The all-solid-state lithium-ion battery is a promising next-generation battery technology. However, the realization of all-solid-state batteries is impeded by limited understanding of solid electrolyte materials and solid electrolyte-electrode interfaces. In this review, we present an overview of recently developed computation techniques and their applications in understanding and advancing materials and interfaces in all-solid-state batteries. We review the role of ab initio molecular dynamics simulations in studying fast ion conductors and discuss the capabilities of thermodynamic calculations powered by materials databases for identifying the chemical and electrochemical stability of solid electrolyte materials and solid electrolyte-electrode interfaces. We highlight the computational studies in the design and discovery of new solid electrolyte materials and outline design guidelines for solid electrolytes and their interfaces. We conclude with discussion of future directions in computation techniques, materials development, and interface engineering for all-solid-state lithium-ion batteries.

全固态锂离子电池是有前途的下一代电池技术。然而，由于对固体电解质材料和固体电解质-电极界面的有限理解，阻碍了全固态电池的实现。在这篇综述中，我们概述了最近开发的计算技术及其在理解和推进全固态电池中的材料和界面方面的应用。我们回顾一下从头开始的作用在研究快速离子导体中的分子动力学模拟，并讨论了由材料数据库提供动力的热力学计算功能，以识别固体电解质材料和固体电解质-电极界面的化学和电化学稳定性。我们重点介绍了新型固体电解质材料的设计和发现中的计算研究，并概述了固体电解质及其界面的设计准则。最后，我们讨论了全固态锂离子电池的计算技术，材料开发和接口工程的未来方向。