Dai-Ming Tang

Low-Temperature Exfoliated Graphenes: Vacuum-Promoted Exfoliation and Electrochemical Energy Storage

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.

Synthesis of graphene sheets with high electrical conductivity and good thermal stability by hydrogen arc discharge exfoliation.

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 approximately 2 x 10(3) S/cm and high thermal stability with oxidization resistance temperature of 601 degrees C, which are much better than those prepared by argon arc discharge exfoliation (approximately 2 x 10(2) S/cm, 525 degrees C) and by conventional thermal exfoliation (approximately 80 S/cm, 507 degrees 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.

Three-dimensional strutted graphene grown by substrate-free sugar blowing for high-power-density supercapacitors

Three-dimensional graphene architectures in the macroworld can in principle maintain all the extraordinary nanoscale properties of individual graphene flakes. However, current 3D graphene products suffer from poor electrical conductivity, low surface area and insufficient mechanical strength/elasticity; the interconnected self-supported reproducible 3D graphenes remain unavailable. Here we report a sugar-blowing approach based on a polymeric predecessor to synthesize a 3D graphene bubble network. The bubble network consists of mono- or few-layered graphitic membranes that are tightly glued, rigidly fixed and spatially scaffolded by micrometre-scale graphitic struts. Such a topological configuration provides intimate structural interconnectivities, freeway for electron/phonon transports, huge accessible surface area, as well as robust mechanical properties. The graphene network thus overcomes the drawbacks of presently available 3D graphene products and opens up a wide horizon for diverse practical usages, for example, high-power high-energy electrochemical capacitors, as highlighted in this work.

Towards ultrahigh volumetric capacitance: graphene derived highly dense but porous carbons for supercapacitors

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.

Ru/ITO: a carbon-free cathode for nonaqueous Li-O2 battery

Ru nanoparticles deposited on a conductive support indium tin oxide (Ru/ITO) were applied as a carbon-free cathode in a nonaqueous Li-O2 battery. The Li-O2 battery with Ru/ITO showed much lower charging overpotentials and better cycling performance at 0.15 mA/cm(2) than those with Super P (SP) and SP loaded with Ru nanoparticles (Ru/SP) as the cathodes. The carbon-free cathode Ru/ITO can effectively reduce formation of Li2CO3 or other Li carbonates in a discharging process, which cannot be completely decomposed upon charging, in comparison with the carbon based cathode. The improved performance of Ru/ITO can be attributed to the superior catalytic activity of Ru nanoparticles toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) and the absence of carbon that has been reported to react with Li2O2 to form Li2CO3.

A sandwich structure of graphene and nickel oxide with excellent supercapacitive performance

Hybrid structures combining graphene nanosheets (GNSs) and metal oxide nanoparticles (NPs) are increasingly attracting researchers due to their potential applications in electrochemical energy storage. Such hybrid structures reported thus far are mostly in random organizations of nanosheets anchored with NPs and macroscopically exist in powder aggregates. In this work, a sandwich structure of GNSs and oxide NPs that are macroscopically a free-standing membrane is reported, and a multi-step strategy conducted under “homogenous” and “mild” conditions is developed to ensure the successful fabrication of the membrane-like structure. Both components, tightly fixed NPs and planar GNSs as the skeleton of such sandwich structures, can avoid aggregation or stacking during electrochemical charge–discharge cycling, which effectively maintains the active surface and leaves stable and open channels for ion transport. Such a layered sandwich structure also acts as an ideal strain buffer to accommodate volume changes of the NPs in a fixed direction, and thus has a better resilience and structural stability in the electrochemical charge/discharge process. Hence, such a GNS/NP sandwich structure represents an ideal structure for electrochemical energy storage and a solution for easy manipulation for various applications due to the membrane morphology.

Self-stacked Co3O4 nanosheets for high-performance lithium ion batteries.

Self-stacked Co(3)O(4) nanosheets separated by carbon layers were synthesized via a facile method. They exhibit excellent electrochemical performance that results from superior electronic conductivity endowed by carbon, a reduced Li(+) diffusion length within the building blocks and a large electrode/electrolyte contact area due to the interspaces between the blocks.

Importance of oxygen in the metal-free catalytic growth of single-walled carbon nanotubes from SiOx by a vapor-solid-solid mechanism

To understand in-depth the nature of the catalyst and the growth mechanism of single-walled carbon nanotubes (SWCNTs) on a newly developed silica catalyst, we performed this combined experimental and theoretical study. In situ transmission electron microscopy (TEM) observations revealed that the active catalyst for the SWCNT growth is solid and amorphous SiO(x) nanoparticles (NPs), suggesting a vapor-solid-solid growth mechanism. From in situ TEM and chemical vapor deposition growth experiments, we found that oxygen plays a crucial role in SWCNT growth in addition to the well-known catalyst size effect. Density functional theory calculations showed that oxygen atoms can enhance the capture of -CH(x) and consequently facilitate the growth of SWCNTs on oxygen-containing SiO(x) NPs.

Li‐O2 Battery Based on Highly Efficient Sb‐Doped Tin Oxide Supported Ru Nanoparticles

Novel cathodes based on Sb-doped tin oxide (STO)-supported Ru particles enable Li-O2 batteries to be operated below 4.0 V, which is of crucial importance for the realization of rechargeable Li-O2 batteries, and to deliver a high specific capacity of 750 mA h g(-1) even after 50 discharge-charge cycles at 0.1 mA cm(-2) .

Mechanical Properties of Si Nanowires as Revealed by in Situ Transmission Electron Microscopy and Molecular Dynamics Simulations

Deformation and fracture mechanisms of ultrathin Si nanowires (NWs), with diameters of down to ~9 nm, under uniaxial tension and bending were investigated by using in situ transmission electron microscopy and molecular dynamics simulations. It was revealed that the mechanical behavior of Si NWs had been closely related to the wire diameter, loading conditions, and stress states. Under tension, Si NWs deformed elastically until abrupt brittle fracture. The tensile strength showed a clear size dependence, and the greatest strength was up to 11.3 GPa. In contrast, under bending, the Si NWs demonstrated considerable plasticity. Under a bending strain of <14%, they could repeatedly be bent without cracking along with a crystalline-to-amorphous phase transition. Under a larger strain of >20%, the cracks nucleated on the tensed side and propagated from the wire surface, whereas on the compressed side a plastic deformation took place because of dislocation activities and an amorphous transition.