Self-standing graphitized hybrid Nanocarbon electrodes towards high-frequency supercapacitors

Carbon materials are considered as the ideal electrode materials for supercapacitors due to their diverse structure and nature. However, their poor frequency response is an obstacle to their application in high-frequency supercapacitors. Herein, an ultra-high temperature graphitization process at 2800 °C is proposed to fabricate carbon nanotubes/graphene hybrid films that are successfully employed as the electrode materials of high-frequency supercapacitors. By rational hybridization, the carbon nanotubes/graphene interlinked networks offer fast ion transport paths. Importantly, via a graphitization process at 2800 °C, the as-obtained hybrid films exhibit an ultrahigh in-plane conductivity of 491.81 S cm−1 and favorable out-plane conductivity of 27.98 mS cm−1. Such design brings the as-constructed high-frequency supercapacitors an unprecedented phase angle (up to −56.23°) and area capacitance (up to 230.56 μF cm−2) at 120 Hz, and their cut-off frequency can be nearly 30 times higher than that of films carbonization at 1600 °C. Such increases, further supported by density functional theory (DFT) calculations, are partly attributable to enhancements of ion response arising from the repair of edge defects of graphene. These findings will provide a new method in designing the structure of carbon electrodes for enhancing SCs frequency response performances.