Graphene quantum dots (GQDs) with uniform sizes of less than 5 nm are synthesized by a novel top-down strategy. Nitric acid as a strong oxidant can be used to cut graphene oxide via sonication and hydrothermal processes. Moreover, purified GQDs are obtained from removing oxygen-containing functional groups in a heat treatment process. Both nanoscale size and edge effect of GQDs improve their abundant active sites and restrain the restack of graphene nanosheets. Meanwhile, their electrochemical performance demonstrates the properties of the GQDs for practical application in energy storage. The GQD electrode material shows an ideal electric double-layer capacitance behavior such as a high specific capacitance of 296.7 F g, a satisfactory energy density of 41.2 W h kg at 1 A g, a low internal resistance, a small relaxation time, and an excellent cycling stability. The results illustrate excellent electrochemical activity, high conductivity, and enhanced ion transport rate on the surface of electrolyte and electrode. The advantages of GQDs confirm their unique characteristics for potential applications in the field of electrode materials for supercapacitors.

The effects of five types of oxygen-containing functional groups (–COOH, –COC–, –OH, –CHO, and –OCH3) on graphene quantum dots (GQDs) are investigated using time-dependent density functional theory (TD-DFT).

The effects of four heteroatoms (B, N, P, and S) with three doping patterns on graphene quantum dots (GQDs) are systematically investigated using time-dependent density functional theory (TD-DFT). The absorption spectra and HOMO-LUMO gaps are quantitatively analyzed to study the correlations between the optical properties and heteroatom doping of doped GQDs. Heteroatom doping can endow GQDs with various new optical and structural properties, depending on the dopants and doping configurations. Compared with the absorption spectra of pristine GQD, both N and S surface doping demonstrate a slight blue shift, whereas B and P doping lead to a blue shift for edge-doped GQDs with heteroatoms in a pentatomic ring. The absorption process is investigated along with excited state analysis, which includes the density of state, natural transition orbital, and charge difference density. The results indicate that large radius atoms assist charge transfer in the excited state and play an important role in recombining the electron density distribution in the doped GQDs.