In this paper, we presented a hybrid composite of graphene quantum dots (GQDs)-modified three-dimensional graphene nanoribbons (3D GNRs) composite linked by Fe3O4 and CoO nanoparticles through reflux and ultrasonic treatment with GQDs, denoted as 3D GQDs-Fe3O4/CoO@GNRs (3D GFCG). In this hybrid, the 3D GNRs framework strengthened the electrical conductivity and the synergistic effects between GQDs and 3D GFCG enhanced the oxygen reduction reaction (ORR) activity of the nanocomposite. The results imply that decorating GQDs with other electro-catalysts is an effective strategy to synergistically improve their ORR activity.

As frontier materials, graphene oxide (GO) and graphene have penetrated almost all research areas and advanced numerous technologies in sensing, electronics, energy storage, catalysis, water treatment, advanced composites, biomedical, and more. However, the affordable large-scale synthesis of high-quality GO and graphene remains a significant challenge that negatively affects its commercialisation. In this article, firstly, a simple, scalable approach was demonstrated to synthesise high-quality, high yield GO by modifying the improved Hummers method. The advantages of the optimised process are reduced oxidation time, straightforward washing steps without using coagulation step, reduction in cost as eliminating the use of phosphoric acid, use of minimum chemical reagents, and increased production of GO per batch (~ 62 g). Subsequently, the produced GO was reduced to reduced graphene oxide (rGO) using three different approaches: green reduction using ascorbic acid, hydrothermal and thermal reduction techniques. The GO and rGO samples were characterised using various microscopy and spectroscopy techniques such as XRD, Raman, SEM, TEM, XPS and TGA. The rGO prepared using different methods were compared thoroughly, and it was noticed that rGO produced by ascorbic acid reduction has high quality and high yield. Furthermore, surface (surface wettability, zeta potential and surface area) and electrical properties of GO and different rGO were evaluated. The presented synthesis processes might be potentially scaled up for large-scale production of GO and rGO.

The reduced graphene oxide (rGO) has attracted more and more attention in recent years. How to choose a suitable reduction method to prepare rGO is a critical problem in the preparation of graphene composites. In this work, the differences of rGO reduced by thermal, microwave, Ultraviolet (UV) and reducing agent were studied. The reduction degree and functional groups of rGO were compared by SEM, XPS, Raman, FTIR and TGA. Thermal can remove most of the oxygen-containing groups of graphene oxide (GO) and the thermal reduction is the most effective reduction method. UV light can directly act on the unstable oxygen-containing groups, and its reduction efficiency is second only to thermal reduction. The efficiency of chemical reduction is not as good as that of UV reduction, because the reducing agent only act on the surface of GO. Microwave reduction is a mild thermal reduction with the lowest efficiency, but the residual oxygen-containing groups increase the hydrophilicity of rGO. To sum up, this work studies that rGO prepared by different reduction methods has different characteristics, which provides a reference for selecting appropriate reduction methods to prepare graphene composites with better properties.

Lately, Raman spectroscopy has become powerful tool for quality assessment of graphene analogues with identification of intensity ratio of Raman active D-band and G-band ( ID/IG ratio) as a vital parameter for quantification of defects. However, during chemical reduction of graphitic oxide (GrO) to reduced GrO (RGrO), the increased ID/ IG ratio is often wrongly recognized as defect augmentation, with “formation of more numerous yet smaller size sp2 domains” as its explanation. Herein, by giving due attention to normalized peak height, full-width half-maxima and integrated peak area of Raman D- and G-bands, and compliment the findings by XRD data, we have shown that in-plane size of sp2 domains actually increases upon chemical reduction. Particularly, contrary to increased ID/ IG ratio, the calculated decrease in integrated peak area ratio ( AD/AG ratio) in conjunction with narrowing of D-band and broadening of G-band, evinced the decrease in in-plane defects. Finally, as duly supported by reduction induced broadening of interlayer-spacing characteristic XRD peak and narrowing of ~ 43° centered XRD hump, we have also shown that the sp2 domains actually expands in size and the observed increase in ID/ IG ratio is indeed due to increase in across-plane defects, formed via along-the-layer slicing of graphitic domains.

We studied the basic properties and fabrication of reduced graphene oxide (rGO) prepared using eco-friendly reduction agents in the graphene solution process. Hydrazine is generally used to reduce graphene oxide (GO), which results in polluting emissions as well as fixed nitrogen functional groups on different defects in the graphene sheets. To replace hydrazine, we developed eco-friendly reduction agents with similar or better reducing properties, and selected of them for further analysis. In this study, GO layers were produced from graphite flakes using a modified Hummer’s method, and rGO layers were reduced using hydrazine hydrate, L-ascorbic acid, and gluconic acid. We measured the particle sizes and the dispersion stabilities in the rGO dispersed solvents for the three agents and analyzed the structural, electrical, and optical properties of the rGO films. The results showed that the degree of reduction was in the order L-ascorbic acid ≥ hydrazine > glucose. GO reduced using L-ascorbic acid had a sheet resistance of 121 kΩ/sq, while that reduced using gluconic acid showed worse electrical properties than the other two reduction agents. Therefore, L-ascorbic acid is the most suitable eco-friendly reduction agent that can be substituted for hydrazine.

A highly facile and eco-friendly green synthesis of Annona squamosa (custard apple) leaf extract reduced graphene oxide (CRG) nanosheets was achieved by the reduction of graphene oxide (GO). The as-prepared CRG was characterized with X-ray diffraction (XRD), transmission electron microscope (TEM), Fourier-transform infrared spectroscopy (FT-IR), ultraviolet-visible (UV-Vis), X-ray photoelectron spectroscopy (XPS) and Raman spectroscopic techniques. Removal of oxygen containing moieties from the GO was confirmed by UV-Vis, FT-IR and XPS spectroscopic data. The XRD and Raman data further confirmed the formation of the CRG. TEM images showed the sheet structure of the synthesized CRG. These results show that the phytochemicals present in custard apple leaf extract act as excellent reducing agents. The CRG showed good dispersion in water.

We report the preparation of sulfonated reduced graphene oxide (SRGO) by the sulfonation of graphene oxide followed by radiation-induced chemical reduction. Graphene oxide prepared by the well-known modified Hummer's method was sulfonated with the aryl diazonium salt of sulfanilic acid. Sulfonated graphene oxide (SGO) dispersed in ethanol was subsequently reduced by γ-ray irradiation at various absorbed doses to produce SRGO. The results of optical, chemical, and thermal analyses revealed that SRGO was successfully prepared by γ-ray irradiation-induced chemical reduction of the SGO suspension. Moreover, the electrical conductivity of SRGO was increased up to 2.94 S/cm with an increase of the absorbed dose.

A novel strategy for the simultaneous reduction and functionalization of graphene oxide (G-O) was developed using polyallylamine hydrochloride (PAAH) as a multi-functional agent. The G-O functionalization by PAAH was carried out under basic conditions to catalyze the epoxide ring opening reaction of G-O with abundant amine groups of PAAH. We found that G-O was not only functionalized with PAAH but also reduced under the reaction condition. Moreover, the synthesized PAAH-functionalized G-O sheets were soluble in water and applicable to the synthesis of nanocomposites with gold nanoparticles.