Facile preparation of flexible binder-free graphene electrodes for high-performance supercapacitors

A facile two-step strategy to prepare flexible graphene electrodes has been developed for supercapacitors using thermal reduction of graphene oxide (GO) and thermally reduced graphene oxide (TRGO) composite films. The tunable porous structure of the GO/TRGO film provided channels to release the high pressure generated by CO₂ gas. The graphene electrode obtained from reduced-GO/TRGO (1 : 1 in mass ratio) film showed great flexibility and high film density (0.52 g cm⁻³). Using the EMI-BF₄ electrolyte with a working voltage of 3.7 V, the as-fabricated free-standing reduced-GO/TRGO (1 : 1) film achieved a great gravimetric capacitance of 180 F g⁻¹ (delivering a gravimetric energy density of 85.6 W h kg⁻¹), a volumetric capacitance of 94 F cm⁻³ (delivering a volumetric energy density of 44.7 W h L⁻¹), and a 92% retention after 10 000 charge/discharge cycles. In addition, the solid state flexible supercapacitor with the free-standing reduced-GO/TRGO (1 : 1) film as the electrodes and the EMI-BF₄/poly (vinylidene fluoride hexafluopropylene) (PVDF-HFP) gel as the electrolyte also demonstrated a high gravimetric capacitance of 146 F g⁻¹ with excellent mechanical flexibility, bending stability, and electrochemical stability. The strategy developed in this study provides great potentials for the synthesis of flexible graphene electrodes for supercapacitors.