As the demand for higher energy density grows rapidly, the development of high-voltage all-solid-state lithium batteries (ASSLBs) becomes essential. However, most existing solid electrolytes (SEs) are still incapable of stable operation at high voltages. Herein, we report a series of fluorinated lithium tantalum oxychlorides (LTOC-F) as amorphous SEs for high-voltage ASSLBs. The optimized LTOC-10%F SE exhibits remarkably improved high-voltage stability and a high ionic conductivity of 2.3 mS cm^–1 at 25 °C. The ASSLB using an LCO cathode and LTOC-10%F SE achieves a high capacity of 180 mAh g^–1 with a cutoff voltage of 4.5 V and high-capacity retention of 81% after 300 cycles. Furthermore, the underlying mechanisms for enhanced performance are identified as the intrinsically extended electrochemical window of SE and the in-situ-formed LiF-rich cathode-electrolyte interface (CEI). Overall, this work provides a fluorination strategy for high-voltage ASSLBs and also offers insights into the analysis of amorphous SEs and CEIs.

中文翻译：

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高压全固态锂电池用氟化超离子氯氧化物固体电解质

随着对更高能量密度的需求迅速增长，高压全固态锂电池（ASSLB）的开发变得至关重要。然而，大多数现有的固体电解质（SE）仍然无法在高电压下稳定运行。在此，我们报告了一系列氟化锂钽氯氧化物（LTOC-F）作为用于高压ASSLB的非晶SE。优化后的 LTOC-10%F SE 表现出显着改善的高电压稳定性和25 °C 时2.3 mS cm ^–1的高离子电导率。使用 LCO 阴极和 LTOC-10%F SE 的 ASSLB 可实现 180 mAh g ^–1的高容量，截止电压为 4.5 V，300 次循环后的高容量保持率为 81%。此外，增强性能的潜在机制被认为是 SE 本质上扩展的电化学窗口和原位形成的富含 LiF 的阴极电解质界面 (CEI)。总体而言，这项工作为高压 ASSLB 提供了一种氟化策略，并为非晶 SE 和 CEI 的分析提供了见解。