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Hydrogels: Synthesis, Characterization and Applications

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

Deadline for manuscript submissions: closed (31 August 2023) | Viewed by 23051

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Prof. Dr. Dezhong Zhou

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School of Chemical Engineering and Technology (SCET), Xi’an Jiaotong University, Xi’an 710049, China
Interests: biomaterials; hyperbranched polymers; cyclized polymers; non-viral gene vector; controlled/living polymerization
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Dr. Shuai Liu

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College of Pharmaceutical Sciences, Zhejiang University, Hangzhou 310058, China
Interests: gene therapy; mRNA delivery; lipid nanoparticles; gene editing; biomaterials
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Dear Colleagues,

Hydrogels, due to their biomimetic nature, have been widely explored for application in regenerative medicine. With the advancements in chemistry, biology and material sciences, diverse new methods for the synthesis and characterization of hydrogels have been proposed; the chemical compositions, topological structures and functionalities of hydrogels can be manipulated more effectively; and the physiological properties and biological functions of hydrogels can be further tailor-made and greatly enhanced. Correspondingly, the utility of hydrogels in regenerative medicine, in terms of tissue engineering, drug delivery and diagnosis, etc., have been intensively assessed, both in vitro and in vivo. This progress in the field has brought hydrogels ever closer to achieving their potential in regenerative medicine. Meanwhile, new challenges associated with translating hydrogels from bench to bedside have also emerged. In this Special Issue, we aim to highlight the most recent progress in the synthesis, characterization and application of hydrogels in regenerative medicine, with the expectation to provide new insights into the development of clinical applicable hydrogels. We invite original research articles and review papers that cover the emerging methods for synthesizing and characterizing hydrogels, new strategies in tailoring the chemical compositions, functionalities, and properties of hydrogels, the in vitro and in vivo performance of hydrogels in tissue engineering, drug delivery and diagnosis, etc., and potential challenges in translating hydrogels to clinical settings.

Prof. Dr. Dezhong Zhou
Dr. Shuai Liu
Guest Editors

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Keywords

regenerative medicine
biomaterials
hydrogels
tissue engineering
drug delivery
diagnosis

Related Special Issue

Hydrogels: Synthesis, Characterization and Applications (2nd Edition) in Gels (3 articles)

Published Papers (11 papers)

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Research

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20 pages, 4392 KiB

Open AccessArticle

Novel Hydrolytic Degradable Crosslinked Interpenetrating Polymeric Networks (IPNs): An Efficient Hybrid System to Manage the Controlled Release and Degradation of Misoprostol

by Yasir Mehmood, Hira Shahid, Kashif Barkat, Numera Arshad, Akhtar Rasul, Mohammad N. Uddin and Mohsin Kazi

Gels 2023, 9(9), 697; https://0-doi-org.brum.beds.ac.uk/10.3390/gels9090697 - 29 Aug 2023

Viewed by 975

Abstract

Purpose: The goal of this study was to make pH-sensitive HPMC/Neocel C19-based interpenetrating polymeric networks (IPNs) that could be used to treat different diseases. An assembled novel carrier system was demonstrated in this study to achieve multiple functions such as drug protection and self-regulated release. Methods: Misoprostol (MPT) was incorporated as a model drug in hydroxyl-propyl-methylcellulose (HPMC)- and Neocel C19-based IPNs for controlled release. HPMC- and Neocel C19-based IPNs were fabricated through an aqueous polymerization method by utilizing the polymers HPMC and Neocel C19, the initiator ammonium peroxodisulfate (APS), the crosslinker methylenebisacrylamide (MBA), and the monomer methacrylic acid (MAA). An IPN based on these materials was created using an aqueous polymerization technique. Samples of IPN were analyzed using scanning electron microscopy (SEM), atomic force microscopy (AFM), differential scanning calorimetry (DSC), thermal analysis (TGA), and powder X-ray diffraction (PXRD). The effects of the pH levels 1.2 and 7.4 on these polymeric networks were also studied in vitro and through swelling experiments. We also performed in vivo studies on rabbits using commercial tablets and hydrogels. Results: The thermal stability measured using TGA and DSC for the revised formulation was higher than that of the individual components. Crystallinity was low and amorphousness was high in the polymeric networks, as revealed using powder X-ray diffraction (PXRD). The results from the SEM analysis demonstrated that the surface of the polymeric networks is uneven and porous. Better swelling and in vitro results were achieved at a high pH (7.4), which endorses the pH-responsive characteristics of IPN. Drug release was also increased in 7.4 pH (80% in hours). The pharmacokinetic properties of the drugs showed improvement in our work with hydrogel. The tablet MRT was 13.17 h, which was decreased in the hydrogels, and its AUC was increased from 314.41 ng h/mL to 400.50 ng h/mL in hydrogels. The blood compatibility of the IPN hydrogel was measured using different weights (100 mg, 200 mg, 400 mg, and 600 mg; 5.34%, 12.51%, 20.23%, and 29.37%, respectively). Conclusions: As a result, IPN composed of HPMC and Neocel C19 was successfully synthesized, and it is now possible to use it for the controlled release of MPT. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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12 pages, 5280 KiB

Open AccessArticle

Controlling the Self-Assembly and Material Properties of β-Sheet Peptide Hydrogels by Modulating Intermolecular Interactions

by James P. Warren, Matthew P. Culbert, Danielle E. Miles, Steven Maude, Ruth K. Wilcox and Paul A. Beales

Gels 2023, 9(6), 441; https://0-doi-org.brum.beds.ac.uk/10.3390/gels9060441 - 26 May 2023

Cited by 2 | Viewed by 1414

Abstract

Self-assembling peptides are a promising biomaterial with potential applications in medical devices and drug delivery. In the right combination of conditions, self-assembling peptides can form self-supporting hydrogels. Here, we describe how balancing attractive and repulsive intermolecular forces is critical for successful hydrogel formation. Electrostatic repulsion is tuned by altering the peptide’s net charge, and intermolecular attractions are controlled through the degree of hydrogen bonding between specific amino acid residues. We find that an overall net peptide charge of +/−2 is optimal to facilitate the assembly of self-supporting hydrogels. If the net peptide charge is too low then dense aggregates form, while a high molecular charge inhibits the formation of larger structures. At a constant charge, altering the terminal amino acids from glutamine to serine decreases the degree of hydrogen bonding within the assembling network. This tunes the viscoelastic properties of the gel, reducing the elastic modulus by two to three orders of magnitude. Finally, hydrogels could be formed from glutamine-rich, highly charged peptides by mixing the peptides in combinations with a resultant net charge of +/−2. These results illustrate how understanding and controlling self-assembly mechanisms through modulating intermolecular interactions can be exploited to derive a range of structures with tuneable properties. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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15 pages, 3240 KiB

Open AccessArticle

L-Lysine-Modified pNIPAm-co-GMA Copolymer Hydrogel for pH- and Temperature-Responsive Drug Delivery and Fluorescence Imaging Applications

by Madhappan Santhamoorthy, Ramkumar Vanaraj, Kokila Thirupathi, Selvakumari Ulagesan, Taek-Jeong Nam, Thi Tuong Vy Phan and Seong-Cheol Kim

Gels 2023, 9(5), 363; https://0-doi-org.brum.beds.ac.uk/10.3390/gels9050363 - 25 Apr 2023

Cited by 4 | Viewed by 1497

Abstract

The development of dual-stimuli-responsive hydrogels attracts much research interest owing to its unique stimuli-responsive characteristics. In this study, a poly-N-isopropyl acrylamide-co-glycidyl methacrylate-based copolymer was synthesized by incorporating N-isopropyl acrylamide (NIPAm) and a glycidyl methacrylate (GMA) monomer. The synthesized copolymer, pNIPAm-co-GMA was further modified with L-lysine (Lys) functional units and further conjugated with fluorescent isothiocyanate (FITC) to produce a fluorescent copolymer pNIPAAm-co-GMA-Lys hydrogel (HG). The in vitro drug loading and dual pH- and temperature-stimuli-responsive drug release behavior of the pNIPAAm-co-GMA-Lys HG was investigated at different pH (pH 7.4, 6.2, and 4.0) and temperature (25 °C, 37 °C, and 45 °C) conditions, respectively, using curcumin (Cur) as a model anticancer drug. The Cur drug-loaded pNIPAAm-co-GMA-Lys/Cur HG showed a relatively slow drug release behavior at a physiological pH (pH 7.4) and low temperature (25 °C) condition, whereas enhanced drug release was achieved at acidic pH (pH 6.2 and 4.0) and higher temperature (37 °C and 45 °C) conditions. Furthermore, the in vitro biocompatibility and intracellular fluorescence imaging were examined using the MDA-MB-231 cell line. Therefore, we demonstrate that the synthesized pNIPAAm-co-GMA-Lys HG system with temperature- and pH-stimuli-responsive features could be promising for various applications in biomedical fields, including drug delivery, gene delivery, tissue engineering, diagnosis, antibacterial/antifouling material, and implantable devices. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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24 pages, 4187 KiB

Open AccessArticle

Temperature- and pH-Responsive Super-Absorbent Hydrogel Based on Grafted Cellulose and Capable of Heavy Metal Removal from Aqueous Solutions

by Hebat-Allah S. Tohamy, Mohamed El-Sakhawy, Beata Strachota, Adam Strachota, Ewa Pavlova, Silvia Mares Barbosa and Samir Kamel

Gels 2023, 9(4), 296; https://0-doi-org.brum.beds.ac.uk/10.3390/gels9040296 - 2 Apr 2023

Cited by 10 | Viewed by 1796

Abstract

In this work, we prepared highly swelling, stimuli-responsive hydrogels capable of the highly efficient adsorption of inorganic pollutants. The hydrogels were based on hydroxypropyl methyl cellulose (HPMC) grafted with acrylamide (AM) and 3-sulfopropyl acrylate (SPA) and were synthesized via the growth (radical polymerization) of the grafted copolymer chains on HPMC, which was activated by radical oxidation. These grafted structures were crosslinked to an infinite network by a small amount of di-vinyl comonomer. HPMC was chosen as a cheap hydrophilic and naturally sourced polymer backbone, while AM and SPA were employed to preferentially bond coordinating and cationic inorganic pollutants, respectively. All the gels displayed a pronounced elastic character, as well as considerably high values of stress at break (several hundred %). The gel with the highest fraction of the ionic comonomer SPA (with an AM/SPA ratio = 0.5) displayed the highest equilibrium swelling ratio (12,100%), the highest volume response to temperature and pH, and the fastest swelling kinetics, but also the lowest modulus. The other gels (with AM/SPA = 1 and 2) displayed several times higher moduli but more modest pH responses and only very modest temperature sensitivity. Cr(VI) adsorption tests indicated that the prepared hydrogels removed this species from water very efficiently: between 90 and 96% in one step. The hydrogels with AM/SPA ratios of 0.5 and 1 appeared to be promising regenerable (via pH) materials for repeated Cr(VI) adsorption. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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15 pages, 8736 KiB

Open AccessArticle

The Development of a Polysaccharide-Based Hydrogel Encapsulating Tobramycin-Loaded Gelatine Microspheres as an Antibacterial System

by Mingsheng Shi, Yongmeng Xu, Shuai Li, Lifeng Wang, Junyao Gu and Yi-Xuan Zhang

Gels 2023, 9(3), 219; https://0-doi-org.brum.beds.ac.uk/10.3390/gels9030219 - 14 Mar 2023

Cited by 5 | Viewed by 1339

Abstract

Bacterial infection contributes to the bioburden of wounds, which is an essential factor in determining whether a wound can heal. Wound dressings with antibacterial properties that can promote wound-healing are highly desired for the treatment of chronic wound infections. Herein, we fabricated a simple polysaccharide-based hydrogel dressing encapsulating tobramycin-loaded gelatine microspheres with good antibacterial activity and biocompatibility. We first synthesised long-chain quaternary ammonium salts (QAS) by the reaction of tertiary amines with epichlorohydrin. The amino groups of carboxymethyl chitosan were then conjugated with QAS through the ring-opening reaction and QAS-modified chitosan (CMCS) was obtained. The antibacterial analysis showed that both QAS and CMCS could kill E. coli and S. aureus at relatively low concentrations. QAS with 16 carbon atoms has a MIC of 16 μg/mL for E. coli and 2 μg/mL for S. aureus. A series of formulations of tobramycin-loaded gelatine microspheres (TOB-G) were generated and the best formulation was selected by comparing the characters of the microspheres. The microsphere fabricated by 0.1 mL GTA was selected as the optimal candidate. We then used CMCS, TOB-G, and sodium alginate (SA) to prepare physically crosslinking hydrogels using CaCl₂ and investigated the mechanical properties, antibacterial activity, and biocompatibility of the hydrogels. In summary, the hydrogel dressing we produced can be used as an ideal alternative for the management of bacteria-infected wounds. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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15 pages, 6126 KiB

Open AccessArticle

Effects of the Amylose/Amylopectin Content and Storage Conditions on Corn Starch Hydrogels Produced by High-Pressure Processing (HPP)

by Oscar Pulgarín, Dominique Larrea-Wachtendorff and Giovanna Ferrari

Gels 2023, 9(2), 87; https://0-doi-org.brum.beds.ac.uk/10.3390/gels9020087 - 19 Jan 2023

Cited by 5 | Viewed by 2243

Abstract

In this study, the effects of the amylose/amylopectin content on starch gelation and the physical characteristics of hydrogels produced by HPP were studied by optical and rheological measurements in steady-state conditions. Additionally, the effects of the storage temperature (4 °C and 20 °C) and type of packaging (plastic bags or sealed Petri dishes) on the physical stability of the hydrogels were evaluated for 30 days of storage by evaluating the shrinkage of the granules, as well as the weight loss, water activity, organoleptic, and rheological properties. The experimental findings suggested that amylose plays an antagonistic role in determining the capacity of the starch granules to absorb water under pressure and to create stable and structured gels and on the physical stability of hydrogels due to its influence over the starch retrogradation extent during storage. Twenty per cent amylose was the minimum concentration to form stable corn starch HPP hydrogels with good physical and rheological properties. Moreover, a storage temperature of 20 °C and the use of polymeric bags were evaluated as the most suitable storage conditions and packaging materials enabling the long storage of corn starch hydrogels. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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17 pages, 6025 KiB

Open AccessArticle

Synthesis of Chemically Cross-Linked pH-Sensitive Hydrogels for the Sustained Delivery of Ezetimibe

by Rahima Khan, Muhammad Zaman, Ahmad Salawi, Mahtab Ahmad Khan, Muhammad Omer Iqbal, Romana Riaz, Muhammad Masood Ahmed, Muhammad Hammad Butt, Muhammad Nadeem Alvi, Yosif Almoshari and Meshal Alshamrani

Gels 2022, 8(5), 281; https://0-doi-org.brum.beds.ac.uk/10.3390/gels8050281 - 1 May 2022

Cited by 14 | Viewed by 2644

Abstract

In recent years, pH-sensitive hydrogels have been developed for the delivery of therapeutic agents to specific target sites that have a defined pH range. The use of pH-responsive polymers in hydrogels allows drug delivery to the desired pH range of the target organ. The primary aim is to increase the retention time of the drug in the small intestine by utilizing the swelling mechanism of the hydrogel at intestinal pH. In this study, polyethylene glycol (PEG) was used as a polymer to formulate a pH-sensitive hydrogel of Ezetimibe to deliver the drug to the small intestine where it inhibits the absorption of cholesterol. Design Expert software was applied to design and optimize the trial formulations in order to obtain an optimized formulation that has all the desired characteristics of the hydrogels. The PEG/Acrylic Acid hydrogels showed the maximum swelling at pH 6.8, which is consistent with the pH of the small intestine (pH 6–7.4). The maximum entrapment efficiency of the hydrogels was 99%. The hydrogel released 80–90% of the drug within 24 h and followed first-order release kinetics, which showed that the release from the drug was sustained. Hence, the results showed that the choice of a suitable polymer can lead to the development of an efficient drug-loaded hydrogel that can deliver the drug at the specific pH of the target organ. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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21 pages, 5644 KiB

Open AccessArticle

Orally Administered, Biodegradable and Biocompatible Hydroxypropyl–β–Cyclodextrin Grafted Poly(methacrylic acid) Hydrogel for pH Sensitive Sustained Anticancer Drug Delivery

by Nighat Batool, Rai Muhammad Sarfraz, Asif Mahmood, Muhammad Zaman, Nadiah Zafar, Ahmad Salawi, Yosif Almoshari and Meshal Alshamrani

Gels 2022, 8(3), 190; https://0-doi-org.brum.beds.ac.uk/10.3390/gels8030190 - 19 Mar 2022

Cited by 18 | Viewed by 3067

Abstract

In the current study, a pH sensitive intelligent hydroxypropyl–β–cyclodextrin-based polymeric network (HP-β-CD-g-MAA) was developed through a solution polymerization technique for site specific delivery of cytarabine in the colonic region. Prepared hydrogel formulations were characterized through cytarabine loading (%), ingredient’s compatibility, structural evaluation, thermal integrity, swelling pattern, release behavior and toxicological profiling in rabbits. Moreover, the pharmacokinetic profile of cytarabine was also determined in rabbits. New polymer formation was evident from FTIR findings. The percentage loaded into the hydrogels was in the range of 37.17–79.3%. Optimum swelling ratio of 44.56 was obtained at pH 7.4. Cytarabine release was persistent and in a controlled manner up to 24 h. In vitro degradation of hydrogels was more pronounced at intestinal pH as compared to acidic pH. Toxicity studies proved absence of any ocular, skin and oral toxicity, thus proving biocompatibility of the fabricated network. Hydrogels exhibited longer plasma half-life (8.75 h) and AUC (45.35 μg.h/mL) with respect to oral cytarabine solution. Thus, the developed hydrogel networks proved to be excellent and biocompatible cargo for prolonged and site-specific delivery of cytarabine in the management of colon cancer. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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12 pages, 2751 KiB

Open AccessArticle

Ultrasound Viscoelastic Properties of Biomass Polysaccharide Hydrogels as Evaluated by Rheometer Equipped with Sono-Device

by Sarara Noguchi and Takaomi Kobayashi

Gels 2022, 8(3), 172; https://0-doi-org.brum.beds.ac.uk/10.3390/gels8030172 - 9 Mar 2022

Cited by 4 | Viewed by 1937

Abstract

A viscoelastic rheometer was equipped with a sono-device and a water bath to enable measurement of storage moduli G′ and loss moduli G″ of biomass polysaccharide hydrogels such as Kanten agarose, κ-carrageenan, and konjac glucomannan under ultrasound (US) exposure. The action of low power of 43 kHz US on their hydrogels significantly decreased G′ of Kanten agarose and carrageenan after a few seconds of US exposure 0.1% strain. When US with 20 W output power was exposed under mechanical strain at 0.1%, lower values were obtained cyclically for 3 min US intervals. The values then reverted to the original moduli values when US was stopped in cases of Kanten agarose and carrageenan hydrogels. As G″ values were increased during US operation, the anhydro-L-galactose segments in their hydrogels were unable to relax the external US forces within the gel sufficiently, thereby leading to gel structure collapse at a higher strain percentage. These results suggest that US exposure induced deformational change in the hydrogel structure formed by hydrogen-bonded cross-links. However, US deformation was less in the case of deacetylated cross-linkage in konjac glucomannan hydrogel. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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Review

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15 pages, 1166 KiB

Open AccessReview

Nanocomposite Hydrogels and Extracellular Matrix—Advantages and Associated Risks

by Garry Kerch

Gels 2023, 9(9), 754; https://0-doi-org.brum.beds.ac.uk/10.3390/gels9090754 - 16 Sep 2023

Viewed by 1016

Abstract

Hydrogels can be considered as mimics of the extracellular matrix (ECM). Through integrins, the cytoskeleton is connected to the ECM, and cytoskeleton tension depends on ECM stiffness. A number of age-related diseases depend on cellular processes related to cytoskeleton function. Some examples of cancer initiation and progression and heart disease in relation to ECM stiffness have been analyzed. The incorporation of rigid particles into the ECM can increase ECM stiffness and promote the formation of internal residual stresses. Water migration, changes in water binding energy to biomactomolecules, and changes in the state of water from tightly bound water to free and loosely bound water lead to changes in the stiffness of the ECM. Cardiac tissue engineering, ECM stiffness and cancer, the equivalence of ECM stiffness, oxidative stress, inflammation, multi-layer polyelectrolyte complex hydrogels and bioprinting, residual internal stresses, viscoelastic hydrogels, hydrogel nanocomposites, and the effect of water have been reported. Special attention has been paid to the role of bound water and internal stresses in ECM stiffness. The risks related to rigid particle incorporation into the ECM have been discussed. The potential effect of polyphenols, chitosan, and chitosan oligosaccharide on ECM stiffness and the potential for anti-TNF-α and anti-NF-κB therapies have been discussed. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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28 pages, 3468 KiB

Open AccessReview

Research Advances of Injectable Functional Hydrogel Materials in the Treatment of Myocardial Infarction

by Wei Hu, Cui Yang, Xiaodan Guo, Yihong Wu, Xian Jun Loh, Zibiao Li, Yun-Long Wu and Caisheng Wu

Gels 2022, 8(7), 423; https://0-doi-org.brum.beds.ac.uk/10.3390/gels8070423 - 6 Jul 2022

Cited by 8 | Viewed by 3472

Abstract

Myocardial infarction (MI) has become one of the serious diseases threatening human life and health. However, traditional treatment methods for MI have some limitations, such as irreversible myocardial necrosis and cardiac dysfunction. Fortunately, recent endeavors have shown that hydrogel materials can effectively prevent negative remodeling of the heart and improve the heart function and long-term prognosis of patients with MI due to their good biocompatibility, mechanical properties, and electrical conductivity. Therefore, this review aims to summarize the research progress of injectable hydrogel in the treatment of MI in recent years and to introduce the rational design of injectable hydrogels in myocardial repair. Finally, the potential challenges and perspectives of injectable hydrogel in this field will be discussed, in order to provide theoretical guidance for the development of new and effective treatment strategies for MI. Full article

(This article belongs to the Special Issue Hydrogels: Synthesis, Characterization and Applications)

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