Novel nanoarchitecture of 3D ion transfer channel containing nanocomposite solid polymer electrolyte membrane based on holey graphene oxide and chitosan biopolymer

In the arena of three-dimensional (3D) nanoarchitecture, holey graphene oxide (HGO)—a class of two-dimensional (2D) graphene oxide porous nanosheet, has emerged as a promising choice of additive material to design advanced 3D nanocomposite for energy and environmental applications. With a facile and cost-effective solution-casting technique, we fabricated here a flexible, wearable, free-standing, and super-thin (∼0.08 mm) solid polymer electrolyte membrane (SPEM) consisting of 2D-HGO, lithium bis(trifluromethanesulfonyl)imide (LiTFSI) salt, polyvinylpyrrolidone (PVP) polymer binder, and chitosan (CH) biopolymer. SPEM exhibited impressive ionic conductivity of 2.76 × 10-3 S⋅cm−1 at room temperature (RT = 23 °C) which is comparable to liquid electrolytes. Robust mechanical property (5.87 MPa) and easy lithium-ion diffusion capability of SPEM were identified by the ultra-low activation energy (Ea) of 0.089 eV, which is one of the best values among the reported solid polymer electrolytes. Good lithium-ion transference number (tLi+= 0.76) and wide electrochemical stability window (ESW = 4.4) indicated single ion conduction and stable battery operation voltage capability of SPEM. Moreover, fast ion transfer mechanism of SPEM was proposed according to the comprehensive characterizations; mostly relating to uniform and strong interconnecting novel 3D ion transferring routes. Temperature and frequency responsive charge carrier mobility trend were also investigated with an in-depth dielectric study. Promising RT galvanostatic Li plating-stripping performance was observed at 5 mA⋅cm−2 with a hybrid symmetric cell. Using Li metal as anode, SPEM, and LiCoO2 as cathode in the full cell, a good RT specific discharge capacity of 142.8 mA⋅h⋅g−1 was achieved at 0.1 C rate.