Shen Xin, Zhang Rui, Shi Peng, Zhang Xue-Qiang, Chen Xiang, Zhao Chen-Zi, Wu Peng, Guo Yi-Ming, Huang Jia-Qi, Zhang Qiang
Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.
Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, China.
Fundam Res. 2022 Nov 23;4(6):1498-1505. doi: 10.1016/j.fmre.2022.11.005. eCollection 2024 Nov.
Lithium metal is one of the most promising anode materials for next-generation high-energy-density rechargeable batteries. A fundamental mechanism understanding of the dead lithium formation under the interplay of electrochemistry and mechanics in lithium metal batteries is strongly considered. Herein, we proposed a mechano-electrochemical phase-field model to describe the lithium stripping process and quantify the dead lithium formation under stress. In particular, the rupture of solid electrolyte interphase and the shift of equilibrium potential caused by stress are coupled into stripping kinetics. The impact of external pressure on dead lithium formation with various electrolyte properties and initial electrodeposited morphologies is revealed. The overlooked detrimental effect of external pressure on Li stripping affords fresh insights into cell configuration and pressure management, which is critical for practical applications of lithium metal batteries.
锂金属是下一代高能量密度可充电电池最有前景的负极材料之一。深入理解锂金属电池中电化学和力学相互作用下死锂形成的基本机制至关重要。在此，我们提出了一个机械电化学相场模型来描述锂剥离过程，并量化应力作用下死锂的形成。特别地，固体电解质界面的破裂和应力引起的平衡电位的变化被耦合到剥离动力学中。揭示了外部压力对具有不同电解质性质和初始电沉积形态的死锂形成的影响。外部压力对锂剥离的被忽视的有害影响为电池结构和压力管理提供了新的见解，这对锂金属电池的实际应用至关重要。
