Sustainable Biopolymer-Based Composites: Processing, Characterization, and Application II

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

Deadline for manuscript submissions: 25 April 2025 | Viewed by 6493

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Guest Editor
Department of Engineering for Innovation, University of Salento, Via per Monteroni, 73100 Lecce, Italy
Interests: photopolymerization; coatings; organic–inorganic hybrids; bio-based materials; waste valorization; biopolymers
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Special Issue Information

Dear Colleagues,

In recent years, significant issues related to environmental pollution, health and safety have pushed global research toward finding valid solutions for substituting petroleum-based materials, which would benefit both the environment and people. Biopolymers have gradually become more popular in several application fields in materials science, such as manufacturing, biomedical engineering, the food industry, packaging, cosmetic and pharmaceutical industries, agriculture, the energy sector, green nanotechnology, and recycling. In attracting the interest of the industrial world, more and more institutions have been forced to comply with restrictions for environmental and health protection.

This Special issue invites all of the research community to contribute its expertise, passion and scientific understanding to expand our knowledge of biopolymers and address new challenges. In particular, we aim to propose new biopolymer-based composites materials that are able to reach and improve upon the properties and performance of traditional synthetic materials, thus guaranteeing environmental sustainability.

This Special Issue welcomes innovative studies (articles, reviews, research reports, etc.) related to the development of biopolymer-based composites and that focus on the processing, characterization and application fields of these new materials.

Dr. Raffaella Striani
Guest Editor

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Keywords

  • biopolymers
  • sustainability
  • biocomposites
  • green engineering
  • bio-based materials
  • renewable resources
  • biocompatibility
  • biodegradability
  • eco-friendly materials
  • natural polymers

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Published Papers (5 papers)

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Research

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33 pages, 5542 KiB  
Article
Wastepaper-Based Cuprammonium Rayon Regenerated Using Novel Gaseous–Ammoniation Injection Process
by Sherif S. Hindi
Polymers 2024, 16(17), 2431; https://doi.org/10.3390/polym16172431 - 27 Aug 2024
Viewed by 979
Abstract
Rayon is an extremely valuable cellulosic fiber in the global textile industry. Since cuprammonium rayon is more eco-friendly than other types of rayon fabrics, it was synthesized by regenerating α–cellulose isolated from wastepaper using a novel gaseous-ammoniation injection (GAI) process. This was achieved [...] Read more.
Rayon is an extremely valuable cellulosic fiber in the global textile industry. Since cuprammonium rayon is more eco-friendly than other types of rayon fabrics, it was synthesized by regenerating α–cellulose isolated from wastepaper using a novel gaseous-ammoniation injection (GAI) process. This was achieved by preparing tetra–ammine copper hydroxide (cuoxam solution) via reacting copper sulfate and sodium hydroxide to produce copper hydroxide that was, finally, ammoniated by injecting the gas directly to the reaction vessel instead of using ammonium hydroxide applied by prior art. After that, the air-dried cellulose was chemically generated by dissolving it in a freshly prepared cuoxam solution and, subsequently, was regenerated by extruding it within a hardening bath constituted mainly from citric acid, producing the cuprammonium rayon (c. rayon). The properties of the fibrous, structural (XRD and mechanical), physical, and chemical features were investigated. It was found that the rayon was produced in a high yield (90.3%) with accepted properties. The fibrous properties of the rayon staple length, linear density, and fiber diameter were found to be 44 mm, 235 Tex, and 19.4 µm, respectively. In addition, the mechanical properties determined, namely tensile strength, elongation at break, modulus of elasticity, and breaking tenacity, were found to be 218.3 MPa, 14.3 GPa, 16.1%, and 27.53 cN/Tex, respectively. Based on this finding, and upon injecting the ammonia gas through the α–cellulose saturated and immersed in the Cu (OH)2 to complete producing the cuoxam solvent, we find that theuse of an injection rate of 120 mL/minute to obtain the highest fibers’ tensile strength for the final product of the c. rayon is preferable. Utilization of higher rates will consume more amounts of the ammonia gas without gaining noticeable enhancement in the c. rayon’s mechanical quality. Accordingly, the GAI invention rendered the c. rayon favorable for use in making sustainable semisynthetic floss for either insulation purposes or spun threads for woven and nonwoven textile clothing. Full article
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20 pages, 6644 KiB  
Article
Fabrication of Electrospun Double Layered Biomimetic Collagen–Chitosan Polymeric Membranes with Zinc-Doped Mesoporous Bioactive Glass Additives
by Dilan Altan, Ali Can Özarslan, Cem Özel, Kadriye Tuzlakoğlu, Yesim Muge Sahin and Sevil Yücel
Polymers 2024, 16(14), 2066; https://doi.org/10.3390/polym16142066 - 19 Jul 2024
Viewed by 1215
Abstract
Several therapeutic approaches have been developed to promote bone regeneration, including guided bone regeneration (GBR), where barrier membranes play a crucial role in segregating soft tissue and facilitating bone growth. This study emphasizes the importance of considering specific tissue requirements in the design [...] Read more.
Several therapeutic approaches have been developed to promote bone regeneration, including guided bone regeneration (GBR), where barrier membranes play a crucial role in segregating soft tissue and facilitating bone growth. This study emphasizes the importance of considering specific tissue requirements in the design of materials for tissue regeneration, with a focus on the development of a double-layered membrane to mimic both soft and hard tissues within the context of GBR. The hard tissue-facing layer comprises collagen and zinc-doped bioactive glass to support bone tissue regeneration, while the soft tissue-facing layer combines collagen and chitosan. The electrospinning technique was employed to achieve the production of nanofibers resembling extracellular matrix fibers. The production of nano-sized (~116 nm) bioactive glasses was achieved by microemulsion assisted sol-gel method. The bioactive glass-containing layers developed hydroxyapatite on their surfaces starting from the first week of simulated body fluid (SBF) immersion, demonstrating that the membranes possessed favorable bioactivity properties. Moreover, all membranes exhibited distinct degradation behaviors in various mediums. However, weight loss exceeding 50% was observed in all tested samples after four weeks in both SBF and phosphate-buffered saline (PBS). The double-layered membranes were also subjected to mechanical testing, revealing a tensile strength of approximately 4 MPa. The double-layered membranes containing zinc-doped bioactive glass demonstrated cell viability of over 70% across all tested concentrations (0.2, 0.1, and 0.02 g/mL), confirming the excellent biocompatibility of the membranes. The fabricated polymer bioactive glass composite double-layered membranes are strong candidates with the potential to be utilized in tissue engineering applications. Full article
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14 pages, 5231 KiB  
Article
Thermal Properties’ Enhancement of PLA-Starch-Based Polymer Composite Using Sucrose
by Sri Yustikasari Massijaya, Muhammad Adly Rahandi Lubis, Rossy Choerun Nissa, Yeyen Nurhamiyah, Wida Banar Kusumaningrum, Resti Marlina, Riska Surya Ningrum, Jajang Sutiawan, Iman Hidayat, Sukma Surya Kusumah, Lina Karlinasari and Rudi Hartono
Polymers 2024, 16(8), 1028; https://doi.org/10.3390/polym16081028 - 9 Apr 2024
Cited by 1 | Viewed by 1683
Abstract
Polylactic-acid–starch-based polymer composite (PLA/TPS) has good thermal stability for biocomposites. However, the physical and mechanical properties of PLA/TPS do not meet the standards. It needed additives to enhance its physical and mechanical properties. The aim was to improve the physical and mechanical properties [...] Read more.
Polylactic-acid–starch-based polymer composite (PLA/TPS) has good thermal stability for biocomposites. However, the physical and mechanical properties of PLA/TPS do not meet the standards. It needed additives to enhance its physical and mechanical properties. The aim was to improve the physical and mechanical properties of PLA/thermoplastic starch using sucrose. In addition, this study evaluated the enhancement of thermal properties of PLA/thermoplastic starch using sucrose. This study used sucrose as an additive to enhance the PLA/TPS composite. The addition of sucrose inhibits the degradation of biocomposites. This means that thermal stability increases. The thermal stability increased because the degree of crystallinity increased with the addition of sucrose, which was also proven in the XRD result. The addition of sucrose caused the morphology of the biocomposite to have pores. The FESEM results showed that biocomposites with the addition of sucrose had pores and gaps. These gaps result from low adhesion between polymers, causing a decrease in the mechanical and physical properties of the sample. Based on the FTIR spectra, biocomposite PLA/TPS blends with the addition of sucrose still have many hydroxyl groups that will lead to attracting other molecules or ions, such as oxygen or water. This phenomenon affects the physical and mechanical properties of materials. The physical and mechanical properties increased with sucrose addition. The best composite was prepared using 3% sucrose. This is because sucrose has a crystalline structure that affects the properties of biocomposites. However, the addition of 3% sucrose was not as effective as that of neat PLA. Full article
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16 pages, 6175 KiB  
Article
Mechanically Tough and Conductive Hydrogels Based on Gelatin and Z–Gln–Gly Generated by Microbial Transglutaminase
by Zhiwei Chen, Ruxin Zhang, Shouwei Zhao, Bing Li, Shuo Wang, Wenhui Lu and Deyi Zhu
Polymers 2024, 16(7), 999; https://doi.org/10.3390/polym16070999 - 5 Apr 2024
Viewed by 1431
Abstract
Gelatin-based hydrogels with excellent mechanical properties and conductivities are desirable, but their fabrication is challenging. In this work, an innovative approach for the preparation of gelatin-based conductive hydrogels is presented that improves the mechanical and conductive properties of hydrogels by integrating Z–Gln–Gly into [...] Read more.
Gelatin-based hydrogels with excellent mechanical properties and conductivities are desirable, but their fabrication is challenging. In this work, an innovative approach for the preparation of gelatin-based conductive hydrogels is presented that improves the mechanical and conductive properties of hydrogels by integrating Z–Gln–Gly into gelatin polymers via enzymatic crosslinking. In these hydrogels (Gel–TG–ZQG), dynamic π–π stacking interactions are created by the introduction of carbobenzoxy groups, which can increase the elasticity and toughness of the hydrogel and improve the conductivity sensitivity by forming effective electronic pathways. Moreover, the mechanical properties and conductivity of the obtained hydrogel can be controlled by tuning the molar ratio of Z–Gln–Gly to the primary amino groups in gelatin. The hydrogel with the optimal mechanical properties (Gel–TG–ZQG (0.25)) exhibits a high storage modulus, compressive strength, tensile strength, and elongation at break of 7.8 MPa at 10 °C, 0.15 MPa at 80% strain, 0.343 MPa, and 218.30%, respectively. The obtained Gel–TG–ZQG (0.25) strain sensor exhibits a short response/recovery time (260.37 ms/130.02 ms) and high sensitivity (0.138 kPa−1) in small pressure ranges (0–2.3 kPa). The Gel–TG–ZQG (0.25) hydrogel-based sensors can detect full-range human activities, such as swallowing, fist clenching, knee bending and finger pressing, with high sensitivity and stability, yielding highly reproducible and repeatable sensor responses. Additionally, the Gel–TG–ZQG hydrogels are noncytotoxic. All the results demonstrate that the Gel–TG–ZQG hydrogel has potential as a biosensor for wearable devices and health-monitoring systems. Full article
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Review

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45 pages, 1576 KiB  
Review
Machine Learning-Based Process Optimization in Biopolymer Manufacturing: A Review
by Ivan Malashin, Dmitriy Martysyuk, Vadim Tynchenko, Andrei Gantimurov, Andrey Semikolenov, Vladimir Nelyub and Aleksei Borodulin
Polymers 2024, 16(23), 3368; https://doi.org/10.3390/polym16233368 - 29 Nov 2024
Viewed by 497
Abstract
The integration of machine learning (ML) into material manufacturing has driven advancements in optimizing biopolymer production processes. ML techniques, applied across various stages of biopolymer production, enable the analysis of complex data generated throughout production, identifying patterns and insights not easily observed through [...] Read more.
The integration of machine learning (ML) into material manufacturing has driven advancements in optimizing biopolymer production processes. ML techniques, applied across various stages of biopolymer production, enable the analysis of complex data generated throughout production, identifying patterns and insights not easily observed through traditional methods. As sustainable alternatives to petrochemical-based plastics, biopolymers present unique challenges due to their reliance on variable bio-based feedstocks and complex processing conditions. This review systematically summarizes the current applications of ML techniques in biopolymer production, aiming to provide a comprehensive reference for future research while highlighting the potential of ML to enhance efficiency, reduce costs, and improve product quality. This review also shows the role of ML algorithms, including supervised, unsupervised, and deep learning algorithms, in optimizing biopolymer manufacturing processes. Full article
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