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Molecular and Macromolecular Interactions of Carbon-Based Nanostructures

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A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Materials Science".

Deadline for manuscript submissions: closed (30 June 2022) | Viewed by 33768

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Prof. Dr. Valentina Villari

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Istituto per i Processi Chimico-Fisici, Consiglio Nazionale delle Ricerche (IPCF-CNR), Messina, Italy
Interests: nanostructured systems; self-assembly; porphyrin derivatives; polymer solutions and microgels; supramolecular aggregates; carbon-based nanomaterials; soft matter; light scattering; optical spectroscopy; induced supramolecular chirality
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Prof. Dr. Paula Ferreira

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Department of Materials and Ceramic Engineering, CICECO-Aveiro Institute of Materials, University of Aveiro, 3810-193 Aveiro, Portugal
Interests: bionanocomposite materials for funcional applications; flexible piezoelectric materials; active and intelligent food packaging; adsorption; catalysis

Special Issue Information

Dear Colleagues,

Scientific interest in carbon-based nanostructures is growing very rapidly thanks to their versatility in terms of preparation methods, covalent and non-covalent surface functionalization, interactions with a wide variety of molecules, and attractive properties for technological and biomedical applications. This category of nanomaterials includes carbon dots, carbon nanotubes, graphene, graphene oxide, and fullerenes, along with their hybrid composites. In this context, covalent and supramolecular interactions or binding of carbon nanostructures with molecules and macromolecules open stimulating perspectives for realizing materials with peculiar optical, electrochemical, mechanical, and thermal properties.

This Special Issue welcomes original research on all aspects of the interactions, covalent or non-covalent, of carbon-based nanostructures with molecules and macromolecules, including those biologically relevant, and the properties of the obtained compounds in the liquid or solid state. Papers devoted to applications of these nanomaterials must be accompanied by the thorough characterization of the related properties (physical, chemical, optical, electrochemical, etc.).

Contributions can be submitted in the form of research articles and short communications.

Dr. Valentina Villari
Prof. Dr. Paula Ferreira
Guest Editors

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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. International Journal of Molecular Sciences is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

Carbon nanostructures
Dispersions in an aqueous or organic solvent
Self-assembly
Hybrid composites
Supramolecular nanostructures
Surface functionalization
Molecular recognition
Electron transfer
Optoelectronic properties
Sensing properties

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Published Papers (12 papers)

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Editorial

Jump to: Research, Review

3 pages, 194 KiB

Open AccessEditorial

Molecular and Macromolecular Interactions of Carbon-Based Nanostructures

by Valentina Villari

Int. J. Mol. Sci. 2023, 24(1), 619; https://doi.org/10.3390/ijms24010619 - 30 Dec 2022

Viewed by 1338

Abstract

The interactions of molecules and macromolecules with carbon nanostructures such as carbon dots, carbon nanotubes, graphene, graphene oxide, and fullerenes, have been stimulating the interest of the researchers working on the preparation, functionalization, properties and applications of carbon-based nanomaterials [...] Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

Research

Jump to: Editorial, Review

12 pages, 2076 KiB

Open AccessArticle

Fullerenol C₆₀(OH)₃₆ Protects the Antioxidant Enzymes in Human Erythrocytes against Oxidative Damage Induced by High-Energy Electrons

by Jacek Grebowski, Paulina Kazmierska-Grebowska, Natalia Cichon, Anna Konarska, Marian Wolszczak and Grzegorz Litwinienko

Int. J. Mol. Sci. 2022, 23(18), 10939; https://doi.org/10.3390/ijms231810939 - 19 Sep 2022

Cited by 6 | Viewed by 2364

Abstract

Ionizing radiation (IR) can pass through the human body easily, potentially causing severe damage to all biocomponents, which is associated with increasing oxidative stress. IR is employed in radiotherapy; however, in order to increase safety, it is necessary to minimize side effects through the use of radioprotectors. Water-soluble derivatives of fullerene exhibit antiradical and antioxidant properties, and these compounds are regarded as potential candidates for radioprotectors. We examined the ability of fullerenol C₆₀(OH)₃₆ to protect human erythrocytes, including the protection of the erythrocytal antioxidant system against high-energy electrons. Human erythrocytes irradiated with high-energy [6 MeV] electrons were treated with C₆₀(OH)₃₆ (150 µg/mL), incubated and haemolyzed. The radioprotective properties of fullerenol were determined by examining the antioxidant enzymes activity in the hemolysate, the concentration of -SH groups, as well as by determining erythrocyte microviscosity. The irradiation of erythrocytes (650 and 1300 Gy) reduces the number of thiol groups; however, an attenuation of this harmful effect is observed (p < 0.05) in the presence of C₆₀(OH)₃₆. Although no significant effect of fullerenol was recorded on catalase activity, which was preserved in both control and test samples, a more active protection of other enzymes was evident. An irradiation-induced decrease in the activity of glutathione peroxidase and glutathione reductase became an increase in the activity of those two enzymes in samples irradiated in the presence of C₆₀(OH)₃₆ (p < 0.05 and p < 0.05, respectively). The fourth studied enzyme, glutathione transferase, decreased (p < 0.05) its activity in the irradiated hemolysate treated with C₆₀(OH)₃₆, thus, indicating a lower level of ROS in the system. However, the interaction of fullerenol with the active centre of the enzyme cannot be excluded. We also noticed that radiation caused a dose-dependent decrease in the erythrocyte microviscosity, and the presence of C₆₀(OH)₃₆ reduced this effect (p < 0.05). Overall, we point to the radioprotective effect of C₆₀(OH)₃₆ manifested as the protection of the antioxidant enzymes of human erythrocytes against IR-induced damage, which has not been the subject of intense research so far. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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13 pages, 4012 KiB

Open AccessArticle

Treating High COD Dyeing Wastewater via a Regenerative Sorption-Oxidation Process Using a Nano-Pored Activated Carbon

by Shih-Fu Ou, Dun-Sheng Yang, Jia-Wei Liao and Shyi-Tien Chen

Int. J. Mol. Sci. 2022, 23(9), 4752; https://doi.org/10.3390/ijms23094752 - 26 Apr 2022

Cited by 6 | Viewed by 2162

Abstract

Nowadays, the structural complexity of dyes used in the textile industry and the widely adopted water-saving strategy in the dyeing processes often fail plants’ biological wastewater treatment units due to chemical oxygen demand (COD) overload. To alleviate this problems, this study investigated a regenerable adsorption–oxidation process to treat dyeing wastewater with COD around 10,000 mg/dm³ using a highly nano-pored activated carbon (AC) as a COD adsorbent, followed by its regeneration using hydrogen peroxide as an oxidizing reagent. In addition to studying AC’s COD adsorption and oxidation performance, its operational treatment conditions in terms of temperature and pH were assessed. The results firstly demonstrated that about 50–60% of the COD was consistently adsorbed during the repeated adsorption operation before reaching AC’s maximum adsorption capacity (q_max) of 0.165 g-COD/g-AC. The optimal pH and temperature during adsorption were 4.7 and 25 °C, respectively. Secondly, AC regeneration was accomplished by using an initial peroxide concentration of 2.5% (by wt %) and EDTA-Fe of 2.12 mmole/dm³. The reuse of the regenerated ACs was doable. Surprisingly, after the first AC regeneration, the COD adsorption capacity of the regenerated AC even increased by ~7% with respect to the virgin AC. Thirdly, the results of a five-consecutive adsorption–regeneration operation showed that a total of 0.3625 g COD was removed by the 5 g AC used, which was equivalent to an adsorption capacity (q) of 0.0725 (= 0.3625/5) g-COD/g-AC during each adsorption stage. Based on the obtained results, a regenerable COD adsorption–oxidation process using a nano-pored AC to treat the high-textile-COD wastewater looks promising. Thus, a conceptual treatment unit was proposed, and its potential benefits and limitations were addressed. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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17 pages, 37023 KiB

Open AccessArticle

Electrospun PEO/rGO Scaffolds: The Influence of the Concentration of rGO on Overall Properties and Cytotoxicity

by Aleksandra Ivanoska-Dacikj, Petre Makreski, Nikola Geskovski, Joanna Karbowniczek, Urszula Stachewicz, Nenad Novkovski, Jelena Tanasić, Ivan Ristić and Gordana Bogoeva-Gaceva

Int. J. Mol. Sci. 2022, 23(2), 988; https://doi.org/10.3390/ijms23020988 - 17 Jan 2022

Cited by 12 | Viewed by 3436

Abstract

Reduced graphene oxide (rGO) is one of the graphene derivatives that can be employed to engineer bioactive and/or electroactive scaffolds. However, the influence of its low and especially high concentrations on scaffolds’ overall properties and cytotoxicity has yet to be explored. In this study, polyethylene oxide (PEO)-based scaffolds containing from 0.1 to 20 wt% rGO were obtained by electrospinning. Morphological, thermal and electrical properties of the scaffolds were characterized by SEM, Raman spectroscopy, XRD, DSC and electrical measurements. The diameter of the fibers decreased from 0.52 to 0.19 µm as the concentration of rGO increased from 0.1 wt% to 20 wt%. The presence of rGO above the percolation threshold (5.7 wt%) resulted in a significantly reduced electrical resistivity of the scaffolds. XRD and Raman analysis revealed delamination of the graphene layers (interlayer spacing increased from 0.36 nm to 0.40–0.41 nm), and exfoliation of rGO was detected for the samples with an rGO concentration lower than 1 wt%. In addition, an evident trend of increasing cell viability as a function of the rGO concentration was evidenced. The obtained results can serve as further guidance for the judicious selection of the rGO content incorporated into the PEO matrix for constructing electroactive scaffolds. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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19 pages, 991 KiB

Open AccessArticle

Spin State Switching in Heptauthrene Nanostructure by Electric Field: Computational Study

by Karol Szałowski

Int. J. Mol. Sci. 2021, 22(24), 13364; https://doi.org/10.3390/ijms222413364 - 13 Dec 2021

Cited by 6 | Viewed by 2616

Abstract

Recent experimental studies proved the presence of the triplet spin state in atomically precise heptauthrene nanostructure of nanographene type (composed of two interconnected triangles with zigzag edge). In the paper, we report the computational study predicting the possibility of controlling this spin state [...] Read more.

S = 1

(triplet) state,

S = 0

antiferromagnetic state and non-magnetic state and predict the switching possibility with the critical electric field of the order of 0.1 V/Å. We discuss the spin distribution across the nanostructure, finding its concentration along the longest zigzag edge. To model our system of interest, we use the mean-field Hubbard Hamiltonian, taking into account the in-plane external electric field as well as the in-plane magnetic field (in a form of the exchange field from the substrate). We also assess the effect of uniaxial strain on the magnetic phase diagram. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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14 pages, 3787 KiB

Open AccessArticle

Dissecting the Supramolecular Dispersion of Fullerenes by Proteins/Peptides: Amino Acid Ranking and Driving Forces for Binding to C₆₀

by Tainah Dorina Marforio, Alessandro Calza, Edoardo Jun Mattioli, Francesco Zerbetto and Matteo Calvaresi

Int. J. Mol. Sci. 2021, 22(21), 11567; https://doi.org/10.3390/ijms222111567 - 26 Oct 2021

Cited by 6 | Viewed by 2531

Abstract

Molecular dynamics simulations were used to quantitatively investigate the interactions between the twenty proteinogenic amino acids and C₆₀. The conserved amino acid backbone gave a constant energetic interaction ~5.4 kcal mol⁻¹, while the contribution to the binding due to the amino acid side chains was found to be up to ~5 kcal mol⁻¹ for tryptophan but lower, to a point where it was slightly destabilizing, for glutamic acid. The effects of the interplay between van der Waals, hydrophobic, and polar solvation interactions on the various aspects of the binding of the amino acids, which were grouped as aromatic, charged, polar and hydrophobic, are discussed. Although π–π interactions were dominant, surfactant-like and hydrophobic effects were also observed. In the molecular dynamics simulations, the interacting residues displayed a tendency to visit configurations (i.e., regions of the Ramachandran plot) that were absent when C₆₀ was not present. The amino acid backbone assumed a “tepee-like” geometrical structure to maximize interactions with the fullerene cage. Well-defined conformations of the most interactive amino acids (Trp, Arg, Met) side chains were identified upon C₆₀ binding. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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15 pages, 3104 KiB

Open AccessArticle

Design of Alginate-Based Bionanocomposites with Electrical Conductivity for Active Food Packaging

by Zélia Alves, Nuno M. Ferreira, Sónia Mendo, Paula Ferreira and Cláudia Nunes

Int. J. Mol. Sci. 2021, 22(18), 9943; https://doi.org/10.3390/ijms22189943 - 14 Sep 2021

Cited by 26 | Viewed by 3209

Abstract

Bionanocomposite materials have been designed as a promising route to enhance biopolymer properties, especially for food packaging application. The present study reports the preparation of bionanocomposite films of alginate with different loadings of pure reduced graphene oxide (rGO) or of mixed zinc oxide-rGO (ZnO-rGO) fillers by solvent casting. Sepiolite is used to make compatible rGO with the hydrophilic matrix. The addition of fillers to alginate matrix maintains the low water solubility promoted by the calcium chloride treatment, and, additionally, they demonstrate a weaker mechanical properties, and a slight increase in water vapor permeability and wettability. Due to the properties of ZnO-rGO, the alginate bionanocomposites show an increase of electrical conductivity with the increase of filler content. While the highest electrical conductivity (0.1 S/m) is achieved by the in-plane measurement, it is in the through-plane measurement the remarkable enhancement of almost 30 times greater than the alginate film. With 50% of ZnO-rGO filler, the bionanocomposites present the highest antioxidant and antibacterial activities. The combination of electrical conductivity with bioactive properties makes these films promising not only to extend food shelf-life but also to allow packaged food sterilization at low temperature. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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17 pages, 4117 KiB

Open AccessArticle

Optical Properties of Composites Based on Poly(o-phenylenediamine), Poly(vinylenefluoride) and Double-Wall Carbon Nanotubes

by Mihaela Baibarac, Monica Daescu, Elena Matei, Daniela Nastac and Oana Cramariuc

Int. J. Mol. Sci. 2021, 22(15), 8260; https://doi.org/10.3390/ijms22158260 - 31 Jul 2021

Cited by 6 | Viewed by 2538

Abstract

In this work, synthesis and optical properties of a new composite based on poly(o-phenylenediamine) (POPD) fiber like structures, poly(vinylidene fluoride) (PVDF) spheres and double-walled carbon nanotubes (DWNTs) are reported. As increasing the PVDF weight in the mixture of the chemical polymerization reaction of o-phenylenediamine, the presence of the PVDF spheres onto the POPD fibers surface is highlighted by scanning electron microscopy (SEM). The down-shift of the Raman line from 1421 cm⁻¹ to 1415 cm⁻¹ proves the covalent functionalization of DWNTs with the POPD-PVDF blends. The changes in the absorbance of the IR bands peaked around 840, 881, 1240 and 1402 cm⁻¹ indicate hindrance steric effects induced of DWNTs to the POPD fiber like structures and the PVDF spheres, as a consequence of the functionalization process of carbon nanotubes with macromolecular compounds. The presence of the PVDF spheres onto the POPD fiber like structures surface induces a POPD photoluminescence (PL) quenching process. An additional PL quenching process of the POPD-PVDF blends is reported to be induced in the presence of DWNTs. The studies of anisotropic PL highlight a change of the angle of the binding of the PVDF spheres onto the POPD fiber like structures surface from 50.2° to 38° when the carbon nanotubes concentration increases in the POPD-PVDF/DWNTs composites mass up to 2 wt.%. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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17 pages, 7409 KiB

Open AccessArticle

Substantial Variations in the Optical Absorption and Reflectivity of Graphene When the Concentrations of Vacancies and Doping with Fluorine, Nitrogen, and Oxygen Change

by Ali Fransuani Jiménez-González, Juan Manuel Ramírez-de-Arellano and Luis Fernando Magaña

Int. J. Mol. Sci. 2021, 22(13), 6832; https://doi.org/10.3390/ijms22136832 - 25 Jun 2021

Cited by 6 | Viewed by 2671

Abstract

We performed ab initio numerical simulations with the density functional theory to investigate the variations in the band structure, optical absorption, and the reflectivity of vacancy-graphene doped with nitrogen, oxygen, and fluorine for different densities. We considered the density values 0.78%, 1.02%, 1.39%, 2.00%, 3.12%, 5.55%, and 12.5% for the vacancies and doping. In the infrared and visible ranges for all cases, vacancies included, there is a substantial increment in the absorption and reflectivity concerning graphene. The most significant changes are for fluorine and oxygen at a concentration of 12.5%. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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10 pages, 2027 KiB

Open AccessCommunication

Carbonized Lysine-Nanogels Protect against Infectious Bronchitis Virus

by Ding-Li Chou, Ju-Yi Mao, Anisha Anand, Han-Jia Lin, John Han-You Lin, Ching-Ping Tseng, Chih-Ching Huang and Hsian-Yu Wang

Int. J. Mol. Sci. 2021, 22(11), 5415; https://doi.org/10.3390/ijms22115415 - 21 May 2021

Cited by 11 | Viewed by 3326

Abstract

In this study, we demonstrate the synthesis of carbonized nanogels (CNGs) from an amino acid (lysine hydrochloride) using a simple pyrolysis method, resulting in effective viral inhibition properties against infectious bronchitis virus (IBV). The viral inhibition of CNGs was studied using both in vitro (bovine ephemeral fever virus (BEFV) and pseudorabies virus (PRV)) and in ovo (IBV) models, which indicated that the CNGs were able to prevent virus attachment on the cell membrane and penetration into the cell. A very low concentration of 30 μg mL⁻¹ was found to be effective (>98% inhibition) in IBV-infected chicken embryos. The hatching rate and pathology of IBV-infected chicken embryos were greatly improved in the presence of CNGs. CNGs with distinctive virus-neutralizing activities show great potential as a virostatic agent to prevent the spread of avian viruses and to alleviate the pathology of infected avian species. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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14 pages, 4798 KiB

Open AccessArticle

Resistive Switching Characteristic Improvement in a Single-Walled Carbon Nanotube Random Network Embedded Hydrogen Silsesquioxane Thin Films for Flexible Memristors

by Shin-Yi Min and Won-Ju Cho

Int. J. Mol. Sci. 2021, 22(7), 3390; https://doi.org/10.3390/ijms22073390 - 25 Mar 2021

Cited by 12 | Viewed by 3072

Abstract

In this study, we evaluated the improved memristive switching characteristics of hydrogen silsesquioxane (HSQ) nanocomposites embedded with a single-walled carbon nanotube (SWCNT) random network. A low-temperature solution process was implemented using a flexible memristor device on a polyethylene naphthalate (PEN) substrate. The difference in the resistive switching (RS) behavior due to the presence of the SWCNT random network was analyzed by the current transport mechanism. Such a random network not only improves the RS operation but also facilitates a stable multilevel RS performance. The multiple-resistance states exhibited highly reliable nonvolatile retention properties over 10⁴ s at room temperature (25 °C) and at a high temperature (85 °C), showing the possibility of an analog synaptic weight modulation. Consequently, the gradual weight potentiation/depression was realized through 3 × 10² synaptic stimulation pulses. These findings suggest that the embedded SWCNT random network can improve the synaptic weight modulation characteristics with high stability for an artificial synapse and hence can be used in future neuromorphic circuits. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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Review

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16 pages, 1987 KiB

Open AccessReview

Green Carbon Nanostructures for Functional Composite Materials

by Ana Barra, Cláudia Nunes, Eduardo Ruiz-Hitzky and Paula Ferreira

Int. J. Mol. Sci. 2022, 23(3), 1848; https://doi.org/10.3390/ijms23031848 - 6 Feb 2022

Cited by 18 | Viewed by 3043

Abstract

Carbon nanostructures are widely used as fillers to tailor the mechanical, thermal, barrier, and electrical properties of polymeric matrices employed for a wide range of applications. Reduced graphene oxide (rGO), a carbon nanostructure from the graphene derivatives family, has been incorporated in composite materials due to its remarkable electrical conductivity, mechanical strength capacity, and low cost. Graphene oxide (GO) is typically synthesized by the improved Hummers’ method and then chemically reduced to obtain rGO. However, the chemical reduction commonly uses toxic reducing agents, such as hydrazine, being environmentally unfriendly and limiting the final application of composites. Therefore, green chemical reducing agents and synthesis methods of carbon nanostructures should be employed. This paper reviews the state of the art regarding the green chemical reduction of graphene oxide reported in the last 3 years. Moreover, alternative graphitic nanostructures, such as carbons derived from biomass and carbon nanostructures supported on clays, are pointed as eco-friendly and sustainable carbonaceous additives to engineering polymer properties in composites. Finally, the application of these carbon nanostructures in polymer composites is briefly overviewed. Full article

(This article belongs to the Special Issue Molecular and Macromolecular Interactions of Carbon-Based Nanostructures)

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