Focusing on energy and optoelectronic applications: a journey for graphene and graphene oxide at large scale.

Carbon is the only element that has stable allotropes in the 0th through the 3rd dimension, all of which have many outstanding properties. Graphene is the basic building block of other important carbon allotropes. Studies of graphene became much more active after the Geim group isolated "free" and "perfect" graphene sheets and demonstrated the unprecedented electronic properties of graphene in 2004. So far, no other individual material combines so many important properties, including high mobility, Hall effect, transparency, mechanical strength, and thermal conductivity. In this Account, we briefly review our studies of bulk scale graphene and graphene oxide (GO), including their synthesis and applications focused on energy and optoelectronics. Researchers use many methods to produce graphene materials: bottom-up and top-down methods and scalable methods such as chemical vapor deposition (CVD) and chemical exfoliation. Each fabrication method has both advantages and limitations. CVD could represent the most important production method for electronic applications. The chemical exfoliation method offers the advantages of easy scale up and easy solution processing but also produces graphene oxide (GO), which leads to defects and the introduction of heavy functional groups. However, most of these additional functional groups and defects can be removed by chemical reduction or thermal annealing. Because solution processing is required for many film and device applications, including transparent electrodes for touch screens, light-emitting devices (LED), field-effect transistors (FET), and photovoltaic devices (OPV), flexible electronics, and composite applications, the use of GO is important for the production of graphene. Because graphene has an intrinsic zero band gap, this issue needs to be tackled for its FET applications. The studies for transparent electrode related applications have made great progress, but researchers need to improve sheet resistance while maintaining reasonable transparency. Proposals for solving these issues include doping or controlling the sheet size and defects, and theory indicates that graphene can match the overall performance of indium tin oxide (ITO). We have significantly improved the specific capacitance in graphene supercapacitor devices, though our results do not yet approach theoretical values. For composite applications, the key issue is to prevent the restacking of graphene sheets, which we achieved by adding blocking molecules. The continued success of graphene studies will require further development in two areas: (1) the large scale and controlled synthesis of graphene, producing different structures and quantities that are needed for a variety of applications and (2) on table applications, such as transparent electrodes and energy storage devices. Overall, graphene has demonstrated performance that equals or surpasses that of other new carbon allotropes. These features, combined with its easier access and better processing ability, offer the potential basis for truly revolutionary applications and as a future fundamental technological material beyond the silicon age.