固态锂电池中的机械力学失效及解决策略

梁宇皓; 范丽珍

doi:10.7498/aps.69.20200713

摘要

固态锂电池中电极材料与固态电解质的力学性能对于电池的机械稳定性有重要影响, 如果电池内部的应力超过材料的强度, 则会在固态电池内部发生不同规模、不同组分的机械力学失效, 从而严重恶化电池的电化学性能. 本文从提高固态电池机械稳定性的角度出发, 阐述了固态电池中各组分的力学性能对固态电池机械稳定性的影响, 并分析了影响材料力学性能的因素. 另外, 固态锂电池在电池充放电过程中出现的机械力学失效问题, 包括电极材料/电解质的破裂/断裂、电极与电解质的接触损失以及由于锂枝晶引发的电池短路等, 也在综述中被讨论. 最后, 总结了目前解决固态锂电池中机械力学失效的一些常用策略, 并对未来该领域的研究方向进行了展望. 本文讨论的固态锂电池中的机械力学失效以及解决策略将有助于研究人员构筑高能量密度、长寿命、更安全的固态锂电池.

关键词:

Abstract

The mechanical properties of electrode materials and solid-state electrolytes in solid-state batteries (SSBs) have an important influence on the mechanical stabilties of SSBs. Mechanical failures in SSBs on different scales and in different components will occur once the stress inside SSBs exceeds the materials’ strengths, which seriously deteriorates the electrochemical performances of SSBs. From the perspective of stabilizing the mechanical stabilities of SSBs, in this review we describe the influences of the mechanical properties of each component in SSBs on the mechanical stabilites of SSBs, and we analyze the factors that affect the mechanical properties of materials. In addition, we also discuss the mechanical failures of SSBs during cycle, including electrode materials’ or solid-state electrolytes’ fractures, electrode-electrolyte contact losses, and short-circuits due to lithium dendrites. Finally, we summarize some common strategies to mitigate the mechanical failures in SSBs, and look forward to the future research directions in this field. Overall, the mechanical failures in SSBs and their strategies discussed in this review will help researchers build SSBs with higher energy density, longer life and higher safety.

Keywords:

作者及机构信息

北京科技大学，新材料技术研究院，北京　100083

通信作者: 范丽珍, fanlizhen@ustb.edu.cn

Authors and contacts

Institute of Advanced Materials and Technology, Beijing University of Science and Technology, Beijing 100083, China

Corresponding author: Fan Li-Zhen, fanlizhen@ustb.edu.cn

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施引文献

图 1 材料典型的应力-应变曲线

Fig. 1. A typical stress-strain curve of materials.

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图 2 NCA89和NCW90材料的　(a) a和c轴晶格参数; (b)晶胞体积随着电池电压的变化图; (c) NCA89和(d) NCW90材料在充电到4.3 V下截面的明场STEM-mosaic图^[61]

Fig. 2. Changes in (a) a- and c-axis lattice parameters and (b) unit cell volumes for NCA89 and NCW90 as a function of the cell voltage; bright-filed STEM mosaic image of a cross-section of (c) NCA89 and (d) NCW90 at charged to 4.3 V^[61].

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图 3 (100–y)(0.75 Li₂S·0.25 P₂S₅) ·yLiI(mol%)(y=0, 5, 10, 20, 和30)玻璃的杨氏模量和LiI含量的关系^[67]

Fig. 3. Relationship between the Young’s moduli and LiI content of (100–y)(0.75 Li₂S·0.25 P₂S₅) ·yLiI(mol%)(y=0, 5, 10, 20, and 30) glasses^[67].

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图 4 LiCoO₂在电池循环后破裂的SEM图^[45]

Fig. 4. SEM images of fracturing of LiCoO₂ particles in cycled battery^[45].

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图 5 NCM811/β-Li₃PS₄/In全固态电池首次循环不可逆容量损失的示意图^[85]

Fig. 5. Schematic diagram of the irreversible first cycle capacity loss of the NCM811/β-Li₃PS₄/In all-solid-state battery^[85].

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图 6 堆叠压力对锂金属固态电池短路行为的影响示意图　(a) 在电池制备期间, 在对电池施加压力之前, 电解质和锂金属之间的接触不良; (b)在25 MPa的压力下, 锂金属和电解质的物理接触得到改善; (c)即使随后将压力降低到5 MPa, 也会使锂对称电池的阻抗大幅降低; (d)在5 MPa的堆叠压力下进行沉积/剥离测试, 未观察到Li在电解质颗粒内部蠕变的现象; (e)在25 MPa的压力下, Li在电解质的晶粒之间缓慢蠕变, 并且在这些枝晶上产生沉积过程, 最终在48 h后电池发生短路; (f)当电池的堆叠压力过高时, Li会通过蠕变在电解质中形成树枝状枝晶, 从而使电池机械短路^[103]

Fig. 6. Schematic of the effect of the stack pressure on the shorting behavior of Li metal solid-state batteries:　(a) During cell fabrication, the contact between the electrolyte and Li metal is poor before pressing the Li metal on the electrolyte pellet; (b) Pressing the Li metal at 25 MPa allows for proper wetting of the electrolyte and (c) induces a large drop in the symmetric cell impedance, even when the pressure is later released to 5 MPa; (d) plating and stripping at a stack pressure of 5 MPa, no creeping of Li inside the SSE pellet is observed; (e) at a stack pressure of 25 MPa, Li slowly creeps between the grains of the SSE and plating occurs on these dendrites, eventually shorting the cell after 48 h; (f) when the stack pressure is too high, Li creeps through the electrolyte and forms dendrites that mechanically short the cell^[103].

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图 7 全固态电池中NCA80和FCG75电极的不同微观结构和界面演化示意图^[105]

Fig. 7. Schematic diagram of the different microstructural and interfical evolutions in the NCA80 and FCG75 electrodes in all-solid-state batteries^[105].

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图 8 PIC–5 μm, CIP–200 nm和多层“三明治”型复合固态电解质的示意图^[130]

Fig. 8. The schematic illustration of the PIC–5 µm, CIP–200 nm, and hierarchical sandwich-type composite electrolytes^[130].

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表 1 固态电池材料的力学性能

Table 1. Mechanical properties of solid-state battery materials.

电池材料		杨氏模量/GPa	剪切模量/GPa	硬度/GPa	泊松比(B/G)	K_c/MPa·m^1/2
氧化物电解质	Li_0.33La_0.57TiO₃^[29]	200	80	9.2	1.66	~1
	Li₇La₃Zr₂O₁₂^[30]	150	59.6	9.1	1.72	0.92–2.73
	Li_1.3Al_0.3Ti_1.7(PO₄)₃^[31]	115		7.1		1.10
	Li_6.5La₃Zr_1.5Ta_0.5O₁₂^[32]	153.8 ± 2.7	61.2 ± 1.1		1.59
硫化物电解质	Li₂S-P₂S₅^[33]	18.5	7.1 ± 0.3	1.9		0.23 ± 0.04
	Li₇P₃S₁₁^[34]
	Li₁₀GeP₂S₁₂^[34]	21.7	7.9		3.44
	Li₁₀SnP₂S₁₂^[34]	29.1	11.2		2.09
	Li₅PS₅Cl^[34]	22.1	8.1		3.57
聚合物电解质	PEO+LiTFSI^[35]	~10^–6
	PEO+ LiClO₄^[36]	14.5 × 10^–3
	PAN+LiClO₄^[37]	1.6 × 10³
	PVDF+LiBF₄^[38]	0.3 × 10^–3
电极材料	LiCoO₂^[33]	178—191		8.3		0.94
	LiFePO₄^[39]	125.9	48.9		2.02
	NCM^[40]	198		11
	石墨^[41]	32	12		2.34
	Si^[42]	113		16.6
	Li^[33]	5	4.25	10^–3

下载: 导出CSV

表 2 电极材料在电池循环过程中的体积变化

Table 2. Volume variation of electrode materials during battery cycle.

电极材料		嵌锂/锂化产物	体积变化/%
正极	LiCoO₂	Li_0.5CoO₂	2^[47]
	LiNiO₂	Li_0.5NiO₂	2.8^[48]
	LiMnO₂	Li_0.5MnO₂	5.6^[48]
	LiNi_1/3Co_1/3 Mn_1/3O₂	Li_0.04Ni_1/3Co_1/3 Mn_1/3O₂	7.2^[49]
	LiFePO₄	FePO₄	7^[50]
	S	Li₂S	76^[51]
负极	Si	Li₁₅Si₄	310^[42]
	石墨	LiC₆	13^[41]
	Li₄Ti₅O12	Li₂[Li_1/3Ti_5/3]O₄	0.2^[52]

下载: 导出CSV

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