Gel-Based Materials: Preparations and Characterization

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

Deadline for manuscript submissions: closed (15 November 2023) | Viewed by 13498

Special Issue Editors


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Guest Editor
Osaka Research Institute of Industrial Science and Technology, Morinomiya Center, Osaka 536-8553, Japan
Interests: hydrogels; low-molecular-weight gels; supramolecular gels; self-assembly; surfactants
Special Issues, Collections and Topics in MDPI journals

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Guest Editor
Chiba Institute of Science, Faculty of Pharmacy, Choshi-shi, Chiba 388-0025, Japan
Interests: hydrogels; low-molecular-weight gels; self-assembly; surfactants; emulsion; TDDS
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Gel-based materials have important applications in our daily lives. Conventionally, they have been widely used in cosmetics, foods, and paints. However, recently, they have been used in a broader range of fields such as energy, the environment, and medicine, partly due to the development of low-molecular-weight gelators that utilize molecular self-assembly and commonly used polymer gelators. This increase in gelation methods is likely because gel-based materials are much easier to control based on their rheological properties. Hence, remarkable progress has been made in developing gels with various functions, such as separation, extraction, and stimulus/biomolecule responses. Thus, this Special Issue invites original papers and review articles on the preparations and characterization of gel-based materials with various functions. Topics include:

  • Tough gels;
  • Supramolecular gels (low-molecular-weight gels);
  • Lamellar gel networks (α-form hydrated crystals);
  • Liquid crystal gels;
  • Ionic gels;
  • Gels with separation and extraction functions;
  • Stimuli- or biomolecule-responsive gels;
  • Emulsion gels.

In addition to the above, we welcome submissions on gel-based materials with various functions.

Dr. Rie Kakehashi
Dr. Yuji Yamashita
Guest Editors

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Gels is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

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Published Papers (10 papers)

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Research

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16 pages, 8207 KiB  
Article
Phase Inversion Gelation Process and Additive Effects on Hydrogel Film Properties of Cotton Cellulose
by Ayano Ibaraki and Takaomi Kobayashi
Gels 2024, 10(1), 34; https://doi.org/10.3390/gels10010034 - 31 Dec 2023
Cited by 1 | Viewed by 1270
Abstract
During the preparation of cotton cellulose hydrogels using the phase inversion gelation method of N,N-dimethylacetamide/LiCl solution under ethanol vapor, acetone (AC), methyl ethyl ketone (MEK), or diethyl ketone (DEK) were added as additives, and their gelation state and the properties [...] Read more.
During the preparation of cotton cellulose hydrogels using the phase inversion gelation method of N,N-dimethylacetamide/LiCl solution under ethanol vapor, acetone (AC), methyl ethyl ketone (MEK), or diethyl ketone (DEK) were added as additives, and their gelation state and the properties of the resulting hydrogels were evaluated. Adding the ketones to the cellulose solution caused an increase in the gelation time, but the solution viscosity decreased, indicating that the cellulose tended to aggregate in the solution. Among the hydrogels prepared by adding ketones, the water content was as high as 2050%, especially for AC and MEK. In these hydrogels, cellulose formed an agglomerated fibrous network of a few micron widths, forming a tuft-like entrapment space of about 10 to 100 μm size. The structure surrounded water and held it in the hydrogels. The FTIR results showed that the water, which formed hydrogen bonds, was retained within the hydrogel network. This structural configuration was determined to be conducive to maintaining the gel state against external deformation forces, especially in the case of the addition of MEK. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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13 pages, 21284 KiB  
Article
Radiation-Driven Polymerisation of Methacrylic Acid in Aqueous Solution: A Chemical Events Monte Carlo Study
by Aleksandras Sevcik, Zilvinas Rinkevicius and Diana Adliene
Gels 2023, 9(12), 947; https://doi.org/10.3390/gels9120947 - 1 Dec 2023
Viewed by 1001
Abstract
This study employed a coarse-grained Monte Carlo (MC) simulation to investigate the radiation-induced polymerisation of methacrylic acid (MAA) in an aqueous solution. This method provides an alternative to traditional kinetic models, enabling a detailed examination of the micro-structure and growth patterns of MAA [...] Read more.
This study employed a coarse-grained Monte Carlo (MC) simulation to investigate the radiation-induced polymerisation of methacrylic acid (MAA) in an aqueous solution. This method provides an alternative to traditional kinetic models, enabling a detailed examination of the micro-structure and growth patterns of MAA polymers, which are often not captured in other approaches. In this work, we generated multiple clones of a simulation box, each containing a specific chemical composition. In these simulations, every coarse-grained (CG) bead represents an entire monomer. The growth function, defined by the chemical behaviour of interacting substances, was determined through repeated random sampling. This approach allowed us to simulate the complex process of radiation-induced polymerisation, enhancing our understanding of the formation of poly(methacrylic acid) hydrogels at a microscopic level; while Monte Carlo simulations have been applied in various contexts of polymerisation, this study’s specific approach to modelling the radiation-induced polymerisation of MAA in an aqueous environment, utilising the data obtained by quantum chemistry modelling, with an emphasis on micro-structural growth, has not been extensively explored in existing studies. This understanding is important for advancing the synthesis of these hydrogels, which have potential applications in diverse fields such as materials science and medicine. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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11 pages, 2072 KiB  
Article
Effects of Counterion on the Formation and Hydration Behavior of α-Form Hydrated Crystals (α-Gels)
by Kenichi Sakai, Shuri Nishimoto, Yuki Hirai, Kyosuke Arakawa, Masaaki Akamatsu, Keisuke Tanaka, Toshiyuki Suzuki and Hideki Sakai
Gels 2023, 9(12), 928; https://doi.org/10.3390/gels9120928 - 25 Nov 2023
Viewed by 1063
Abstract
α-Form hydrated crystals form a lamellar gel in which the alkyl chains of the amphiphilic molecules are hexagonally arranged within bilayers below the gel–liquid crystal phase transition temperature. In practice, the lamellar gel network with excess water is called an “α-gel”, particularly in [...] Read more.
α-Form hydrated crystals form a lamellar gel in which the alkyl chains of the amphiphilic molecules are hexagonally arranged within bilayers below the gel–liquid crystal phase transition temperature. In practice, the lamellar gel network with excess water is called an “α-gel”, particularly in the cosmetics industry. In this study, the hydration or water sorption of amphiphilic materials in water vapor was assessed using a humidity-controlled quartz crystal microbalance with dissipation monitoring (QCM-D) technique. The amphiphilic materials used in this study were hexadecyl phosphate salts neutralized with L-arginine (C16P-Arg), CsOH (C16P-Cs), KOH (C16P-K), and NaOH (C16P-Na). Small- and wide-angle X-ray scattering measurements revealed that C16P-Arg and C16P-Cs yielded α-form hydrated crystals. Humidity-controlled QCM-D measurements demonstrated that C16P-Arg and C16P-Cs more readily underwent hydration or water sorption than C16P-K and C16P-Na. The key conclusion is that the significant hydration ability of C16P-Arg and C16P-Cs promotes the formation of the corresponding α-form hydrated crystals. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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19 pages, 6914 KiB  
Article
Thrombin-Free Fibrillogenesis and Gelation of Fibrinogen Triggered by Magnesium Sulfate
by Dominik Hense and Oliver I. Strube
Gels 2023, 9(11), 892; https://doi.org/10.3390/gels9110892 - 11 Nov 2023
Viewed by 1024
Abstract
Self-assembly of the blood protein fibrinogen is a highly relevant topic in materials science and medical research. This originates from fibrinogen’s beneficial material properties such as cell interaction and biocompatibility. Within recent decades, several enzyme-free strategies to create fibers and hydrogels out of [...] Read more.
Self-assembly of the blood protein fibrinogen is a highly relevant topic in materials science and medical research. This originates from fibrinogen’s beneficial material properties such as cell interaction and biocompatibility. Within recent decades, several enzyme-free strategies to create fibers and hydrogels out of fibrinogen have been presented, broadening the spectrum of fibrinogen-based material enormously. Herein, we describe a further method to obtain such a material by adding specifically MgSO4 to fibrinogen. The key of this material is the combination of Mg2+ and a kosmotropic anion, for example sulfate or (hydrogen)phosphate. This effect is most likely related to occupancy of fibrinogen’s well-known binding sites for Mg2+, resulting in a significant increase in fiber yield and gel stability. Here, we shine light on the question of how electrostatic interactions via Mg2+ enhance fibrillogenesis and the gelation of fibrinogen and discuss first insights into the material’s properties. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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19 pages, 4928 KiB  
Article
Explorative Image Analysis of Methylene Blue Interactions with Gelatin in Polypropylene Nonwoven Fabric Membranes: A Potential Future Tool for the Characterization of the Diffusion Process
by Jan Zidek, Anna Sudakova, Jiri Smilek, Duc Anh Nguyen, Hung Le Ngoc and Le Minh Ha
Gels 2023, 9(11), 888; https://doi.org/10.3390/gels9110888 - 9 Nov 2023
Viewed by 1446
Abstract
This manuscript explores the interaction between methylene blue dye and gelatin within a membrane using spectroscopy and image analysis. Emphasis is placed on methylene blue’s unique properties, specifically its ability to oscillate between two distinct resonance states, each with unique light absorption characteristics. [...] Read more.
This manuscript explores the interaction between methylene blue dye and gelatin within a membrane using spectroscopy and image analysis. Emphasis is placed on methylene blue’s unique properties, specifically its ability to oscillate between two distinct resonance states, each with unique light absorption characteristics. Image analysis serves as a tool for examining dye diffusion and absorption. The results indicate a correlation between dye concentrations and membrane thickness. Thinner layers exhibit a consistent dye concentration, implying an even distribution of the dye during the diffusion process. However, thicker layers display varying concentrations at different edges, suggesting the establishment of a diffusion gradient. Moreover, the authors observe an increased concentration of gelatin at the peripheries rather than at the center, possibly due to the swelling of the dried sample and a potential water concentration gradient. The manuscript concludes by suggesting image analysis as a practical alternative to spectral analysis, particularly for detecting whether methylene blue has been adsorbed onto the macromolecular network. These findings significantly enhance the understanding of the complex interactions between methylene blue and gelatin in a membrane and lay a solid foundation for future research in this field. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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12 pages, 2743 KiB  
Article
The Preparation of Electrolyte Hydrogels with the Water Solubilization of Polybenzoxazine
by Yutaka Ohsedo and Ami Kaneizumi
Gels 2023, 9(10), 819; https://doi.org/10.3390/gels9100819 - 14 Oct 2023
Viewed by 1269
Abstract
Polybenzoxazine (PBZ) exhibits excellent heat resistance, and PBZ derivatives have been designed and synthesized to achieve high performance. However, the application range of PBZ is limited by the strong interactions between molecular chains and its low solubility in organic solvents, thereby limiting its [...] Read more.
Polybenzoxazine (PBZ) exhibits excellent heat resistance, and PBZ derivatives have been designed and synthesized to achieve high performance. However, the application range of PBZ is limited by the strong interactions between molecular chains and its low solubility in organic solvents, thereby limiting its processability. This study focused on the benzoxazine structure as the molecular backbone of new hydrogel materials that can be applied as electrolyte materials and prepared functional gel materials. Here, we prepared hydrogels by water-solubilizing PBZ derivatives, which typically exhibit low solubility in organic solvents. Although studies on the hydrophilization of PBZ and its complexation with hydrophilic polymers have been conducted, no studies have been performed on the hydrogelation of PBZ. First, the phenol in the organic solvent-insoluble PBZ thin film obtained after the thermal ring-opening polymerization of the monomer was transformed into sodium phenoxide by immersion in a NaOH aqueous solution to water-solubilize it and obtain a hydrogel thin film. Although the hydrogel thin film exhibited low mechanical strength, a free-standing hydrogel film with improved strength was obtained through the double network gelation method with an acrylamide monomer system. The physical properties of the polymer composite hydrogel thin film were evaluated. The ionic conductivity of the hydrogel thin films was in the order of 10−4 S cm−1, indicating the potential of PBZ as an electrolyte hydrogel material. However, improving its ionic conductivity will be undertaken in future studies. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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18 pages, 3028 KiB  
Article
Enhancing Rheological and Textural Properties of Gelatin-Based Composite Gels through Incorporation of Sesame Seed Oleosome-Protein Fillers
by Fatemeh Sheikh, Maryam Hasani, Hossein Kiani, Mohammad Javad Asadollahzadeh and Farzaneh Sabbagh
Gels 2023, 9(10), 774; https://doi.org/10.3390/gels9100774 - 23 Sep 2023
Cited by 2 | Viewed by 1072
Abstract
In this study, the protein and oleosomes of sesame seeds were extracted individually and used to prepare a gel composed of gelatin, protein, and oleosomes. Mixtures of gelatin and sesame seeds protein were prepared, and oleosomes with different percentages (0, 10, 20 and [...] Read more.
In this study, the protein and oleosomes of sesame seeds were extracted individually and used to prepare a gel composed of gelatin, protein, and oleosomes. Mixtures of gelatin and sesame seeds protein were prepared, and oleosomes with different percentages (0, 10, 20 and 30% of their weight) were used. Different amounts of oleosomes in the composite gel samples were examined for their morphological, rheological, and textural properties. The results of the viscoelastic properties of different composite gel samples indicated that a higher percentage of oleosomes would increase the storage modulus (G′), loss modulus (G″), and complex viscosity (η*). The storage modulus of all gel samples was greater than the loss modulus, suggesting a solid behavior. So, in the sample with 30% oleosome, the storage modulus and the loss modulus reached 143,440 Pascals and 44,530 Pascals. The hardness and breaking force in samples containing 30% oleosome reached 1.29 ± 0.02 and 0.17 ± 0.02, respectively. In general, it can be said that composite gels based on gelatin-sesame seed protein modified with oleosome can be used as a part of food components in various dairy products, gelatin desserts, lean meat products and the production of useful products. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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21 pages, 4687 KiB  
Article
Quality by Design-Optimized Glycerosome-Enabled Nanosunscreen Gel of Rutin Hydrate
by Md. Shabbir Alam, Niha Sultana, Md. Abdur Rashid, Yahya Alhamhoom, Asad Ali, Ayesha Waheed, Mo. Suheb Ansari, Mohd. Aqil and Mohd Mujeeb
Gels 2023, 9(9), 752; https://doi.org/10.3390/gels9090752 - 15 Sep 2023
Viewed by 1520
Abstract
Sunburn is caused by prolonged exposure to ultraviolet (UV) rays from the sun, resulting in redness of the skin as well as tenderness, swelling, and blistering issues. During the healing process, it can cause peeling, irritation, and some long-term effects, including premature aging, [...] Read more.
Sunburn is caused by prolonged exposure to ultraviolet (UV) rays from the sun, resulting in redness of the skin as well as tenderness, swelling, and blistering issues. During the healing process, it can cause peeling, irritation, and some long-term effects, including premature aging, pigmentation, and a high risk of skin cancer. Rutin has antioxidant and anti-inflammatory effects, which could potentially reduce inflammation and soothe sunburned skin. The objective of the current proposal is to develop and create carbopol gel-encased glycerosomes for the treatment of sunburn. The Design of Expert (DoE) technique was used to optimize the proposed formulation and was subjected to various characterization parameters such as nanovesicles size, polydispersity index (PDI), surface charge, entrapment efficiency (EE), and surface morphology. The optimized rutin-loaded glycerosomes (opt-RUT-loaded-GMs) were further characterised for drug release, 2,2-Diphenyl-1-picrylhydrazyl (DPPH) assay, and confocal laser scanning microscopy (CLSM). The formulation showed sustained release, greater permeation into the skin, and good antioxidant activity. The dermatokinetic study of opt-RUT-loaded-GMs confirms that the Rutin hydrate had better retention in the epidermis as compared to the dermis, owing to its potential for long lasting protection after topical application. It was observed that the prepared formulation was stable, highly safe, and had good sun protection factor (SPF) values that could be used as a suitable option for topical drug administration to maximize the therapeutic efficacy of the drugs. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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28 pages, 15070 KiB  
Article
Statistically Optimized Tacrolimus and Thymoquinone Co-Loaded Nanostructured Lipid Carriers Gel for Improved Topical Treatment of Psoriasis
by Meraj Alam, Md. Rizwanullah, Showkat R. Mir and Saima Amin
Gels 2023, 9(7), 515; https://doi.org/10.3390/gels9070515 - 25 Jun 2023
Cited by 7 | Viewed by 1636
Abstract
The aim of this investigation was to develop and analyze a tacrolimus and thymoquinone co-loaded nanostructured lipid carriers (TAC-THQ-NLCs)-based nanogel as a new combinatorial approach for the treatment of psoriasis. The NLCs were formulated by an emulsification-solvent-evaporation technique using glyceryl monostearate, Capryol 90 [...] Read more.
The aim of this investigation was to develop and analyze a tacrolimus and thymoquinone co-loaded nanostructured lipid carriers (TAC-THQ-NLCs)-based nanogel as a new combinatorial approach for the treatment of psoriasis. The NLCs were formulated by an emulsification-solvent-evaporation technique using glyceryl monostearate, Capryol 90 (oil), and a mixture of Tween 80 and Span 20 as a solid lipid, liquid lipid, and surfactant, respectively. Their combination was optimized using a three-factor and three-level Box–Behnken design (33-BBD). The optimized TAC-THQ-NLCs were observed to be smooth and spherical with a particle size of 144.95 ± 2.80 nm, a polydispersity index of 0.160 ± 0.021, a zeta potential of −29.47 ± 1.9 mV, and an entrapment efficiency of >70% for both drugs. DSC and PXRD studies demonstrated the amorphous state of TAC and THQ in the lipid matrix of the NLCs. An FTIR analysis demonstrated the excellent compatibility of the drugs with the excipients without interactions. The TAC-THQ-NLC-based nanogel (abbreviated as TAC-THQ-NG) exhibited a good texture profile and good spreadability. The in vitro release study demonstrated a sustained drug release for 24 h from the TAC-THQ-NG that followed the Korsmeyer–Peppas kinetic model with a Fickian diffusion mechanism. Moreover, the TAC-THQ-NG revealed significantly higher dose-dependent toxicity against an HaCaT cell line compared to a TAC-THQ suspension gel (abbreviated as TAC-THQ-SG). Furthermore, the developed formulations demonstrated antioxidant activity comparable to free THQ. Confocal microscopy revealed improved permeation depth of the dye-loaded nanogel in the skin compared to the suspension gel. Based on these findings, it was concluded that TAC-THQ-NG is a promising combinatorial treatment approach for psoriasis. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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Review

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20 pages, 1467 KiB  
Review
Application of Injectable Hydrogels as Delivery Systems in Spinal Cord Injury
by Rong Ji, Zhizhong Hao, Hao Wang, Xingfan Li, Linyan Duan, Fangxia Guan and Shanshan Ma
Gels 2023, 9(11), 907; https://doi.org/10.3390/gels9110907 - 16 Nov 2023
Cited by 4 | Viewed by 1339
Abstract
Spinal cord injury (SCI) is a severe neurological injury caused by traffic accidents, trauma, or falls, which leads to significant loss of sensory, motor, and autonomous functions and seriously affects the patient’s life quality. Although considerable progress has been made in mitigating secondary [...] Read more.
Spinal cord injury (SCI) is a severe neurological injury caused by traffic accidents, trauma, or falls, which leads to significant loss of sensory, motor, and autonomous functions and seriously affects the patient’s life quality. Although considerable progress has been made in mitigating secondary injury and promoting the regeneration/repair of SCI, the therapeutic effects need to be improved due to drug availability. Given their good biocompatibility, biodegradability, and low immunogenicity, injectable hydrogels can be used as delivery systems to achieve controlled release of drugs and other substances (cells and proteins, etc.), offering new hope for SCI repair. In this article, we summarized the types of injectable hydrogels, analyzed their application as delivery systems in SCI, and further discussed the mechanisms of hydrogels in the treatment of SCI, such as anti-inflammatory, antioxidant, anti-apoptosis, and pro-neurogenesis. Moreover, we highlighted the potential benefits of hydrogels in the treatment of SCI in combination with therapies, including the recent advances and achievements of these promising tools. Our review may offer new strategies for the development of SCI treatments based on injectable hydrogels as delivery systems. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization)
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