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Synthesis, Properties and Applications of Graphene Oxide

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A special issue of Coatings (ISSN 2079-6412).

Deadline for manuscript submissions: closed (31 December 2020) | Viewed by 24629

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Special Issue Editor

Prof. Dr. Mercedes Velazquez

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Departamento de Química Física, Facultad de Ciencias Químicas, Universidad de Salamanca, Salamanca 37008, Spain
Interests: graphene oxides; nanoparticle films; surfactants; polymers; interfaces; langmuir monolayers; langmuir-blodgett films
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Special Issue Information

Dear Colleagues,

Graphene has emerged as a new material with a bright future due to its unique properties that include high charge mobility, high thermal conductivity, transparency and good mechanical properties. Due to these extraordinary properties, graphene has been proposed as a promising candidate for the manufacture of transparent conducting electrodes, transistors, hydrogen storage, and gas sensors. However, each application requires a different set of properties. Thus, graphene synthesized by chemical vapor deposition (CVD) or micromechanical exfoliation renders high-quality sheets suitable for electronic applications; however, these materials cannot be used for the fabrication of inks or composites because they do not present functionalized groups. In these cases, Graphene Oxides (GO) is preferred because it contains reactive O-groups that can attach small molecules, polymers, or nanoparticles to the basal plane for potential use in polymer composites, gas sensors, or photovoltaic applications. Despite the great interest raised by graphene oxide, its chemical structure is still subject to debate. The variability of the starting material and the oxidation protocols seem to be the main cause for differences. Therefore, an understanding and control of the GO structure is crucial in the preparation of films based on graphene oxide for designing new technological devices. Therefore, the understanding and control of the GO structure is crucial in the preparation of films based on graphene oxide with improving properties. This special issue has the purpose of addressing the recent fundamental and applied aspects used in the design of new materials based on graphene oxide with potential technological applications.

In particular, the topics of interest include, but are not limited to:

Preparation and characterization of graphene oxide films;
Graphene oxide-based sensors;
Graphene oxide-based nanocomposites;
Transparent Conductive Films;
Graphene Oxide films for energy harvesting and storage;
Biomedical applications of Graphene Oxide

Prof. Dr. Mercedes Velazquez
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Coatings is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Related Special Issue

Graphene-Based Nanomaterials: Synthesis, Properties, and Applications in Coatings (1 article)

Published Papers (7 papers)

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Research

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10 pages, 818 KiB

Open AccessFeature PaperArticle

Multi-Layer Graphene Oxide in Human Keratinocytes: Time-Dependent Cytotoxicity, Proliferation, and Gene Expression

by Beatriz Salesa and Ángel Serrano-Aroca

Coatings 2021, 11(4), 414; https://0-doi-org.brum.beds.ac.uk/10.3390/coatings11040414 - 02 Apr 2021

Cited by 13 | Viewed by 2365

Abstract

Few-layer graphene oxide (GO) has shown no or very weak cytotoxicity and anti-proliferative effects in a wide range of cell lines, such as glioma cells and human skin HaCaT cells at concentrations up to 100 µg/mL. However, as multi-layer GO has hardly been explored in the biomedical field, in this study, this other type of GO was examined in human keratinocyte HaCaT cells treated with different concentrations, ranging from 0.01 to 150 µg/mL, for different periods of time (3, 12, and 24 h). The results revealed a time–concentration dependence with two non-cytotoxic concentrations (0.01 and 0.05 µg/mL) and a median effective concentration value of 4.087 µg/mL at 24 h GO exposure. Contrary to what has previously been reported for few-layer GO, cell proliferation of the HaCaT cells in contact with the multi-layer GO at 0.01 μg/mL showed identical proliferative activity to an epidermal growth factor (1.6-fold greater than the control group) after 96 h. The effects of the multi-layer GO on the expression of 13 genes (SOD1, CAT, MMP1, TGFB1, GPX1, FN1, HAS2, LAMB1, LUM, CDH1, COL4A1, FBN, and VCAN) at non-cytotoxic concentrations of GO in the HaCaT cells were analyzed after 24 h. The lowest non-cytotoxic GO concentration was able to upregulate the CAT, TGFB1, FN1, and CDH1 genes, which confirms multi-layer GO’s great potential in the biomedical field. Full article

(This article belongs to the Special Issue Synthesis, Properties and Applications of Graphene Oxide)

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18 pages, 3895 KiB

Open AccessArticle

The Role of the Oxidation and Reduction Parameters on the Properties of the Reduced Graphene Oxide

by Marta Sieradzka, Czesław Ślusarczyk, Włodzimierz Biniaś and Ryszard Fryczkowski

Coatings 2021, 11(2), 166; https://0-doi-org.brum.beds.ac.uk/10.3390/coatings11020166 - 31 Jan 2021

Cited by 19 | Viewed by 2889

Abstract

One of the methods of obtaining reduced graphene oxide (rGO) involves the oxidation of graphite to graphene oxide, which is then exfoliated and reduced. Each of these stages has a decisive influence on the properties of the produced nanoadditive, which determines its subsequent application. The process conditions which are examined during the oxidation stage are related to: The mixing time of the reactants before oxidation, sonication of the reaction mixture, and its composition. During reduction optimization, in turn, the form of the GO sample and the method of its purification, as well as the temperature at which this process took place, are examined. At each stage, the determined structural parameters of the produced materials (GO and rGO) are related to their morphology (SEM—scanning electron microscope), oxidation state (FTIR—Fourier transform infrared spectroscopy, EDS—energy-dispersive spectrometer), structure defect (Raman spectroscopy), as well as the number of layers and crystalline structure (WAXS—wide-angle X-ray scattering). The obtained results show that the shorter mixing time of the reactants determines the formation of more oxygen functional groups. On the basis of the obtained results, the process conditions that enable the production of multilayer, well-exfoliated reduced graphene oxide, with only a slightly defected structure, are established. Full article

(This article belongs to the Special Issue Synthesis, Properties and Applications of Graphene Oxide)

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11 pages, 2156 KiB

Open AccessArticle

Graphene Oxide/Polyaniline Nanocomposites Used in Anticorrosive Coatings for Environmental Protection

by Shuanqiang Yang, Shu Zhu and Ruoyu Hong

Coatings 2020, 10(12), 1215; https://0-doi-org.brum.beds.ac.uk/10.3390/coatings10121215 - 12 Dec 2020

Cited by 56 | Viewed by 4060

Abstract

In recent years, metal corrosion causes serious threats to the economy of the world and the living environment. Hence, it is very important to seek non-toxic and environmentally friendly materials with metal anti-corrosion properties for the sustainable development of society. The barrier properties of graphene oxide (GO) and the special electrochemical property of polyaniline (PANI) can significantly improve the corrosion resistance of metals. Herein, we developed an in-situ polymerization method to prepare graphene oxide/polyaniline (GO/PANI) nanocomposites with unique anti-corrosion properties. The obtained GO/PANI nanocomposites were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, thermalgravimetric analysis, UV–vis spectroscopy and scanning electron microscopy. The as-prepared composite materials were uniformly dispersed in epoxy resin to prepare anticorrosive coatings and coated on the surface of steel. The anti-corrosion performance of the coatings was measured by electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization technique. The EIS results showed that the total impedance of epoxy/GO/PANI coatings is greater than epoxy/PANII coatings, and the impedance module value can reach 8.67 × 10⁸ Ω·cm². In general, it is concluded that the anti-corrosion performance of GO/PANI coating is significantly higher than PANI coating and pure GO coating. Full article

(This article belongs to the Special Issue Synthesis, Properties and Applications of Graphene Oxide)

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10 pages, 3223 KiB

Open AccessArticle

Variable Angle Spectroscopic Ellipsometry Characterization of Reduced Graphene Oxide Stabilized with Poly(Sodium 4-Styrenesulfonate)

by Grazia Giuseppina Politano, Carlo Vena, Giovanni Desiderio and Carlo Versace

Coatings 2020, 10(8), 743; https://0-doi-org.brum.beds.ac.uk/10.3390/coatings10080743 - 29 Jul 2020

Cited by 12 | Viewed by 2986

Abstract

Lately, the optical properties of Graphene Oxide (GO) and Reduced Graphene Oxide (RGO) films have been studied in the ultraviolet and visible spectral range. However, the accurate optical properties in the extended near-infrared and mid-infrared range have not been published yet. In this work, we report a Variable Angle Spectroscopic Ellipsometry (VASE) characterization of GO thin films dip-coated on SiO₂/Si substrates and thermally reduced GO films in the 0.38–4.1 eV photon energy range. Moreover, the optical properties of RGO stabilized with poly(sodium 4-styrenesulfonate) (PSS) films dip-coated on SiO₂/Si substrates are studied in the same range for the first time. The Lorentz optical models fit well with the experimental data. In addition, the morphological properties of the samples were investigated by Scanning Electron Microscopy (SEM) analysis. Full article

(This article belongs to the Special Issue Synthesis, Properties and Applications of Graphene Oxide)

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12 pages, 4947 KiB

Open AccessArticle

Enhancement of the Electrochemical Properties of an Open-Pore Graphite Foam with Electrochemically Reduced Graphene Oxide and Alternating Current Dispersed Platinum Particles

by Javier Fernández, José Bonastre, José Miguel Molina and Francisco Cases

Coatings 2020, 10(6), 551; https://0-doi-org.brum.beds.ac.uk/10.3390/coatings10060551 - 08 Jun 2020

Cited by 2 | Viewed by 1998

Abstract

This paper aimed to improve the electrochemical activity of a pitch-derived open-pore graphite foam (GF) by an electrochemical coating of reduced graphene oxide (RGO) and platinum particles without significantly affecting its 3D-structure. RGO was synthesized using cyclic voltammetry (CV) from a 3 g L⁻¹ GO and 0.1 M LiClO₄ solution. For the electrodeposition of Pt particles, an alternating current method based on electrochemical impedance spectroscopy (EIS) was used. A sinusoidal voltage from a fixed potential Ei was varied following a selected amplitude (ΔE_ac = ± 0.35 V) in a frequency range of 8 Hz ≤ f_i ≤ 10Hz, where i = 500. This method proved its efficiency when compared to the traditional CV by obtaining more highly electroactive coatings in less synthesis time. For samples’ characterization, physical measures included permeability, pressure drop, and nitrogen adsorption isotherms. The electrochemical characterization was performed by CV. The surface morphology and chemical composition were examined using field emission electron microscopy (FESEM) and energy-dispersive X-ray spectroscopy (EDX), respectively. RGO improved the electron transfer rate constant of GF, and a more homogeneous coating distribution of reduced size Pt particles was obtained. Full article

(This article belongs to the Special Issue Synthesis, Properties and Applications of Graphene Oxide)

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12 pages, 1722 KiB

Open AccessArticle

Towards Understanding the Raman Spectrum of Graphene Oxide: The Effect of the Chemical Composition

by David López-Díaz, Juan A. Delgado-Notario, Vito Clericò, Enrique Diez, María Dolores Merchán and María Mercedes Velázquez

Coatings 2020, 10(6), 524; https://0-doi-org.brum.beds.ac.uk/10.3390/coatings10060524 - 29 May 2020

Cited by 43 | Viewed by 6391

Abstract

Raman spectroscopy is a technique widely used to detect defects in semiconductors because it provides information of structural or chemical defects produced in its structure. In the case of graphene monolayer, the Raman spectrum presents two bands centered at 1582 cm⁻¹ (G band) and 2700 cm⁻¹ (2D band). However, when the periodic lattice of graphene is broken by different types of defects, new bands appear. This is the situation for the Raman spectrum of graphene oxide. It is well established that the existence of these bands, the position and the intensity or width of peaks can provide information about the origin of defects. However, in the case of the graphene oxide spectrum, we can find in the literature several discrepant results, probably due to differences in chemical composition and the type of defects of the graphene oxide used in these studies. Besides, theoretical calculations proved that the shape of bands, intensity and width, and the position of graphene oxide Raman spectrum depend on the atomic configuration. In the current work, we will summarize our current understanding of the effect of the chemical composition on the Raman spectrum of graphene oxide. Finally, we apply all this information to analyze the evolution of the structure of graphene oxide during the thermal annealing of the heterostructures formed by graphene oxide sandwiches in a hexagonal boron nitride. Full article

(This article belongs to the Special Issue Synthesis, Properties and Applications of Graphene Oxide)

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Review

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18 pages, 7413 KiB

Open AccessReview

Reduction of Graphene Oxide Using an Environmentally Friendly Method and Its Application to Energy-Related Materials

by Ichiro Imae

Coatings 2021, 11(3), 297; https://0-doi-org.brum.beds.ac.uk/10.3390/coatings11030297 - 04 Mar 2021

Cited by 10 | Viewed by 3080

Abstract

Since graphene oxide can be synthesized in large quantities by oxidation of inexpensively available natural graphite and can be dispersed in water, it can be coated onto a variety of substrates by solution processes. Graphene oxide can also be reduced to yield reduced graphene oxide, which has similar electronic features to graphene. This review introduces the environmentally friendly methods for the synthesis of reduced graphene oxide utilizing electrochemical and thermal methods and summarizes our recent research results on their application to energy-related materials such as electric double-layer capacitors, thermoelectric devices, transparent conductive films, and lithium-ion secondary batteries. Full article

(This article belongs to the Special Issue Synthesis, Properties and Applications of Graphene Oxide)

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