0%CP; 1.0 mol/L LiPF₆-EC∶EMC(1∶2)，1.0% CP	2.5~4.0; 3.0~4.5	76.70(1.0C,200cycles,60 ℃); 81.50(1.0C, 50cycles, 25 ℃)	[50] [53]
LiCoO₂/graphite	1.0 mol/L LiPF₆-EC∶DEC∶EMC(1∶1∶1)，0.5%四氟对苯二腈(TFTPN)	3.0~4.4	91.00(0.5C,300cycles, 25 ℃)	[74]
LiCoO₂/graphite	1.0 mol/L LiPF₆-EC∶DEC∶EMC(1∶1∶1，体积比)，5.0% FEC，1.0% BFBN	3.0~4.55	80.00(0.5C,556cycles, 25 ℃; 148cycles, 45 ℃)	[48]

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