Unprecedented Improvement of Single Li‐Ion Conductive Solid Polymer Electrolyte Through Salt Additive

Abstract Solid‐state lithium metal (Li°) batteries (SSLMBs) are believed to be the most promising technologies to tackle the safety concerns and the insufficient energy density encountered in conventional Li‐ion batteries. Solid polymer electrolytes (SPEs) inherently own good processability and flexibility, enabling large‐scale preparation of SSLMBs. To minimize the growth of Li° dendrites and cell polarization in SPE‐based SSLMBs, an additive‐containing single Li‐ion conductive SPE is reported. The characterization results show that a small dose of electrolyte additive (2 wt%) substantially increases the ionic conductivity of single Li‐ion conductive SPEs as well as the interfacial compatibility between electrode and SPE, allowing the cycling of SPE‐based cells with good electrochemical performance. This work may provide a paradigm shift on the design of highly cationic conductive electrolytes, which are essential for developing safe and high‐performance rechargeable batteries.