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Advanced Bio-Based Polymers: Synthesis, Characterization and Applications

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A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Biomaterials".

Deadline for manuscript submissions: closed (30 November 2021) | Viewed by 44745

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Dr. Uroš Maver

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1. Institute of Biomedical Sciences, Faculty of Medicine, University of Maribor, Taborska Ulica 8, SI-2000 Maribor, Slovenia
2. Department of Pharmacology, Faculty of Medicine, University of Maribor, Taborska Ulica 8, SI-2000 Maribor, Slovenia
Interests: biomaterials; pharmacology; drug delivery systems; regenerative medicine; tissue engineering; aerogels
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Dr. Tina Maver

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1. The Institute of Biomedical Sciences, Faculty of Medicine, University of Maribor, Taborska ulica 8, 2000 Maribor, Slovenia
2. The Department of Pharmacology, Faculty of Medicine, University of Maribor, Taborska ulica 8, 2000 Maribor, Slovenia
Interests: in vitro skin model; 3D bioprinting; tissue engineering; wound dressings; electrospinning
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Bio-based polymers are polymers produced from a biomass source, in contrast to those originating from an oleochemical source. Regardless of their abundance and the fact that some have been known for decades, these are still not as widespread as their “petroleum” counterparts, mainly due to barriers facing production, cost and the scalability of their functionalization, as well as finding the best niche applications with high added value (e.g. medicine and electronics). Nevertheless, thanks to innovations in synthetic biology, material science, chemistry and pharmaceutical technology, these polymers are becoming more affordable and therefore increasingly used for various purposes.

In this Special Issue the structural aspects and properties, synthesis, characterization and application of bio-based polymers will be discussed. Original articles, communications, as well as review articles that describe the current state-of-the-art in the proposed field of research are of high interest.

Dr. Uroš Maver
Dr. Tina Maver
Guest Editors

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Keywords

bio-based polymers
functionalization
biodegradability
bioactivity
biomedical applications

Related Special Issue

Advanced Bio-Based Polymers: Synthesis, Characterization and Applications (Second Volume) in Materials (4 articles)

Published Papers (13 papers)

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Research

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14 pages, 4174 KiB

Open AccessArticle

Computational Analysis of Mechanical Performance for Composite Polymer Biodegradable Stents

by Žiga Donik, Branko Nečemer, Matej Vesenjak, Srečko Glodež and Janez Kramberger

Materials 2021, 14(20), 6016; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14206016 - 13 Oct 2021

Cited by 7 | Viewed by 2506

Abstract

Bioresorbable stents (BRS) represent the latest generation of vascular scaffolds used for minimally invasive interventions. They aim to overcome the shortcomings of established bare-metal stents (BMS) and drug-eluting stents (DES). Recent advances in the field of bioprinting offer the possibility of combining biodegradable polymers to produce a composite BRS. Evaluation of the mechanical performance of the novel composite BRS is the focus of this study, based on the idea that they are a promising solution to improve the strength and flexibility performance of single material BRS. Finite element analysis of stent crimping and expansion was performed. Polylactic acid (PLA) and polycaprolactone (PCL) formed a composite stent divided into four layers, resulting in sixteen unique combinations. A comparison of the mechanical performance of the different composite configurations was performed. The resulting stresses, strains, elastic recoil, and foreshortening were evaluated and compared to existing experimental results. Similar behaviour was observed for material configurations that included at least one PLA layer. A pure PCL stent showed significant elastic recoil and less shortening compared to PLA and composite structures. The volumetric ratio of the materials was found to have a more significant effect on recoil and foreshortening than the arrangement of the material layers. Composite BRS offer the possibility of customising the mechanical behaviour of scaffolds. They also have the potential to support the fabrication of personalised or plaque-specific stents. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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17 pages, 3064 KiB

Open AccessArticle

Clindamycin-Based 3D-Printed and Electrospun Coatings for Treatment of Implant-Related Infections

by Tina Maver, Tinkara Mastnak, Mihela Mihelič, Uroš Maver and Matjaž Finšgar

Materials 2021, 14(6), 1464; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14061464 - 17 Mar 2021

Cited by 29 | Viewed by 3148

Abstract

This study presents the development and characterisation of two novel bioactive coatings deposited on TiAlV and AISI 316LVM substrates. The coatings were prepared using 3D printing and electrospinning. The 3D-printed coating consisted of the cellulose nanofibril suspension, alginate, and carboxymethylcellulose (CMC), while CMC and polyethylene oxide were used to prepare the electrospun coating. Both coatings were loaded with the antibiotic clindamycin (CLIN), which is a bacteriostatic lincosamide known for its activity against streptococci, staphylococci, pneumococci, Bacteroides species, and other anaerobes. Initial characterisation of the coatings was performed by attenuated total reflectance Fourier transform infrared spectroscopy, field emission scanning electron microscopy, and atomic force microscopy. Furthermore, the contact angle measurements, swelling rate, and biodegradability of the coatings were investigated. The released concentration of CLIN in PBS (pH = 7.4 at 25 °C) was determined by UV-VIS spectrophotometry. The coatings’ biocompatibility was determined using an MTT (3(4,5 dimethylthiazolyl-2)-2,5-diphenyltetrazolium bromide) assay using an osteoblast cell culture (hFOB 1.19, ATCC CRL 11372). Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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26 pages, 2981 KiB

Open AccessArticle

Electrospun Composite Nanofibrous Materials Based on (Poly)-Phenol-Polysaccharide Formulations for Potential Wound Treatment

by Lidija Fras Zemljič, Uroš Maver, Tjaša Kraševac Glaser, Urban Bren, Maša Knez Hrnčič, Gabrijela Petek and Zdenka Peršin

Materials 2020, 13(11), 2631; https://0-doi-org.brum.beds.ac.uk/10.3390/ma13112631 - 09 Jun 2020

Cited by 14 | Viewed by 2232

Abstract

In this paper, we focus on the preparation of electrospun composite nanofibrous materials based on (poly)-phenol-polysaccharide formulation. The prepared composite nanofibres are ideally suited as a controlled drug delivery system, especially for local treatment of different wounds, owing to their high surface and volume porosity and small fibre diameter. To evaluate the formulations, catechin and resveratrol were used as antioxidants. Both substances were embedded into chitosan particles, and further subjected to electrospinning. Formulations were characterized by determination of the particle size, encapsulation efficiency, as well as antioxidant and antimicrobial properties. The electrospinning process was optimised through fine-tuning of the electrospinning solution and the electrospinning parameters. Scanning electron microscopy was used to evaluate the (nano)fibrous structure, while the successful incorporation of bio substances was assessed by X-ray Photoelectron Spectroscopy and Fourier transform infrared spectroscopy. The bioactive properties of the formed nanofibre -mats were evaluated by measuring the antioxidative efficiency and antimicrobial properties, followed by in vitro substance release tests. The prepared materials are bioactive, have antimicrobial and antioxidative properties and at the same time allow the release of the incorporated substances, which assures a promising use in medical applications, especially in wound care. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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18 pages, 4875 KiB

Open AccessFeature PaperArticle

PDMS-PMOXA-Nanoparticles Featuring a Cathepsin B-Triggered Release Mechanism

by Daniel Ehrsam, Fabiola Porta, Janine Hussner, Isabell Seibert and Henriette E Meyer zu Schwabedissen

Materials 2019, 12(17), 2836; https://0-doi-org.brum.beds.ac.uk/10.3390/ma12172836 - 03 Sep 2019

Cited by 7 | Viewed by 3148

Abstract

Background: It was our intention to develop cathepsin B-sensitive nanoparticles for tumor-site-directed release. These nanoparticles should be able to release their payload as close to the tumor site with a decrease of off-target effects in mind. Cathepsin B, a lysosomal cysteine protease, is associated with premalignant lesions and invasive stages of cancer. Previous studies have shown cathepsin B in lysosomes and in the extracellular matrix. Therefore, this enzyme qualifies as a trigger for such an approach. Methods: Poly(dimethylsiloxane)-b-poly(methyloxazoline) (PDMS-PMOXA) nanoparticles loaded with paclitaxel were formed by a thin-film technique and standard coupling reactions were used for surface modifications. Despite the controlled release mechanism, the physical properties of the herein created nanoparticles were described. To characterize potential in vitro model systems, quantitative polymerase chain reaction and common bioanalytical methods were employed. Conclusions: Stable paclitaxel-loaded nanoparticles with cathepsin B digestible peptide were formed and tested on the ovarian cancer cell line OVCAR-3. These nanoparticles exerted a pharmacological effect on the tumor cells suggesting a release of the payload. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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11 pages, 5035 KiB

Open AccessArticle

Hydrogen and Water Bonding between Glycosaminoglycans and Phospholipids in the Synovial Fluid: Molecular Dynamics Study

by Piotr Bełdowski, Adam Mazurkiewicz, Tomasz Topoliński and Tomasz Małek

Materials 2019, 12(13), 2060; https://0-doi-org.brum.beds.ac.uk/10.3390/ma12132060 - 27 Jun 2019

Cited by 11 | Viewed by 4115

Abstract

Synovial fluid is a lubricant of the synovial joint that shows remarkable tribological properties. These properties originate in the synergy between its components, with two of its major components, glycosaminoglycans (GAGs) and phospholipids (PLs), playing a major role in boundary and mixed lubrication regimes. All-atom molecular dynamic simulations were performed to investigate the way these components bond. Hyaluronic acid (HA) and chondroitin sulphate (CS) bonding with three types of lipids was tested. The results show that both glycosaminoglycans bind lipids at a similar rate, except for 1,2-d-ipalmitoyl-sn-glycero-3-phosphoethanolamine lipids, which bind to chondroitin at a much higher rate than to hyaluronan. The results suggest that different synovial fluid lipids may play a different role when binding to both hyaluronan and chondroitin sulphate. The presented results may help in understanding a process of lubrication of articular cartilage at a nanoscale level. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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15 pages, 2447 KiB

Open AccessFeature PaperArticle

Enzyme-Catalyzed Production of Potato Galactan-Oligosaccharides and Its Optimization by Response Surface Methodology

by Mirian Angelene González-Ayón, Ángel Licea-Claveríe, José Benigno Valdez-Torres, Lorenzo A. Picos-Corrales, Rosabel Vélez-de la Rocha, Juan Carlos Contreras-Esquivel, John M. Labavitch and Josefa Adriana Sañudo-Barajas

Materials 2019, 12(9), 1465; https://0-doi-org.brum.beds.ac.uk/10.3390/ma12091465 - 07 May 2019

Cited by 4 | Viewed by 2909

Abstract

This work shows an optimized enzymatic hydrolysis of high molecular weight potato galactan yielding pectic galactan-oligosaccharides (PGOs), where endo-β-1,4-galactanase (galactanase) from Cellvibrio japonicus and Clostridium thermocellum was used. For this, response surface methodology (RSM) by central composite design (CCD) was applied. The parameters varied were temperature (°C), pH, incubation time (min), and enzyme/substrate ratio (U/mg). The optimized conditions for the production of low degree of polymerization (DP) PGOs were obtained for each enzyme by spectrophotometric assay and confirmed by chromatography. The optimal conditions predicted for the use of C. japonicus galactanase to obtain PGOs of DP = 2 were T = 51.8 °C, pH 5, E/S = 0.508 U/mg, and t = 77.5 min. For DP = 3, they were T = 21 °C, pH 9, E/S = 0.484 U/mg, and t = 12.5 min; and for DP = 4, they were T = 21 °C, pH 5, E/S = 0.462 U/mg, and t = 12.5 min. The efficiency results were 51.3% for substrate hydrolysis. C. thermocellum galactanase had a lower yield (35.7%) and optimized conditions predicted for PGOs of DP = 2 were T = 60 °C, pH 5, E/S = 0.525 U/mg, and time = 148 min; DP = 3 were T = 59.7 °C, pH 5, E/S = 0.506 U/mg, and time = 12.5 min; and DP = 4, were T = 34.5 °C, pH 11, E/S = 0.525 U/mg, and time = 222.5 min. Fourier transformed infrared (FT-IR) and nuclear magnetic resonance (NMR) characterizations of PGOs are presented. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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8 pages, 2192 KiB

Open AccessCommunication

Freeform Perfusable Microfluidics Embedded in Hydrogel Matrices

by Gabriela Štumberger and Boštjan Vihar

Materials 2018, 11(12), 2529; https://0-doi-org.brum.beds.ac.uk/10.3390/ma11122529 - 12 Dec 2018

Cited by 26 | Viewed by 4132

Abstract

We report a modification of the freeform reversible embedding of suspended hydrogels (FRESH) 3D printing method for the fabrication of freeform perfusable microfluidics inside a hydrogel matrix. Xanthan gum is deposited into a CaCl₂ infused gelatine slurry to form filaments, which are consequently rinsed to produce hollow channels. This provides a simple method for rapid prototyping of microfluidic devices based on biopolymers and potentially a new approach to the construction of vascular grafts for tissue engineering. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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13 pages, 2488 KiB

Open AccessArticle

Deposition of Cellulose-Based Thin Films on Flexible Substrates

by Werner Schlemmer, Armin Zankel, Katrin Niegelhell, Mathias Hobisch, Michael Süssenbacher, Krisztina Zajki-Zechmeister, Michael Weissl, David Reishofer, Harald Plank and Stefan Spirk

Materials 2018, 11(12), 2433; https://0-doi-org.brum.beds.ac.uk/10.3390/ma11122433 - 30 Nov 2018

Cited by 7 | Viewed by 4075

Abstract

This study investigates flexible (polyamide 6.6 PA-6.6, polyethylene terephthalate PET, Cu, Al, and Ni foils) and, for comparison, stiff substrates (silicon wafers and glass) differing in, for example, in surface free energy and surface roughness and their ability to host cellulose-based thin films. Trimethylsilyl cellulose (TMSC), a hydrophobic acid-labile cellulose derivative, was deposited on these substrates and subjected to spin coating. For all the synthetic polymer and metal substrates, rather homogenous films were obtained, where the thickness and the roughness of the films correlated with the substrate roughness and its surface free energy. A particular case was the TMSC layer on the copper foil, which exhibited superhydrophobicity caused by the microstructuring of the copper substrate. After the investigation of TMSC film formation, the conversion to cellulose using acidic vapors of HCl was attempted. While for the polymer foils, as well as for glass and silicon, rather homogenous and smooth cellulose films were obtained, for the metal foils, there is a competing reaction between the formation of metal chlorides and the generation of cellulose. We observed particles corresponding to the metal chlorides, while we could not detect any cellulose thin films after HCl treatment of the metal foils as proven by cross-section imaging using scanning electron microscopy (SEM). Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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12 pages, 2339 KiB

Open AccessArticle

Preparation of Renewable Bio-Polyols from Two Species of Colliguaja for Rigid Polyurethane Foams

by Diana Abril-Milán, Oscar Valdés, Yaneris Mirabal-Gallardo, Alexander F. de la Torre, Carlos Bustamante and Jorge Contreras

Materials 2018, 11(11), 2244; https://0-doi-org.brum.beds.ac.uk/10.3390/ma11112244 - 11 Nov 2018

Cited by 15 | Viewed by 3491

Abstract

In this study, we investigated the potential of two non-edible oil extracts from seeds of Colliguaja integerrima (CIO) and Colliguaja salicifolia (CSO) to use as a renewable source for polyols and, eventually, polyurethane foams or biodiesel. For this purpose, two novel polyols from the aforementioned oils were obtained in a one-single step reaction using a mixture of hydrogen peroxide and acetic acid. The polyol derivatives obtained from the two studied oils were characterized by spectral (FTIR, ¹H NMR, and ¹³C NMR), physicochemical (e.g., chromatographic analysis, acid value, oxidizability values, iodine value, peroxide value, saponification number, kinematic viscosity, density, theorical molecular weight, hydroxyl number, and hydroxyl functionality) and thermal (TGA) analyses according to standard methods. Physicochemical results revealed that all parameters, with the exception of the iodine value, were higher for bio-polyols (CSP and CIP) compared to the starting oils. The NMR, TGA, and FTIR analyses demonstrated the formation of polyols. Finally, the OH functionality values for CIP and CSP were 4.50 and 5.00, respectively. This result indicated the possible used of CIP and CSP as a raw material for the preparation of polyurethane rigid foams. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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22 pages, 3592 KiB

Open AccessFeature PaperReview

Neurosurgical Approaches to Brain Tissue Harvesting for the Establishment of Cell Cultures in Neural Experimental Cell Models

by Lidija Gradišnik, Roman Bošnjak, Gorazd Bunc, Janez Ravnik, Tina Maver and Tomaž Velnar

Materials 2021, 14(22), 6857; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14226857 - 13 Nov 2021

Cited by 3 | Viewed by 1810

Abstract

In recent decades, cell biology has made rapid progress. Cell isolation and cultivation techniques, supported by modern laboratory procedures and experimental capabilities, provide a wide range of opportunities for in vitro research to study physiological and pathophysiological processes in health and disease. They can also be used very efficiently for the analysis of biomaterials. Before a new biomaterial is ready for implantation into tissues and widespread use in clinical practice, it must be extensively tested. Experimental cell models, which are a suitable testing ground and the first line of empirical exploration of new biomaterials, must contain suitable cells that form the basis of biomaterial testing. To isolate a stable and suitable cell culture, many steps are required. The first and one of the most important steps is the collection of donor tissue, usually during a surgical procedure. Thus, the collection is the foundation for the success of cell isolation. This article explains the sources and neurosurgical procedures for obtaining brain tissue samples for cell isolation techniques, which are essential for biomaterial testing procedures. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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19 pages, 3458 KiB

Open AccessReview

Recent Advancements in 3D Printing of Polysaccharide Hydrogels in Cartilage Tissue Engineering

by Jakob Naranda, Matej Bračič, Matjaž Vogrin and Uroš Maver

Materials 2021, 14(14), 3977; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14143977 - 16 Jul 2021

Cited by 32 | Viewed by 4121

Abstract

The application of hydrogels coupled with 3-dimensional (3D) printing technologies represents a modern concept in scaffold development in cartilage tissue engineering (CTE). Hydrogels based on natural biomaterials are extensively used for this purpose. This is mainly due to their excellent biocompatibility, inherent bioactivity, and special microstructure that supports tissue regeneration. The use of natural biomaterials, especially polysaccharides and proteins, represents an attractive strategy towards scaffold formation as they mimic the structure of extracellular matrix (ECM) and guide cell growth, proliferation, and phenotype preservation. Polysaccharide-based hydrogels, such as alginate, agarose, chitosan, cellulose, hyaluronan, and dextran, are distinctive scaffold materials with advantageous properties, low cytotoxicity, and tunable functionality. These superior properties can be further complemented with various proteins (e.g., collagen, gelatin, fibroin), forming novel base formulations termed “proteo-saccharides” to improve the scaffold’s physiological signaling and mechanical strength. This review highlights the significance of 3D bioprinted scaffolds of natural-based hydrogels used in CTE. Further, the printability and bioink formation of the proteo-saccharides-based hydrogels have also been discussed, including the possible clinical translation of such materials. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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19 pages, 2645 KiB

Open AccessReview

Advanced Bio-Based Polymers for Astrocyte Cell Models

by Lidija Gradišnik, Roman Bošnjak, Tina Maver and Tomaž Velnar

Materials 2021, 14(13), 3664; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14133664 - 30 Jun 2021

Cited by 6 | Viewed by 2278

Abstract

The development of in vitro neural tissue analogs is of great interest for many biomedical engineering applications, including the tissue engineering of neural interfaces, treatment of neurodegenerative diseases, and in vitro evaluation of cell–material interactions. Since astrocytes play a crucial role in the regenerative processes of the central nervous system, the development of biomaterials that interact favorably with astrocytes is of great research interest. The sources of human astrocytes, suitable natural biomaterials, guidance scaffolds, and ligand patterned surfaces are discussed in the article. New findings in this field are essential for the future treatment of spinal cord and brain injuries. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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24 pages, 5387 KiB

Open AccessReview

Chemical Synthesis of Silk-Mimetic Polymers

by Amrita Sarkar, Alexander J. Connor, Mattheos Koffas and R. Helen Zha

Materials 2019, 12(24), 4086; https://0-doi-org.brum.beds.ac.uk/10.3390/ma12244086 - 06 Dec 2019

Cited by 13 | Viewed by 5592

Abstract

Silk is a naturally occurring high-performance material that can surpass man-made polymers in toughness and strength. The remarkable mechanical properties of silk result from the primary sequence of silk fibroin, which bears semblance to a linear segmented copolymer with alternating rigid (“crystalline”) and flexible (“amorphous”) blocks. Silk-mimetic polymers are therefore of great emerging interest, as they can potentially exhibit the advantageous features of natural silk while possessing synthetic flexibility as well as non-natural compositions. This review describes the relationships between primary sequence and material properties in natural silk fibroin and furthermore discusses chemical approaches towards the synthesis of silk-mimetic polymers. In particular, step-growth polymerization, controlled radical polymerization, and copolymerization with naturally derived silk fibroin are presented as strategies for synthesizing silk-mimetic polymers with varying molecular weights and degrees of sequence control. Strategies for improving macromolecular solubility during polymerization are also highlighted. Lastly, the relationships between synthetic approach, supramolecular structure, and bulk material properties are explored in this review, with the aim of providing an informative perspective on the challenges facing chemical synthesis of silk-mimetic polymers with desirable properties. Full article

(This article belongs to the Special Issue Advanced Bio-Based Polymers: Synthesis, Characterization and Applications)

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