Graphene oxide (GO) and reduced graphene oxide (rGO) have congregated much interest as promising active materials for a variety of applications such as electrodes for supercapacitors. Yet, partially given the absence of comparative studies in synthesis methodologies, a lack of understanding persists on how to best tailor these materials. In this work, the effect of using different graphene oxidation-reduction strategies in the structure and chemistry of rGOs is systematically discussed. Two of the most popular oxidation routes in the literature were used to obtain GO. Subsequently, two sets of rGO powders were synthesised employing three different reduction routes, totalling six separate products. It is shown that the extension of the structural rearrangement in rGOs is not just dependent on the reduction step but also on the approach followed for the initial graphite oxidation.
The impact of post-synthesis processing in reduced graphene oxide materials for supercapacitor electrodes has been analyzed. A comparative study of vacuum, freeze and critical point drying was carried out for hydrothermally reduced graphene oxide demonstrating that the optimization of the specific surface area and preservation of the porous network are critical to maximize its supercapacitance performance. As described below, using a supercritical fluid as the drying medium, unprecedented values of the specific surface area (364 m g) and supercapacitance (441 F g) for this class of materials have been achieved.
Research in the field of aluminum batteries has focused heavily on electrodes made of carbonaceous materials. Still, the capacities reported for these multivalent systems remain stubbornly low. It is believed that a high structural quality of graphitic carbons and/or specific surface areas of >1000 m2 g‐1 are key factors to obtain optimal performance and cycling stability. Here an aluminum chloride battery is presented in which reduced graphene oxide (RGO) powder, dried under supercritical conditions, is used as the active cathode material and niobium foil as the current collector. With a specific surface area of just 364 m2 g‐1, the RGO enables a gravimetric capacity of 171 mAh g‐1 at 100 mA g‐1 and remarkable stability over a wide range of current densities (<15% decrease over 100 cycles in the interval 100–20000 mA g‐1). These properties, up to now achieved only with much larger surface area materials, result from the cathode's tailored mesoporosity. The 20 nm wide mesopores facilitate the movement of the chloroaluminate ions through the RGO, effectively minimizing the inactive mass content of the electrode. This more than compensates for the ordinary micropore volume of the graphene powder.
Doping/decorating of graphene or reduced graphene oxide (rGO) with heteroatoms provides a promising route for the development of electrocatalysts useful in many technologies, including water splitting. However, current doping approaches are complicated, not eco-friendly and not costeffective. Herein, we report the synthesis of doped/decorated rGO for oxygen evolution reaction (OER) using a simple approach that is cost-effective, sustainable and easy to scale up. The OER catalyst was derived from the reduction of GO by an exo-electron transferring bacterium, Geobacter sulfurreducens. Various analytical tools indicate that OER active elements such as Fe, Cu, N, P, and S decorate the rGO flakes. The hybrid catalyst (i.e., Geobacter/rGO) produces a geometric current density of 10 mA cm −2 at an overpotential of 270 mV vs. the reversible hydrogen electrode (RHE) with a Tafel slope of 43 mV dec −1 , and possesses high durability, evidenced through 10 hours of stability testing. Electrochemical analyses suggest the importance of Fe and its possible role as active site for OER. Overall, this work represents a simple approach towards the development of earthabundant, eco-friendly and highly active OER electrocatalyst for various applications such as solar fuel production, rechargeable metal-air batteries, and microbial electrosynthesis.
Strategies to synthesize reduced graphene oxide (rGO) abound but, in most studies, research teams select one particular oxidation-reduction method without providing a methodic reasoning for doing so. Herein, it is analyzed how diverse oxidation-reduction strategies commonly used can result in considerable performance differences of rGO for supercapacitor applications. Depending on the graphite oxidation method followed, the surface chemistry analysis of the products confirms that there is a marked disparity in the degree of oxidation and the nature of the oxygen functional groups present. Subsequent reduction of the oxidized graphite (using three different methods) showed that the maximum specific capacitance of rGOs produced from the classical Hummers' method was 128 F g −1 whereas an analogous material obtained from an improved Hummers' method reached ~274 F g −1 (both via an hydrothermal reduction route). Besides showing that the improved oxidation method results in superior capacitance performance, explained by the higher number of structural defects allied to a surface chemistry where residual hydroxyl and epoxy functional groups predominate, this study highlights the need to rationalize the oxidation-reduction strategies followed when investigating applications of rGO materials.
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