Synthesis of graphene oxides particle of high oxidation degree using a modified Hummers method

Abstract

High-oxidation-degree graphene oxide particles were synthesized using a modified Hummers' method. Six different types of particles were synthesized by varying the operating conditions, including the temperature, the reactant ratios, and the oxidation time. The oxidation degree, represented by the oxygen content, and the atomic oxygen/carbon (O/C) ratio were determined using CHNSO elemental analysis, X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy-universal attenuated total reflectance sensor (FTIR-UATR) and Raman spectroscopy. The structural morphology of graphene oxide was evaluated using scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The thermal stability of the particles was studied using thermogravimetric analysis (TGA). The SEM images showed that the prepared GO samples had different graphitic layer structures. The TEM images showed different stacking levels and transparency of GO flakes caused by the difference in oxidation level. The oxygen content and O/C ratios ranged between 34.7 and 50.0 wt% and 0.43 and 0.8, respectively. The highest oxygen content and O/C ratio were found to be 50 wt% and 0.8, respectively, for GO prepared at 95 °C with a 1-hr reaction time (GO2-a). A quantitative analysis on the FTIR-UATR spectra was performed and was in reasonable agreement with the CHNSO analysis results. The Raman spectra showed two characteristic bands (D and G) with different relative intensities, as characterized by the ID/IG ratio, suggesting that the prepared samples had different crystallite sizes and defects. The crystallite size (La) of the prepared GO particles was estimated using the Tuinstra-Koenig model and were ranging between 9 and 24 nm. The TGA results were correlated with the elemental analysis results and showed a clear dependence of the weight loss on the GO elemental compositions. GO2-a exhibited the lowest thermal stability because of a high oxygen content, whereas GO1-b exhibited the highest thermal stability.