Nanostructure of highly aromatic graphene nanosheets -- From optoelectronics to electrochemical energy storage applications

The exceptional electrical properties along with intriguing physical and chemical aspects of graphene nanosheets can only be realized by nanostructuring these materials through the homogeneous and orderly distribution of these nanosheets without compromising the aromaticity of the native basal plane. Graphene nanosheets prepared by direct exfoliation as opposed to the graphene oxide route are necessary in order to preserve the native chemical properties of graphene basal planes. This research has been directed at optimally combining the diverse physical and chemical aspects of graphene nanosheets such as particle size, surface area and edge chemistry to fabricate nanostructured architectures for optoelectronics and high power electrochemical energy storage applications.;In the first nanostructuring effort, a monolayer of these ultrathin, highly hydrophobic graphene nanosheets was prepared on a large area substrate via self-assembly at the liquid-liquid interface. Driven by the minimization of interfacial energy these planar graphene nanosheets produce a close packed monolayer structure at the liquid-liquid interface. The resulting monolayer film exhibits high electrical conductivity of more than 1000 S/cm and an optical transmission of more than 70-80% between wavelengths of 550 nm and 2000 nm making it an ideal candidate for optoelectronic applications. In the second part of this research, nanostructuring was used to create a configuration suitable for supercapacitor applications. A free standing, 100% binder free multilayer, flexible film consisting of monolayers of graphene nanosheets was prepared by utilizing the van der Waals forces of attraction between the basal plans of the graphene nanosheets coupled with capillary driven and drying-induced collapse. A major benefit in this approach is that the graphene nanosheet's attractive physical and chemical characteristics can be synthesized into an architecture consisting of large and small nanosheets to create an aligned network designed to maximize device performance. Monolayers of large sized graphene nanosheets function as highly electrically conducting current collectors within a mesoporous network of smaller graphene nanosheets for improved rate capability of the electrical double layer capacitor (EDLC) electrode. This nano-architecture produces an electrode with superior performance for high power EDLC applications: a high frequency capacitative response; a nearly rectangular cyclic voltammogram at a scanning rate of 1000 mv/sec; a rapid current response; small equivalent series resistance (ESR); and fast ionic diffusion. Integration of this nanostructured graphene nanosheet architecture with conductive polymers or metal oxide nanostructurcs was also investigated to produce similar multilayered structures for electrochemical energy storage applications.;These inexpensive graphene nanosheets coupled with this facile and robust nanostructuring process make both this new material and method highly advantageous for many potential applications ranging from optoelectronics to high power electrochemical energy storage applications.