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Macromol, Volume 5, Issue 3 (September 2025) – 10 articles

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13 pages, 1293 KB  
Article
Development of a Drug Delivery System with Bacterial Cellulose and Gelatin: Physicochemical and Microbiological Evaluation
by Gabriel P. Machado, Natasha L. A. Ibanez, Patricia L. M. Alves, Ana C. Chacon, Larissa Simões, Victoria Schultz, Samanta Oliveira, Denise Grotto and Angela F. Jozala
Macromol 2025, 5(3), 39; https://doi.org/10.3390/macromol5030039 - 27 Aug 2025
Abstract
The growing threat of antimicrobial resistance drives the need for innovative and multifunctional therapeutic systems. In this study, a controlled-release system based on a bioactive film composed of gelatin, bacterial cellulose (BC), sericin, citric acid, PEG 400, and nisin was developed for topical [...] Read more.
The growing threat of antimicrobial resistance drives the need for innovative and multifunctional therapeutic systems. In this study, a controlled-release system based on a bioactive film composed of gelatin, bacterial cellulose (BC), sericin, citric acid, PEG 400, and nisin was developed for topical applications in infected wound treatment. BC membranes were produced using Komagataeibacter xylinus and enzymatically treated to optimize dispersion within the polymer matrix. The resulting system exhibited a semi-rigid, homogeneous morphology with appropriate visual characteristics for dermatological use. Microbiological assays demonstrated significant antimicrobial activity against Gram-positive (Staphylococcus aureus) and resistant Gram-negative strains (Escherichia coli and Enterobacter cloacae), attributed to the synergistic action of nisin and citric acid, which enhanced bacterial outer membrane permeability. The antioxidant capacity was confirmed through DPPH radical scavenging assays, indicating a progressive release of bioactive compounds over time. Scanning electron microscopy (SEM) analyses revealed good integration of biopolymers within the matrix. These results suggest that the strategic combination of natural biopolymers and antimicrobial agents produced a functional system with improved mechanical properties, a broadened antimicrobial spectrum, and promising potential as a bioactive wound dressing for the treatment of infected skin lesions. Full article
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18 pages, 1160 KB  
Review
Machine Learning for the Optimization of the Bioplastics Design
by Neelesh Ashok, Pilar Garcia-Diaz, Marta E. G. Mosquera and Valentina Sessini
Macromol 2025, 5(3), 38; https://doi.org/10.3390/macromol5030038 - 14 Aug 2025
Viewed by 263
Abstract
Biodegradable polyesters have gained attention due to their sustainability benefits, considering the escalating environmental challenges posed by synthetic polymers. Advances in artificial intelligence (AI), including machine learning (ML) and deep learning (DL), are expected to significantly accelerate research in polymer science. This review [...] Read more.
Biodegradable polyesters have gained attention due to their sustainability benefits, considering the escalating environmental challenges posed by synthetic polymers. Advances in artificial intelligence (AI), including machine learning (ML) and deep learning (DL), are expected to significantly accelerate research in polymer science. This review article explores “bio” polymer informatics by harnessing insights from the AI techniques used to predict structure–property relationships and to optimize the synthesis of bioplastics. This review also discusses PolyID, a machine learning-based tool that employs message-passing graph neural networks to provide a framework capable of accelerating the discovery of bioplastics. An extensive literature review is conducted on explainable AI (XAI) and generative AI techniques, as well as on benchmarking data repositories in polymer science. The current state-of-the art in ML methods for ring-opening polymerizations and the synthesizability of biodegradable polyesters is also presented. This review offers an in-depth insight and comprehensive knowledge of current AI-based models for polymerizations, molecular descriptors, structure–property relationships, predictive modeling, and open-source benchmarked datasets for sustainable polymers. This study serves as a reference and provides critical insights into the capabilities of AI for the accelerated design and discovery of green polymers aimed at achieving a sustainable future. Full article
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18 pages, 1307 KB  
Review
Smart Theranostic Platforms Based on Carbohydrate Hydrogels
by Silvia Romano, Sorur Yazdanpanah, Raffaele Conte, Agnello De Rosa, Antonio Fico, Gianfranco Peluso, Parisa Pedram and Arash Moeini
Macromol 2025, 5(3), 37; https://doi.org/10.3390/macromol5030037 - 14 Aug 2025
Viewed by 211
Abstract
Carbohydrate-based hydrogels represent a new advancement in the development of multifunctional biomedical systems, thanks to their intrinsic biocompatibility, structural versatility, and capacity for functional modification. This review examines the latest progress made in employing these materials as intelligent theranostic platforms, with a particular [...] Read more.
Carbohydrate-based hydrogels represent a new advancement in the development of multifunctional biomedical systems, thanks to their intrinsic biocompatibility, structural versatility, and capacity for functional modification. This review examines the latest progress made in employing these materials as intelligent theranostic platforms, with a particular focus on their role as biosensors and therapeutic drug delivery devices. Engineered to interact dynamically with the biological environment, carbohydrate hydrogels enable the site-specific release of therapeutic agents while simultaneously supporting the monitoring of key physiological markers. Their dual functionality offers significant advantages in managing complex pathologies such as cancer, metabolic disorders, and chronic inflammation, where personalized treatment and real-time feedback are essential. By exploring their biological application, this review underscores the pivotal role played by carbohydrate hydrogels in advanced therapeutic technologies. Full article
(This article belongs to the Special Issue Recent Trends in Carbohydrate-Based Therapeutics)
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26 pages, 1016 KB  
Review
Chemically Modified Alginate-Based Hydrogel-Matrices in Drug Delivery
by Angélica Román-Guerrero, Stefani Cortés-Camargo, Erik Alpizar-Reyes, Miriam Fabiola Fabela-Morón, Julian Cruz-Olivares, Sandra Karina Velázquez-Gutiérrez and César Pérez-Alonso
Macromol 2025, 5(3), 36; https://doi.org/10.3390/macromol5030036 - 12 Aug 2025
Viewed by 457
Abstract
Alginate is a biomaterial that has demonstrated considerable potential and adaptability in the field of controlled drug delivery due to its unique physicochemical properties. Chemical modification of alginate has significantly enhanced its functionality, allowing the development of matrices with improved characteristics, such as [...] Read more.
Alginate is a biomaterial that has demonstrated considerable potential and adaptability in the field of controlled drug delivery due to its unique physicochemical properties. Chemical modification of alginate has significantly enhanced its functionality, allowing the development of matrices with improved characteristics, such as increased affinity for hydrophobic drugs, sustained and controlled release, and improved cell and tissue adhesion. Hydrogels, microspheres, nanoparticles, and porous scaffolds are among the most extensively studied alginate-based drug delivery systems. It is estimated that over 50% of these systems have shown successful outcomes in in vitro testing, particularly in applications such as oral delivery of proteins and peptides, wound healing, tissue regeneration, and cancer therapy. Recent clinical advances involving alginate include the development of wound dressings, growth factor delivery systems, and cell-based therapies for treating degenerative diseases. Chemically modified alginate thus emerges as a highly adaptable and promising candidate for the design of advanced drug delivery systems across a wide range of biomedical applications. This review encompasses more than 100 research articles and aims to provide an updated overview of the current state of knowledge regarding the use of chemically modified alginate-based hydrogel systems in drug delivery. Full article
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15 pages, 2161 KB  
Article
Preparation of PLLA and PLGA Copolymers with Poly(ethylene adipate) Through Reactive Melt Mixing: Structural Characterization, Thermal Properties, and Molecular Mobility Insights
by Evi Christodoulou, Christina Samiotaki, Alexandra Zamboulis, Rizos Evangelos Bikiaris, Panagiotis A. Klonos, Apostolos Kyritsis and Dimitrios N. Bikiaris
Macromol 2025, 5(3), 35; https://doi.org/10.3390/macromol5030035 - 7 Aug 2025
Viewed by 261
Abstract
In this study, a series of copolymers was synthesized using the promising biodegradable polymers Poly(L-lactic acid) (PLLA), Poly(lactic-co-glycolic acid) (PLGA), and Poly(ethylene adipate) (PEAd), known for their high potential. PEAd was synthesized through a two-step melt polycondensation process and then used to prepare [...] Read more.
In this study, a series of copolymers was synthesized using the promising biodegradable polymers Poly(L-lactic acid) (PLLA), Poly(lactic-co-glycolic acid) (PLGA), and Poly(ethylene adipate) (PEAd), known for their high potential. PEAd was synthesized through a two-step melt polycondensation process and then used to prepare copolymers with PLLA (PLLA-co-PEAd) and PLGA (PLGA-co-PEAd) at weight ratios of 90/10 and 75/25, respectively. The synthesized materials, along with the starting polymers, were extensively characterized for their structure, molecular weight, crystallinity, and thermal behavior. These novel systems exhibit single thermal transitions, e.g., glass transition. The incorporation of PEAd into the copolymers induced a plasticizing effect, evidenced by a consistent decrease in the glass transition temperature. Due to the latter effect in combination with the Mw drop, the facilitation of crystal nucleation was observed. Finally, the results by dielectric spectroscopy on the local and segmental molecular mobility provided additional proof for the homogeneity of the systems, as manifested, e.g., by the recording of single segmental relaxation processes. Overall, the findings indicate that the PLLA-co-PEAd and PLGA-co-PEAd copolymers hold significant potential, and the use of complementary experimental techniques offers valuable insights and indirect indications of their properties. Full article
(This article belongs to the Collection Advances in Biodegradable Polymers)
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30 pages, 2013 KB  
Review
Biopolymers in Biotechnology and Tissue Engineering: A Comprehensive Review
by Maciej Grabowski, Dominika Gmyrek, Maria Żurawska and Anna Trusek
Macromol 2025, 5(3), 34; https://doi.org/10.3390/macromol5030034 - 21 Jul 2025
Viewed by 1094
Abstract
Since the mid-19th century, researchers have explored the potential of bio-based polymeric materials for diverse applications, with particular promise in medicine. This review provides a focused and detailed examination of natural and synthetic biopolymers relevant to tissue engineering and biomedical applications. It emphasizes [...] Read more.
Since the mid-19th century, researchers have explored the potential of bio-based polymeric materials for diverse applications, with particular promise in medicine. This review provides a focused and detailed examination of natural and synthetic biopolymers relevant to tissue engineering and biomedical applications. It emphasizes the structural diversity, functional characteristics, and processing strategies of major classes of biopolymers, including polysaccharides (e.g., hyaluronic acid, alginate, chitosan, bacterial cellulose) and proteins (e.g., collagen, silk fibroin, albumin), as well as synthetic biodegradable polymers such as polycaprolactone, polylactic acid, and polyhydroxybutyrate. The central aim of this manuscript is to elucidate how intrinsic properties—such as molecular weight, crystallinity, water retention, and bioactivity—affect the performance of biopolymers in biomedical contexts, particularly in drug delivery, wound healing, and scaffold-based tissue regeneration. This review also highlights recent advancements in polymer functionalization, composite formation, and fabrication techniques (e.g., electrospinning, bioprinting), which have expanded the application potential of these materials. By offering a comparative analysis of structure–property–function relationships across a diverse range of biopolymers, this review provides a comprehensive reference for selecting and engineering materials tailored to specific biomedical challenges. It also identifies key limitations, such as production scalability and mechanical performance, and suggests future directions for developing clinically viable and environmentally sustainable biomaterial platforms. Full article
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17 pages, 6691 KB  
Article
Antibiotic-Coated Melt Electrowritten Polycaprolactone Meshes: Fabrication and In Vitro Antibacterial Evaluation
by Joana Pinheiro Martins, Ana Sofia de Sousa, Sofia Costa de Oliveira, António Augusto Fernandes and Elisabete Teixeira da Silva
Macromol 2025, 5(3), 33; https://doi.org/10.3390/macromol5030033 - 16 Jul 2025
Viewed by 388
Abstract
In recent years, pelvic organ prolapse (POP) cases have been rising, affecting women’s quality of life. Synthetic surgical transvaginal meshes used for POP treatment were withdrawn from the United States market in 2019 due to high risks, including infection, vaginal mesh erosion, and [...] Read more.
In recent years, pelvic organ prolapse (POP) cases have been rising, affecting women’s quality of life. Synthetic surgical transvaginal meshes used for POP treatment were withdrawn from the United States market in 2019 due to high risks, including infection, vaginal mesh erosion, and POP reoccurrence. Biodegradable mesh implants with three-dimensional printing technology have emerged as an innovative alternative. In this study, polycaprolactone (PCL) meshes for POP repair were fabricated using melt electrospinning writing (MEW) and mechanically evaluated through uniaxial tensile tests. Following this, they were coated with antibiotics—azithromycin, gentamicin sulfate, and ciprofloxacin—commonly used for genitourinary tract infections. Zone inhibition and biofilm assays evaluated antibiotic effectiveness in preventing mesh infections by Escherichia coli, and methicillin-susceptible (MSSA) and methicillin-resistant (MRSA) Staphylococcus aureus. The meshes presented a mechanical behavior closer to vaginal tissue than commercially available meshes. Fourier transform infrared analysis confirmed antibiotic incorporation. Ciprofloxacin demonstrated antibacterial activity against MRSA, with a 92% reduction in metabolic activity and a 99% biomass reduction. Gentamicin and ciprofloxacin displayed inhibitory activity against MSSA and E. coli. Scanning electron microscopy images support these conclusions. This methodology may offer a more effective, patient-friendly solution for POP repair, improving healing and the quality of life for affected women. Full article
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16 pages, 1822 KB  
Article
Upcycling Microalgal Residues: Physicochemical Insights and Biocomposite Enhancement
by Valerio Cuboni, Raffaella Lettieri, Alice Caravella, Martina Corvino, Viviana Scognamiglio, Amina Antonacci and Emanuela Gatto
Macromol 2025, 5(3), 32; https://doi.org/10.3390/macromol5030032 - 8 Jul 2025
Viewed by 422
Abstract
The growing concern for environmental sustainability has led to an increased interest in biodegradable materials derived from renewable resources. This study explores the innovative use of residual biomass from the green photosynthetic microalga Chlamydomonas reinhardtii, left over after polysaccharide extraction, as a [...] Read more.
The growing concern for environmental sustainability has led to an increased interest in biodegradable materials derived from renewable resources. This study explores the innovative use of residual biomass from the green photosynthetic microalga Chlamydomonas reinhardtii, left over after polysaccharide extraction, as a natural filler in the development of the compostable protein-based material SP-Milk®. The microalgal biomass was characterized using Fourier transform infrared spectroscopy (FTIR) and UV-Visible Spectroscopy to assess its chemical and structural composition. Subsequently, it was incorporated into a biodegradable protein matrix, and the resulting biocomposites were evaluated for mechanical and thermal properties. The results demonstrate that the incorporation of algal filler improves the mechanical strength and elasticity of the material while reducing its glass transition temperature, highlighting its potential for use in sustainable applications as a possible substitute for conventional plastics. The biocomposite materials developed, based on the protein-based material SP-Milk® and residual microalgal biomass, are environmentally friendly, contributing to the reduction in pollution and the risks associated with plastic accumulation. Thus, this study offers a simple, effective, and sustainable strategy for the valorization of microalgal biomass, enabling the production of biodegradable materials with enhanced mechanical performance, suitable for applications such as sustainable packaging within a circular economy framework. Full article
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16 pages, 2885 KB  
Article
In Situ Synthesis, Crystallization Behavior, and Physical Properties of Biobased Poly(propyl thiophenedicarboxylate)/Multi-Walled Carbon Nanotubes Composites
by Chaoran Zhang, Shiwei Feng and Zhaobin Qiu
Macromol 2025, 5(3), 31; https://doi.org/10.3390/macromol5030031 - 3 Jul 2025
Viewed by 300
Abstract
Poly(propylene thiophenedicarboxylate) (PPTh) is a new type of fully biobased polyester with excellent thermal, mechanical, and barrier properties; however, its practical application has been seriously restricted by the relatively slow crystallization rate. To further improve the crystallization rate and broaden the potential application [...] Read more.
Poly(propylene thiophenedicarboxylate) (PPTh) is a new type of fully biobased polyester with excellent thermal, mechanical, and barrier properties; however, its practical application has been seriously restricted by the relatively slow crystallization rate. To further improve the crystallization rate and broaden the potential application field of PPTh, PPTh/multi-walled carbon nanotubes (MWCNTs) composites were successfully synthesized via an in situ melt polycondensation process in this research. Low contents of MWCNTs were well dispersed in the PPTh matrix. MWCNTs significantly increased the melt crystallization temperature and isothermal crystallization rate of PPTh, indicating the effective heterogeneous nucleating agent role. PPTh/MWCNTs composites displayed the same crystal structure as PPTh. In addition, the introduction of MWCNTs significantly enhanced both the Young’s modulus and the tensile strength of PPTh. From a sustainable viewpoint, biobased PPTh/MWCNTs composites reported in this research were of significant importance and interest as they showed remarkably improved crystallization rates and mechanical properties. Full article
(This article belongs to the Collection Advances in Biodegradable Polymers)
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22 pages, 3213 KB  
Article
Innovative Cold Processing of PVOH-Based Composites: A Gate-to-Gate Life Cycle Assessment of Environmental Benefits
by Andrea Marinelli, Fulvio Seva, Alberto Cigada, Luca Paterlini, MariaPia Pedeferri, Maria Vittoria Diamanti and Barbara Del Curto
Macromol 2025, 5(3), 30; https://doi.org/10.3390/macromol5030030 - 3 Jul 2025
Viewed by 320
Abstract
Conventional thermoplastic polymer composites are produced using energy-intensive equipment. From an environmental perspective, reducing energy and material consumption, as well as selecting polymers and fillers that biodegrade without harmful consequences for the environment, is considered good practice. In this work, polyvinyl alcohol (PVOH), [...] Read more.
Conventional thermoplastic polymer composites are produced using energy-intensive equipment. From an environmental perspective, reducing energy and material consumption, as well as selecting polymers and fillers that biodegrade without harmful consequences for the environment, is considered good practice. In this work, polyvinyl alcohol (PVOH), a biodegradable and water-soluble polymer, was compounded with 30 w%, 40 µm long cellulose fibres. Conventional melt blending production and innovative cold processing were compared from a tensile testing, thermogravimetric, and life cycle assessment (LCA) perspective through primary data collection. The granule production process significantly affects the mechanical performance of injected samples, with a 23.4% drop in tensile strength and an increase of 67.9% in elongation at break. The thermogravimetric analysis reported slight differences due to an additional thermal process involved in the melt blending of PVOH. From an LCA perspective, the innovative cold blending of PVOH-based composites drops all environmental indicators by 58–92%, maximizing the reduction of the “Water use” indicator. The most impactful production phase in the analysed production processes was drying, accounting for 46% and 85% of the conventional melt blending and innovative cold-blending processes, respectively. Full article
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