金属锂固体电解质界面膜的研究进展

doi:10.11949/0438-1157.20231155

摘要/Abstract

摘要：

固体电解质界面（solid electrolyte interphase， SEI）是锂金属电池在首次充放电时，锂金属负极表面形成的一层钝化膜，对电池的循环性能和安全性能等具有至关重要的影响。充分地认识SEI膜将有助于开发具有更长循环寿命和更高安全性能的锂金属电池。综述了锂金属电池SEI膜的研究进展，介绍了SEI膜的组成和结构，梳理了各种常见组分的形成条件和作用，论证了两种用于描述SEI膜结构的模型，即马赛克模型和层状模型，总结了影响SEI膜组成和结构的关键因素，如电解质添加剂、电极电位、温度和电流密度等。并介绍了通过引入电解质添加剂和构建人工SEI膜实现界面稳定调控的最新研究进展，最后展望了SEI膜未来的研究方向。

关键词: 金属锂, 电化学, 显微结构, 锂金属电池, 固体电解质界面膜

Abstract:

Solid electrolyte interphase (SEI) is a passivation film formed on the surface of the lithium metal anode when the lithium metal battery is first charged and discharged. This interphase has a crucial impact on the cycle performance and safety of lithium metal batteries. A good understanding of SEI will help researchers develop lithium metal batteries with longer cycle life and higher safety. This paper reviews the research progress on solid electrolyte interphase in lithium metal batteries. It introduces the composition and structure of SEI, organizes the formation conditions and roles of various common components. Two main models used to describe the structure of SEI, namely the mosaic model and the laminar model, are demonstrated. Additionally, it summarizes key factors that affect the composition and structure of SEI such as electrolyte additives, electrode potentials, temperature, and current density etc. We also introduced the latest research progress in achieving interface stability control by introducing electrolyte additives and constructing artificial SEI membranes, and finally looked forward to the future research directions of SEI membranes.

Key words: lithium metal, electrochemistry, microstructure, lithium metal battery, solid electrolyte interphase

中图分类号:

TM 912

郑立涵, 沈之川, 施志聪. 金属锂固体电解质界面膜的研究进展[J]. 化工学报, 2023, 74(12): 4764-4776.

Lihan ZHENG, Zhichuan SHEN, Zhicong SHI. Research progress on solid electrolyte interphase of lithium metal[J]. CIESC Journal, 2023, 74(12): 4764-4776.

图/表 8

图1 由ISDN添加剂和LiFSI形成的SEI膜双层结构示意图[27]

Fig.1 Diagram of SEI bilayer structure formed by ISDN additive and LiFSI[27]

表1 SEI膜中常见成分的来源以及其作用

Table 1 The sources and functions of common components in SEI

成分	来源	作用	文献
Li₂O	在碳酸酯类或醚类电解液中产生	提高SEI膜的稳定性、离子电导率和机械强度	[15,20-22]
Li₂CO₃	由碳酸脂类电解质中的烷基碳酸锂与痕量水反应产生	提高SEI膜的机械强度，是所有成分中吸湿性最小的稳定化合物	[15,19-20]
LiN _x O _y	由LiNO₃或ISDN分解产生	改善SEI膜的均匀性，有效抑制了电解质和锂金属负极之间的副反应	[23-24,27]
Li₃N	LiNO₃添加剂或电解质中的 $N O_{3}^{-}$ 生成	具有高电导率，可以促进SEI膜中Li⁺的运输	[23-24,26]
Li₂S	由电解质中的多硫化物与Li⁺反应生成或从含有LiTFSI 或LiFTFSI的电解质中还原形成	可以提高SEI膜的稳定性，改善Li⁺在SEI膜的扩散，促进均匀的Li沉积	[28-31]
LiF	由电解质中的含氟锂盐（如LiPF₆、LiTFSI、LiFSI等）或添加剂（如FEC等）产生	具有高的化学稳定性和机械强度以及低的Li⁺扩散势垒，可以抑制负极表面的锂枝晶生长	[32-39]
LiH	由氢和沉积Li反应生成或者通过溶剂、H₂O和LiOH产生	消耗活性Li，破坏锂金属负极的循环稳定性	[40-41]
有机成分	由电解质分解产生	调节SEI膜的力学性能，提高柔韧性，降低SEI膜的致密性，影响Li⁺扩散	[42-46]

表1 SEI膜中常见成分的来源以及其作用

Table 1 The sources and functions of common components in SEI

成分	来源	作用	文献
Li₂O	在碳酸酯类或醚类电解液中产生	提高SEI膜的稳定性、离子电导率和机械强度	[15,20-22]
Li₂CO₃	由碳酸脂类电解质中的烷基碳酸锂与痕量水反应产生	提高SEI膜的机械强度，是所有成分中吸湿性最小的稳定化合物	[15,19-20]
LiN _x O _y	由LiNO₃或ISDN分解产生	改善SEI膜的均匀性，有效抑制了电解质和锂金属负极之间的副反应	[23-24,27]
Li₃N	LiNO₃添加剂或电解质中的 $N O_{3}^{-}$ 生成	具有高电导率，可以促进SEI膜中Li⁺的运输	[23-24,26]
Li₂S	由电解质中的多硫化物与Li⁺反应生成或从含有LiTFSI 或LiFTFSI的电解质中还原形成	可以提高SEI膜的稳定性，改善Li⁺在SEI膜的扩散，促进均匀的Li沉积	[28-31]
LiF	由电解质中的含氟锂盐（如LiPF₆、LiTFSI、LiFSI等）或添加剂（如FEC等）产生	具有高的化学稳定性和机械强度以及低的Li⁺扩散势垒，可以抑制负极表面的锂枝晶生长	[32-39]
LiH	由氢和沉积Li反应生成或者通过溶剂、H₂O和LiOH产生	消耗活性Li，破坏锂金属负极的循环稳定性	[40-41]
有机成分	由电解质分解产生	调节SEI膜的力学性能，提高柔韧性，降低SEI膜的致密性，影响Li⁺扩散	[42-46]

图2 不同电解液条件下形成的SEI膜的冷冻电镜图像以及结构示意图：(a)EC/DEC电解质中形成的SEI膜的原子分辨率图像；(b)EC/DEC电解质中形成的镶嵌状SEI膜的结构示意图；(c)FEC电解质中形成的SEI膜的原子分辨率图像；(d)FEC电解质中形成的层状SEI膜的结构示意图[56]

Fig.2 Cryo-electron microscopy images and structural diagrams of SEI under different electrolyte conditions: (a) Atomic-resolution image of the SEI formed in EC/DEC electrolyte; (b) Schematic of the mosaic-type SEI formed in EC/DEC electrolyte; (c) Atomic-resolution image of the SEI formed in FEC electrolyte; (d) Schematic of the multilayered SEI formed in FEC electrolyte[56]

图3 SEI膜结构随电极电位变化的演变示意图[64]

Fig.3 Schematic diagram of the evolution of SEI structure with the change of electrode potential[64]

图4 定制的PEEK电池示意图[70]

Fig.4 Diagram of the custom PEEK cell[70]

表2 影响SEI膜组成和形态结构的因素及其影响作用

Table 2 Factors and their effects on the composition and morphological structure of SEI

影响因素	影响作用	文献
电解质添加剂	不同的添加剂与各种电解质盐具有不同的电化学稳定性窗口，可以促进或抑制电解质中某种反应的发生或某种物质的分解，又或者是自身参与反应，从而改变SEI膜的结构和成分	[56-58,62-63]
电极电位	阳极的电极电位能够显著影响溶剂在阳极表面还原反应的ΔG_m，当电位较低时，无机成分和有机成分还原反应的ΔG_m不同，无机成分优先在电极表面还原，SEI膜呈层状结构。当电位较高时有机和无机化合物同时生成，形成的SEI膜呈镶嵌结构	[64]
温度	当温度较低时，Li⁺的扩散速度和电解质体系的反应动力学减慢，容易产生锂枝晶；当温度较高时，由于反应动力学加快，生成的SEI膜更厚，并且某些组分可能发生自发分解或者倾向于在表面呈大晶粒状	[65-66]
电流密度	不同的电流密度可以影响离子的浓度梯度、扩散速率以及电极表面的电化学反应速率。在低电流密度下形成的SEI膜主要由有机物组成，呈无定形结构；在高电流密度下形成的SEI膜是镶嵌结构，无机物嵌入在由有机物组成的无定形基质中，可能对SEI膜造成破坏	[67-68]
交流电场	在SEI膜形成时对电极表面施加交流电场可以促进大量阴离子在锂金属负极表面聚集并分解，可形成由阴离子衍生的SEI膜	[69]
压力	较低的压力会促进富含有机物的SEI膜和非均质、细丝状、分布有孔隙的锂沉积物生成，较高的压力可促进富含氟元素的无机SEI膜生成，能够形成更均匀、更致密的锂薄膜	[70]

图5 PyF添加剂加入碳酸酯电解液中形成的富阴离子溶剂化环境和SEI膜成分示意图[76]

Fig.5 Schematic diagram of anion-dominant solvation environment and SEI composition formed by PyF additive in carbonate electrolyte[76]

图6 使用催化化学方法设计的锂金属负极人工SEI膜的示意图及合成机理[79]

Fig.6 Schematic diagram and the corresponding synthesis mechanism of designing artificial SEI for lithium metal anode via catalytic chemistry[79]

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