We developed a hydrogen arc discharge exfoliation method for the synthesis of graphene sheets (GSs) with excellent electrical conductivity and good thermal stability from graphite oxide (GO), in combination with solution-phase dispersion and centrifugation techniques. It was found that efficient exfoliation and considerable deoxygenation of GO, and defect elimination and healing of exfoliated graphite can be simultaneously achieved during the hydrogen arc discharge exfoliation process. The GSs obtained by hydrogen arc discharge exfoliation exhibit a high electrical conductivity of ϳ2 ؋ 10 3 S/cm and high thermal stability with oxidization resistance temperature of 601 °C, which are much better than those prepared by argon arc discharge exfoliation (ϳ2 ؋ 10 2 S/cm, 525 °C) and by conventional thermal exfoliation (ϳ80 S/cm, 507 °C) with the same starting GO. These results demonstrate that this hydrogen arc discharge exfoliation method is a good approach for the preparation of GSs with a good quality.
A preheated high-temperature environment is believed to be critical for a chemical-exfoliation-based production of graphenes starting from graphite oxide, a belief that is based on not only experimental but also theoretical viewpoints. A novel exfoliation approach is reported in this study, and the exfoliation process is realized at a very low temperature, which is far below the proposed critical exfoliation temperature, by introducing a high vacuum to the exfoliation process. Owing to unique surface chemistry, low-temperature exfoliated graphenes demonstrate an excellent energy storage performance, and the electrochemical capacitance is much higher than that of the high-temperature exfoliated ones. The low-temperature exfoliation approach presents us with a possibility for a mass production of graphenes at low cost and great potentials in energy storage applications of graphene-based materials.
Lacking strategies to simultaneously address the intrinsic activity, site density, electrical transport, and stability problems of chalcogels is restricting their application in catalytic hydrogen production. Herein, we resolve these challenges concurrently through chemically activating the molybdenum disulfide (MoS2) surface basal plane by doping with a low content of atomic palladium using a spontaneous interfacial redox technique. Palladium substitution occurs at the molybdenum site, simultaneously introducing sulfur vacancy and converting the 2H into the stabilized 1T structure. Theoretical calculations demonstrate the sulfur atoms next to the palladium sites exhibit low hydrogen adsorption energy at –0.02 eV. The final MoS2 doped with only 1wt% of palladium demonstrates exchange current density of 805 μA cm−2 and 78 mV overpotential at 10 mA cm−2, accompanied by a good stability. The combined advantages of our surface activating technique open the possibility of manipulating the catalytic performance of MoS2 to rival platinum.
Homogeneous single‐layer graphene films are fabricated using an electrophoretic deposition technique, and their field‐emission properties are investigated. The graphene films show high density, uniform thickness, numerous edges normal to the film surface, and good interface contact and adhesion with the substrate, and consequently show excellent field‐emission properties.
A small volumetric capacitance resulting from a low packing density is one of the major limitations for novel nanocarbons finding real applications in commercial electrochemical energy storage devices. Here we report a carbon with a density of 1.58 g cm−3, 70% of the density of graphite, constructed of compactly interlinked graphene nanosheets, which is produced by an evaporation-induced drying of a graphene hydrogel. Such a carbon balances two seemingly incompatible characteristics: a porous microstructure and a high density, and therefore has a volumetric capacitance for electrochemical capacitors (ECs) up to 376 F cm−3, which is the highest value so far reported for carbon materials in an aqueous electrolyte. More promising, the carbon is conductive and moldable, and thus could be used directly as a well-shaped electrode sheet for the assembly of a supercapacitor device free of any additives, resulting in device-level high energy density ECs.
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