Mechanically Robust Gel Polymer Electrolyte for an Ultrastable Sodium Metal Battery

Sodium dendrite growth is responsible for short circuiting and fire hazard of metal batteries, which limits the potential application of sodium metal anode. Sodium dendrite can be effectively suppressed by applying mechanically robust electrolyte in battery systems. Herein, a composite gel polymer electrolyte (GPE) is designed and fabricated, mainly consisting of graphene oxide (GO) and polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP). With the addition of an appropriate amount of GO content, the compressive Young's modulus of 2 wt% GO+PVDF-HFP (2-GPH) composite GPE is greatly enhanced by a factor of 10, reaching 2.5 GPa, which is crucial in the suppression of sodium dendrite growth. As a result, uniform sodium deposition and ultralong reversible sodium plating/stripping (over 400 h) at high current density (5 mA cm^-2 ) are achieved. Furthermore, as evidenced by molecular dynamics simulation, the GO content facilitates the sodium ion transportation, giving a high ionic conductivity of 2.3 × 10^-3 S cm^-1 . When coupled with Na₃ V₂ (PO₄ )₃ cathode in a full sodium metal battery, a high initial capacity of 107 mA h g^-1 at 1 C (1 C = 117 mA g^-1 ) is recorded, with an excellent capacity retention rate of 93.5% and high coulombic efficiency of 99.8% after 1100 cycles.