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Polymers
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Natural Additives for Special and High Performance Polymeric Materials
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Natural Additives for Special and High Performance Polymeric Materials

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

Deadline for manuscript submissions: closed (31 December 2023) | Viewed by 43826

Special Issue Editors

Prof. Dr. Cornelia Vasile

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Guest Editor
Romanian Academy, “P.Poni” Institute of Macromolecular Chemistry, Physical Chemistry of Polymers Department, 41A Gr. Ghica Voda Alley, RO 700487 Iasi, Romania
Interests: polymeric (bionano)composites; biomaterials; biodegradation; polymer compatibility and biocompatibility; kinetics and thermodynamics of polymeric systems; food packaging, (active, bioactive, smart, (bio)degradable); drugs delivery; recovery of polymer wastes by destructive and non-destructive procedures; environmental pollution and protection; smart polymers
Special Issues, Collections and Topics in MDPI journals
Dr. Elena Stoleru

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Guest Editor
Department of Physical Chemistry of Polymers, Petru Poni Institute of Macromolecular Chemistry, 41 A Grigore Ghica Voda Alley, 700487 Iasi, Romania
Interests: surface modification/grafting of polymers; food packaging (bioactive, responsive, biodegradable); stabilization of bioactive compounds; influence of radiation on polymers; polymer biodegradation; composites and nanocomposites; biocompatibility; electrospinning
Special Issues, Collections and Topics in MDPI journals
Dr. Bogdan Munteanu

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Guest Editor
Faculty of Physics, “Al. I. Cuza” University of Iasi, 11, Carol I blvd, RO 700506 Iasi, Romania
Interests: polymer physics; electrospinning/electrospraying; nanostructures; polymer surface physical chemistry; polymer degradation; synthetic/natural polymer copolymers ; blends; composite and nanocomposites; antioxidative action; biomaterials; drug delivery systems; controlled and targeting drug release

Special Issue Information

Dear Colleagues,

This Special Issue is dedicated to natural additives which, incorporated in small amounts  by various techniques or as nanoencapsulants, are destined to the delivery of nutrients (nutrition and neutraceuticals), flavors, aromas, drugs, antimicrobial and antioxidant compounds. The natural additives can be incorporated into different polymeric materials such as bioplastics, hybrid composites, antimicrobial materials, multifunctional polymeric biomaterials, pharmaceutical polymers, nanostructured polymers and nanocomposites, smart polymeric materials/nanoparticles, smart textiles, electrospun materials, polymer-clay nano-composites,   biodegradable materials and  waste-recycling materials, materials for tissue engineering, functionally responsive polymeric materials, etc.. The inclusion of these additives confers to the receiving materials special characteristics, such as antibacterial/antioxidant properties, biological functions, advanced functionalities, external stimuli responsiveness, flexibility, etc. Research on natural additives has recently become extremely fascinating, especially in relation to vegetable extracts (from plants and agricultural waste), nanoclays, biological polymers (such as alginate, chitosan (nanochitosan), chitin, etc. and their derivatives), lignocellulosics (lignin and its derivatives, nanocellulose). Compared to synthetic additives, natural additives have the advantages of being accepted in the medical and pharmaceutical fields, by the food industry, and by consumers as they are biocompatible, biodegradable, and sustainable.

The aim of this Special Issue is to bring the attention of contributors and readers the various aspects of natural additives: their obtainment, modification, morphology, the characterization of their physical and chemical properties, the thermodynamics and kinetics of multicomponent polymer systems, their degradation and stabilization, the effects of various kinds of radiation (electron beam, gamma irradiation, plasma, etc.) on their properties, and the stability of the special materials with high performance mentioned above. Also, their applications in the biomedical, nanomedicine, green industry fields, and food industry are of great interest, as well as the technological developments related to them.

Both research and review articles are welcome. Since you are working in this intriguing area, it is our pleasure to invite you to contribute a full paper, letter, communication, or review to this Special Issue. The authors are encouraged to submit manuscripts reporting unexpected results, providing they can present scientifically spotless explanations.

Prof. Dr. Cornelia Vasile
Dr. Elena Stoleru
Dr. Bogdan Munteanu
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • vegetable extracts (from plants and agricultural waste)
  • nanoclays
  • biological polymers (chitosan, chitin, etc., and their derivatives)
  • lignocellulosics (lignin and its derivatives, nanocellulose, nanochitosan)
  • thermodynamics and kinetics of multicomponent polymer systems
  • degradation and stabilization
  • composites and nanocomposites
  • blends
  • formulations
  • biomaterials
  • pharmaceutics
  • food industry
  • polymeric carriers

Published Papers (7 papers)

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Research

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28 pages, 23202 KiB  
Article
Effect of Gamma Irradiation on the PLA-Based Blends and Biocomposites Containing Rosemary Ethanolic Extract and Chitosan
by Cornelia Vasile, Daniela Pamfil, Traian Zaharescu, Raluca-Petronela Dumitriu, Gina Mihaela Pricope, Maria Râpă and Gabriel Vasilievici
Polymers 2022, 14(7), 1398; https://doi.org/10.3390/polym14071398 - 29 Mar 2022
Cited by 9 | Viewed by 2612
Abstract
The irradiation of polymeric materials with ionizing radiation (γ-rays, X-rays, accelerated electrons, ion beams, etc.) may lead to disproportion, hydrogen abstraction, arrangements, degradation, and/or the formation of new bonds. The purpose of this paper is to evaluate the effect of gamma irradiation on [...] Read more.
The irradiation of polymeric materials with ionizing radiation (γ-rays, X-rays, accelerated electrons, ion beams, etc.) may lead to disproportion, hydrogen abstraction, arrangements, degradation, and/or the formation of new bonds. The purpose of this paper is to evaluate the effect of gamma irradiation on some new poly(lactic acid) (PLA)-based blends and biocomposites, which is crucial when they are used for food packaging or medical purposes. The polymeric blends and biocomposites based on PLA and rosemary ethanolic extract (R) and poly(ethylene glycol) (PEG) (20 wt%) plasticized PLA, chitosan (CS) (3–6 wt%) and R (0.5 wt%) biocomposites were subjected to gamma irradiation treatment using three low γ-doses of 10, 20, and 30 kGy. The effect of irradiation was evaluated by Scanning Electron Microscopy (SEM), Fourier Transform Infrared Spectroscopy (FTIR), Differential Scanning Calorimetry (DSC), thermogravimetry (TG), chemiluminescence method (CL), migration studies, and antibacterial activity tests. It was found that in comparison with neat PLA, the gamma irradiation in the oxidative conditions of the PLA-based blends and biocomposites, causes modifications in the structure, morphology, and thermal properties of the materials depending on irradiation dose and the presence of natural additives such as rosemary and chitosan. It was established that under a gamma-irradiation treatment with dose of 10–20 kGy, the PLA materials showed minor changes in structure and properties being suitable for application in packaging and in addition after irradiation with such doses their antimicrobial activity against Escherichia coli, Staphylococcus aureus, and Salmonella typhimurium is improved. Full article
(This article belongs to the Special Issue Natural Additives for Special and High Performance Polymeric Materials)
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23 pages, 4708 KiB  
Article
Influence of the Chitosan and Rosemary Extract on Fungal Biodegradation of Some Plasticized PLA-Based Materials
by Elena Stoleru, Cornelia Vasile, Lăcramioara Oprică and Onur Yilmaz
Polymers 2020, 12(2), 469; https://doi.org/10.3390/polym12020469 - 18 Feb 2020
Cited by 9 | Viewed by 3046
Abstract
The fungal degradation of the complex polymeric systems based on poly(lactic acid) (PLA) and natural bioactive compounds (chitosan and powdered rosemary alcoholic extract) was studied. Two fungal strains, Chaetomium globosum and Phanerochaete chrysosporium were tested. Both fungi characteristics and changes in morphology, structure [...] Read more.
The fungal degradation of the complex polymeric systems based on poly(lactic acid) (PLA) and natural bioactive compounds (chitosan and powdered rosemary alcoholic extract) was studied. Two fungal strains, Chaetomium globosum and Phanerochaete chrysosporium were tested. Both fungi characteristics and changes in morphology, structure and thermal properties were monitored. Biochemical parameters as superoxide dismutase, catalase, soluble protein and malondialdehyde have been determined at different time periods of fungal degradation. The fungi extracellular enzyme activities are slightly decreased in the case of composites containing bioactive compounds. The presence of natural compounds in the PLA-based polymeric system determines an acceleration of fungal degradation and probably the chemical hydrolysis, which further helps the attachment of fungi on the surface of polymeric samples. Significant decreases in average molecular mass of the polymeric samples were observed by fungi action; accompanied by structural changes, increase in crystallinity and decrease of thermal properties and the loss of the physical integrity and finally to degradation and integration of fungal degradation products into environmental medium. It was found that both fungi tested are efficient for PLA-based materials degradation, the most active from them being Chaetomium globosum fungus. Full article
(This article belongs to the Special Issue Natural Additives for Special and High Performance Polymeric Materials)
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19 pages, 7222 KiB  
Article
Tough Polyelectrolyte Hydrogels with Antimicrobial Property via Incorporation of Natural Multivalent Phytic Acid
by Hoang Linh Bui and Chun-Jen Huang
Polymers 2019, 11(10), 1721; https://doi.org/10.3390/polym11101721 - 21 Oct 2019
Cited by 25 | Viewed by 5603
Abstract
Tough and antimicrobial dual-crosslinked poly((trimethylamino)ethyl methacrylate chloride)-phytic acid hydrogel (pTMAEMA-PA) has been synthesized by adding a chemical crosslinker and docking a physical crosslinker of multivalent phytic acid into a cationic polyelectrolyte network. By increasing the loading concentration of PA, the tough hydrogel exhibits [...] Read more.
Tough and antimicrobial dual-crosslinked poly((trimethylamino)ethyl methacrylate chloride)-phytic acid hydrogel (pTMAEMA-PA) has been synthesized by adding a chemical crosslinker and docking a physical crosslinker of multivalent phytic acid into a cationic polyelectrolyte network. By increasing the loading concentration of PA, the tough hydrogel exhibits compressive stress of >1 MPa, along with high elasticity and fatigue-resistant properties. The enhanced mechanical properties of pTMAEMA-PA stem from the multivalent ion effect of PA via the formation of ion bridges within polyelectrolytes. In addition, a comparative study for a series of pTMAEMA-counterion complexes was conducted to elaborate the relationship between swelling ratio and mechanical strength. The study also revealed secondary factors, such as ion valency, ion specificity and hydrogen bond formation, holding crucial roles in tuning mechanical properties of the polyelectrolyte hydrogel. Furthermore, in bacteria attachment and disk diffusion tests, pTMAEMA-PA exhibits superior fouling resistance and antibacterial capability. The results reflect the fact that PA enables chelating strongly with divalent metal ions, hence, disrupting the outer membrane of bacteria, as well as dysfunction of organelles, DNA and protein. Overall, the work demonstrated a novel strategy for preparation of tough polyelectrolyte with antibacterial capability via docking PA to open up the potential use of PA in medical application. Full article
(This article belongs to the Special Issue Natural Additives for Special and High Performance Polymeric Materials)
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19 pages, 3482 KiB  
Article
Chitosan-Graft-Poly(N-Isopropylacrylamide)/PVA Cryogels as Carriers for Mucosal Delivery of Voriconazole
by Catalina Natalia Cheaburu-Yilmaz, Onur Yilmaz, Fadime Aydin Kose and Nela Bibire
Polymers 2019, 11(9), 1432; https://doi.org/10.3390/polym11091432 - 31 Aug 2019
Cited by 34 | Viewed by 3899
Abstract
The objective of this study was to prepare and characterize physically crosslinked gel formulations of chitosan (CS)-graft-poly(N-isopropyl acrylamide) (PNIPAAm) and polyvinyl alcohol (PVA) for smart delivery of an antifungal drug, Voriconazole, for mucosal applications. For this purpose, cryogels of CS-g-PNIPAAm/PVA and [...] Read more.
The objective of this study was to prepare and characterize physically crosslinked gel formulations of chitosan (CS)-graft-poly(N-isopropyl acrylamide) (PNIPAAm) and polyvinyl alcohol (PVA) for smart delivery of an antifungal drug, Voriconazole, for mucosal applications. For this purpose, cryogels of CS-g-PNIPAAm/PVA and CS/PVA were tested by means of texture profile analysis and rheology to determine optimal matrix properties for topical application. The ratio of 75/25 v/v % CS-g-PNIPAAm/PVA was selected to be used for formulation since it gave low compressibility and hardness (1.2 and 0.6 N) as well as high adhesion properties and non-Newtonian flow behavior. The cryogels and formulations were further characterized by means of FTIR spectroscopy, swelling behavior, texture analysis, scanning electron microscopy (SEM), thermal (differential scanning calorimetry (DSC) and TGA), and rheological behavior. The drug loading capacity and in vitro release profile of the drug, storage stability, and cytotoxicity tests were also performed for the gel formulation. The FTIR, DSC, and TGA results verified the successful formation of cryogels. Swelling studies revealed a pH-dependent swelling ability with a maximum swelling degree of 1200% in acid and 990% in phosphate buffer (pH = 7.4). Thermal studies showed that CS-g-PNIPAAm/PVA 75/25 had higher thermal stability proving the structural complexity of the polymer. The loading capacity of Voriconazole was found to be 70% (w/w). The in vitro release profiles of Voriconazole showed Fickian release behavior for CS-g-PNIPAAm/PVA 75/25 gel with an approximate delivery of 38% within 8 h, slower than matrices containing unmodified chitosan. The storage stability test exhibited that the gel formulation was still stable even after aging for two months. Moreover, the cell culture assays revealed a non-toxic character of the polymeric matrix. Overall results showed that the CS-g-PNIPAAm/PVA 75/25 hydrogel has the potential to be used as a smart polymeric vehicle for topical applications. Full article
(This article belongs to the Special Issue Natural Additives for Special and High Performance Polymeric Materials)
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28 pages, 3162 KiB  
Article
Biocompatible Materials Based on Plasticized Poly(lactic acid), Chitosan and Rosemary Ethanolic Extract I. Effect of Chitosan on the Properties of Plasticized Poly(lactic acid) Materials
by Cornelia Vasile, Elena Stoleru, Raluca Nicoleta Darie-Niţa, Raluca Petronela Dumitriu, Daniela Pamfil and Liliana Tarţau
Polymers 2019, 11(6), 941; https://doi.org/10.3390/polym11060941 - 30 May 2019
Cited by 47 | Viewed by 5742
Abstract
The purpose of the present study is to develop new multifunctional environmentally friendly materials having applications both in medical and food packaging fields. New poly(lactic acid) (PLA)-based multifunctional materials containing additives derived from natural resources like chitosan (CS) and rosemary extract (R) were [...] Read more.
The purpose of the present study is to develop new multifunctional environmentally friendly materials having applications both in medical and food packaging fields. New poly(lactic acid) (PLA)-based multifunctional materials containing additives derived from natural resources like chitosan (CS) and rosemary extract (R) were obtained by melt mixing. Each of the selected components has its own specific properties such as: PLA is a biodegradable thermoplastic aliphatic polyester derived from renewable biomass, heat-resistant, with mechanical properties close to those of polystyrene and polyethylene terephthalate, and CS offers good antimicrobial activity and biological functions, while R significantly improves antioxidative action necessary in all applications. A synergy of their combination, an optimum choice of their ratio, and processing parameters led to high performance antimicrobial/antioxidant/biocompatible/environmentally degradable materials. The polyethylene glycol (PEG)-plasticized PLA/chitosan/powdered rosemary extract biocomposites of various compositions were characterized in respect to their mechanical and rheological properties, structure by spectroscopy, antioxidant and antimicrobial activities, and in vitro and in vivo biocompatibility. Scanning electron microscopy images evidence the morphology features added by rosemary powder presence in polymeric materials. Incorporation of additives improved elongation at break, antibacterial and antioxidant activity and also biocompatibility. Migration of bioactive components into D1 simulant is slower for PEG-plasticized PLA containing 6 wt % chitosan and 0.5 wt % rosemary extract (PLA/PEG/6CS/0.5 R) biocomposite and it occurred by a diffusion-controlled mechanism. The biocomposites show high hydrophilicity and good in vitro and in vivo biocompatibility. No hematological, biochemical and immunological modifications are induced by subcutaneous implantation of biocomposites. All characteristics of the PEG-plasticized PLA-based biocomposites recommend them as valuable materials for biomedical implants, and as well as for the design of innovative drug delivery systems. Also, the developed biocomposites could be a potential nature-derived active packaging with controlled release of antimicrobial/antioxidant compounds. Full article
(This article belongs to the Special Issue Natural Additives for Special and High Performance Polymeric Materials)
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Review

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22 pages, 1316 KiB  
Review
Environmental Degradation of Plastic Composites with Natural Fillers—A Review
by Mihai Brebu
Polymers 2020, 12(1), 166; https://doi.org/10.3390/polym12010166 - 08 Jan 2020
Cited by 100 | Viewed by 10857
Abstract
Polymer composites are widely used modern-day materials, specially designed to combine good mechanical properties and low density, resulting in a high tensile strength-to-weight ratio. However, materials for outdoor use suffer from the negative effects of environmental factors, loosing properties in various degrees. In [...] Read more.
Polymer composites are widely used modern-day materials, specially designed to combine good mechanical properties and low density, resulting in a high tensile strength-to-weight ratio. However, materials for outdoor use suffer from the negative effects of environmental factors, loosing properties in various degrees. In particular, natural fillers (particulates or fibers) or components induce biodegradability in the otherwise bio inert matrix of usual commodity plastics. Here we present some aspects found in recent literature related to the effect of aggressive factors such as temperature, mechanical forces, solar radiation, humidity, and biological attack on the properties of plastic composites containing natural fillers. Full article
(This article belongs to the Special Issue Natural Additives for Special and High Performance Polymeric Materials)
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34 pages, 2152 KiB  
Review
Vegetable Additives in Food Packaging Polymeric Materials
by Silvestru Bogdănel Munteanu and Cornelia Vasile
Polymers 2020, 12(1), 28; https://doi.org/10.3390/polym12010028 - 22 Dec 2019
Cited by 45 | Viewed by 10807
Abstract
Plants are the most abundant bioresources, providing valuable materials that can be used as additives in polymeric materials, such as lignocellulosic fibers, nano-cellulose, or lignin, as well as plant extracts containing bioactive phenolic and flavonoid compounds used in the healthcare, pharmaceutical, cosmetic, and [...] Read more.
Plants are the most abundant bioresources, providing valuable materials that can be used as additives in polymeric materials, such as lignocellulosic fibers, nano-cellulose, or lignin, as well as plant extracts containing bioactive phenolic and flavonoid compounds used in the healthcare, pharmaceutical, cosmetic, and nutraceutical industries. The incorporation of additives into polymeric materials improves their properties to make them suitable for multiple applications. Efforts are made to incorporate into the raw polymers various natural biobased and biodegradable additives with a low environmental fingerprint, such as by-products, biomass, plant extracts, etc. In this review we will illustrate in the first part recent examples of lignocellulosic materials, lignin, and nano-cellulose as reinforcements or fillers in various polymer matrices and in the second part various applications of plant extracts as active ingredients in food packaging materials based on polysaccharide matrices (chitosan/starch/alginate). Full article
(This article belongs to the Special Issue Natural Additives for Special and High Performance Polymeric Materials)
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