Zeolite-templated carbon (ZTC), which can be obtained as a negative replica of a zeolite, consists of buckybowllike nanographenes assembled into a three-dimensional regular network. ZTC is characterized not only by this unique framework structure but also by a very large number of carbon edge sites. In this paper, we report that the edge sites of ZTC are easily functionalized by a large amount of quinone groups through electrochemical oxidation unlike general carbonaceous materials, and the quinone-functionalized ZTC shows a high electrochemical capacitance (ca. 300 500 F g ¹1 ) in an aqueous electrolyte solution (1 M H 2 SO 4 ) as a result of the large pseudocapacitance derived from a quinone/hydroquinone redox couple. Moreover, ZTC keeps its high capacitance even after thousands of charge discharge cycles.Fullerenes, 1 single-walled carbon nanotubes (SWCNTs), 2,3 and graphenes 4,5 are nanocarbon materials with 0D, 1D, and 2D topologies, respectively. Though fullerenes form poorly conductive van der Waals crystals, SWCNTs 6,7 and graphenes 811 are electrically conductive, and are promising as electrode materials for electrochemical capacitors. 12 Their building unit, a graphene sheet, has a large theoretical surface area (2630 m 2 g ¹1 ), and therefore potentially has a large capacitance. However, the actual BrunauerEmmettTeller (BET) surface areas of SWCNTs 13 and graphenes 8 are at most 1250 and 705 m 2 g ¹1 , respectively, because of the aggregation/stacking of the graphene sheets as a result of strong van der Waals interactions. To expose the entire surface, a graphene sheet has to be formed into a self-standing 3D network, like carbon schwarzite 14,15 or pillared graphene, 16 both of which are imaginary materials and have only been proposed theoretically. Thus far our group has demonstrated that it is possible to synthesize a graphene-based architecture with a 3D topology inside the confined-nanospace network of a zeolite crystal, as shown in Figures 1a1c.
1720The zeolite-templated carbon (ZTC) thus obtained consists of a buckybowl-like nanographene assembled into a 3D regular network (Figures 1c and 1d). Both sides of the buckybowllike unit are fully exposed, and, in addition, the narrow nanographene-based framework has a significant number of edge sites. 18 Consequently, ZTC has a very large geometric (theoretical) surface area of 3432 m 2 g ¹1 , and such a large surface area has indeed been observed experimentally.18 ZTC possesses unique spin/magnetic properties 21 and is predicted to have a unique band structure. 22 Moreover, it has a high hydrogen-storage capacity 23,24 and superior performance as an electrode for electrochemical capacitors.2527 Modifications of ZTC with electrochemically active species are expected to further enhance its performance. Graphene-based materials are generally modified by doping of graphene with other functional components such as metal nanoparticles, 2830 metal oxides/ hydroxides, 3134 and conductive polymers. 35 Another modification method is to functionalize graphenes...