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Progress in Polymer Research: From Sustainable Materials to Biomedical Application

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

Deadline for manuscript submissions: closed (31 January 2022) | Viewed by 37914

Special Issue Editors


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Guest Editor
Department of Chemistry, University of Bari, Via Orabona 4, 70126 Bari, Italy
Interests: biomaterials; physical chemistry; drug delivery systems; colloids; lipids; proteins; photosynthetic systems; natural products; renewable resources; nanomaterials; nanotechnology

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Guest Editor
Chemistry Department, University of Bari, Via Orabona 4, 70126 Bari, Italy
Interests: physical chemistry; drug delivery systems; lipids; proteins; nanotechnology; nanomaterials

Special Issue Information

Dear Colleagues,

Research in the field of polymeric materials today accepts the challenge of developing ever more sustainable materials while preserving their performance and applicability in extremely wide sectors. In addition to more traditional uses (i.e., for packaging, textiles and consumer products), natural, synthetic, and blends of biopolymers have proven to be competitive to conventional ones also in emerging fields of application such as smart materials and (bio)medical devices. These materials indeed have proven to be able to effectively interface with living matter from the tissue to the cellular scale, providing indispensable features, such as biocompatibility, biodegradability, non-immunogenicity, and many others.

This Special Issue on “Progress in Polymer Research: From Sustainable Materials to Biomedical Application” will focus on the latest advances in research in the field of (bio)polymeric materials, including all aspects of polymers and composites prepared from renewable resources and/or with a sustainable process, intended especially (but not only) for biomedicine and drug delivery. While covering a broad range of fundamental and experimental topics, we invite researchers to contribute to this Special Issue with original research papers, short communications, and review articles.

Prof. Dr. Lucia Catucci
Dr. Vincenzo De Leo
Guest Editors

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

  • Progress in polymeric biomaterials
  • Progress in sustainable polymers
  • (Bio)polymers in drug delivery
  • (Bio)polymers in medical application
  • (Bio)polymers for packaging
  • (Bio)active and (multi)functional biopolymers
  • Therapeutic (bio)polymeric materials
  • Nanosized and nanostructured polymeric (bio)materials

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Published Papers (9 papers)

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Research

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13 pages, 4055 KiB  
Article
Concerning Synthesis of New Biobased Polycarbonates with Curcumin in Replacement of Bisphenol A and Recycled Diphenyl Carbonate as Example of Circular Economy
by Vincenzo De Leo, Michele Casiello, Giuseppe Deluca, Pietro Cotugno, Lucia Catucci, Angelo Nacci, Caterina Fusco and Lucia D’Accolti
Polymers 2021, 13(3), 361; https://doi.org/10.3390/polym13030361 - 23 Jan 2021
Cited by 10 | Viewed by 5246
Abstract
Curcumin (CM) is a natural polyphenol well-known for its antioxidant and pharmaceutical properties, that can represent a renewable alternative to bisphenol A (BPA) for the synthesis of bio-based polycarbonates (PC). In the presented strategy, preparation of the CM-based PC was coupled with chemical [...] Read more.
Curcumin (CM) is a natural polyphenol well-known for its antioxidant and pharmaceutical properties, that can represent a renewable alternative to bisphenol A (BPA) for the synthesis of bio-based polycarbonates (PC). In the presented strategy, preparation of the CM-based PC was coupled with chemical recycling of the fossil-based BPA polycarbonate (BPA-PC) conducting a two-steps trans-polymerization that replaces BPA monomer with CM or its tetrahydrogenated colorless product (THCM). In the first step of synthetic strategy, depolymerization of commercial BPA-PC was carried out with phenol as nucleophile, according to our previous procedure based on zinc derivatives and ionic liquids as catalysts, thus producing quantitatively diphenyl carbonate (DPC) e BPA. In the second step, DPC underwent a melt transesterification with CM or THCM monomers affording the corresponding bio-based polycarbonates, CM-PC and THCM-PC, respectively. THCM was prepared by reducing natural bis-phenol with cyclohexene as a hydrogen donor and characterized by 1H-NMR and MS techniques. Polymerization reactions were monitored by infrared spectroscopy and average molecular weights and dispersity of the two biobased polymers THCM-PC and CM-PC were determined by means of gel permeation chromatography (GPC). Optical properties of the prepared polymers were also measured. Full article
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16 pages, 6866 KiB  
Article
Nanocellulose/Fullerene Hybrid Films Assembled at the Air/Water Interface as Promising Functional Materials for Photo-electrocatalysis
by Francesco Milano, Maria Rachele Guascito, Paola Semeraro, Shadi Sawalha, Tatiana Da Ros, Alessandra Operamolla, Livia Giotta, Maurizio Prato and Ludovico Valli
Polymers 2021, 13(2), 243; https://doi.org/10.3390/polym13020243 - 12 Jan 2021
Cited by 7 | Viewed by 2948
Abstract
Cellulose nanomaterials have been widely investigated in the last decade, unveiling attractive properties for emerging applications. The ability of sulfated cellulose nanocrystals (CNCs) to guide the supramolecular organization of amphiphilic fullerene derivatives at the air/water interface has been recently highlighted. Here, we further [...] Read more.
Cellulose nanomaterials have been widely investigated in the last decade, unveiling attractive properties for emerging applications. The ability of sulfated cellulose nanocrystals (CNCs) to guide the supramolecular organization of amphiphilic fullerene derivatives at the air/water interface has been recently highlighted. Here, we further investigated the assembly of Langmuir hybrid films that are based on the electrostatic interaction between cationic fulleropyrrolidines deposited at the air/water interface and anionic CNCs dispersed in the subphase, assessing the influence of additional negatively charged species that are dissolved in the water phase. By means of isotherm acquisition and spectroscopic measurements, we demonstrated that a tetra-sulfonated porphyrin, which was introduced in the subphase as anionic competitor, strongly inhibited the binding of CNCs to the floating fullerene layer. Nevertheless, despite the strong inhibition by anionic molecules, the mutual interaction between fulleropyrrolidines at the interface and the CNCs led to the assembly of robust hybrid films, which could be efficiently transferred onto solid substrates. Interestingly, ITO-electrodes that were modified with five-layer hybrid films exhibited enhanced electrical capacitance and produced anodic photocurrents at 0.4 V vs Ag/AgCl, whose intensity (230 nA/cm2) proved to be four times higher than the one that was observed with the sole fullerene derivative (60 nA/cm2). Full article
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17 pages, 3355 KiB  
Article
A 3D Printed Composite Scaffold Loaded with Clodronate to Regenerate Osteoporotic Bone: In Vitro Characterization
by Stefania Cometa, Maria Addolorata Bonifacio, Elisabetta Tranquillo, Antonio Gloria, Marco Domingos and Elvira De Giglio
Polymers 2021, 13(1), 150; https://doi.org/10.3390/polym13010150 - 1 Jan 2021
Cited by 10 | Viewed by 3609
Abstract
Additive manufacturing (AM) is changing our current approach to the clinical treatment of bone diseases, providing new opportunities to fabricate customized, complex 3D structures with bioactive materials. Among several AM techniques, the BioCell Printing is an advanced, integrated system for material manufacture, sterilization, [...] Read more.
Additive manufacturing (AM) is changing our current approach to the clinical treatment of bone diseases, providing new opportunities to fabricate customized, complex 3D structures with bioactive materials. Among several AM techniques, the BioCell Printing is an advanced, integrated system for material manufacture, sterilization, direct cell seeding and growth, which allows for the production of high-resolution micro-architectures. This work proposes the use of the BioCell Printing to fabricate polymer-based scaffolds reinforced with ceramics and loaded with bisphosphonates for the treatment of osteoporotic bone fractures. In particular, biodegradable poly(ε-caprolactone) was blended with hydroxyapatite particles and clodronate, a bisphosphonate with known efficacy against several bone diseases. The scaffolds’ morphology was investigated by means of Scanning Electron Microscopy (SEM) and micro-Computed Tomography (micro-CT) while Energy Dispersive X-ray Spectroscopy (EDX) and X-ray Photoelectron Spectroscopy (XPS) revealed the scaffolds’ elemental composition. A thermal characterization of the composites was accomplished by Thermogravimetric analyses (TGA). The mechanical performance of printed scaffolds was investigated under static compression and compared against that of native human bone. The designed 3D scaffolds promoted the attachment and proliferation of human MSCs. In addition, the presence of clodronate supported cell differentiation, as demonstrated by the normalized alkaline phosphatase activity. The obtained results show that the BioCell Printing can easily be employed to generate 3D constructs with pre-defined internal/external shapes capable of acting as a temporary physical template for regeneration of cancellous bone tissues. Full article
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18 pages, 3177 KiB  
Article
An In-Silico Pipeline for Rapid Screening of DNA Aptamers against Mycotoxins: The Case-Study of Fumonisin B1, Aflatoxin B1 and Ochratoxin A
by Fulvio Ciriaco, Vincenzo De Leo, Lucia Catucci, Michelangelo Pascale, Antonio F. Logrieco, Maria C. DeRosa and Annalisa De Girolamo
Polymers 2020, 12(12), 2983; https://doi.org/10.3390/polym12122983 - 14 Dec 2020
Cited by 11 | Viewed by 3177
Abstract
Aptamers are single-stranded oligonucleotides selected by SELEX (Systematic Evolution of Ligands by EXponential Enrichment) able to discriminate target molecules with high affinity and specificity, even in the case of very closely related structures. Aptamers have been produced for several targets including small molecules [...] Read more.
Aptamers are single-stranded oligonucleotides selected by SELEX (Systematic Evolution of Ligands by EXponential Enrichment) able to discriminate target molecules with high affinity and specificity, even in the case of very closely related structures. Aptamers have been produced for several targets including small molecules like mycotoxins; however, the high affinity for their respective target molecules is a critical requirement. In the last decade, the screening through computational methods of aptamers for their affinity against specific targets has greatly increased and is becoming a commonly used procedure due to its convenience and low costs. This paper describes an in-silico approach for rapid screening of ten ssDNA aptamer sequences against fumonisin B1 (FB1, n = 3), aflatoxin B1 (AFB1, n = 2) and ochratoxin A (OTA, n = 5). Theoretical results were compared with those obtained by testing the same aptamers by fluorescent microscale thermophoresis and by magnetic beads assay for their binding affinity (KD) revealing a good agreement. Full article
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12 pages, 5428 KiB  
Article
Mechanistic Study of Synergistic Antimicrobial Effects between Poly (3-hydroxybutyrate) Oligomer and Polyethylene Glycol
by Ziheng Zhang, Jun Li, Linlin Ma, Xingxing Yang, Bin Fei, Polly H. M. Leung and Xiaoming Tao
Polymers 2020, 12(11), 2735; https://doi.org/10.3390/polym12112735 - 18 Nov 2020
Cited by 9 | Viewed by 3281
Abstract
Extended from our previous finding that poly (3-hydroxybutyrate) (PHB) oligomer is an effective antimicrobial agent against gram-positive bacteria, gram-negative bacteria, fungi and multi-drug resistant bacteria, this work investigates the effect of polyethylene glycol (PEG) on the antimicrobial effect of PHB oligomer. To investigate [...] Read more.
Extended from our previous finding that poly (3-hydroxybutyrate) (PHB) oligomer is an effective antimicrobial agent against gram-positive bacteria, gram-negative bacteria, fungi and multi-drug resistant bacteria, this work investigates the effect of polyethylene glycol (PEG) on the antimicrobial effect of PHB oligomer. To investigate and explain this promoting phenomenon, three hypothetic mechanisms were proposed, that is, generation of new antimicrobial components, degradation of PHB macromolecules and dissolution/dispersion of PHB oligomer by PEG. With a series of systematic experiments and characterizations of high-performance liquid chromatography–mass spectrometry (HPLC-MS), it was deducted that PEG promotes the antimicrobial effect of PHB oligomer synergistically through dissolution/dispersion, owing to its amphipathy, which improves the hydrophilicity of PHB oligomer. Full article
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16 pages, 742 KiB  
Article
Manufacture of Reduced Fat White-Brined Cheese with the Addition of β-Glucans Biobased Polysaccharides as Textural Properties Improvements
by Efthymia Kondyli, Eleni C. Pappa, Alexandra Kremmyda, Dimitris Arapoglou, Maria Metafa, Christos Eliopoulos and Cleanthes Israilides
Polymers 2020, 12(11), 2647; https://doi.org/10.3390/polym12112647 - 10 Nov 2020
Cited by 18 | Viewed by 2811
Abstract
β-Glucan, isolated from the mushroom Pleurotus ostreatus, at a concentration of 0.4%, was used in the manufacture of reduced-fat white-brined cheese from sheep milk. Control reduced-fat cheese was also produced from the same milk without the addition of β-glucan. The resultant cheeses [...] Read more.
β-Glucan, isolated from the mushroom Pleurotus ostreatus, at a concentration of 0.4%, was used in the manufacture of reduced-fat white-brined cheese from sheep milk. Control reduced-fat cheese was also produced from the same milk without the addition of β-glucan. The resultant cheeses were examined for their physicochemical characteristics, color and textural properties, and level of proteolysis and lipolysis. Furthermore, cheeses were evaluated organoleptically. In general, there were no statistical differences in the physicochemical characteristics and proteolysis levels found between both cheeses. The addition of β-glucan improved textural properties, and the cheeses received favorable grades for all the organoleptic characteristics. There were no flavor defects (such as a bitter taste) described by the panellists in this study. Generally, the addition of β-glucan did not significantly affect total free fatty acid content; however, at 180 days of ripening and storage, cheeses with the addition of β-glucan had a higher (p < 0.05) content than cheeses without β-glucan. The major fatty acids were acetic acid and capric acid. Full article
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14 pages, 2767 KiB  
Article
Biomimetic Polyurethane 3D Scaffolds Based on Polytetrahydrofuran Glycol and Polyethylene Glycol for Soft Tissue Engineering
by Kun Luo, Li Wang, Xiaohu Chen, Xiyang Zeng, Shiyi Zhou, Peicong Zhang and Junfeng Li
Polymers 2020, 12(11), 2631; https://doi.org/10.3390/polym12112631 - 9 Nov 2020
Cited by 23 | Viewed by 3629
Abstract
In this study, a novel polyurethane porous 3D scaffold based on polyethylene glycol (PEG) and polytetrahydrofuran glycol (PTMG) was developed by in situ polymerization and freeze drying. Aliphatic hexamethylene diisocyanate (HDI) as a nontoxic and safe agent was adopted to produce the rigid [...] Read more.
In this study, a novel polyurethane porous 3D scaffold based on polyethylene glycol (PEG) and polytetrahydrofuran glycol (PTMG) was developed by in situ polymerization and freeze drying. Aliphatic hexamethylene diisocyanate (HDI) as a nontoxic and safe agent was adopted to produce the rigid segment in polyurethane polymerization. The chemical structure, macrostructure, and morphology—as well as mechanical strength of the scaffolds—were characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscope (SEM), and tensile tests. The results show that the HDI can react mildly with hydroxyl (–OH) groups of PEG and PTMG, while gas foaming action caused by the release of CO2 occurred simultaneously in the reactive process, resulting in a uniform porous structure of PU scaffold. Moreover, the scaffolds were soaked in water and freeze dried to obtain higher porosity and more interconnective microstructures. The scaffolds have a porosity of over 70% and pore size from 100 to 800 μm. The mechanical properties increased with increasing PEG content, while the hydrophilicity increased as well. After immersion in simulated body fluid (SBF), the scaffolds presented a stable surface structure. The gas foaming/freezing drying process is an excellent method to prepare skin tissue engineering scaffold from PTMG/PEG materials with high porosity and good inter connectivity. Full article
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18 pages, 4169 KiB  
Article
Preparation and Barrier Performance of Layer-Modified Soil-Stripping/Cassava Starch Composite Films
by Lijie Huang, Xiaoxue Han, Haobin Chen, Shuxiang An, Hanyu Zhao, Hao Xu, Chongxing Huang, Shuangfei Wang and Yang Liu
Polymers 2020, 12(7), 1611; https://doi.org/10.3390/polym12071611 - 20 Jul 2020
Cited by 12 | Viewed by 3006
Abstract
In this study, we investigated the barrier properties of a montmorillonite-reinforced biomass material, starch. Organically modified montmorillonite materials were prepared from natural montmorillonite by reacting it with dodecyl trimethyl ammonium chloride, dodecyl dimethyl benzyl ammonium chloride or octadecyl trimethyl ammonium chloride under ultrasonic [...] Read more.
In this study, we investigated the barrier properties of a montmorillonite-reinforced biomass material, starch. Organically modified montmorillonite materials were prepared from natural montmorillonite by reacting it with dodecyl trimethyl ammonium chloride, dodecyl dimethyl benzyl ammonium chloride or octadecyl trimethyl ammonium chloride under ultrasonic conditions. The composite starch films incorporated with these organically modified montmorillonite samples were characterized by scanning electron microscopy, transmission electron microscopy, infrared spectroscopy and X-ray diffraction. The results showed that the introduction of montmorillonite decreases the transmittance of the composite film by 10% in the visible region and significantly inhibits UV-light transmittance. The decomposition temperature of the composite film ranges from 200 to 500 °C, with a weight loss rate of 80%. The distance between the montmorillonite layers increases from 0.14 nm in the non-magnetized state to 1.49 nm after magnetization. The oxygen permeability of the starch film modified by organic montmorillonite (0.067 cm3/m2·d) is lower than that of the montmorillonite starch film without magnetization (0.097cm3/m2·d). The oxygen barrier capacity is close to zero. Particularly in the ordered magnetic montmorillonite starch composite film, the oxygen barrier ability is the best. Therefore, modified montmorillonite could serve as an excellent reinforcing agent for cassava starch films and effectively improve the oxygen barrier performance of the films. Full article
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Review

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24 pages, 4476 KiB  
Review
Recent Advancements in Polymer/Liposome Assembly for Drug Delivery: From Surface Modifications to Hybrid Vesicles
by Vincenzo De Leo, Francesco Milano, Angela Agostiano and Lucia Catucci
Polymers 2021, 13(7), 1027; https://doi.org/10.3390/polym13071027 - 26 Mar 2021
Cited by 113 | Viewed by 9218
Abstract
Liposomes are consolidated and attractive biomimetic nanocarriers widely used in the field of drug delivery. The structural versatility of liposomes has been exploited for the development of various carriers for the topical or systemic delivery of drugs and bioactive molecules, with the possibility [...] Read more.
Liposomes are consolidated and attractive biomimetic nanocarriers widely used in the field of drug delivery. The structural versatility of liposomes has been exploited for the development of various carriers for the topical or systemic delivery of drugs and bioactive molecules, with the possibility of increasing their bioavailability and stability, and modulating and directing their release, while limiting the side effects at the same time. Nevertheless, first-generation vesicles suffer from some limitations including physical instability, short in vivo circulation lifetime, reduced payload, uncontrolled release properties, and low targeting abilities. Therefore, liposome preparation technology soon took advantage of the possibility of improving vesicle performance using both natural and synthetic polymers. Polymers can easily be synthesized in a controlled manner over a wide range of molecular weights and in a low dispersity range. Their properties are widely tunable and therefore allow the low chemical versatility typical of lipids to be overcome. Moreover, depending on their structure, polymers can be used to create a simple covering on the liposome surface or to intercalate in the phospholipid bilayer to give rise to real hybrid structures. This review illustrates the main strategies implemented in the field of polymer/liposome assembly for drug delivery, with a look at the most recent publications without neglecting basic concepts for a simple and complete understanding by the reader. Full article
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