A passivation layer called the solid electrolyte interphase (SEI) is formed on electrode surfaces from decomposition products of electrolytes. The SEI allows Li⁺ transport and blocks electrons in order to prevent further electrolyte decomposition and ensure continued electrochemical reactions. The formation and growth mechanism of the nanometer thick SEI films are yet to be completely understood owing to their complex structure and lack of reliable in situ experimental techniques. Significant advances in computational methods have made it possible to predictively model the fundamentals of SEI. This review aims to give an overview of state-of-the-art modeling progress in the investigation of SEI films on the anodes, ranging from electronic structure calculations to mesoscale modeling, covering the thermodynamics and kinetics of electrolyte reduction reactions, SEI formation, modification through electrolyte design, correlation of SEI properties with battery performance, and the artificial SEI design. Multi-scale simulations have been summarized and compared with each other as well as with experiments. Computational details of the fundamental properties of SEI, such as electron tunneling, Li-ion transport, chemical/mechanical stability of the bulk SEI and electrode/(SEI/) electrolyte interfaces have been discussed. This review shows the potential of computational approaches in the deconvolution of SEI properties and design of artificial SEI. We believe that computational modeling can be integrated with experiments to complement each other and lead to a better understanding of the complex SEI for the development of a highly efficient battery in the future.

由电解质的分解产物在电极表面形成称为固体电解质中间相（SEI）的钝化层。SEI允许Li ⁺为了防止电解质进一步分解并确保持续的电化学反应，电子会迁移并阻挡电子。纳米厚的SEI膜的形成和生长机理由于其复杂的结构和缺乏可靠的原位实验技术而尚未得到完全的了解。计算方法的重大进步使人们可以对SEI的基本原理进行预测建模。这篇综述旨在概述阳极SEI膜研究中的最新建模进展，涵盖从电子结构计算到中尺度建模，涵盖电解质还原反应的热力学和动力学，SEI的形成，修饰通过电解质设计，SEI特性与电池性能的关联以及人工SEI设计。总结了多尺度模拟，并将其与实验进行了比较。已经讨论了SEI基本特性的计算细节，例如电子隧穿，锂离子迁移，本体SEI的化学/机械稳定性以及电极/（SEI /）电解质界面。这篇综述显示了计算方法在SEI属性反卷积和人工SEI设计中的潜力。我们相信，计算模型可以与实验相结合，以相互补充，并导致对复杂SEI的更好理解，从而在将来开发高效电池。讨论了锂离子传输，本体SEI和电极/（SEI /）电解质界面的化学/机械稳定性。这篇综述显示了计算方法在SEI属性反卷积和人工SEI设计中的潜力。我们相信，计算模型可以与实验相结合，以相互补充，并导致对复杂SEI的更好理解，从而在将来开发高效电池。讨论了锂离子传输，本体SEI和电极/（SEI /）电解质界面的化学/机械稳定性。这篇综述显示了计算方法在SEI属性反卷积和人工SEI设计中的潜力。我们相信，计算模型可以与实验相结合，以相互补充，并导致对复杂SEI的更好理解，从而在将来开发高效电池。