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A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Composites and Nanocomposites".

Deadline for manuscript submissions: closed (31 December 2019) | Viewed by 65148

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Dr. Artur M. Pinto

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LEPABE-Laboratory for Process Engineering, Environment, Biotechnology and Energy, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias s/n, 4200-465 Porto, Portugal
Interests: graphene-based materials; polymer composites; biomaterials; phototherapy; antibacterial materials; graphene inks
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Dr. Fernão D. Magalhães

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Departamento de Engenharia Química, Faculdade de Engenharia da Universidade do Porto, Rua Roberto Frias, 4200-465 Porto, Portugal
Interests: high-performance coatings; natural and synthetic-based adhesives; lignocellulosic composites; 2D-based biomaterials
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Special Issue Information

Dear Colleagues,

The mechanical, electrical, thermal, magnetic, optical and biological properties of graphene have attracted a significant amount of attention from the research community since the isolation of single-atom-thick graphene layers by Geim and co-workers in 2004. Presenting a very high surface-to-volume ratio, relatively simple processability and low cost, graphene and graphene-based materials (GBMs) were soon identified as promising nanofillers for polymer matrices. Reports have shown notorious property enhancements for graphene-polymer composites (GPC) at very low filler loadings. Uses of GPC in varied fields, such as energy, electronics, catalysis, separation and purification, biomedicine, aerospace, tribology, etc., have been demonstrated and, in some cases, put into industrial practice. However, challenges still exist. Platelet agglomeration within the polymer matrix is often seen to hinder performance improvements. Poor interfacial adhesion between filler and matrix is also a limiting factor in many systems, demanding the tuning of the surface chemistry to promote physical or chemical interactions with the polymer chains. The range of routes for the fabrication of GBMs, leading to different morphologies, oxidation states, and degrees of platelet exfoliation, have an impact on the final properties of the composites that has not yet been fully addressed. Some argue that the potential of graphene, and its advantages in relation to other nanofillers, has not yet been fully demonstrated for polymer composites. On the other hand, recent findings suggest that some graphene forms are potentially biodegradable and biocompatible, which constitutes a major advantage, compared for example with carbon black or some forms of carbon-nanotubes, which have been demonstrated to be carcinogenic. Further studies are required, concerning not only the biological properties of GBMs, but also their potential applications in multiple fields.

This Special Issue invites original papers and reviews reporting on recent progress in the following areas:

Chemical and physical surface modifications of graphene and GBMs for improving dispersibility and compatibility with polymer matrices.
Fabrication methods of GPC in coating, film, bulk or particulate forms.
Properties of GPC (chemical, mechanical, thermal, electrical, magnetic, etc.).
Applications of GPC.
Biological properties of GBMs and GPC (biocompatibility, biointeractions, environmental toxicity, etc.).

It must be noted that the term “composite” should be understood here in its broader sense, describing a material, of any geometry and size, made of two or more constituent materials that do not lose their individual identities when combined.

Dr. Artur Pinto
Prof. Dr. Fernão D. Magalhães
Guest Editors

Keywords

Graphene
Graphene oxide
Composites
Coatings
Adhesives
Fibers
Particles
Surface modification
Surface functionalization
Materials properties
Biological properties

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Related Special Issues

Graphene-Polymer Composites III in Polymers (9 articles)
Graphene-Polymer Composites in Polymers (12 articles)

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Editorial

Jump to: Research

5 pages, 208 KiB

Open AccessEditorial

Graphene-Polymer Composites

by Artur M. Pinto and Fernão D. Magalhães

Polymers 2021, 13(5), 685; https://doi.org/10.3390/polym13050685 - 25 Feb 2021

Cited by 12 | Viewed by 2557

Abstract

Graphene-polymer nanocomposites continue to gain interest in diverse scientific and technological fields [...] Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

Research

Jump to: Editorial

19 pages, 3379 KiB

Open AccessArticle

Near-Infrared Radiation-Based Mild Photohyperthermia Therapy of Non-Melanoma Skin Cancer with PEGylated Reduced Nanographene Oxide

by Raquel Costa-Almeida, Diana Bogas, José R. Fernandes, Licínia Timochenco, Filipa A. L. S. Silva, João Meneses, Inês C. Gonçalves, Fernão D. Magalhães and Artur M. Pinto

Polymers 2020, 12(8), 1840; https://doi.org/10.3390/polym12081840 - 17 Aug 2020

Cited by 25 | Viewed by 4305

Abstract

Using a one-step thermal reduction and non-covalent chemical functionalization process, PEGylated reduced nanographene oxide (rGOn-PEG) was produced from nanographene oxide (GOn) and characterized in terms of particle size, dispersion stability, chemistry, and photothermal properties, in view of its use for photothermal therapy (PTT) of non-melanoma skin cancer. GOn infrared spectrum presented more intense bands assigned to oxygen containing functional groups than observed for rGOn-PEG. GOn C/O ratio decreased more than 50% comparing with rGOn-PEG and nitrogen was present in the latter (N at % = 20.6) due to introduction of PEG-NH₂. Thermogravimetric analysis allowed estimating the amount of PEG in rGOn-PEG to be of about 56.1%. Simultaneous reduction and PEGylation increased the lateral dimensions from 287 ± 139 nm to 521 ± 397 nm, as observed by transmission electron microscopy and dynamic light scattering. rGOn-PEG exhibited ≈13-fold higher absorbance in the near-infrared radiation (NIR) region, as compared to unmodified GOn. Low power (150 mW cm⁻²) NIR irradiation using LEDs resulted in rGOn-PEG heating up to 47 °C, which is within the mild PTT temperature range. PEGylation strongly enhanced the dispersibility of rGOn in physiological media (phosphate buffered saline, fetal bovine serum, and cell culture medium) and also improved the biocompatibility of rGOn-PEG, in comparison to GOn (25–250 μg mL⁻¹). After a single NIR LED irradiation treatment of 30 min, a decrease of ≈38% in A-431 cells viability was observed for rGOn-PEG (250 μg mL⁻¹). Together, our results demonstrate the potential of irradiating rGOn-PEG using lower energy, cheaper, smaller, and safer LEDs, as alternative to high power lasers, for NIR mild hyperthermia therapy of cancer, namely non-melanoma skin cancer. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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16 pages, 4506 KiB

Open AccessArticle

Fracture Toughness Analysis of Epoxy-Recycled Rubber-Based Composite Reinforced with Graphene Nanoplatelets for Structural Applications in Automotive and Aeronautics

by Alaeddin Burak Irez, Emin Bayraktar and Ibrahim Miskioglu

Polymers 2020, 12(2), 448; https://doi.org/10.3390/polym12020448 - 14 Feb 2020

Cited by 41 | Viewed by 5271

Abstract

This study proposes a new design of lightweight and cost-efficient composite materials for the aeronautic industry utilizing recycled fresh scrap rubber, epoxy resin, and graphene nanoplatelets (GnPs). After manufacturing the composites, their bending strength and fracture characteristics were investigated by three-point bending (3PB) tests. Halpin–Tsai homogenization adapted to composites containing GnPs was used to estimate the moduli of the composites, and satisfactory agreement with the 3PB test results was observed. In addition, 3PB tests were simulated by finite element method incorporating the Halpin–Tsai homogenization, and the resulting stress–strain curves were compared with the experimental results. Mechanical test results showed that the reinforcement with GnPs generally increased the modulus of elasticity as well as the fracture toughness of these novel composites. Toughening mechanisms were evaluated by SEM fractography. The typical toughening mechanisms observed were crack deflection and cavity formation. Considering the advantageous effects of GnPs on these novel composites and cost efficiency gained by the use of recycled rubber, these composites have the potential to be used to manufacture various components in the automotive and aeronautic industries as well as smart building materials in civil engineering applications. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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16 pages, 4408 KiB

Open AccessArticle

Effects of Graphene Nanoplatelets and Cellular Structure on the Thermal Conductivity of Polysulfone Nanocomposite Foams

by Hooman Abbasi, Marcelo Antunes and José Ignacio Velasco

Polymers 2020, 12(1), 25; https://doi.org/10.3390/polym12010025 - 20 Dec 2019

Cited by 10 | Viewed by 2999

Abstract

Polysulfone (PSU) foams containing 0–10 wt% graphene nanoplatelets (GnP) were prepared using two foaming methods. Alongside the analysis of the cellular structure, their thermal conductivity was measured and analyzed. The results showed that the presence of GnP can affect the cellular structure of the foams prepared by both water vapor induced phase separation (WVIPS) and supercritical CO₂ (scCO₂) dissolution; however, the impact is greater in the case of foams prepared by WVIPS. In terms of thermal conductivity, the analysis showed an increasing trend by incrementing the amount of GnP and increasing relative density, with the tortuosity of the cellular structure, dependent on the used foaming method, relative density, and amount of GnP, playing a key role in the final value of thermal conductivity. The combination of all these factors showed the possibility of preparing PSU-GnP foams with enhanced thermal conductivity at lower GnP amount by carefully controlling the cellular structure and relative density, opening up their use in lightweight heat dissipators. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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16 pages, 3101 KiB

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Nano-Level Damage Characterization of Graphene/Polymer Cohesive Interface under Tensile Separation

by S. S. R. Koloor, S. M. Rahimian-Koloor, A. Karimzadeh, M. Hamdi, Michal Petrů and M. N. Tamin

Polymers 2019, 11(9), 1435; https://doi.org/10.3390/polym11091435 - 2 Sep 2019

Cited by 35 | Viewed by 4495

Abstract

The mechanical behavior of graphene/polymer interfaces in the graphene-reinforced epoxy nanocomposite is one of the factors that dictates the deformation and damage response of the nanocomposites. In this study, hybrid molecular dynamic (MD) and finite element (FE) simulations of a graphene/polymer nanocomposite are developed to characterize the elastic-damage behavior of graphene/polymer interfaces under a tensile separation condition. The MD results show that the graphene/epoxy interface behaves in the form of elastic-softening exponential regressive law. The FE results verify the adequacy of the cohesive zone model in accurate prediction of the interface damage behavior. The graphene/epoxy cohesive interface is characterized by normal stiffness, tensile strength, and fracture energy of 5 × 10⁻⁸ (aPa·nm⁻¹), 9.75 × 10⁻¹⁰ (nm), 2.1 × 10⁻¹⁰ (N·nm⁻¹) respectively, that is followed by an exponential regressive law with the exponent, α = 7.74. It is shown that the commonly assumed bilinear softening law of the cohesive interface could lead up to 55% error in the predicted separation of the interface. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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12 pages, 5448 KiB

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Study on Graphene/CNC-Coated Bamboo Pulp Fabric Preparation of Fabrics with Thermal Conductivity

by Feng Yang, Cuiqin Lan, Haiming Zhang, Jian Guan, Fan Zhang, Benhua Fei and Jilei Zhang

Polymers 2019, 11(8), 1265; https://doi.org/10.3390/polym11081265 - 31 Jul 2019

Cited by 15 | Viewed by 5122

Abstract

Functional fabrics have gained attention as an environmentally-friendly synthesis route. In the current study, novelty bamboo pulp fabrics with thermal conductivity properties were prepared by coating the fabric with graphene and cellulose nanocrystal (G/CNC) solutions. The influences of G and CNC concentrations on properties of fabrics were studied. The viscosities of the G/CNC solutions increased with an increase of G contents. G had an obvious thickening effect. Furthermore, compounded fabrics with different G and CNC contents (GCBPFs) were prepared and extensively characterized in terms of thermal and mechanical properties, and morphology. The ultimate thermal conductivity, bursting strength, and tensile strength of the GCBPF were 0.136 W/m·K, 1.514 MPa, and 25.8 MPa, with 4 wt.% CNC and 3 wt.% G contents, respectively. The results demonstrated that the as-fabricated GCBPFs with favorable thermal conductivity could be applied as a novel fast cooling textile for the clothing industry. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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16 pages, 5565 KiB

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Effect of Conducting Polyaniline/Graphene Nanosheet Content on the Corrosion Behavior of Zinc-Rich Epoxy Primers in 3.5% NaCl Solution

by Yanhua Lei, Zhichao Qiu, Jiurong Liu, Dongdong Li, Ning Tan, Tao Liu, Yuliang Zhang, Xueting Chang, Yanhong Gu and Yansheng Yin

Polymers 2019, 11(5), 850; https://doi.org/10.3390/polym11050850 - 10 May 2019

Cited by 31 | Viewed by 4052

Abstract

The corrosion behavior of zinc-rich epoxy primers or paints (ZRPs) with different conducting polyaniline-grafted graphene (PANI/Gr) contents was investigated. Conductivity of the formed PANI/Gr nanosheets was significantly improved by employing the Gr as the inner template to synthesize the PANI. The protective properties and electrochemical behavior of coatings with artificial defects were investigated by monitoring the free corrosion potential versus time and by using localized electrochemical impedance spectroscopy (LEIS). A synergetic enhancement of the physical barrier role of the coating and the zinc sacrificial cathodic protection was achieved in the case of ZRP including PANI/Gr nanosheets. In addition, the ZRP mixed with the PANI/Gr at a content of 0.6% exhibited the best anticorrosion performance across the range of investigated PANI/Gr contents. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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23 pages, 4486 KiB

Open AccessArticle

Graphene Oxide–Platinum Nanoparticle Nanocomposites: A Suitable Biocompatible Therapeutic Agent for Prostate Cancer

by Sangiliyandi Gurunathan, Muniyandi Jeyaraj, Min-Hee Kang and Jin-Hoi Kim

Polymers 2019, 11(4), 733; https://doi.org/10.3390/polym11040733 - 23 Apr 2019

Cited by 40 | Viewed by 6047

Abstract

Metal nanoparticles and the combination of metal nanoparticles with graphene oxide are widely used in environmental, agriculture, textile, and therapeutic applications. The effect of graphene oxide–green platinum nanoparticles (GO-PtNPs) on human prostate cancer cells (LNCaP) is unclear. Therefore, this study aimed to synthesize a nanocomposite of GO-PtNPs and evaluate their effect on prostate cancer cells. Herein, we synthesized GO-PtNPs using vanillin and characterized GO-PtNPs. GO-PtNP cytotoxicity in LNCaP cells was demonstrated by measuring cell viability and proliferation. Both decreased in a dose-dependent manner compared to that by GO or PtNPs alone. GO-PtNP cytotoxicity was confirmed by increased lactate dehydrogenase release and membrane integrity loss. Oxidative stress induced by GO-PtNPs increased malondialdehyde, nitric oxide, and protein carbonyl contents. The effective reactive oxygen species generation impaired the cellular redox balance and eventually impaired mitochondria by decreasing the membrane potential and ATP level. The cytotoxicity to LNCaP cells was correlated with increased expression of proapoptotic genes (p53, p21, Bax, Bak, caspase 9, and caspase 3) and decreased levels of antiapoptotic genes (Bcl2 and Bcl-xl). Activation of the key regulators p53 and p21 inhibited the cyclin-dependent kinases Cdk2 and Cdk4, suggesting that p53 and p21 activation in GO-PtNP-treated cells caused genotoxic stress and apoptosis. The increased expression of genes involved in cell cycle arrest and DNA damage and repair, and increased levels of 8-oxo-deoxyguanosine and 8-oxoguanine suggested that GO-PtNPs potentially induce oxidative damage to DNA. Thus, GO-PtNPs are both cytotoxic and genotoxic. LNCaP cells appear to be more susceptible to GO-PtNPs than to GO or PtNPs. Therefore, GO-PtNPs have potential as an alternate and effective cancer therapeutic agent. Finally, this work shows that the combination of graphene oxide with platinum nanoparticles opens new perspectives in cancer therapy. However further detailed mechanistic studies are required to elucidate the molecular mechanism of GO-PtNPs induced cytotoxicity in prostate cancer. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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15 pages, 2143 KiB

Open AccessArticle

Anisotropic Cellulose Nanofibers/Polyvinyl Alcohol/Graphene Aerogels Fabricated by Directional Freeze-drying as Effective Oil Adsorbents

by Lijie Zhou, Shengcheng Zhai, Yiming Chen and Zhaoyang Xu

Polymers 2019, 11(4), 712; https://doi.org/10.3390/polym11040712 - 18 Apr 2019

Cited by 97 | Viewed by 9745

Abstract

Under the current situation of frequent oil spills, the development of green and recyclable high-efficiency oil-absorbing aerogel materials has attracted wide attention from researchers. In this study, we report a high-strength, three-dimensional hydrophobic cellulose nanofiber (CNF)/polyvinyl alcohol (PVA)/graphene oxide (GO) composite aerogel with an anisotropic porous structure, which was fabricated by directional freeze-drying technology using anisotropically grown ice crystals as a template, followed by hydrophobic treatment with a simple dip coating process. The prepared composite aerogel presented anisotropic multi-level pore microstructures, low density (17.95 mg/cm³) and high porosity (98.8%), good hydrophobicity (water contact angle of 142°) and great adsorption capacity (oil absorption reaching 96 times its own weight). More importantly, the oriented aerogel had high strength, whose compressive stress at 80% strain reached 0.22 MPa and could bear more than 22,123 times its own weight without deformation. Therefore, the CNF/PVA/GO composite aerogel prepared by a simple and easy-to-operate directional freeze-drying method is a promising absorbent for oil-water separation. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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23 pages, 7401 KiB

Open AccessArticle

Electrospun Graphene Nanosheet-Filled Poly(Trimethylene Terephthalate) Composite Fibers: Effects of the Graphene Nanosheet Content on Morphologies, Electrical Conductivity, Crystallization Behavior, and Mechanical Properties

by Chien-Lin Huang, Hsuan-Hua Wu, Yung-Ching Jeng and Wei-Zhi Liang

Polymers 2019, 11(1), 164; https://doi.org/10.3390/polym11010164 - 17 Jan 2019

Cited by 15 | Viewed by 4602

Abstract

In this study the effects of increased graphene nanosheet (GNS) concentration on variations in the structure and properties of electrospun GNS-filled poly(trimethylene terephthalate) (PTT/GNS) composite fiber, such as its morphologies, crystallization behavior, mechanical properties, and electrical conductivity, were investigated. The effects of GNS addition on solution rheology and conductivity were also investigated. GNSs were embedded in the fibers and formed protrusions. The PTT cold crystallization rate of PTT/GNS composite fibers increased with the gradual addition of GNSs. A PTT mesomorphic phase was formed during electrospinning, and GNSs could induce the PTT mesomorphic phase significantly during PTT/GNS composite fiber electrospinning. The PTT/GNS composite fiber mats (CFMs) became ductile with the addition of GNSs. The elastic recoveries of the PTT/GNS CFMs with 170 °C annealing were better than those of the as-spun PTT/GNS CFMs. Percolation scaling laws were applied to the magnitude of conductivity to reveal the percolation network of electrospun PTT/GNS CFMs. The electrical conductivity mechanism of the PTT/GNS CFMs differed from that of the PTT/GNS composite films. Results showed that the porous structure of the PTT CFMs influenced the performance of the mats in terms of electrical conductivity. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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14 pages, 3952 KiB

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Evaluation of Exfoliated Graphite to Graphene in Polyamide 66 Using Novel High Shear Elongational Flow

by Justin W. Hendrix, Ryan Szeto, Thomas Nosker, Jennifer Lynch-Branzoi and Thomas J. Emge

Polymers 2018, 10(12), 1399; https://doi.org/10.3390/polym10121399 - 17 Dec 2018

Cited by 10 | Viewed by 5231

Abstract

Graphene has been publicized as the game changing material of this millennium. To this day, scalable production leading to exceptional material properties has been difficult to attain. Most methods require harsh chemicals, which result in destroying the graphene surface. A method was developed, exploiting high speed elongational flow in a novel designed batch mixer; creating a distribution of pristine few to many layer graphene flakes. The method focuses on exfoliating in a molten polyamide 66 (PA66) matrix, creating a graphene reinforced polymer matrix composite (G-PMC). The process revealed that high speed elongational flow was able to create few layer graphene. Graphite exfoliation was found driven in part by diffusion, leading to intercalation of PA66 in graphite. The intercalated structure lead to increases in the hydrogen bonding domain, creating anisotropic crystal domains. The thermal stability of the G-PMC was found to be dependent to the degree of exfoliation, PA66 crystal structure and composite morphology. The aim of this research is to characterize uniquely produced graphene containing polymer matrix composites using a newly created elongational flow field. Using elongational flow, graphite will be directly exfoliated into graphene within a molten polymer. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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14 pages, 2835 KiB

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High-Performance Biobased Unsaturated Polyester Nanocomposites with Very Low Loadings of Graphene

by Chengguo Liu, Cuina Wang, Jijun Tang, Jing Zhang, Qianqian Shang, Yun Hu, Hongxiao Wang, Qiong Wu, Yonghong Zhou, Wen Lei and Zengshe Liu

Polymers 2018, 10(11), 1288; https://doi.org/10.3390/polym10111288 - 20 Nov 2018

Cited by 14 | Viewed by 5251

Abstract

Graphene-reinforced tung oil (TO)-based unsaturated polyester nanocomposites were prepared via in situ melt polycondensation intergrated with Diels–Alder addition. Functionalized graphene sheets derived from graphene oxide (GO) were then extracted from the obtained nanocomposites and carefully characterized. Furthermore, dispersion state of the graphene nanosheets in the cured polymer composites and ultimate properties of the resultant biobased nanocomposites were investigated. Mechanical and thermal properties of the TO-based unsaturated polyester resin (UPR) were greatly improved by the incorporation of GO. For example, at the optimal GO content (only 0.10 wt %), the obtained biobased nanocomposite showed tensile strength and modulus of 43.2 MPa and 2.62 GPa, and T_g of 105.2 °C, which were 159%, 191%, and 49.4% higher than those of the unreinforced UPR/TO resin, respectively. Compared to neat UPR, the biobased UPR nanocomposite with 0.1 wt % of GO even demonstrated superior comprehensive properties (comparable stiffness and T_g, while better toughness and thermal stability). Therefore, the developed biobased UPR nanocomposites are very promising to be applied in structural plastics. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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9 pages, 2658 KiB

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Effect of Compatibilizer on the Interface Bonding of Graphene Oxide/Polypropylene Composite Fibers

by Miao Miao, Chunyan Wei, Ying Wang and Yongfang Qian

Polymers 2018, 10(11), 1283; https://doi.org/10.3390/polym10111283 - 18 Nov 2018

Cited by 16 | Viewed by 4564

Abstract

To improve the interfacial bonding and thermal stability of graphene oxide (GO)/polypropylene (PP) composite fibers, a composite fiber with PP as the matrix, GO as reinforcement and maleic anhydride-grafted PP (PP-g-MAH) as a compatibilizer was prepared by a simple and efficient melt-blending method. The GO content was 0.0–5.0 wt %. According to the Fourier Transform Infrared (FT-IR) spectroscopy results, the interfacial bonding in the PP/MAH/GO composite fibers was improved. The Dynamic Mechanical Analysis (DMA) results show that the addition of GO resulted in better interfacial adhesion and higher storage modulus (E′). The loss modulus (E″) of the PP/MAH/GO-x composite fibers increased with increasing amount of added GO, whereas the loss factor (tan δ) decreased. GO and PP-g-MAH were analyzed by Thermogravimetric Analysis (TGA). The thermal stability of the composite fibers was improved compared to PP. Differential Scanning Calorimetry (DSC) analysis showed that the addition of PP-g-MAH to the composite fiber improved the interfacial bonding of GO in the PP matrix. Thus, compatibility between the two components was obtained. Based on the Scanning Electron Microscopy (SEM) results, the PP fibers exhibited relative orientation due to the strong crystalline morphology. The rough section, PP/GO blend fiber exhibits a very clear phase separation morphology due to the incompatibility between the two and the compatibility of GO and PP in PP/MAH/GO-3 composite fiber is improved, resulting in the interface between the two has improved. Full article

(This article belongs to the Special Issue Graphene-Polymer Composites II)

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