Anode interface in all-solid-state lithium-metal batteries: Challenges and strategies

Yu Qi-Peng; Liu Qi; Wang Zi-Qiang; Li Bao-Hua

doi:10.7498/aps.69.20201218

Abstract

The developing of all-solid-state lithium-metal batteries promises to improve safety and energy density. The challenges in the anode|electrolyte interface are crucial and divided into static and dynamic issues in this review. The static issues are mainly shown as the huge resistances appearing in the assembled batteries, while the dynamic issues are reflected in the rapid deterioration of cycling performance. The static issues are mainly due to the poor chemical stability and interfacial contact, while dendrite growth and void formation are contained in the dynamic issues. Solving dynamic issues on the basis of static issues can conduce to the construction of stable all-solid-state lithium-metal batteries.

Keywords:

Authors and contacts

1.
Shenzhen Key Laboratory on Power Battery Safety Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
2.
School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
3.
Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States

Corresponding author: Li Bao-Hua, libh@mail.sz.tsinghua.edu.cn

Funds: Project supported by the National Nature Science Foundation of China (Grant No. 51872157), the Department of Science and Technology of Guangdong Province, China (Grant No. 2017BT01N111), Bureau of Industrial and Information Technology of Shenzhen, China (Grant No. 20170428145209110) and the Science and Technology Innovation Committee of Shenzhen, China (Grants Nos. JCYJ20170817161753629, JCYJ20170412170911187)

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Figure 1. Schema of static and dynamic challenges of anode|electrolyte interface in all-solid-state lithium-metal batteries^[25-28].

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Figure 4. Timeline of imaging and characterization of Li-metal anode|solid electrolyte interfaces^[30].

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图 5 三种不同金属锂不规则沉积空隙型的　(a) X射线断层扫描图, (b) 三维重构图, (c)生长机理示意图; 球状型的 (d) X射线断层扫描图, (e) 三维重构图, (f) 生长机理示意图; 非球型的 (g) X射线断层扫描图, (h) 三维重构图, (i) 生长机理示意图^[82]

Figure 5. Three different irregular deposition of lithium metal: (a) X-ray tomography, (b) three-dimensional reconstruction, (c) schematic diagram of growth mechanism of void type; (d) X-ray tomography, (e) three-dimensional reconstruction, (f) schematic diagram of growth mechanism of globule type; (g) X-ray tomography, (h) three-dimensional reconstruction, (i) schematic diagram of growth mechanism of protruding nonglobular type^[82].

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图 6 不同阶段锂枝晶生长的局部电流密度分布图　(a) 0−8.27 C/cm²; (b) 8.27−6.53 C/cm²; (c) 16.53−35.82 C/cm²; (d) 35.82−54.72 C/cm²^[89]

Figure 6. Mapping of local current density for different stages during the growth of lithium globule: (a) 0−8.27 C/cm²; (b) 8.27−16.53 C/cm²; (c) 16.53−35.82 C/cm²; (d) 35.82−54.72 C/cm²^[89].

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图 7 (a) 金属锂负极边缘上针状枝晶的SEM图; (b) 聚焦离子束(FIB)打磨后针状枝晶的SEM图; (c) (d) 纳米操纵器推动针状锂枝晶后弯折的SEM图; (e) (f) 纳米操纵器在金属锂表面刮擦的SEM图^[90]

Figure 7. SEM images showing (a) dendrite on the edge of the anode; (b) milled dendrite using focused ion beam (FIB) showing hollow morphology; (c) the nanomanipulator shown by red circle before scratching the dendrite; (d) the nanomanipulator after scratching the dendrite showing the bent in the nanomanipulator; (e) the nanomanipulator before scratching metallic Li sheet; and (f) the nanomanipulator after scratching metallic Li sheet showing the accumulation of Li on the tip.

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图 8 (a)锂枝晶在固态电解质中的简化示意图, 其中枝晶顶部的箭头表示来自金属锂的施加压力, 沿着侧面的箭头表示由于沿该界面的摩擦而产生的剪切力; (b) 锂沉积过电势及裂纹拓展应力与缺陷尺寸的关系^[26]

Figure 8. (a) Simplified schematic of a Li filament in a solid electrolyte matrix; (b) Inverse square root dependence of Li plating overpotential and crack-extension stress (σ_{0, max}) on defect size. Curves for glassy LPS and LLZTO are shown^[26].

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图 9 金属锂在含有缺陷的LLZO表面沉积行为示意图^[114]

Figure 9. Schematic descriptions of uneven lithium-ion flux induced by surface morphological fluctuations and the corresponding inhomogeneous lithium deposition^[114].

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图 10 金属锂在含有金界面层的LLZO表面沉积行为示意图^[114]

Figure 10. Schematic description of lithium redistribution through the gold layer and lithium nucleation. ^[114].

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图 11 (a) LLCZN及 (b) LLCZN@LAO的金属锂对称电池的极化曲线; (c) 稳态电流与施加电压的关系图(插图: 电流与施加施加电压的时间关系图); (d)锂枝晶在电解质内部生长及抑制枝晶生长的示意图^[130]

Figure 11. Lithium platting/stripping performance of (a) LLCZN and (b) LLCZN@LAO in Li symmetric cells at different current densities; (c) values of I_s for LLCZN and LLCZN@LAO with different applied external voltages; chronoamperometry results of LLCZN and LLCZN@LAO with an applied external voltage of 1 V (inset); (d) schematic illustrations of Li formation within LLCZN and how to suppress it through surface coating ^[130].

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图 12 (a)“电化学过滤”法示意图; (b)“电化学过滤”法对应的电化学曲线; (c) 处理前的X射线断层扫描图; (d)和(e)“电化学过滤”法处理后的X射线断层扫描图^[131]

Figure 12. (a) Schematic of the electrochemical filtering treatment; (b) Current density and voltage of one electrochemical filtering treatment over time; (c) Slice through a reconstructed volume of a symmetric cell after 14 conditioning cycles. No inhomogeneities were observed at the interfaces, (d) (e) Slices through a reconstructed volume of the symmetric cell in (c) after an electrochemical filtering treatment ^[131].

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图 13 基于LAGP高性能金属锂电池中自愈合界面的设计与构造: Li |LAGP| LMO电池在不同界面修饰层作用下循环过程中的界面演变行为示意图　(a) 无界面修饰层; (b) 凝胶电解质修饰层; (c) 自愈合界面修饰层^[135]

Figure 13. Design and fabrication of the SHE Janus interfaces for high-performance LAGP-based lithium metal batteries. (a)−(c) Schematic illustrations of the interfacial evolution in Li|LAGP|LMO batteries without interface layers and with GPEs and SHEs as Janus interface layers during cycling, respectively^[135].

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图 14 (a)原始金属锂电极和石榴石型固态电解质在剥离/沉积过程相互作用示意图; (b)金属锂-PDMS复合电极和石榴石型固态电解质在剥离/沉积过程相互作用示意图^[54]

Figure 14. Schematic illustration of the (a) pristine lithium foil with garnet-type electrolyte; (b) stress self-adapted interface by using compressible PDMS/Li metal anode^[54].

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图 15 (a)基于MIEC三维管状集流体的金属锂负极结构示意图; (b)金属锂在碳基小管内以单晶形式沉积的TEM图; (c)碳基小管在沉积金属锂前后的高分辨TEM图^[141]

Figure 15. (a)Schematic process of creep-enabled Li deposition/stripping in an MIEC tubular matrix, where Coble creep dominates via interfacial diffusion along the MIEC/Li_bcc incoherent interface; (b) TEM images of the Li metal deposition inside the carbon tubule as a single crystal; (c) high-resolution TEM imaging of a tubule before plating ^[141].

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表 1 不同界面问题解决策略的优劣比较

Table 1. Comparison of advantages and disadvantages of different interfacial strategies.

界面问题	解决策略	优点	不足	参考文献
静态问题	加热	易实现、对聚合物电解质效果显著	对疏锂的无机固态电解质无效、无法解决化学稳定性差问题	[61,62]
	加压	易实现、效果显著	仅在装配前加压不能解决动态问题、电池运行加压实用性低、无法解决化学稳定性差问题	[57—60]
	掺杂	对无机固态电解质有效、能一定程度解决化学稳定性差问题	易降低离子电导率	[63—65]
	电解质纯化	有望促使金属锂均匀沉积	无法避免杂质再次形成	[66,68—70]
	NH₄F预处理	避免污染物再次形成、有望抑制锂枝晶	需防范HF污染	[67]
	界面修饰	能同时解决两种静态问题	薄膜制备工艺成本高、生产效率较低	[28,55,62,71—74]
	锂合金负极	能同时解决两种静态问题、对动态问题也有帮助	降低负极比能量密度	[75—77,132—134]
动态问题	聚合物电解质改性	综合提高固态电解质的离子电导率、机械强度等	影响因素较多且效果相对有限	[86,124—127]
	引入反应界面层	结合界面层与锂合金负极的优点	薄膜制备工艺成本高、生产效率低	[28,55,62,71,72, 114,128,129]
	晶粒表面包覆	降低固态电解质电子电导率抑制枝晶生长	热处理时需要避免元素扩散	[130]
	金属锂负极纯化	有效避免金属锂的不均匀沉积及剥离	亟需开发大规模、低成本的生产方法	[131]
	聚合物复合界面	有效解决静态问题及消除体积变化所带来的应力	引入额外的界面阻碍电荷转移、制备超薄的聚合物界面层难度大	[135,136]
	弹性集流体	可逆地储存及释放应力	降低金属负极的电子电导率	[54]
	三维结构	为金属锂沉积预留体积	大规模制备具挑战	[138—141]

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