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Recent Developments in Biodegradable and Biobased Polymers II

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

Deadline for manuscript submissions: closed (20 August 2024) | Viewed by 10827

Special Issue Editor


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Guest Editor
Department of Biobased Materials Science, Kyoto Institute of Technology, Kyoto 606-8585, Japan
Interests: nanostructure analysis; small-angle X-ray scattering; block copolymer; polymer physics; polymer crystallization; pattern formation
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Special Issue Information

Dear Colleagues,

Biodegradable polymers are considered promising materials to solve the problem of microplastic pollution in marine environments. In addition, biobased polymers utilizing plants can be used to reduce the concentration of carbon dioxide in the atmosphere and can contribute to carbon neutralization. However, these polymers have some crucial drawbacks such as poor crystallizability and insufficient mechanical properties, compared to commodity polymers synthesized using monomers from fossil fuels.  Therefore, many research studies have been devoted to improving their crystallizability and mechanical properties. For crystallizability, the addition of a nucleation agent, diluent, or plasticizer has been reported. To ameliorate the mechanical properties, block copolymerization and polymer blending are main strategies, but it is important to use additives derived from natural sources and components of block copolymers or polymer blends that are biobased and/or biodegradable. In this context, new biobased monomers and synthetic routes of biobased polymers from such biobased monomers should be investigated. The biodegradable behaviors of such new biobased polymers should also be examined.  This Special Issue focuses on these topics, including biomedical applications and recent developments in biodegradable and biobased polymers.

Prof. Dr. Shinichi Sakurai
Guest Editor

Manuscript Submission Information

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Keywords

  • biobased monomer
  • synthesis
  • biodegradable behavior
  • mechanical property
  • crystallization
  • biobased additives
  • block copolymerization
  • polymer blending
  • biomedical application

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Related Special Issue

Published Papers (7 papers)

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Research

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20 pages, 3049 KiB  
Article
Coassembly of a Hybrid Synthetic–Biological Chitosan-g-Poly(N-isopropylacrylamide) Copolymer with DNAs of Different Lengths
by Maria Karayianni, Elena-Daniela Lotos, Marcela Mihai and Stergios Pispas
Polymers 2024, 16(21), 3101; https://doi.org/10.3390/polym16213101 - 4 Nov 2024
Viewed by 686
Abstract
Natural polysaccharides can serve as carriers of genes owing to their intrinsic biocompatibility, biodegradability, and low toxicity. Additionally, they can be easily chemically modified, e.g., through grafting, leading to hybrid synthetic–biological copolymers with additional functionalities. In this work we report on the electrostatic [...] Read more.
Natural polysaccharides can serve as carriers of genes owing to their intrinsic biocompatibility, biodegradability, and low toxicity. Additionally, they can be easily chemically modified, e.g., through grafting, leading to hybrid synthetic–biological copolymers with additional functionalities. In this work we report on the electrostatic interaction between a chitosan-g-poly(N-isopropylacrylamide) (Chit-g-PNIPAM) copolymer and DNA macromolecules of different lengths (i.e., 50 and 2000 bp), towards the construction of polyplexes that can serve as potential gene delivery systems. At the basic science level, the work aims to elucidate the effects of DNA length on the structural and physicochemical properties of the thermoresponsive hybrid macromolecular assemblies. The protonated amino groups on the chitosan backbone enable electrostatic binding with the anionic phosphate groups of the DNA molecules, while the PNIPAM side chains are expected to impart thermoresponsive properties to the formed polyplexes. Different amino to phosphate group (N/P) mixing ratios were examined, aiming to produce stable dispersions. The physicochemical properties of the resulting polyplexes were investigated by dynamic and electrophoretic light scattering (DLS and ELS), while their morphology was studied by scanning-transmission electron microscopy (STEM). Moreover, their response to changes in temperature and ionic strength, as well as their stability against biological media, was also examined. Finally, the binding affinity of the copolymer towards DNA was evaluated through fluorescence spectroscopy, using ethidium bromide quenching assays, while infrared spectroscopy was used to investigate the structure of the incorporated DNA chains. Full article
(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers II)
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15 pages, 2799 KiB  
Article
Bio-Epoxy Resins Based on Lignin and Tannic Acids as Wood Adhesives—Characterization and Bonding Properties
by Ivana Gavrilović-Grmuša, Milica Rančić, Tamara Tešić, Stevan Stupar, Milena Milošević and Jelena Gržetić
Polymers 2024, 16(18), 2602; https://doi.org/10.3390/polym16182602 - 14 Sep 2024
Viewed by 1038
Abstract
The possibility of producing and designing bio-epoxides based on the natural polyphenol lignin/epoxidized lignin and tannic acids for application as wood adhesives is presented in this work. Lignin and tannic acids contain numerous reactive hydroxyl phenolic moieties capable of being efficiently involved in [...] Read more.
The possibility of producing and designing bio-epoxides based on the natural polyphenol lignin/epoxidized lignin and tannic acids for application as wood adhesives is presented in this work. Lignin and tannic acids contain numerous reactive hydroxyl phenolic moieties capable of being efficiently involved in the reaction with commercial epoxy resins as a substitute for commercial, non-environmentally friendly, toxic amine-based hardeners. Furthermore, lignin was epoxidized in order to obtain an epoxy lignin that can be a replacement for diglycidyl ether bisphenol A (DGEBA). Cross-linking of bio-epoxy epoxides was investigated via FTIR spectroscopy and their prospects for wood adhesive application were evaluated. This study determined that the curing reaction of epoxy resin can be conducted using lignin/epoxy lignin or tannic acid. Tensile shear strength testing results showed that lignin and tannic acid can effectively replace amine hardeners in epoxy resins. Examination of the failure of the samples showed that all samples had a 100% fracture through the wood. All samples of bio-epoxy adhesives displayed significant tensile shear strength in the range of 5.84–10.87 MPa. This study presents an innovative approach to creating novel cross-linked networks of eco-friendly and high-performance wood bio-adhesives. Full article
(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers II)
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15 pages, 2821 KiB  
Article
Plant-Based Films for Food Packaging as a Plastic Waste Management Alternative: Potato and Cassava Starch Case
by Luna Valentina Angulo Arias, Viviane de Souza Silva, Jorge Miguel Magalhães Vieira, Farayde Matta Fakhouri and Rafael Augustus de Oliveira
Polymers 2024, 16(17), 2390; https://doi.org/10.3390/polym16172390 - 23 Aug 2024
Viewed by 1245
Abstract
The escalating environmental impact of plastic packaging waste necessitates sustainable alternatives in food packaging. This study explores starch-based films derived from cassava and potato as viable substitutes, aiming to mitigate plastic pollution and enhance environmental sustainability. Utilizing a casting method, formulations optimized by [...] Read more.
The escalating environmental impact of plastic packaging waste necessitates sustainable alternatives in food packaging. This study explores starch-based films derived from cassava and potato as viable substitutes, aiming to mitigate plastic pollution and enhance environmental sustainability. Utilizing a casting method, formulations optimized by CCRD were characterized for their physical, physicochemical, and morphological properties. Comprehensive analysis revealed both cassava and potato starch films to exhibit robust structural integrity, high tensile strength (up to 32.6 MPa for cassava starch films), and semi-crystalline morphology. These films demonstrated low water vapor permeability and moderate solubility, akin to conventional low-density polyethylene used in packaging. Differential scanning calorimetry indicated glass transition temperatures between 116.36 °C and 119.35 °C, affirming thermal stability suitable for packaging applications. Scanning electron microscopy confirmed homogeneous film surfaces, with cassava starch films (C4-15) exhibiting superior transparency and uniformity. X-ray diffraction corroborated the films’ semi-crystalline nature, unaffected by sorbitol content variations. Despite their mechanical and thermal suitability, further enhancements in thermal degradation resistance are essential for broader thermoprocessing applicability. These findings underscore the potential of starch-based films to be used as lids or other part of a food package, decreasing the plastic dependency in food packaging, contributing decisively to waste reduction and environmental preservation. Full article
(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers II)
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14 pages, 3027 KiB  
Article
Changes in the Chemical Composition of Polyethylene Terephthalate under UV Radiation in Various Environmental Conditions
by Sara Rostampour, Rachel Cook, Song-Syun Jhang, Yuejin Li, Chunlei Fan and Li-Piin Sung
Polymers 2024, 16(16), 2249; https://doi.org/10.3390/polym16162249 - 8 Aug 2024
Viewed by 2658
Abstract
Polyethylene terephthalate has been widely used in the packaging industry. Degraded PET micro(nano)plastics could pose public health concerns following release into various environments. This study focuses on PET degradation under ultraviolet radiation using the NIST SPHERE facility at the National Institute of Standards [...] Read more.
Polyethylene terephthalate has been widely used in the packaging industry. Degraded PET micro(nano)plastics could pose public health concerns following release into various environments. This study focuses on PET degradation under ultraviolet radiation using the NIST SPHERE facility at the National Institute of Standards and Technology in saturated humidity (i.e., ≥95% relative humidity) and dry conditions (i.e., ≤5% relative humidity) with varying temperatures (30 °C, 40 °C, and 50 °C) for up 20 days. ATR-FTIR was used to characterize the chemical composition change of degraded PET as a function of UV exposure time. The results showed that the cleavage of the ester bond at peak 1713 cm−1 and the formation of the carboxylic acid at peak 1685 cm−1 were significantly influenced by UV radiation. Furthermore, the formation of carboxylic acid was considerably higher at saturated humidity and 50 °C conditions compared with dry conditions. The ester bond cleavage was also more pronounced in saturated humidity conditions. The novelty of this study is to provide insights into the chemical degradation of PET under environmental conditions, including UV radiation, humidity, and temperature. The results can be used to develop strategies to reduce the environmental impact of plastic pollution. Full article
(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers II)
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12 pages, 2668 KiB  
Article
Terephthalate Copolyesters Based on 2,3-Butanediol and Ethylene Glycol and Their Properties
by Marian Blom, Robert-Jan van Putten, Kevin van der Maas, Bing Wang, Gerard P. M. van Klink and Gert-Jan M. Gruter
Polymers 2024, 16(15), 2177; https://doi.org/10.3390/polym16152177 - 30 Jul 2024
Viewed by 1308
Abstract
This study explores the synthesis and performance of novel copolyesters containing 2,3-butanediol (2,3-BDO) as a biobased secondary diol. This presents an opportunity for improving their thermal properties and reducing crystallinity, while also being more sustainable. It is, however, a challenge to synthesize copolyesters [...] Read more.
This study explores the synthesis and performance of novel copolyesters containing 2,3-butanediol (2,3-BDO) as a biobased secondary diol. This presents an opportunity for improving their thermal properties and reducing crystallinity, while also being more sustainable. It is, however, a challenge to synthesize copolyesters of sufficient molecular weight that also have high 2,3-BDO content, due to the reduced reactivity of secondary diols compared to primary diols. Terephthalate-based polyesters were synthesized in combination with different ratios of 2,3-BDO and ethylene glycol (EG). With a 2,3-BDO to EG ratio of 28:72, an Mn of 31.5 kDa was reached with a Tg of 88 °C. The Mn dropped with increasing 2,3-BDO content to 18.1 kDa for a 2,3-BDO to EG ratio of 78:22 (Tg = 104 °C) and further to 9.8 kDa (Tg = 104 °C) for the homopolyester of 2,3-BDO and terephthalate. The water and oxygen permeability both increased significantly with increasing 2,3-BDO content and even the lowest content of 2,3-BDO (28% of total diol) performed significantly worse than PET. The incorporation of 2,3-BDO had little effect on the tensile properties of the polyesters, which were similar to PET. The results suggest that 2,3-BDO can be potentially applied for polyesters requiring higher Tg and lower crystallinity than existing materials (mainly PET). Full article
(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers II)
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17 pages, 3313 KiB  
Article
A Comparison of Laboratory and Industrial Processes Reveals the Effect of Dwell Time and UV Pre-Exposure on the Behavior of Two Polymers in a Disintegration Trial
by Simon Schick, Robert Groten, Andreas Weinberger and Gunnar H. Seide
Polymers 2024, 16(12), 1650; https://doi.org/10.3390/polym16121650 - 11 Jun 2024
Cited by 1 | Viewed by 806
Abstract
Biodegradable biopolymers such as polylactic acid and polybutylene succinate are sustainable alternatives to traditional petroleum-based plastics. However, the factors affecting their degradation must be characterized in detail to enable successful utilization. Here we compared the extruder dwell time at three different melt-spinning scales [...] Read more.
Biodegradable biopolymers such as polylactic acid and polybutylene succinate are sustainable alternatives to traditional petroleum-based plastics. However, the factors affecting their degradation must be characterized in detail to enable successful utilization. Here we compared the extruder dwell time at three different melt-spinning scales and its influence on the degradation of both polymers. The melt temperature was the same for all three processes, but the shear stress and dwell time were key differences, with the latter being the easiest to measure. Accelerated degradation tests, including quick weathering and disintegration, were used to evaluate the influence of dwell time on the structural, mechanical, and thermal properties of the resulting fibers. We found that longer dwell times accelerated degradation. Quick weathering by UV pre-exposure before the disintegration trial, however, had a more significant effect than dwell time, indicating that degradation studies with virgin material in a laboratory-scale setting only show the theoretical behavior of a product in the laboratory. A weathered fiber from an industrial-scale spinning line more accurately predicts the behavior of a product placed on the market before ending up in the environment. This highlights the importance of optimizing process parameters such as the dwell time to adapt the degradability of biopolymers for specific applications and environmental requirements. By gaining a deeper insight into the relationship between manufacturing processes and fiber degradability, products can be adapted to meet suitable performance criteria for different applications. Full article
(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers II)
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Review

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24 pages, 5936 KiB  
Review
Advanced Mechanical Testing Technologies at the Cellular Level: The Mechanisms and Application in Tissue Engineering
by Yingxuan Zhu, Mengqi Zhang, Qingqing Sun, Xiaofeng Wang, Xiaomeng Li and Qian Li
Polymers 2023, 15(15), 3255; https://doi.org/10.3390/polym15153255 - 31 Jul 2023
Cited by 3 | Viewed by 2441
Abstract
Mechanics, as a key physical factor which affects cell function and tissue regeneration, is attracting the attention of researchers in the fields of biomaterials, biomechanics, and tissue engineering. The macroscopic mechanical properties of tissue engineering scaffolds have been studied and optimized based on [...] Read more.
Mechanics, as a key physical factor which affects cell function and tissue regeneration, is attracting the attention of researchers in the fields of biomaterials, biomechanics, and tissue engineering. The macroscopic mechanical properties of tissue engineering scaffolds have been studied and optimized based on different applications. However, the mechanical properties of the overall scaffold materials are not enough to reveal the mechanical mechanism of the cell–matrix interaction. Hence, the mechanical detection of cell mechanics and cellular-scale microenvironments has become crucial for unraveling the mechanisms which underly cell activities and which are affected by physical factors. This review mainly focuses on the advanced technologies and applications of cell-scale mechanical detection. It summarizes the techniques used in micromechanical performance analysis, including atomic force microscope (AFM), optical tweezer (OT), magnetic tweezer (MT), and traction force microscope (TFM), and analyzes their testing mechanisms. In addition, the application of mechanical testing techniques to cell mechanics and tissue engineering scaffolds, such as hydrogels and porous scaffolds, is summarized and discussed. Finally, it highlights the challenges and prospects of this field. This review is believed to provide valuable insights into micromechanics in tissue engineering. Full article
(This article belongs to the Special Issue Recent Developments in Biodegradable and Biobased Polymers II)
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