Abstract
Poly(ethylene oxide) (PEO)-based electrolytes are promising for all-solid-state batteries but can only be used above room temperature due to the high-degree crystallization of PEO and the intimate affinity between ethylene oxide (EO) chains and lithium ions. Here, a homogeneous-inspired design of PEO-based solid-state electrolytes with fast ion conduction is proposed. The homogeneous PEO-based solid-state electrolyte with an adjusted succinonitrile (SN) and PEO molar ratio simultaneously suppresses the PEO crystallization and mitigates the affinity between EO and Li+. By adjusting the molar ratio of SN to PEO (SN:EO approximate to 1:4), channels providing fast Li(+)transport are formed within the homogeneous solid-state polymer electrolyte, which increases the ionic conductivity by 100 times and enables their application at a low temperature (0-25 degrees C), together with the uniform lithium deposition. This modified PEO-based electrolyte also enables a LiFePO(4)cathode to achieve a superior Coulombic efficiency (>99%) and have a long life (>750 cycles) at room temperature. Moreover, even at a low temperature of 0 degrees C, 82% of its room-temperature capacity remains, demonstrating the great potential of this electrolyte for practical solid-state lithium battery applications.