Biobased and Biodegradable Polymers

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

Deadline for manuscript submissions: closed (15 December 2020) | Viewed by 85958

Special Issue Editors

Laboratory of Polymer Chemistry and Technology, Department of Chemistry, Aristotle University of Thessaloniki, GR 54124 Thessaloniki, Greece
Interests: synthesis and characterization of polyesters; development of biobased polymers; biodegradable polymers; polymer composites and nanocomposites; synthesis and characterization of copolymers; polymer blends; recycling of polymers with various techniques; enzymatic hydrolysis studies; modification of natural polymers; polymer for wastewater treatment pollutant removal; polymers for tissue engineering and drug delivery applications; drug–polymer solid dispersions; drug targeting; drug nanoencapsulation and microencapsulation
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Special Issue Information

Dear Colleagues,

Following their initial discovery, the use of polymers has expanded to almost all human activities, making a significant contribution to better living conditions over the years. This is due to their low cost and unique mechanical and thermal properties, in combination with being lightweight and easy to formulate into different shapes and articles. This has led to the development of new polymers not previously found in nature; however, scientists did not also foresee that these materials should be environmentally friendly and degraded shortly after their use, as is the case with natural polymers. It is estimated that most synthetic plastics need 400–500 years to fully disintegrate; therefore, over time, they began to accumulate in the environment. The most important problem now arises from plastic packaging materials and single-use products, the majority of which end up in the marine ecosystem where they degrade slowly in small pieces or so-called “microplastic”. It is estimated that about 50 trillion pieces of plastic, in sizes less than 1 cm, are floating in the seas and are transferred into humans through the food chain. Hence, one solution to prevent this process is to produce eco-friendly polymers.

In recent years, as a potential replacement of fossil fuels, the production of appropriate monomers using inexpensive and renewable starting materials, such as cellulose, is being increasingly explored, with the aim of developing a more sustainable biobased economy. Cellulose is the main part of plant cell walls and the most abundant natural polymer, however, starch, chitin, lignin, proteins, and vegetable oils can also be used as renewable starting materials, and are currently being used to make new materials known as ‘bioplastics’. The production of polymers from renewable resources is an old practice, and the first approach involved the modification of natural polymers and monomer extraction for production of new polymers. Thus, during the middle of 18th century, Parkesine plastic was discovered, followed later by Galalith resin production, Bakelite, and cellophane at the beginning of 19th century. This practice has, however, been diminishing in the years following petroleum discovery. This is because monomers for polymer synthesis can be easily derived during oil refinery, at low cost and high purity, and at a large scale suitable for mass production. Due to the environmental pollution, this practice should change drastically in the next years, and most scientific efforts are focused on the production of plastics using monomers derived from natural and renewable sources.

Biobased polyesters are one of the most important classes of polymers. Various bioderived monomers are available on the market for polymer synthesis, including acids (levulinic acid, succinic, sebacic, adipic, aspartic, terephthalic, 2,5-furandicarboxylic, vanillic, itaconic, lactic, hydroxybutyric, 3-hydroxypropionic acid, etc.), glycols (ethylene glycol, 1,3-propanediol, 1,4-butanediol, isosorbide, xylitol, sorbitol, glycerol, etc.), as well as other monomers (ethylene, propylene, styrene, etc). Some biomass-derived polyesters (such as poly(lactic acid) (PLA), poly(butylene succinate) (PBS), poly(butylene adipate) (PBA), poly(butylene succinate adipate) (PBSA), etc.) and non-degradable alipharomatic polymers (such as poly(ethylene terephthalate) (PET), poly(butylene teraphtahlate) (PBT), poly(ethylene furan dicarboxylate) (PEF), poly(ethylene vanillate) (PEV), polyethylene (bio-PE), polypropylene (bio-PP), polystyrene (bio-PS), polyamides (bio-PA), etc.), and several of their copolymers, are currently among the most promising biobased polymers. Bioplastics can contribute to a better life and environment sustainability. It is estimated that by 2050 they will cover more than 40%–50% of the global plastics market. The development of new forms of plastics originating from natural sources also has the benefit of carbon footprint reduction by up to 60% when compared to conventional plastics. Hence, the future of plastics is indeed ‘green’.

The aim of this Special Issue is to highlight the progress and fundamental aspects of biobased monomers derived from renewable resources, as well as of the synthesis, characterization, properties, and applications of biobased and biodegradable polymers, and also of related copolymers, blends, composites, and nanocomposites.

Prof. Dimitrios Bikiaris
Prof. Dr. George Z. Papageorgiou
Guest Editors

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Keywords

  • biobased polymers
  • monomers from renewable resources
  • biodegradable polymers
  • bioplastics
  • sustainable materials
  • eco-friendly materials
  • benign polymer synthesis
  • enzymatic hydrolysis
  • aliphatic polyesters
  • copolymers
  • thermal properties
  • mechanical properties
  • lifecycle

Published Papers (18 papers)

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10 pages, 667 KiB  
Article
Is the Polylactic Acid Fiber in Green Compost a Risk for Lumbricus terrestris and Triticum aestivum?
by Esperanza Huerta-Lwanga, Jorge Mendoza-Vega, Oriana Ribeiro, Henny Gertsen, Piet Peters and Violette Geissen
Polymers 2021, 13(5), 703; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13050703 - 26 Feb 2021
Cited by 32 | Viewed by 2489
Abstract
Polylactic acid (PLA) bioplastic was introduced to the market as an environmentally friendly potential solution for plastic pollution. However, the effects of bioplastic debris mixed with composts on soil macroinvertebrates, plant growth and soil conditions are still unknown. Soil macroinvertebrates are soil health [...] Read more.
Polylactic acid (PLA) bioplastic was introduced to the market as an environmentally friendly potential solution for plastic pollution. However, the effects of bioplastic debris mixed with composts on soil macroinvertebrates, plant growth and soil conditions are still unknown. Soil macroinvertebrates are soil health indicators. A reduction in their abundance is a sign of soil degradation. The objectives of this study were (i) to assess PLA debris in greenhouse composts, and (ii) to test the ecotoxicological effects of PLA debris mixed with compost on Lumbricus terrestris, a soil organism model, and on Triticum aestevium, a plant growth model. The study was comprised of three stages: (1) determine the PLA debris size distribution in composts; (2) assess the ecotoxicological effects of real-world concentrations (0% to 5%) of PLA mixed with compost on earthworm mortality and reproduction; and (3) assess the influence of compost mixed with real-world PLA concentrations on plant growth and physicochemical soil conditions. One percent of PLA debris was found in green composts, 40% of composted PLA debris measured between 1–10 mm, with a concentration of 82.8 ± 17.4 microplastics.gram−1 compost. A concentration of 1% PLA in composts resulted in significant mortality in earthworms. No significant effects of PLA mixed with composts were observed on plant growth or soil physicochemical conditions. Further studies are required in order to test the effect of this biopolymer on different earthworm and plant’ species. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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18 pages, 4926 KiB  
Article
Preparation and Evaluation of Collagen-Based Patches as Curcumin Carriers
by Zoi Terzopoulou, Anna Michopoulou, Artemis Palamidi, Elena Koliakou and Dimitrios Bikiaris
Polymers 2020, 12(10), 2393; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12102393 - 17 Oct 2020
Cited by 20 | Viewed by 3816
Abstract
Patients with psoriasis are dissatisfied with the standard pharmacological treatments, whether systemic or topical, with many of them showing interest in complementary and alternative medicine. Curcumin (Cur), a natural polyphenol derived from turmeric, has recently gained attention for skin-related diseases because of its [...] Read more.
Patients with psoriasis are dissatisfied with the standard pharmacological treatments, whether systemic or topical, with many of them showing interest in complementary and alternative medicine. Curcumin (Cur), a natural polyphenol derived from turmeric, has recently gained attention for skin-related diseases because of its proven anti-inflammatory action. However, topical treatment with Cur would be inadequate because of its hydrophobicity, instability, and low bioavailability. In addition, hyperkeratosis and lack of moisture in psoriatic skin result in low penetration that would prevent actives from permeating the stratum corneum. In this work, a polymer-based formulation of Cur for the topical treatment of psoriasis is reported. To improve the physicochemical stability of Cur, it was first encapsulated in chitosan nanoparticles. The Cur-loaded nanoparticles were incorporated in a hydrophilic, biocompatible collagen-based patch. The nanoparticle-containing porous collagen patches were then chemically cross-linked. Morphology, chemical interactions, swelling ratio, enzymatic hydrolysis, and Cur release from the patches were evaluated. All patches showed excellent swelling ratio, up to ~1500%, and after cross-linking, the pore size decreased, and their hydrolysis rates decelerated. The in vitro release of Cur was sustained with an initial burst release, reaching 55% after 24 h. Cur within the scaffolds imparted a proliferation inhibitory effect on psoriatic human keratinocytes in vitro. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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11 pages, 1719 KiB  
Article
Anatase Incorporation to Bioactive Scaffolds Based on Salmon Gelatin and Its Effects on Muscle Cell Growth
by Cristian A. Acevedo, Yusser Olguín, Nicole Orellana, Elizabeth Sánchez, Marzena Pepczynska and Javier Enrione
Polymers 2020, 12(9), 1943; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12091943 - 28 Aug 2020
Cited by 2 | Viewed by 2006
Abstract
The development of new polymer scaffolds is essential for tissue engineering and for culturing cells. The use of non-mammalian bioactive components to formulate these materials is an emerging field. In our previous work, a scaffold based on salmon gelatin was developed and tested [...] Read more.
The development of new polymer scaffolds is essential for tissue engineering and for culturing cells. The use of non-mammalian bioactive components to formulate these materials is an emerging field. In our previous work, a scaffold based on salmon gelatin was developed and tested in animal models to regenerate tissues effectively and safely. Here, the incorporation of anatase nanoparticles into this scaffold was formulated, studying the new composite structure by scanning electron microscopy, differential scanning calorimetry and dynamic mechanical analysis. The incorporation of anatase nanoparticles modified the scaffold microstructure by increasing the pore size from 208 to 239 µm and significantly changing the pore shape. The glass transition temperature changed from 46.9 to 55.8 °C, and an increase in the elastic modulus from 79.5 to 537.8 kPa was observed. The biocompatibility of the scaffolds was tested using C2C12 myoblasts, modulating their attachment and growth. The anatase nanoparticles modified the stiffness of the material, making it possible to increase the growth of myoblasts cultured onto scaffolds, which envisions their use in muscle tissue engineering. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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12 pages, 1992 KiB  
Article
Effect of Ultrasonic and Microwave Dual-Treatment on the Physicochemical Properties of Chestnut Starch
by Meng Wang, Yanwen Wu, Yongguo Liu and Jie Ouyang
Polymers 2020, 12(8), 1718; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12081718 - 31 Jul 2020
Cited by 48 | Viewed by 3744
Abstract
This work examined the effect of ultrasound and microwave treatments, separate and in combination, on the physicochemical and functional properties of chestnut starch. The results revealed that the ultrasonic-microwave (UM) and microwave-ultrasonic (MU) dually modified samples exhibited more severe surface damage, weaker birefringence, [...] Read more.
This work examined the effect of ultrasound and microwave treatments, separate and in combination, on the physicochemical and functional properties of chestnut starch. The results revealed that the ultrasonic-microwave (UM) and microwave-ultrasonic (MU) dually modified samples exhibited more severe surface damage, weaker birefringence, and lower relative crystallinity and gelatinization enthalpy than the native and single-treated starches. The UM samples showed the highest oil absorption capacity, and the MU samples showed the highest water absorption capacity and the best freeze-thaw stability (five cycles) among all samples. The swelling power, peak, trough, final, and breakdown viscosities, and pasting temperature all decreased regardless of single or dual modification. This study provides a reference for potential industrial applications of ultrasound and microwave treatments for the modification of chestnut starch. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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15 pages, 6762 KiB  
Article
Influence of Composition and Plasma Power on Properties of Film from Biodegradable Polymer Blends
by Leona Omaníková, Ján Bočkaj, Mirko Černák, Roderik Plavec, Jozef Feranc and Patrik Jurkovič
Polymers 2020, 12(7), 1592; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071592 - 17 Jul 2020
Cited by 6 | Viewed by 2352
Abstract
The work is focused on the study of surface plasma treatment (DCSBD) of films from biodegradable polymers from renewable sources based on polylactic acid (PLA) and polyhydroxybutyrate (PHB). A 4-factor design of experiment was used where the selected variable parameters were the plasma [...] Read more.
The work is focused on the study of surface plasma treatment (DCSBD) of films from biodegradable polymers from renewable sources based on polylactic acid (PLA) and polyhydroxybutyrate (PHB). A 4-factor design of experiment was used where the selected variable parameters were the plasma device power, the time of plasma treatment, the ratio of PHB in the polymer blend with PLA, and the content of acetyl tributyl citrate (ATBC) plasticizer in the PLA + PHB blend. The surface total energy and the polar component were evaluated immediately after surface plasma treatment and after 5 h of sitting. Topography of foil surfaces was also studied by AFM. In terms of plasma power and activation time, the greatest increase in surface energy values was observed with a short plasma time of 2 s and a high power of 400 W. Increasing the content of ATBC in interaction with the high concentration of PHB in the blend results in a reduction in the difference of both the polar component and the total free surface energy. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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17 pages, 3509 KiB  
Article
Rheological and Structural Study of Salmon Gelatin with Controlled Molecular Weight
by Javier Enrione, Cielo Char, Marzena Pepczynska, Cristina Padilla, Adrian González-Muñoz, Yusser Olguín, Claudia Quinzio, Laura Iturriaga and Paulo Díaz-Calderón
Polymers 2020, 12(7), 1587; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071587 - 17 Jul 2020
Cited by 24 | Viewed by 3098
Abstract
This study explores the molecular structuring of salmon gelatin (SG) with controlled molecular weight produced from salmon skin, and its relationship with its thermal and rheological properties. SG was produced under different pH conditions to produce samples with well-defined high (SGH), medium (SGM), [...] Read more.
This study explores the molecular structuring of salmon gelatin (SG) with controlled molecular weight produced from salmon skin, and its relationship with its thermal and rheological properties. SG was produced under different pH conditions to produce samples with well-defined high (SGH), medium (SGM), and low (SGL) molecular weight. These samples were characterized in terms of their molecular weight (MW, capillary viscometry), molecular weight distribution (electrophoresis), amino acid profile, and Raman spectroscopy. These results were correlated with thermal (gelation energy) and rheological properties. SGH presented the higher MW (173 kDa) whereas SGL showed shorter gelatin polymer chains (MW < 65 kDa). Raman spectra and gelation energy suggest that amount of helical structures in gelatin is dependent on the molecular weight, which was well reflected by the higher viscosity and G′ values for SGH. Interestingly, for all the molecular weight and molecular configuration tested, SG behaved as a strong gel (tan δ < 1), despite its low viscosity and low gelation temperature (3–10 °C). Hence, the molecular structuring of SG reflected directly on the thermal and viscosity properties, but not in terms of the viscoelastic strength of gelatin produced. These results give new insights about the relationship among structural features and macromolecular properties (thermal and rheological), which is relevant to design a low viscosity biomaterial with tailored properties for specific applications. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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27 pages, 3233 KiB  
Article
Innovative Skin Product Emulsions with Enhanced Antioxidant, Antimicrobial and UV Protection Properties Containing Nanoparticles of Pure and Modified Chitosan with Encapsulated Fresh Pomegranate Juice
by Nikolaos D. Bikiaris, Georgia Michailidou, Maria Lazaridou, Evi Christodoulou, Eleni Gounari, Anna Ofrydopoulou, Dimitra A. Lambropoulou, Souzan Vergkizi-Nikolakaki, Smaro Lykidou and Nikolaos Nikolaidis
Polymers 2020, 12(7), 1542; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071542 - 12 Jul 2020
Cited by 19 | Viewed by 3999
Abstract
In the present study, a chitosan (CS) derivative with the 2-(Methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl)ammonium hydroxide (SDAEM) zwitterionic monomer was prepared through chemical modification. The successful synthesis of CS-SDAEM was confirmed by Fourier-transform Infrared (FTIR) and Nuclear Magnetic Resonance (1H-NMR) spectroscopies. Its crystallinity was studied [...] Read more.
In the present study, a chitosan (CS) derivative with the 2-(Methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl)ammonium hydroxide (SDAEM) zwitterionic monomer was prepared through chemical modification. The successful synthesis of CS-SDAEM was confirmed by Fourier-transform Infrared (FTIR) and Nuclear Magnetic Resonance (1H-NMR) spectroscopies. Its crystallinity was studied by X-ray Diffraction (XRD), while in vitro cytotoxicity and cell viability assays established its biocompatibility. Filtered fresh pomegranate juice (PJ) was loaded in nanoparticles of neat CS and its derivative via ionic gelation method. Dynamic Light Scattering (DLS) revealed nanoparticles sizes varying between 426 nm and 4.5 μm, indicating a size-dependence on the polymer concentration used during encapsulation. High-performance liquid chromatography coupled with photodiode array and electrospray ionization mass spectrometry detection (LC-PDA-ESI/MS) revealed that PJ active compounds were successfully and in sufficient amounts encapsulated in the nanoparticles interior, whereas XRD indicated a crystalline structure alteration after nanoencapsulation. The resulted PJ-loaded nanoparticles were further utilized for the preparation of innovative O/W cosmetic emulsions. All produced emulsions exhibited good pH and viscosity stability for up to 90 days, while the sun protection factor (SPF) was enhanced due to the presence of the PJ. Enhanced antioxidant and antimicrobial properties due to the phenolic compounds of PJ were also observed. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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19 pages, 4891 KiB  
Article
Bio-Based Polyamide 1010 with a Halogen-Free Flame Retardant Based on Melamine–Gallic Acid Complex
by Nicoleta Levinta, Mihai Cosmin Corobea, Zina Vuluga, Cristian-Andi Nicolae, Augusta Raluca Gabor, Valentin Raditoiu, Mariana Osiac, George-Mihail Teodorescu and Mircea Teodorescu
Polymers 2020, 12(7), 1482; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071482 - 02 Jul 2020
Cited by 10 | Viewed by 4088
Abstract
This work aims at developing polyamide 1010 (PA1010) composites with improved fire behavior using a halogen-free flame-retardant system based on melamine (Me) and gallic acid (GA) complexes (MA). The MA complexes were formed by hydrogen bonding, starting from 1:2, 1:1, 2:1 Me:GA molar [...] Read more.
This work aims at developing polyamide 1010 (PA1010) composites with improved fire behavior using a halogen-free flame-retardant system based on melamine (Me) and gallic acid (GA) complexes (MA). The MA complexes were formed by hydrogen bonding, starting from 1:2, 1:1, 2:1 Me:GA molar ratios. PA1010 composites were obtained by melt mixing, followed by compression molding. MA provided a plasticizing effect on the PA1010 matrix by decreasing the glass transition temperature. The influence of MA on PA1010 chain packaging was highlighted in the X-ray diffraction patterns, mainly in the amorphous phase, but affected also the α and γ planes. This was reflected in the dynamic mechanical properties by the reduction of the storage modulus. H-bonds occurrence in MA complexes, improved the efficiency in the gaseous form during fire exposure, facilitating the gas formation and finally reflected in thermal stability, thermo-oxidative stability, LOI results, and vertical burning behavior results. PA1010 containing a higher amount of GA in the complex (MA12) displayed a limiting oxygen index (LOI) value of 33.6%, much higher when compared to neat PA1010 (25.8%). Vertical burning tests showed that all the composites can achieve the V-0 rating in contrast with neat PA1010 that has V-2 classification. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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22 pages, 5788 KiB  
Article
Bio-Based Poly(butylene succinate)/Microcrystalline Cellulose/Nanofibrillated Cellulose-Based Sustainable Polymer Composites: Thermo-Mechanical and Biodegradation Studies
by Oskars Platnieks, Sergejs Gaidukovs, Anda Barkane, Aleksandrs Sereda, Gerda Gaidukova, Liga Grase, Vijay Kumar Thakur, Inese Filipova, Velta Fridrihsone, Marite Skute and Marianna Laka
Polymers 2020, 12(7), 1472; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071472 - 30 Jun 2020
Cited by 55 | Viewed by 7919
Abstract
Biodegradable polymer composites from renewable resources are the next-generation of wood-like materials and are crucial for the development of various industries to meet sustainability goals. Functional applications like packaging, medicine, automotive, construction and sustainable housing are just some that would greatly benefit. Some [...] Read more.
Biodegradable polymer composites from renewable resources are the next-generation of wood-like materials and are crucial for the development of various industries to meet sustainability goals. Functional applications like packaging, medicine, automotive, construction and sustainable housing are just some that would greatly benefit. Some of the existing industries, like wood plastic composites, already encompass given examples but are dominated by fossil-based polymers that are unsustainable. Thus, there is a background to bring a new perspective approach for the combination of microcrystalline cellulose (MCC) and nanofibrillated cellulose (NFC) fillers in bio-based poly (butylene succinate) matrix (PBS). MCC, NFC and MCC/NFC filler total loading at 40 wt % was used to obtain more insights for wood-like composite applications. The ability to tailor the biodegradable characteristics and the mechanical properties of PBS composites is indispensable for extended applications. Five compositions have been prepared with MCC and NFC fillers using melt blending approach. Young’s modulus in tensile test mode and storage modulus at 20 °C in thermo-mechanical analysis have increased about two-fold. Thermal degradation temperature was increased by approximately 60 °C compared to MCC and NFC. Additionally, to estimate the compatibility of the components and morphology of the composite’s SEM analysis was performed for fractured surfaces. The contact angle measurements testified the developed matrix interphase. Differential scanning calorimetry evidenced the trans-crystallization of the polymer after filler incorporation; the crystallization temperature shifted to the higher temperature region. The MCC has a stronger effect on the crystallinity degree than NFC filler. PBS disintegrated under composting conditions in a period of 75 days. The NFC/MCC addition facilitated the specimens’ decomposition rate up to 60 days Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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13 pages, 1919 KiB  
Article
Synthesis, Characterization, Self-Assembly, and Irritation Studies of Polyglyceryl-10 Caprylates
by Guangyan Zhang, Chenhui Bao, Kaiqiao Fu, Yaolin Lin, Tianlong Li and Huping Yang
Polymers 2020, 12(2), 294; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12020294 - 02 Feb 2020
Cited by 1 | Viewed by 4634
Abstract
1,4-dioxane should be less than or equal to 10 ppm in finished cosmetic products according to the recommendation of the Scientific Committee on Consumer Safety, but it is often generated as a by-product during the manufacturing process of poly(ethylene glycol) (PEG)-based derivatives. In [...] Read more.
1,4-dioxane should be less than or equal to 10 ppm in finished cosmetic products according to the recommendation of the Scientific Committee on Consumer Safety, but it is often generated as a by-product during the manufacturing process of poly(ethylene glycol) (PEG)-based derivatives. In order to avoid the possible risk caused by 1,4-dioxane, it might be a good choice for preparing cosmetic ingredients by using polyglycerin (PG) instead of PEG as a hydrophilic segment. In the present study, polyglyceryl-10 caprylates were synthesized by the esterification reaction between polyglycerin-10 and caprylic acid. FTIR and 1H NMR were utilized to confirm the chemical structures of the obtained polyglyceryl-10 caprylates. Light transmittance was availed to investigate the water solubility of polyglyceryl-10 caprylates. The self-assembly behavior, size, and size distribution of polyglyceryl-10 caprylates were investigated by dynamic light scattering. The makeup cleansing effect was also evaluated by in vitro and in vivo methods. Irritation was evaluated by hen’s egg test-chorioallantoic membrane assay (HET-CAM). Results showed that polyglyceryl-10 monocaprylate could self-assemble into nanoparticles in the water at the concentration range of 2.5–10 wt% with a transparent appearance. The diameter of formed nanoparticles was around 100 nm with a narrow particle size distribution around 0.1 at the concentration of 2.5 wt% or 5 wt%. Polyglyceryl-10 monocaprylate exhibited good removal effect against makeup and excellent removal efficacy against pen eyeliner. The irritation of polyglyceryl-10 monocaprylate evaluated by HET-CAM at the concentration of 4 wt% was moderate irritant (irritation score = 8.4), which was lower than that of PEG-6 caprylic/capric glycerides (severe irritant, irritation score = 14.1). Therefore, polyglyceryl-10 monocaprylate might be a promising cosmetic ingredient for transparent makeup removing water. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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21 pages, 5948 KiB  
Article
Sustainable Plastics from Biomass: Blends of Polyesters Based on 2,5-Furandicarboxylic Acid
by Niki Poulopoulou, Dimitra Smyrnioti, George N. Nikolaidis, Ilektra Tsitsimaka, Evi Christodoulou, Dimitrios N. Bikiaris, Maria Anna Charitopoulou, Dimitris S. Achilias, Maria Kapnisti and George Z. Papageorgiou
Polymers 2020, 12(1), 225; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12010225 - 16 Jan 2020
Cited by 34 | Viewed by 6037
Abstract
Intending to expand the thermo-physical properties of bio-based polymers, furan-based thermoplastic polyesters were synthesized following the melt polycondensation method. The resulting polymers, namely, poly(ethylene 2,5-furandicarboxylate) (PEF), poly(propylene 2,5-furandicarboxylate) (PPF), poly(butylene 2,5-furandicarboxylate) (PBF) and poly(1,4-cyclohexanedimethylene 2,5-furandicarboxylate) (PCHDMF) are used in blends together with various [...] Read more.
Intending to expand the thermo-physical properties of bio-based polymers, furan-based thermoplastic polyesters were synthesized following the melt polycondensation method. The resulting polymers, namely, poly(ethylene 2,5-furandicarboxylate) (PEF), poly(propylene 2,5-furandicarboxylate) (PPF), poly(butylene 2,5-furandicarboxylate) (PBF) and poly(1,4-cyclohexanedimethylene 2,5-furandicarboxylate) (PCHDMF) are used in blends together with various polymers of industrial importance, including poly(ethylene terephthalate) (PET), poly(ethylene 2,6-naphthalate) (PEN), poly(L-lactic acid) (PLA) and polycarbonate (PC). The blends are studied concerning their miscibility, crystallization and solid-state characteristics by using wide-angle X-ray diffractometry (WAXD), differential scanning calorimetry (DSC) and polarized light microscopy (PLM). PEF blends show in general dual glass transitions in the DSC heating traces for the melt quenched samples. Only PPF–PEF blends show a single glass transition and a single melt phase in PLM. PPF forms immiscible blends except with PEF and PBF. PBF forms miscible blends with PCHDMF and PPF, whereas all other blends show dual glass transitions in DSC and phase separation in PLM. PCHDMF–PEF and PEN–PEF blends show two glass transition temperatures, but they shift to intermediate temperature values depending on the composition, indicating some partial miscibility of the polymer pairs. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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13 pages, 3101 KiB  
Article
Effect of Gellan Gum and Xanthan Gum Synergistic Interactions and Plasticizers on Physical Properties of Plant-Based Enteric Polymer Films
by Na Zhang, Xiaohui Li, Jing Ye, Yucheng Yang, Yayan Huang, Xueqin Zhang and Meitian Xiao
Polymers 2020, 12(1), 121; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12010121 - 05 Jan 2020
Cited by 26 | Viewed by 5179
Abstract
The mechanical and barrier properties of plant-based enteric polymer films were enhanced by synergistic interactions between binary gum mixtures and adding plasticizers. The results indicated that the best ratio of gellan gum (GG) and xanthan gum (XG) was 7:3 by comparing tensile strength, [...] Read more.
The mechanical and barrier properties of plant-based enteric polymer films were enhanced by synergistic interactions between binary gum mixtures and adding plasticizers. The results indicated that the best ratio of gellan gum (GG) and xanthan gum (XG) was 7:3 by comparing tensile strength, tensile elongation, transmittance, and water vapor permeability of plant-based enteric polymer films and rheological properties of solutions. Polyethylene glycol 400 (PEG-400) was an effective plasticizer in improving plasticity and water vapor barrier property of the plant-based enteric polymer film. Rheology measurement and different characterization methods, including Fourier transform infrared spectroscopy, thermogravimetric analysis, differential scanning calorimetry, X-ray diffraction, and scanning electron microscopy, were used to explain interactions between GG and XG as well as PEG-400 and components of the film. The new mixed system, composed of GG/XG mixture with ratio of 7:3 as a novel gelling agent and PEG-400 as a plasticizer, was applied to prepare plant-based enteric hard capsules, which have potential applications in medicines and functional food preparations. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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16 pages, 2525 KiB  
Article
Thermal Analysis of Aliphatic Polyester Blends with Natural Antioxidants
by Olga Olejnik, Anna Masek and Adam Kiersnowski
Polymers 2020, 12(1), 74; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12010074 - 02 Jan 2020
Cited by 16 | Viewed by 5413
Abstract
The aim of this research was to enhance thermal stability of aliphatic polyester blends via incorporation of selected natural antioxidants of plant origin. Thermal methods of analysis, including differential scanning calorimetry (DSC) and thermogravimetry (TGA), are significant tools for estimating the stabilization effect [...] Read more.
The aim of this research was to enhance thermal stability of aliphatic polyester blends via incorporation of selected natural antioxidants of plant origin. Thermal methods of analysis, including differential scanning calorimetry (DSC) and thermogravimetry (TGA), are significant tools for estimating the stabilization effect of polyphenols in a polymer matrix. Thermal stability was determined by analyzing thermogravimetric curves. Polymers with selected antioxidants degraded more slowly with rising temperature in comparison to reference samples without additives. This property was also confirmed by results obtained from differential scanning calorimetry (DSC), where the difference between the oxidation temperatures of pure material and polymer with natural stabilizers was observed. According to the results, the materials with selected antioxidants, including trans-chalcone, flavone and lignin have higher oxidation temperature than the pure ones, which confirms that chosen phytochemicals protect polymers from oxidation. Moreover, based on the colour change results or FT-IR spectra analysis, some of the selected antioxidants, including lignin and trans-chalcone, can be utilized as colorants or aging indicators. Taking into account the data obtained, naturally occurring antioxidants, including polyphenols, can be applied as versatile pro-ecological additives for biodegradable and bio-based aliphatic polyesters to obtain fully environmentally friendly materials dedicated for packaging industry. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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23 pages, 4176 KiB  
Article
Assessment of Photodegradation and Biodegradation of RPU/PIR Foams Modified by Natural Compounds of Plant Origin
by Joanna Liszkowska, Marcin Borowicz, Joanna Paciorek-Sadowska, Marek Isbrandt, Bogusław Czupryński and Krzysztof Moraczewski
Polymers 2020, 12(1), 33; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12010033 - 24 Dec 2019
Cited by 24 | Viewed by 3812
Abstract
Four types of rigid polyurethane-polyisocyanurate foams (RPU/PIR) were obtained. Three of them were modified by powder fillers, such as cinnamon extract (C10 foam), green coffe extract (KZ10), and cocoa extract (EK10) in an amount of 10 wt %. The last foam was obtained [...] Read more.
Four types of rigid polyurethane-polyisocyanurate foams (RPU/PIR) were obtained. Three of them were modified by powder fillers, such as cinnamon extract (C10 foam), green coffe extract (KZ10), and cocoa extract (EK10) in an amount of 10 wt %. The last foam was obtained without a filler (W foam). The basic properties and thermal properties of obtained foams were examined. All foams were subjected to degradation in the climatic chamber acting on samples of foams in a defined temperature, humidity, and UV radiation for 7, 14, and 21 days. The physico-mechanical properties of foams were tested. The compressive strength of degraded foams after 7, 14, and 21 days was compared with the compressive strength of nondegraded foams (0 days). The chosen properties of degraded foams, such as cellular structure by scanning electron microscopy (SEM) and changes of chemical structure by FTIR spectroscopy were compared. The obtained foams were also subjected to degradation in a circulating air dryer in an increased temperature (120 °C) for 48 h. Additionally, W, C10, ZK10, EK10 foams were placed in a soil environment and subjected to 28 days biodegradation process. The biochemical oxygen demand (BOD), the theoretical oxygen demand (TOD), and the degree of biodegradation (Dt) of foams were determined in this measurment. Test results showed that the compressive strength of foams decreased with the longer time of foam degradation in the conditioner. The foam subjected to degradation darkened and became more red and yellow in color. The addition of natural compounds of plant origin to foams increased their susceptibility to biodegradation. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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16 pages, 5046 KiB  
Article
Properties of Luffa Fiber Reinforced PHBV Biodegradable Composites
by Yong Guo, Li Wang, Yuxia Chen, Panpan Luo and Tong Chen
Polymers 2019, 11(11), 1765; https://0-doi-org.brum.beds.ac.uk/10.3390/polym11111765 - 27 Oct 2019
Cited by 24 | Viewed by 4845
Abstract
In this study, composites of poly (hydroxybutyrate-co-valerate) (PHBV) with untreated luffa fibers (ULF) and NaOH-H2O2 treated luffa fibers (TLF) were prepared by hot press forming. The properties of luffa fibers (LFs) and composites were characterized by scanning electron microscopy (SEM), [...] Read more.
In this study, composites of poly (hydroxybutyrate-co-valerate) (PHBV) with untreated luffa fibers (ULF) and NaOH-H2O2 treated luffa fibers (TLF) were prepared by hot press forming. The properties of luffa fibers (LFs) and composites were characterized by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), and other analysis methods. Results showed that pre-treatment effectively removed pectin, hemicellulose, and lignin, thus reducing the moisture absorptivity of LFs. The flexural strength of TLF/PHBV was higher than that of ULF/PHBV. With 60% LF content, the flexural strengths of ULF/PHBV and TLF/PHBV reached 75.23 MPa and 90.73 MPa, respectively, 219.7% and 285.6% more than that of pure PHBV. Water absorptivities of composites increased with increase in LF content. Water absorptivity of TLF/PHBV was lower than that of ULF/PHBV. The flexural strengths of composites decreased after immersion in water at room temperature. Meanwhile, flexural strength of TLF/PHBV was lower than that of ULF/PHBV. Pretreatment of LFs effectively improved the bonding between fibers and PHBV, resulting in enhanced and thus improved the moisture resistance of composites. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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19 pages, 5645 KiB  
Article
Composting of Polylactide Containing Natural Anti-Aging Compounds of Plant Origin
by Krzysztof Moraczewski, Rafał Malinowski, Wanda Sikorska, Tomasz Karasiewicz, Magdalena Stepczyńska, Bartłomiej Jagodziński and Piotr Rytlewski
Polymers 2019, 11(10), 1582; https://0-doi-org.brum.beds.ac.uk/10.3390/polym11101582 - 27 Sep 2019
Cited by 9 | Viewed by 2772
Abstract
The paper presents the effects of biodegradation of polylactide containing natural anti-aging compounds. Polymer containing 0.5; 5 and 10 wt % of coffee, cocoa or cinnamon extracts were subjected to industrial composting for 7, 14, 21 or 28 days. The effect of the [...] Read more.
The paper presents the effects of biodegradation of polylactide containing natural anti-aging compounds. Polymer containing 0.5; 5 and 10 wt % of coffee, cocoa or cinnamon extracts were subjected to industrial composting for 7, 14, 21 or 28 days. The effect of the composting process on polylactide properties was examined based on visual assessment, scanning electron microscopy, average molecular weight, differential scanning calorimetry, thermogravimetry, and tensile strength. The impact of the tested extracts on the effects of the composting process was compared with the impact of a commercially available anti-aging compound. It was found that the tested extracts in most cases did not adversely affect the effects of the composting process compared to pure polylactide, often resulting in intensification of biodegradation processes. As a result of the composting process, changes in the macro- and microscopic appearance of the samples and a decrease in molecular weight, phase transition temperatures, thermal resistance, and thermal strength were observed on a scale close to or greater than the reference anti-aging compound. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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Review

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67 pages, 16635 KiB  
Review
Chitosan and its Derivatives for Ocular Delivery Formulations: Recent Advances and Developments
by Alexandra Zamboulis, Stavroula Nanaki, Georgia Michailidou, Ioanna Koumentakou, Maria Lazaridou, Nina Maria Ainali, Eleftheria Xanthopoulou and Dimitrios N. Bikiaris
Polymers 2020, 12(7), 1519; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12071519 - 08 Jul 2020
Cited by 91 | Viewed by 8188
Abstract
Chitosan (CS) is a hemi-synthetic cationic linear polysaccharide produced by the deacetylation of chitin. CS is non-toxic, highly biocompatible, and biodegradable, and it has a low immunogenicity. Additionally, CS has inherent antibacterial properties and a mucoadhesive character and can disrupt epithelial tight junctions, [...] Read more.
Chitosan (CS) is a hemi-synthetic cationic linear polysaccharide produced by the deacetylation of chitin. CS is non-toxic, highly biocompatible, and biodegradable, and it has a low immunogenicity. Additionally, CS has inherent antibacterial properties and a mucoadhesive character and can disrupt epithelial tight junctions, thus acting as a permeability enhancer. As such, CS and its derivatives are well-suited for the challenging field of ocular drug delivery. In the present review article, we will discuss the properties of CS that contribute to its successful application in ocular delivery before reviewing the latest advances in the use of CS for the development of novel ophthalmic delivery systems. Colloidal nanocarriers (nanoparticles, micelles, liposomes) will be presented, followed by CS gels and lenses and ocular inserts. Finally, instances of CS coatings, aiming at conferring mucoadhesiveness to other matrixes, will be presented. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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51 pages, 36084 KiB  
Review
Tuning the Properties of Furandicarboxylic Acid-Based Polyesters with Copolymerization: A Review
by Zoi Terzopoulou, Lazaros Papadopoulos, Alexandra Zamboulis, Dimitrios G. Papageorgiou, George Z. Papageorgiou and Dimitrios N. Bikiaris
Polymers 2020, 12(6), 1209; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12061209 - 26 May 2020
Cited by 100 | Viewed by 9844
Abstract
Polyesters based on 2,5-furandicarboxylic acid (FDCA) are a new class of biobased polymers with enormous interest, both from a scientific and industrial perspective. The commercialization of these polymers is imminent as the pressure for a sustainable economy grows, and extensive worldwide research currently [...] Read more.
Polyesters based on 2,5-furandicarboxylic acid (FDCA) are a new class of biobased polymers with enormous interest, both from a scientific and industrial perspective. The commercialization of these polymers is imminent as the pressure for a sustainable economy grows, and extensive worldwide research currently takes place on developing cost-competitive, renewable plastics. The most prevalent method for imparting these polymers with new properties is copolymerization, as many studies have been published over the last few years. This present review aims to summarize the trends in the synthesis of FDCA-based copolymers and to investigate the effectiveness of this approach in transforming them to a more versatile class of materials that could potentially be appropriate for a number of high-end and conventional applications. Full article
(This article belongs to the Special Issue Biobased and Biodegradable Polymers)
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