Chenguang Zhang

3-Dimensional graphene carbon nanotube carpet-based microsupercapacitors with high electrochemical performance.

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.

A seamless three-dimensional carbon nanotube graphene hybrid material.

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 >2,000 m(2) g(-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.

Towards hybrid superlattices in graphene

The controllable and reversible modification of graphene by chemical functionalization can modulate its optical and electronic properties. Here we demonstrate the controlled patterning of graphane/graphene superlattices within a single sheet of graphene. By exchanging the sp(3) C-H bonds in graphane with sp(3) C-C bonds through functionalization, sophisticated multifunctional superlattices can be fabricated on both the macroscopic and microscopic scales. These patterns are visualized using fluorescence quenching microscopy techniques and confirmed using Raman spectroscopy. By tuning the extent of hydrogenation, the density of the sp(3) C functional groups on graphenes basal plane can be controlled from 0.4% to 3.5% with this two-step method. Using such a technique, which allows for both spatial and density control of the functional groups, a route to multifunctional electrical circuits and chemical sensors with specifically patterned recognition sites might be realized across a single graphene sheet, facilitating the development of graphene-based devices.

Splitting of a vertical multiwalled carbon nanotube carpet to a graphene nanoribbon carpet and its use in supercapacitors.

Potassium vapor was used to longitudinally split vertically aligned multiwalled carbon nanotubes carpets (VA-CNTs). The resulting structures have a carpet of partially split MWCNTs and graphene nanoribbons (GNRs). The split structures were characterized by scanning electron microscopy, transmission electron microscopy, atomic force microscopy, Raman spectroscopy and X-ray photoelectron spectroscopy. When compared to the original VA-CNTs carpet, the split VA-CNTs carpet has enhanced electrochemical performance with better specific capacitance in a supercapacitor. Furthermore, the split VA-CNTs carpet has excellent cyclability as a supercapacitor electrode material. There is a measured maximum power density of 103 kW/kg at an energy density of 5.2 Wh/kg and a maximum energy density of 9.4 Wh/kg. The superior electrochemical performances of the split VA-CNTs can be attributed to the increased surface area for ion accessibility after splitting, and the lasting conductivity of the structure with their vertical conductive paths based on the preserved GNR alignment.

Closed-Edged Graphene Nanoribbons from Large-Diameter Collapsed Nanotubes

The diameter dependence of the collapse of single- and double-walled carbon nanotubes to two- and four-walled graphene nanoribbons with closed edges (CE(x)GNRs) has been experimentally determined and compared to theory. TEM and AFM were used to characterize nanotubes grown from preformed 4.0 nm diameter aluminum-iron oxide particles. Experimental data indicate that the energy equivalence point (the diameter at which the energy of a round and fully collapsed nanotube is the same) is 2.6 and 4.0 nm for single- and double-walled carbon nanotubes, respectively. Molecular dynamics simulations predict similar energy equivalence diameters with the use of ε = 54 meV/pair to calculate the carbon-carbon van der Waals interaction.

Effect of Ni, Fe and Fe-Ni alloy catalysts on the synthesis of metal contained carbon nano-onions and studies of their electrochemical hydrogen storage properties

Abstract Three types of carbon nano-onions (CNOs) including Ni@CNOs, Fe 3 C@CNOs and Fe 0.64 Ni 0.36 @CNOs nanoparticles have been synthesized by catalytic decomposition of methane at 850 °C using nickel, iron and iron-nickel alloy catalysts. Comparative and systematic studies have been carried out on the morphology, structural characteristics and graphitic crystallinity of these CNOs products. Furthermore, the electrochemical hydrogen storage properties of three types of CNOs have been investigated. Measurements show that the Ni@CNOs have the highest discharge capacity of 387.2 mAh/g, corresponding to a hydrogen storage of 1.42%. This comparison study shows the advantages of each catalyst in the growth of CNOs, enabling the controllable synthesis and tuning the properties of CNOs by mediating different metals and their alloy for using in the fuel cell system.

Self-anchored catalysts for substrate-free synthesis of metal-encapsulated carbon nano-onions and study of their magnetic properties

We demonstrate the synthesis of a novel self-anchored catalyst structure containing a Fe-Ni alloy nanosheet generated by phase separation for the substrate-free synthesis of carbon nanostructures. Fast Fourier transform analysis was carried out in order to investigate both the phase and structural evolution of the alloy nanosheet during reduction and chemical vapor deposition (CVD) growth. γ-Fe-Ni (Fe0.64Ni0.36) and α-Fe-Ni (kamacite) phases were formed and separated on the NiFe2O4 nanosheet catalyst precursor during H2 reduction, forming selfanchored mono-dispersed γ-Fe-Ni nanocrystals on a α-Fe-Ni matrix. The Fe-Ni alloy nanosheet serves both as a catalyst for growing metal-encapsulated carbon nano-onions (CNOs), and as a support for anchoring these preformed nanoparticles, yielding mono-dispersed catalyst nanoparticles with no requirement of additional substrates for the CVD growth. This synthesis is capable of mitigating the coalescence and Ostwald ripening without the assistance of an additional substrate. This structure allows for the growth of uniform-sized CNOs despite the aggregation, crumbling, and stacking of the alloy sheet. This study provides a promising design for novel catalyst structures by phase separation towards the substrate-free synthesis of carbon nanostructures in large scale. Finally, the ferromagnetic Fe0.64Ni0.36@CNOs particles demonstrate their application in both magnetic storage and water purification, as a non-toxic water treatment material.