Bio-Based Polymers' Application and Technology for Better Quality of Life

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

Deadline for manuscript submissions: closed (31 March 2024) | Viewed by 21449

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Guest Editor
School of Life Sciences Weihenstephan, Technical University of Munich, 85354 Freising, Germany
Interests: active food packaging; biopolymers; biodegradable polymers; green synthesis; polymerization; nanotechnology; nanocomposites; polysaccharides; semiconductors; wound dressing; drug formulation; release control
Special Issues, Collections and Topics in MDPI journals

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Guest Editor
Institute for Polymers, Composites and Biomaterials (IPCB-CNR), Via Campi Flegrei 34, 80078 Pozzuoli, Italy
Interests: sustainable polymers; blends and composites; stimuli-responsive micro and nanostructured polymer materials
Special Issues, Collections and Topics in MDPI journals

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Guest Editor
Institute for Polymers, Composites and Biomaterials (IPCB-CNR), Via Campi Flegrei 34, 80078 Pozzuoli, Italy
Interests: biodegradable polymers; chemical physical properties; mechanical properties; agri-food waste; circular economy process; food packaging; agriculture
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The environmental impact of petroleum-based polymers has generated a tremendous mass of plastic waste worldwide. To overcome this critical problem, biopolymers with a wide range of properties like biodegradability, biocompatibility, and decent mechanical properties can be the promising alternative for synthetic polymers in different fields such as food packaging, medical, pharmaceutical, cosmetic, and agriculture. This Special Issue plans to feature the application of bio-based polymers in various areas and technologies that make these materials more tangible and help us have a better environment. We invite the authors to participate in this Special Issue of Polymers and contribute to building a better life and a greener environment through their fascinating research and innovation.

Dr. Arash Moeini
Dr. Pierfrancesco Cerruti
Dr. Gabriella Santagata
Guest Editors

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Keywords

  • biopolymers
  • degradability
  • agri-food waste
  • polysaccharides
  • surface modification
  • drug formulation
  • nanotechnology
  • food packaging
  • active biomaterial
  • releasing Control
  • antimicrobial
  • wound dressing
  • insecticides
  • herbicides
  • cosmetics
  • pharmaceutical
  • drug delivery
  • scaffold
  • natural compounds
  • composites
  • copolymers

Published Papers (10 papers)

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Research

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20 pages, 1064 KiB  
Article
Biosynthesis of Polyhydroxyalkanoates in Cupriavidus necator B-10646 on Saturated Fatty Acids
by Natalia O. Zhila, Kristina Yu. Sapozhnikova, Evgeniy G. Kiselev, Ekaterina I. Shishatskaya and Tatiana G. Volova
Polymers 2024, 16(9), 1294; https://doi.org/10.3390/polym16091294 - 05 May 2024
Viewed by 140
Abstract
It has been established that the wild-type Cupriavidus necator B-10646 strain uses saturated fatty acids (SFAs) for growth and polyhydroxyalkanoate (PHA) synthesis. It uses lauric (12:0), myristic (14:0), palmitic (16:0) and stearic (18:0) acids as carbon sources; moreover, the elongation of the C-chain [...] Read more.
It has been established that the wild-type Cupriavidus necator B-10646 strain uses saturated fatty acids (SFAs) for growth and polyhydroxyalkanoate (PHA) synthesis. It uses lauric (12:0), myristic (14:0), palmitic (16:0) and stearic (18:0) acids as carbon sources; moreover, the elongation of the C-chain negatively affects the biomass and PHA yields. When bacteria grow on C12 and C14 fatty acids, the total biomass and PHA yields are comparable up to 7.5 g/L and 75%, respectively, which twice exceed the values that occur on longer C16 and C18 acids. Regardless of the type of SFAs, bacteria synthesize poly(3-hydroxybutyrate), which have a reduced crystallinity (Cx from 40 to 57%) and a molecular weight typical for poly(3-hydroxybutyrate) (P(3HB)) (Mw from 289 to 465 kDa), and obtained polymer samples demonstrate melting and degradation temperatures with a gap of about 100 °C. The ability of bacteria to assimilate SFAs opens up the possibility of attracting the synthesis of PHAs on complex fat-containing substrates, including waste. Full article
20 pages, 6290 KiB  
Article
Microfluidic-Assisted Formulation of ε-Polycaprolactone Nanoparticles and Evaluation of Their Properties and In Vitro Cell Uptake
by Ewa Rybak, Piotr Kowalczyk, Sylwia Czarnocka-Śniadała, Michał Wojasiński, Jakub Trzciński and Tomasz Ciach
Polymers 2023, 15(22), 4375; https://doi.org/10.3390/polym15224375 - 10 Nov 2023
Viewed by 933
Abstract
The nanoprecipitation method was used to formulate ε-polycaprolactone (PCL) into fluorescent nanoparticles. Two methods of mixing the phases were evaluated: introducing the organic phase into the aqueous phase dropwise and via a specially designed microfluidic device. As a result of the nanoprecipitation process, [...] Read more.
The nanoprecipitation method was used to formulate ε-polycaprolactone (PCL) into fluorescent nanoparticles. Two methods of mixing the phases were evaluated: introducing the organic phase into the aqueous phase dropwise and via a specially designed microfluidic device. As a result of the nanoprecipitation process, fluorescein-loaded nanoparticles (NPs) with a mean diameter of 127 ± 3 nm and polydispersity index (PDI) of 0.180 ± 0.009 were obtained. The profiles of dye release were determined in vitro using dialysis membrane tubing, and the results showed a controlled release of the dye from NPs. In addition, the cytotoxicity of the NPs was assessed using an MTT assay. The PCL NPs were shown to be safe and non-toxic to L929 and MG63 cells. The results of the present study have revealed that PCL NPs represent a promising system for developing new drug delivery systems. Full article
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15 pages, 3292 KiB  
Article
Curing Kinetics of Bioderived Furan-Based Epoxy Resins: Study on the Effect of the Epoxy Monomer/Hardener Ratio
by Angela Marotta, Noemi Faggio and Cosimo Brondi
Polymers 2022, 14(23), 5322; https://doi.org/10.3390/polym14235322 - 05 Dec 2022
Cited by 2 | Viewed by 1389
Abstract
The potential of furan-based epoxy thermosets as a greener alternative to diglycidyl ether of Bisphenol A (DGEBA)-based resins has been demonstrated in recent literature. Therefore, a deep investigation of the curing behaviour of these systems may allow their use for industrial applications. In [...] Read more.
The potential of furan-based epoxy thermosets as a greener alternative to diglycidyl ether of Bisphenol A (DGEBA)-based resins has been demonstrated in recent literature. Therefore, a deep investigation of the curing behaviour of these systems may allow their use for industrial applications. In this work, the curing mechanism of 2,5-bis[(oxiran-2-ylmethoxy)methyl]furan (BOMF) with methyl nadic anhydride (MNA) in the presence of 2-methylimidazole as a catalyst is analyzed. In particular, three systems characterized by different epoxy/anhydride molar ratios are investigated. The curing kinetics are studied through differential scanning calorimetry, both in isothermal and non-isothermal modes. The total heat of reaction of the epoxy resin as well as its activation energy are estimated by the non-isothermal measurements, while the fitting of isothermal data with Kamal’s autocatalytic model provides the kinetic parameters. The results are discussed as a function of the resin composition. The global activation energy for the curing process of BOMF/MNA resins is in the range 72–79 kJ/mol, depending on both the model used and the sample composition; higher values are experienced by the system with balanced stoichiometry. By the fitting of the isothermal analysis, it emerged that the order of reaction is not only dependent on the temperature, but also on the composition, even though the values range between 0.31 and 1.24. Full article
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11 pages, 1063 KiB  
Article
Impact of Crosslinking on the Characteristics of Pectin Monolith Cryogels
by Aleksandra Nesic, Sladjana Meseldzija, Antonije Onjia and Gustavo Cabrera-Barjas
Polymers 2022, 14(23), 5252; https://doi.org/10.3390/polym14235252 - 01 Dec 2022
Cited by 4 | Viewed by 1237
Abstract
In this research, the pectin monoliths were prepared via the sol-gel process through different routes of crosslinking and additional freeze-drying. The crosslinking reaction was induced by the use of calcium ions in aqueous solutions and in alcohol/water solutions. The resulting pectin monoliths obtained [...] Read more.
In this research, the pectin monoliths were prepared via the sol-gel process through different routes of crosslinking and additional freeze-drying. The crosslinking reaction was induced by the use of calcium ions in aqueous solutions and in alcohol/water solutions. The resulting pectin monoliths obtained by freeze-drying were macroporous with open cells, limited specific surface area, moderate mechanical stability and moderate biodegradation rate. The presence of alcohol in crosslinking solution significantly changed the morphology of final pectin monoliths, which was evidenced by the reduction of their pore size for one order. The specific surface area of pectin monoliths obtained through the calcium-water-alcohol route was 25.7 m2/g, the Young compressive modulus was 0.52 MPa, and the biodegradation rate was 45% after 30 days of immersion in compost media. Considering that pectin can be obtained from food waste, and its physical properties could be tailored by different crosslinking routes, the pectin monoliths could find wide application in the pharmaceutical, agricultural, medical and food industries, providing sustainable development concepts. Full article
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14 pages, 5009 KiB  
Article
Upcycling of Poly(Lactic Acid) by Reactive Extrusion with Recycled Polycarbonate: Morphological and Mechanical Properties of Blends
by Vito Gigante, Laura Aliotta, Maria-Beatrice Coltelli and Andrea Lazzeri
Polymers 2022, 14(23), 5058; https://doi.org/10.3390/polym14235058 - 22 Nov 2022
Cited by 1 | Viewed by 1577
Abstract
Poly(lactic acid) (PLA) is one of the most promising renewable polymers to be employed to foster ecological and renewable materials in many fields of application. To develop high-performance products, however, the thermal resistance and the impact properties should be improved. At the same [...] Read more.
Poly(lactic acid) (PLA) is one of the most promising renewable polymers to be employed to foster ecological and renewable materials in many fields of application. To develop high-performance products, however, the thermal resistance and the impact properties should be improved. At the same time, it is also necessary to consider the end of life through the exploration of property assessment, following reprocessing. In this context the aim of the paper is to develop PLA/PC blends, obtained from recycled materials, in particular scraps from secondary processing, to close the recycling loop. Indeed, the blending of PLA with polycarbonate (PC) was demonstrated to be a successful strategy to improve thermomechanical properties that happens after several work cycles. The correlation between the compositions and properties was then investigated by considering the morphology of the blends; in addition, the reactive extrusions resulting in the formation of a PLA-PC co-polymer were investigated. The materials obtained are then examined by means of a dynamic-mechanical analysis (DMTA) to study the relaxations and transitions. Full article
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20 pages, 1790 KiB  
Article
Slow-Release Nitrogen Fertilizers with Biodegradable Poly(3-hydroxybutyrate) Coating: Their Effect on the Growth of Maize and the Dynamics of N Release in Soil
by Soňa Kontárová, Radek Přikryl, Petr Škarpa, Tomáš Kriška, Jiří Antošovský, Zuzana Gregušková, Silvestr Figalla, Vojtěch Jašek, Marek Sedlmajer, Přemysl Menčík and Mária Mikolajová
Polymers 2022, 14(20), 4323; https://doi.org/10.3390/polym14204323 - 14 Oct 2022
Cited by 7 | Viewed by 5344
Abstract
Fertilizers play an essential role in agriculture due to the rising food demand. However, high input fertilizer concentration and the non-controlled leaching of nutrients cause an unwanted increase in reactive, unassimilated nitrogen and induce environmental pollution. This paper investigates the preparation and properties [...] Read more.
Fertilizers play an essential role in agriculture due to the rising food demand. However, high input fertilizer concentration and the non-controlled leaching of nutrients cause an unwanted increase in reactive, unassimilated nitrogen and induce environmental pollution. This paper investigates the preparation and properties of slow-release fertilizer with fully biodegradable poly(3-hydroxybutyrate) coating that releases nitrogen gradually and is not a pollutant for soil. Nitrogen fertilizer (calcium ammonium nitrate) was pelletized with selected filler materials (poly(3-hydroxybutyrate), struvite, dried biomass). Pellets were coated with a solution of poly(3-hydroxybutyrate) in dioxolane that formed a high-quality and thin polymer coating. Coated pellets were tested in aqueous and soil environments. Some coated pellets showed excellent resistance even after 76 days in water, where only 20% of the ammonium nitrate was released. Pot experiments in Mitscherlich vegetation vessels monitored the effect of the application of coated fertilizers on the development and growth of maize and the dynamics of N release in the soil. We found that the use of our coated fertilizers in maize nutrition is a suitable way to supply nutrients to plants concerning their needs and that the poly(3-hydroxybutyrate) that was used for the coating does not adversely affect the growth of maize plants. Full article
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17 pages, 6479 KiB  
Article
Controlled Release Mechanism of Vancomycin from Double-Layer Poly-L-Lactic Acid-Coated Implants for Prevention of Bacterial Infection
by Papon Thamvasupong and Kwanchanok Viravaidya-Pasuwat
Polymers 2022, 14(17), 3493; https://doi.org/10.3390/polym14173493 - 26 Aug 2022
Cited by 2 | Viewed by 1883
Abstract
Implantation failure due to bacterial infection incurs significant medical expenditure annually, and treatment tends to be complicated. This study proposes a method to prevent bacterial infection in implants using an antibiotic delivery system consisting of vancomycin loaded into poly-L-lactic acid (PLLA) matrices. A [...] Read more.
Implantation failure due to bacterial infection incurs significant medical expenditure annually, and treatment tends to be complicated. This study proposes a method to prevent bacterial infection in implants using an antibiotic delivery system consisting of vancomycin loaded into poly-L-lactic acid (PLLA) matrices. A thin layer of this antibiotic-containing polymer was formed on stainless steel surfaces using a simple dip-coating method. SEM images of the polymeric layer revealed a honeycomb structure of the PLLA network with the entrapment of vancomycin molecules inside. In the in vitro release study, a rapid burst release was observed, followed by a sustained release of vancomycin for approximately 3 days. To extend the release time, a drug-free topcoat of PLLA was introduced to provide a diffusion resistance layer. As expected, the formulation with the drug-free topcoat exhibited a significant extension of the release time to approximately three weeks. Furthermore, the bonding strength between the double-layer polymer and the stainless steel substrate, which was an important property reflecting the quality of the coating, significantly increased compared to that of the single layer to the level that met the requirement for medical coating applications. The release profile of vancomycin from the double-layer PLLA film was best fitted with the Korsmeyer–Peppas model, indicating a combination of Fickian diffusion-controlled release and a polymer relaxation mechanism. More importantly, the double-layer vancomycin-PLLA coating exhibited antibacterial activity against S. aureus, as confirmed by the agar diffusion assay, the bacterial survival assay, and the inhibition of bacterial surface colonization without being toxic to normal cells (L929). Our results showed that the proposed antibiotic delivery system using the double-layer PLLA coating is a promising solution to prevent bacterial infection that may occur after orthopedic implantation. Full article
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16 pages, 3775 KiB  
Article
Spontaneous Gelation of Adhesive Catechol Modified Hyaluronic Acid and Chitosan
by Guillermo Conejo-Cuevas, Leire Ruiz-Rubio, Virginia Sáez-Martínez, Raul Pérez-González, Oihane Gartziandia, Amaia Huguet-Casquero and Leyre Pérez-Álvarez
Polymers 2022, 14(6), 1209; https://doi.org/10.3390/polym14061209 - 17 Mar 2022
Cited by 6 | Viewed by 2952
Abstract
Spontaneously formed hydrogels are attracting increasing interest as injectable or wound dressing materials because they do not require additional reactions or toxic crosslinking reagents. Highly valuable properties such as low viscosity before external application, adequate filmogenic capacity, rapid gelation and tissue adhesion are [...] Read more.
Spontaneously formed hydrogels are attracting increasing interest as injectable or wound dressing materials because they do not require additional reactions or toxic crosslinking reagents. Highly valuable properties such as low viscosity before external application, adequate filmogenic capacity, rapid gelation and tissue adhesion are required in order to use them for those therapeutic applications. In addition, biocompatibility and biodegradability are also mandatory. Accordingly, biopolymers, such as hyaluronic acid (HA) and chitosan (CHI), that have shown great potential for wound healing applications are excellent candidates due to their unique physiochemical and biological properties, such as moisturizing and antimicrobial ability, respectively. In this study, both biopolymers were modified by covalent anchoring of catechol groups, and the obtained hydrogels were characterized by studying, in particular, their tissue adhesiveness and film forming capacity for potential skin wound healing applications. Tissue adhesiveness was related to o-quinone formation over time and monitored by visible spectroscopy. Consequently, an opposite effect was observed for both polysaccharides. As gelation advances for HA-CA, it becomes more adhesive, while competitive reactions of quinone in CHI-CA slow down tissue adhesiveness and induce a detriment of the filmogenic properties. Full article
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Review

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48 pages, 17876 KiB  
Review
Self-Assembled Block Copolymers as a Facile Pathway to Create Functional Nanobiosensor and Nanobiomaterial Surfaces
by Marion Ryan C. Sytu, David H. Cho and Jong-in Hahm
Polymers 2024, 16(9), 1267; https://doi.org/10.3390/polym16091267 - 01 May 2024
Viewed by 450
Abstract
Block copolymer (BCP) surfaces permit an exquisite level of nanoscale control in biomolecular assemblies solely based on self-assembly. Owing to this, BCP-based biomolecular assembly represents a much-needed, new paradigm for creating nanobiosensors and nanobiomaterials without the need for costly and time-consuming fabrication steps. [...] Read more.
Block copolymer (BCP) surfaces permit an exquisite level of nanoscale control in biomolecular assemblies solely based on self-assembly. Owing to this, BCP-based biomolecular assembly represents a much-needed, new paradigm for creating nanobiosensors and nanobiomaterials without the need for costly and time-consuming fabrication steps. Research endeavors in the BCP nanobiotechnology field have led to stimulating results that can promote our current understanding of biomolecular interactions at a solid interface to the never-explored size regimes comparable to individual biomolecules. Encouraging research outcomes have also been reported for the stability and activity of biomolecules bound on BCP thin film surfaces. A wide range of single and multicomponent biomolecules and BCP systems has been assessed to substantiate the potential utility in practical applications as next-generation nanobiosensors, nanobiodevices, and biomaterials. To this end, this Review highlights pioneering research efforts made in the BCP nanobiotechnology area. The discussions will be focused on those works particularly pertaining to nanoscale surface assembly of functional biomolecules, biomolecular interaction properties unique to nanoscale polymer interfaces, functionality of nanoscale surface-bound biomolecules, and specific examples in biosensing. Systems involving the incorporation of biomolecules as one of the blocks in BCPs, i.e., DNA–BCP hybrids, protein–BCP conjugates, and isolated BCP micelles of bioligand carriers used in drug delivery, are outside of the scope of this Review. Looking ahead, there awaits plenty of exciting research opportunities to advance the research field of BCP nanobiotechnology by capitalizing on the fundamental groundwork laid so far for the biomolecular interactions on BCP surfaces. In order to better guide the path forward, key fundamental questions yet to be addressed by the field are identified. In addition, future research directions of BCP nanobiotechnology are contemplated in the concluding section of this Review. Full article
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21 pages, 1004 KiB  
Review
Edible Polymers and Secondary Bioactive Compounds for Food Packaging Applications: Antimicrobial, Mechanical, and Gas Barrier Properties
by Arash Moeini, Parisa Pedram, Ehsan Fattahi, Pierfrancesco Cerruti and Gabriella Santagata
Polymers 2022, 14(12), 2395; https://doi.org/10.3390/polym14122395 - 13 Jun 2022
Cited by 23 | Viewed by 4105
Abstract
Edible polymers such as polysaccharides, proteins, and lipids are biodegradable and biocompatible materials applied as a thin layer to the surface of food or inside the package. They enhance food quality by prolonging its shelf-life and avoiding the deterioration phenomena caused by oxidation, [...] Read more.
Edible polymers such as polysaccharides, proteins, and lipids are biodegradable and biocompatible materials applied as a thin layer to the surface of food or inside the package. They enhance food quality by prolonging its shelf-life and avoiding the deterioration phenomena caused by oxidation, humidity, and microbial activity. In order to improve the biopolymer performance, antimicrobial agents and plasticizers are also included in the formulation of the main compounds utilized for edible coating packages. Secondary natural compounds (SC) are molecules not essential for growth produced by some plants, fungi, and microorganisms. SC derived from plants and fungi have attracted much attention in the food packaging industry because of their natural antimicrobial and antioxidant activities and their effect on the biofilm’s mechanical properties. The antimicrobial and antioxidant activities inhibit pathogenic microorganism growth and protect food from oxidation. Furthermore, based on the biopolymer and SC used in the formulation, their specific mass ratio, the peculiar physical interaction occurring between their functional groups, and the experimental procedure adopted for edible coating preparation, the final properties as mechanical resistance and gas barrier properties can be opportunely modulated. This review summarizes the investigations on the antimicrobial, mechanical, and barrier properties of the secondary natural compounds employed in edible biopolymer-based systems used for food packaging materials. Full article
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