Luo Shuting, Wang Zhenyu, Li Xuelei, Liu Xinyu, Wang Haidong, Ma Weigang, Zhang Lianqi, Zhu Lingyun, Zhang Xing
Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Department of Engineering Mechanics, Tsinghua University, Beijing, 100084, China.
Guilin Electrical Equipment Scientific Research Institute Co. Ltd., Guilin, 541004, Guangxi, China.
Nat Commun. 2021 Nov 29;12(1):6968. doi: 10.1038/s41467-021-27311-7.
All-solid-state lithium-based batteries with inorganic solid electrolytes are considered a viable option for electrochemical energy storage applications. However, the application of lithium metal is hindered by issues associated with the growth of mossy and dendritic Li morphologies upon prolonged cell cycling and undesired reactions at the electrode/solid electrolyte interface. In this context, alloy materials such as lithium-indium (Li-In) alloys are widely used at the laboratory scale because of their (electro)chemical stability, although no in-depth investigations on their morphological stability have been reported yet. In this work, we report the growth of Li-In dendritic structures when the alloy material is used in combination with a LiPSCl solid electrolyte and Li(NiCoMn)O positive electrode active material and cycled at high currents (e.g., 3.8 mA cm) and high cathode loading (e.g., 4 mAh cm). Via ex situ measurements and simulations, we demonstrate that the irregular growth of Li-In dendrites leads to cell short circuits after room-temperature long-term cycling. Furthermore, the difference between Li and Li-In dendrites is investigated and discussed to demonstrate the distinct type of dendrite morphology.
具有无机固体电解质的全固态锂基电池被认为是电化学储能应用的一个可行选择。然而,锂金属的应用受到了一些问题的阻碍,这些问题包括在长时间的电池循环过程中出现苔藓状和树枝状锂形态的生长,以及在电极/固体电解质界面发生不期望的反应。在这种情况下,诸如锂铟(Li-In)合金之类的合金材料因其(电)化学稳定性而在实验室规模中被广泛使用,尽管尚未有关于其形态稳定性的深入研究报道。在这项工作中,我们报告了当合金材料与LiPSCl固体电解质和Li(NiCoMn)O正极活性材料结合使用,并在高电流(例如3.8 mA cm)和高阴极负载(例如4 mAh cm)下循环时,Li-In树枝状结构的生长情况。通过非原位测量和模拟,我们证明了Li-In树枝状晶体的不规则生长会导致室温长期循环后电池短路。此外,还对Li和Li-In树枝状晶体之间的差异进行了研究和讨论,以展示不同类型的树枝状晶体形态。