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

Deadline for manuscript submissions: closed (31 December 2021) | Viewed by 33031

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Special Issue Editors

Prof. Dr. Ana Vallés-Lluch

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Centre for Biomaterials and Tissue Engineering, Universitat Politècnica de València, 46022 Valencia, Spain
Interests: biomaterials; tissue engineering; the development of materials with controlled chemistry and microporous structures; the morphological, physicochemical, and mechanical characterization of materials; interactions with the biological environment
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Dr. Guillermo Vilariño-Feltrer

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Centre for Biomaterials and Tissue Engineering, Universitat Politècnica de València, 46022 Valencia, Spain
Interests: polymers; biomedical applications; polymer nanocomposites; hyperbranched polyesters; scaffolds; hydrogels; spatial gradient; structure/property relationships in polymers; molecular structure
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Prof. Dr. José Carlos Rodríguez Hernández

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Centre for Biomaterials and Tissue Engineering, Universitat Politècnica de València, 46022 Valencia, Spain
Interests: biomaterials; polymers; cell–material interactions; ECM protein adsorption on substrates; atomic force microscopy; porous materials for regenerative therapies
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Special Issue Information

Dear Colleagues,

Polymeric biomolecules (a.k.a. biopolymers), either produced by living organisms or chemically synthesized from a biological material, have endless applications in the medical field, as culture platforms, as cell vehicles for tissue engineering strategies and drug carriers, in fixing and wound-healing devices, or testing and clinical diagnosis.

This Special Issue covers newly designed biopolymer-based systems with potential in the biomedical field and their biological development towards a targeted application. The Special Issue will collect original papers and reviews covering, but not restricted to, the following topics:

Biopolymer design attending to particular needs (functionalization of biopolymers, cross-linking techniques; multicomponent systems, nanocomposites; modulation of relevant properties)
Advances in conventional and novel (rapid prototyping and bioprinting) fabrication techniques of scaffolds
Injectable hydrogels and microparticles; smart materials; biosensors
Biopolymers for encapsulation and controlled delivery of drugs/biologically active substances
Interaction with the biological medium (molecular, cellular or tissue responses; surface-protein-cell interaction; biocompatibility, bioactivity and hydrolysis; culture protocols and sterilization issues)

Prof. Dr. Ana Vallés-Lluch
Prof. Dr. Guillermo Vilariño-Feltrer
Prof. Dr. José Carlos Rodríguez Hernández
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

Natural polymer
biodegradable
biopolymer design
functionalization
cross-linking
scaffold
hydrogel
microparticle
biocompatibility
hydrolysis
tissue engineering
drug delivery

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Published Papers (7 papers)

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Research

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13 pages, 2181 KiB

Open AccessArticle

α-Mangostin/γ-Cyclodextrin Inclusion Complex: Formation and Thermodynamic Study

by Ine Suharyani, Muchtaridi Muchtaridi, Ahmed Fouad Abdelwahab Mohammed, Khaled M. Elamin, Nasrul Wathoni and Marline Abdassah

Polymers 2021, 13(17), 2890; https://doi.org/10.3390/polym13172890 - 27 Aug 2021

Cited by 12 | Viewed by 3302

Abstract

α-Mangostin (α-M) has various biological activities, such as anti-cancer, antibacterial, anti-fungal, anti-tyrosin, anti-tuberculosis, anti-inflammatory, and antioxidant. However, it has very low solubility in water. The formulation of this compound requires high amounts of solubilizers, which limits its clinical application. In addition, its low solubility in water is a barrier to the distribution of this drug, thus affecting its potency. Cyclodextrin (CD) is widely used as a solubility enhancer of poorly soluble drugs. This study aimed to increase the solubility of α-M in water through complex formation with CD. The complex of α-Mangostin and γ-Cyclodextrin (α-M/γ-CD CX) was prepared by the solubilization method, resulting in a solubility improvement of α-M in water. Characterization of α-M/γ-CD CX by using FTIR-Spectrometry, XRD, H-, C-, and HMBC-NMR showed that α-M was able to form an inclusion complex with γ-CD. The complex yielded an entrapment efficiency of 84.25 and the thermodynamic study showed that the α-M/γ-CD CX was formed spontaneously, based on the negative values of Gibbs energy and ΔH. Interestingly, the solubility of α-M/γ-CD CX significantly increased by 31.74-fold compared with α-M. These results suggest that α-M/γ-CD CX has the potential in the formulation of water-based preparation for clinical applications. Full article

(This article belongs to the Special Issue Biopolymers for Medical and Pharmaceutical Applications)

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17 pages, 20848 KiB

Open AccessArticle

Investigating the Viability of Epithelial Cells on Polymer Based Thin-Films

by Boštjan Vihar, Jan Rožanc, Boštjan Krajnc, Lidija Gradišnik, Marko Milojević, Laura Činč Ćurić and Uroš Maver

Polymers 2021, 13(14), 2311; https://doi.org/10.3390/polym13142311 - 14 Jul 2021

Cited by 7 | Viewed by 4322

Abstract

The development of novel polymer-based materials opens up possibilities for several novel applications, such as advanced wound dressings, bioinks for 3D biofabrication, drug delivery systems, etc. The aim of this study was to evaluate the viability of vascular and intestinal epithelial cells on different polymers as a selection procedure for more advanced cell-polymer applications. In addition, possible correlations between increased cell viability and material properties were investigated. Twelve polymers were selected, and thin films were prepared by dissolution and spin coating on silicon wafers. The prepared thin films were structurally characterized by Fourier transform infrared spectroscopy, atomic force microscopy, and goniometry. Their biocompatibility was determined using two epithelial cell lines (human umbilical vein endothelial cells and human intestinal epithelial cells), assessing the metabolic activity, cell density, and morphology. The tested cell lines showed different preferences regarding the culture substrate. No clear correlation was found between viability and individual substrate characteristics, suggesting that complex synergistic effects may play an important role in substrate design. These results show that a systematic approach is required to compare the biocompatibility of simple cell culture substrates as well as more complex applications (e.g., bioinks). Full article

(This article belongs to the Special Issue Biopolymers for Medical and Pharmaceutical Applications)

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11 pages, 4227 KiB

Open AccessArticle

Role of Electrospinning Parameters on Poly(Lactic-co-Glycolic Acid) and Poly(Caprolactone-co-Glycolic acid) Membranes

by María Herrero-Herrero, José Antonio Gómez-Tejedor and Ana Vallés-Lluch

Polymers 2021, 13(5), 695; https://doi.org/10.3390/polym13050695 - 25 Feb 2021

Cited by 18 | Viewed by 3246

Abstract

Poly(lactic-co-glycolic acid) (PLGA) and poly(caprolactone-co-glycolic acid) (PCLGA) solutions were electrospun into membranes with tailored fiber diameter of 1.8 μm. This particular fiber diameter was tuned depending on the used co-polymer by adjusting the electrospinning parameters that mainly influence the fiber diameter. The greatest setting of the fiber diameter was achieved by varying the polymer solution parameters (polymer concentration, solvents and solvents ratio). PLGA was adequately electrospun with 1,1,1,3,3,3-hexafluoro-2-propanol (HFIP), whereas PCLGA required a polar solvent (such as chloroform) with a lower dielectric constant. Moreover, due to the amorphous morphology of PCLGA, pyridine as salt had to be added to the starting solution to increase its conductivity and make it electrospinnable. Indeed, the electrospinning of this co-polymer presents notable difficulties due to its amorphous structure. Interestingly, PCLGA, having a higher glycolic acid molar fraction than commonly electrospun co-polymers (caprolactone:glycolic acid ratio of 45:55 instead of 90:10), could be successfully electrospun, which has not been reported to date. To an accurate setting of fiber diameter, the voltage and the distance from needle to collector were varied. Finally, the study of the surface tension, conductivity and viscosity of the polymer solutions allowed to correlate these particular characteristics of the solutions with the electrospinning variables so that prior knowledge of them enables predicting the required processing conditions. Full article

(This article belongs to the Special Issue Biopolymers for Medical and Pharmaceutical Applications)

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14 pages, 6765 KiB

Open AccessArticle

Role of Curing Temperature of Poly(Glycerol Sebacate) Substrates on Protein-Cell Interaction and Early Cell Adhesion

by Rubén Martín-Cabezuelo, José Carlos Rodríguez-Hernández, Guillermo Vilariño-Feltrer and Ana Vallés-Lluch

Polymers 2021, 13(3), 382; https://doi.org/10.3390/polym13030382 - 26 Jan 2021

Cited by 7 | Viewed by 3100

Abstract

A novel procedure to obtain smooth, continuous polymeric surfaces from poly(glycerol sebacate) (PGS) has been developed with the spin-coating technique. This method proves useful for separating the effect of the chemistry and morphology of the networks (that can be obtained by varying the synthesis parameters) on cell-protein-substrate interactions from that of structural variables. Solutions of the PGS pre-polymer can be spin-coated, to then be cured. Curing under variable temperatures has been shown to lead to PGS networks with different chemical properties and topographies, conditioning their use as a biomaterial. Particularly, higher synthesis temperatures yield denser networks with fewer polar terminal groups available on the surface. Material-protein interactions were characterised by using extracellular matrix proteins such as fibronectin (Fn) and collagen type I (Col I), to unveil the biological interface profile of PGS substrates. To that end, atomic force microscopy (AFM) images and quantification of protein adsorbed in single, sequential and competitive protein incubations were used. Results reveal that Fn is adsorbed in the form of clusters, while Col I forms a characteristic fibrillar network. Fn has an inhibitory effect when incubated prior to Col I. Human umbilical endothelial cells (HUVECs) were also cultured on PGS surfaces to reveal the effect of synthesis temperature on cell behaviour. To this effect, early focal adhesions (FAs) were analysed using immunofluorescence techniques. In light of the results, 130 °C seems to be the optimal curing temperature since a preliminary treatment with Col I or a Fn:Col I solution facilitates the formation of early focal adhesions and growth of HUVECs. Full article

(This article belongs to the Special Issue Biopolymers for Medical and Pharmaceutical Applications)

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14 pages, 2377 KiB

Open AccessArticle

In Vitro Investigation of Thiol-Functionalized Cellulose Nanofibrils as a Chronic Wound Environment Modulator

by Anna Blasi-Romero, Carlos Palo-Nieto, Corine Sandström, Jonas Lindh, Maria Strømme and Natalia Ferraz

Polymers 2021, 13(2), 249; https://doi.org/10.3390/polym13020249 - 13 Jan 2021

Cited by 12 | Viewed by 4026

Abstract

There is currently a huge need for new, improved therapeutic approaches for the treatment of chronic wounds. One promising strategy is to develop wound dressings capable of modulating the chronic wound environment (e.g., by controlling the high levels of reactive oxygen species (ROS) and proteases). Here, we selected the thiol-containing amino acid cysteine to endow wood-derived cellulose nanofibrils (CNF) with bioactivity toward the modulation of ROS levels and protease activity. Cysteine was covalently incorporated into CNF and the functionalized material, herein referred as cys-CNF, was characterized in terms of chemical structure, degree of substitution, radical scavenging capacity, and inhibition of protease activity. The stability of the thiol groups was evaluated over time, and an in vitro cytotoxicity study with human dermal fibroblasts was performed to evaluate the safety profile of cys-CNF. Results showed that cys-CNF was able to efficiently control the activity of the metalloprotease collagenase and to inhibit the free radical DPPH (1,1-Diphenyl-2-picrylhydrazyl radical), activities that were correlated with the presence of free thiol groups on the nanofibers. The stability study showed that the reactivity of the thiol groups challenged the bioactivity over time. Nevertheless, preparing the material as an aerogel and storing it in an inert atmosphere were shown to be valid approaches to increase the stability of the thiol groups in cys-CNF. No signs of toxicity were observed on the dermal fibroblasts when exposed to cys-CNF (concentration range 0.1–0.5 mg/mL). The present work highlights cys-CNF as a promising novel material for the development of bioactive wound dressings for the treatment of chronic wounds. Full article

(This article belongs to the Special Issue Biopolymers for Medical and Pharmaceutical Applications)

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14 pages, 1909 KiB

Open AccessArticle

pH-Sensitive Starch-Based Hydrogels: Synthesis and Effect of Molecular Components on Drug Release Behavior

by Juan Carlos Quintanilla de Stéfano, Vanessa Abundis-Correa, Sergio Daniel Herrera-Flores and Alejandro J. Alvarez

Polymers 2020, 12(9), 1974; https://doi.org/10.3390/polym12091974 - 31 Aug 2020

Cited by 45 | Viewed by 4624

Abstract

The drug release behavior of pH-sensitive starch-based hydrogels was systematically studied. Hydrogels were synthesized by copolymerization of acrylic acid (AA) and other acrylate comonomers onto the starch backbone. The hydrophilic agents 2-hydroxy ethyl methacrylate (HEMA), and acrylamide (AAm), as well as the hydrophobic butyl-methacrylate (BMA), were utilized as comonomers. Methylene-bisacrylamide (MBA) was employed as a crosslinking agent. The synthesized hydrogels were loaded with caffeine as a model drug. The effects of the hydrophobic/hydrophilic character of the comonomers and chemical crosslinking on the swelling capacity and the release rate of caffeine were investigated. The use of the crosslinking agent and hydrophobic monomers decreased the swelling capacity of the hydrogels. The release rate of caffeine increased with the presence of a hydrophobic monomer. The fastest release was obtained with the AA/BMA/AAm formulation, and the slowest release was observed with the AA/HEMA/AAm formulation. The transport mechanism was controlled by Fickian diffusion in formulations containing AAm, and controlled by the polymer-relaxation mechanism in formulations containing MBA. Overall, our results showed that the swelling and drug delivery behavior can be tuned by varying the chemical composition of the copolymer formulations. These starch-based hydrogels can be useful as drug delivery devices in many biomedical applications. Full article

(This article belongs to the Special Issue Biopolymers for Medical and Pharmaceutical Applications)

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Review

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17 pages, 459 KiB

Open AccessReview

Antibacterial-Integrated Collagen Wound Dressing for Diabetes-Related Foot Ulcers: An Evidence-Based Review of Clinical Studies

by Ibrahim N. Amirrah, Mohd Farhanulhakim Mohd Razip Wee, Yasuhiko Tabata, Ruszymah Bt Hj Idrus, Abid Nordin and Mh Busra Fauzi

Polymers 2020, 12(9), 2168; https://doi.org/10.3390/polym12092168 - 22 Sep 2020

Cited by 51 | Viewed by 8675

Abstract

Diabetic foot ulcer (DFU) is a chronic wound frequently delayed from severe infection. Wound dressing provides an essential barrier between the ulcer and the external environment. This review aimed to analyse the effectiveness of antibacterial collagen-based dressing for DFU treatment in a clinical setting. An electronic search in four databases, namely, Scopus, PubMed, Ovid MEDLINE(R), and ISI Web of Science, was performed to obtain relevant articles published within the last ten years. The published studies were included if they reported evidence of (1) collagen-based antibacterial dressing or (2) wound healing for diabetic ulcers, and (3) were written in English. Both randomised and non-randomised clinical trials were included. The search for relevant clinical studies (n) identified eight related references discussing the effectiveness of collagen-based antibacterial wound dressings for DFU comprising collagen impregnated with polyhexamethylene biguanide (n = 2), gentamicin (n = 3), combined-cellulose and silver (n = 1), gentian violet/methylene blue mixed (n = 1), and silver (n = 1). The clinical data were limited by small sample sizes and multiple aetiologies of chronic wounds. The evidence was not robust enough for a conclusive statement, although most of the studies reported positive outcomes for the use of collagen dressings loaded with antibacterial properties for DFU wound healing. This study emphasises the importance of having standardised clinical trials, larger sample sizes, and accurate reporting for reliable statistical evidence confirming DFU treatment efficiency. Full article

(This article belongs to the Special Issue Biopolymers for Medical and Pharmaceutical Applications)

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