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Recent Developments in Chitosan Hydrogels

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A special issue of Gels (ISSN 2310-2861). This special issue belongs to the section "Gel Chemistry and Physics".

Deadline for manuscript submissions: closed (31 March 2024) | Viewed by 24687

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Special Issue Editors

Dr. Sara Moradi

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Guest Editor

Arak University Visiting Scholar, North Carolina State University, Raleigh, NC 27606, USA
Interests: biopolymers; biomaterials; hydrogels; drug delivery; nanoemulsions

Dr. Hamid Hamedi

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Guest Editor

Department of Biomedical Engineering, The Ohio State University, Columbus, OH 43210, USA
Interests: wound dressing; smart polymer; biomedical textile; bioadhesives

Dr. Kummara Madhusudana Rao

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Guest Editor

School of Chemical Engineering, Yeungnam University, Gyeongsan 38541, Republic of Korea
Interests: polymer synthesis; hydrogels; drug delivery; wound dressing; tissue engineering; stimuli responsive gels

Special Issue Information

Dear Colleagues,

Hydrogels are three-dimensional, cross-linked networks that can absorb and retain significant amounts of water, making them an excellent candidate for biomedical applications such as soft contact lenses, tissue-engineering scaffolds, controlled drug release carriers and wound dressings. Hydrogels can be prepared from synthetic or natural polymers with a wide range of chemical compositions and different mechanical, physical and chemical properties.

Chitosan, a natural polymer derived from chitin, is a polysaccharide with excellent biocompatibility, low toxicity, immune-stimulatory activities and biodegradability, qualities that are required for medical devices. The generic term chitosan describes a range of presumably pure poly-(beta-1-4) N-acetyl-D-glucosamine materials whose properties are highly dependent on their degree of deacetylation, average molecular weight, polydispersity and structure.

Due to their unique properties, various chitosan hydrogels with desirable functionalities have been developed. This Special Issue aims to present a collection of articles covering the preparation, characterization and application of chitosan hydrogels in the biomedical field. We welcome original research articles, rapid communications and reviews for this Special Issue.

Dr. Sara Moradi
Dr. Hamid Hamedi
Dr. Kummara Madhusudana Rao
Guest Editors

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Published Papers (10 papers)

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Research

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12 pages, 4845 KiB

Open AccessArticle

Nanowire-Enhanced Fully Transparent and Flexible Indium Gallium Zinc Oxide Transistors with Chitosan Hydrogel Gate Dielectric: A Pathway to Improved Synaptic Properties

by Dong-Hee Lee, Hamin Park and Won-Ju Cho

Gels 2023, 9(12), 931; https://doi.org/10.3390/gels9120931 - 27 Nov 2023

Cited by 2 | Viewed by 1575

Abstract

In this study, a transparent and flexible synaptic transistor was fabricated based on a random-network nanowire (NW) channel made of indium gallium zinc oxide. This device employs a biocompatible chitosan-based hydrogel as an electrolytic gate dielectric. The NW structure, with its high surface-to-volume ratio, facilitated a more effective modulation of the channel conductance induced by protonic-ion polarization. A comparative analysis of the synaptic properties of NW- and film-type devices revealed the distinctive features of the NW-type configuration. In particular, the NW-type synaptic transistors exhibited a significantly larger hysteresis window under identical gate-bias conditions. Notably, these transistors demonstrated enhanced paired-pulse facilitation properties, synaptic weight modulation, and transition from short- to long-term memory. The NW-type devices displayed gradual potentiation and depression of the channel conductance and thus achieved a broader dynamic range, improved linearity, and reduced power consumption compared with their film-type counterparts. Remarkably, the NW-type synaptic transistors exhibited impressive recognition accuracy outcomes in Modified National Institute of Standards and Technology pattern-recognition simulations. This characteristic enhances the efficiency of practical artificial intelligence (AI) processes. Consequently, the proposed NW-type synaptic transistor is expected to emerge as a superior candidate for use in high-efficiency artificial neural network systems, thus making it a promising technology for next-generation AI semiconductor applications. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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16 pages, 5569 KiB

Open AccessArticle

Hydrogel Membranes from Chitosan-Fish Gelatin-Glycerol for Biomedical Applications: Chondroitin Sulfate Incorporation Effect in Membrane Properties

by Andreas Karydis-Messinis, Dimitrios Moschovas, Maria Markou, Kyriaki Tsirka, Christina Gioti, Eleni Bagli, Carol Murphy, Aris E. Giannakas, Alkis Paipetis, Michael A. Karakassides, Apostolos Avgeropoulos, Constantinos E. Salmas and Nikolaos E. Zafeiropoulos

Gels 2023, 9(11), 844; https://doi.org/10.3390/gels9110844 - 25 Oct 2023

Cited by 3 | Viewed by 2357

Abstract

Chondroitin sulfate (ChS), chitosan (Chi), and fish gelatin (FG), which are byproducts of a fish-treatment small enterprise, were incorporated with glycerol (Gly) to obtain dense hydrogel membranes with reduced brittleness, candidates for dressing in wound healing applications. The mechanical properties of all samples were studied via Dynamic Mechanical Analysis (DMA) and tensile tests while their internal structure was characterized using Attenuated Total Reflectance-Fourier Transform Infrared Spectroscopy (ATR-FTIR) and X-ray Diffraction (XRD) instruments. Their surface morphology was analyzed by ThermoGravimetric Analysis (TGA) method, while their water permeability was estimated via Water Vapor Transmission Rate (WVTR) measurements. Wettability and degradation rate measurements were also carried out. Characterization results indicated that secondary interactions between the natural polymers and the plasticizer create the hydrogel membranes. The samples were amorphous due to the high concentration of plasticizer and the amorphous nature of the natural polymers. The integration of ChS led to decreased decomposition temperature in comparison with the glycerol-free sample, and all the materials had dense structures. Finally, the in vitro endothelial cell attachment studies indicate that the hydrogel membranes successfully support the attachment and survival of primary on the hydrogel membranes and could be appropriate for external application in wound healing applications as dressings. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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15 pages, 2776 KiB

Open AccessArticle

Chitosan Hydrogels Crosslinked with Oxidized Sucrose for Antimicrobial Applications

by Sayaka Fujita, Hijiri Takeda, Junki Noda, Haruki Wakamori and Hiroyuki Kono

Gels 2023, 9(10), 786; https://doi.org/10.3390/gels9100786 - 29 Sep 2023

Cited by 1 | Viewed by 1912

Abstract

Oxidized sucrose (OS) reacts with amino-group-containing polysaccharides, including chitosan, without catalyst, resulting in hydrogels entirely composed of carbohydrates. The presence of imine bonds with low structural stabilities and unreacted aldehydes in the structures of these hydrogels hinder their application as biomaterials. Therefore, herein, the chitosan hydrogels (CTSGs) obtained after the crosslinking of chitosan with OS were reduced using sodium borohydride to convert imine bonds to secondary amines and aldehydes to alcohols. The structures of CTSGs were comprehensively characterized using Fourier transform infrared and ¹³C nuclear magnetic resonance spectroscopies, and the results implied that the degree of crosslinking (CR) depended on the OS feed amount used during CTSG preparation. The properties of CTSGs were significantly dependent on CR; with an increase in CR, the thermal stabilities and dynamic moduli of CTSGs increased, whereas their swelling properties decreased. CTSGs exhibited antimicrobial properties against the gram-negative bacterium Escherichia coli, and their performances were also dependent on CR. The results indicated the potentials of CTSGs completely based on carbohydrates as antimicrobial hydrogels for various medical and pharmaceutical applications. We believe that this study will contribute to the development of hydrogels for application in the food, medical, and pharmaceutical fields. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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17 pages, 19564 KiB

Open AccessArticle

Thymol@Natural Zeolite Nanohybrids for Chitosan/Polyvinyl-Alcohol-Based Hydrogels Applied as Active Pads

by Constantinos E. Salmas, Eleni Kollia, Learda Avdylaj, Anna Kopsacheili, Konstantinos Zaharioudakis, Stavros Georgopoulos, Areti Leontiou, Katerina Katerinopoulou, George Kehayias, Anastasios Karakassides, Charalampos Proestos and Aris E. Giannakas

Gels 2023, 9(7), 570; https://doi.org/10.3390/gels9070570 - 12 Jul 2023

Cited by 3 | Viewed by 2510

Abstract

Currently, food saving, a circular economy, and zero environmental fingerprints are of major interest. Scientific efforts for enhanced food preservation using “green” methods have been intensified. Even though chemicals could achieve such targets effectively, the global trend against the “greenhouse effect” suggests the use of environmentally friendly biobased materials for this purpose. In this study, the promising biopolymer chitosan is incorporated with the promising biodegradable polymer polyvinyl alcohol to produce an improved biopolymeric matrix. This biodegradable biopolymer was further mixed homogeneously with 15% thymol/nano-zeolite nanohybrid material. The properties of the final developed film were improved compared to the relevant values of chitosan/polyvinyl alcohol film. The mechanical properties were enhanced significantly, i.e., there was a 34% increase in Young’s modulus and a 4.5% increase in the ultimate tensile strength, while the antioxidant activity increased by 53.4%. The antibacterial activity increased by 134% for Escherichia coli, 87.5% for Staphylococcus aureus, 32% for Listeria monocytogenes, and 9% for Salmonella enterica. The water vapor diffusion coefficient and the oxygen permeability coefficient decreased to −51% and −74%, respectively, and thus, the water vapor and oxygen barrier increased significantly. The active pads were used in strawberries, and the antimicrobial activity evaluation against the mold of fungi was carried out. The visual evaluation shows that the active pads could extend the shelf life duration of strawberries. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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14 pages, 5050 KiB

Open AccessEditor’s ChoiceArticle

Tissue Adhesive, Biocompatible, Antioxidant, and Antibacterial Hydrogels Based on Tannic Acid and Fungal-Derived Carboxymethyl Chitosan for Wound-Dressing Applications

by Kummara Madhusudana Rao, Uluvangada Thammaiah Uthappa, Hyeon Jin Kim and Sung Soo Han

Gels 2023, 9(5), 354; https://doi.org/10.3390/gels9050354 - 22 Apr 2023

Cited by 12 | Viewed by 2455

Abstract

This study aimed to develop hydrogels for tissue adhesion that are biocompatible, antioxidant, and antibacterial. We achieved this by using tannic acid (TA) and fungal-derived carboxymethyl chitosan (FCMCS) incorporated in a polyacrylamide (PAM) network using free-radical polymerization. The concentration of TA greatly influenced the physicochemical and biological properties of the hydrogels. Scanning electron microscopy showed that the nanoporous structure of the FCMCS hydrogel was retained with the addition of TA, resulting in a nanoporous surface structure. Equilibrium-swelling experiments revealed that increasing the concentration of TA significantly improved water uptake capacity. Antioxidant radical-scavenging assays and porcine skin adhesion tests confirmed the excellent adhesive properties of the hydrogels, with adhesion strengths of up to 39.8 ± 1.2 kPa for 1.0TA-FCMCS due to the presence of abundant phenolic groups on TA. The hydrogels were also found to be biocompatible with skin fibroblast cells. Furthermore, the presence of TA significantly enhanced the antibacterial properties of the hydrogels against both Gram-positive (Staphylococcus aureus) and Gram-negative (Escherichia coli) bacteria. Therefore, the developed drug-free antibacterial and tissue-adhesive hydrogels can potentially be used as wound dressings for infected wounds. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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13 pages, 5587 KiB

Open AccessArticle

Ethyl Vanillin Rapid Crystallization from Carboxymethyl Chitosan Ion-Switchable Hydrogels

by Chenghong Huang, Hong Tang, Xiaorong Huang, Hongjie Chen, Kang Yang, Qi Yin, Lin Zhang, Xia Li, Xue Mou, Shuangkou Chen, Yuchan Zhang and Yan Hu

Gels 2023, 9(4), 335; https://doi.org/10.3390/gels9040335 - 14 Apr 2023

Viewed by 2154

Abstract

Polymer gels are usually used for crystal growth as the recovered crystals have better properties. Fast crystallization under nanoscale confinement holds great benefits, especially in polymer microgels as its tunable microstructures. This study demonstrated that ethyl vanillin can be quickly crystallized from carboxymethyl chitosan/ethyl vanillin co-mixture gels via classical swift cooling method and supersaturation. It found that EVA appeared with bulk filament crystals accelerated by a large quantity of nanoconfinement microregions resulted from space-formatted hydrogen network between EVA and CMCS when their concentration exceeds 1:1.4 and may occasionally arise when the concentration less than 1:0.8. It was observed that EVA crystal growth has two models involving hang-wall growth at the air-liquid interface at the contact line, as well as extrude-bubble growth at any sites on the liquid surface. Further investigations found that EVA crystals can be recovered from as-prepared ion-switchable CMCS gels by 0.1 M hydrochloric acid or acetic acid without defects. Consequently, the proposed method may offer an available scheme for a large-scale preparation of API analogs. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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17 pages, 3734 KiB

Open AccessEditor’s ChoiceArticle

Injectable Chitosan-Based Hydrogels for Trans-Cinnamaldehyde Delivery in the Treatment of Diabetic Foot Ulcer Infections

by Henry Chijcheapaza-Flores, Nicolas Tabary, Feng Chai, Mickaël Maton, Jean-Noel Staelens, Frédéric Cazaux, Christel Neut, Bernard Martel, Nicolas Blanchemain and Maria José Garcia-Fernandez

Gels 2023, 9(3), 262; https://doi.org/10.3390/gels9030262 - 22 Mar 2023

Cited by 8 | Viewed by 3417

Abstract

Diabetic foot ulcers (DFU) are among the most common complications in diabetic patients and affect 6.8% of people worldwide. Challenges in the management of this disease are decreased blood diffusion, sclerotic tissues, infection, and antibiotic resistance. Hydrogels are now being used as a new treatment option since they can be used for drug delivery and to improve wound healing. This project aims to combine the properties of hydrogels based on chitosan (CHT) and the polymer of β cyclodextrin (PCD) for local delivery of cinnamaldehyde (CN) in diabetic foot ulcers. This work consisted of the development and characterisation of the hydrogel, the evaluation of the CN release kinetics and cell viability (on a MC3T3 pre-osteoblast cell line), and the evaluation of the antimicrobial and antibiofilm activity (S. aureus and P. aeruginosa). The results demonstrated the successful development of a cytocompatible (ISO 10993-5) injectable hydrogel with antibacterial (99.99% bacterial reduction) and antibiofilm activity. Furthermore, a partial active molecule release and an increase in hydrogel elasticity were observed in the presence of CN. This leads us to hypothesise that a reaction between CHT and CN (a Schiff base) can occur and that CN could act as a physical crosslinker, thus improving the viscoelastic properties of the hydrogel and limiting CN release. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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12 pages, 4056 KiB

Open AccessArticle

Fungal Carboxymethyl Chitosan-Impregnated Bacterial Cellulose Hydrogel as Wound-Dressing Agent

by Maduru Suneetha, So-Yeon Won, Sun Mi Zo and Sung Soo Han

Gels 2023, 9(3), 184; https://doi.org/10.3390/gels9030184 - 27 Feb 2023

Cited by 18 | Viewed by 2262

Abstract

Bacterial cellulose (BC) produced by Gluconoacetobacter hansenii is a suitable polymeric fiber network for wound-dressing purposes, but its lack of antibacterial properties limits it from healing bacterial wounds. We developed hydrogels by impregnating fungal-derived carboxymethyl chitosan to BC fiber networks using a simple solution immersion method. The CMCS–BC hydrogels were characterized using various characterization techniques such as XRD, FTIR, water contact angle measurements, TGA, and SEM to know the physiochemical properties. The results show that the impregnation of CMCS into BC fiber networks greatly influences BC’s improving hydrophilic nature, which is crucial for wound healing applications. Furthermore, the CMCS–BC hydrogels were studied for biocompatibility analysis with skin fibroblast cells. The results revealed that by increasing the CMCS content in the BC, biocompatibility, cell attachment, and spreading capacity also increase. The antibacterial activity of CMCS–BC hydrogels is shown using the CFU method against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). As a result, the CMCS–BC hydrogels exhibit more suitable antibacterial properties than those without BC due to the CMCS having amino groups that enhance antibacterial properties. Therefore, CMCS–BC hydrogels can be considered suitable for antibacterial wound dressing applications. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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Review

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28 pages, 3351 KiB

Open AccessReview

Biomedical Trends in Stimuli-Responsive Hydrogels with Emphasis on Chitosan-Based Formulations

by Weronika Kruczkowska, Julia Gałęziewska, Katarzyna Grabowska, Gabriela Liese, Paulina Buczek, Karol Kamil Kłosiński, Mateusz Kciuk, Zbigniew Pasieka, Żaneta Kałuzińska-Kołat and Damian Kołat

Gels 2024, 10(5), 295; https://doi.org/10.3390/gels10050295 - 25 Apr 2024

Cited by 3 | Viewed by 1855

Abstract

Biomedicine is constantly evolving to ensure a significant and positive impact on healthcare, which has resulted in innovative and distinct requisites such as hydrogels. Chitosan-based formulations stand out for their versatile utilization in drug encapsulation, transport, and controlled release, which is complemented by their biocompatibility, biodegradability, and non-immunogenic nature. Stimuli-responsive hydrogels, also known as smart hydrogels, have strictly regulated release patterns since they respond and adapt based on various external stimuli. Moreover, they can imitate the intrinsic tissues’ mechanical, biological, and physicochemical properties. These characteristics allow stimuli-responsive hydrogels to provide cutting-edge, effective, and safe treatment. Constant progress in the field necessitates an up-to-date summary of current trends and breakthroughs in the biomedical application of stimuli-responsive chitosan-based hydrogels, which was the aim of this review. General data about hydrogels sensitive to ions, pH, redox potential, light, electric field, temperature, and magnetic field are recapitulated. Additionally, formulations responsive to multiple stimuli are mentioned. Focusing on chitosan-based smart hydrogels, their multifaceted utilization was thoroughly described. The vast application spectrum encompasses neurological disorders, tumors, wound healing, and dermal infections. Available data on smart chitosan hydrogels strongly support the idea that current approaches and developing novel solutions are worth improving. The present paper constitutes a valuable resource for researchers and practitioners in the currently evolving field. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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Other

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11 pages, 934 KiB

Open AccessPerspective

Chitosan Schiff-Base Hydrogels—A Critical Perspective Review

by Ioana A. Duceac and Sergiu Coseri

Gels 2022, 8(12), 779; https://doi.org/10.3390/gels8120779 - 28 Nov 2022

Cited by 14 | Viewed by 2993

Abstract

Chitosan is quite a unique polysaccharide due to the presence of the amine groups naturally occurring in its structure. This feature renders it into a polycation which makes it appealing for preparing polyelectrolyte complexes or imine bonds gels. Therefore, the vast majority of hydrogels prepared using Schiff base chemistry have chitosan as one component. Usually, the counterpart is a low molecular weight aldehyde or a macromolecular periodate-oxidized polysaccharide, i.e., cellulose, pullulan, starch, alginate, hyaluronic acid, etc. Indisputable advantages of hydrogels include their quick gelation, no need for crosslinking agents, and self-healing and injectability properties. This gives grounds for further research, both fundamental in materials science and applicative in various domains. This article is a critical assessment of the most relevant aspects of this topic. It also provides a short review of some of the most interesting research reported in the literature supporting the main observations of this perspective. Full article

(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)

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