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Graphene-based materials are extensively studied as promising candidates for supercapacitors (SCs) owing to the high surface area, electrical conductivity, and mechanical flexibility of graphene. Reduced graphene oxide (RGO), a close graphene-like material studied for SCs, offers limited specific capacitances (100 F·g–1) as the reduced graphene sheets partially restack through π–π interactions. This paper presents pillared graphene materials designed to minimize such graphitic restacking by cross-linking the graphene sheets with a bifunctional pillar molecule. Solid-state NMR, X-ray diffraction, and electrochemical analyses reveal that the synthesized materials possess covalently cross-linked graphene galleries that offer additional sites for ion sorption in SCs. Indeed, high specific capacitances in SCs are observed for the graphene materials synthesized with an optimized number of pillars. Specifically, the straightforward synthesis of a graphene hydrogel containing pillared structures and an interconnected porous network delivered a material with gravimetric capacitances two times greater than that of RGO (200 F·g–1vs107 F·g–1) and volumetric capacitances that are nearly four times larger (210 F·cm–3vs54 F·cm–3). Additionally, despite the presence of pillars inside the graphene galleries, the optimized materials show efficient ion transport characteristics. This work therefore brings perspectives for the next generation of high-performance SCs.

Fe3–xO4raspberry shaped nanostructures/graphene nanocomposites were synthesized by a one-step polyol-solvothermal method to be tested as electrode materials for Li-ion battery (LIB). Indeed, Fe3–xO4raspberry shaped nanostructures consist of original oriented aggregates of Fe3–xO4magnetite nanocrystals, ensuring a low oxidation state of magnetite and a hollow and porous structure, which has been easily combined with graphene sheets. The resulting nanocomposite powder displays a very homogeneous spatial distribution of Fe3–xO4nanostructures at the surface of the graphene sheets. These original nanostructures and their strong interaction with the graphene sheets resulted in very small capacity fading upon Li+ion intercalation. Reversible capacity, as high as 660mAh/g, makes this material promising for anode in Li-ion batteries application.

Understanding ion adsorption in nanoporous carbon electrodes is of great importance for designing the next-generation of high energy density electrical double-layer capacitors. In this work, X-ray scattering is used for investigating the impregnation of nanoporous carbons with electrolytes in the absence of applied potential. We are able to show that interactions between the carbon surface and electrolytes allow adsorption to take place in sub-nanopores, thus confirming experimentally for the first time the results predicted by molecular dynamic simulations.

Two graphene-like carbide derived carbons (CDC-Gs) were produced by chlorination of SiC nanosheets obtained by magnesio-thermal reduction at moderate temperature of silica/graphene oxide nanocomposites. These CDC-Gs were evaluated as supercapacitor electrode materials in an organic electrolyte. Starting from a low SiO2/GO ratio in the precursor, the resulting CDC-G nanosheets are composed of a few layers of graphite, partially coated with microporous CDC. In contrast, a high SiO2/GO ratio leads to micropores generated on the basal plane of individual carbon nanosheets. The latter CDC-G shows a remarkable high power capability with 76 % of retention of the initial capacity at scan rates up to 3Vs−1. Notably, the equivalent series resistance (ESR) and time constant of the cell were found to be extremely low at 0.45Ω·cm2and 0.4s, respectively, thanks to the unique 2D open surface and enhanced access to micropores. These features were attributed to the unique nanostructure of the microporous graphene.

Supercapacitors are electricity storage systems with high power performances. Their short charge/discharge times are due to fast adsorption/desorption rates for the ions of the electrolyte on the electrode surface. Nanoporous carbon electrodes, which give larger capacitances than simpler geometries, might be expected to show poorer power performances because of the longer times taken by the ions to access the electrode interior. Experiments do not show such trends, however, and this remains to be explained at the molecular scale. Here we show that carbide-derived carbons exhibit heterogeneous and fast charging dynamics. We perform molecular dynamics simulations, with realistically modeled nanoporous electrodes and an ionic liquid electrolyte, in which the system, originally at equilibrium in the uncharged state, is suddenly perturbed by the application of an electric potential difference between the electrodes. The electrodes respond by charging progressively from the interface to the bulk as ions are exchanged between the nanopores and the electrolyte region. The simulation results are then injected into an equivalent circuit model, which allows us to calculate charging times for macroscopic-scale devices.

Thin films of (TTF)(TCNQ) (TTF=tetrathiafulvalene, TCNQ=tetracyanoquinodimethane) are deposited on Si (001), KBr, and stainless steel conversion coatings (SSCC) using chemical vapor deposition. These films are characterized by IR, XRD, conductivity measurements, and SEM. Conducting nanowires and nanorings of (TTF)(TCNQ) and nanowires of (TTF)[Ni(dmit) 2 ] 2 (typically, 20 nm×20 μm) are prepared by successively dipping SSCC in acetonitrile solutions of TTF and TCNQ, or (TTF) 3 (BF 4 ) and (Bu 4 N)[Ni(dmit) 2 ], respectively. These nanowires are observed by SEM. The (TTF)(TCNQ) nanowires are also observed by TEM and AFM and characterized by current-voltage measurements. Nanowires of (TTF)[Ni(dmit) 2 ] 2 are also obtained on silicon conversion coatings (SiCC) and characterized by Raman spectroscopy.