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Intrinsically Biocompatible Polymer Systems II

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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 (20 November 2021) | Viewed by 32472

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Prof. Dr. Marek M. Kowalczuk

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1. Wolverhampton School of Biology, Chemistry and Forensic Science, Faculty of Science and Engineering, University of Wolverhampton, Wolverhampton WV1 1LY, UK
2. Centre of Polymer and Carbon Materials, Polish Academy of Sciences, 41-800 Zabrze, Poland
Interests: biocompatible and biodegradable polymer systems; polymer mass spectrometry; bioactive oligomers; controlled drug delivery systems; ring-opening polymerization; forensic engineering of advanced polymeric materials
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Dr. Abhishek Gupta

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School of Allied Health and Midwifery, Faculty of Education, Health and Wellbeing, University of Wolverhampton, Walsall, UK
Interests: biopolymers; wound management; hydrogels; nanotechnology; natural healing agents
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Special Issue Information

Dear Colleagues,

The definition of biocompatibility was redefined ten years ago as follows: “Biocompatibility refers to the ability of a biomaterial to perform its desired function with respect to a medical therapy, without eliciting any undesirable local or systemic effects in the recipient or beneficiary of that therapy, but generating the most appropriate beneficial cellular or tissue response in that specific situation, and optimising the clinically relevant performance of that therapy,” which reflects current developments in the area of intrinsically biocompatible polymer systems. Polymeric biomaterials are presently used as, e.g., long-term implantable medical devices, degradable implantable systems, transient invasive intravascular devices, and, recently, as tissue engineering scaffolds.

The biosafety of polymeric biomaterials needs prediction, evaluation, and indication on potential complications arising from their use and on the formation of their degradation products. Thus, the methodology of forensic engineering of advanced polymeric materials is currently being developed in the area of polymeric biomaterials.

This Special Issue welcomes full papers and short communications highlighting the aspects of the current trends in the area of intrinsically biocompatible polymer systems.

Prof. Dr. Marek M. Kowalczuk
Dr. Abhishek Gupta
Guest Editor

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Keywords

Structure–property relationships of biocompatible polymer system
Characterization of polymeric biomaterials
Biodegradable polymers for medical applications
Biosafety of polymeric biomaterials
3D polymeric scaffolds

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Intrinsically Biocompatible Polymer Systems in Polymers (16 articles)

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Research

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17 pages, 33931 KiB

Open AccessArticle

Biocompatible Hydrogel for Intra-Articular Implantation Comprising Cationic and Anionic Polymers of Natural Origin: In Vivo Evaluation in a Rabbit Model

by Karina L. Bierbrauer, Roxana V. Alasino, Fernando E. Barclay, Eduardo M. Belotti, Hugo H. Ortega and Dante M. Beltramo

Polymers 2021, 13(24), 4426; https://doi.org/10.3390/polym13244426 - 16 Dec 2021

Cited by 3 | Viewed by 2727

Abstract

We describe the functional capability of a cross-linked hydrogel composed of sulfated glycosaminoglycans and a cationic cellulose by conducting trials on experimental animal models using intra-articular implants to treat an articular disease called osteoarthritis. Forty-eight mature New Zealand white rabbits were divided into three experimental groups: A, B, and C. Group A and B underwent unilateral anterior cruciate ligament transection (ACLT) of the right knee. Subsequently, both knees of group A were treated with the injectable formulation under study. Meanwhile, group B was treated with sterile PBS (placebo). The animals of group C were surgically operated in both knees: Commercial hyaluronic acid (HA) was implanted in the left knee, and the formulation under study was implanted in the right knee. After implantation, all specimens underwent several evaluations at 3, 6, and 12 months postoperatively. At 6 months, no significant differences were detected between the right and left knees of the different groups. However, significant differences were observed between both knees at 12 months in group C, with less cartilage damage in the right knees implanted with our hydrogel. Therefore, in vivo studies have demonstrated hydrogel safety, superior permanence, and less cartilage damage for long-term follow up 12 months after implantation for the formulation under study compared with commercial HA. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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22 pages, 4776 KiB

Open AccessArticle

Biomedical PEVA Nanocomposite with Dual Clay Nanofiller: Cytotoxicity, Mechanical Properties, and Biostability

by Tuty Fareyhynn Mohammed Fitri, Azlin Fazlina Osman, Eid M. Alosime, Rahimah Othman, Fatimah Hashim and Mohd Aidil Adhha Abdullah

Polymers 2021, 13(24), 4345; https://doi.org/10.3390/polym13244345 - 12 Dec 2021

Cited by 4 | Viewed by 2970

Abstract

Poly(ethylene-vinyl acetate) (PEVA) nanocomposite incorporating dual clay nanofiller (DCN) of surface modified montmorillonite (S-MMT) and bentonite (Bent) was studied for biomedical applications. In order to overcome agglomeration of the DCN, the S-MMT and Bent were subjected to a physical treatment prior to being mixed with the copolymer to form nanocomposite material. The S-MMT and Bent were physically treated to become S-MMT(P) and Bent(pH-s), respectively, that could be more readily dispersed in the copolymer matrix due to increments in their basal spacing and loosening of their tactoid structure. The biocompatibility of both nanofillers was assessed through a fibroblast cell cytotoxicity assay. The mechanical properties of the neat PEVA, PEVA nanocomposites, and PEVA-DCN nanocomposites were evaluated using a tensile test for determining the best S-MMT(P):Bent(pH-s) ratio. The results were supported by morphological studies by transmission electron microscopy (TEM) and scanning electron microscopy (SEM). Biostability evaluation of the samples was conducted by comparing the ambient tensile test data with the in vitro tensile test data (after being immersed in simulated body fluid at 37 °C for 3 months). The results were supported by surface degradation analysis. Our results indicate that the cytotoxicity level of both nanofillers reduced upon the physical treatment process, making them safe to be used in low concentration as dual nanofillers in the PEVA-DCN nanocomposite. The results of tensile testing, SEM, and TEM proved that the ratio of 4:1 (S-MMT(P):Bent(pH-s)) provides a greater enhancement in the mechanical properties of the PEVA matrix. The biostability assessment indicated that the PEVA-DCN nanocomposite can achieve much better retention in tensile strength after being subjected to the simulated physiological fluid for 3 months with less surface degradation effect. These findings signify the potential of the S-MMT(P)/Bent(pH-s) as a reinforcing DCN, with simultaneous function as biostabilizing agent to the PEVA copolymer for implant application. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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19 pages, 3289 KiB

Open AccessArticle

Cellulosic/Polyvinyl Alcohol Composite Hydrogel: Synthesis, Characterization and Applications in Tissue Engineering

by Mathilde Stricher, Claude-Olivier Sarde, Erwann Guénin, Christophe Egles and Frédéric Delbecq

Polymers 2021, 13(20), 3598; https://doi.org/10.3390/polym13203598 - 19 Oct 2021

Cited by 6 | Viewed by 3767

Abstract

The biomedical field still requires composite materials for medical devices and tissue engineering model design. As part of the pursuit of non-animal and non-proteic scaffolds, we propose here a cellulose-based material. In this study, 9%, 18% and 36% dialdehyde-functionalized microcrystalline celluloses (DAC) were synthesized by sodium periodate oxidation. The latter was subsequently coupled to PVA at ratios 1:2, 1:1 and 2:1 by dissolving in N-methyl pyrrolidone and lithium chloride. Moulding and successive rehydration in ethanol and water baths formed soft hydrogels. While oxidation effectiveness was confirmed by dialdehyde content determination for all DAC, we observed increasing hydrolysis associated with particle fragmentation. Imaging, FTIR and XDR analysis highlighted an intertwined DAC/PVA network mainly supported by electrostatic interactions, hemiacetal and acetal linkage. To meet tissue engineering requirements, an interconnected porosity was optimized using 0–50 µm salts. While the role of DAC in strengthening the hydrogel was identified, the oxidation ratio of DAC showed no distinct trend. DAC 9% material exhibited the highest indirect and direct cytocompatibility creating spheroid-like structures. DAC/PVA hydrogels showed physical stability and acceptability in vivo that led us to propose our DAC 9%/PVA based material for soft tissue graft application. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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16 pages, 5511 KiB

Open AccessArticle

Influence of HRGO Nanoplatelets on Behaviour and Processing of PMMA Bone Cement for Surgery

by Jaime Orellana, Ynés Yohana Pastor, Fernando Calle and José Ygnacio Pastor

Polymers 2021, 13(12), 2027; https://doi.org/10.3390/polym13122027 - 21 Jun 2021

Cited by 8 | Viewed by 2328

Abstract

Bone cement, frequently based on poly (methyl methacrylate), is commonly used in different arthroplasty surgical procedures and its use is essential for prosthesis fixation. However, its manufacturing process reaches high temperatures (up to 120 °C), producing necrosis in the patients’ surrounding tissues. To help avoid this problem, the addition of graphene could delay the polymerisation of the methyl methacrylate as it could, simultaneously, favour the optimisation of the composite material’s properties. In this work, we address the effect of different percentages of highly reduced graphene oxide with different wt.% (0.10, 0.50, and 1.00) and surface densities (150, 300, 500, and 750 m²/g) on the physical, mechanical, and thermal properties of commercial poly (methyl methacrylate)-based bone cement and its processing. It was noted that a lower sintering temperature was achieved with this addition, making it less harmful to use in surgery and reducing its adverse effects. In contrast, the variation of the density of the materials did not introduce significant changes, which indicates that the addition of highly reduced graphene oxide would not significantly increase bone porosity. Lastly, the mechanical properties (strength, elastic modulus, and fracture toughness) were reduced by almost 20%. Nevertheless, their typical values are high enough that these new materials could still fulfil their structural function. In conclusion, this paper presents a way to control the sintering temperature, without significant degradation of the mechanical performance, by adding highly reduced graphene oxide so that local necrosis of bone cement based on poly (methyl methacrylate) used in surgery is avoided. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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11 pages, 2117 KiB

Open AccessArticle

Effect of Molecular Weight on Gelling and Viscoelastic Properties of Poly(caprolactone)–b-Poly(ethylene glycol)–b-Poly(caprolactone) (PCL–PEG–PCL) Hydrogels

by Noam Y. Steinman, Noam Y. Bentolila and Abraham J. Domb

Polymers 2020, 12(10), 2372; https://doi.org/10.3390/polym12102372 - 15 Oct 2020

Cited by 22 | Viewed by 4923

Abstract

Hydrogels based on poly(caprolactone)–b-poly(ethylene glycol)–b-poly(caprolactone) (PCL–PEG–PCL) have been evaluated extensively as potential injectable fillers or depots for controlled release of drugs. Common drawbacks of these copolymer systems include instability of aqueous solutions and low mechanical strength of gels, issues which are commonly overcome by adding pendant groups to the end of the copolymer chains. Here, a systematic study of the effects of increasing polymer molecular weight (MW) is presented, utilizing PEG blocks of MW 2, 4 or 8 kDa. Triblock copolymers were prepared by the ring-opening polymerization of Ɛ-caprolactone by PEG. Copolymers prepared with PEG MW 2 kDa did not form hydrogels at any copolymer molecular weight. Copolymers prepared with PEG MW 4 kDa formed gels at MW between 11 and 13.5 kDa, and copolymers prepared with PEG MW 8 kDa formed gels at MW between 16 and 18 kDa. Copolymers with PEG block 8 kDa formed hydrogels with high viscosity (17,000 Pa·s) and mechanical strength (G′ = 14,000 Pa). The increased gel strength afforded by increased molecular weight represents a simple modification of the reactants used in the reaction feed without added synthetic or purification steps. Shear-thinning of PCL-PEG-PCL triblock copolymer hydrogels allowed for injection through a standard 23G syringe, allowing for potential use as dermal fillers or drug delivery depots. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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11 pages, 3513 KiB

Open AccessArticle

Investigation of the Cytotoxicity of Electrospun Polysuccinimide-Based Fiber Mats

by Kristof Molnar, Rita Varga, Benjamin Jozsa, Dora Barczikai, Eniko Krisch, Krisztina S. Nagy, Gabor Varga, Angela Jedlovszky-Hajdu and Judit E. Puskas

Polymers 2020, 12(10), 2324; https://doi.org/10.3390/polym12102324 - 11 Oct 2020

Cited by 9 | Viewed by 2424

Abstract

This study investigated cell viability in the presence of allylamine-modified and plasma-treated electrospun polysuccinimide fiber mats (PSI-AAmp). Low pressure non-equilibrium plasma was used for crosslinking the PSI-AAm. Comparison of FTIR and XPS analyses demonstrated that crosslinking occurred on the surface of the samples. Cell viability was investigated using the MG-63 osteosarcoma cell line and WST-1 viability reagent. Since PSI hydrolyzes to poly(aspartic acid) (PASP), PASP was used in addition to the regular controls (cells only). Phase contrast showed normal morphology in all cases at 24 h; however, in the presence of PSI-AAmp at 72 h, some rounded, dead cells could also be seen, and proliferation was inhibited. Since proliferation in the presence of PASP alone was not inhibited, the cause of inhibition was not the final product of the hydrolysis. Further investigations will be carried out to pinpoint the cause. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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18 pages, 6156 KiB

Open AccessArticle

Production of Chitosan/Hyaluronan Complex Nanofibers. Characterization and Physical Properties as a Function of the Composition

by Christian Enrique Garcia Garcia, Félix Armando Soltero Martínez, Frédéric Bossard and Marguerite Rinaudo

Polymers 2020, 12(9), 2004; https://doi.org/10.3390/polym12092004 - 3 Sep 2020

Cited by 17 | Viewed by 2892

Abstract

In this work, optimized conditions for preparation of chitosan and hyaluronan polyelectrolyte complex are proposed. The objective was to produce new biomaterials being biocompatible and bioresorbable in the body as well as approaching the extracellular matrix (ECM) structure. These materials will be tested for chondrocyte development in tissue engineering and wound healing applications. Nanofibers made of the polyelectrolyte complex (PEC) were successfully manufactured by electrospinning, and casted films were used as a model for properties comparison. To our knowledge, it is the first time that stable chitosan/hyaluronan fibers are produced, which were observed to be long-lasting in buffer at pH~7.4. The role of thermal treatment at 120 °C for 4 h is examined to control the degree of swelling by crosslinking of the two polysaccharides by H-bonds and amide bonds formation. The properties of the materials are tested for different PEC compositions at different pH values, based on swelling and solubility degrees, diameters of nanofibers and mechanical performances. The influence of the solvent (acidic potential and composition) utilized to process biomaterials is also examined. Acid formic/water 50/50 v/v is observed to be the more appropriated solvent for the carried-out procedures. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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22 pages, 5890 KiB

Open AccessArticle

Synthesis of Poly(Dimethylmalic Acid) Homo- and Copolymers to Produce Biodegradable Nanoparticles for Drug Delivery: Cell Uptake and Biocompatibility Evaluation in Human Heparg Hepatoma Cells

by Ali Khalil, Saad Saba, Catherine Ribault, Manuel Vlach, Pascal Loyer, Olivier Coulembier and Sandrine Cammas-Marion

Polymers 2020, 12(8), 1705; https://doi.org/10.3390/polym12081705 - 29 Jul 2020

Cited by 2 | Viewed by 2638

Abstract

Hydrophobic and amphiphilic derivatives of the biocompatible and biodegradable poly(dimethylmalic acid) (PdiMeMLA), varying by the nature of the lateral chains and the length of each block, respectively, have been synthesized by anionic ring-opening polymerization (aROP) of the corresponding monomers using an initiator/base system, which allowed for very good control over the (co)polymers’ characteristics (molar masses, dispersity, nature of end-chains). Hydrophobic and core-shell nanoparticles (NPs) were then prepared by nanoprecipitation of hydrophobic homopolymers and amphiphilic block copolymers, respectively. Negatively charged NPs, showing hydrodynamic diameters (Dh) between 50 and 130 nm and narrow size distributions (0.08 < PDI < 0.22) depending on the (co)polymers nature, were obtained and characterized by dynamic light scattering (DLS), zetametry, and transmission electron microscopy (TEM). Finally, the cytotoxicity and cellular uptake of the obtained NPs were evaluated in vitro using the hepatoma HepaRG cell line. Our results showed that both cytotoxicity and cellular uptake were influenced by the nature of the (co)polymer constituting the NPs. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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Review

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21 pages, 2425 KiB

Open AccessReview

Polymeric Carriers for Delivery Systems in the Treatment of Chronic Periodontal Disease

by Magdalena Zięba, Paweł Chaber, Khadar Duale, Magdalena Martinka Maksymiak, Maciej Basczok, Marek Kowalczuk and Grazyna Adamus

Polymers 2020, 12(7), 1574; https://doi.org/10.3390/polym12071574 - 15 Jul 2020

Cited by 45 | Viewed by 6710

Abstract

Periodontitis (PD) is a chronic inflammatory disease of periodontal tissues caused by pathogenic microorganisms and characterized by disruption of the tooth-supporting structures. Conventional drug administration pathways in periodontal disease treatment have many drawbacks such as poor biodistribution, low selectivity of the therapeutic effect, burst release of the drug, and damage to healthy cells. To overcome this limitation, controlled drug delivery systems have been developed as a potential method to address oral infectious disease ailments. The use of drug delivery devices proves to be an excellent auxiliary method in improving the quality and effectiveness in periodontitis treatment, which includes inaccessible periodontal pockets. This review explores the current state of knowledge regarding the applications of various polymer-based delivery systems such as hydrogels, liposomes, micro-, and nanoparticles in the treatment of chronic periodontal disease. Furthermore, to present a more comprehensive understanding of the difficulties concerning the treatment of PD, a brief description of the mechanism and development of the disease is outlined. Full article

(This article belongs to the Special Issue Intrinsically Biocompatible Polymer Systems II)

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