Scaffold-engineered PVDF–graphene oxide membranes for gel and quasi-solid electrolytes in lithium metal batteries

In this study, asymmetric polyvinylidene fluoride (PVDF) membranes incorporating graphene oxide (GO) are developed as multifunctional electrolyte scaffolds for both gel and quasi-solid-state lithium metal batteries. Introduction of GO is found to enhance β-phase crystalline of PVDF, thereby improving the ion transport properties. At an optimal loading, the GO-modified PVDF (PVDF-GO 100 ) membrane achieves a favourable performance, including low interfacial resistance, high Li + transference number, and reduced nucleation overpotential, which collectively promote uniform Li deposition and suppress dendrite growth. In Li||LiFePO 4 full cells, gel electrolytes based on PVDF-GO 100 enable excellent rate capability of 100 mAh g -1 at 10 C and 80% capacity retention after 300 cycles at 0.5 C. When employed as a porous scaffold for in-situ polymerization of 1,3-dioxolane (DOL), the resulting PVDF-GO 100 -polyDOL quasi-solid electrolyte further demonstrates superior cycling performance, maintaining 77 mAh g -1 at 10 C and 77% capacity retention after 300 cycles under 0.5 C at room temperature. These findings highlight GO-modified PVDF membranes as a versatile and durable platform for high-performance gel and quasi-solid-state lithium metal batteries with enhanced stability and prolonged cycle life. • Asymmetric PVDF-GO membranes are engineered as multifunctional scaffolds. • GO promotes β-phase PVDF formation and boosts Li + transport properties. • Li||LFP cells with PVDF-GO gel electrolytes deliver 100 mAh g -1 at high rate of 10 C. • Li||LFP cells with PVDF-GO gel electrolytes retain 80% capacity after 300 cycles at 0.5 C. • PVDF-GO-polyDOL quasi-solid cells outperform PVDF-polyDOL in cycling durability.