Li metal anode is the “Holy Grail” material of advanced Lithium‐ion‐batteries (LIBs). However, it is plagued by uncontrollable dendrite growth resulting in poor cycling efficiency and short‐circuiting of batteries. This has spurred a plethora of research to understand the underlying mechanism of dendrite formation. While experimental studies suggest that there are complex physical and chemical interactions between heterogeneous solid‐electrolyte interphase (SEI) and dendrite growth, most of the studies do not reveal the mechanisms triggering these interactions. To deal with this knowledge gap, we propose a multiscale modeling framework which couples kinetic Monte Carlo and Molecular Dynamics simulations. Specifically, the model has been developed to account for (a) heterogeneous SEI, (b) dendrite‐SEI interactions, and (c) effect of electrolyte on Li electrodeposition and potential dendrite formation. This allows the proposed computational model to be extended to various electrolytes and SEI species and generate results consistent with previous experimental studies.

中文翻译：

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一种表征锂金属阳极钝化层形成的计算方法

锂金属阳极是高级锂离子电池（LIB）的“圣杯”材料。但是，它受到无法控制的枝晶生长的困扰，导致不良的循环效率和电池短路。这激发了许多研究来理解枝晶形成的潜在机理。尽管实验研究表明异质固-电解质界面相（SEI）与枝晶生长之间存在复杂的物理和化学相互作用，但大多数研究并未揭示触发这些相互作用的机理。为了解决这一知识鸿沟，我们提出了一个多尺度建模框架，该框架将动力学蒙特卡洛模拟和分子动力学模拟相结合。具体来说，该模型的开发考虑了（a）异构SEI，（b）枝晶-SEI相互作用，（c）电解质对锂电沉积和潜在枝晶形成的影响。这使得所提出的计算模型可以扩展到各种电解质和SEI种类，并产生与以前的实验研究一致的结果。