Solid-state batteries are on the roadmap for commercialization as the next generation of batteries because of their potential for improved safety, power density, and energy density compared with conventional Li-ion batteries. However, the interfacial reactivity and resulting resistance between the cathode and solid-state electrolyte (SSE) lead to deterioration of cell performance. Although reduction of the cathode/SSE interfacial impedance can be achieved using cathode coatings, optimizing their compositions remains a challenge. In this work, we employ a computational framework to evaluate and screen Li-containing materials as cathode coatings, focusing on their phase stability, electrochemical and chemical stability, and ionic conductivity. From this tiered screening, polyanionic oxide coatings were identified as exhibiting optimal properties, with LiH₂PO₄, LiTi₂(PO₄)₃, and LiPO₃ being particularly appealing candidates. Some lithium borates exhibiting excellent (electro)chemical stability at various interfaces are also highlighted. These results highlight the promise of using optimized polyanionic materials as cathode coatings for solid-state batteries.

固态电池正处于与下一代锂离子电池相比具有改善安全性，功率密度和能量密度的潜力的下一代电池商业化路线图上。但是，阴极与固态电解质（SSE）之间的界面反应性和所得电阻会导致电池性能下降。尽管使用阴极涂层可以降低阴极/ SSE界面阻抗，但优化其组成仍然是一个挑战。在这项工作中，我们采用一个计算框架来评估和筛选含锂材料作为阴极涂层，重点是它们的相稳定性，电化学和化学稳定性以及离子电导率。通过这种分层筛选，可以确定聚阴离子氧化物涂层具有最佳性能，₂ PO ₄，LiTi ₂（PO ₄）₃和LiPO ₃是特别吸引人的候选人。还强调了一些在各种界面上表现出优异的（电化学）化学稳定性的硼酸锂。这些结果突显了使用优化的聚阴离子材料作为固态电池阴极涂层的前景。