Hybrid multilayer thin film supercapacitor of graphene nanosheets with polyaniline: importance of establishing intimate electronic contact through nanoscale blending

A hybrid electrode consisting of an electric double-layer capacitor of graphene nanosheets and a pseudocapacitor of the conducting polymer polyaniline exhibits a synergistic effect with excellent electrochemical performance for flexible thin film supercapacitors. This hybrid supercapacitor is constructed by a nanoscale blending method of layer-by-layer (LbL) assembly based on the electrostatic interactions between positively charged polyaniline (PANi) and negatively charged graphene oxide (GO) nanosheets. The hybrid electrode provides not only improved electronic conductivity through the intimate contact with the graphene nanosheet, but also enhanced chemical stability during the charge-discharge process. We also investigated the dependence of the electrochemical performance on the various parameters of LbL assembly such as the number of bilayers and the post-thermal and chemical treatments that could affect the degree of reduction of GO and PANi. We found that after thermal treatment, the LbL-assembled thin film of PANi with GO nanosheets exhibited an excellent gravimetric capacitance of 375.2 F g(-1) at a discharge current density of 0.5 A g(-1) that outperformed many other hybrid supercapacitors reported to date. The hybrid supercapacitor maintained its capacity up to 90.7% over 500 cycles at a high current density of 3.0 A g(-1). This study opens up the possibility for the production of diverse graphene-based hybrid nanocomposites that are promising for future flexible supercapacitors.