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A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Biobased and Biodegradable Polymers".

Deadline for manuscript submissions: closed (30 November 2020) | Viewed by 50493

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Prof. Dr. Raul Fangueiro

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1. Fibrenamics, Institute of Innovation on Fiber-Based Materials and Composites, University of Minho, 4710-057 Guimarães, Portugal
2. Centre for Textile Science and Technology (2C2T), University of Minho, 4710-057 Guimarães, Portugal
Interests: fibrous and composite materials; nanofibers; advanced textiles; smart composites
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Prof. Dr. Seeram Ramakrishna

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Department of Mechanical Engineering, National University of Singapore, Singapore 119077, Singapore
Interests: circular economy; sustainability; energy; biomaterials; nanofibers
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Prof. Dr. Sabu Thomas

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Guest Editor

Vice Chancellor, Mahatma Gandhi University, Priyadarshini Hills, Kottayam 686 560, Kerala, India
Interests: nanomaterials; polymer blends; fiber-filled polymer composites; polymer nanocomposites; aging and degradation; pervaporation phenomena; sorption and diffusion; interpenetrating polymer systems; recyclability and reuse of waste plastics and rubbers; elastomer crosslinking; dual porous nanocomposite scaffolds for tissue engineering; polymer nanocomposites for electronic applications; water purification; energy storage
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Special Issue Information

The aim of this Special Issue is to attract leading researchers in the area of multifunctional ecocomposites in an effort to highlight the latest exciting developments to promote concrete applications.

Tremendous growth in the use of nonrenewable and nonbiodegradable synthetic materials and associated emission of greenhouse gases is presently a major concern for the environment and future generations. In this context, the use of ecomposites based on biobased sources, like natural fibers and polymers, has been investigated in recent decades by several research groups from all over the world.

Ecomposites are greatly enlarging their range of applications in different industrial sectors, including automobiles, sports, architecture, design, and many others. For this, intensive research is being done on the functionalization of ecocomposites to perform several functions and/or to overcome some of their inherent characteristics. Strong efforts are also being undertaken to design the performance of ecomposites at different scales, from nano to macro, based on hierarchical and multigrade approaches. Besides, the use of nonexplored natural sources, and the use of the basic constituents of natural-based polymers, like cellulose, is also being thoroughly explored.

In this context, the accepted contributions for this Special Issue include topics like

· Natural-fiber-reinforced composites;
· Hierarchical ecocomposites;
· Nanocellulose-based materials;
· Lignin-based composites;
· Nano biocomposites;
· Nano functionalization of ecocomposites;
· Waste-based composites;
· Multiscale ecocomposites;
· Multigrade ecocomposites;
· Biopolymer composites;
· Bionanocomposites;
· Chitin- and chitosan-based composites;
· Natural polymer composites.

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Published Papers (10 papers)

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8 pages, 24881 KiB

Open AccessArticle

Effects of the Face/Core Layer Ratio on the Mechanical Properties of 3D Printed Wood/Polylactic Acid (PLA) Green Biocomposite Panels with a Gyroid Core

by Nadir Ayrilmis, Rajini Nagarajan and Manja Kitek Kuzman

Polymers 2020, 12(12), 2929; https://doi.org/10.3390/polym12122929 - 7 Dec 2020

Cited by 14 | Viewed by 2955

Abstract

Gyroid structured green biocomposites with different thickness face layers (0.5, 1, 2 and 2.5 mm) were additively manufactured from wood/ polylactic acid (PLA) filaments using a 3D printer. The mechanical properties of the composite panels, bending properties, compressive strength (parallel to the surface), Brinell hardness, and face screw withdrawal resistance, were determined. The surface layer thickness significantly affects the mechanical properties of the composite materials. As the surface layer thickness was increased from 0.5 to 2.5 mm, all the mechanical properties significantly improved. In particular, the Brinell hardness and face screw withdrawal resistance of the specimens improved sharply when the skin thickness was higher than 2 mm. The bending strength, bending modulus, compressive strength (parallel to the surface), Brinell hardness, and face screw withdrawal resistance of the specimens with a skin of 0.5 mm were found to be 8.10, 847.5, 3.52, 2.12 and 445 N, respectively, while they were found to be 65.8, 11.82, 2492.2, 14.62, 26 and 1475 N for the specimens with a 2.5 mm skin. Based on the findings from the present study, gyroid structured composites with a thickness of 2 mm or higher are recommended due to their better mechanical properties as compared to the composites with skins that are thinner. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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18 pages, 2622 KiB

Open AccessArticle

Preparation and Characterization of Electrospun Double-layered Nanocomposites Membranes as a Carrier for Centella asiatica (L.)

by Cláudia Mouro, Raul Fangueiro and Isabel C. Gouveia

Polymers 2020, 12(11), 2653; https://doi.org/10.3390/polym12112653 - 11 Nov 2020

Cited by 20 | Viewed by 3355

Abstract

A wide range of naturally derived and synthetic biodegradable and biocompatible polymers are today regarded as promising materials for improving skin regeneration. Alongside this, these materials have been explored in conjunction with different types of antimicrobial and bioactive agents, especially natural-derived compounds, to enhance their biological properties. Herein, a double-layered nanocomposite dressing membrane was fabricated with two distinct layers. A bottom layer from Chitosan-Sodium tripolyphosphate (CS-TPP) and Poly(vinyl alcohol) (PVA) containing Centella asiatica (L.) (CA) was electrospun directly over a Polycaprolactone (PCL) layer to improve the biologic performance of the electrospun nanofibers. In turn, the PCL layer was designed to provide mechanical support to the damaged tissue. The results revealed that the produced double-layered nanocomposite membrane closely resembles the mechanical, porosity, and wettability features required for skin tissue engineering. On the other hand, the in vitro drug release profile of the PCL/PVA_CS-TPP containing CA exhibited a controlled release for 10 days. Moreover, the PVA_CS-TPP_CA’s bottom layer displayed the highest antibacterial activity against Staphylococcus aureus (S. aureus) (99.96 ± 6.04%) and Pseudomonas aeruginosa (P. aeruginosa) (99.94 ± 0.67%), which is responsible for avoiding bacterial penetration while endowing bioactive properties. Finally, the 3-(4,5-Dimethyl-2-thiazolyl)-2,5-diphenyl-2H-tetrazolium bromide (MTT) assay showed that this nanocomposite membrane was not cytotoxic for normal human dermal fibroblasts (NHDF) cells. Therefore, these findings suggest the potential use of the double-layered PCL/PVA_CS-TPP_CA as an efficient bionanocomposite dressing material. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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23 pages, 2549 KiB

Open AccessEditor’s ChoiceArticle

Effect of Clay Nanofillers on the Mechanical and Water Vapor Permeability Properties of Xylan–Alginate Films

by Darrel S. Naidu and Maya J. John

Polymers 2020, 12(10), 2279; https://doi.org/10.3390/polym12102279 - 4 Oct 2020

Cited by 44 | Viewed by 4263

Abstract

In this study, xylan–alginate-based films were reinforced with nanoclays (bentonite or halloysite) by the solvent casting technique. The effect of the nanoclay loadings (1–5 wt %) on various properties—mechanical, optical, thermal, solubility, water sorption, and water vapor permeability (WVP)—of the xylan–alginate films were examined for their application as food packaging materials. A 5 wt % loading of either bentonite or halloysite resulted in a 49% decrease of the WVP due to the impermeable nature of the silicate layers that make up both bentonite and halloysite. Thermal stability and solubility of the nanocomposite films were not significantly influenced by the presence of the nanoclays, whereas the optical properties were significantly improved when compared to neat xylan–alginate blend. In general, films reinforced with bentonite exhibited superior mechanical and optical properties when compared to both halloysite-based nanocomposite and neat films. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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17 pages, 5631 KiB

Open AccessArticle

Chitosan-Grafted Halloysite Nanotubes-Fe₃O₄ Composite for Laccase-Immobilization and Sulfamethoxazole-Degradation

by Avinash A. Kadam, Surendra K. Shinde, Gajanan S. Ghodake, Ganesh D. Saratale, Rijuta G. Saratale, Bharat Sharma, Seunghun Hyun and Jung-Suk Sung

Polymers 2020, 12(10), 2221; https://doi.org/10.3390/polym12102221 - 27 Sep 2020

Cited by 28 | Viewed by 4174

Abstract

A surface-engineered nano-support for enzyme laccase-immobilization was designed by grafting the surface of halloysite nanotubes (HNTs) with Fe₃O₄ nanoparticles and chitosan. Herein, HNTs were magnetized (HNTs-M) by a cost-effective reduction-precipitation method. The synthesized HNTs-M were grafted with 0.25%, 0.5%, 1%, and 2% chitosan (HNTs-M-chitosan), respectively. Synthesized HNTs-M-chitosan (0.25%), HNTs-M-chitosan (0.5%), HNTs-M-chitosan (1%) and HNTs-M-chitosan (2%) were linked with glutaraldehyde (GTA) for laccase immobilization. Among these formulations, HNTs-M-chitosan (1%) exhibited the highest laccase immobilization with 95.13% activity recovery and 100.12 mg/g of laccase loading. The optimized material was characterized thoroughly by scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HR-TEM), X-ray powder diffraction (XRD), thermal gravimetric analysis (TGA), and vibrating sample magnetometer (VSM) analysis. The immobilized laccase (HNTs-M-chitosan (1%)-GTA-Laccase) exhibited higher pH, temperature, and storage stabilities. The HNTs-M-chitosan (1%)-GTA-Laccase possesses excellent reusability capabilities. At the end of 10 cycles of the reusability experiment, HNTs-M-chitosan (1%)-GTA-Laccase retained 59.88% of its initial activity. The immobilized laccase was utilized for redox-mediated degradation of sulfamethoxazole (SMX), resulting in 41%, 59%, and 62% degradation of SMX in the presence of 2,2′-Azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) diammonium salt (ABTS), guaiacol (GUA), and syringaldehyde (SA), respectively. Repeated SMX degradation (57.10% after the sixth cycle) confirmed the potential of HNTs-M-chitosan (1%)-GTA-Laccase for environmental pollutant degradation. Thus, we successfully designed chitosan-based, rapidly separable super-magnetic nanotubes for efficacious enhancement of laccase biocatalysis, which can be applied as nano-supports for other enzymes. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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18 pages, 4554 KiB

Open AccessArticle

The Potential of Graphene Nanoplatelets in the Development of Smart and Multifunctional Ecocomposites

by Pedro Pereira, Diana P. Ferreira, Joana C. Araújo, Armando Ferreira and Raul Fangueiro

Polymers 2020, 12(10), 2189; https://doi.org/10.3390/polym12102189 - 24 Sep 2020

Cited by 39 | Viewed by 3432

Abstract

Graphene and its derivatives have shown outstanding potential in many fields and textile/composites industry are not an exception. Giving their extraordinary properties, Graphene Nanoplatelets (GNPs) are excellent candidates for providing new functionalities to fibers and composites. In this work, natural fabrics (flax) were functionalized with chitosan (CS) based polymeric formulations of GNPs to develop fibrous systems with electrical properties as well as other functionalities. One of the greatest disadvantages of using carbon-based materials for fabrics’ impregnation is their difficult dispersion. Therefore, several polymers were used as matrices, binding and dispersive agents including chitosan, polyethylene glycol (PEG), and glycerol. All the systems were characterized using several techniques that demonstrated the presence and incorporation of the GNPs onto the composites. Besides their characterization, considering their use as smart materials for monitoring and sensing applications, electrical properties were also evaluated. The highest value obtained for electrical conductivity was 0.04 S m⁻¹ using 2% of GNPs. Furthermore, piezoresistive behavior was observed with Gauge Factor (GF) of 1.89 using 0.5% GNPs. Additionally, UV (ultraviolet) protection ability and hydrophobicity were analyzed, confirming the multifunctional behavior of the developed systems extending their potential of application in several areas. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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25 pages, 10539 KiB

Open AccessArticle

Diffusion and Controlled Release in Physically Crosslinked Poly (Vinyl Alcohol)/Iota-Carrageenan Hydrogel Blends

by Catalin Croitoru, Ionut Claudiu Roata, Alexandru Pascu and Elena Manuela Stanciu

Polymers 2020, 12(7), 1544; https://doi.org/10.3390/polym12071544 - 13 Jul 2020

Cited by 30 | Viewed by 4699

Abstract

This paper reports the obtaining of poly (vinyl alcohol) and ι-carrageenan blend hydrogels by physical crosslinking (consecutive freeze–thaw cycles). The two polymers were completely miscible in the weight ratio interval used in this study, as determined by solution viscometry data. Strong interactions through hydrogen bonding and forming of mixed interpolymer crystalline domains were observed, which are responsible for the formation of stable drug release-tunable matrices. The release profiles of three model antibiotic drugs (amoxicillin, tetracycline hydrochloride, and gentamicin sulfate) were assessed in a pH interval between 3 and 7.3. They were found to be strongly dependent on the drug chemistry, mesh size of the hydrogels, swelling mechanism, and pH of the release medium. A decrease of up to 40% in the release rates and up to 10% in the diffusion coefficients of the model drugs was registered with the increase in ι-carrageenan content. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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19 pages, 3296 KiB

Open AccessArticle

Mercerization Optimization of Bamboo (Bambusa vulgaris) Fiber-Reinforced Epoxy Composite Structures Using a Box–Behnken Design

by Mohamad Zaki Hassan, Siti Amni Roslan, S. M. Sapuan, Zainudin A. Rasid, Ariff Farhan Mohd Nor, Mohd Yusof Md Daud, Rozzeta Dolah and Mohd Zuhri Mohamed Yusoff

Polymers 2020, 12(6), 1367; https://doi.org/10.3390/polym12061367 - 17 Jun 2020

Cited by 65 | Viewed by 4805

Abstract

The objective of this research is to optimize the alkaline treatment variables, including sodium hydroxide (NaOH) concentration, soaking, and drying time, that influence the mechanical behavior of bamboo fiber-reinforced epoxy composites. In this study, a Box–Behnken design (BBD) of the response surface methodology (RSM) was employed to design an experiment to investigate the mercerization effect of bamboo fiber-reinforced epoxy composites. The evaluation of predicted tensile strength as a variable parameter of bamboo fiber (Bambusa vulgaris) reinforced epoxy composite structures was determined using analysis of variance (ANOVA) of the quadratic model. In this study, a total of 17 experiment runs were measured and a significant regression for the coefficient between the variables was obtained. Further, the triangular and square core structures made of treated and untreated bamboo fiber-reinforced epoxy composites were tested under compressive loading. It was found that the optimum mercerization condition lies at 5.81 wt.% of the NaOH, after a soaking time of 3.99 h and a drying time of 72 h. This optimum alkaline treatment once again had a great effect on the structures whereby all the treated composite cores with square and triangular structures impressively outperformed the untreated bamboo structures. The treated triangular core of bamboo reinforced composites gave an outstanding performance compared to the treated and untreated square core composite structures for compressive loading and specific energy absorbing capability. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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27 pages, 6394 KiB

Open AccessEditor’s ChoiceArticle

Enhancement of Oil Palm Waste Nanoparticles on the Properties and Characterization of Hybrid Plywood Biocomposites

by Arif Nuryawan, C. K. Abdullah, Che Mohamad Hazwan, N. G. Olaiya, Esam Bashir Yahya, Iwan Risnasari, Nanang Masruchin, M. S. Baharudin, Hasmawi Khalid and H. P. S. Abdul Khalil

Polymers 2020, 12(5), 1007; https://doi.org/10.3390/polym12051007 - 27 Apr 2020

Cited by 25 | Viewed by 5195

Abstract

Using oil palm trunk (OPT) layered with empty fruit bunch (EFB), so-called hybrid plywood enhanced with palm oil ash nanoparticles, with phenol-formaldehyde (PF) resin as a binder, was produced in this study. The phenol-formaldehyde (PF) resins filled with different loading of oil palm ash (OPA) nanoparticles were prepared and used as glue for layers of the oil palm trunk (OPT) veneer and empty fruit bunch fibre mat. The resulting hybrid plywood produced was characterised. The physical, mechanical, thermal, and morphological properties of the hybrid plywood panels were investigated. The results obtained showed that the presence of OPA nanoparticles significantly affected the physical, mechanical, and thermal properties of the plywood panels. Significant improvements in dimension from water absorption and thickness swelling experiments were obtained for the plywood panels with the highest OPA nanoparticles loading in PF resin. The mechanical properties indicated that plywood composites showed improvement in flexural, shear, and impact properties until a certain loading of OPA nanoparticles in PF resin. Fracture surface morphology also showed the effectiveness of OPA nanoparticles in the reduction of layer breakage due to force and stress distribution. The thermal stability performance showed that PF filled OPA nanoparticles contributed to the thermal stability of the plywood panels. Therefore, the results obtained in this study showed that OPA nanoparticles certainly improved the characteristic of the hybrid plywood. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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21 pages, 3357 KiB

Open AccessReview

Surface-Modified Highly Biocompatible Bacterial-poly(3-hydroxybutyrate-co-4-hydroxybutyrate): A Review on the Promising Next-Generation Biomaterial

by Jun Meng Chai, Tan Suet May Amelia, Govindan Kothandaraman Mouriya, Kesaven Bhubalan, Al-Ashraf Abdullah Amirul, Sevakumaran Vigneswari and Seeram Ramakrishna

Polymers 2021, 13(1), 51; https://doi.org/10.3390/polym13010051 - 25 Dec 2020

Cited by 14 | Viewed by 4442

Abstract

Polyhydroxyalkanoates (PHAs) are bacteria derived bio-based polymers that are synthesised under limited conditions of nutritional elements with excess carbon sources. Among the members of PHAs, poly(3-hydroxybutyrate-co-4-hydroxybutyrate) [(P(3HB-co-4HB)] emerges as an attractive biomaterial to be applied in medical applications owing to its desirable mechanical and physical properties, non-genotoxicity and biocompatibility eliciting appropriate host tissue responses. The tailorable physical and chemical properties and easy surface functionalisation of P(3HB-co-4HB) increase its practicality to be developed as functional medical substitutes. However, its applicability is sometimes limited due to its hydrophobic nature due to fewer bio-recognition sites. In this review, we demonstrate how surface modifications of PHAs, mainly P(3HB-co-4HB), will overcome these limitations and facilitate their use in diverse medical applications. The integration of nanotechnology has drastically enhanced the functionality of P(3HB-co-4HB) biomaterials for application in complex biological environments of the human body. The design of versatile P(3HB-co-4HB) materials with surface modifications promise a non-cytotoxic and biocompatible material without inducing severe inflammatory responses for enhanced effective alternatives in healthcare biotechnology. The enticing work carried out with P(3HB-co-4HB) promises to be one of the next-generation materials in biomedicines which will facilitate translation into the clinic in the future. Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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29 pages, 1286 KiB

Open AccessReview

PLA Composites Reinforced with Flax and Jute Fibers—A Review of Recent Trends, Processing Parameters and Mechanical Properties

by Usha Kiran Sanivada, Gonzalo Mármol, F. P. Brito and Raul Fangueiro

Polymers 2020, 12(10), 2373; https://doi.org/10.3390/polym12102373 - 15 Oct 2020

Cited by 116 | Viewed by 12167

Abstract

Multiple environmental concerns such as garbage generation, accumulation in disposal systems and recyclability are powerful drivers for the use of many biodegradable materials. Due to the new uses and requests of plastic users, the consumption of biopolymers is increasing day by day. Polylactic Acid (PLA) being one of the most promising biopolymers and researched extensively, it is emerging as a substitute for petroleum-based polymers. Similarly, owing to both environmental and economic benefits, as well as to their technical features, natural fibers are arising as likely replacements to synthetic fibers to reinforce composites for numerous products. This work reviews the current state of the art of PLA compounds reinforced with two of the high strength natural fibers for this application: flax and jute. Flax fibers are the most valuable bast-type fibers and jute is a widely available plant at an economic price across the entire Asian continent. The physical and chemical treatments of the fibers and the production processing of the green composites are exposed before reporting the main achievements of these materials for structural applications. Detailed information is summarized to understand the advances throughout the last decade and to settle the basis of the next generation of flax/jute reinforced PLA composites (200 Maximum). Full article

(This article belongs to the Special Issue Multifunctional Ecocomposites)

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