金属锂在固态电池中的沉积机理、策略及表征

曹文卓; 李泉; 王胜彬; 李文俊; 李泓

doi:10.7498/aps.69.20201293

摘要

全固态金属锂电池的能量密度有望达到现有商业化锂离子电池的2—5倍, 且有可能从本质上解决现有液态电解质锂离子电池的安全性问题. 要想实现全固态金属锂电池这一颠覆性技术, 克服金属锂/固态电解质界面存在的副反应严重、界面接触差、锂枝晶生长等一系列挑战至关重要. 本文探讨了金属锂在有机、无机固态电解质中的沉积机理及其控制策略, 以及金属锂负极的表征手段等, 为固态锂电池的实用化研究提供了建议. 在固态电池中, 电解质与负极之间固-固接触不良、缺陷、晶界、裂纹、孔隙、尖端附近较强的电场以及固态电解质自身的电子电导都可导致金属锂沉积, 进而演变成锂枝晶. 针对这些诱因, 可以通过提高固态电解质的机械强度, 增大并改善固态电解质和负极的界面接触, 减少固态电解质内部及表面的缺陷、杂质和孔隙, 限制固态电解质内部的阴离子运动, 诱导锂的均匀沉积, 修复不均匀沉积形成的锂枝晶等方法均匀化锂沉积. 固态锂电池走向应用仍然存在诸多挑战, 需要扎实的基础研究, 有目标导向的设计思路和全面、系统、创新的综合解决方案.

关键词:

Abstract

Commercial lithium-ion batteries have inherent safety problems due to the usage of non-aqueous electrolyte as the electrolytes. The development of solid state lithium metal batteries is expected to solve these problems while achieving higher energy density. However, the problem of lithium plating still exists. This article reviews the deposition behavior of lithium metal anodes in solid-state batteries, and provides suggestions for high-energy-density and high-safety solid-state lithium batteries. This paper systematically summarizes the mechanism of Li deposition in polymers and inorganic solid state electrolytes, and discusses the strategies of controlling lithium deposition and preventing lithium dendrites and the characterization of Li metal anodes. In solid-state batteries, poor solid-solid contact between the electrolyte and the anode, defects, grain boundaries, cracks, pores, enhanced electric and ionic fields near the tip, and high electronic conductivity of the solid state electrolyte can all lead to lithium deposition, which may evolve into lithium dendrites. There are several strategies to control lithium deposition: 1). Use functional materials and structure design to induce uniform deposition of lithium, such as improving the solid state electrolyte/anode interfacial contact, using lithiophilic coatings or sites, and designing three-dimensional structure electrodes and solid state electrolytes. 2). Suppress the generation of lithium dendrites, such as limiting the free movement of anions in solid state electrolytes (especially polymer solid electrolytes), to reduce local space charge which induces lithium dendrites. In addition, optimizing the solid electrolyte synthesis process to reduce lithium dendrites caused by defects is also an important method. 3). Strategies for dendrites already formed are essential for safety concern. The dendritic deposition is one of the intrinsic properties of lithium. Thus, there is no guarantee that there will be no lithium dendrites, especially at high current density. Once lithium dendrites are formed, countermeasures are required. For example, improving the mechanical strength of solid state electrolytes, and using self-healing materials, structures, and cycling conditions are proposed to avoid safety hazards caused by lithium dendrites piercing. This article focuses on the control of lithium deposition. Suppressing lithium dendrites only solves a little problem of the application of lithium metal anodes. In the future, in order to use lithium metal as a negative electrode in practical all-solid-state batteries, many challenges need to be overcome, such as irreversible side reactions between lithium and other materials, safety and volume change of composite lithium anodes. In addition, in order to allow the laboratory's research results to be quickly transformed into applications, it is also necessary to establish battery design, assembly, and test standards that are in agreement with practical requirements. In short, all-solid-state lithium batteries still have a long way to go, but they have great potential for safe, high-performance, and low-cost energy storage systems in the future.

Keywords:

作者及机构信息

1.
中国科学院物理研究所，可再生能源重点实验室，北京　100190

2.
中国科学院大学，材料科学与光电技术学院，北京　100049

3.
北京卫蓝新能源科技有限公司，北京　102402

通信作者: 李泓, hli@iphy.ac.cn

基金项目: 国家重点研发计划(批准号: 2016YFB0100100)和北京市科技计划(批准号: Z191100004719001)资助的课题

Authors and contacts

1.
Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

2.
University of Chinese Academy of Sciences, Beijing 100049, China

3.
Beijing WeLion New Energy Technology Co., LTD, Beijing 102402, China

Corresponding author: Li Hong, hli@iphy.ac.cn

Funds: Project supported by the National Key R&D Program of China (Grant No. 2016YFB0100100) and the Beijing Municipal Science and Technology Program, China (Grant No. Z191100004719001)

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施引文献

图 1 电沉积锂的电极表面示意图^[9]

Fig. 1. Schematic of the electrode surface on which lithium is electrodeposited^[9].

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图 2 枝晶横向生长的示意图^[10]

Fig. 2. Schematic drawing showing a lateral growth for dendrites^[10].

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图 3 同步硬X射线显微断层扫描切片探测到的锂从电极底部开始沉积生长　(a)−(d) 循环到各个阶段的对称锂电池的横截面的X射线断层扫描切片; (e)−(h) 显示在顶部的扫描切片对应的放大3D体重构电池图像^[11]

Fig. 3. Subsurface structures underneath dendrites detected by synchrotron hard X-ray tomography slices: (a)−(d) X-ray tomography slices showing the cross-sections of symmetric lithium cells cycled to various stages; (e)−(h) magnified, 3D reconstructed volumes of cells shown in the top panel^[11].

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图 4 无机固态电解质与锂负极之间的“点对点”式接触^[16]

Fig. 4. Point-to-point contact between the inorganic solid state electrolyte and Li anode^[16].

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图 5 锂枝晶沿晶界生长的SEM图像　(a) 未循环和(b) 循环后的Li_6.25Al_0.25La₃Zr₂O₁₂^[18]

Fig. 5. SEM image of dendrite propagation through the grain boundary: (a) Uncycled and (b) cycled Li_6.25Al_0.25La₃Zr₂O₁₂^[18].

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图 6 原位聚合过程的示意图^[42]

Fig. 6. Schematic illustration of in situ polymerization processes^[42].

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图 7 PAN/LATP/PEO三层复合固态电解质示意图　(a) LATP; (b) PAN/LATP/PEO; (c) PAN/LATP/PEO固态电解质的SEM图像^[65]

Fig. 7. Schematic diagram of PAN/LATP/PEO three-layer composite solid electrolyte. Illustrations of the solid full battery: (a) Pristine LATP; (b) PAN/LATP/PEO solid electrolyte; (c) SEM image of PAN/LATP/PEO solid electrolyte^[65].

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图 8 在有Ag-C纳米复合涂层的集流体上Li沉积脱出的示意图^[71]

Fig. 8. Schematic of Li plating–stripping on the current collector with a Ag–C nanocomposite layer^[71].

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图 9 使用聚亚胺防止颗粒间锂生长的自我修复机制示意图^[72]

Fig. 9. Schematic of the self-healing mechanism for inter-particle lithium growth prevention using polyimine^[72].

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图 10 锂在　(a)无骨架结构和(b)具有“自我校正”行为的周期性导电/介电骨架材料中的沉积行为示意图^[73]

Fig. 10. Schematic diagram of Li metal evolution in (a) hostless configuration and (b) periodic conductive/dielectric host with a “self-correction” behavior^[73].

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图 11 室温下Li/LLZO/Li对称电池的恒电流循环(插图显示最后两个循环)^[18]

Fig. 11. Galvanostatic cycling (the inset shows the last two cycles) of a Li/LLZO/Li symmetric cell at room temperature^[18].

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图 12 有LiNb_0.5Ta_0.5O₃涂层的LiCoO₂首次充电后全固态电池的奈奎斯特图^[79]

Fig. 12. Nyquist plots for all-solid-state battery after the initial charge with LiNb_0.5Ta_0.5O₃-coated LiCoO₂^[79].

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图 13 (a) 光学显微照片显示Li枝晶沿着两个Cu集流体之间的LiPON界面生长^[80]; (b) 无3D Ti电极的全固态锂金属电池沉积锂后的截面图(23 μAh/cm²)^[81]

Fig. 13. (a) Optical micrograph showing Li dendrites growing along lithium phosphorus oxynitride (LiPON) interface between two Cu current collectors^[80]; (b) cross-sectional view of all-solid-state lithium metal battery w/o 3D Ti electrode after lithium plating (23 μAh/cm²)^[81].

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图 14 原位NDP的实验装置示意图^[25]

Fig. 14. Schematic diagram of the experimental set-up for operando NDP^[25].

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图 15 (a) 同步辐射X射线断层扫描装置图; (b) 含有重元素的石榴石电解质会使得X射线衰减, 无法成像. 相比之下, 使用APS(白光束)的高能X射线, 可以独立识别孔和陶瓷相; (c) 使用高能X射线获取孔隙率, 晶粒和纹理细节^[83]

Fig. 15. (a) Diagram of the synchrotron X-ray tomography setup; (b) garnet electrolytes dominated by heavy elements attenuate X-rays, and thus, imaging is impossible. In contrast, using high-energy X-rays at APS (white beam), the pore phase and ceramic phase can be identified independently; (c) the porosity, grain, and textural details can be extracted using high-energy X-rays^[83].

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[1]	李泓 2018 储能科学与技术 7 188 Li H 2018 Energy Stor. Sci. Technol. 7 188
[2]	Zu C, Li H 2011 Energy Environ. Sci. 4 2614 Google Scholar
[3]	Cao W, Zhang J, Li H 2020 Energy Stor. Mater. 26 46 Google Scholar
[4]	Monroe C, Newman J 2005 J. Electrochem. Soc. 152 A396 Google Scholar
[5]	Xue Z G, He D, Xie X L 2015 J. Mater. Chem. A 3 19218 Google Scholar
[6]	Bockris J L B a J O M 1962 Proc. R. Soc. London, Ser. A 268 485 Google Scholar
[7]	Monroe C, Newman J 2003 J. Electrochem. Soc. 150 A1377 Google Scholar
[8]	Akolkar R 2013 J. Power Sources 232 23 Google Scholar
[9]	Akolkar R 2014 J. Power Sources 246 84 Google Scholar
[10]	Dollé M l, Sannier L, Beaudoin B, Trentin M, Tarascon J M 2002 Electrochem. Solid-State Lett. 5 Google Scholar
[11]	Harry K J, Hallinan D T, Parkinson D Y, MacDowell A A, Balsara N P 2014 Nat. Mater. 13 69 Google Scholar
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[13]	Kushima A, So K P, Su C, Bai P, Kuriyama N, Maebashi T, Fujiwara Y, Bazant M Z, Li J 2017 Nano Energy 32 271 Google Scholar
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金属锂在固态电池中的沉积机理、策略及表征