Changsheng Xiang

Toward the Synthesis of Wafer-Scale Single-Crystal Graphene on Copper Foils

In this research, we constructed a controlled chamber pressure CVD (CP-CVD) system to manipulate graphenes 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 nanoribbon and nanostructured SnO2 composite anodes for lithium ion batteries.

A composite made from graphene nanoribbons (GNRs) and tin oxide (SnO2) nanoparticles (NPs) is synthesized and used as the anode material for lithium ion batteries (LIBs). The conductive GNRs, prepared using sodium/potassium unzipping of multiwall carbon nanotubes, can boost the lithium storage performance of SnO2 NPs. The composite, as an anode material for LIBs, exhibits reversible capacities of over 1520 and 1130 mAh/g for the first discharge and charge, respectively, which is more than the theoretical capacity of SnO2. The reversible capacity retains ~825 mAh/g at a current density of 100 mA/g with a Coulombic efficiency of 98% after 50 cycles. Further, the composite shows good power performance with a reversible capacity of ~580 mAh/g at the current density of 2 A/g. The high capacity, good power performance and retention can be attributed to uniformly distributed SnO2 NPs along the high-aspect-ratio GNRs. The GNRs act as conductive additives that buffer the volume changes of SnO2 during cycling. This work provides a starting point for exploring the composites made from GNRs and other transition metal oxides for lithium storage applications.

Edge-oriented MoS2 nanoporous films as flexible electrodes for hydrogen evolution reactions and supercapacitor devices.

A simple method to fabricate edge-oriented MoS2 films with sponge-like morphologies is demonstrated. They are directly fabricated through the reaction of sulfur vapor with anodically formed Mo oxide sponge-like films on flexible Mo substrates. The edge-oriented MoS2 film delivers excellent hydrogen evolution reaction (HER) activity with enhanced kinetics and long-term cycling stability. The material also has superior energy-storage performance when working as a flexible, all-solid-state supercapacitor device.

Coal as an abundant source of graphene quantum dots

Coal is the most abundant and readily combustible energy resource being used worldwide. However, its structural characteristic creates a perception that coal is only useful for producing energy via burning. Here we report a facile approach to synthesize tunable graphene quantum dots from various types of coal, and establish that the unique coal structure has an advantage over pure sp2-carbon allotropes for producing quantum dots. The crystalline carbon within the coal structure is easier to oxidatively displace than when pure sp2-carbon structures are used, resulting in nanometre-sized graphene quantum dots with amorphous carbon addends on the edges. The synthesized graphene quantum dots, produced in up to 20% isolated yield from coal, are soluble and fluorescent in aqueous solution, providing promise for applications in areas such as bioimaging, biomedicine, photovoltaics and optoelectronics, in addition to being inexpensive additives for structural composites.

Efficient Electrocatalytic Oxygen Evolution on Amorphous Nickel–Cobalt Binary Oxide Nanoporous Layers

Nanoporous Ni-Co binary oxide layers were electrochemically fabricated by deposition followed by anodization, which produced an amorphous layered structure that could act as an efficient electrocatalyst for water oxidation. The highly porous morphologies produced higher electrochemically active surface areas, while the amorphous structure supplied abundant defect sites for oxygen evolution. These Ni-rich (10-40 atom % Co) binary oxides have an increased active surface area (roughness factor up to 17), reduced charge transfer resistance, lowered overpotential (∼325 mV) that produced a 10 mA cm(-2) current density, and a decreased Tafel slope (∼39 mV decade(-1)). The present technique has a wide range of applications for the preparation of other binary or multiple-metals or metal oxides nanoporous films. Fabrication of nanoporous materials using this method could provide products useful for renewable energy production and storage applications.

Three-Dimensional Metal–Graphene–Nanotube Multifunctional Hybrid Materials

Graphene was grown directly on porous nickel films, followed by the growth of controlled lengths of vertical carbon nanotube (CNT) forests that seamlessly emanate from the graphene surface. The metal-graphene-CNT structure is used to directly fabricate field-emitter devices and double-layer capacitors. The three-dimensional nanostructured hybrid materials, with better interfacial contacts and volume utilization, can stimulate the development of several energy-efficient technologies.

Large Flake Graphene Oxide Fibers with Unconventional 100% Knot Efficiency and Highly Aligned Small Flake Graphene Oxide Fibers

Two types of graphene oxide fibers are spun from high concentration aqueous dopes. Fibers extruded from large flake graphene oxide dope without drawing show unconventional 100% knot efficiency. Fibers spun from small sized graphene oxide dope with stable and continuous drawing yield in good intrinsic alignment with a record high tensile modulus of 47 GPa.

Large-Area Bernal-Stacked Bi-, Tri-, and Tetralayer Graphene

Few-layer graphene, with Bernal stacking order, is of particular interest to the graphene community because of its unique tunable electronic structure. A synthetic method to produce such large area graphene films with precise thickness from 2 to 4 layers would be ideal for chemists and physicists to explore the promising electronic applications of these materials. Here, large-area uniform Bernal-stacked bi-, tri-, and tetralayer graphene films were successfully synthesized on a Cu surface in selective growth windows, with a finely tuned total pressure and CH(4)/H(2) gas ratio. On the basis of the analyses obtained, the growth mechanism is not an independent homoexpitaxial layer-by-layer growth, but most likely a simultaneous-seeding and self-limiting process.

Hydrothermally formed three-dimensional nanoporous Ni(OH)2 thin-film supercapacitors.

A three-dimensional nanoporous Ni(OH)2 thin-film was hydrothermally converted from an anodically formed porous layer of nickel fluoride/oxide. The nanoporous Ni(OH)2 thin-films can be used as additive-free electrodes for energy storage. The nanoporous layer delivers a high capacitance of 1765 F g(-1) under three electrode testing. After assembly with porous activated carbon in asymmetric supercapacitor configurations, the devices deliver superior supercapacitive performances with capacitance of 192 F g(-1), energy density of 68 Wh kg(-1), and power density of 44 kW kg(-1). The wide working potential window (up to 1.6 V in 6 M aq KOH) and stable cyclability (∼90% capacitance retention over 10,000 cycles) make the thin-film ideal for practical supercapacitor devices.

Functionalized Low Defect Graphene Nanoribbons and Polyurethane Composite Film for Improved Gas Barrier and Mechanical Performances

A thermoplastic polyurethane (TPU) composite film containing hexadecyl-functionalized low-defect graphene nanoribbons (HD-GNRs) was produced by solution casting. The HD-GNRs were well distributed within the polyurethane matrix, leading to phase separation of the TPU. Nitrogen gas effective diffusivity of TPU was decreased by 3 orders of magnitude with only 0.5 wt % HD-GNRs. The incorporation of HD-GNRs also improved the mechanical properties of the composite films, as predicted by the phase separation and indicated by tensile tests and dynamic mechanical analyses. The improved properties of the composite film could lead to potential applications in food packaging and lightweight mobile gas storage containers.