Iodine Adsorption in Nanoporous Carbon to Fabricate Assimilated Battery Electrodes for Durable Hybrid Supercapacitors

A hybrid supercapacitor is designed by coupling a battery electrode with a capacitive electrode in a single device/cell to enhance energy density. In iodine-based hybrid supercapacitors, the nanoporous carbon serves as the electrode material; however, the cathode or positive electrode is charged with iodine via electrodeposition from a redox aqueous electrolyte, while a negative electrode stores charges at the electric double-layer. In this work, iodine is loaded via physical adsorption into the porosity of a carbon electrode, keeping the aqueous electrolyte free from iodide redox moieties. By this way, the risk of polyiodide (I3- and I5-) generation at the positive electrode leading to a shuttling-related performance loss of the hybrid supercapacitor is prevented. Chemical interactions of iodine with the carbon surface and within the pores have been investigated with Raman spectroscopy, thermogravimetry and electron microscopy. Electrochemical methods have been used to test individual electrodes and hybrid supercapacitors in aqueous NaNO3 and aqueous LiTFSI at 5 mol/L concentration for performance parameters such as energy efficiency, capacitance, self-discharge and cyclability. The hybrid supercapacitor in aqueous LiTFSI exhibits stable capacitance and energy efficiency during long-term aging tests at 1.5 V. Carbon nanoarchitecturing with iodine as shown in the present work offers an economical approach to enhance the performance of hybrid supercapacitors.