Nanohybrids consisting of both carbon and pseudocapacitive metal oxides are promising as high-performance electrodes to meet the key energy and power requirements of supercapacitors. However, the development of high-performance nanohybrids with controllable size, density, composition and morphology remains a formidable challenge. Here, we present a simple and robust approach to integrating manganese oxide (MnO x ) nanoparticles onto flexible graphite paper using an ultrathin carbon nanotube/ reduced graphene oxide (CNT/RGO) supporting layer. Supercapacitor electrodes employing the MnO x /CNT/RGO nanohybrids without any conductive additives or binders yield a specific capacitance of 1070 F g − 1 at 10 mV s − 1 , which is among the highest values reported for a range of hybrid structures and is close to the theoretical capacity of MnO x . Moreover, atmosphericpressure plasmas are used to functionalize the CNT/RGO supporting layer to improve the adhesion of MnO x nanoparticles, which results in theimproved cycling stability of the nanohybrid electrodes. These results provide information for the utilization of nanohybrids and plasma-related effects to synergistically enhance the performance of supercapacitors and may create new opportunities in areas such as catalysts, photosynthesis and electrochemical sensors. NPG Asia Materials (2014) 6, e140; doi:10.1038/am.2014.100; published online 31 October 2014
INTRODUCTIONSupercapacitors are promising energy storage systems for diverse applications such as portable electronics, roll-up displays, hybrid electric vehicles, self-powered sensors, artificial muscles and biomedical implants. 1,2 The performance of supercapacitors fills the gap between batteries and conventional electrolytic capacitors, with such advantages as fast dynamic response, high power density, high rate capability, safe operation and long lifespan. The most common materials for current supercapacitor electrodes are high-surface-area carbon-based nanostructures, including activated carbons, porous/ templated graphite, carbon nanotubes (CNTs) and graphene. [3][4][5][6] However, the relatively low specific capacitance and energy density of these carbon-based electrodes have so far hampered their widespread applications in real devices.To address this challenge, hybrid materials that can synergistically combine the attributes of both carbon and pseudocapacitive materials such as metal oxides and conductive polymers have been actively pursued. [7][8][9] Pseudocapacitive materials store electrochemical energy in a similar manner as carbon-based materials but have a specific capacitance that is usually one order of magnitude larger. Among various pseudocapacitive materials, manganese oxides (MnO x ) have attracted the strongest interest because of their natural abundance, low cost and environmental friendliness. 10 Numerous studies have