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Constructing interfacial gradient layers and enhancing lithium salt dissolution kinetics for high-rate solid-state batteries
Nano Energy ( IF 17.6 ) Pub Date : 2022-08-18 , DOI: 10.1016/j.nanoen.2022.107716
Jin Li , Haitao Zhang , Yingyue Cui , Haoran Da , Yingjun Cai , Suojiang Zhang

The stability of the interfacial layers depends mainly on the composition and distribution of the decomposition products from solid-state electrolytes (SSEs) in lithium metal batteries. Therefore, the design of SSEs becomes an attractive way to construct a homogeneous stable interfacial layer. Herein, pentafluorostyrene (PFS) as a block is used to generate robust interfacial layers for solid-state batteries. Meanwhile, PFS facilitates the dissociation of lithium salts to produce more free Li-ions which can enhance the ionic conductivity from the results of 7Li solid-state NMR spectra, density functional theory, and molecular dynamics calculations. Subsequently, XPS depth etching and TOF-SIMS characterizations together show that the gradient interfacial layer is composed of a rich C-F bond surface layer and a rich–LiF&Li3N bottom layer, enabling rapid transport and uniform deposition of lithium ions. As a result, the Li/Li symmetric cell can achieve a stable ultra-long cycle time of more than 3000 h at 0.2 mA cm−2 and a critical current density of 2.4 mA cm−2. The as-prepared SSE exhibits a high ionic conductivity of 4.3 × 10−4 S cm−1 at 25 °C and remarkable cycling stability at 0 °C and − 20 °C. Moreover, the lithium metal batteries based on as-prepared SSEs deliver high-rate (2 C) capability and high-voltage (NCM811) stability at room temperatures.



中文翻译:

构建界面梯度层并增强高速固态电池的锂盐溶解动力学

界面层的稳定性主要取决于锂金属电池中固态电解质(SSE)分解产物的组成和分布。因此,SSE 的设计成为构建均匀稳定界面层的一种有吸引力的方式。在此,五氟苯乙烯 (PFS) 作为块体用于为固态电池生成坚固的界面层。同时,PFS 促进锂盐的解离,产生更多的游离锂离子,从而提高离子电导率(7锂固态核磁共振光谱、密度泛函理论和分子动力学计算。随后,XPS 深度蚀刻和 TOF-SIMS 表征共同表明,梯度界面层由丰富的 CF 键表面层和丰富的-LiF&Li 3 N 底层组成,能够实现锂离子的快速传输和均匀沉积。因此,Li/Li 对称电池在 0.2 mA cm -2和 2.4 mA cm -2的临界电流密度下可以实现超过 3000 小时的稳定超长循环时间。所制备的 SSE 具有 4.3 × 10 -4 S cm -1的高离子电导率在 25 °C 下,在 0 °C 和 − 20 °C 下具有显着的循环稳定性。此外,基于所制备的 SSE 的锂金属电池在室温下具有高倍率 (2 C) 能力和高电压 (NCM811) 稳定性。

更新日期:2022-08-23
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