Thin-film solid electrolytes with wide electrochemical stability windows are required to develop solid-state lithium (Li) metal batteries with high energy densities. In this work, free-standing Li₃InCl₆ (30 μm)|Li₆PS₅Cl (30 μm) bilayer thin films are prepared by slurry casting, drying, and lamination. This combination of solid electrolytes is stable at both the cathode interface (high voltages) and anode interface (low voltages). The bilayer thin films exhibit >10× lower area-specific resistance than thick (∼1 mm) pellets fabricated by traditional powder pressing. The free-standing bilayer electrolytes are laminated onto electrodeposited LiCoO₂ cathodes. Subsequently a Li–In anode is laminated on top of the stack, and stable cycling of all-solid-state batteries is demonstrated. Because of reduced ohmic losses, cells fabricated with thin-film electrolytes exhibit lower cell polarization and improved rate capability compared with cells with a traditional pellet geometry. This study offers a general strategy to fabricate free-standing bilayer thin-film solid electrolytes for high-energy-density solid-state batteries.

中文翻译：

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使用浆料加工和层压用于固态电池的薄独立式硫化物/卤化物双层电解质

开发具有高能量密度的固态锂（Li）金属电池需要具有宽电化学稳定性窗口的薄膜固体电解质。在这项工作中，通过浆料浇铸、干燥和层压制备了独立式Li ₃ InCl ₆ (30 μm)|Li ₆ PS ₅ Cl (30 μm)双层薄膜。这种固体电解质组合在阴极界面（高电压）和阳极界面（低电压）下都很稳定。双层薄膜的面积比电阻比传统粉末压制制造的厚（约 1 毫米）颗粒低 10 倍以上。将独立式双层电解质层压到电沉积的LiCoO ₂阴极上。随后，Li-In阳极被层压在电池堆的顶部，并证明了全固态电池的稳定循环。由于欧姆损耗减少，与具有传统颗粒几何形状的电池相比，使用薄膜电解质制造的电池表现出较低的电池极化和改进的倍率性能。这项研究提供了制造用于高能量密度固态电池的独立式双层薄膜固体电解质的总体策略。