Uniform Lithium Plating for Dendrite-Free Lithium Metal Batteries: Role of Dipolar Channels in Poly(vinylidene fluoride) and PbZr<sub><i>x</i></sub>Ti<sub>1-<i>x</i></sub>O<sub>3</sub> Interface.
basic_science · Level V
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- Record sourced from PubMed, PMID 37405783.
- Also identified by DOI 10.1021/acsnano.3c04684.
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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)-PbZr<sub><i>x</i></sub>Ti<sub>1-<i>x</i></sub>O<sub>3</sub> (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<sup>+</sup>) at the PVDF-PZT interface to transport through dipolar channels and promotes the dissociation of lithium salts into free Li<sup>+</sup>. 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<sup>-2</sup> at 25 °C, outperforming Li/PVDF solid-state electrolyte/Li cells that fail after 120 h. The LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mo<sub>0.1</sub>O<sub>2</sub>/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<sup>+</sup> transport mechanism and inhibiting dendrite growth.