Abstract
AbstractAll‐solid‐state lithium batteries with solid‐state electrolytes (SSEs) have gained worldwide attention due to their intrinsic safety and high energy density. However, there is no single electrolyte that can satisfy the out‐of‐sync requirements of both the anode and cathode interface. Herein, an ultrathin asymmetric composite electrolyte (ACE) is prepared by a simple slurry‐casting method, in which a Li6.75La3Zr1.75Ta0.25O12 (LLZTO) enrichment layer with high modulus is used to match the lithium anode and a polymer layer with high electrochemical stability is formed at the cathode. Meanwhile, a polyimide (PI) film is used as a scaffold to improve the mechanical properties of the electrolyte. As a result, the ACE with a thickness of 35 μm exhibits an ionic conductivity of 1.34×10−4 S cm−1 at room temperature. Furthermore, both the LiNi0.5Co0.2Mn0.3O2/ACE/Li and LiFePO4/ACE/Li full cells exhibit excellent electrochemical performances.
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