Improving the reversibility of lithium (Li) metal anodes is critical to enable next-generation batteries. However, a comprehensive understanding of the factors that influence the nucleation and dynamic evolution of Li morphology is lacking. In this study, a platform for plan-view operando video microscopy is presented. Using this platform, we quantitatively study (1) differences in the nucleation density of dendrites and pits as a function of current density, (2) the influence of the Li surface grain boundaries on nucleation location, (3) the role of pits formed in the first cycle on dendrite reversibility and extended cycling, (4) the temporal evolution of individual dendrite size, and (5) the impacts of individual dendrite size on “dead Li” formation. The results provide mechanistic insight into the influence of surface spatial heterogeneity on nucleation and growth behavior and suggest that dead Li formation is influenced more by nucleation than by growth.

中文翻译：

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平面图Operando李金属阳极视频显微镜：确定核，形态和可逆性之间的耦合关系

改善锂（Li）金属阳极的可逆性对于下一代电池至关重要。然而，缺乏对影响锂形态成核和动态演化的因素的全面理解。在这项研究中，平面视图操作平台视频显微镜。使用该平台，我们定量研究（1）树枝状晶核和晶核的成核密度随电流密度变化的差异；（2）Li表面晶界对晶核形成位置的影响；（3）晶核形成的晶穴的作用第一个循环是树枝状晶体的可逆性和扩展循环，（4）单个树枝状晶体尺寸的时间演变，以及（5）单个树枝状晶体尺寸对“死锂”形成的影响。该结果提供了对表面空间异质性对成核和生长行为的影响的机械学见解，并表明死锂的形成受成核的影响大于受生长的影响。