锂硫电池电解液研究进展：分子设计与应用

doi:10.11949/0438-1157.20250331

化工学报 ›› 2025, Vol. 76 ›› Issue (12): 6196-6217.DOI: 10.11949/0438-1157.20250331

锂硫电池电解液研究进展：分子设计与应用

王梦涵¹^,²^,³^,⁴(), 于淼¹^,²^,³^,⁴, 吴桐¹^,²^,³^,⁴()

^1.内蒙古民族大学化学与材料学院，内蒙古通辽 028000
^2.内蒙古民族大学纳米创新研究院，内蒙古通辽 028000
^3.内蒙古自治区纳米碳材料重点实验室，内蒙古通辽 028000
^4.锂硫电池储能内蒙古自治区工程研究中心，内蒙古通辽 028000

收稿日期:2025-04-01 修回日期:2025-05-22 出版日期:2025-12-31 发布日期:2026-01-23
通讯作者: 吴桐
作者简介:王梦涵（2001—），女，硕士研究生，1146532814@qq.com
基金资助:
2020年度自治区本级事业单位引进人才科研启动绩效项目(RCQD20002);2021年科研启动金(BS416);三氟甲基苯类分子可控调制氟化SEI与增强锂硫电池机制研究(22461030);含氟电解液添加剂实现快充RinNM膜锂硫电池(GXKY25Z039)

Research progress of electrolyte for lithium-sulfur batteries: molecular design and application

Menghan WANG¹^,²^,³^,⁴(), Miao YU¹^,²^,³^,⁴, Tong WU¹^,²^,³^,⁴()

^1.School of Chemistry and Materials Science, Inner Mongolia University for Nationalities, Tongliao 028000, Inner Mongolia, China
^2.Nanoinnovation Research Institute of Inner Mongolia University for Nationalities, Tongliao 028000, Inner Mongolia, China
^3.Key Laboratory of Nanocarbon Materials in Inner Mongolia Autonomous Region, Tongliao 028000, Inner Mongolia, China
^4.Lithium sulfur battery energy storage Inner Mongolia Autonomous Region Engineering Research Center, Tongliao 028000, Inner Mongolia, China

Received:2025-04-01 Revised:2025-05-22 Online:2025-12-31 Published:2026-01-23
Contact: Tong WU

摘要/Abstract

摘要：

锂硫（Li-S）电池作为一种具有高能量密度的储能体系，是能源领域的重点研究对象。但其在充放电过程中可溶性多硫化锂的穿梭效应及氧化还原动力学缓慢等问题，严重影响了锂硫电池的商业化发展进程。电解液作为锂硫电池体系中不可或缺的一部分，通常由锂盐、有机溶剂以及各类添加剂共同组成，在充放电过程中起到保护锂负极、传导锂离子的作用，其功能对电池的反应过程、循环寿命和安全性能等方面均产生影响。近年来，电解液添加剂备受研究者的关注，将其加入到电解液中可实现抑制多硫化物（LiPSs）穿梭、增强电极界面稳定性和提高离子电导率等功能。通过对近期相关文献的调查，介绍了含氮、氟、硫和多原子协同作用的添加剂的分子设计，及其提升电池充放电的氧化还原动力学和抑制多硫化物穿梭效应的策略及研究进展，并分析其因电负性的差异，在调控多硫化物和电极界面表现出的不同机制。简要阐述了锂盐在电解液中的重要作用，包括提供锂离子，参与电极反应过程，维持电荷平衡和保障离子传导等，为锂硫电池电解液添加剂的分子设计与实际应用拓展了思路。最后展望了锂硫电池电解液添加剂的未来发展方向。

关键词: 锂硫电池, 电解液添加剂, 界面, 动力学, 多硫化物

Abstract:

Lithium sulfur(Li-S) batteries, as an energy storage system with high energy density, are a key research object in the field of energy. However, problems such as the shuttle effect of soluble lithium polysulfides and slow redox kinetics during charge and discharge have seriously hampered the commercialization of Li-S batteries. As an indispensable part of the lithium sulfur battery system, the electrolyte is usually composed of lithium salts, organic solvents, and various additives. It plays a role in protecting the lithium negative electrode and conducting lithium ions during the charging and discharging process. Its function has an impact on the reaction process, cycle life, and safety performance of the battery. In recent years, electrolyte additives have attracted much attention from researchers. Adding them to electrolytes can achieve functions such as inhibiting polysulfide (LiPSs) shuttle, enhancing electrode interface stability, and improving ion conductivity. Through a survey of recent relevant literature, this article introduces the molecular design of additives containing nitrogen, fluorine, sulfur, and multi atom synergistic effects, as well as strategies and research progress to enhance the redox kinetics of battery charging and discharging and suppress the shuttle effect of polysulfides. It also analyzes the different mechanisms exhibited by these additives in regulating the interface between polysulfides and electrodes due to differences in electronegativity. At the same time, the important role of lithium salts in electrolytes was briefly explained, including providing lithium ions, participating in electrode reaction processes, maintaining charge balance, and ensuring ion conduction, which expanded the ideas for the molecular design and practical application of lithium sulfur battery electrolyte additives. Finally, we provide some perspectives on the future development of electrolyte additives for lithium-sulfur batteries.

Key words: lithium-sulfur battery, electrolytes additive, interface, kinetics, polysulfides

中图分类号:

TQ 152

王梦涵, 于淼, 吴桐. 锂硫电池电解液研究进展：分子设计与应用[J]. 化工学报, 2025, 76(12): 6196-6217.

Menghan WANG, Miao YU, Tong WU. Research progress of electrolyte for lithium-sulfur batteries: molecular design and application[J]. CIESC Journal, 2025, 76(12): 6196-6217.

图/表 17

图1 锂硫电池电解液添加剂及其作用

Fig.1 Electrolyte additives and their functions for lithium-sulfur batteries

图2 （a）Li2S8溶液与QASs、T1Br、T2Br、T3Br、T4Br、T8Br和T3TFSI的紫外-可见光谱；（b）反应方程；（c）T3Br电解液中正极放电时的S K边近边结构（XANES）谱；（d）电极在T3Br和空白电解液中放电过程电压曲线；（e）空白电解液和T3Br电解液对锂表面电化学界面演变影响的示意图；（f）1C（相应电流下，一次放电持续1小时）的长循环性能[45]

Fig.2 (a) Ultraviolet-visible spectra of Li2S8 solution with QASs, T1Br, T2Br, T3Br, T4Br, T8Br and T3TFSI; (b) Reaction equation; (c) S-K-edge Near Edge Structure (XANES) Spectrum during Positive Electrode Discharge in T3Br Electrolyte; (d) Voltage curves of the electrode during the discharge process in T3Br and blank electrolyte; (e) Schematic diagram of the influence of blank electrolytes and T3Br electrolytes on the evolution of the electrochemical interface on the lithium surface; (f) Long cycle performance of 1C (Under the corresponding current, one discharge lasts for 1 hour)[45]

图3 （a）唑-Li2S n （n=4，6，8）配合物的结构及唑类化合物参与固体电解质界面膜的形成并抑制锂枝晶形成示意图；（b）离子电导率和 Li+转移数；（c）循环50次后Li|Li对称电池锂负极扫描电子显微镜（SEM）图相应横截面SEM图像；（d）0.1C，硫负载为3.4 mg·cm-2、3.7 mg·cm-2，使用Ta、Tta基电解液的高负载Li-S电池的循环性能[46]

Fig.3 (a) The structure of the oxazole Li2S n (n=4,6,8) complex and the schematic diagram of the oxazole compounds participating in the formation of solid electrolyte interface facial mask and inhibiting the formation of lithium dendrites; (b) Ionic conductivity and Li+transfer number; (c) S After 50 cycles, the scanning electron microscope (SEM) image of the Li | Li symmetric battery’s lithium negative electrode corresponds to the cross-sectional SEM image; (d) 0.1C, Cycle performance of high load Li-S batteries with sulfur loadings of 3.4 mg·cm-2 and 3.7 mg·cm-2 using Ta and Tta based electrolytes[46]

图4 （a）TFBCA和多硫化物之间反应的示意图；（b）含和不含TFBCA的电解液的离子电导率；（c）含和不含TFBCA的SEI示意图；（d）0.1C，硫负载为7.1 mg·cm-2条件下使用TFBCA电池循环性能[47]

Fig.4 (a) Schematic diagram of the reaction between TFBCA and polysulfides; (b) Ionic conductivity of electrolytes with and without TFBCA; (c) SEI schematic diagram with and without TFBCA; (d) Cycle performance of TFBCA battery under 0.1C, sulfur load of 7.1 mg·cm-2[47]

图5 （a）TFMSA添加剂对锂硫电池电极/电解液界面的影响示意图；（b）含空白电解液和含TFMSA电解液电池在0.5C倍率下的充放电曲线；（c）使用空白电解液和TFMSA电解液循环后的表面F 1s和S 2p XPS光谱；（d）0.2C，硫负载为5.2 mg·cm-2锂硫电池循环性能[50]

Fig.5 (a) Schematic diagram of the effect of TFMSA additive on the electrode/electrolyte interface of lithium sulfur batteries; (b) Charge discharge curves of batteries containing blank electrolyte and TFMSA electrolyte at 0.5C rate; (c) Surface F 1s and S 2p XPS spectra after cycling with blank electrolyte and TFMSA electrolyte; (d) 0.2C, Cycle performance of lithium sulfur battery with sulfur load of 5.2 mg·cm-2[50]

图6 （a）TFEB-Li2S x 介质氧化还原催化硫转化；（b）2 mmol·L-1 Li2S8正极电解液与不同浓度TFEB在200 mV·S-1下的循环伏安图；(c)添加TFEB和不添加TFEB电解液中循环锂负极的XPS光谱；（d）0.1C，硫负载为5 mg·cm-2不同TFEB含量的锂硫电池循环稳定性[51]

Fig.6 (a) TFEB-Li2S x medium redox catalytic sulfur conversion; (b) Cyclic voltammetry of 2 mmol·L-1 Li2S8 positive electrode electrolyte with different concentrations of TFEB at 200 mV·S-1; (c) XPS spectra of circulating lithium negative electrode with and without TFEB electrolyte; (d) 0.1C, Cycle stability of lithium sulfur batteries with sulfur loading of 5 mg·cm-2 and different TFEB contents[51]

图7 （a）石墨/LiMn2O4电池的放电容量和（b）库仑效率(10 mA·g-1 LiMn2O4）在无FSE和0.5%（质量分数）FSE添加条件下，在室温下进行10次初始循环后，再在60℃下进行第11至30次循环[53]

Fig.7 (a) Discharge capacity and (b) Coulombic efficiency (10 mA·g-1 LiMn2O4) of graphite/LiMn2O4 battery under the conditions of no FSE and 0.5% (mass) FSE addition, after 10 initial cycles at room temperature, the 11th to 30th cycles were carried out at 60℃[53]

图8 正极上多硫化锂的反应路径和Li-S电池的充放电曲线无添加剂（a）和有添加剂（c）；napp/n图（b）；（d）有和没有噻吩电池的对称硫/碳电池在105至10-2 Hz的频率范围内具有10 mV幅度扰动的电化学阻抗谱（EIS）图；（e）C/40，硫负载为3.6 mg·cm-2锂硫电池电化学性能[62]

Fig.8 Reaction pathway of lithium polysulfide on the positive electrode and charge discharge curve of Li-S battery (a) without additives and (c) additives; (b) napp/n diagram; (d) Electrochemical impedance spectroscopy (EIS) plots of symmetric sulfur/carbon batteries with and without thiophene batteries exhibiting a 10 mV amplitude perturbation in the frequency range of 105 to 10-2 Hz; (e) C/40, Electrochemical performance of lithium sulfur battery with sulfur loading of 3.6 mg·cm-2[62]

图9 （a）固体电解质界面膜的形成示意图；（b）5次循环后锂负极的含和不含BTB添加剂的SEI的XPS深度剖面；（c）20次循环后Li-S电池中含和不含BTB添加剂的循环锂负极的SEM图；（d）0.1C，高负载S正极、低E/S比及超薄锂负极时的循环性能[63]

Fig. 9 (a) Schematic diagram of the formation of solid electrolyte interface facial mask; (b) XPS depth profiles of SEI with and without BTB additive for lithium negative electrode after 5 cycles; (c) SEM of cycling Li negative electrode with and without BTB additive in Li-S battery after 20 cycles; (d) 0.1C, Cycle performance of high load S positive electrode, low E/S ratio, and ultra-thin Li negative electrode[63]

图10 （a）未加入和（b）加入BPD的Li2S4溶液ESI-MS图；在（c）放电和（d）充电过程中，添加5 mmol·L-1 BPD的碱性电解液中获得的硫-碳正极的CV和在217、228、234、526和534 cm-1处的拉曼峰；（e）0.1C循环后，在有和没有添加25 mmol·L-1的BPD的锂负极SEM图；（f）0.1C不同硫醇基添加剂对硫碳正极的循环性能[64]

Fig.10 (a) not included; (b) Electrospray ionization mass spectrum of Li2S4 solution added with BPD; The CV and Raman peaks at 217, 228, 234, 526, and 534 cm-1 of the sulfur carbon cathode obtained in alkaline electrolyte with 5 mmol·L-1 BPD during (c) discharge and (d) charge processes; (e) SEM of lithium negative electrode with and without the addition of 25 mmol·L-1 BPD after 0.1C cycling; (f) The cyclic performance of sulfur carbon cathode with different thiol based additives at 0.1C[64]

图11 添加4Mpy的锂硫电池的放电产物的液相色谱-质谱（LC-MS）谱图（a）锂-吡啶硫醇盐（Li-pyS）和（b）（Li-pyS2）；充电产物的LC-MS谱图（c）4,4-吡啶二硫化物（4,4-pyS2）和（d）4,4-吡啶四硫化物（4,4-pyS4）；（e）含有4Mpy添加剂的锂硫电池放电还原过程反应过程；（f）在高硫负载0.05C下的循环性能；（g）0.1C至4C下的倍率性能[73]

Fig.11 LC-MS spectra of discharged products in Li-S batteries with 4Mpy additive: (a) lithium-pyridinethiolate (Li-pyS) and (b) Li-pyS2; LC-MS spectra of recharged products: (c) 4,4-pyridinedisulfide (4,4-pyS2) and (d) 4,4-pyridinetetrasulfide (4,4-pyS4)；(e) Discharge reduction process of Li-S batteries with 4Mpy additive; (f) Cycle performance under high sulfur load of 0.05C; (g) Rate performance at 0.1C to 4C[73]

图12 （a）不同电解液的自熄时间测试；（b）不同电解液的极限氧指数；（c）PFPN阻燃机理示意图及其对电极表面SEI的影响；（d）乙醚基电解液中含PFPN的循环硫正极在50次循环后的燃烧测试；（e）0.2C循环性能[74]

Fig.12 (a) Self extinguishing time test of different electrolytes; (b) Limit oxygen index of different electrolytes; (c) Schematic diagram of PFPN flame retardant mechanism and its influence on electrode surface SEI; (d) Combustion test of cyclic sulfur positive electrode containing PFPN in ether based electrolyte after 50 cycles; (e) 0.2C Cycle performance[74]

表1 采用不同电解液添加剂组装锂硫电池的性能参数

Table 1 Performance parameters of lithium sulfur batteries assembled using different electrolyte additives

特征原子	添加剂	面载量/ (mg·cm^-2)	放电比容量/面积容量	循环性能	文献
N	卤化季铵盐-四丙基溴化铵（T3Br）	1.5~2.0	1132 mAh·g^-1（0.1C）	1C，700次循环后放电比容量590 mAh·g^-1	[45]
	三唑（Ta）、四唑（Tta）	3.4、3.7	800 mAh·g^-1、约790 mAh·g^-1（0.1C）	0.1C，100次循环后容量保持率96.5％（Ta）87.5％（Tta）	[46]
	4-（三氟甲基）硫代苯甲酰胺（TFBCA）	7.1	8.1 mAh cm^-2 (0.2C)	0.1C，50次循环后面积容量7 mAh·cm^-2	[47]
F	三氟甲磺酰胺（TFMSA）	5.2	1000 mAh·g^-1（0.2C）	0.2C，100次循环后放电比容量828 mAh·g^-1	[50]
	三（2，2，2-三氟乙基）硼酸酯（TFEB）	5.0	1084 mAh·g^-1（0.1C）	0.1C，200次循环后容量保持率63.3％	[51]
	1，2-双（二氟甲基硅基）乙烷（FSE）（锂离子电池）	—	约90 mAh (g of LiMn₂O₄)^-1 （60℃ 10 mA (g of LiMn₂O₄)^-1）	60℃，20次循环后放容量保持率超过62％；从室温升到60℃时，电池的库仑效率立即恢复	[53]
S	噻吩	3.6	1016 mAh·g^-1（C/40）	C/40，100次循环后容量保持率74％	[62]
	3，5-双（三氟甲基）苯硫酚（BTB）	4.5	950 mAh·g^-1(0.1C)	0.1C，82次循环后放电比容量700 mAh·g^-1	[63]
	联苯-4，4′-二硫醇（BPD）	0.7~1.2	900 mAh·g^-1(0.1C)	0.1C，300次循环后放电比容量575 mAh·g^-1	[64]
N、S	4-巯基吡啶（4Mpy）	5.59	6 mAh·cm^-2（0.05C）	0.05C，50次循环后面积容量4.85 mAh·cm^-2	[73]
N、F	乙氧基（五氟）环三磷腈（PFPN）	2.3	1103.4 mAh·g^-1（0.2C）	0.2C，100次循环后放电比容量904.6 mAh·g^-1；使用PFPN电池循环50次后硫正极点燃后迅速熄灭	[74]

图13 （a）离子电导率的Arrhenius图；（b）电解质的热重（TGA）曲线；（c）LiTCM和LiTFSI电池中锂负极上形成的固体电解质界面膜的示意图；（d）不同盐含量下，LiTCM/PEO电解质的倍率性能；（e）在相同环氧乙烷单元（EO）/Li比为20的情况下，使用LiX/PEO（X = TCM-或TFSI-）电解质的锂硫电池循环性能对比[88]

Fig.13 (a) Arrhenius plot of ion conductivity; (b) Thermogravimetric analysis (TGA) curve of electrolyte; (c) Schematic diagram of solid electrolyte interface facial mask formed on lithium cathode in LiTCM and LiTFSI batteries; (d) The rate performance of LiTCM/PEO electrolyte under different salt contents; (e) Comparison of cycling performance of lithium sulfur batteries using Li X /PEO (X=TCM- or TFSI-) electrolyte under the same ethylene oxide unit (EO) / Li ratio of 20[88]

图14 （a）紫外-可见吸收光谱；（b）锂电极表面的Li 1s、O 2s 和F 2s XPS的高分辨率光谱；（c）0.3C，不同电解质下Li-S电池的长期循环性能；（d）使用双盐中浓度电解液（MCE）和新型的稀释中浓度电解液（DMCE）时Li-S电池的倍率性能[89]

Figure 14 (a) UV visible absorption spectrum; High resolution spectra of (b) Li 1s、O 2s and F 2s XPS on the surface of lithium electrode; (c) 0.3C, Long term cycling performance of Li-S batteries under different electrolytes; (d) Rate performance of Li-S batteries using dual salt medium concentration electrolyte (MCE) and a novel diluted medium concentration electrolyte (DMCE) electrolyte[89]

图15 （a）LiI凝胶抑制现象的光学图像；（b）Li-S电池在空白电解液和LiI电解液中的反应途径示意图；（c）0.05C，400 Wh·kg-1级软包电池的循环性能[90]

Fig.15 (a) Optical image of LiI gel suppression phenomenon; (b) Schematic diagram of reaction pathways of Li-S battery in blank electrolyte and LiI electrolyte; (c) 0.05C, Cycle performance of 400 Wh·kg-1 soft pack battery[90]

表2 运用不同锂盐组装锂硫电池的性能参数

Table 2 Performance parameters of lithium-sulfur batteries assembled with different lithium salts

体系	锂盐	面载量/(mg·cm^-2)	放电比容量	循环性能	文献
单盐体系	三氰甲烷化物（LiTCM）^①	0.8~1.1	≈0.7 mAh·cm ^-2(0.1C)	0.2C，库仑效率约100％，保持30次循环	[88]
双盐体系	LiTFSI-LiFSI^②	2.0	682 mAh·g^-1（0.3C）	0.3C，500次循环放电比容量626 mAh·g^-1	[89]
双盐体系	LiTFSI-LiI^③	7.1（单面）	416 Wh·kg^-1（0.05C）	0.05C，16次循环保持稳定的库仑效率	[92]

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锂硫电池电解液研究进展：分子设计与应用

Research progress of electrolyte for lithium-sulfur batteries: molecular design and application

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