锂离子电池电解液SEI成膜添加剂的研究进展

doi:10.11949/0438-1157.20211571

摘要/Abstract

摘要：

稳定的固体电解质界面（SEI）是提高锂离子电池电化学性能的关键，用电解液添加剂是改善锂离子电池性能最经济有效的方法之一。本文综述了近五年间包括不饱和酯化合物、含硫化合物、锂盐、无机化合物等作为电解液成膜添加剂在锂离子电池中的研究进展和作用机理，对它们的优缺点进行了评价，最后进行了总结和展望。未来成膜类添加剂的研究思路应该为：（1）应以有机物种为主，能够形成弹性模量小的SEI膜，便于适应阳极材料产生的膨胀行为。（2）添加剂要尽量保证形成的SEI膜与石墨等阳极材料产生良好的黏结，因此添加剂形成的聚合物的聚合度不能太小。（3）在没有性能极其优秀的成膜添加剂出现之前，添加剂的分子结构可以在现有的添加剂的基础上进行结构的优化或者官能团的设计。（4）重点攻关当前添加剂的应用的问题，提高添加剂的合成技术，降低合成成本。

关键词: 锂离子电池, 膜, 成膜添加剂, 固体电解质界面

Abstract:

A stable solid electrolyte interface (SEI) is the key to improving the electrochemical performance of the lithium-ion battery. Electrolyte additives are one of the most economical and effective methods to improve the performance of the lithium-ion battery. The existence of additives significantly improves the recyclability and service life of lithium-ion batteries, so it has been widely studied by researchers. This paper evaluates the research progress and action mechanism of unsaturated ester compounds, sulfur compounds, lithium salts and inorganic compounds as electrolyte film-forming additives in lithium-ion batteries in recent five years, evaluates their advantages and disadvantages and finally combines them with prospects. The future development trend of film-forming additives is proposed: (1) It is a general trend to use multiple additives or design new additives with multiple functional groups to make up for the shortcomings of a single additive in some aspects and facilitate the complementarity of functional advantages. (2) Quantum chemical calculation is an efficient method to screen film-forming additives, which is helpful to understand the action mechanism between additives and electrodes and speed up the research and development efficiency. (3) The characterization method of the SEI membrane needs to be further improved. To further study the action mechanism of additives, the in-situ analysis method can be considered in the future characterization process. The main ideas for developing film-forming additives in the future include: (1) The additives shall be mainly organic species, which can form SEI film with small elastic modulus, to adapt to the expansion behavior of anode materials. (2) The additive should try to ensure that the formed SEI film and graphite and other anode materials have good adhesion, so the polymerization degree of the polymer formed by the additive should not be too small. (3) Before there is no film-forming additive with excellent performance, the molecular structure of the additive should be similar to the current film-forming additive as far as possible, to facilitate industrial production. (4) Focus on the application of current additives, improve the synthesis technology of additives, reduce the synthesis cost, facilitate large-scale use, and benefit society.

Key words: lithium ion battery, film, film forming additives, SEI

中图分类号:

TM 912

胡华坤, 薛文东, 霍思达, 李勇, 蒋朋. 锂离子电池电解液SEI成膜添加剂的研究进展[J]. 化工学报, 2022, 73(4): 1436-1454.

Huakun HU, Wendong XUE, Sida HUO, Yong LI, Peng JIANG. Review of SEI film forming additives for electrolyte of lithium ion battery[J]. CIESC Journal, 2022, 73(4): 1436-1454.

图/表 16

图1 常见不饱和酯类添加剂的分子结构

Fig.1 Molecular structure of common unsaturated ester additives

图2 在含有1%VC的1.0 mol/L LiPF6/EC/DMC中，HOPG电极上不同表面演化阶段的示意图[29]

Fig.2 The schematic of different surface evolution stage on HOPG electrode in 1.0 mol/L LiPF6/EC/DMC with 1% VC[29]

图3 向电解液中添加VC时表面保护层形成过程的示意图[34]

Fig.3 Schematic illustrations of the postulated formation process of surface protective layer when VC was added to the electrolyte[34]

图4 锂离子电池中基于微胶囊的VC添加剂释放示意图[37]

Fig.4 Schematic of microcapsule-based release of VC additives in a Li-ion battery[37]

图5 在EC和FEC电解液形成过程中计算的微分电容图[54]

Fig.5 The calculated capacity plots during the formation step of EC and FEC electrolyte[54]

图6 五种电解液中10次充放电循环后硅微柱阵列电极的SEM图像[(a)~(e)]; 晶体Si〈100〉晶面原子分布示意图(f) [63]

Fig.6 SEM images of Si micropillar array electrodes after 10 charge/discharge cycles in five electrolytes[(a)~(e)]; Schematic diagram of the atomic distribution of crystal Si〈100〉 crystal plane (f) [63]

图7 常见含硫成膜添加剂的分子结构

Fig.7 Molecular structure of common sulfur containing additives

图8 PS的主要还原过程[74]

Fig.8 Main reduction process of PS[74]

表1 偶极矩、HOMO和LUMO能级能量、电离势（IP）、电子亲和性（EA）、化学硬度（η）以及与锂离子相互作用的Gibbs自由能（ΔG）［95］

Table 1 Dipole moments， HOMO and LUMO level energies， ionization potentials （IP）， electron affinities （EA）， chemical hardnesses （η）， and Gibbs free energies of interaction with lithium cation （ΔG）［95］

参数	DTD	PS	SPA	PES	EC
dipole/D(1D = 3.33563 ×10^-30 C·m)	7.99	8.45	7.40	8.64	7.33
HOMO/eV	-10.77	-10.33	-10.67	-9.89	-10.62
LOMO/eV	0.04	0.03	-0.10	-0.27	0.06
IP/eV	9.6	9.02	9.21	8.78	9.55
EA/eV	0.66	0.69	1.08	1.45	0.65
η/eV	4.48	4.16	4.06	3.67	4.36
ΔG(Li⁺)(neutral)/(kJ/mol)	3.76	0.85	3.70	1.20	0.45
ΔG(Li⁺)(anion)/(kJ/mol)	-19.56	-15.72	-24.73	-18.42	-41.54

图9 常见锂盐添加剂的分子结构

Fig.9 Molecular structure of common lithium salt additives

图10 基于标准和改良电解液的全电池EIS[109]

Fig.10 EIS of full-cells based on standard and modified electrolyte[109]

图11 不同电解质体系的离子电导率与温度的关系[112]

Fig.11 Dependence of ionic conductivity on temperature for different electrolyte systems[112]

表2 无添加剂和1.0%LiPO2F2样品的EIS拟合结果［118］

Table 2 EIS fitting results of samples with no additive and 1.0% LiPO2F2［118］

Sample	After the 1st cycle		After the 50th cycle		After the 150th cycle
Sample	r_SEI/Ω	r_ct/Ω	r_SEI/Ω	r_ct/Ω	r_SEI/Ω	r_ct/Ω
no additive	14.4	8.6	1.7	30.2	4.6	162.5
1% LiPO₂F₂	10.3	5.7	1.9	3.1	2.8	3.8

图12 LiPO2F2参与CEI膜形成的机制[119]

Fig.12 Mechanism of the LiPO2F2 participating in the formation of CEI film[119]

图13 1 mol/L LiPF6在无CO2和CO2饱和的EC/DEC溶液中的红外光谱[130]

Fig.13 IR spectra of 1 mol/L LiPF6 in EC/DEC solutions without CO2 and saturated with CO2[130]

图14 裸锂箔和均匀Ag-Li合金层上Li形核和生长过程的示意图[135]

Fig.14 Schematic diagrams of the Li nucleation and growth process on the bare Li foil and uniform Ag-Li alloy layer[135]

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