Significant Reduction in Interface Resistance and Super-Enhanced Performance of Lithium-Metal Battery by In Situ Construction of Poly(vinylidene fluoride)-Based Solid-State Membrane with Dual Ceramic Fillers

Due to the degradation of lithium-metal anode, lithium dendritic growth and other challenging problems like interface resistance among electrolyte and electrode may damage the actual performance of lithium-metal batteries (LMB). Recently, ceramic nanofillers Li_1.3Al_0.3Ti_1.7P­(O₄)₃ (LATP) and Li_0.33La_0.557TiO₃ (LLTO) seem to be suitable solid-state electrolytes for lithium metallic solid-state batteries with outstanding energy densities and highly safer energy storage devices. Herein, the solid-state electrolytic materials are composed of a fast ion-conducting solid-state LATP, LLTO, and optimized amount of adequate polarized poly­(vinylidene fluoride) (PVDF) electrolyte with lithium salt (LiClO₄) to fabricate the dual semi-solid-state polymer electrolyte (DSPE) membrane. The prepared membrane provides a promising solution for battery safety and the most challenging problems of interface resistance. The proposed DSPE membrane is investigated via analytical techniques; testing results showed that the DSPE membrane possesses excellent electrochemical performance, including suitable Li-transference numbers and improved ionic conductivities with enhanced stability. Furthermore, the DSPE membrane is beneficial to resist the growth of Li dendrites effectively. The symmetrical cell Li//DSPE//Li exhibits excellent stability at a high current density of 1 mA/cm² over 1000 h, and the membrane sustains long-cycle performance with a high retention of 95% after 100 cycles. The designed DSPE membrane opens a path of fabricating a safe electrolyte membrane for elevated temperature metal-ion battery applications.