Intrinsic Properties of GO/RGO Bilayer Electrodes Dictate Their Inter-/Intralayer Intractability to Modulate Their Capacitance Performance

[Image: see text] The demand for high-capacity energy storage along with high power output and faster charging has made supercapacitors a key area of energy research. The charge storage capacity of capacitors is largely dependent on the electrode materials utilized. To that end, graphene oxide (GO) and reduced GO (RGO) have been extensively employed for preparing supercapacitors. However, to date, no study has reported utilizing a GO/RGO bilayer electrode material for supercapacitor application. Herein, we report the synthesis of GO/RGO bilayer electrodes on fluorine-doped tin oxide (FTO) conducting substrates with four different combinations, namely, RGO-RGO, RGO-GO, GO-RGO, and GO-GO. Electrochemical capacitance analysis based on a symmetrical electrode configuration revealed that FTO-GO-RGO electrodes had the best areal capacitance performance. However, the highest specific areal capacitance (27.85 mF/cm(2)) for both symmetric/asymmetric configurations was achieved with FTO-GO-RGO as the anode and FTO-GO-GO as the cathode. The heterogeneous capacitance performance of the GO/RGO bilayer systems was analyzed based on structural characterization and computational simulation methods. Based on our analysis, we identified that inter-/intralayer molecular interaction of the GO/RGO bilayer sheets through the confinement pressure effect might have prompted their unique physicochemical properties. This work highlights the importance of probing multilayer GO/RGO electrode fabrication methods for preparation of high-capacity supercapacitors through fine-tuning their structural and molecular properties.