Synthesis and Applications of Hydrogels (2nd Edition)

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

Deadline for manuscript submissions: closed (10 January 2025) | Viewed by 22504

Special Issue Editor

School of Mechanical Engineering, Shandong University, Jinan 250061, China
Interests: hydrogels; colloids and interfaces; 3D printing; surface forces
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Special Issue Information

Dear Colleagues,

Hydrogels have been used for producing contact lenses, flexible sensors and actuators, adhesives, wound dressings, and hygiene products and are critical to achieving the controlled release of bioactive molecules. The synthesis and application of hydrogels have received increasing attention across a number of disciplines over the past twenty years. We have seen increasing publications in hydrogel research, and the scientific field is evolving rapidly. For example, three-dimensional (3D) bioprinting using cell-loaded hydrogel composites has been one of the emerging topics for realizing artificial organs in biomedical research. The significant point of synthesizing a hydrogel is that the obtained gel should have reasonable mechanical and electrical properties and form effective interfacial connections with various substrates. Double- or even triple-network hydrogels have been fabricated to overcome the drawbacks of weak mechanical properties and low interfacial toughness. Additionally, mechanical training, salt precipitation, and the application of electric or magnetic fields have also been applied to hydrogel synthesis to achieve the desired properties. Challenges remain for commercialization, although a number of hydrogel-related patents are filed each year.

This Special Issue aims to report the most recent research and advances in hydrogel synthesis and applications, such as sensors and actuators, adhesives, 3D printing, etc. Research on new methodologies, mechanism studies, and the modeling of hydrogels are also welcome.

Prof. Dr. Jun Huang
Guest Editor

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Keywords

  • biomaterials
  • sensors and actuators
  • adhesives
  • flexible electronics
  • 3D printing
  • drug delivery
  • network

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Published Papers (10 papers)

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Research

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18 pages, 9926 KiB  
Article
Cannabidiol-Loaded Lipid Nanoparticles Incorporated in Polyvinyl Alcohol and Sodium Alginate Hydrogel Scaffold for Enhancing Cell Migration and Accelerating Wound Healing
by Sarawut Lapmanee, Sakkarin Bhubhanil, Natthawut Charoenphon, Anjaree Inchan, Phichaporn Bunwatcharaphansakun, Mattaka Khongkow and Katawut Namdee
Gels 2024, 10(12), 843; https://doi.org/10.3390/gels10120843 - 20 Dec 2024
Viewed by 1088
Abstract
Chronic wounds represent a persistent clinical challenge due to prolonged inflammation and impaired tissue repair mechanisms. Cannabidiol (CBD), recognized for its anti-inflammatory and pro-healing properties, shows therapeutic promise in wound care. However, its delivery via lipid nanoparticles (LNPs) remains challenging due to CBD’s [...] Read more.
Chronic wounds represent a persistent clinical challenge due to prolonged inflammation and impaired tissue repair mechanisms. Cannabidiol (CBD), recognized for its anti-inflammatory and pro-healing properties, shows therapeutic promise in wound care. However, its delivery via lipid nanoparticles (LNPs) remains challenging due to CBD’s inherent instability and low bioavailability. This study developed and characterized a novel hydrogel scaffold composed of CBD-loaded LNPs (CBD/LNPs) integrated into a polyvinyl alcohol (PVA) and sodium alginate (SA) matrix, designed to enhance wound repair and mitigate inflammation. The characteristics of the hydrogel scaffold were observed including the degree of swelling and LNPs’ release profiles. Furthermore, in the results, CBD/LNPs displayed enhanced stability and reduced cytotoxicity compared to unencapsulated CBD. In vitro assays demonstrated that CBD/LNPs significantly promoted fibroblast migration in gap-closure wound models and reduced intracellular reactive oxygen species, supporting their potential as a biocompatible and efficacious agent for cellular repair and oxidative stress attenuation. In vivo experiments using adult male Wistar rats with aseptic cutaneous wounds revealed that treatment with CBD/LNP-PVA/SA hydrogel scaffold significantly accelerated wound closure relative to blank hydrogel controls, demonstrating a substantial reduction in the wound area over time. Histological analysis confirms notable improvements in skin morphology in wounds treated with CBD/LNP-PVA/SA hydrogel scaffold with evidence of accelerated epithelialization, enhanced collagen deposition, and increased dermal thickness and vascularization. Additionally, skin histology showed a more organized epidermal layer and reduced inflammatory cell infiltration in CBD/LNP-PVA/SA hydrogel scaffold-treated wounds, corresponding to a 35% increase in the wound closure rate by day 28 post-treatment. These findings suggest that CBD/LNP-PVA/SA hydrogel scaffolds facilitate inflammation resolution and structural wound healing through localized, sustained CBD delivery. The dual anti-inflammatory and wound-healing effects position CBD/LNP-PVA/SA hydrogel scaffold as a promising approach for chronic wound management. Future investigations are warranted to elucidate the mechanistic pathways by which CBD modulates the skin architecture and to explore its translational applications in clinical wound care. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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16 pages, 6306 KiB  
Article
L-Cysteine/Silver Nitrate/Iodate Anions System: Peculiarities of Supramolecular Gel Formation with and Without Visible-Light Exposure
by Dmitry V. Vishnevetskii, Elizaveta E. Polyakova, Yana V. Andrianova, Arif R. Mekhtiev, Alexandra I. Ivanova, Dmitry V. Averkin, Vladimir G. Alekseev, Alexey V. Bykov and Mikhail G. Sulman
Gels 2024, 10(12), 809; https://doi.org/10.3390/gels10120809 - 9 Dec 2024
Viewed by 858
Abstract
In this study, novel anion photo-responsive supramolecular hydrogels based on cysteine–silver sol (CSS) and iodate anions (IO3) were prepared. The peculiarities of the self-assembly process of gel formation in the dark and under visible-light exposure were studied using a complex [...] Read more.
In this study, novel anion photo-responsive supramolecular hydrogels based on cysteine–silver sol (CSS) and iodate anions (IO3) were prepared. The peculiarities of the self-assembly process of gel formation in the dark and under visible-light exposure were studied using a complex of modern physico-chemical methods of analysis, including viscosimetry, UV spectroscopy, dynamic light scattering, electrophoretic light scattering, scanning electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. In the dark phase, the formation of weak snot-like gels takes place in a quite narrow IO3 ion concentration range. The visible-light exposure of these gels leads to an increase in their viscosity and dramatic change in their color. The morphology of gels alters after light irradiation that is reflected in the formation of a huge number of spherical/elliptical particles and the thickening of the fibers of the gel network. The interaction of CSS with IO3 anions has features of a redox process, which leads to the formation of silver iodide/silver oxide nanoparticles inside and on the surface of CSS particles. CSS possesses selectivity only to IO3 anions compared to many other inorganic ions relevant for humans and the environment. Thus, the CSS/IO3 system is non-trivial and can be considered as a novel low-molecular-weight gelator with photosensitive properties, as another way to produce silver iodide nanoparticles, and as a new approach for IO3 ion detection. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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18 pages, 12677 KiB  
Article
A Simple Preparation of Crosslinked, Highly Alkaline Diallyldimethylammonium Hydroxide Hydrogel Particles via Inverse Static Anion Exchange
by Tim B. Mrohs and Oliver Weichold
Gels 2024, 10(11), 743; https://doi.org/10.3390/gels10110743 - 15 Nov 2024
Viewed by 621
Abstract
Highly alkaline hydrogels are gaining increasing attention in building materials research. Specifically, cationic alkaline hydrogels based on diallyldimethylammonium hydroxide (DADMAOH) as the monomer have been effectively used to seal water-bearing cracks or serve as coupling media for electrochemical chloride extraction. However, the residual [...] Read more.
Highly alkaline hydrogels are gaining increasing attention in building materials research. Specifically, cationic alkaline hydrogels based on diallyldimethylammonium hydroxide (DADMAOH) as the monomer have been effectively used to seal water-bearing cracks or serve as coupling media for electrochemical chloride extraction. However, the residual halogen content and challenges in scaling up monomer production have hindered broader application. Attempts to use a commercially available cation-selective membrane for ion exchange achieved up to 90% chloride-to-hydroxide switch, but the approach proved ineffective due to significant monomer decomposition during the process. By contrast, neutral gels and gel particles can be readily prepared from diallyldimethylammonium chloride (DADMAC) in large quantities and with a wide range of compositions. It is demonstrated here that these neutral gel particles undergo inverse static anion exchange when suspended in NaOH solution, generating DADMAOH particles with residual halide contents of <0.3%, without the need for ion-selective or dialysis membranes. This corresponds to an up to 100-fold reduction in residual chloride content compared to particles produced directly from alkaline monomer solutions, thereby significantly enhancing the efficiency of hydroxide ion release. The swelling behaviour of the particles is primarily influenced by the initial monomer concentration, while conductivity remains largely unaffected, indicating that charge transport occurs mainly along the particle surface. Despite the pronounced increase in swelling with decreasing particle radii, the specific conductivity of 2.8 Ω−1 m−1 is still sufficient for their use as coupling media in concrete applications. In summary, the alkaline particles prepared via inverse static anion exchange meet all necessary requirements for building materials applications, offering a broader range of tuneable properties and greater ease of production compared to gels or particles derived from DADMAOH. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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17 pages, 4400 KiB  
Article
Preparation of Composite Hydrogels Based on Cysteine–Silver Sol and Methylene Blue as Promising Systems for Anticancer Photodynamic Therapy
by Dmitry V. Vishnevetskii, Fedor A. Metlin, Yana V. Andrianova, Elizaveta E. Polyakova, Alexandra I. Ivanova, Dmitry V. Averkin and Arif R. Mekhtiev
Gels 2024, 10(9), 577; https://doi.org/10.3390/gels10090577 - 5 Sep 2024
Cited by 1 | Viewed by 1388
Abstract
In this study, a novel supramolecular composite, “photogels”, was synthesized by mixing of cysteine–silver sol (CSS) and methylene blue (MB). A complex of modern physico-chemical methods of analysis such as viscosimetry, UV spectroscopy, dynamic and electrophoretic light scattering, scanning electron microscopy and energy-dispersive [...] Read more.
In this study, a novel supramolecular composite, “photogels”, was synthesized by mixing of cysteine–silver sol (CSS) and methylene blue (MB). A complex of modern physico-chemical methods of analysis such as viscosimetry, UV spectroscopy, dynamic and electrophoretic light scattering, scanning electron microscopy and energy-dispersive X-ray spectroscopy showed that MB molecules are uniformly localized mainly in the space between fibers of the gel-network formed by CSS particles. Molecules of the dye also bind with the surface of CSS particles by non-covalent interactions. This fact is reflected in the appearance of a synergistic anticancer effect of gels against human squamous cell carcinoma even in the absence of light irradiation. A mild toxic influence of hydrogels was observed in normal keratinocyte cells. Photodynamic exposure significantly increased gel activity, and there remained a synergistic effect. The study of free-radical oxidation in cells has shown that gels are not only capable of generating reactive oxygen species, but also have other targets of action. Flow cytometric analysis allowed us to find out that obtained hydrogels caused cell cycle arrest both without irradiation and with light exposure. The obtained gels are of considerable interest both from the point of view of academics and applied science, for example, in the photodynamic therapy of superficial neoplasms. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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15 pages, 3914 KiB  
Article
Cyclodextrin—Polymethylsilsesquioxane Combined System as a Perspective Iron Delivery System for Oral Administration
by Polina Orlova, Ivan Meshkov, Egor Latipov, Sergey Vasiliev, Ivan Mikheev, Daria-Maria Ratova, Alexandra Kalinina, Aziz Muzafarov and Irina Le-Deygen
Gels 2024, 10(9), 564; https://doi.org/10.3390/gels10090564 - 30 Aug 2024
Viewed by 965
Abstract
Anemia is a global health problem that affects both adults and children, but treatment is hampered by serious side effects, primarily associated with the gastrointestinal tract with oral administration of drugs. In this study, we aimed to develop an oral form of iron [...] Read more.
Anemia is a global health problem that affects both adults and children, but treatment is hampered by serious side effects, primarily associated with the gastrointestinal tract with oral administration of drugs. In this study, we aimed to develop an oral form of iron compounds using polymethylsilsesquioxane hydrogels. To boost loading efficiency and prolong release, the iron compounds (FeCl3 and ferrous D-Gluconate) are incorporated into a guest–host complex with 2-hydroxypropyl-beta-cyclodextrin. We used PRXD, SEM, EDX mapping, and FTIR to investigate the complex formation, as well as the incorporation of such complexes into hydrogels. The optimal system underlines a combination of ferrous D-Gluconate and HPCD in a 1:1 molar ratio, embedded into a hydrogel with a modest quantity of silicate crosslinks. We demonstrated the slowing of iron release in a gastric media. Mathematical investigation revealed that the Higuchi mechanism releases iron from the hydrogel. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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21 pages, 5030 KiB  
Article
Physically Crosslinked Poly(methacrylic acid)/Gelatin Hydrogels with Excellent Fatigue Resistance and Shape Memory Properties
by Vukasin Ugrinovic, Maja Markovic, Bojan Bozic, Vesna Panic and Djordje Veljovic
Gels 2024, 10(7), 444; https://doi.org/10.3390/gels10070444 - 4 Jul 2024
Viewed by 1967
Abstract
Hydrogels endure various dynamic stresses, demanding robust mechanical properties. Despite significant advancements, matching hydrogels’ strength to biological tissues and plastics is often challenging without applying potentially harmful crosslinkers. Using hydrogen bonds as sacrificial bonds offers a promising strategy to produce tough, versatile hydrogels [...] Read more.
Hydrogels endure various dynamic stresses, demanding robust mechanical properties. Despite significant advancements, matching hydrogels’ strength to biological tissues and plastics is often challenging without applying potentially harmful crosslinkers. Using hydrogen bonds as sacrificial bonds offers a promising strategy to produce tough, versatile hydrogels for biomedical and industrial applications. Poly(methacrylic acid) (PMA)/gelatin hydrogels were synthesized by thermally induced free-radical polymerization and crosslinked only by physical bonds, without adding any chemical crosslinker. The addition of gelatin increased the formation of hydrophobic domains in the structure of the hydrogels, which acted as permanent crosslinking points. The increase in PMA and gelatin contents generally led to a lower equilibrium water content (WC), higher thermal stability and better mechanical properties. The values of tensile strength and toughness reached up to 1.44 ± 0.17 MPa and 4.91 ± 0.51 MJ m−3, respectively, while the compressive modulus and strength reached up to 0.75 ± 0.06 MPa and 24.81 ± 5.85 MPa, respectively, with the WC being higher than 50 wt.%. The obtained values for compressive mechanical properties are comparable with super-strong hydrogels reported in the literature. In addition, hydrogels exhibited excellent fatigue resistance and biocompatibility, as well as great shape memory properties, which make them prominent candidates for a wide range of biomedical applications. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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14 pages, 3676 KiB  
Article
Fluoride-Ion-Responsive Sol–Gel Transition in an L-Cysteine/AgNO3 System: Self-Assembly Peculiarities and Anticancer Activity
by Dmitry V. Vishnevetskii, Yana V. Andrianova, Elizaveta E. Polyakova, Alexandra I. Ivanova and Arif R. Mekhtiev
Gels 2024, 10(5), 332; https://doi.org/10.3390/gels10050332 - 14 May 2024
Cited by 3 | Viewed by 1914
Abstract
Supramolecular hydrogels based on low-molecular-weight compounds are a unique class of so-called “soft” materials, formed by weak non-covalent interactions between precursors at their millimolar concentrations. Due to the variety of structures that can be formed using different low-molecular-weight gelators, they are widely used [...] Read more.
Supramolecular hydrogels based on low-molecular-weight compounds are a unique class of so-called “soft” materials, formed by weak non-covalent interactions between precursors at their millimolar concentrations. Due to the variety of structures that can be formed using different low-molecular-weight gelators, they are widely used in various fields of technology and medicine. In this study, we report for the first time an unusual self-assembly process of mixing a hydrosol obtained from L-cysteine and silver nitrate (cysteine–silver sol—CSS) with sodium halides. Modern instrumental techniques such as viscosimetry, UV spectroscopy, dynamic light scattering, zeta potential measurements, SEM and EDS identified that adding fluoride anions to CSS is able to form stable hydrogels of a thixotropic nature, while Cl, Br and I lead to precipitation. The self-assembly process proceeds using a narrow concentration range of F. An increase in the fluoride anion content in the system leads to a change in the gel network morphology from elongated structures to spherical ones. This fact is reflected in a decrease in the gel viscosity and a number of gel–sol–gel transition cycles. The mechanism of F’s interaction with hydrosol includes the condensation of anions on the positive surface of the CSS nanoparticles, their binding via electrostatic forces and the formation of a resulting gel carcass. In vitro analysis showed that the hydrogels suppressed human squamous carcinoma cells at a micromolar sample concentration. The obtained soft gels could have potential applications against cutaneous malignancy and as carriers for fluoride anion and other bioactive substance delivery. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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12 pages, 2537 KiB  
Article
Cysteine–Silver–Polymer Systems for the Preparation of Hydrogels and Films with Potential Applications in Regenerative Medicine
by Dmitry V. Vishnevetskii, Arif R. Mekhtiev, Dmitry V. Averkin and Elizaveta E. Polyakova
Gels 2023, 9(12), 924; https://doi.org/10.3390/gels9120924 - 23 Nov 2023
Cited by 3 | Viewed by 1855
Abstract
Herein, the problem concerning the poorer mechanical properties of gels based on low molecular weight gelators (LMWGs)—L-cysteine and silver nitrate—was solved by the addition of various polymers—polyvinyl alcohol (PVA), polyvinyl pyrrolidone (PVP) and polyethylene glycol (PEG)—to the initial cysteine–silver sol (CSS). The physicochemical [...] Read more.
Herein, the problem concerning the poorer mechanical properties of gels based on low molecular weight gelators (LMWGs)—L-cysteine and silver nitrate—was solved by the addition of various polymers—polyvinyl alcohol (PVA), polyvinyl pyrrolidone (PVP) and polyethylene glycol (PEG)—to the initial cysteine–silver sol (CSS). The physicochemical methods of analysis—viscosimetry, UV spectroscopy, DLS, and SEM—identified that cysteine–silver hydrogels (CSG) based on PVA possess the best rheological properties and porous microstructure (the average pore size is 2–10 µm) compared to gels without the polymer or with PVP or PEG. Such gels are able to form cysteine–silver cryogels (CSC) and then porous cysteine–silver films (CSF) with an average pore size of 10–20 µm and good mechanical, swelling, and adhesion to skin characteristics as long as the structure of CSS particles remains stable. In vitro experiments have shown that hydrogels are non-toxic to normal human fibroblast cells. The obtained materials could potentially be applied to regenerative medicine. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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Review

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27 pages, 14223 KiB  
Review
Antibacterial Hydrogels for Wound Dressing Applications: Current Status, Progress, Challenges, and Trends
by Jie Zhu, Hongju Cheng, Zixian Zhang, Kaikai Chen, Qinchen Zhang, Chen Zhang, Weihong Gao and Yuansheng Zheng
Gels 2024, 10(8), 495; https://doi.org/10.3390/gels10080495 - 26 Jul 2024
Cited by 3 | Viewed by 2844
Abstract
Bacterial infection treatment for chronic wounds has posed a major medical threat and challenge. Bacteria at the wounded sites can compete with the immune system and subsequently invade live tissues, leading to more severe tissue damage. Therefore, there is an urgent demand for [...] Read more.
Bacterial infection treatment for chronic wounds has posed a major medical threat and challenge. Bacteria at the wounded sites can compete with the immune system and subsequently invade live tissues, leading to more severe tissue damage. Therefore, there is an urgent demand for wound dressings with antibacterial and anti-inflammatory properties. Considering the concept of moist healing, hydrogels with a three-dimensional (3D) network structure are widely used as wound dressings due to their excellent hydrophilicity, water retention properties, and biocompatibility. Developing antibacterial hydrogels for the treatment of infected wounds has been receiving extensive attention recently. This article categorizes antibacterial hydrogels according to their materials and antibacterial modes, and introduces the recent findings and progress regarding their status. More importantly, with the development of emerging technologies, new therapies are utilized to prepare antibacterial hydrogels such as nanoenzymes, photothermal therapy (PTT), photodynamic therapy (PDT), metal–organic frameworks (MOFs), and other external stimuli-responsive methods. Therefore, this review also examines their progress, challenges, and future trends as wound dressings. In the following studies, there will still be a focus on antibacterial hydrogels that have a high performance, multi-functions, and intelligence, especially biocompatibility, a high and long-lasting antibacterial property, responsiveness, and on-demand therapeutic ability. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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31 pages, 5162 KiB  
Review
Recent Advances in the Development of Biomimetic Materials
by Maria G. Ciulla, Alessio Massironi, Michela Sugni, Matthew A. Ensign, Stefania Marzorati and Mahdi Forouharshad
Gels 2023, 9(10), 833; https://doi.org/10.3390/gels9100833 - 20 Oct 2023
Cited by 11 | Viewed by 7632
Abstract
In this review, we focused on recent efforts in the design and development of materials with biomimetic properties. Innovative methods promise to emulate cell microenvironments and tissue functions, but many aspects regarding cellular communication, motility, and responsiveness remain to be explained. We photographed [...] Read more.
In this review, we focused on recent efforts in the design and development of materials with biomimetic properties. Innovative methods promise to emulate cell microenvironments and tissue functions, but many aspects regarding cellular communication, motility, and responsiveness remain to be explained. We photographed the state-of-the-art advancements in biomimetics, and discussed the complexity of a “bottom-up” artificial construction of living systems, with particular highlights on hydrogels, collagen-based composites, surface modifications, and three-dimensional (3D) bioprinting applications. Fast-paced 3D printing and artificial intelligence, nevertheless, collide with reality: How difficult can it be to build reproducible biomimetic materials at a real scale in line with the complexity of living systems? Nowadays, science is in urgent need of bioengineering technologies for the practical use of bioinspired and biomimetics for medicine and clinics. Full article
(This article belongs to the Special Issue Synthesis and Applications of Hydrogels (2nd Edition))
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