Enhancing Interfacial Lithiophilicity and Stability with PVDF/In(NO3)3 Composite Separators for Durable Lithium Metal Anodes

Abstract

Separator modification is a promising method for advancing lithium metal anodes; however, achieving homogeneous lithium-ion flux and uniform plating/stripping processes remains challenging. In this work, we introduce a novel approach by developing a composite separator, termed PVDF-INO, which integrates In(NO3)3 (INO) into polyvinylidene fluoride (PVDF) to create a 12 μm thick layer. This addition significantly enhances the interaction between the separator and the electrolyte, creating a lithophilic matrix that ensures an even distribution of lithium ions. This uniform ion distribution promotes consistent lithium deposition and dissolution, resulting in a durable, dendrite-free lithium metal anode. Moreover, the PVDF-INO separator not only enhances the affinity with electrolytes but also maintains stable lithium-ion flux, which is essential for reliable and safe battery operation. Consequently, it sustains operation over 750 h in a Li||Li symmetric battery configuration, with a low overpotential of just 28 mV. Additionally, full cells equipped with LiFePO4 cathodes and the PVDF-INO separator exhibit superior cycling performance, maintaining a capacity retention of 92.9% after 800 cycles at 1 C. This work paves the way for significant advancements in the field of lithium metal batteries, offering a promising solution to longstanding energy storage challenges.