论文标题
一种有效的策略，可以使Argyrodite硫化物成为出色的固态电解质：维护出色的离子电导率和用电极的界面稳定性
An Effective Strategy to Enable Argyrodite Sulfides as Superb Solid-State Electrolytes: Safeguarding Remarkable Ionic Conductivity and Interfacial Stability with Electrodes
论文作者
论文摘要
由于其高离子电导率，足够的可塑性和体面的机械强度，因此，随着高性能全稳态电池（ASSB）的高性能全稳态电池（ASSB），Argyrodite硫化物的吸引力越来越有吸引力。但是，它们与Li金属阳极和高压阴极不良的不兼容以及对空气的严重敏感性显着阻碍了它们的实际应用。在此，我们制定了一种有效的策略，以通过理论建模的指导来修改chalcogen化学来克服这些具有挑战性的缺点。所得的LI6.25PS4O1.25CL0.75与纯LI阳极和高压LiCoo2阴极提供了出色的电化学兼容性，而对原始硫化物的出色离子电导率产生了不利影响。此外，当前的SSE还表现出高度改善的空气中氧气和水分的稳定性，进一步的优势对电子的绝缘性更大。与电极的兼容性明显增强归因于固体阳极电解质间相（AEI）和阴极电解质相（CEI）层的原位形成。原位AEI的形成在创纪录的高电流密度下启用了超稳定的LI电镀/剥离，在LI | LI6.25PS4O1.25CL0.75 | Li对称性细胞中，在1800小时内。原位CEI促进了SSE在高压电压下的分解。因此，AEI和CEI的协同效应帮助LICOO2 | LI6.25PS4O1.25CL0.75 | LI电池电池与使用原始的LI6PS5CL作为SSE的循环稳定性明显更好，以SSE，在高度的活性阴极材料（4 mg cm cm-2）的高面积上。这项工作在Argyrodite硫化物家族中增加了理想的SSE，因此甚至可以在环境空气中制造高性能的实心电池电池。
The argyrodite sulfides are getting more and more attractive as highly promising solid-state electrolytes (SSEs) for high-performance all-solid-state batteries (ASSBs), owing to their high ionic conductivity, adequate plasticity, and decent mechanical strength. However, their poor incompatibility with Li metal anode and high voltage cathodes and as well as serious sensitivity to air significantly hinder their practical applications. Herein, we have devised an effective strategy to overcome these challenging shortcomings through modification of chalcogen chemistry under the guidance of theoretical modeling. The resultant Li6.25PS4O1.25Cl0.75 delivered excellent electrochemical compatibility with both pure Li anode and high-voltage LiCoO2 cathode, without detrimental impact upon the superb ionic conductivity of the pristine sulfide. Furthermore, the current SSE also exhibited highly improved stability to oxygen and moisture in air, with further advantage being more insulating to electrons. The remarkably enhanced compatibility with electrodes is attributed to in situ formation of solid anode electrolyte interphase (AEI) and cathode electrolyte interphase (CEI) layers. The formation of in situ AEI enabled ultra-stable Li plating/stripping at a record high current density up to 1 mAh cm-2 in Li|Li6.25PS4O1.25Cl0.75|Li symmetric cells over 1800 hours. The in situ CEI facilitated protection of the SSE from decomposition at elevated voltage. Consequently, the synergistic effect of AEI and CEI helped the LiCoO2|Li6.25PS4O1.25Cl0.75|Li battery cell to achieve markedly better cycling stability than that using the pristine Li6PS5Cl as SSE, at a high areal loading of the active cathode material (4 mg cm-2). This work adds a desirable SSE in the argyrodite sulfide family, so that high-performance solid battery cells could even be fabricated in ambient air.
