Effects of H2O on Improving the Performance of a Solid Composite Electrolyte Fabricated Via an Air-Processable Technique

Xine Fan, Yanmin Zhou,Mingda Wang, Junbao Lai,Wenzhe Shan,Zhen Xing,Hao Tang,Guiping Dai, Gaixia Zhang,Long Tan

ACS Applied Materials & Interfaces（2024）

Nanchang Univ | Ecole Technol Superieure ETS

Cited 1|Views7

Abstract

Inert atmosphere is normally necessary for fabrication of solid composite electrolytes (SCEs) as a crucial part of solid-state Li-metal batteries in order to avoid undesirable reactions induced by ambient moisture. Herein, we developed an air-processable technique to fabricate SCEs by employing LiCF3SO3 (LiOTf) as the Li salt, which was combined with Li6.4La3Zr1.4Ta0.6O12 (LLZTO) as the fast Li-conductor and polyvinylidene difluoroethylene/polyvinyl acetate (PVDF/PVAC) as the polymer matrix. With the assistance of trace H2O dissolved in electrolyte solution, the room-temperature Li+ conductivity of the obtained aSCE reached as high as 5.09 x 10(-4) S cm(-1), which was over 3 orders of magnitude higher than that of the one (iSCE, 1.93 x 10(-7) S cm(-1)) cast by the electrolyte solution prepared in an inert atmosphere. The theoretical calculation results reveal that the oxygen atom of H2O exhibits a high propensity to interact with the Li atom in LiOTf (LiO), thereby establishing a hydrogen bond with the oxygen atom (HO) in N,N-dimethylformamide (solvent). Such interactions promoted the dissociation of LiOTf and led to the formation of uniform Li+ transportation channels. Simultaneously, the composition distribution was also altered, resulting in a smoother surface of aSCE and lowered crystallinity of PVDF. On this basis, the LiOTf/LLZTO/PVDF/PVAC solution at 60 degrees C was directly coated onto the surface of the LiFePO4 (LFP) cathode to fabricate the LFP-aSCE film after drying in an oven. The assembled LFP-aSCE/Li battery wetted by trace sulfolane exhibited an initial Coulombic efficiency of 94.7% and a capacity retention rate of up to 96% at 0.2 C (137 mAh g(-1)) after 180 cycles and a high capacity of 143.7 mAh g(-1) at 0.5 C (150 cycles). Overall, this work could pave the way for the facile fabrication of solid electrolytes.

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Key words

energy storage,lithium metal battery,solid-stateelectrolyte,air-processable,lithium triflate

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Ultrastable Solid-State Lini0.8co0.1mn0.1o2/Li Battery by Suppressed Defluorination Reaction and in Situ Passivation on Electrodes

Junbao Lai, Kaibo Fan, Pengwei Zhou, Yanmin Zhou,Hao Tang,Guiping Dai,Gaixia Zhang,Long Tan

JOURNAL OF POWER SOURCES 2024

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【要点】：本研究开发了一种在空气中可处理的固态复合电解质（SCE）制备技术，通过在电解质溶液中加入微量的水，显著提高了SCE的离子导电性，为固态锂金属电池的简便制造提供了新方法。

【方法】：采用LiCF3SO3（LiOTf）作为锂盐，与快速锂导体Li6.4La3Zr1.4Ta0.6O12（LLZTO）和聚合物基体PVDF/PVAC结合，利用微量水分子促进LiOTf解离，形成均匀的Li+传输通道。

【实验】：通过将LiOTf/LLZTO/PVDF/PVAC溶液在60°C下直接涂覆在LiFePO4（LFP）电极表面，并在烤箱中干燥后制备得到LFP-aSCE膜。实验使用的数据集为所制备的SCE的离子导电性数据，结果显示在室温下，含水的SCE（aSCE）的离子导电性高达5.09 x 10^-4 S cm^-1，比在惰性气氛下制备的SCE（iSCE）高出三个数量级（iSCE的离子导电性为1.93 x 10^-7 S cm^-1）。所组装的LFP-aSCE/Li电池在经过180个循环后，其库仑效率初始值为94.7%，容量保留率高达96% at 0.2 C（137 mAh g^-1），并在0.5 C（150 cycles）下展现出高容量143.7 mAh g^-1。