Uniting Young's modulus and the flexibility of solid-state electrolytes for high-performance Li-batteries at room temperature

Abstract

The use of solid-state composite electrolytes is a promising strategy to advance all-solid-state batteries. Great efforts have been devoted to improving the ionic conductivity of electrolytes, while little attention has been paid to studying the effect of their mechanical properties on electrochemical performance. The Young's modulus and flexibility are two important and contrary mechanical properties co-existing in electrolytes. Their effect on the electrochemical performance of all-solid-state batteries is important. Here, we study the effect of Young's modulus and flexibility based on a designed sandwich-structured solid-state composite electrolyte (SSCE) with high ionic conductivity (4.57 × 10⁻⁴ S cm⁻¹ at 25 °C). In the SSCE, the middle layer with 9 : 1 : 0.5 mass ratio of Li_6.4La₃Zr_1.4Ta_0.6O₁₂, poly(vinylidene fluoride-co-hexafluoropropylene) and bis(trifluoromethane)sulfonimide lithium is sandwiched by two outer layers with a 0.1 : 1 : 0.5 mass ratio among them, which can effectively suppress lithium dendrites and have intimate contact with the electrodes, leading to Li|SSCE|LiFePO₄ with promising rate performance (155.5 mA h g⁻¹ at 0.05 C and 124.4 mA h g⁻¹ at 1 C) and excellent cycling stability with 98.8% capacity retention after 450 cycles at 25 °C. This work demonstrates that all-solid-state batteries have greatly enhanced electrochemical performance by uniting Young's modulus and flexibility via SSCEs, and provides a feasible strategy for the development of all-solid-state batteries.