In this article, we present a novel theory for the long term evolution of the solid electrolyte interphase (SEI) in lithium-ion batteries and propose novel validation measurements. Both SEI thickness and morphology are predicted by our model as we take into account two transport mechanisms, i.e., solvent diffusion in the SEI pores and charge transport in the solid SEI phase. We show that a porous SEI is created due to the interplay of these transport mechanisms. Different dual layer SEIs emerge from different electrolyte decomposition reactions. We reveal the behavior of such dual layer structures and discuss its dependence on system parameters. Model analysis enables us to interpret SEI thickness fluctuations and link them to the rate-limiting transport mechanism. Our results are general and independent of specific modeling choices, e.g., for charge transport and reduction reactions.

中文翻译：

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揭示 SEI 形态：建模方法的深入分析

在本文中，我们提出了锂离子电池中固体电解质中间相 (SEI) 长期演变的新理论，并提出了新的验证测量方法。SEI 厚度和形态都由我们的模型预测，因为我们考虑了两种传输机制，即 SEI 孔中的溶剂扩散和固体 SEI 相中的电荷传输。我们表明，由于这些传输机制的相互作用，产生了多孔 SEI。不同的双层 SEI 产生于不同的电解质分解反应。我们揭示了这种双层结构的行为并讨论了它对系统参数的依赖。模型分析使我们能够解释 SEI 厚度波动并将它们与限速传输机制联系起来。我们的结果是通用的，独立于特定的建模选择，例如，