Solid polymer electrolytes (SPEs) are urgently required for achieving practical all-solid-state lithium metal batteries (ASSLMBs) but remain plagued by low ionic conductivity. Herein, we propose a strategy of salt polarization to fabricate a highly ion-conductive SPE by employing a high-dielectric polymer that can interact strongly with lithium salts. Such a polymer with large dipole moments can guide lithium cations (Li+) to be arranged along the chain, forming a continuous pathway for Li+ hopping within the SPE. The as-fabricated SPE, poly(vinylidene difluoride) (PVDF)-LiN(SO2F)2 (LiFSI), has an extraordinarily high dielectric constant (up to 108) and ultrahigh ionic conductivity (0.77 × 10−3 S cm−1). Based on the PVDF–LiFSI SPE, the assembled Li metal symmetrical cell shows excellent Li plating/stripping reversibility at 0.1 mA cm−2, 0.1 mAh cm−2 over 1500 h; the ASS LiFePO4 batteries deliver long-term cycling stability at 1 C over 350 cycles (2.74 mg cm−2) and an ultralong cycling lifespan of over 2600 h (100 cycles) with high loading (11.5 mg cm−2) at 28 °C. First-principles calculations further reveal the ion-dipole interactions-controlled conduction of Li+ in PVDF–LiFSI SPE along the PVDF chain. This work highlights the critical role of dielectric permittivity in SPE, and provides a promising path towards high-energy, long-cycling lifespan ASSLMBs.

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