High performance supercapacitor using N-doped graphene prepared via supercritical fluid processing with an oxime nitrogen source

•N-functionalised graphene synthesized via supercritical fluid processing.•DMG, an oxime based nitrogen precursor.•Maximum specific capacitance of 286 F/g at 0.5 A/g in aqueous solution.•Pyridinic as well as quarternary nitrogen for enhanced capacitance.

Heteroatom doped graphene has been proved for its promising applications in electrochemical energy storage systems. Here, nitrogen (N) doped graphene was prepared via two different techniques namely supercritical fluid assisted processing and hydrothermal heat treatment using dimethylglyoxime (DMG) as an oxime nitrogen precursor. The FT-IR and Raman spectra showed the N-containing functional group in the graphene. The XRD analysis revealed the complete reduction of graphene oxide during the supercritical fluid processing. The elemental analysis and X-ray photoelectron spectroscopy revealed the amount and nature of N-doping in the graphene, respectively. The surface morphology and physical nature of the samples were analyzed using scanning and transmission electron microscopic analysis. The electrochemical performance of prepared electrode materials was evaluated using cyclic voltammetry, galvanostatic charge-discharge analysis and electrochemical impedance spectroscopy. The N-doped graphene prepared via supercritical fluid assisted processing exhibit enhanced capacitive behaviour with a maximum specific capacitance of 286 F g−1 at a current density of 0.5 A/g. The cycling studies showed 98% specific capacity retention with 100% coulombic efficiency over 1000 cycles at 5 A/g. The enhanced specific capacitance of N-doped graphene prepared via supercritical fluid heat treatment over the hydrothermal heat treatment is ascribed to the nature of N-doping in the graphene.

Graphical abstractN-doped graphene prepared via supercritical fluid processing with oxime nitrogen source (DMG) showed enhanced performance in electrochemical supercapacitor application. A maximum specific capacitance of 286 F g−1 at a current density of 0.5 A/g was achieved with a high specific capacity retention of 98% after 1000 cycles at 5 A/g.Figure optionsDownload full-size imageDownload as PowerPoint slide