Interface Stability in Solid-State Batteries
Interface Stability in Solid-State Batteries
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DOI：
10.1021/acs.chemmater.5b04082
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发表时间：
2016-01-12
影响因子：
8.6
通讯作者：
Ceder, Gerbrand
中科院分区：
文献类型：
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作者：
Richards, William D.;Miara, Lincoln J.;Ceder, Gerbrand
近年来，锂离子电池用高导电性固态电解液的开发进展迅速，但将这些新材料整合到高性能电池中却是困难的。界面阻力现在是许多体系中的限制因素，但这种阻力的确切机制尚未完全解释，部分原因是界面的实验评估可能非常困难。在这项工作中，我们发展了一种计算方法来研究阻性界面相形成的热力学。预测的界面相形成与实验界面观察和电池性能有很好的相关性。计算结果表明，硫代磷酸盐电解液与高压阴极的反应活性特别高，电化学稳定窗口较窄。我们还发现，一些已知的电解液本身并不稳定，而是与电极发生原位反应，形成钝化但离子导电的势垒层。作为实验人员的参考，我们列出了各种电解液、涂层和电极材料的稳定性和预期分解产物，包括一些尚未在实验中尝试的高性能组合。
Development of high conductivity solid-state electrolytes for lithium ion batteries has proceeded rapidly in recent years, but incorporating these new materials into high-performing batteries has proven difficult. Interfacial resistance is now the limiting factor in many systems, but the exact mechanisms of this resistance have not been fully explained in part because experimental evaluation of the interface can be very difficult. In this work, we develop a computational methodology to examine the thermodynamics of formation of resistive interfacial phases. The predicted interfacial phase formation is well correlated with experimental interfacial observations and battery performance. We calculate that thiophosphate electrolytes have especially high reactivity with high voltage cathodes and a narrow electrochemical stability window. We also find that a number of known electrolytes are not inherently stable but react in situ with the electrode to form passivating but ionically conducting barrier layers. As a reference for experimentalists, we tabulate the stability and expected decomposition products for a wide range of electrolyte, coating, and electrode materials including a number of high-performing combinations that have not yet been attempted experimentally.