Alexander Karger, Simon E. J. O’Kane, Marcel Rogge, Cedric Kirst, Jan P. Singer, Monica Marinescu, Gregory J. Offer and Andreas Jossen
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引用次数: 0
摘要
降解模型是了解和缓解锂离子电池老化的重要工具,然而,能够预测所有工作条件下降解情况的通用模型仍然遥不可及。其中一个挑战是日历和循环老化阶段对降解机制的耦合影响,例如固体电解质相(SEI)的形成。在这项工作中,我们确定并系统比较了文献中三种不同的 SEI 相互作用理论,并将它们应用到商用锂离子电池的实验降解数据中。经过一步步的研究和对数据的仔细筛选,我们发现,没有任何活性颗粒裂纹的 SEI 分层和 SEI 微裂纹(循环仅在循环过程中影响 SEI 的生长)都是不可能的候选理论。相反,结果表明,在循环过程中,SEI 和活性颗粒都会开裂,我们提供了一个简单的 4 参数方程,可以预测颗粒开裂率。与广为接受的帕里斯定律相反,颗粒开裂率会随着循环次数的增加而降低,这可能是由于活性颗粒的表面体积比不断增加,导致插层动力学发生了变化。所提出的模型可以准确预测不同存储条件下 SEI 的形成,而简单地将纯日历和循环老化产生的降解相加,则会低估总降解量。
Modeling Particle Versus SEI Cracking in Lithium-Ion Battery Degradation: Why Calendar and Cycle Aging Cannot Simply be Added
Degradation models are important tools for understanding and mitigating lithium-ion battery aging, yet a universal model that can predict degradation under all operating conditions remains elusive. One challenge is the coupled influence of calendar and cycle aging phases on degradation mechanisms, such as solid electrolyte interphase (SEI) formation. In this work, we identify and systematically compare three different SEI interaction theories found in the literature, and apply them to experimental degradation data from a commercial lithium-ion cell. In a step-by-step process, and after careful data selection, we show that SEI delamination without any cracking of the active particles, and SEI microcracking, where cycling only affects SEI growth during the cycle itself, are both unlikely candidates. Instead, the results indicate that upon cycling, both the SEI and the active particle crack, and we provide a simple, 4-parameter equation that can predict the particle crack rate. Contrary to the widely-accepted Paris’ law, the particle crack rate decreases with increasing cycles, potentially due to changing intercalation dynamics resulting from the increasing surface-to-volume ratio of the active particles. The proposed model predicts SEI formation accurately at different storage conditions, while simply adding the degradation from pure calendar and cycle aging underestimates the total degradation.
期刊介绍:
The Journal of The Electrochemical Society (JES) is the leader in the field of solid-state and electrochemical science and technology. This peer-reviewed journal publishes an average of 450 pages of 70 articles each month. Articles are posted online, with a monthly paper edition following electronic publication. The ECS membership benefits package includes access to the electronic edition of this journal.