Herein, we report a straigthforward procedure to prepare an excellent intertwined nanosponge solid-state polymer electrolyte (INSPE) for highly bendable, rollable, and foldable lithium-ion batteries (LIBs). The mechanically reliable and electrochemically superior INSPE is conjugated with intertwined nanosponge (IN) poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-co-HFP) and ion-conducting polymer electrolyte (PE) containing poly(ethylene glycol) diacrylate (PEGDA), succinonitrile (SCN) plasticizer, and lithium bis(trifluoromethanesilfonyl)imide (LiTFSI). The conjugated INSPE has both high strength with great flexibility (tensile strength of 2.1 MPa, elongation of 36.7%), and excellent ionic conductivity (1.04 × 10-3 S·cm-1, similar to the values of liquid electrolytes). As a result of such special combination, the as-prepared INSPE retains almost 100% of its ionic conductivity when subjected to many types of severe mechanical deformations. Therefore, the INSPE is successfully applied to bendable, rollable, and foldable LIBs that show excellent energy storage performance despite the intense mechanical deformations.
Keywords: foldable; intertwined nanosponge; lithium-ion battery; rollable; solid-state polymer electrolyte.