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Register a new userEffect of the degree of oxidation of graphene oxide on As(III) adsorption
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Eddie Lopez-Honorato Dr
Publication date
2019
fields
Physics
and research's language is
English
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The study of the interaction between graphene oxide and arsenic is of great relevance towards the development of adsorbent materials and as a way to understand how these two materials interact in the environment. In this work we show that As(III) adsorption, primarily H3AsO3, by graphene oxide is dependent on its degree of oxidation. Variations in the concentration of potassium permanganate resulted in an increase on the C/O ratio from 1.98 to 1.35 with C-OH and C-O-C concentrations of 18 and 32%, respectively. Three oxidation degrees were studied, the less oxidized material reached a maximum As(III) adsorption capacity of 124 mg/g, whereas the graphene with the highest degree of oxidation reached a value of 288 mg/g at pH 7, to the authors knowledge, the highest reported in the literature. The interaction between graphene oxide and As(III) was also studied by Density Functional Theory (DFT) computer models showing that graphene oxide interacts with As(III) primarily through hydrogen bonds, having interaction energies with the hydroxyl and epoxide groups of 378 and 361 kcal/mol, respectively. Finally, cytotoxicity tests showed that the graphene oxide had a cellular viability of 57% with 50 {mu}g/ml, regardless of its degree of oxidation.
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The laminated structure of graphene oxide (GO) confers unique interactions with water molecules which may be utilised in a range of applications that require materials with tuneable hygroscopic properties. Precise roles of the expandable interlayer spacing and functional groups in GO laminates are not fully understood till date. Herein, we report experimental and theoretical study on the adsorption and desorption behaviour of water in GO laminates as a function of relative pressure. We have observed that GO imparts excellent water uptake capacity of up to 0.58 gram of water per gram of GO (g g-1), which is much higher than silica gel a conventional desiccant material. More interestingly, the adsorption and desorption kinetics of GO is one order of magnitude higher than silica gel. The observed extraordinary adsorption/desorption rate can be attributed to the high capillary pressure in GO laminates as well as micro meter sized tunnel like wrinkles located at the surface.
The effect of oxygen adsorption on the local structure and electronic properties of monolayer graphene grown on SiC(0001) has been studied by means of Low Energy Electron Microscopy (LEEM), microprobe Low Energy Electron Diffraction (muLEED) and microprobe Angle Resolved Photoemission (muARPES). We show that the buffer layer of epitaxial graphene on SiC(0001) is partially decoupled after oxidation. The monitoring of the oxidation process demonstrates that the oxygen saturates the Si dangling bonds, breaks some Si-C bonds at the interface and intercalates the graphene layer. Accurate control over the oxidation parameters enables us to tune the charge density modulation in the layer.
The adsorption energies and orientation of methanol on graphene are determined from first-principles density functional calculations. We employ the well-tested vdW-DF method that seamlessly includes dispersion interactions with all of the more close-ranged interactions that result in bonds like the covalent and hydrogen bonds. The adsorption of a single methanol molecule and small methanol clusters on graphene are studied at various coverages. Adsorption in clusters or at high coverages (less than a monolayer) is found to be preferable, with the methanol C-O axis approximately parallel to the plane of graphene. The adsorption energies calculated with vdW-DF are compared with previous DFT-D and MP2-based calculations for single methanol adsorption on flakes of graphene (polycyclic aromatic hydrocarbons). For the high coverage adsorption energies we also find reasonably good agreement with previous desorption measurements.
Graphene oxide (GO), the functionalized graphene with oxygenated groups (mainly epoxy and hydroxyl), has attracted resurgent interests in the past decade owing to its large surface area, superior physical and chemical properties, and easy composition with other materials via surface functional groups. Usually, GO is used as an important raw material for mass production of graphene via reduction. However, under different conditions, the coverage, types, and arrangements of oxygen-containing groups in GO can be varied, which give rise to excellent and controllable physical properties, such as tunable electronic and mechanical properties depending closely on oxidation degree, suppressed thermal conductivity, optical transparency and fluorescence, and nonlinear optical properties. Based on these outstanding properties, many electronic, optical, optoelectronic, and thermoelectric devices with high performance can be achieved on the basis of GO. Here we present a comprehensive review on recent progress of GO, focusing on the atomic structures, fundamental physical properties, and related device applications, including transparent and flexible conductors, field-effect transistors, electrical and optical sensors, fluorescence quenchers, optical limiters and absorbers, surface enhanced Raman scattering detectors, solar cells, light-emitting diodes, and thermal rectifiers.
Vanadium dioxide (VO2) is a phase transition material that undergoes a reversible insulator-metal phase transition at ~ 68 C. Atmospheric pressure thermal oxidation (APTO) of vanadium (V) is a simple VO2 synthesis method in which V thin film is oxidized in open air. For an optimum oxidation duration, VO2 films are obtained with good phase transition properties. We recently reported a modified APTO process using a step temperature profile for oxidation (Thin Solid Films 706, 138003 (2020)). We demonstrated an ultra-low thermal budget synthesis of VO2 thin films with good electrical and optical phase transition properties. For a 130 nm room-temperature RF sputtered V thin film, an optimum oxidation duration of ~ 30 s was obtained. In this work, we study how the starting V film thickness and deposition temperature affects the optimum oxidation duration. V thin films of varying thickness (15-212 nm) and 120 nm thick V films with varying deposition temperature (~27-450 C) are prepared using RF magnetron sputtering. These films are oxidized for different oxidation durations and characterized using Raman and four-probe measurements to find the optimum oxidation duration for each deposition condition. We find that the optimum oxidation duration increases with the increase in V film thickness and V deposition temperature. We model the effect of V film thickness and deposition temperature on the optimal oxidation time using a parabolic law which can be used to obtain the optimal oxidation times for intermediate V thicknesses/deposition temperatures.
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