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Technical breakthrough of composite polymer electrolyte (CPE) is one of the key factors that determines the commercial process of the current solid-state lithium battery. However, high interface impedance limits its electrochemical performances. It is crucial to optimize the design of multiphase interfaces among different components in CPE for regulating Li+ transport. Herein, a multi-affinity self-assembled 12-crown-4-TFSI (12C4-TFSI) supramolecular nanolayer is introduced into poly(vinylidene difluoride)-Li6.75La3Zr1.75Ta0.25O12 (PVDF-LLZTO) CPE as interface modifier. As a result, enhanced Li+ conductivity of 4.29 × 10−4 S·cm−1, Li+ transfer number of 0.44, and stable electrochemical window voltage of 4.8 V vs. Li/Li+ at 30 °C are obtained. The symmetric Li||Li cell exhibits an improved critical current density (CCD) of 1.2 mA·cm−2 and steady cycling at 0.2 mA·cm−2 for over 850 h without visible voltage fluctuation. The assembled LiǁLiFePO4 coin solid-state cell delivers a high initial discharge capacity of 172.9 mAh·g−1 at 0.1 C, rate capability (up to 5.0 C) and outstanding cycling stability with a capacity retention of 87.2% after over 750 cycles at 1.0 C. The associated LiǁLiFePO4 pouch cell presents an initial specific discharge capacity of 112.3 mAh·g−1 and successfully runs 30 cycles with a final capacity of 101.8 mAh·g−1. This work offers a facile strategy to optimize multiphase interfaces of PVDF-LLZTO CPE for stable solid-state lithium battery.
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