Three-Layer-Structured Garnet-Dominant Composite Solid Electrolyte for Solid-State Batteries

Abstract

Solid-state batteries utilizing oxide, sulfide, and polymer electrolytes have garnered significant attention due to their robust safety and their applicability in high-energy-density advanced Li-ion batteries. In this study, we present an innovative three-layer-structured solid electrolyte, including the garnet-dominant composite solid electrolyte (GD-CSE) for solid-state batteries. This newly structured composite solid electrolyte (CSE) demonstrates a high ionic conductivity of around 1 mS/cm, substantial potential stability exceeding 5.0 V versus Li⁺/Li, and an exceptionally high Li-ion transference number of about 0.8 at room temperature. Upon evaluating its application in batteries, symmetric Li cells employing the three-layer CSE exhibit remarkable cycle stability lasting over 800 h at 0.1 mA/cm². Furthermore, a solid-state Li-metal battery configuration (LiFePO₄ (LFP)|three-layer-CSE|Li-metal) demonstrates favorable C-rate performance, achieving 63% at 5.0 C compared to 0.1 C capacity, along with an impressive cycle retention of 99% during 200 cycles at 0.5 C. Additionally, we manufacture solid-state Li-metal pouch-type cells measuring 3.4 × 5.0 cm². These pouch-type cells offer a capacity of 4.5 mAh and exhibit secure behavior even under bending and cutting conditions.

Keywords

composite solid electrolyte / garnet-type / solid state-batteries / three layer-structure

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