Uniform Lithium Plating for Dendrite-Free Lithium Metal Batteries: Role of Dipolar Channels in Poly(vinylidene fluoride) and PbZrxTi1-xO3 Interface.

Abstract

Conventional polymer/ceramic composite solid-state electrolytes (CPEs) have limitations in inhibiting lithium dendrite growth and fail to meet the contradictory requirements of anodes and cathodes. Herein, an asymmetrical poly(vinylidene fluoride) (PVDF)-PbZrxTi1-xO3 (PZT) CPE was prepared. The CPE incorporates high dielectric PZT nanoparticles, which enrich a dense thin layer on the anode side, making their dipole ends strongly electronegative. This attracts lithium ions (Li+) at the PVDF-PZT interface to transport through dipolar channels and promotes the dissociation of lithium salts into free Li+. Consequently, the CPE enables homogeneous lithium plating and suppresses dendrite growth. Meanwhile, the PVDF-enriched region at the cathode side ensures intermediate contact with positive active materials. Therefore, Li/PVDF-PZT CPE/Li symmetrical cells exhibit a stable cycling performance exceeding 1900 h at 0.1 mA cm-2 at 25 °C, outperforming Li/PVDF solid-state electrolyte/Li cells that fail after 120 h. The LiNi0.8Co0.1Mo0.1O2/PVDF-PZT CPE/Li cells show low interfacial impedances and maintain stable cycling performance for 500 cycles with a capacity retention of 86.2% at 0.5 C and 25 °C. This study introduces a strategy utilizing dielectric ceramics to construct dipolar channels, providing a uniform Li+ transport mechanism and inhibiting dendrite growth.