Role of Li‐Ion Depletion on Electrode Surface: Underlying Mechanism for Electrodeposition Behavior of Lithium Metal Anode,Advanced Energy Materials

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Role of Li‐Ion Depletion on Electrode Surface: Underlying Mechanism for Electrodeposition Behavior of Lithium Metal Anode
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-10-13 , DOI: 10.1002/aenm.202002390
Xieyu Xu ₁ , Yangyang Liu ₂ , Jang‐Yeon Hwang ₃ , Olesya O. Kapitanova _{1,

4} , Zhongxiao Song ₂ , Yang‐Kook Sun ₅ , Aleksandar Matic ₆ , Shizhao Xiong _{2,

6}

Affiliation

The application of lithium metal as an anode material for next generation high energy‐density batteries has to overcome the major bottleneck that is the seemingly unavoidable growth of Li dendrites caused by non‐uniform electrodeposition on the electrode surface. This problem must be addressed by clarifying the detailed mechanism. In this work the mass‐transfer of Li‐ions is investigated, a key process controlling the electrochemical reaction. By a phase field modeling approach, the Li‐ion concentration and the electric fields are visualized to reveal the role of three key experimental parameters, operating temperature, Li‐salt concentration in electrolyte, and applied current density, on the microstructure of deposited Li. It is shown that a rapid depletion of Li‐ions on electrode surface, induced by, e.g., low operating temperature, diluted electrolyte and a high applied current density, is the underlying driving force for non‐uniform electrodeposition of Li. Thus, a viable route to realize a dendrite‐free Li plating process would be to mitigate the depletion of Li‐ions on the electrode surface. The methodology and results in this work may boost the practical applicability of Li anodes in Li metal batteries and other battery systems using metal anodes.

中文翻译：

锂离子消耗在电极表面上的作用：锂金属阳极电沉积行为的潜在机制

锂金属作为下一代高能量密度电池的负极材料的应用必须克服主要瓶颈，这是由于电极表面电沉积不均匀而导致的锂枝晶生长不可避免的问题。必须通过阐明详细的机制来解决此问题。在这项工作中，研究了锂离子的传质，这是控制电化学反应的关键过程。通过相场建模方法，可以看到锂离子浓度和电场，以揭示三个关键实验参数，工作温度，电解液中锂盐浓度和施加的电流密度对沉积的锂微结构的作用。结果表明，由于工作温度低等原因，锂离子在电极表面迅速耗尽，稀电解质和高施加电流密度是锂电沉积不均匀的根本驱动力。因此，实现无枝晶锂电镀工艺的可行途径是减轻电极表面锂离子的消耗。这项工作的方法论和结果可能会提高锂阳极在锂金属电池和其他使用金属阳极的电池系统中的实用性。

更新日期：2020-11-25

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