Monolayer graphene was first obtained as a transferable material in 2004 and has stimulated intense activity among physicists, chemists and material scientists. Much research has been focused on developing routes for obtaining large sheets of monolayer or bilayer graphene. This has been recently achieved by chemical vapour deposition (CVD) of CH(4) or C(2)H(2) gases on copper or nickel substrates. But CVD is limited to the use of gaseous raw materials, making it difficult to apply the technology to a wider variety of potential feedstocks. Here we demonstrate that large area, high-quality graphene with controllable thickness can be grown from different solid carbon sources-such as polymer films or small molecules-deposited on a metal catalyst substrate at temperatures as low as 800 °C. Both pristine graphene and doped graphene were grown with this one-step process using the same experimental set-up.

In this research, 3-dimensional (3D) graphene/carbon nanotube carpets (G/CNTCs)-based microsupercapacitors (G/CNTCs-MCs) were fabricated in situ on nickel electrodes. The G/CNTCs-MCs show impedance phase angle of -81.5° at a frequency of 120 Hz, comparable to commercial aluminum electrolytic capacitors (AECs) for alternating current (ac) line filtering applications. In addition, G/CNTCs-MCs deliver a high volumetric energy density of 2.42 mWh/cm(3) in the ionic liquid, more than 2 orders of magnitude higher than that of AECs. The ultrahigh rate capability of 400 V/s enables the microdevices to demonstrate a maximum power density of 115 W/cm(3) in aqueous electrolyte. The high-performance electrochemical properties of G/CNTCs-MCs can provide more compact ac filtering units and discrete power sources in future electronic devices. These elevated electrical features are likely enabled by the seamless nanotube/graphene junctions at the interface of the differing carbon allotropic forms.

In this research, we constructed a controlled chamber pressure CVD (CP-CVD) system to manipulate graphene's domain sizes and shapes. Using this system, we synthesized large (~4.5 mm(2)) single-crystal hexagonal monolayer graphene domains on commercial polycrystalline Cu foils (99.8% purity), indicating its potential feasibility on a large scale at low cost. The as-synthesized graphene had a mobility of positive charge carriers of ~11,000 cm(2) V(-1) s(-1) on a SiO(2)/Si substrate at room temperature, suggesting its comparable quality to that of exfoliated graphene. The growth mechanism of Cu-based graphene was explored by studying the influence of varied growth parameters on graphene domain sizes. Cu pretreatments, electrochemical polishing, and high-pressure annealing are shown to be critical for suppressing graphene nucleation site density. A pressure of 108 Torr was the optimal chamber pressure for the synthesis of large single-crystal monolayer graphene. The synthesis of one graphene seed was achieved on centimeter-sized Cu foils by optimizing the flow rate ratio of H(2)/CH(4). This work should provide clear guidelines for the large-scale synthesis of wafer-scale single-crystal graphene, which is essential for the optimized graphene device fabrication.

Graphene and single-walled carbon nanotubes are carbon materials that exhibit excellent electrical conductivities and large specific surface areas. Theoretical work suggested that a covalently bonded graphene/single-walled carbon nanotube hybrid material would extend those properties to three dimensions, and be useful in energy storage and nanoelectronic technologies. Here we disclose a method to bond graphene and single-walled carbon nanotubes seamlessly during the growth stage. The hybrid material exhibits a surface area 42,000 m 2 g À 1 with ohmic contact from the vertically aligned single-walled carbon nanotubes to the graphene. Using aberration-corrected scanning transmission electron microscopy, we observed the covalent transformation of sp 2 carbon between the planar graphene and the single-walled carbon nanotubes at the atomic resolution level. These findings provide a new benchmark for understanding the three-dimensional graphene/ single-walled carbon nanotube-conjoined materials.

Ni-based metal organic frameworks (Ni-MOFs) with unique hierarchical hollow ball-in-ball nanostructure were synthesized by solvothermal reactions. After successive carbonization and oxidation treatments, hierarchical NiO/Ni nanocrystals covered with a graphene shell were obtained with the hollow ball-in-ball nanostructure intact. The resulting materials exhibited superior performance as the anode in lithium ion batteries (LIBs): they provide high reversible specific capacity (1144 mAh/g), excellent cyclability (nearly no capacity loss after 1000 cycles) and rate performance (805 mAh/g at 15 A/g). In addition, the hierarchical NiO/Ni/Graphene composites demonstrated promising performance as anode materials for sodium-ion batteries (SIBs). Such a superior lithium and sodium storage performance is derived from the well-designed hierarchical hollow ball-in-ball structure of NiO/Ni/Graphene composites, which not only mitigates the volume expansion of NiO during the cycles but also provides a continuous highly conductive graphene matrix to facilitate the fast charge transfer and form a stable SEI layer.