Failure mechanism of lithium metal anode under practical conditions

Wang Xin-Meng; Shi Peng; Zhang Xue-Qiang; Chen Ai-Bing; Zhang Qiang

doi:10.7498/aps.69.20200906

Abstract

Lithium (Li) metal is regarded as one of the most promising anodes in the next-generation high-energy-density rechargeable batteries due to its ultrahigh theoretical specific capacity and low reduction potential. Nevertheless, the unstable solid electrolyte interphase on the surface of Li metal anode and the nonuniform Li deposition seriously hinder its practical applications. Currently, mild conditions are employed in the researches of Li metal anode, which is of great significance for fundamentally understanding the physicochemical features of the anode interface and the mechanisms of Li deposition. However, practical conditions including ultrathin Li metal anode (< 50 μm), low negative/positive electrode areal capacity ratio (< 3.0), and lean electrolyte (< 3.0 g·Ah^–1) are the premise to realize high energy density of Li metal batteries (> 350 W·h·kg^–1). Herein, the gaps of Li metal anode under mild and practical conditions in terms of the cycling stability and surface morphology are compared and the reasons for the gaps are analyzed carefully. The total quantity of active Li metal decreases and the utilization depth of Li per cycle has been greatly improved under practical conditions. Therefore, the huge volume fluctuation and uneven Li deposition result in ceaseless destruction and regeneration of solid electrolyte interphase, and thus consuming the lean electrolyte and generating a large quantity of dead Li rapidly. Consequently, the polarization voltage of Li metal anode increases rapidly and the cycling stability of Li metal batteries deteriorates evidently under practical conditions. Moreover, the electrochemical reaction of Li metal anode is accelerated while fast charge/discharge process is employed, which further aggravates the stability of Li metal anode. This work reveals the challenges of Li metal anode under practical conditions and present the perspectives for the further researches in practical Li metal anode, which conduces to the solid development of high-energy-density Li metal batteries.

Keywords:

Authors and contacts

1.
College of Chemical and Pharmaceutical Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, China
2.
Department of Chemical Engineering, Tsinghua University, Beijing 100084, China

Corresponding author: Chen Ai-Bing, chen_ab@163.com ; Zhang Qiang, zhang-qiang@mails.tsinghua.edu.cn

Funds: Project supported by the National Key Research and Development Program (Grant Nos. 2016YFA0202500, 2016YFA0200102), the National Natural Scientific Foundation of China (Grant No. 21676160), the National Science Fund for Distinguished Young Scholars of China (Grant No. 21825501), the Fund for Less Developed Regions of the National Natural Science Foundation of China (Grant No. U1801257), and the Tsinghua University Initiative Scientific Research Program of China

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Cited By

图 1 金属锂负极厚度对电池循环的影响　(a)不同锂负极厚度条件下电池结构示意图; (b) Li | NCM523全电池的循环性能; (c) Li | NCM523全电池第3圈和第60圈对应的充放电曲线

Figure 1. The effect of the thickness of Li metal anode on the cycling of batteries: (a) The schematics of batteries with Li metal anode in different thicknesses; (b) the cycling performance of Li | NCM523 batteries; (c) the corresponding charge and discharge curves of Li | NCM523 batteries at the 3^rd and 60^th cycle.

DownLoad: Full-Size Img PowerPoint

图 2 金属锂厚度对锂负极沉积形貌的影响　(a) 锂负极厚度为600 μm, 电流密度为1.0 mA·cm^–2, 循环容量为1.0 mA·h·cm^–2条件下, Li | Li对称电池的沉积形貌; (b) 锂负极厚度为50 μm, 电流密度为1.0 mA· cm^–2, 循环容量为1.0 mA·h·cm^–2条件下, Li | Li对称电池的沉积形貌; (c) 锂负极厚度为600 μm, 电流密度为3.0 mA·cm^–2, 循环容量为3.0 mA·h·cm^–2条件下, Li | Li对称电池的沉积形貌; (d)锂负极厚度为50 μm, 电流密度为3.0 mA·cm^–2, 循环容量为3.0 mA·h·cm^–2条件下, Li | Li对称电池的沉积形貌

Figure 2. The effect of the thickness of Li metal anode on the morphology of Li deposition: The morphology of the deposited Li in Li | Li symmetrical cells at (a, b) a current density of 1.0 mA·cm^–2 and a capacity of 1.0 mA·h·cm^–2, and (c, d) a current density of 3.0 mA·cm^–2 and a capacity of 3.0 mA·h·cm^–2. The thickness of the Li anode is 600 μm in (a, c) and 50 μm in (b, d).

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图 3 N/P比对电池循环的影响　(a)不同N/P比条件下的电池示意图; (b) Li | NCM523全电池循环性能; (c) Li | NCM523全电池第3圈和第50圈对应的充放电曲线

Figure 3. The effect of the N/P ratio on the cycling of batteries: (a) The schematics of batteries with different N/P ratios; (b) the cycling performance of Li | NCM523 batteries; (c) the corresponding charge and discharge curves of Li | NCM523 batteries at the 3^rd and 50^th cycle.

DownLoad: Full-Size Img PowerPoint

图 4 电解液量对电池循环的影响　(a)不同电解液量下的电池示意图; (b) Li | NCM523全电池的循环性能; (c) Li | NCM523电池第3圈和第40圈对应的充放电曲线

Figure 4. The effect of the amount of electrolyte on the cycling of batteries: (a) The schematics of batteries with different amounts of electrolyte; (b) the cycling performance of Li | NCM523 batteries; (c) the corresponding charge and discharge curves of Li | NCM523 batteries at the 3^rd and 40^th cycle.

DownLoad: Full-Size Img PowerPoint

图 5 循环倍率对电池循环的影响　(a)不同循环倍率下的电池示意图; (b) Li | NCM523全电池的循环性能; (c) Li | NCM523电池第3圈和第70圈对应的充放电曲线

Figure 5. The effect of the rate on the cycling of batteries: (a) The schematics of batteries with different rates; (b) the cycling performance of Li | NCM523 batteries; (c) the corresponding charge and discharge curves of Li | NCM523 batteries at the 3^rd and 70^th cycle.

DownLoad: Full-Size Img PowerPoint

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Vol. 69, Issue 22 - 2020-11-20

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