Transport properties of progressively reduced graphene oxide (GO) are described. Evolution of the electronic properties reveals that as-synthesized GO undergoes insulator-semiconductor-semi-metal transitions with reduction. The apparent transport gap ranges from 10 ~ 50 meV and approaches zero with extensive reduction. Measurements at varying degrees of reduction reveal that transport in reduced GO occurs via variable-range hopping and further reduction leads to increased number of available hopping sites.
Here, the possibility of the existence of nitro-graphene derivatives with undisturbed graphene backbone is considered. Based on the first-principles calculation, it is shown that while NO$_2$ is unable to form a covalent bond with bare graphene, it becomes possible in some structures of graphane, fluorographene, and graphene oxide. This paper presents, among others, an analysis of the surrounding influence on the C-NO$_2$ bond strength. The author believes, that potential prospects of these materials and discussion about possible synthesizing routes may help further research on graphene-based …
Graphene oxide continues to amaze scientific community for multiple potentials in a broad span of applications such as catalysts, adsorbents, oxidants, etc., determined by constant unveiling of its fantastic natures. Of them, magnetism is not ultimately identified and directly observed by naked eyes. Herein, we report graphene oxide directionally migrated and deposited together simply under external magnetic field from common Nd-Fe-B magnet, whereas the ferromagnetism of graphene oxide did not exhibit that strong as iron. Therefore, we illustrated this interesting pathway to keep close to such…
Environmental contamination and human exposure to dyes have dramatically increased over the past decades because of their increasing use in such industries as textiles, paper, plastics, tannery and paints. These dyes can cause deterioration in water quality by imparting color to the water and inducing the photosynthetic activity of aquatic organisms by hindering light penetration. Moreover, some of the dyes are considered carcinogenic and mutagenic for human health. Therefore, efficient treatment and removal of dyes from wastewater have attracted considerable attention in recent years. Photoca…
Graphene oxide (GO) is regarded as one typical two-dimension structured oxygenated planar molecular material. Researchers across multiple disciplines have paid enormous attention to it due to unique physiochemical properties. However, models used to describe the structure of GO are still in argument and ongoing to update. Currently, synthesis methods for massive production are seemingly abundant but in fact, dominated by few thought systems. We herein aim to give a mini but critical review over the synthesis of graphene oxide as well as its structure, involving relative peer work.
In this study, we report a different strategy to prepare graphene nanopapers from direct vacuum filtration. Instead of the conventional method, i.e. thermal annealing nanopapers at extremely high temperatures prepared from graphene oxide (GO) or partially reduced GO, we fabricate our graphene nanopapers directly from suspensions of fully reduced graphene oxide (RGO), obtained after RGO and thermally annealing at 1700 °C in vacuum. By using this approach, we studied the effect of thermal annealing on the physical properties of the macroscopic graphene-based papers. Indeed, we demonstrated that …
Molybdenum disulfide (MoS$_2$) attracts attention as a high efficient and low cost photocatalyst for hydrogen production, but suffers from low conductance and high recombination rate of photo-generated charge carriers. In this work, we investigate the MoS$_2$ heterostructures with graphene variants (GVs), including graphene, graphene oxide, and their boron- and nitrogen-doped variants, by using first-principles calculations. Systematic comparison between graphene and graphene oxide composites is performed, and contrary effect of B and N doping on interface function and hydrogen evolution is cl…
Reduced graphene oxide becomes one of the most popular materials for applications in various optical, electronic and sensor devices. Even though many methods have been already reported for reduced graphene oxide synthesis, they usually rise issues related to their efficiency, quality and environmental impact. This work demonstrates a simple, environmentally friendly and effective method for reducing graphene oxide under ambient conditions using nanosecond infrared laser irradiation. As a result, a Raman band intensity ratio of I(G)/I(D) of 4.59 was achieved with an average crystallite size of …
Plane Wave Density Functional Theory Studies of the Structural and the Electronic Properties of Amino Acids Attached to Graphene Oxide via Peptide Bonding
The integration of two-dimensional (2D) materials with functional non-2D materials such as metal oxides is of key importance for many applications, but underlying mechanisms for such non-2D/2D interfacing remain largely elusive at the atomic scale. To address this, we here investigate the nucleation stage in atomic layer deposition (ALD) of the important metal oxide HfO2 on chemical vapor deposited graphene using atomically resolved and element specific scanning transmission electron microscopy (STEM). To avoid any deleterious influence of polymer residues from pre-ALD graphene transfers we em…
Graphene oxide is a rising star among 2D materials, yet its interaction with liquid water remains a fundamentally open question: experimental characterization at the atomic scale is difficult, and modelling by classical approaches cannot properly describe chemical reactivity. Here, we bridge the gap between simple computational models and complex experimental systems, by realistic first-principles molecular simulations of graphene oxide (GO) in liquid water. We construct chemically accurate GO models and study their behavior in water, showing that oxygen-bearing functional groups (hydroxyl and…
Among the recent achievements of sodium-ion battery (SIB) electrode materials, hybridization of two-dimentional (2D) materials is one of the most interesting appointments. In this work, we propose to use the 2D hybrid composites of SnS2 with graphene or graphene oxide (GO) layers as SIB anode, based on the first-principles calculations of their atomic structures, sodium intercalation energetics and electronic properties. The calculations reveal that graphene or GO film can effectively support not only the stable formation of hetero-interface with the SnS2 layer but also the easy intercalation …
Thermoplastic elastomeric nanocomposites based on poly(trimethylene terephthalate-block-poly(tetramethylene oxide) copolymer (PTT-PTMO) and graphene oxide-Fe3O4 nanoparticle hybrid were prepared by in situ polymerization. Superparamagnetic GO-Fe3O4 hybrid nanoparticles before introducing to elastomeric matrix were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), thermogravimetric analysis (TGA) and scanning electron microscopy (SEM). The effect of loading (0.3 and 0.5 wt%) of GO-Fe3O4 nanoparticle hybrid on the phase structure, tensile and magnetic properties o…
The ring opening polymerization of cyclic butylene terephthalate into poly (butylene terephthalate) (pCBT) in the presence of reduced graphene oxide (RGO) is an effective method for the preparation of polymer nanocomposites. The inclusion of RGO nanoflakes dramatically affects the crystallization of pCBT, shifting crystallization peak temperature to higher temperatures and, overall, increasing the crystallization rate. This was due to a super nucleating effect caused by RGO, which is maximized by highly reduced graphene oxide. Furthermore, combined analyses by differential scanning calorimetry…
Adsorption is one important way applied to water decontamination, where carbon is commonly used as highly effective absorbent. Carbon of different morphologies and structures normally demonstrate distinct capabilities to adsorption-typed decontaminations. Graphene oxide is regarded as the oxidative derivative of graphene, maintaining its 2D morphology-featuring structure while location-dependently immobilized with a large amount of various oxygen-involving functional moieties on both sides. Free-standing graphene oxide tends to fully unfold in water and behave in macromolecular-like Brownian m…
Broadband Dielectric Spectroscopy (BDS) measurements of Pοlyaniline/Graphene oxide composites were conducted for an as-prepared and a thermally annealed specimen, respectively, from 15K to room temperature. Electrical conductivity values of the annealed composite display a very modest rise denoting the important contributions of the GO component to achieving electrical stability of the polymer. Patterns of the dc conductivity as a function of temperature also reveal a metal to insulator transition around 75K. The transition is dominated by two key factors; temperature and annealing process. Me…
The author reports an experimental study of electrical and thermal transport in reduced graphene oxide (RGO)/polystyrene (PS) composites. The electrical conductivity ($σ$) of RGO/PS composites with different RGO concentrations at room temperature shows a percolation behavior with the percolation threshold of ~ 0.25 vol.%. Their temperature-dependent electrical conductivity follows Efros-Shklovskii (ES) variable range hopping (VRH) conduction in the temperature range of 30 to 300 K. The thermal conductivity ($κ$) of composites is enhanced by ~ 90 % as the concentration is increased from 0 to 10…
The epitaxial-graphene/graphene-oxide junction, an essential step towards epitaxial graphene electronics
已经沉积氧化石墨烯(GO)薄片以桥接两个外延石墨烯电极之间的间隙以产生全石墨烯装置。电学测量表明,由于GO中的带隙,在石墨烯/氧化石墨烯结处存在肖特基势垒(SB)。发现势垒高度约为0.7 eV,并且在180 $^\circ$ C退火后降低,这意味着可以通过改变氧化程度来调节间隙。发现GO迁移率的下限为850 cm $^2$ /Vs,与硅相当。已经实现了图案化外延石墨烯的{ \it In situ}局部氧化。
We investigate nanoscale local anodic oxidation (LAO) on hydrogen-intercalated graphene grown by controlled sublimation of silicon carbide (SiC). Scanning probe microscopy (SPM) was used as a lithographic and characterization tool in order to investigate the local properties of the nanofabricated structures. The anomalous thickness observed after the graphene oxidation process is linked to the impact of LAO on the substrate. Micro-Raman spectroscopy was employed to demonstrate the presence of two oxidation regimes depending on the applied bias. We show that partial and total etching of monolay…
Growth of perovskite oxide thin films on Si in crystalline form has long been a critical obstacle for the integration of multifunctional oxides into Si-based technologies. In this study, we propose pulsed laser deposition of a crystalline SrTiO3 thin film on a Si using graphene substrate. The SrTiO3 thin film on graphene has a highly (00l)-oriented crystalline structure which results from the partial epitaxy. Moreover, graphene promotes a sharp interface by highly suppressing the chemical intermixing. The important role of graphene as a 2D substrate and diffusion barrier allows expansion of de…
We study local electronic properties of graphene oxide (GO) and reduced graphene oxide (RGO) on metallic (Pt) and insulating (Si3N4) substrates in controlled humidity environment. We demonstrate that the supporting substrate plays a crucial role in interaction of these materials with water, with Pt making both GO and RGO insensitive to humidity variations and change in environment. On the other hand, in the case of Si3N4 substrate a significant difference between GO and RGO with respect to humidity variations is demonstrated, indicating complete water coverage at ~60% R.H for RGO and ~30% R.H.…
Hydration properties of graphene oxide (GO) are essential for most of its potential applications. In this work, we employ atomistic molecular dynamics simulations to investigate seven GO compositions with different levels of oxygenation. Two atomic charge models for GO are compared: (1) sp2 carbons are purely Lennard-Jones sites; (2) sp2 carbon charges are consistent with the CHELPG scheme. Structural properties were found to depend insignificantly on the charge model, whereas thermodynamics appeared very sensitive. In particular, the simplified model provides systematically stronger GO/water …
Covalent Hybrid of Spinel Manganese-Cobalt Oxide and Gra-phene as Advanced Oxygen Reduction Electrocatalysts
通过在氮掺杂的还原氧化石墨烯片上直接成核和生长纳米颗粒以及阳离子取代尖晶石Co 3 O 4纳米颗粒,开发了锰-钴尖晶石MnCo 2 O 4/石墨烯杂化物作为碱性条件下氧还原反应(ORR)的高效电催化剂。电化学和X射线近边结构(XANES)研究表明,形成无机纳米碳杂化物的成核和生长方法导致尖晶石氧化物纳米颗粒和N掺杂的还原氧化石墨烯(N-rmGO)片之间的共价偶联。碳K边和氮K边XANES显示N-rmGO片中的C-O和C-N键强烈扰动,表明N掺杂的氧化石墨烯和尖晶石氧化物纳米颗粒之间形成C-O-金属和C-N-金属键。Co L-edge和Mn L-edge XANES分析表明,Mn 3+取代了Co 3+位,提高了杂化材料中催化位的活性,从而进一步提高了杂化材料的ORR活性.共价键合的杂化物比纳米颗粒和包括N-rmGO的碳材料的物理混合物提供更大的活性和耐久性。在相同的质量负载下,MnCo 2 O 4/N-graphene杂化物在中等过电位下的ORR电流密度可以超过Pt/C,并且在碱性溶液中具有优于Pt/C的稳定性。
The reduction of graphene oxide is one of the most facile methods to fabricate a large amount of graphene and the reduction rate of graphene oxide is related with the quality of synthesized graphene for its possible application. The reduction rate is usually determined by using various spectroscopy measurements such as Raman spectroscopy, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. Here we propose that the magnetic data can be used as a means of determining the quality of graphene oxide (GO) and reduced graphene oxide (RGO) by the investigation of close relat…
Magnetic insulators with strong perpendicular magnetic anisotropy (PMA) play a key role in exploring pure spin current phenomena and developing ultralow-dissipation spintronic devices, thereby it is highly desirable to develop new material platforms. Here we report epitaxial growth of La2/3Sr1/3MnO3 (LSMO)-SrIrO3 (SIO) composite oxide films (LSMIO) with different crystalline orientations fabricated by sequential two-target ablation process using pulsed laser deposition. The LSMIO films exhibit high crystalline quality with homogeneous mixture of LSMO and SIO at atomic level. Ferrimagnetic and …
Graphene oxide membranes show exceptional molecular permeation properties, with a promise for many applications. However, their use in ion sieving and desalination technologies is limited by a permeation cutoff of ~9 Angstrom, which is larger than hydrated ion diameters for common salts. The cutoff is determined by the interlayer spacing d ~13.5 Angstrom, typical for graphene oxide laminates that swell in water. Achieving smaller d for the laminates immersed in water has proved to be a challenge.Here we describe how to control d by physical confinement and achieve accurate and tuneable ion sie…
Cubic spinel lithium manganese oxide (LiMn2O4) has been able to attract a great deal of attention over the years as a promising cathode material for large scale lithium ion batteries. Here a facile hydrothermal route followed by solid state reaction is developed using as grown ultrafine alpha-MnO2 nanorods to prepare one dimensional LiMn2O4 with 10-50nm diameters. To enhance the cathodic property of these nanorods, a unique synthesis technique of heat treatment is developed to grow 2D graphene oxide sheet enveloping 1D LiMn2O4 as interconnected framework. This nanocomposite 3D porous cathode e…
Large variety of structure and chemical-composition of reduced graphene oxide (RGO) is explained from a quantum-chemical standpoint. The related molecular theory of graphene oxide, supported by large experience gained by the modern graphene science, has led the foundation of the concept of a multi-stage graphene oxide reduction. This microscopic approach has found a definite confirmation when analyzing the available empirical data concerning both synthetic and natural RGO products, the latter in view of shungite carbon, suggesting the atomic-microscopic model for its structure.