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Gels
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Polysaccharide: Gelation Arts
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Polysaccharide: Gelation Arts

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

Deadline for manuscript submissions: 31 January 2025 | Viewed by 8356

Special Issue Editor

Dr. Gabriela Ionita

E-Mail Website
Guest Editor
“Ilie Murgulescu” Institute of Physical Chemistry of the Romanian Academy, 202 Splaiul Independentei, 060021 Bucharest, Romania
Interests: protein; polysaccharide gels; supramolecular chemistry; mesoporous materials

Special Issue Information

Dear Colleagues,

Polysaccharides represent a wide class of bio-macromolecules that can play a variety of functions determined by their structural characteristics. In particular, their biocompatibility makes them attractive for biomedical applications, the food industry, cosmetic industry, and water purification. Their common features are represented by the presence of hydrophilic functional groups, such as hydroxyl, carboxyl, and amino acids, and the rigidity of the polymeric chain. In consequence, many polysaccharides are soluble in water and in certain conditions can form hydrogels.

The gelation process is determined by the structural diversity of polysaccharides which arise from a variety of sugar units, the sequence of these units in the case of hetero-polysaccharides, their ability to be functionalized, etc. In many cases, polysaccharide gels are the resultant of non-covalent intra- and inter-molecular associations, involving hemiacetal oxygen, hydroxyl, or methyl groups of the sugar residues. Complexation by metal ions can also be a driving force to generate gel networks as in the case of alginate. Using a variety of crosslinking agents that can be chosen depending on the presence of functional groups in the polysaccharide structure, it is possible to generate new gel networks or, in the particular case of a mixture of two polysaccharides, interpenetrated networks. These networks can lead to the formation of new covalent bonds.

This Special Issue, entitled “Polysaccharide: Gelation Arts”, will focus on the  various aspects of the polysaccharide gelation process: monitoring the gelation process, capacity to entrap various species from low molecular weight to proteins or cells, physicochemical methods that can highlight special properties of polysaccharide gels, applications, and modulation of gel properties. Researchers investigating polysaccharide gelation processes are invited to publish their original results, reviews, or perspectives related to these topics.

Dr. Gabriela Ionita
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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 2100 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.

Keywords

  • polysaccharides
  • noncovalent polymer gelation
  • covalent crosslinking
  • noncovalent crosslinking
  • ipn and semi-ipn networks
  • viscoelastic properties of polysaccharide gels
  • biomaterials

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Published Papers (5 papers)

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Research

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18 pages, 3303 KiB  
Article
Design and Evaluation of New Gel-Based Floating Matrix Tablets Utilizing the Sublimation Technique for Gastroretentive Drug Delivery
by Worawut Kriangkrai, Satit Puttipipatkhachorn, Pornsak Sriamornsak and Srisagul Sungthongjeen
Gels 2024, 10(9), 581; https://doi.org/10.3390/gels10090581 - 9 Sep 2024
Cited by 1 | Viewed by 1219
Abstract
A gel-based floating matrix tablet was formulated and evaluated using the sublimation technique to enhance gastroretentive drug delivery. Anhydrous theophylline was employed as the active pharmaceutical ingredient, combined with sublimation agents and hydroxypropyl methylcellulose as the gel-forming polymer. The resulting tablets exhibited high [...] Read more.
A gel-based floating matrix tablet was formulated and evaluated using the sublimation technique to enhance gastroretentive drug delivery. Anhydrous theophylline was employed as the active pharmaceutical ingredient, combined with sublimation agents and hydroxypropyl methylcellulose as the gel-forming polymer. The resulting tablets exhibited high porosity, immediate floatation, and sustained buoyancy for over 8 h. Optimization of the floating behavior and drug release profiles was achieved by adjusting the viscosity of and hydroxypropyl methylcellulose and the concentration of sublimation agents, specifically ammonium carbonate and menthol. These agents were selected for their effectiveness in creating a porous structure, thus reducing tablet density and enhancing floatation. Higher HPMC viscosity resulted in increased floating force, slower drug release, and improved swelling properties due to a slower erosion rate. A critical assessment of the balance between tablet porosity, mechanical strength, and drug release kinetics indicates that ammonium carbonate provided superior tablet hardness and lower friability compared to menthol, favoring a controlled release mechanism. The release dynamics of theophylline were best described by the anomalous (non-Fickian) diffusion model, suggesting a combined effect of diffusion and erosion. This research advances the development of gastroretentive drug delivery systems, highlighting the potential of sublimation-based floating matrix tablets for sustained drug release. Full article
(This article belongs to the Special Issue Polysaccharide: Gelation Arts)
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26 pages, 19363 KiB  
Article
Temperature-Regulated Synthesis of Hyaluronic Acid-Interpenetrated Polyacrylamide/Poly(Acrylic Acid Sodium Salt) Semi-Interpenetrated Polymer Network Gel for the Removal of Methyl Violet
by Nida Özcan and Nermin Orakdogen
Gels 2024, 10(9), 556; https://doi.org/10.3390/gels10090556 - 28 Aug 2024
Cited by 1 | Viewed by 1409
Abstract
An alternative synthetic pathway was proposed for the optimization of synthesis to find a better correlation between the swelling and elasticity of hyaluronic acid-interpenetrated gels via temperature regulation. An experimental design methodology was presented for the synthesis of polyacrylamide/poly(acrylic acid sodium salt)/hyaluronic acid, [...] Read more.
An alternative synthetic pathway was proposed for the optimization of synthesis to find a better correlation between the swelling and elasticity of hyaluronic acid-interpenetrated gels via temperature regulation. An experimental design methodology was presented for the synthesis of polyacrylamide/poly(acrylic acid sodium salt)/hyaluronic acid, PAAm/PSA/HyA, gels by modifying the one-pot procedure using free radical crosslinking copolymerization of AAm with the addition of anionic linear PSA chains in the presence of various amount of HyA, ranging between 0.05% and 0.20% (w/v). Semi-interpenetrated polymer network (IPN)-structured gels were designed with tunable elasticity, in which the extent of covalent crosslinking interactions is controlled by polymerization temperature ranging between −18 and 45 °C. Depending on the HyA content added in the synthesis and the polymerization temperature, the swelling ratio could be controlled. The addition of 0.05% (w/v) HyA increased the swelling of semi-IPNs, while the elastic modulus increased with increasing HyA content and decreased with the polymerization temperature. PAAm/PSA/HyA semi-IPNs showed the typical pH-sensitive swelling of anionic gels, and the swelling reached a maximum at a pH of 11.2. PAAm/PSA/HyA gels were tested for the removal of methyl violet from wastewater. Adsorption kinetics were shown to be well-fitted with the pseudo-second-order model using linear and nonlinear regression analysis. With the clear relationship between increased modulus and composition, this study enabled the fine-tuning of semi-IPN interactions by varying the polymerization temperature. Full article
(This article belongs to the Special Issue Polysaccharide: Gelation Arts)
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24 pages, 3881 KiB  
Article
Tailoring the Structure and Physico-Chemical Features of Cellulose-Based Hydrogels Using Multi-Epoxy Crosslinking Agents
by Raluca Nicu, Gabriela Lisa, Raluca Nicoleta Darie-Nita, Mihaela Iuliana Avadanei, Alexandra Bargan, Daniela Rusu and Diana Elena Ciolacu
Gels 2024, 10(8), 523; https://doi.org/10.3390/gels10080523 - 9 Aug 2024
Cited by 1 | Viewed by 976
Abstract
Hydrogel features can be designed and optimized using different crosslinking agents to meet specific requirements. In this regard, the present work investigates the physico-chemical features of cellulose-based hydrogels, designed by using different epoxy crosslinkers from the same glycidyl family, namely epichlorohydrin (ECH), 1,4-butanediol [...] Read more.
Hydrogel features can be designed and optimized using different crosslinking agents to meet specific requirements. In this regard, the present work investigates the physico-chemical features of cellulose-based hydrogels, designed by using different epoxy crosslinkers from the same glycidyl family, namely epichlorohydrin (ECH), 1,4-butanediol diglycidyl ether (BDDE), and trimethylolpropane triglycidyl ether (TMPTGE). The effect of the crosslinker’s structure (from simple to branched) and functionality (mono-, bi- and tri-epoxy groups) on the hydrogels’ features was studied. The performances of the hydrogels were investigated through the gel fraction, as well as by ATR-FTIR, DVS, SEM, DSC, and TG analyses. Also, the swelling and rheological behaviors of the hydrogels were examined. The advantages and limitations of each approach were discussed and a strong correlation between the crosslinker structure and the hydrogel properties was established. The formation of new ether bonds was evidenced by ATR-FTIR spectroscopy. It was emphasized that the pore size is directly influenced by the crosslinker type, namely, it decreases with the increasing number of epoxy groups from the crosslinker molecule, i.e., from 46 ± 11.1 µm (hydrogel CE, with ECH) to 12.3 ± 2.5 µm (hydrogel CB, with BDDE) and 6.7 ± 1.5 µm (hydrogel CT, with TMPTGE). The rheological behavior is consistent with the swelling data and hydrogel morphology, such as CE with the highest Qmax and the largest pore size being relatively more elastic than CB and CT. Instead, the denser matrices obtained by using crosslinkers with more complex structures have better thermal stability. The experimental results highlight the possibility of using a specific crosslinking agent, with a defined structure and functionality, in order to establish the main characteristics of hydrogels and, implicitly, to design them for a certain field of application. Full article
(This article belongs to the Special Issue Polysaccharide: Gelation Arts)
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16 pages, 7275 KiB  
Article
Gelation Behaviour of Pluronic F127/Polysaccharide Systems Revealed via Thioflavin T Fluorescence
by George-Alin Balan, Aurica Precupas and Iulia Matei
Gels 2023, 9(12), 939; https://doi.org/10.3390/gels9120939 - 30 Nov 2023
Cited by 2 | Viewed by 2040
Abstract
Fast, reliable methods for characterizing the micelle-to-gel transition in emerging Pluronic F127/polysaccharide materials are essential for tailoring their applications as in situ gelling delivery systems. This study describes a simple fluorimetric method based on the response to gelation of the molecular probe thioflavin [...] Read more.
Fast, reliable methods for characterizing the micelle-to-gel transition in emerging Pluronic F127/polysaccharide materials are essential for tailoring their applications as in situ gelling delivery systems. This study describes a simple fluorimetric method based on the response to gelation of the molecular probe thioflavin T (ThT). The techniques employed are (second derivative) steady-state and synchronous fluorescence. The capabilities of ThT as gelation reporter are tested for three model systems: Pluronic F127 (P16.6%), Pluronic F127/alginate (P16.6%ALG2%) and Pluronic F127/hyaluronic acid (P16.6%HA0.5%). We demonstrate that the changes in the short and long wavelength emissions of ThT allow accurate determination of the critical gelation temperatures in the investigated systems. The spectroscopic data providing information at molecular level are complemented with differential scanning microcalorimetric results revealing additional macroscopic insight into the micellization process. The gelation study is preceded by a solvatochromic analysis of ThT. Full article
(This article belongs to the Special Issue Polysaccharide: Gelation Arts)
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Review

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12 pages, 2655 KiB  
Review
Hydrogelation from Self-Assembled and Scaled-Down Chitin Nanofibers by the Modification of Highly Polar Substituents
by Jun-ichi Kadokawa
Gels 2023, 9(6), 432; https://doi.org/10.3390/gels9060432 - 23 May 2023
Cited by 3 | Viewed by 1674
Abstract
Chitin nanofibers (ChNFs) with a bundle structure were fabricated via regenerative self-assembly at the nanoscale from a chitin ion gel with an ionic liquid using methanol. Furthermore, the bundles were disentangled by partial deacetylation under alkaline conditions, followed by cationization and electrostatic repulsion [...] Read more.
Chitin nanofibers (ChNFs) with a bundle structure were fabricated via regenerative self-assembly at the nanoscale from a chitin ion gel with an ionic liquid using methanol. Furthermore, the bundles were disentangled by partial deacetylation under alkaline conditions, followed by cationization and electrostatic repulsion in aqueous acetic acid to obtain thinner nanofibers called scaled-down ChNFs. This review presents a method for hydrogelation from self-assembled and scaled-down ChNFs by modifying the highly polar substituents on ChNFs. The modification was carried out by the reaction of amino groups on ChNFs, which were generated by partial deacetylation, with reactive substituent candidates such as poly(2-oxazoline)s with electrophilic living propagating ends and mono- and oligosaccharides with hemiacetallic reducing ends. The substituents contributed to the formation of network structures from ChNFs in highly polar dispersed media, such as water, to produce hydrogels. Moreover, after the modification of the maltooligosaccharide primers on ChNFs, glucan phosphorylase-catalyzed enzymatic polymerization was performed from the primer chain ends to elongate the amylosic graft chains on ChNFs. The amylosic graft chains formed double helices between ChNFs, which acted as physical crosslinking points to construct network structures, giving rise to hydrogels. Full article
(This article belongs to the Special Issue Polysaccharide: Gelation Arts)
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