Single crystalline graphene synthesized by thermal annealing of humic acid over copper foils

Production of graphene by thermal annealing on copper foil substrates has been studied with different sources of carbon. The three carbon sources include humic acid derived from leonardite, graphenol, and activated charcoal. Hexagonal single crystalline graphene has been synthesized over the copper foil substrates by thermal annealing of humic acid, derived from leonardite, in argon and hydrogen atmosphere (Ar/H₂=20). The annealing temperature was varied between 1050 °C and 1100 °C at atmospheric pressure. Samples have been investigated using scanning electron microscope (SEM) and Raman spectroscopy. At lower temperatures the thermal annealing of the three carbon sources used in this study produces pristine graphene nanosheets which cover almost the whole substrate. However when the annealing temperature has been increased up to 1100 °C, hexagonal single crystalline graphene have been observed only in the case of the humic acid. Raman analysis showed the existence of 2D band around 2690 cm⁻¹.     

Self-assembly of metal–organic frameworks and graphene oxide as precursors for lithium-ion battery applications

We fabricated composites of Fe₂O₃/reduced graphene oxide as lithium-ion batteries anode material with controlled structures by employing self-assembly of metal–organic frameworks (MOFs) and polymer-functionalized graphene oxide as precursors. By electrostatic interaction, the negatively charged MOFs, Prussian Blue (PB), are assembled on poly(diallyldimethylammonium chloride) (PDDA)-functionalized graphene oxide (positive charge). Then the PB cubes become FeOOH nanosheets when treated with sodium hydroxide. Upon further annealing, the FeOOH nanosheets transform to Fe₂O₃ nanoparticles while the graphene oxide become reduced graphene oxide simultaneously. It was found that the composites have good performance as anode of lithium-ion battery. This work shows a new way for self-assembling MOFs and 2D materials.     

Hydrothermal synthesis of graphene oxide/multiwalled carbon nanotube/Fe<Subscript>3</Subscript>O<Subscript>4</Subscript> ternary nanocomposite for removal of Cu (II) and methylene blue

In this work, highly activated graphene oxide/multiwalled carbon nanotube/Fe₃O₄ ternary nanocomposite adsorbent was prepared from a simple hydrothermal route by using ferrous sulfate as precursor. For this purpose, the graphene oxide/multiwalled carbon nanotube architectures were formed through the π-π attractions between them, followed by attaching Fe₃O₄ nanoparticles onto their surface. The structure and composition of as-prepared ternary nanocomposite were characterized by XRD, FTIR, XPS, SEM, TEM, Raman, TGA, and BET. It was found that the resultant porous graphene oxide/multiwalled carbon nanotube/Fe₃O₄ ternary nanocomposite with large surface area could effectively prevent the π-π stacking interactions between graphene oxide nanosheets and greatly improve sorption sites on the surfaces. Thus, owing to the unique ternary nanocomposite architecture and synergistic effect among various components, as-prepared ternary nanocomposite exhibited high separation efficiency when they were used to remove the Cu (II) and methylene blue from aqueous solutions. Furthermore, the adsorption isotherms of ternary nanocomposite structures for Cu (II) and methylene blue removal fitted the Langmuir isotherm model. This work demonstrated that the graphene oxide/multiwalled carbon nanotube/Fe₃O₄ ternary nanocomposite was promising as an efficient adsorbent for heavy metal ions and organic dye removal from wastewater in low concentration.     

Graphene nanosheets: Ultrasound assisted synthesis and characterization

A facile sonochemical route for the synthesis of graphene nanosheets via reduction of graphene oxide (GO) has been reported. The synthesized graphene sheets are characterized using UV–vis spectra, Fourier transform infra-red (FT-IR) spectra, transmission electron microscope, X-ray photoelectron spectra (XPS) and Raman spectroscopic techniques. The UV–vis spectroscopy results showed that the absorption peak was red shifted due to the reduction of GO into graphene. FT-IR and XPS spectra revealed the removal of oxygenated functional groups in graphene after the reduction process. Raman spectra confirmed the restoration of new sp² carbon domains in graphene sheets after the reduction. The sonochemical approach for the synthesis of graphene nanosheets is relatively fast, cost-effective and efficient as compared to other methods.     

Preparation and electrochemical properties of LiFePO<Subscript>4</Subscript>/graphene composites from tailoring graphene oxides

LiFePO₄/graphene composites have been prepared by using tailoring graphene oxide (GO) nanosheets as precursors. The structure and electrochemical properties of the composites were investigated by X-ray diffraction (XRD), atomic force microscopy (AFM), scanning electron microscopy (SEM), Raman microscopy, and a variety of electrochemical testing techniques. The decrease in graphene size reduces the contact resistance between activated materials, and enhances the lithium-ion transport in LiFePO₄/graphene composites. With low weight fractions of small-size graphene sheets, the composites show better electrochemical performance than those with large size graphene sheets.     

Buffer layer free large area bi-layer graphene on SiC(0 0 0 1)

The influence of hydrogen exposures on monolayer graphene grown on the silicon terminated SiC(0 0 0 1) surface is investigated using photoelectron spectroscopy (PES), low-energy electron microscopy (LEEM) and micro low-energy electron diffraction (μ-LEED). Exposures to ionized hydrogen are shown to have a pronounced effect on the carbon buffer (interface) layer. Exposures to atomic hydrogen are shown to actually convert/transform the monolayer graphene plus carbon buffer layer to bi-layer graphene, i.e. to produce carbon buffer layer free bi-layer graphene on SiC(0 0 0 1). This process is shown to be reversible, so the initial monolayer graphene plus carbon buffer layer situation is recreated after heating to a temperature of about 950 °C. A tentative model of hydrogen intercalation is suggested to explain this single to bi-layer graphene transformation mechanism. Our findings are of relevance and importance for various potential applications based on graphene-SiC structures and hydrogen storage.     

Frictional behavior of oxide graphene nanosheets as water-base lubricant additive

Oxide graphene (GO) nanosheets were prepared by modified Hummers and Offeman methods. The products were analyzed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectrometry (FTIR), and thermogravimetric analysis (TGA). The tribological properties of GO nanosheets as water-base lubricant additive were investigated using a UMT-2 ball-plate tribotester. By the addition of GO nanosheets in pure water, the antiwear ability was improved and the friction coefficient was decreased. The water with GO nanosheets showed better tribological properties than the water with oxide multiwall carbon nanotubes (CNTs-COOH). It is concluded that the formation of a thin physical tribofilms on the substrate can explain the good friction and wear properties of GO nanosheets.     

Low-temperature growth and properties of flower-shaped - Ni(OH)2 and NiO structures composed of thin nanosheets networks

Flower-shaped β- Ni(OH)₂ structures composed of thin nanosheet networks have been synthesized via the simple aqueous solution route by using nickel chloride and ammonium hydroxide at 65 C in 4 h. The general morphological observations revealed that the flowers are composed of thin nanosheets which were connected to each other in such a manner that they form network-like morphologies. Moreover, single-crystalline flower-shaped NiO structures composed of thin nanosheets were also obtained by thermal decomposition of flower-shaped β- Ni(OH)₂ structures. The shape of nanosheet networks in β- Ni(OH)₂ was sustained after thermal decomposition to NiO however, some broken nanosheets were also observed from the flower-shaped structures of NiO. The as-prepared products were characterized by X-ray powder diffraction (XRD), field emission scanning electron microscope (FESEM), transmission electron microscope (TEM), high-resolution TEM (HRTEM), Fourier transform infrared spectroscopy (FTIR), and Thermogravimetric analysis (TGA).     

Large single-crystal monolayer graphene by decomposition of methanol

We present a novel method for the synthesis of monolayer graphene with large single-crystal domains extending over 10–30 μm², produced by the decomposition of methanol on Cu in a single process step, in a flow of pure Ar gas, without H₂. Eliminating H₂ as a process gas offers increased safety and greatly facilitates fabrication scaling. The graphene grain size and orientation were characterized by selected area electron diffraction in transmission electron microscopy. Based on analyses of effluents from the furnace during the synthesis, a possible mechanism for graphene formation from methanol, involving carbon monoxide as an intermediate, is proposed.     

Bigraphene nanomeshes: Structure,properties, and formation

New carbon structures of nanomeshes have been considered, which are formed from bilayer graphene by cutting hexagonal holes in it. Edges of these holes by joining chemically active atoms, transforming into folds of graphene, form a closed structure of sp ₂ hybridized C atoms. The structure and electron properties of several typical nanomeshes, which are superlattices made of joined nanotube and bigraphene fragments, have been studied. Their stability and essential difference of the electronic band structure from those of their analogs-monolayer graphene nanomeshes—have been demonstrated.     

Density functional study of TaSin (n = 1-3, 12) clusters adsorbed to graphene surface

A plane-wave density functional theory (DFT) calculations have been performed to investigate structural and electronic properties of TaSi_n (n = 1-3, 12) clusters supported by graphene surface. The resulting adsorption structures are described and discussed in terms of stability, bonding, and electron transfer between the cluster and the graphene. The TaSi_n clusters on graphene surface favor their free-standing ground-state structures. Especially in the cases of the linear TaSi₂ and the planar TaSi₃, the graphene surface may catalyze the transition of the TaSi_n clusters from an isomer of lower dimensionality into the ground-state structure. The adsorption site and configuration of TaSi_n on graphene surface are dominated by the interaction between Ta atom and graphene. Ta atom prefers to adsorb on the hollow site of graphene, and Si atoms tend to locate on the bridge site. Further, the electron transfer is found to proceed from the cluster to the surface for n = 1 and 2, while its direction reverses as n > 2. For the case of TaSi, chemisorption is shown to prevail over physisorption as the dominant mode of surface-adsorbate interaction by charge density analysis.     

Effects of green laser fluence on the characteristics of graphene nanosheets synthesized by laser ablation method in liquid nitrogen medium

We have studied the effects of laser fluence on the characteristics of graphene nanosheets produced by pulsed laser ablation technique. In this work, The second harmonic of a Q-switched Nd:YAG laser at 532 nm wavelength and 5 Hz repetition rate with different laser fluences in the range of 0.5–1.8 J/cm² was used to irradiate the graphite target in liquid nitrogen medium. The products of ablation were characterized using Fourier transform infrared spectroscopy, field emission scanning electron microscopy, X-ray diffraction pattern, UV–Vis absorption spectroscopy, Raman spectrum and transmission electron microscopy. The Raman spectroscopy indicates that the quality of the graphene nanosheets was decreased while their structure defects were increased as the laser fluence was increased from 0.5 to 1.4 J/cm². Our results suggest that the amount of defects and the number of layers in graphene nanosheets can be changed by adjusting the laser fluence. This study could be a useful guidance for producing of high quality of graphene nanosheets by laser ablation method.     

Development of Novel Graphene/g‐C3N4 Composite with Broad‐Frequency and Light‐Weight Features

In this study, a novel graphene/g‐C₃N₄ microwave absorber is developed to solve the electromagnetic wave interference problem. Graphene/g‐C₃N₄ composite is synthesized by loading g‐C₃N₄ nanosheets on graphene through a simple liquid‐phase approach. High‐performance electromagnetic absorption performance can be achieved. The optimal reflection loss value is up to ?29.6 dB under a thin coating layer of 1.5 mm. At the same time, the corresponding absorption bandwidth of this composite can reach 5.2 GHz (12.8–18 GHz). Excellent electromagnetic absorption property may be attributed to the current attenuation theory which has been proven by replacing graphene with porous graphene or graphene oxide. The results reveal that free electron numbers and loading mass of g‐C₃N₄ on graphene play the key roles in the intensity of current attenuation and resistance value.     

Full Protection for Graphene‐Incorporated Micro‐/Nanocomposites Containing Ultra‐small Active Nanoparticles: the Best Li‐Storage Properties

In recent years, graphene‐incorporated micro‐/nanocomposites represent one of the hottest developing directions for the composite materials. However, a large number of active nanoparticles (NPs) are still in the unprotected state in most constructed graphene‐containing designs, which will seriously impair the effects of the graphene additives. Here, a fully protected Fe₃O₄‐based micro‐/nanocomposite (G/Fe₃O₄@C) is rationally developed by carbon‐boxing the common graphene/Fe₃O₄ microparticulates (G/Fe₃O₄). The processes and results of full protection are tracked in detail and characterized by X‐ray diffraction, X‐ray photoelectron spectroscopy, and nitrogen absorption–desorption isotherms, as well as scanning and transition electron microscopy. When used as the anode for lithium‐ion batteries, the fully protected G/Fe₃O₄@C exhibits the best lithium‐storage properties in terms of the highest rate capabilities and the longest cycle life compared to the common G/Fe₃O₄ composites and commercial Fe₃O₄ products. These much improved properties are mainly attributed to its novel structural features including complete protection of active Fe₃O₄ nanoparticles by the surface carbon box, a robust conductive network composed of nitrogen‐doped graphene nanosheets, ultra‐small Fe₃O₄ NPs of 4–5 nm, abundant mesopores to accommodate the volume variation during cycling, and micrometer‐sized secondary particles.     

Novel nanostructures of β-Ga2O3 synthesized by thermal evaporation

In this study, we report the novel β-Ga₂O₃ nanostructures synthesized by the thermal evaporation of Ga droplet in the presence of Au catalysts at 900 °C. The morphology and structure of the products were analyzed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray diffraction (XRD). The single-crystalline β-Ga₂O₃ nanosheets have lateral dimensions up to several tens of microns. Large arrays of column-like layered crystal β-Ga₂O₃ structures that consisted of many nanosheets were formed on the Au-coated silicon substrate under the suitable vapor concentration. These novel β-Ga₂O₃ nanostructures are expected to have potential application in functional nanodevices.     

Unique combination of zero–one–two dimensional carbon–titania hybrid for cold cathode application

A unique multi-dimensional hybrid system has been developed by incorporating titania nanoparticle into chemically synthesized amorphous carbon nanotubes (a-CNTs)-amorphous graphene composites. The as-synthesized samples were characterized by x-ray diffraction, scanning and transmission electron microscopy; Raman spectroscopy and photoluminescence spectroscopy. The microscopic studies confirm the attachment of the TiO₂ nanoparticles on carbon structures. The performance of the both the pure and hybrid samples as cold cathode emitter has been investigated and it has been found that cold emission performance of the pure carbon system improves considerably after TiO₂ nanoparticles being added to it giving a turn on field as low as 2.1 V/μm and enhancement factor 2746. The enhancement of field emission characteristic after TiO₂ addition was justified from the ‘ANSYS- Maxwell’ software based simulation study.     

Magnetic properties of carbon nanosheets

Two-dimensional carbon nanosheets have been fabricated using inductively coupled radio frequency plasma-enhanced chemical vapour deposition. The structural properties of the nanosheets have been characterised using atomic force microscopy, scanning electron microscopy and X-ray diffractometer. The magnetisation of the samples was studied using vibrating sample magnetometer. The magnetisation of the nanosheets was found to be diamagnetic for fast synthesis processes (30 and 60 min). On the other hand, the nanosheets exhibited a weak ferromagnetic response for the slow (120 min) synthesis process. Energy dispersive spectrometry and atomic absorption spectroscopy confirmed that the magnetisation exhibited by the carbon nanosheets was an intrinsic property and that it was not due to contamination from the substrate. Raman spectroscopy studies revealed that the ferromagnetic carbon nanosheets have a higher ratio (1.20) of graphite peak (I _G) to disordered peak (I _D) than normally expected (0.75–0.90). Available data indicated that the magnetisation was due to the presence of structural disorders.     

Rapid,Microwave‐Assisted,and One‐Pot Synthesis of Magnetic Palladium–CoFe2O4–Graphene Composite Nanosheets and Their Applications as Recyclable Catalysts

Here, a microwave‐assisted approach has been demonstrated to rapidly prepare magnetic Pd–CoFe₂O₄–graphene (GE) composite nanosheets in ethylene glycol (EG) solvent. The generation of both Pd and CoFe₂O₄ nanoparticles is accompanied with the reduction process of graphene oxide (GO) by EG. The surface morphologies and chemical composition of the composite nanosheets are characterized by transmission electron microscopy (TEM), energy‐dispersive X‐ray spectrometer (EDS), powder X‐ray diffraction (XRD), X‐ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR) measurements. The as‐prepared Pd–CoFe₂O₄–GE composite nanosheets exhibit a remarkable catalytic activity towards the reduction of 4‐nitrophenol by sodium borohydride (NaBH₄) at room temperature. The apparent kinetic rate constant (K _app) of this catalytic reaction could reach about 11.0 × 10^?3 s^?1. Moreover, the CoFe₂O₄ component exhibits a magnetic property, which could make the Pd–CoFe₂O₄–GE composite nanocatalysts separated from the suspension system. The catalytic conversion of the 4‐nitrophenol to 4‐aminophenol could reach 87.2% after four cycles. This work presents a simple, rapid, and versatile method to fabricate both metal and spinel‐type complex oxides on GE nanosheets, providing a new opportunity for their applications in the recyclable catalytic reaction.     

In situ growth of ultrashort rice-like CuO nanorods supported on reduced graphene oxide nanosheets and their lithium storage performance

A facile refluxing strategy in aqueous solution was engaged to synthesize ultrashort rice-like CuO nanorods/reduced graphene oxide (CuO-NRs/rGO) composite. The result of the high-resolution transmission electron microscopy shows that the as-synthesized rice-like CuO nanorods have a uniform size of about 8 nm in width and 28 nm in length and are homogenously dispersed on rGO nanosheets. The CuO nanorods are uniformly dispersed and immobilized by the graphene nanosheets reduced from GO. The resultant CuO-NRs/rGO composite as anode material for lithium-ion batteries displays better electrochemical properties than those of pure CuO-NRs and rGO nanosheets. The high reversible capacity and good stability can be ascribed to the presence of rGO nanosheets.     

Sulfonated reduced graphene oxide as a highly efficient catalyst for direct amidation of carboxylic acids with amines using ultrasonic irradiation

Sulfonated reduced graphene oxide nanosheets (rGO-SO₃H) were prepared by grafting sulfonic acid-containing aryl radicals onto chemically reduced graphene oxide (rGO) under sonochemical conditions. rGO-SO₃H catalyst was characterized by Fourier-transform infrared (FT-IR) spectroscopy, Raman spectroscopy, scanning electron microscopy (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC) and X-ray photoelectron spectroscopy (XPS). rGO-SO₃H catalyst was successfully applied as a reusable solid acid catalyst for the direct amidation of carboxylic acids with amines into the corresponding amides under ultrasonic irradiation. The direct sonochemical amidation of carboxylic acid takes place under mild conditions affording in good to high yields (56–95%) the corresponding amides in short reaction times.