Mechanism, strategies, and characterizations of Li plating in solid state batteries

Cao Wen-Zhuo; Li Quan; Wang Sheng-Bin; Li Wen-Jun; Li Hong

doi:10.7498/aps.69.20201293

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:

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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Cited By

图 1 电沉积锂的电极表面示意图^[9]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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].

DownLoad: Full-Size Img PowerPoint

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[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
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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
[14]	Steiger J, Kramer D, Mönig R 2014 J. Power Sources 261 112 Google Scholar
[15]	郑碧珠, 王红春, 马嘉林, 龚正良, 杨勇 2017 中国科学: 化学 47 Zheng B, Wang H, Ma J, Gong Z, Yang Y 2017 Sci. Chin. Chem. 47
[16]	Han X, Gong Y, Fu K, He X, Hitz G T, Dai J, Pearse A, Liu B, Wang H, Rubloff G, Mo Y, Thangadurai V, Wachsman E D, Hu L 2017 Nat. Mater. 16 572
[17]	Nagao M, Hayashi A, Tatsumisago M, Kanetsuku T, Tsuda T, Kuwabata S 2013 Phys. Chem. Chem. Phys. 15 18600 Google Scholar
[18]	Cheng E J, Sharafi A, Sakamoto J 2017 Electrochim. Acta 223 85 Google Scholar
[19]	Yu S, Siegel D 2017 Chem. Mater. 29
[20]	Raj R, Wolfenstine J 2017 J. Power Sources 343 119 Google Scholar
[21]	Yu S, Siegel D J 2018 ACS Appl. Mater. Interfaces 10 38151 Google Scholar
[22]	Pesci Federico M, Brugge R H, Hekselman A K O, Cavallaro A, Chater R J, Aguadero A 2018 J. Mater. Chem. A 6 19817 Google Scholar
[23]	Ren Y, Shen Y, Lin Y, Nan C W 2015 Electrochem. Commun. 57 27 Google Scholar
[24]	Aguesse F, Manalastas W, Buannic L, Lopez Del Amo J M, Singh G, Llordes A, Kilner J 2017 ACS Appl. Mater. Interfaces 9 3808 Google Scholar
[25]	Han F, Westover A S, Yue J, Fan X, Wang F, Chi M, Leonard D N, Dudney N J, Wang H, Wang C 2019 Nat. Energy 4 187 Google Scholar
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[33]	Ni J E, Case E D, Sakamoto J S, Rangasamy E, Wolfenstine J B 2012 J. Mater. Sci 47 7978 Google Scholar
[34]	Wu J F, Pu B W, Wang D, Shi S Q, Zhao N, Guo X, Guo X 2019 ACS Appl. Mater. Interfaces 11 898 Google Scholar
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