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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: closed (31 July 2023) | Viewed by 22347

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Dr. Chiara Ingrosso

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CNR-Istituto per i Processi Chimico Fisici (CNR-IPCF), SS Bari, Via Orabona 4, 70126 Bari, Italy
Interests: synthesis and characterization of colloidal nanoparticles; surface chemistry and functionalization of colloidal nanoparticles; synthesis and characterization of graphene based hybrid nanocomposites; preparation and characterization of polymer based hybrid nanocomposites; assembly; photodetectors, (bio)sensors and energy conversion applications

Special Issue Information

Dear Colleagues,

Graphene is a single-layer two-dimensional material that has interested the scientific community as an extraordinarily attractive component for applications in biomedicine, energy storage, energy conversion, and environmental science. Graphene has unique structural properties, such as a high optical transparency from visible to infrared, high surface area, good biocompatibility, excellent thermal and electrical conductivity, high mechanical strength, and high flexibility. The high chemical reactivity of the two-dimensional graphene basal plane opens the possibility for the implementation of a large variety of chemical strategies for functionalization. When graphene is modified with organic and inorganic nanoparticles by means of an interface designed to allow electronic coupling between the components, nanostructured nanocomposites exhibiting enhanced component pristine functionalities and/or novel properties arising from the merging of the outstanding properties of graphene and nanoparticles can be achieved for a plethora of advanced technological applications.

This Special Issue aims to publish research articles, short communications, and review articles reporting new avenues in the synthesis, characterization, and application of hybrid nanocomposites based on graphene and nanoparticles; exhibiting novel/enhanced functionalities; and/or with potential applications in sensors, energy conversion, storage, and photocatalysis that have not yet been published or that are not currently under review by other journals or peer-reviewed conferences.

Dr. Chiara Ingrosso
Guest Editor

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Keywords

nanostructures
graphene nanocomposites
synthesis
surface functionalization
sustainable procedures
green chemistry
electrodes
thin films
sensors
photocatalysis
energy conversion
energy storage

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Published Papers (9 papers)

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Research

14 pages, 4451 KiB

Open AccessArticle

Graphene Oxide Enhanced Cisplatin Cytotoxic Effect in Glioblastoma and Cervical Cancer

by Kacper Kregielewski, Wiktoria Fraczek and Marta Grodzik

Molecules 2023, 28(17), 6253; https://doi.org/10.3390/molecules28176253 - 25 Aug 2023

Cited by 4 | Viewed by 1501

Abstract

Graphene oxide (GO) is an oxidized derivative of graphene. So far, GO has mostly been studied as a drug delivery method rather than a standalone drug for treating cancers like glioblastoma or cervical cancer. However, we propose a promising new approach—using GO as a sensitizer for cisplatin chemotherapy. Here, we analyze the effects of triple GO pretreatment, followed by cisplatin treatment, on cancerous cell lines U87 and HeLa, as well as the noncancerous cell line HS-5, through morphology analysis, viability assay, flow cytometry, and LDH release assay. The viability assay results showed that GO treatment made U87 and HeLa cells more responsive to cisplatin, leading to a significant reduction in cell viability to 40% and 72%, respectively, without affecting HS-5 cells viability, while the Annexin V/Propidium iodine assay showed that GO pretreatment did not cause a change in live cells in all three examined cell lines, while GO-pretreated HeLa cells treated with cisplatin showed significant decrease around two times compared to cells treated with cisplatin standalone. The U87 cell line showed a significant increase in LDH release, approximately 2.5 times higher than non-GO-pretreated cells. However, GO pretreatment did not result in LDH release in noncancerous HS-5 cells. It appears that this phenomenon underlays GO’s ability to puncture the cell membrane of cancerous cells depending on its surface properties without harming noncancerous cells. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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13 pages, 2185 KiB

Open AccessArticle

Atmospheric Pressure Plasma Deposition of Hybrid Nanocomposite Coatings Containing TiO₂ and Carbon-Based Nanomaterials

by Regina Del Sole, Chiara Lo Porto, Sara Lotito, Chiara Ingrosso, Roberto Comparelli, Maria Lucia Curri, Gianni Barucca, Francesco Fracassi, Fabio Palumbo and Antonella Milella

Molecules 2023, 28(13), 5131; https://doi.org/10.3390/molecules28135131 - 30 Jun 2023

Cited by 2 | Viewed by 1848

Abstract

Among the different applications of TiO₂, its use for the photocatalytic abatement of organic pollutants has been demonstrated particularly relevant. However, the wide band gap (3.2 eV), which requires UV irradiation for activation, and the fast electron-hole recombination rate of this n-type semiconductor limit its photocatalytic performance. A strategy to overcome these limitations relies on the realization of a nanocomposite that combines TiO₂ nanoparticles with carbon-based nanomaterials, such as rGO (reduced graphene oxide) and fullerene (C₆₀). On the other hand, the design and realization of coatings formed of such TiO₂-based nanocomposite coatings are essential to make them suitable for their technological applications, including those in the environmental field. In this work, aerosol-assisted atmospheric pressure plasma deposition of nanocomposite coatings containing both TiO₂ nanoparticles and carbon-based nanomaterials, as rGO or C₆₀, in a siloxane matrix is reported. The chemical composition and morphology of the deposited films were investigated for the different types of prepared nanocomposites by means of FT-IR, FEG-SEM, and TEM analyses. The photocatalytic activity of the nanocomposite coatings was evaluated through monitoring the photodegradation of methylene blue (MB) as a model organic pollutant. Results demonstrate that the nanocomposite coatings embedding rGO or C₆₀ show enhanced photocatalytic performance with respect to the TiO₂ counterpart. In particular, TiO₂/C₆₀ nanocomposites allow to achieve 85% MB degradation upon 180 min of UV irradiation. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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8 pages, 19202 KiB

Open AccessCommunication

Vertical Stress Induced Anomalous Spectral Shift of 13.17° Moiré Superlattice in Twist Bilayer Graphene

by Wenjing Miao, Hao Sheng and Jingang Wang

Molecules 2023, 28(7), 3015; https://doi.org/10.3390/molecules28073015 - 28 Mar 2023

Cited by 3 | Viewed by 1631

Abstract

The electronic states of the twist bilayer graphene (TBG) moiré superlattice are usually regulated by the rotation angle, applied electric field, applied magnetic field, carrier concentration and applied stress, and thus exhibit novel physical properties. Squeezing, that is, applying vertical compressive stress to the graphene layers, has profound significance in regulating the photoelectric properties of the moiré superlattice and constructing optical nanodevices. This paper presents the photoelectric properties of a TBG moiré superlattice with a twist angle of 13.17° and tunability under vertical stress. Interlayer distance decreases nonlinearly with compressive stress from 0 to 10 GPa, giving rise to weakened interlayer coupling compared to a Bernal-stacked graphene bilayer and an enhanced repulsive effect between the layers. The calculated Bloch wave functions show a strong dependence on stress. With the increase in stress, the band gaps of the system present a nonlinear increase, which induces and enhances the interlayer charge transfer and leads to the redshift of the absorption spectrum of the moiré superlattice system. By analyzing the differences in the Bloch wave function and charge density differences, we explain the nature of the physical mechanism of photoelectric property change in a stress-regulated twist superlattice system. This study provides a theoretical basis for the identification of piezoelectric properties and the stress regulation of photoelectric devices based on TBG, and also provides a feasible method for regulating the performance of TBG. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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16 pages, 4341 KiB

Open AccessArticle

Pedot:PSS/Graphene Oxide (GO) Ternary Nanocomposites for Electrochemical Applications

by Giuseppe Greco, Antonella Giuri, Sonia Bagheri, Miriam Seiti, Olivier Degryse, Aurora Rizzo, Claudio Mele, Eleonora Ferraris and Carola Esposito Corcione

Molecules 2023, 28(7), 2963; https://doi.org/10.3390/molecules28072963 - 26 Mar 2023

Cited by 9 | Viewed by 3578

Abstract

Among conductive polymers, poly(3,4 ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) has been widely used as an electrode material for supercapacitors, solar cells, sensors, etc. Although PEDOT:PSS-based thin films have acceptable properties such as good capacitive and electrical behaviour and biocompatibility, there are still several challenges to be overcome in their use as an electrode material for supercapacitors. For this reason, the aim of this work is to fabricate and characterise ternary nanocomposites based on PEDOT:PSS and graphene oxide (GO), blended with green additives (glucose (G) or ascorbic acid (AA)), which have the benefits of being environmentally friendly, economical, and easy to use. The GO reduction process was first accurately investigated and demonstrated by UV-Vis and XRD measurements. Three-component inks have been developed, and their morphological, rheological, and surface tension properties were evaluated, showing their printability by means of Aerosol Jet^® Printing (AJ^®P), an innovative direct writing technique belonging to the Additive Manufacturing (AM) for printed electronics applications. Thin films of the ternary nanocomposites were produced by drop casting and spin coating techniques, and their capacitive behaviour and chemical structures were evaluated through Cyclic Voltammetry (CV) tests and FT-IR analyses. CV tests show an increment in the specific capacitance of AAGO-PEDOT up to 31.4 F/g and excellent overtime stability compared with pristine PEDOT:PSS, suggesting that this ink can be used to fabricate supercapacitors in printed (bio)-electronics. The inks were finally printed by AJ^®P as thin films (10 layers, 8 × 8 mm) and chemically analysed by FT-IR, demonstrating that all components of the formulation were successfully aerosolised and deposited on the substrate. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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18 pages, 1925 KiB

Open AccessArticle

Effective Removal of Metal ion and Organic Compounds by Non-Functionalized rGO

by Viviana Sarmiento, Malcolm Lockett, Emigdia Guadalupe Sumbarda-Ramos and Oscar Vázquez-Mena

Molecules 2023, 28(2), 649; https://doi.org/10.3390/molecules28020649 - 8 Jan 2023

Cited by 4 | Viewed by 2352

Abstract

Effective removal of heavy metals from water is critical for environmental safety and public health. This work presents a reduced graphene oxide (rGO) obtained simply by using gallic acid and sodium ascorbate, without any high thermal process or complex functionalization, for effective removal of heavy metals. FTIR and Raman analysis show the effective conversion of graphene oxide (GO) into rGO and a large presence of defects in rGO. Nitrogen adsorption isotherms show a specific surface area of 83.5 m²/g. We also measure the zeta-potential of the material showing a value of −52 mV, which is lower compared to the −32 mV of GO. We use our rGO to test adsorption of several ion metals (Ag (I), Cu (II), Fe (II), Mn (II), and Pb(II)), and two organic contaminants, methylene blue and hydroquinone. In general, our rGO shows strong adsorption capacity of metals and methylene blue, with adsorption capacity of q_max = 243.9 mg/g for Pb(II), which is higher than several previous reports on non-functionalized rGO. Our adsorption capacity is still lower compared to functionalized graphene oxide compounds, such as chitosan, but at the expense of more complex synthesis. To prove the effectiveness of our rGO, we show cleaning of waste water from a paper photography processing operation that contains large residual amounts of hydroquinone, sulfites, and AgBr. We achieve 100% contaminants removal for 20% contaminant concentration and 63% removal for 60% contaminant concentration. Our work shows that our simple synthesis of rGO can be a simple and low-cost route to clean residual waters, especially in disadvantaged communities with low economical resources and limited manufacturing infrastructure. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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18 pages, 6110 KiB

Open AccessArticle

On the HKUST-1/GO and HKUST-1/rGO Composites: The Impact of Synthesis Method on Physicochemical Properties

by Paulina Jagódka, Krzysztof Matus and Agata Łamacz

Molecules 2022, 27(20), 7082; https://doi.org/10.3390/molecules27207082 - 20 Oct 2022

Cited by 16 | Viewed by 4260

Abstract

The chemical stability and adsorptive/catalytic properties of the most widely studied metal–organic framework (MOF), which is HKUST-1, can be improved by its combination with graphene oxide (GO) or reduced graphene oxide (rGO). The chemistry of GO or rGO surfaces has a significant impact on their interaction with MOFs. In this work, we demonstrate that GO and rGO interaction with HKUST-1 influences the morphology and textural properties but has no impact on the thermal stability of the final composites. We also show that synthesis environment, e.g., stirring, to some extent influences the formation of HKUST-1/GO and HKUST-1/rGO composites. Homogeneous samples of the sandwich-type composite can be obtained when using reduced graphene oxide decorated with copper (Cu/rGO), which, owing to the presence of Cu sites, allows the direct crystallisation of HKUST-1 and its further growth on the graphene surface. This work is the first part of our research on HKUST-1/GO and HKUST-1/rGO and deals with the influence of the type of graphene material and synthesis parameters on the composites’ physicochemical properties that were determined by using X-ray diffraction, scanning and transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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19 pages, 8852 KiB

Open AccessArticle

Is It Possible to Restrain OER on Simple Carbon Electrodes to Efficiently Electrooxidize Organic Pollutants?

by Marija Ječmenica Dučić, Danka Aćimović, Branislava Savić, Lazar Rakočević, Marija Simić, Tanja Brdarić and Dragana Vasić Anićijević

Molecules 2022, 27(16), 5203; https://doi.org/10.3390/molecules27165203 - 15 Aug 2022

Cited by 3 | Viewed by 1771

Abstract

This paper presents a comparative analysis of three carbon-based electrodes: bare multiwalled carbon nanotubes (MWCNT), SnO₂/MWCNT, and PbO₂/graphene-nanoribbons (PbO₂/GNR) composites, as anodes for the electrooxidative degradation of Rhodamine B as a model organic pollutant. Anodic electrooxidation of Rhodamine B was performed on all three electrodes, and the decolorization efficiency was found to increase in the order MWCNT < PbO₂/GNR < SnO₂/MWCNT. The electrodes were characterized by X-ray photoelectron spectroscopy (XPS) and linear sweep voltammetry (LSV). It was proposed that, in the 0.1 M Na₂SO₄ applied as electrolyte, observed decolorization mainly occurs in the interaction of Rhodamine B with OH radical adsorbed on the anode. Finally, the obtained results were complemented with Density Functional Theory (DFT) calculations of OH-radical interaction with appropriate model surfaces: graphene(0001), SnO₂(001), and PbO₂(001). It was found that the stabilization of adsorbed OH-radical on metal oxide spots (SnO₂ or PbO₂) compared to carbon is responsible for the improved efficiency of composites in the degradation of Rhodamine B. The observed ability of metal oxides to improve the electrooxidative potential of carbon towards organic compounds can be useful in the future design of appropriate anodes. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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12 pages, 4077 KiB

Open AccessArticle

Formation of GeO₂ under Graphene on Ge(001)/Si(001) Substrates Using Water Vapor

by Ewa Dumiszewska, Paweł Ciepielewski, Piotr A. Caban, Iwona Jóźwik, Jaroslaw Gaca and Jacek M. Baranowski

Molecules 2022, 27(11), 3636; https://doi.org/10.3390/molecules27113636 - 6 Jun 2022

Viewed by 2028

Abstract

The problem of graphene protection of Ge surfaces against oxidation is investigated. Raman, X-Ray diffraction (XRD), atomic force microscopy (AFM) and scanning electron microscopy (SEM) measurements of graphene epitaxially grown on Ge(001)/Si(001) substrates are presented. It is shown that the penetration of water vapor through graphene defects on Gr/Ge(001)/Si(001) samples leads to the oxidation of germanium, forming GeO₂. The presence of trigonal GeO₂ under graphene was identified by Raman and XRD measurements. The oxidation of Ge leads to the formation of blisters under the graphene layer. It is suggested that oxidation of Ge is connected with the dissociation of water molecules and penetration of OH molecules or O to the Ge surface. It has also been found that the formation of blisters of GeO₂ leads to a dramatic increase in the intensity of the graphene Raman spectrum. The increase in the Raman signal intensity is most likely due to the screening of graphene by GeO₂ from the Ge(001) surface. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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18 pages, 13764 KiB

Open AccessArticle

Influence of Homogenizing Methodology on Mechanical and Tribological Performance of Powder Metallurgy Processed Titanium Composites Reinforced by Graphene Nanoplatelets

by Sultan Mahmood, Amjad Iqbal, Rafi-ud-Din, Abdul Wadood, Abdul Mateen, Muhammad Amin, Ibrahim S. Yahia and Heba Y. Zahran

Molecules 2022, 27(9), 2666; https://doi.org/10.3390/molecules27092666 - 21 Apr 2022

Cited by 10 | Viewed by 2284

Abstract

In the present work, 0.25 wt%GNP-Ti composites were prepared through powder metallurgy route by adopting three types of mixing modes to investigate the extent of mixing on the mechanical and tribological properties. Dry ball milling, wet ball milling, and rotator mixing were independently employed to homogenize the composite constituents. Three types of composite powders obtained were subsequently sintered into composite pellets by cold compaction followed by vacuum sintering. Morphological investigation of composite powders performed by SEM revealed better homogenization of GNPs in Ti matrix for dry ball milled composite powder, whereas wet ball milled and rotator mixed composite powders showed aggregation and bundling of GNPs. Micro Vickers hardness of composites produced via dry ball milling is 4.56% and 15.7% higher than wet ball milled and rotator mixed samples, respectively. Wear test performed by pin-on-disk tribometer showed higher wear loss for wet ball milled and rotator mixed composites in comparison to dry ball milled. Full article

(This article belongs to the Special Issue Graphene-Based Nanocomposites for Advanced Applications)

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