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Biodegradable Polymeric Composites: Development and Industrial Applications

A special issue of Materials (ISSN 1996-1944).

Deadline for manuscript submissions: closed (30 November 2018) | Viewed by 57302

Special Issue Editors

Department of Materials, Loughborough University, Loughborough, UK
Interests: biocompatible and natural polymers for regenerative medicine; nanofibrous wound dressings with antimicrobial activity and enhanced cell proliferation; functional nanocomposites with controlled surface and mechanical properties; microfluidic devices for biological assays and food safety; nanofabrication approaches for polymers
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Smart Materials, Istituto Italiano di Tecnologia, Via Morego 30, 16163 Genova, Italy

Special Issue Information

Dear Colleagues,

Plastics derived from fossil fuels are extensively used for the large-scale production of commodities, due to the availability of well-developed manufacturing processes and to the possibility of achieving good control over their physicochemical properties. However, once commodity plastics end up in landfills and the oceans, their limited biodegradability is a concern for biodiversity, ecosystems, food security and human health. It has been estimated that 6–12 metric tons of plastic enter the oceans each year, with plastic debris found on coastal areas and in every marine habitat.

The global threat of plastic pollution has stimulated the research of materials that can be broken down to CO2, CH4 and water by the action of microorganisms. These biodegradable polymers can be produced from fossil fuels (polycaprolactone, aromatic or aliphatic co-polyesters), biomasses (polysaccharides, lignin, proteins, cutin) or micro-organisms/biotechnology (polyhydroxy-alkanoates, polylactides). An interesting perspective is represented by composite systems based on this class of polymers for their enhanced properties and retained biodegradability.

In this Special Issue, we aim to publish original work and reviews about the current strategies and technologies for the fabrication of biodegradable polymeric composites and their industrial applications, such as in food packaging and biomedical devices, among others.

Dr. Elisa Mele
Dr. José Alejandro Heredia-Guerrero
Dr. Athanassia Athanassiou
Guest Editors

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Keywords

  • Biodegradable polymer composites/nanocomposites
  • Fabrication strategies for biodegradable polymer composites
  • Industrial applications
  • Food packaging
  • Biomedical devices
  • Tissue engineering and drug delivery
  • Membranes and filters for water purification
  • Antimicrobial materials
  • Energy technologies

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Published Papers (9 papers)

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Research

12 pages, 2512 KiB  
Article
Photodegradation and Biodegradation of Poly(Lactic) Acid Containing Orotic Acid as a Nucleation Agent
by Jan Salač, Jana Šerá, Martin Jurča, Vincent Verney, Adam A. Marek and Marek Koutný
Materials 2019, 12(3), 481; https://doi.org/10.3390/ma12030481 - 4 Feb 2019
Cited by 32 | Viewed by 4714
Abstract
Orotic acid is a natural heterocyclic compound that acts as a nucleation agent in poly(lactic acid) (PLA). PLA materials with increasing orotic acid content were prepared and characterized. It was found that crystallinity of about 28% was reached with 0.3% content of the [...] Read more.
Orotic acid is a natural heterocyclic compound that acts as a nucleation agent in poly(lactic acid) (PLA). PLA materials with increasing orotic acid content were prepared and characterized. It was found that crystallinity of about 28% was reached with 0.3% content of the agent. Further enhancement in the content of the agent did not provoke any additional significant increase of crystallinity. Subsequently, it was investigated whether the orotic acid content affected photodegradation of PLA and, in the next phase, its biodegradation. The results of rheological measurements showed that the compound slightly accelerates photodegradation of the material, which was accompanied by the cleavage of PLA chains. Previous photodegradation was shown to accelerate the subsequent biodegradation by shortening the lag phase of the process, where the explanation is probably in the reduction of the polymer molecular weight during the photodegradation. Moreover, the presence of orotic acid in both initial and photodegraded samples was found to influence biodegradation positively by shortening the lag phase and increasing the observed maximal rate of the biodegradation. Full article
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17 pages, 2749 KiB  
Article
Functional Chitosan Derivative and Chitin as Decolorization Materials for Methylene Blue and Methyl Orange from Aqueous Solution
by Abdelkader Labidi, Asier M. Salaberria, Susana C. M. Fernandes, Jalel Labidi and Manef Abderrabba
Materials 2019, 12(3), 361; https://doi.org/10.3390/ma12030361 - 24 Jan 2019
Cited by 41 | Viewed by 5156
Abstract
Dyes are classified as one of the major pollutants of water. They have negative impacts not only on environment but also on human health. In fact, wastewater that contains these harmful substances requires many types of treatments. Therefore, alternative methods and adsorption agents [...] Read more.
Dyes are classified as one of the major pollutants of water. They have negative impacts not only on environment but also on human health. In fact, wastewater that contains these harmful substances requires many types of treatments. Therefore, alternative methods and adsorption agents are needed. Herein, we propose to evaluate the decolorization of methylene blue (MB) and methyl orange (MO) as two models of soluble dyes from water using chitin and chitosan-graft-polyacrylamide. Furthermore, the applicability of these biomacromolecules as alternative adsorption agents, their sticking probability and desorption were also examined. Experimental parameters such as dye concentration, contact time, pH solution, adsorbent dosage and temperature were thoroughly examined for the grafted chitosan and chitin. The activation energy ( E a ) and the thermodynamic variables (i.e., standard Gibb’s free energy ( Δ G 0 ), standard enthalpy ( Δ H 0 ), and standard entropy ( Δ S 0 )) were determined using the Van’t Hoff and Arrhenius equations. The sticking probability ( S *) model for MB and MO removal by chitin and the chitosan derivative demonstrated that both dyes were successfully removed under the proposed conditions. Desorption studies of MB and MO showed the reusability of both materials, suggesting their application for removing dyes from aqueous solution. Full article
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11 pages, 4687 KiB  
Article
3D Arrays of Super-Hydrophobic Microtubes from Polypore Mushrooms as Naturally-Derived Systems for Oil Absorption
by Gianluca Balzamo, Naval Singh, Ningjing Wang, Goran T. Vladisavljević, Guido Bolognesi and Elisa Mele
Materials 2019, 12(1), 132; https://doi.org/10.3390/ma12010132 - 3 Jan 2019
Cited by 7 | Viewed by 4109
Abstract
Porous materials derived from natural resources, such as Luffa sponges, pomelo peel and jute fibres, have recently emerged as oil adsorbents for water purification, due to their suitability, low environmental impact, biodegradability and low cost. Here we show, for the first time, that [...] Read more.
Porous materials derived from natural resources, such as Luffa sponges, pomelo peel and jute fibres, have recently emerged as oil adsorbents for water purification, due to their suitability, low environmental impact, biodegradability and low cost. Here we show, for the first time, that the porosity of the fruiting body of polypore mushrooms can be used to absorb oils and organic solvents while repelling water. We engineered the surface properties of Ganoderma applanatum fungi, of which the fruiting body consists of a regular array of long capillaries embedded in a fibrous matrix, with paraffin wax, octadecyltrichlorosilane (OTS) and trichloro(1H,1H,2H,2H-perfluorooctyl)silane. Morphological and wettability analyses of the modified fungus revealed that the OTS treatment was effective in preserving the 3D porosity of the natural material, inducing super-hydrophobicity (water contact angle higher than 150°) and improving oil sorption capacity (1.8–3.1 g/g). The treated fungus was also inserted into fluidic networks as a filtration element, and its ability to separate water from chloroform was demonstrated. Full article
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13 pages, 3371 KiB  
Article
Hybrid Composites of Polylactide with Basalt and Carbon Fibers and Their Thermal Treatment
by Stanisław Kuciel and Paulina Romańska
Materials 2019, 12(1), 95; https://doi.org/10.3390/ma12010095 - 28 Dec 2018
Cited by 16 | Viewed by 3290
Abstract
In this research, polylactide was hybrid-reinforced and heat-treated in order to obtain durable structural materials with the use of eco-friendly components. Differential scanning calorimetry (DSC) analysis, tensile tests at various temperatures, Vicat tests, impact tests, and microscopic observations were conducted on the annealed [...] Read more.
In this research, polylactide was hybrid-reinforced and heat-treated in order to obtain durable structural materials with the use of eco-friendly components. Differential scanning calorimetry (DSC) analysis, tensile tests at various temperatures, Vicat tests, impact tests, and microscopic observations were conducted on the annealed and non-heat-treated specimens. The theoretical and true density, as well as water absorption, were also determined. The simultaneous introduction of chopped carbon and basalt fibers in equal mass fractions of 7.5% and 12.5% resulted in satisfactory increases in stiffness and tensile strength. The reinforcing effect was more efficient for the heat-treated composites, especially at elevated temperatures. Heat treatment significantly increased the degree of crystallinity of the matrix, improving heat resistance and reducing water absorption. It also reduced the stress concentrations in the injection-molded specimens. Full article
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13 pages, 1344 KiB  
Article
Valorization of Tomato Processing by-Products: Fatty Acid Extraction and Production of Bio-Based Materials
by José J. Benítez, Paula M. Castillo, José C. Del Río, Manuel León-Camacho, Eva Domínguez, Antonio Heredia, Susana Guzmán-Puyol, Athanassia Athanassiou and José A. Heredia-Guerrero
Materials 2018, 11(11), 2211; https://doi.org/10.3390/ma11112211 - 7 Nov 2018
Cited by 54 | Viewed by 5533
Abstract
A method consisting of the alkaline hydrolysis of tomato pomace by-products has been optimized to obtain a mixture of unsaturated and polyhydroxylated fatty acids as well as a non-hydrolysable secondary residue. Reaction rates and the activation energy of the hydrolysis were calculated to [...] Read more.
A method consisting of the alkaline hydrolysis of tomato pomace by-products has been optimized to obtain a mixture of unsaturated and polyhydroxylated fatty acids as well as a non-hydrolysable secondary residue. Reaction rates and the activation energy of the hydrolysis were calculated to reduce costs associated with chemicals and energy consumption. Lipid and non-hydrolysable fractions were chemically (infrared (IR) spectroscopy, gas chromatography/mass spectrometry (GC-MS)) and thermally (differential scanning calorimetry (DSC), thermogravimetric analysis (TGA)) characterized. In addition, the fatty acid mixture was used to produce cutin-based polyesters. Freestanding films were prepared by non-catalyzed melt-polycondensation and characterized by Attenuated Total Reflected-Fourier Transform Infrared (ATR-FTIR) spectroscopy, solid-state nuclear magnetic resonance (NMR), DSC, TGA, Water Contact Angles (WCA), and tensile tests. These bio-based polymers were hydrophobic, insoluble, infusible, and thermally stable, their physical properties being tunable by controlling the presence of unsaturated fatty acids and oxygen in the reaction. The participation of an oxidative crosslinking side reaction is proposed to be responsible for such modifications. Full article
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20 pages, 4532 KiB  
Article
Significance of a Non-Thermal Plasma Treatment on LDPE Biodegradation with Pseudomonas Aeruginosa
by Laurence Scally, Miroslav Gulan, Lars Weigang, Patrick J. Cullen and Vladimir Milosavljevic
Materials 2018, 11(10), 1925; https://doi.org/10.3390/ma11101925 - 10 Oct 2018
Cited by 24 | Viewed by 4334
Abstract
The use of plastics has spanned across almost all aspects of day to day life. Although their uses are invaluable, they contribute to the generation of a lot of waste products that end up in the environment and end up polluting natural habitats [...] Read more.
The use of plastics has spanned across almost all aspects of day to day life. Although their uses are invaluable, they contribute to the generation of a lot of waste products that end up in the environment and end up polluting natural habitats such as forests and the ocean. By treating low-density polyethylene (LDPE) samples with non-thermal plasma in ambient air and with an addition of ≈4% CO2, the biodegradation of the samples can be increased due to an increase in oxidative species causing better cell adhesion and acceptance on the polymer sample surface. It was, however, found that the use of this slight addition of CO2 aided in the biodegradation of the LDPE samples more than with solely ambient air as the carbon bonds measured from Raman spectroscopy were seen to decrease even more with this change in gas composition and chemistry. The results show that the largest increase of polymer degradation occurs when a voltage of 32 kV is applied over 300 s and with a mixture of ambient air and CO2 in the ratio 25:1. Full article
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13 pages, 3867 KiB  
Article
3D-Printed PCL/PLA Composite Stents: Towards a New Solution to Cardiovascular Problems
by Antonio J. Guerra, Paula Cano, Marc Rabionet, Teresa Puig and Joaquim Ciurana
Materials 2018, 11(9), 1679; https://doi.org/10.3390/ma11091679 - 11 Sep 2018
Cited by 124 | Viewed by 13324
Abstract
Biodegradable stents (BRS) offer enormous potential but first they must meet five specific requirements: (i) their manufacturing process must be precise; (ii) degradation should have minimal toxicity; (iii) the rate of degradation should match the recovery rate of vascular tissue; (iv) ideally, they [...] Read more.
Biodegradable stents (BRS) offer enormous potential but first they must meet five specific requirements: (i) their manufacturing process must be precise; (ii) degradation should have minimal toxicity; (iii) the rate of degradation should match the recovery rate of vascular tissue; (iv) ideally, they should induce rapid endothelialization to restore the functions of vascular tissue, but at the same time reduce the risk of restenosis; and (v) their mechanical behavior should comply with medical requirements, namely, the flexibility required to facilitate placement but also sufficient radial rigidity to support the vessel. Although the first three requirements have been comprehensively studied, the last two have been overlooked. One possible way of addressing these issues would be to fabricate composite stents using materials that have different mechanical, biological, or medical properties, for instance, Polylactide Acid (PLA) or Polycaprolactone (PCL). However, fashioning such stents using the traditional stent manufacturing process known as laser cutting would be impossible. Our work, therefore, aims to produce PCL/PLA composite stents using a novel 3D tubular printer based on Fused Deposition Modelling (FDM). The cell geometry (shape and area) and the materials (PCL and PLA) of the stents were analyzed and correlated with 3T3 cell proliferation, degradation rates, dynamic mechanical and radial expansion tests to determine the best parameters for a stent that will satisfy the five strict BRS requirements. Results proved that the 3D-printing process was highly suitable for producing composite stents (approximately 85–95% accuracy). Both PCL and PLA demonstrated their biocompatibility with PCL stents presenting an average cell proliferation of 12.46% and PLA 8.28% after only 3 days. Furthermore, the PCL/PLA composite stents demonstrated their potential in degradation, dynamic mechanical and expansion tests. Moreover, and regardless of the order of the layers, the composite stents showed (virtually) medium levels of degradation rates and mechanical modulus. Radially, they exhibited the virtues of PCL in the expansion step (elasticity) and those of PLA in the recoil step (rigidity). Results have clearly demonstrated that composite PCL/PLA stents are a highly promising solution to fulfilling the rigorous BRS requirements. Full article
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11 pages, 3594 KiB  
Article
Effect of Antibacterial Plant Extracts on the Morphology of Electrospun Poly(Lactic Acid) Fibres
by Peiwen Wang and Elisa Mele
Materials 2018, 11(6), 923; https://doi.org/10.3390/ma11060923 - 30 May 2018
Cited by 29 | Viewed by 5446
Abstract
Essential oils (EOs) of clary sage and black pepper induce changes in the morphology of poly(lactic acid) (PLA) electrospun fibres. The chemical composition of the oils is analysed by gas chromatography-mass spectrometry and Fourier-transform infrared spectroscopy; while the evaporation rate of the EOs [...] Read more.
Essential oils (EOs) of clary sage and black pepper induce changes in the morphology of poly(lactic acid) (PLA) electrospun fibres. The chemical composition of the oils is analysed by gas chromatography-mass spectrometry and Fourier-transform infrared spectroscopy; while the evaporation rate of the EOs and their main chemical components is characterised by Thermogravimetric Analysis. The addition of EOs generate thermodynamic instabilities during the electrospinning process, leading to the formation of fibres with either wrinkled (for clary sage oil) or nano-textured surfaces (for black pepper oil). The morphology of the PLA-EOs fibres is investigated by Scanning Electron Microscopy. Together with a well-defined structure, the fibres produced also possess antibacterial activity, as demonstrated by viability loss tests conducted on E. coli and S. epidermidis. Bacteria inactivation efficiency of 76 and 100% is reported for the composite PLA/essential oils electrospun mats. The composite mats produced are promising in the biomedical field, where nanotopography offers physical cues to regulate cell behaviour, and the delivery of therapeutic compounds (essential oils) limits microbial growth. Full article
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18 pages, 10098 KiB  
Article
Protein-Based Nanoparticle Preparation via Nanoprecipitation Method
by Mohamad Tarhini, Ihsane Benlyamani, Selim Hamdani, Géraldine Agusti, Hatem Fessi, Hélène Greige-Gerges, Abderrazzak Bentaher and Abdelhamid Elaissari
Materials 2018, 11(3), 394; https://doi.org/10.3390/ma11030394 - 7 Mar 2018
Cited by 96 | Viewed by 10525
Abstract
Nanoparticles are nowadays largely investigated in the field of drug delivery. Among nanoparticles, protein-based particles are of paramount importance since they are natural, biodegradable, biocompatible, and nontoxic. There are several methods to prepare proteins containing nanoparticles, but only a few studies have been [...] Read more.
Nanoparticles are nowadays largely investigated in the field of drug delivery. Among nanoparticles, protein-based particles are of paramount importance since they are natural, biodegradable, biocompatible, and nontoxic. There are several methods to prepare proteins containing nanoparticles, but only a few studies have been dedicated to the preparation of protein- based nanoparticles. Then, the aim of this work was to report on the preparation of bovine serum albumin (BSA)-based nanoparticles using a well-defined nanoprecipitation process. Special attention has been dedicated to a systematic study in order to understand separately the effect of each operating parameter of the method (such as protein concentration, solvent/non-solvent volume ratio, non-solvent injection rate, ionic strength of the buffer solution, pH, and cross-linking) on the colloidal properties of the obtained nanoparticles. In addition, the mixing processes (batch or drop-wise) were also investigated. Using a well-defined formulation, submicron protein-based nanoparticles have been obtained. All prepared particles have been characterized in terms of size, size distribution, morphology, and electrokinetic properties. In addition, the stability of nanoparticles was investigated using Ultraviolet (UV) scan and electrophoresis, and the optimal conditions for preparing BSA nanoparticles by the nanoprecipitation method were concluded. Full article
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