The development of superconcentrated or water-in-salt electrolytes (WISEs) has paved a new way toward realizing environmentally friendly, nonflammable batteries and supercapacitors based on aqueous electrolytes. The development of new electrolytes, such as WISEs, needs to be accompanied by further studies of the charging mechanism. This is essential to guide the choice of the electrode/electrolyte pairs for optimizing the performance of WISE-based supercapacitors. Therefore, to optimize the performance of carbon/carbon supercapacitors when using new, superconcentrated electrolytes, we present a detailed investigation of the carbon/electrolyte interface by combining electrochemical measurements with Raman and NMR spectroscopy and mass spectrometry. In particular, NMR provides crucial information about the local environment of electrolyte ions inside the carbon pores of the electrode. The results show that the structure of the electrolyte strongly depends on the concentration of the electrolyte and affects the mechanism of charge storage at the positive and negative electrodes.
Keywords: aqueous supercapacitors; carbon/carbon supercapacitors; charge storage mechanism; concentration effect; electrode/electrolyte interface; electrolyte structures; highly concentrated electrolytes; water-in-salt electrolytes.