On the Origin of the Enhanced Supercapacitor Performance of Nitrogen-Doped Graphene

Abstract

Graphene-based electrodes have been widely tested and used in electrochemical double layer capacitors due to their high surface area and electrical conductivity. Nitrogen doping of graphene has recently been demonstrated to significantly enhance capacitance, but the underlying mechanisms remain ambiguous. We present the doping effect on the interfacial capacitance between graphene and [BMIM][PF 6 ] ionic liquid, particularly the relative changes in the double layer and electrode (quantum) capacitances. The electrode capacitance change was evaluated based on density functional theory calculations of doping-induced electronic structure modifications in graphene, while the microstructure and capacitance of the double layers forming near undoped/ doped graphene electrodes were calculated using classical molecular dynamics. Our computational study clearly demonstrates that nitrogen doping can lead to significant enhancement in the electrode capacitance as a result of electronic structure modifications while there is virtually no change in the double layer capacitance. This finding sheds some insight into the impact of the chemical and/or mechanical modifications of graphene-like electrodes on supercapacitor performance.

On the influence of polarization effects in predicting the interfacial structure and capacitance of graphene-like electrodes in ionic liquids

“…[22][23][24][25][26][27] The quantum capacitance is related to the electronic density of states (DOS), which can be evaluated using quantum mechanical calculations. Prior efforts have typically evaluated the DOS of the electrode in the absence of the electrolyte.…”

Sustainable process for all-carbon electrodes: Horticultural doping of natural-resource-derived nano-carbons for high-performance supercapacitors

“…S6. Our CV curves show that all the doped VGNS exhibit broad and weak redox peaks in regions 0.4-0.5 V and À0.3 V. These correspond to the redox reactions related to nitrogen and oxygen functional groups [31,51].…”

Nitrogen-Doped Graphene Materials for Supercapacitor Applications

“…Schematic of (a) the substitutional nitrogen site (N1) and (b) the trimerized pyridine-type nitrogen site (N3V) considered in this work. Gray and blue balls are C and N atoms, respectively, and bond lengths are given in Å. Reprinted with permission from [127], E. Paek, et al, J. Phys. Chem.…”