Solid-state electrolytes hold great promise for advancing electrochemical energy storage devices. Advanced batteries based on solid electrolytes, particularly all-solid-state lithium-metal batteries, hold the potential to simultaneously address both high energy density and safety concerns associated with traditional lithium-ion batteries. Ideally, solid electrolytes should exhibit a high ionic conductivity at room temperature. In practical applications, other properties, such as electrochemical stability and compatibility with electrodes, are equally important. However, the pursuit of a single solid electrolyte possessing all of these properties remains challenging. Simulation techniques play an important role in the design of solid electrolyte materials, bypassing the difficulty of chemical synthesis and structural characterization. In these simulations, ionic conduction within bulk electrolytes and the ion deposition and stripping processes at the charged electrode–electrolyte interface can be investigated. By providing the flexibility to construct electrolyte models and explore structural evolution at multiple scales, simulation techniques facilitate the rational design of advanced solid electrolytes that maximizes their advantages and mitigates limitations. This account is initiated by introducing fundamental theories and simulation techniques to investigate the ionic conductivity of an inorganic solid electrolyte. Subsequently, we present our recent progress in designing high ionic conductivity electrolytes by increasing the concentration of Li vacancies, by tuning the type of defects, by constructing diffusion pathways, and by avoiding ion crowding. At last, the electrochemical stability of inorganic solid electrolytes and their compatibility with lithium-metal electrodes are addressed.

中文翻译：

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锂离子电池无机固态电解质材料的计算设计


固态电解质对于推进电化学储能设备具有广阔的前景。基于固体电解质的先进电池，特别是全固态锂金属电池，有可能同时解决与传统锂离子电池相关的高能量密度和安全问题。理想情况下，固体电解质应在室温下表现出高离子电导率。在实际应用中，其他性能，例如电化学稳定性和与电极的兼容性也同样重要。然而，追求具有所有这些特性的单一固体电解质仍然具有挑战性。模拟技术在固体电解质材料的设计中发挥着重要作用，绕过了化学合成和结构表征的困难。在这些模拟中，可以研究本体电解质内的离子传导以及带电电极-电解质界面处的离子沉积和剥离过程。通过提供构建电解质模型和探索多个尺度的结构演化的灵活性，模拟技术有助于先进固体电解质的合理设计，从而最大限度地发挥其优势并减轻局限性。本说明首先介绍基础理论和模拟技术来研究无机固体电解质的离子电导率。随后，我们介绍了通过增加锂空位浓度、调整缺陷类型、构建扩散路径和避免离子拥挤来设计高离子电导率电解质的最新进展。 最后，讨论了无机固体电解质的电化学稳定性及其与锂金属电极的相容性。