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Modeling of Void-Mediated Cracking and Lithium Penetration in All-Solid-State Batteries
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-05-31 , DOI: 10.1002/adfm.202303484 Wei Wang 1 , Jiaxuan Wang 1 , Chen Lin 2 , Haihui Ruan 1
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-05-31 , DOI: 10.1002/adfm.202303484 Wei Wang 1 , Jiaxuan Wang 1 , Chen Lin 2 , Haihui Ruan 1
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All-solid-state batteries (ASSBs) are expected to have an exceptional energy density and safety owing to the possibilities of direct usage of lithium as an anode and the suppression of dendrites by a solid-state electrolyte (SSE). However, recent experiments unveil discharging-induced voids in lithium-SSE interfaces and charging-induced cracks in SSE, wherein lithium penetration occurs. To avoid such cell failures, a theoretical model rendering high-credibility simulations is needed to assist ASSB designs. Herein, such a model coupling the electrochemical processes and mechanical responses of an ASSB are proposed, in which the kinetics of voids and cracks are the key ingredients. Numerical simulations based on the model reveal that void growth is the result of stripping with disparate diffusivity in the surface layer and the bulk of lithium. They bring about the non-uniform distribution of Li+ during electroplating, a damage zone near the interface, SSE cracking, and then lithium plating in the cracks. It is noted that the cracks and lithium dendrites revealed by the simulations are very similar to those observed in in situ experiments and that a high stack pressure cannot inhibit cracking and lithium penetration. Instead, suitable lateral compressive stresses can prevent SSE from cracking and therefore inhibit lithium dendrites.
中文翻译：
全固态电池中空洞介导的裂纹和锂渗透的建模
由于可以直接使用锂作为阳极并通过固态电解质（SSE）抑制枝晶，全固态电池（ASSB）预计将具有出色的能量密度和安全性。然而，最近的实验揭示了锂-SSE 界面中放电引起的空隙和 SSE 中充电引起的裂纹，其中发生锂渗透。为了避免此类电池故障，需要一个能够进行高可信度模拟的理论模型来辅助 ASSB 设计。在此，提出了一种耦合 ASSB 的电化学过程和机械响应的模型，其中空隙和裂纹的动力学是关键因素。基于该模型的数值模拟表明，空洞生长是表面层和锂本体中不同扩散率剥离的结果。+电镀时，界面附近出现损伤区，SSE裂纹，然后在裂纹中镀锂。值得注意的是，模拟揭示的裂纹和锂枝晶与原位实验中观察到的裂纹和锂枝晶非常相似，并且高堆压不能抑制裂纹和锂渗透。相反，适当的横向压应力可以防止 SSE 破裂，从而抑制锂枝晶。
更新日期：2023-05-31
中文翻译：
全固态电池中空洞介导的裂纹和锂渗透的建模
由于可以直接使用锂作为阳极并通过固态电解质（SSE）抑制枝晶，全固态电池（ASSB）预计将具有出色的能量密度和安全性。然而，最近的实验揭示了锂-SSE 界面中放电引起的空隙和 SSE 中充电引起的裂纹，其中发生锂渗透。为了避免此类电池故障，需要一个能够进行高可信度模拟的理论模型来辅助 ASSB 设计。在此，提出了一种耦合 ASSB 的电化学过程和机械响应的模型，其中空隙和裂纹的动力学是关键因素。基于该模型的数值模拟表明，空洞生长是表面层和锂本体中不同扩散率剥离的结果。+电镀时，界面附近出现损伤区，SSE裂纹，然后在裂纹中镀锂。值得注意的是，模拟揭示的裂纹和锂枝晶与原位实验中观察到的裂纹和锂枝晶非常相似，并且高堆压不能抑制裂纹和锂渗透。相反，适当的横向压应力可以防止 SSE 破裂，从而抑制锂枝晶。
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