Electrochemical performance improvement of N-doped graphene as electrode materials for supercapacitors by optimizing the functional groups

Abstract

Graphene material prepared by reducing graphene oxide (GO, prepared by the modified Hummers method) has been considered as one of the most promising candidates for electrode materials for supercapacitors due to its mass producibility, high electrical conductivity, large specific surface area, and superior mechanical strength. However, it usually exhibits an unfavorable cycling performance, mainly large capacitance fading in the initial thousands of cycles, as shown but not discussed in some previous reports. In this paper, we not only find a similar phenomenon to a commercial graphene material, but also develop a very simple method to successfully enhance its electrochemical properties in terms of cycle life as well as high-rate performance, leakage current and alternating current impedance. For example, the relatively low capacitance retention of about 89.9% at the initial 1000^th cycle was increased up to 99.7% after improvement, the capacitance retention was raised to 73% from 43% at a scan rate of 100 mV s⁻¹ in cyclic voltammetry, and leakage current density was significantly more than halved (from 2.42 mA g⁻¹ to 1.01 mA g⁻¹). Additionally, the reasons for the improvement are also disclosed by analyzing the characterization results of X-ray photoelectron spectroscopy, electrochemical impedance spectroscopy, X-ray diffraction, Fourier transform infrared spectroscopy and Raman spectroscopy. It is found that the optimization of the functional groups of doped nitrogen and oxygen atoms may contribute to the improvement of cycle life and decrease of leakage current density, and the enhanced rate performance can be attributed to the increase of electrical conductivity.