Tailorable Synthesis of Highly Oxidized Graphene Oxides via an Environmentally-Friendly Electrochemical Process

Graphene oxide (GO) is an attractive alternative to graphene for many applications due to its captivating optical, chemical, and electrical characteristics. In this work, GO powders with a different amount of surface groups were synthesized from graphite via an electrochemical two-stage process. Many synthesis conditions were tried to maximize the oxidation level, and comprehensive characterization of the resulting samples was carried out via elemental analysis, microscopies (TEM, SEM, AFM), X-ray diffraction, FT-IR and Raman spectroscopies as well as electrical resistance measurements. SEM and TEM images corroborate that the electrochemical process used herein preserves the integrity of the graphene flakes, enabling to obtain large, uniform and well exfoliated GO sheets. The GOs display a wide range of C/O ratios, determined by the voltage and time of each stage as well as the electrolyte concentration, and an unprecedented minimum C/O value was obtained for the optimal conditions. FT-IR evidences strong intermolecular interactions between neighbouring oxygenated groups. The intensity ratio of D/G bands in the Raman spectra is high for samples prepared using concentrated H₂SO₄ as an electrolyte, indicative of many defects. Furthermore, these GOs exhibit smaller interlayer spacing than that expected according to their oxygen content, which suggests predominant oxidation on the flake edges. Results point out that the electrical resistance is conditioned mostly by the interlayer distance and not simply by the C/O ratio. The tuning of the oxidation level is useful for the design of GOs with tailorable structural, electrical, optical, mechanical, and thermal properties.