Tuning Oxygen-Containing Functional Groups of Graphene for Supercapacitors with High Stability

To investigate the relationship between the oxygen-containing functional groups of graphene and the stability of supercapacitors, reduced graphene oxide (rGO) containing different oxygenic functional groups was prepared by varying the reduction time of GO using hydrazine as the reducing agent. TEM, XRD, Raman, and XPS characterizations revealed that, as the reduction time increased, the sp2 structure in the rGO sheet was restored and the obtained rGO had good crystallinity accompanied by removal of the oxygenic functional groups. The analysis of the content of the different functional groups also suggested that the reduction rate of the oxygenic functional group was C-O > C[double bond, length as m-dash]O > O-C[double bond, length as m-dash]O. The supercapacitive performance of rGO showed that the oxygenic functional groups contributed to some pseudocapacitance and resulted in a larger specific capacitance. At the same time, however, it is also accompanied by poorer rate performance and durability, which will be improved by removing the oxygenic functional groups by extending the reduction time. With an optimized reaction condition of a reduction time of 24 h, the obtained rGO exhibited excellent stability in floating tests at 3.0 V and 45 °C for 60 days. These findings pave the way for the development of high quality graphene materials for cost-effective and practical graphene supercapacitors.