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Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry

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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 (20 September 2021) | Viewed by 23241

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Dr. Bozena Tyliszczak

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Institute of Materials Science, Cracow University of Technology, Krakow, Poland
Interests: biomaterials; advanced materials; biodegradable polymers; biomimetic materials; nanomaterials; material science
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Dear Colleagues,

Bioactive materials are characterized by their adaptiveness to biological environments, being designed to stimulate and/or direct appropriate cellular and tissue responses or to control interactions with microbiological species. Hydrogels are a special type of bioactive materials. They are three-dimensional, hydrophilic, polymeric networks capable of absorbing large amounts of water or biological fluids.

This Special Issue “Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry” of the journal Materials will focus on biomedical hydrogels and bioactive materials, their design and development, characterization, modification/functionalization, and the application of new materials.

Potential topics include, but are not limited to, the following: biomedical hydrogels, smart hydrogels, protein and DNA hydrogels, wound dressings, bioactive polymers and gels, bioactive metals and alloys, bioactive inorganics (ceramics, glasses, and carbon-based materials), bioactive materials sourced from nature, and bioactive composites for use in human or veterinary medicine as implants, tissue-engineering scaffolds, cell/drug/gene carriers, imaging and sensing devices.

Dr. Bozena Tyliszczak
Guest Editor

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Keywords

biomedical hydrogels
smart hydrogels
protein and DNA hydrogels
crosslinked hydrogels
biodegradable hydrogels
wound dressings
contact lenses
bioactive materials
polymers
biopolymers
metallic biomaterials
composites
nanomaterials
drug discovery
drug design
biomaterials
tissue engineering
regenerative medicine
biofabrication and bioprinting

Published Papers (10 papers)

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Research

11 pages, 1909 KiB

Open AccessArticle

CuO Bionanocomposite with Enhanced Stability and Antibacterial Activity against Extended-Spectrum Beta-Lactamase Strains

by Hina Qamar, Adil Saeed, Mohammad Owais, Touseef Hussain, Kashif Hussain, Aziz ur Rahman, Sarfraz Ahmed, Sachin Kumar and Zulfiqar Ahmad Khan

Materials 2021, 14(21), 6336; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14216336 - 23 Oct 2021

Cited by 2 | Viewed by 1560

Abstract

Worldwide, bacterial resistance to beta-lactam antibiotics is the greatest challenge in public health care. To overcome the issue, metal-based nanoparticles were extensively used as an alternative to traditional antibiotics. However, their unstable nature limits their use. In the present study a very simple, environmentally friendly, one-pot synthesis method that avoids the use of organic solvents has been proposed to design stable, novel nanocomposites. Formulation was done by mixing biogenic copper oxide (CuO) nanomaterial with glycerol and phospholipids isolated from egg yolk in an appropriate ratio at optimum conditions. Characterization was done using dynamic light scattering DLS, Zeta potential, high performance liquid chromatography (HPLC), and transmission electron microscopy (TEM). Further, its antibacterial activity was evaluated against the extended-spectrum beta-lactamase strains based on zone of inhibition and minimal inhibitory concentration (MIC) indices. Results from this study have demonstrated the formulation of stable nanocomposites with a zeta potential of 34.9 mV. TEM results indicated clear dispersed particles with an average of 59.3 ± 5 nm size. Furthermore, HPLC analysis of the egg yolk extract exhibits the presence of phospholipids in the sample and has significance in terms of stability. The newly formed nanocomposite has momentous antibacterial activity with MIC 62.5 μg/mL. The results suggest that it could be a good candidate for drug delivery in terms of bactericidal therapeutic applications. Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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26 pages, 10702 KiB

Open AccessArticle

Physicochemical Characteristics of Chitosan-Based Hydrogels Containing Albumin Particles and Aloe vera Juice as Transdermal Systems Functionalized in the Viewpoint of Potential Biomedical Applications

by Sonia Kudłacik-Kramarczyk, Magdalena Głąb, Anna Drabczyk, Aleksandra Kordyka, Marcin Godzierz, Paweł S. Wróbel, Marcel Krzan, Marimuthu Uthayakumar, Magdalena Kędzierska and Bożena Tyliszczak

Materials 2021, 14(19), 5832; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14195832 - 06 Oct 2021

Cited by 13 | Viewed by 2338

Abstract

In recent years, many investigations on the development of innovative dressing materials with potential applications, e.g., for cytostatics delivery, have been performed. One of the most promising carriers is albumin, which tends to accumulate near cancer cells. Here, chitosan-based hydrogels containing albumin spheres and Aloe vera juice, designed for the treatment of skin cancers or burn wounds resulting from radiotherapy, were developed. The presence of albumin in hydrogel matrices was confirmed via Fourier transform infrared (FT-IR) and Raman spectroscopy. Albumin spheres were clearly visible in microscopic images. It was proved that the introduction of albumin into hydrogels resulted in their increased resistance to the tensile load, i.e., approximately 30% more force was needed to break such materials. Modified hydrogels showed approximately 10% more swelling ability. All hydrogels were characterized by hydrophilicity (contact angles were <90°) which may support the regeneration of epithelial cells and non-cytotoxicity towards murine fibroblasts L929 and released Aloe vera juice more effectively in an acidic environment than in a neutral one wherein spheres introduced into the hydrogel matrix extended the release time. Thus, the developed materials, due to their chemical composition and physicochemical properties, constitute promising materials with great application potential for biomedical purposes. Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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20 pages, 5715 KiB

Open AccessArticle

Multistep Chemical Processing of Crickets Leading to the Extraction of Chitosan Used for Synthesis of Polymer Drug Carriers

by Magdalena Głąb, Sonia Kudłacik-Kramarczyk, Anna Drabczyk, Martin Duarte Guigou, Agnieszka Sobczak-Kupiec, Dariusz Mierzwiński, Paweł Gajda, Janusz Walter and Bożena Tyliszczak

Materials 2021, 14(17), 5070; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14175070 - 04 Sep 2021

Cited by 3 | Viewed by 1974

Abstract

Chitosan belongs to the group of biopolymers with increasing range of potential applications therefore searching for new raw materials as well as new techniques of obtaining of this polysaccharide are currently a subject of interest of many scientists. Presented manuscript describes preparation of chitosan from crickets. Obtainment of final product required a number of processes aimed at removal of undesirable substances such as waxes, mineral salts, proteins or pigments from above-mentioned insects. Chemical structure of fractions obtained after each step was compared with the structure of commercial chitosan by means of techniques such as X-ray diffraction and FT-IR spectroscopy. Final product was subsequently used for preparation of polymer capsules that were modified with active substance characterized by antibacterial and anticancer activity—nisin. Next, sorption capacity of obtained materials was evaluated as well as a release profile of active substance in different environments. Based on the conducted research it can be concluded that crickets constitute an alternative for shellfish and other conventional sources of chitosan. Furthermore, obtained capsules on the basis of such prepared chitosan can be considered as drug delivery systems which efficiency of release of active substance is bigger in alkaline environments. Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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18 pages, 4401 KiB

Open AccessArticle

Starch Solutions Prepared under Different Conditions as Modifiers of Chitosan/Poly(aspartic acid)-Based Hydrogels

by Magdalena Głąb, Anna Drabczyk, Sonia Kudłacik-Kramarczyk, Martin Duarte Guigou, Agnieszka Makara, Paweł Gajda, Josef Jampilek and Bożena Tyliszczak

Materials 2021, 14(16), 4443; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14164443 - 08 Aug 2021

Cited by 2 | Viewed by 1847

Abstract

Recently, there has been great interest in the application of polysaccharides in the preparation of diverse biomaterials which result from their biocompatibility, biodegradability and biological activity. In this work, the investigations on chitosan/poly(aspartic acid)-based hydrogels modified with starch were described. Firstly, a series of hydrogel matrices was prepared and investigated to characterize their swelling properties, structure via FT-IR spectroscopy, elasticity and tensile strength using the Brookfield texture analyzer as well as their impact on simulated physiological liquids. Hydrogels consisting of chitosan and poly(aspartic acid) in a 2:1 volume ratio were elastic (9% elongation), did not degrade after 30-day incubation in simulated physiological liquids, exhibited a relative biocompatibility towards these liquids and similar swelling in each absorbed medium. This hydrogel matrix was modified with starch wherein two of its form were applied—a solution obtained at an elevated temperature and a suspension obtained at room temperature. Hydrogels modified with hot starch solution showed higher sorption that unmodified materials. This was probably due to the higher starch inclusion (i.e., a larger number of hydrophilic groups able to interact with the adsorbed liquid) when this polysaccharide was given in the form of a hot solution. Hydrogels modified with a cold starch suspension had visible heterogeneous inequalities on their surfaces and this modification led to the obtainment materials with unrepeatable structures which made the analysis of their properties difficult and may have led to misleading conclusions. Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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18 pages, 3947 KiB

Open AccessArticle

The Development of the Innovative Synthesis Methodology of Albumin Nanoparticles Supported by Their Physicochemical, Cytotoxic and Hemolytic Evaluation

by Sonia Kudłacik-Kramarczyk, Anna Drabczyk, Magdalena Głąb, Paweł Gajda, Anna Czopek, Agnieszka Zagórska, Anna Jaromin, Jerzy Gubernator, Agnieszka Makara and Bożena Tyliszczak

Materials 2021, 14(16), 4386; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14164386 - 05 Aug 2021

Cited by 6 | Viewed by 1811

Abstract

Many studies are being performed to develop effective carriers for controlled cytostatic delivery wherein albumin is a promising material due to its tendency to accumulate near cancer cells. The novelty of this work involves the development of the synthesis methodology of albumin nanoparticles and their biological and physicochemical evaluation. Albumin particles were obtained via the salt-induced precipitation and K₃PO₄ was used as a salting-out agent. Various concentrations of protein and salting-out agent solutions were mixed using a burette or a syringe system. It was proved that the size of the particles depended on the concentrations of the reagents and the methodology applied. As a result of a process performed using a burette and 2 M K₃PO₄, albumin spheres having a size 5–25 nm were obtained. The size of nanospheres and their spherical shape was confirmed via TEM analysis. The use of a syringe system led to preparation of particles of large polydispersity. The highest albumin concentration allowing for synthesis of homogeneous particles was 2 g/L. The presence of albumin in spheres was confirmed via the FT-IR technique and UV-Vis spectroscopy. All samples showed no cytotoxicity towards normal human dermal fibroblasts and no hemolytic properties against human erythrocytes (the hemolysis did not exceed 2.5%). Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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20 pages, 6323 KiB

Open AccessArticle

Synthesis and Physicochemical Evaluation of Bees’ Chitosan-Based Hydrogels Modified with Yellow Tea Extract

by Sonia Kudłacik-Kramarczyk, Anna Drabczyk, Magdalena Głąb, Paweł Gajda, Anna Jaromin, Anna Czopek, Agnieszka Zagórska and Bożena Tyliszczak

Materials 2021, 14(12), 3379; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14123379 - 18 Jun 2021

Cited by 3 | Viewed by 1989

Abstract

The novelty of the research involves designing the measurement methodology aimed at determining the structure–property relationships in the chitosan-based hydrogels containing yellow tea extract. Performed investigations allowed us to determine the swelling properties of hydrogels in selected time intervals, evaluate the mutual interactions between the hydrogels and simulated physiological liquids via pH measurements and directly assess the impact of such interactions on the chemical structure of hydrogels using Fourier transform infrared (FT-IR) spectroscopy and their wettability by the measurements of the flatness of the drop on the surface of the tested samples via the static drop method. Next, the surface morphology of hydrogels was characterized by the Scanning Electron Miscorcopy (SEM) and their elasticity under the tension applied was also verified. It was proved that incubation in simulated physiological liquids resulted in a decrease in contact angles of hydrogels, even by 60%. This also caused their certain degradation which was reflected in lower intensities of bands on FT-IR spectra. Further, 23% v/v yellow tea extract in hydrogel matrices caused the decrease of their tensile strength. An increase in the amount of the crosslinker resulted in a decrease in the sorption capacity of hydrogels wherein their modification caused greater swelling ability. In general, the investigations performed provided much information on the tested materials which may be meaningful considering their application, e.g., as dressing materials. Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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17 pages, 18955 KiB

Open AccessFeature PaperArticle

Formation and Investigation of Physicochemical, Biological and Bacteriostatic Properties of Nanocomposite Foils Containing Silver Nanoparticles and Graphene Oxide in Hyaluronic Acid Matrix

by Karen Khachatryan, Lusine Khachatryan, Marcel Krzan, Magdalena Krystyjan, Lidia Krzemińska-Fiedorowicz, Anna Lenart-Boroń, Aneta Koronowicz, Mariola Drozdowska and Gohar Khachatryan

Materials 2021, 14(12), 3377; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14123377 - 18 Jun 2021

Cited by 8 | Viewed by 2282

Abstract

Natural polysaccharides, including hyaluronic acid, find a wide range of applications in biomedical sciences. There is a growing interest in nanocomposites containing hyaluronic acid and nanoparticles such as nanometals or graphene. In this study, we prepared foils of pure sodium hyaluronate and sodium hyaluronate containing nanosilver, graphene oxide, nanosilver/graphene oxide and characterized their properties. UV-vis spectroscopy and scanning electron microscopy (SEM) confirmed the formation of 10–20 nm silver nanoparticles. The structural changes were investigated using Fourier transforms infrared (FTIR) spectra and size exclusion chromatography. The obtained results suggest changes in molecular weights in the samples containing nanoparticles, which was highest in a sample containing nanosilver/graphene oxide. We also assessed the mechanical properties of the foils (thickness, tensile strength and elongation at break) and their wettability. The foils containing nanosilver and nanosilver/graphene oxide presented bacteriostatic activity against E. coli, Staphylococcus spp. and Bacillus spp., which was not observed in the control and sample containing graphene oxide. The composites containing graphene oxide and nanosilver/graphene oxide exhibited a cytotoxic effect on human melanoma WM266-4 cell lines (ATCC, Manassas, VA, USA). Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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17 pages, 3175 KiB

Open AccessArticle

Curdlan-Based Hydrogels for Potential Application as Dressings for Promotion of Skin Wound Healing—Preliminary In Vitro Studies

by Aleksandra Nurzynska, Katarzyna Klimek, Krzysztof Palka, Łukasz Szajnecki and Grazyna Ginalska

Materials 2021, 14(9), 2344; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14092344 - 30 Apr 2021

Cited by 23 | Viewed by 2523

Abstract

The aim of this work was to establish whether novel curdlan-based hydrogels enriched with Ca²⁺ ions may be considered as potential candidates for dressings, for the acceleration of skin wound healing. Firstly, biomaterials were allocated for evaluation of structural and mechanical properties. Subsequently, the ability of hydrogels to absorb simulated wound fluid and water vapor permeability, as well their capacity to release calcium ions, was evaluated. The biocompatibility of biomaterials was assessed using normal human skin fibroblasts. Importantly, the main features of the obtained curdlan-based hydrogels were compared with those of KALTOSTAT^® (a commercial calcium sodium alginate wound dressing). The obtained results showed that curdlan-based biomaterials possessed a mesoporous structure (pore diameter ranged from 14–48 nm) and exhibited a good ability to absorb simulated wound fluid (swelling ratio close to 974–1229%). Moreover, in a wet state, they enabled proper water vapor transmission rate (>2000 g/m²/day), thanks to their hydrogel structure. Finally, it was found that biomaterial composed of 11 wt.% of curdlan (Cur_11%) possessed the most desirable biological properties in vitro. It released a beneficial amount of calcium ions to the aqueous environment (approximately 6.12 mM), which significantly enhanced fibroblast viability and proliferation. Taking into account the beneficial properties of Cur_11% biomaterial, it seems justified to subject it to more advanced cell culture experiments in vitro and to in vivo studies in order to determine its precise influence on skin wound healing. Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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14 pages, 5235 KiB

Open AccessArticle

Preparation of a Fucoidan-Grafted Hyaluronan Composite Hydrogel for the Induction of Osteoblast Differentiation in Osteoblast-Like Cells

by Fu-Yin Hsu, Jheng-Jie Chen, Wen-Chieh Sung and Pai-An Hwang

Materials 2021, 14(5), 1168; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14051168 - 02 Mar 2021

Cited by 12 | Viewed by 2088

Abstract

A suitable bone substitute is necessary in bone regenerative medicine. Hyaluronan (HA) has excellent biocompatibility and biodegradability and is widely used in tissue engineering. Additionally, research on fucoidan (Fu), a fucose- and sulfate-rich polysaccharide from brown seaweed, for the promotion of bone osteogenic differentiation has increased exponentially. In this study, HA and Fu were functionalized by grafting methacrylic groups onto the backbone of the chain. Methacrylate-hyaluronan (MHA) and methacrylate-fucoidan (MFu) were characterized by FTIR and ¹H NMR spectroscopy to confirm functionalization. The degrees of methacrylation (DMs) of MHA and MFu were 9.2% and 98.6%, respectively. Furthermore, we evaluated the mechanical properties of the hydrogels formed from mixtures of photo-crosslinkable MHA (1%) with varying concentrations of MFu (0%, 0.5%, and 1%). There were no changes in the hardness values of the hydrogels, but the elastic modulus decreased upon the addition of MFu, and these mechanical properties were not significantly different with or without preosteoblastic MG63 cell culture for up to 28 days. Furthermore, the cell morphologies and viabilities were not significantly different after culture with the MHA, MHA-MFu0.5, or MHA-MFu1.0 hydrogels, but the specific activity and mineralization of alkaline phosphatase (ALP) were significantly higher in the MHA-MFu1.0 hydrogel group compared to the other hydrogels. Hence, MHA-MFu composite hydrogels are potential bone graft materials that can provide a flexible structure and favorable niche for inducing bone osteogenic differentiation. Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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19 pages, 4318 KiB

Open AccessArticle

Evaluation of the In Vitro Cytotoxic Activity of Caffeic Acid Derivatives and Liposomal Formulation against Pancreatic Cancer Cell Lines

by Magdalena Zaremba-Czogalla, Anna Jaromin, Katarzyna Sidoryk, Agnieszka Zagórska, Marcin Cybulski and Jerzy Gubernator

Materials 2020, 13(24), 5813; https://0-doi-org.brum.beds.ac.uk/10.3390/ma13245813 - 19 Dec 2020

Cited by 14 | Viewed by 2971

Abstract

Pancreatic cancer belongs to the most aggressive group of cancers, with very poor prognosis. Therefore, there is an important need to find more potent drugs that could deliver an improved therapeutic approach. In the current study we searched for selective and effective caffeic acid derivatives. For this purpose, we analyzed twelve compounds and evaluated their in vitro cytotoxic activity against two human pancreatic cancer cell lines, along with a control, normal fibroblast cell line, by the classic MTT assay. Six out of twelve tested caffeic acid derivatives showed a desirable effect. To improve the therapeutic efficacy of such active compounds, we developed a formulation where caffeic acid derivative (7) was encapsulated into liposomes composed of soybean phosphatidylcholine and DSPE-PEG₂₀₀₀. Subsequently, we analyzed the properties of this formulation in terms of basic physical parameters (such as size, zeta potential, stability at 4 °C and morphology), hemolytic and cytotoxic activity and cellular uptake. Overall, the liposomal formulation was found to be stable, non-hemolytic and had activity against pancreatic cancer cells (IC₅₀ 19.44 µM and 24.3 µM, towards AsPC1 and BxPC3 cells, respectively) with less toxicity against normal fibroblasts. This could represent a promising alternative to currently available treatment options. Full article

(This article belongs to the Special Issue Advanced Biomedical Hydrogels and Bioactive Materials in Medicinal Chemistry)

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