ABSTRACT
The presence of oxygen-containing functional groups on the basal plane and at the edges endows graphene oxide (GO) with an insulating nature, which makes it rather unsuitable for electronic applications. Fortunately, the reduction process makes it possible to restore the sp2 conjugation. Among various protocols, chemical reduction is appealing because of its compatibility with large-scale production. Nevertheless, despite the vast number of reported chemical protocols, their comparative assessment has not yet been the subject of an in-depth investigation, rendering the establishment of a structure-performance relationship impossible. We report a systematic study on the chemical reduction of GO by exploring different reducing agents (hydrazine hydrate, sodium borohydride, ascorbic acid (AA), and sodium dithionite) and reaction times (2 or 12 hours) in order to boost the performance of chemically reduced GO (CrGO) in electronics and in electrochemical applications. In this work, we provide evidence that the optimal reduction conditions should vary depending on the chosen application, whether it is for electrical or electrochemical purposes. CrGO exhibiting a good electrical conductivity (>1800 S m-1) can be obtained by using AA (12 hours of reaction), Na2S2O4 and N2H4 (independent of the reaction time). Conversely, CrGO displaying a superior electrochemical performance (specific capacitance of 211 F g-1, and capacitance retention >99.5% after 2000 cycles) can be obtained by using NaBH4 (12 hours of reaction). Finally, the compatibility of the different CrGOs with wearable and flexible electronics is also demonstrated using skin irritation tests. The strategy described represents a significant advancement towards the development of environmentally friendly CrGOs with ad hoc properties for advanced applications in electronics and energy storage.
ABSTRACT
Carbon nanostructures are utilized in a plethora of applications ranging from biomedicine to electronics. Particularly interesting are carbon nanostructured quantum dots that can be simultaneously used for bimodal therapies with both targeting and imaging capabilities. Here, magnetic and optical properties of graphene oxide quantum dots (GOQDs) prepared by the top-down technique from graphene oxide and obtained using the Hummers' method were studied. Graphene oxide was ultra-sonicated, boiled in HNO3, ultra-centrifuged, and finally filtrated, reaching a mean flake size of ~30 nm with quantum dot properties. Flake size distributions were obtained from scanning electron microscopy (SEM) images after consecutive preparation steps. Energy-dispersive X-ray (EDX) confirmed that GOQDs were still oxidized after the fabrication procedure. Magnetic and photoluminescence measurements performed on the obtained GOQDs revealed their paramagnetic behavior and broad range optical photoluminescence around 500 nm, with magnetic moments of 2.41 µB. Finally, electron paramagnetic resonance (EPR) was used to separate the unforeseen contributions and typically not taken into account metal contaminations, and radicals from carbon defects. This study contributes to a better understanding of magnetic properties of carbon nanostructures, which could in the future be used for the design of multimodal imaging agents.
