Abstract

The energy storage capability of the aqueous supercapacitors is mainly attributed to the relatively low operating voltage of the device, as the thermodynamic decomposition voltage of water is 1.23 V. Therefore, the extension of the working voltage of the aqueous capacitor beyond the electrolyte decomposition limit is an important subject for the development of environmentally friendly energy storage devices. In this study, a commercial activated carbon (AC) and synthesized phosphorus-doped reduced graphene oxide (P-rGO) were used to gain insight into the influence of both textural properties and the surface chemistry on the electrochemical performance of high-voltage aqueous supercapacitors. Materials on the opposite end of the spectrum (highly porous, undoped AC and heteroatom-rich phosphorus-doped reduced graphene oxide with low porosity) were compared in a symmetric cell, operating in a wide voltage window of 2.0 V in 2 M NaClO4 electrolyte. Additionally, AC-based cell was tested in 1 M Na2SO4 solution to assess the differences in its performance in different sodium-based electrolytes. The obtained results demonstrate that both a porous structure and high contribution of heteroatoms, which improve the hydrophilicity of the electrode, are required to achieve high specific energy density values. However, with increasing current and higher power densities, a developed porous structure is required to maintain good energy storage characteristics. Achieving high operating voltage in the aqueous symmetric full-carbon supercapacitors is a promising energy storage solution. The assembled devices show a good specific energy density of up to 13 Wh kg−1 at a power density of 30 W kg−1.Graphical abstract

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