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Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition)
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Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition)

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

Deadline for manuscript submissions: 30 May 2025 | Viewed by 13307

Special Issue Editors

Dr. Irina Elena Raschip

E-Mail Website
Guest Editor
Petru Poni Institute of Macromolecular Chemistry, Grigore Ghica Voda Alley 41A, 700487 Iasi, Romania
Interests: biomaterials; porous gels; cryogel; functional materials
Special Issues, Collections and Topics in MDPI journals
Dr. Raluca Nicoleta Darie-Nita

E-Mail Website
Guest Editor
Petru Poni Institute of Macromolecular Chemistry, Grigore Ghica Voda Alley 41A, 700487 Iasi, Romania
Interests: reactive processing (natural and synthetic polymers); physico-chemical characterization of polymers and composites (rheological, mechanical, thermal, and surface properties); biodegradable polymers; applications of bio-based materials
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

This Special Issue on “Properties of Hydrogel, Aerogel, and Cryogel Composites” is dedicated to the latest advances in the preparation, properties, and applications of gel-type materials, highlighting key concepts relevant to the unique properties of hydrogels, aerogels, and cryogels.

Hydrogels have the ability to absorb impressive amounts of water or biological fluids within their peculiar structure of physically or chemically cross-linked 3D polymer networks. Hydrogels can be converted to aerogels following water removal via different approaches. Their distinctive features, such as super-absorbency, fluffiness, biocompatibility, viscoelasticity, and softness, underpin various applications, especially in the biomedical field.

Lately, porous gel materials have been found to offer more benefits than conventional hydrogels when applied as scaffolds for tissue engineering and regenerative medicine, substrates for cell culture, chromatographic materials, and carriers for controlled delivery of drugs or proteins. In this regard, cryogels have revolutionized the field of biomedical research with their super-elasticity and highly interconnected and open macroporous structure obtained by conducting polymerization/cross-linking at subzero temperatures. Furthermore, the development of sustainable composites has been a priority for polymer engineering research over the past two decades. Composite materials have been designed by blending two or more polymers or by entrapping inorganic or natural fillers of nano- or micro-sizes within a polymer matrix in order to tune the physical, chemical, and biological properties of hydrogels, aerogels and cryogels.

This Special Issue will cover new discoveries in the production of hydrogels, aerogels, and cryogels with a broad variety of morphologies and properties, which can be tailored for a particular application.

Dr. Irina Elena Raschip
Dr. Raluca-Nicoleta Darie-Nita
Guest Editors

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

  • biomaterials
  • porous gels
  • functional materials
  • viscoelasticity
  • interconnectivity
  • swelling
  • biomedical and environmental applications

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Published Papers (7 papers)

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Research

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17 pages, 9486 KiB  
Article
Effect of Ultrasound Time on Structural and Gelling Properties of Pea, Lupin, and Rice Proteins
by Natalia Riquelme, Paulo Díaz-Calderón, Alejandro Luarte and Carla Arancibia
Gels 2025, 11(4), 270; https://doi.org/10.3390/gels11040270 - 4 Apr 2025
Viewed by 209
Abstract
Plant proteins are garnering interest due to the growing demand for plant-based products, but their functionality in gel-based foods remains limited. Ultrasound (US) technology may improve the technological properties of proteins. Thus, the effect of US treatment time (0–15 min) on the structure [...] Read more.
Plant proteins are garnering interest due to the growing demand for plant-based products, but their functionality in gel-based foods remains limited. Ultrasound (US) technology may improve the technological properties of proteins. Thus, the effect of US treatment time (0–15 min) on the structure and gelling properties of pea, lupin, and rice proteins was evaluated. The results showed that the whiteness (~60%) of all freeze-dried proteins remained unchanged (p > 0.05), regardless of the US time. However, FT-IR analysis revealed progressive reductions in α-helix and β-sheet for pea and lupin proteins (~50%) with US time, indicating partial unfolding. In addition, microstructure analysis showed an ~80% reduction in aggregate size for these proteins, while rice protein exhibited minimal changes. Conversely, weak gels were formed with pea and lupin proteins treated after 5 and 10 min of US, respectively, whereas rice protein did not form gels. Furthermore, US treatment time significantly increased (p < 0.05) the mechanical moduli, resulting in more structured gels after longer treatment times (tan δ ~0.3 at 15 min of US). These findings suggest that US treatment enhances the gelling properties of pea and lupin proteins, making them more suitable for plant-based food applications such as yogurt or desserts. Full article
(This article belongs to the Special Issue Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition))
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23 pages, 4213 KiB  
Article
Deep Cleaning of Crystal Violet and Methylene Blue Dyes from Aqueous Solution by Dextran-Based Cryogel Adsorbents
by Maria Marinela Lazar, Roxana P. Damaschin, Irina Volf and Maria Valentina Dinu
Gels 2024, 10(9), 546; https://doi.org/10.3390/gels10090546 - 23 Aug 2024
Cited by 3 | Viewed by 1701
Abstract
Polysaccharides have recently attracted growing attention as adsorbents for various pollutants, since they can be extracted from a variety of renewable sources at low cost. An interesting hydrophilic and biodegradable polysaccharide is dextran (Dx), which is well-known for its applications in the food [...] Read more.
Polysaccharides have recently attracted growing attention as adsorbents for various pollutants, since they can be extracted from a variety of renewable sources at low cost. An interesting hydrophilic and biodegradable polysaccharide is dextran (Dx), which is well-known for its applications in the food industry and in medicine. To extend the application range of this biopolymer, in this study, we investigated the removal of crystal violet (CV) and methylene blue (MB) dyes from an aqueous solution by Dx-based cryogels using the batch technique. The cryogel adsorbents, consisting of cross-linked Dx embedding a polyphenolic (PF) extract of spruce bark, were prepared by the freeze-thawing approach. It was shown that the incorporation of PF into the Dx-based matrix induced a decrease in porosity, pore sizes and swelling ratio values. Moreover, the average pore sizes of the DxPF cryogels loaded with dyes further decreased from 42.30 ± 7.96 μm to 23.68 ± 2.69 μm, indicating a strong interaction between the functional groups of the cryogel matrix and those of the dye molecules. The sorption performances of the DxPF adsorbents were evaluated in comparison to those of the Dx cryogels and of the PF extract. The experimental sorption capacities of the DxPF cryogel adsorbents were higher in comparison to those of the Dx cryogels and the PF extract. The DxPF cryogels, particularly those with the highest PF contents (sample DxPF2), demonstrated sorption capacities of 1.2779 ± 0.0703 mmol·g−1, for CV, and 0.3238 ± 0.0121 mmol·g−1, for MB. The sorption mechanisms were analyzed using mathematical models, including Langmuir, Freundlich, Sips and Dubinin–Radushkevich isotherms, and kinetic models, like pseudo-first-order (PFO), pseudo-second-order (PSO), Elovich and intra-particle diffusion (IPD). The sorption process was best described by the Sips isotherm and PSO kinetic models, indicating chemisorption as the dominant mechanism. This study outlines the importance of developing advanced renewable materials for environmental applications. Full article
(This article belongs to the Special Issue Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition))
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20 pages, 2454 KiB  
Article
Impact of Hydroxyapatite on Gelatin/Oxidized Alginate 3D-Printed Cryogel Scaffolds
by Ainur Zhanbassynova, Fariza Mukasheva, Madi Abilev, Dmitriy Berillo, Alexander Trifonov and Dana Akilbekova
Gels 2024, 10(6), 406; https://doi.org/10.3390/gels10060406 - 18 Jun 2024
Cited by 2 | Viewed by 1742
Abstract
Fabrication of scaffolds via 3D printing is a promising approach for tissue engineering. In this study, we combined 3D printing with cryogenic crosslinking to create biocompatible gelatin/oxidized alginate (Gel/OxAlg) scaffolds with large pore sizes, beneficial for bone tissue regeneration. To enhance the osteogenic [...] Read more.
Fabrication of scaffolds via 3D printing is a promising approach for tissue engineering. In this study, we combined 3D printing with cryogenic crosslinking to create biocompatible gelatin/oxidized alginate (Gel/OxAlg) scaffolds with large pore sizes, beneficial for bone tissue regeneration. To enhance the osteogenic effects and mechanical properties of these scaffolds, we evaluated the impact of hydroxyapatite (HAp) on the rheological characteristics of the 2.86% (1:1) Gel/OxAlg ink. We investigated the morphological and mechanical properties of scaffolds with low, 5%, and high 10% HAp content, as well as the resulting bio- and osteogenic effects. Scanning electron microscopy revealed a reduction in pore sizes from 160 to 180 µm (HAp-free) and from 120 to 140 µm for both HAp-containing scaffolds. Increased stability and higher Young’s moduli were measured for 5% and 10% HAp (18 and 21 kPa, respectively) compared to 11 kPa for HAp-free constructs. Biological assessments with mesenchymal stem cells indicated excellent cytocompatibility and osteogenic differentiation in all scaffolds, with high degree of mineralization in HAp-containing constructs. Scaffolds with 5% HAp exhibited improved mechanical characteristics and shape fidelity, demonstrated positive osteogenic impact, and enhanced bone tissue formation. Increasing the HAp content to 10% did not show any advantages in osteogenesis, offering a minor increase in mechanical strength at the cost of significantly compromised shape fidelity. Full article
(This article belongs to the Special Issue Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition))
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12 pages, 2537 KiB  
Article
How the Crosslinker Amount Influences the Final Properties of Hydroxyethyl Methacrylate Cryogels
by Giuseppe Proietto Salanitri, Enrica Luzzi, Daniele Caretti, Tommaso Mecca, Sabrina C. Carroccio and Andrea A. Scamporrino
Gels 2024, 10(3), 163; https://doi.org/10.3390/gels10030163 - 22 Feb 2024
Cited by 1 | Viewed by 2038
Abstract
The investigation of the mechanical, thermal, and adsorption properties of hydroxyethyl methacrylate (HEMA) cryogels as a function of a reactant ratio is herein reported to better address materials for specific applications. To this aim, cryogels have been synthesized using different monomer/crosslinker (N,N′-methylene-bisacrylamide–MBAA) ratios. [...] Read more.
The investigation of the mechanical, thermal, and adsorption properties of hydroxyethyl methacrylate (HEMA) cryogels as a function of a reactant ratio is herein reported to better address materials for specific applications. To this aim, cryogels have been synthesized using different monomer/crosslinker (N,N′-methylene-bisacrylamide–MBAA) ratios. The study of SEM images made it possible to identify the trend in the material’s macroporosity. As would be expected, the average measured pore width decreased as the amount of MBAA increased while the number of pores grew. Swelling capacity ranges from 8.7 gW/ggel (grams of water per gram of gel) to 9.3 gW/ggel. These values are strictly connected with the pore’s size and distribution, revealing that the water uptake for the most crosslinked sample is inferior to other samples. The equilibrium-adsorption capacity (Qe) towards the methylene violet (MV) was also assessed, revealing no remarkable differences after 24 h of a batch test. As expected, thermogravimetric analysis (TGA) also showed no significant changes in stability that ranged from a maximum weight loss temperature (T Max) of 420 °C to 425 °C, which increased as a function of crosslinker content. Conversely, compression strength measurements showed a notable difference of about 50% in modulus (Ec), moving from the higher to the lower HEMA/MBAA ratio. These new comparative results indicate how slight variations in the reactant’s ratio can steadily improve the mechanical properties of the HEMA cryogel without affecting its adsorption efficiency. This can be helpful in the design of materials for water and energy purposes. Since swelling properties are needed in the case of biomedical applications, the HEMA/MBAA ratio should be tuned versus high values. Full article
(This article belongs to the Special Issue Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition))
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18 pages, 3752 KiB  
Article
Agarose Cryogels: Production Process Modeling and Structural Characterization
by Raffaele Mancino, Diego Caccavo, Anna Angela Barba, Gaetano Lamberti, Alice Biasin, Angelo Cortesi, Gabriele Grassi, Mario Grassi and Michela Abrami
Gels 2023, 9(9), 765; https://doi.org/10.3390/gels9090765 - 20 Sep 2023
Cited by 1 | Viewed by 2169
Abstract
A cryogel is a cross-linked polymer network with different properties that are determined by its manufacturing technique. The formation of a cryogel occurs at low temperatures and results in a porous structure whose pore size is affected by thermal conditions. The adjustable pore [...] Read more.
A cryogel is a cross-linked polymer network with different properties that are determined by its manufacturing technique. The formation of a cryogel occurs at low temperatures and results in a porous structure whose pore size is affected by thermal conditions. The adjustable pore sizes of cryogels make them attractive for diverse applications. In this study, the influence of the external operational temperature, which affects the cooling and freezing rates, on the production of cryogels with 2% w/w agarose is investigated. Moreover, a mathematical model is developed to simulate the cryogel production process and provide an initial estimate of the pore size within the structure. The predictions of the model, supported by qualitative light microscopy images, demonstrate that cryogels produced at higher process temperatures exhibit larger pore sizes. Moreover, the existence of pore size distribution within the gel structure is confirmed. Finally, stress relaxation tests, coupled with an image analysis, validates that cryogels produced at lower temperatures possess a higher stiffness and slower water release rates. Full article
(This article belongs to the Special Issue Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition))
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15 pages, 5584 KiB  
Article
Ice-Templated and Cross-Linked Xanthan-Based Hydrogels: Towards Tailor-Made Properties
by Irina Elena Raschip, Nicusor Fifere, Maria Marinela Lazar, Gabriela-Elena Hitruc and Maria Valentina Dinu
Gels 2023, 9(7), 528; https://doi.org/10.3390/gels9070528 - 29 Jun 2023
Cited by 5 | Viewed by 2108
Abstract
The use of polysaccharides with good film-forming properties in food packaging systems is a promising area of research. Xanthan gum (XG), an extracellular polysaccharide, has many industrial uses, including as a common food additive (E415). It is an effective thickening agent, emulsifier, and [...] Read more.
The use of polysaccharides with good film-forming properties in food packaging systems is a promising area of research. Xanthan gum (XG), an extracellular polysaccharide, has many industrial uses, including as a common food additive (E415). It is an effective thickening agent, emulsifier, and stabilizer that prevents ingredients from separating. Nevertheless, XG-based polymer films have some disadvantages, such as poor mechanical properties and high hydrophilic features, which reduce their stability when exposed to moisture and create difficulties in processing and handling. Thus, the objective of this work was to stabilize a XG matrix by cross-linking it with glycerol diglycidyl ether, 1,4-butanediol diglycidyl ether, or epichlorohydrin below the freezing point of the reaction mixture. Cryogelation is an ecological, friendly, and versatile method of preparing biomaterials with improved physicochemical properties. Using this technique, XG-based cryogels were successfully prepared in the form of microspheres, monoliths, and films. The XG-based cryogels were characterized by FTIR, SEM, AFM, swelling kinetics, and compressive tests. A heterogeneous morphology with interconnected pores, with an average pore size depending on both the nature of the cross-linker and the cross-linking ratio, was found. The use of a larger amount of cross-linker led to both a much more compact structure of the pore walls and to a significant decrease in the average pore size. The uniaxial compression tests indicated that the XG-based cryogels cross-linked with 1,4-butanediol diglycidyl ether exhibited the best elasticity, sustaining maximum deformations of 97.67%, 90.10%, and 81.80%, respectively. Full article
(This article belongs to the Special Issue Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition))
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Review

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20 pages, 2552 KiB  
Review
Advances and Functional Integration of Hydrogel Composites as Drug Delivery Systems in Contemporary Dentistry
by Dragos Nicolae Fratila, Dragos Ioan Virvescu, Ionut Luchian, Monica Hancianu, Elena Raluca Baciu, Oana Butnaru and Dana Gabriela Budala
Gels 2024, 10(10), 661; https://doi.org/10.3390/gels10100661 - 16 Oct 2024
Viewed by 2535
Abstract
This study explores the recent advances of and functional insights into hydrogel composites, materials that have gained significant attention for their versatile applications across various fields, including contemporary dentistry. Hydrogels, known for their high water content and biocompatibility, are inherently soft but often [...] Read more.
This study explores the recent advances of and functional insights into hydrogel composites, materials that have gained significant attention for their versatile applications across various fields, including contemporary dentistry. Hydrogels, known for their high water content and biocompatibility, are inherently soft but often limited by mechanical fragility. Key areas of focus include the customization of hydrogel composites for biomedical applications, such as drug delivery systems, wound dressings, and tissue engineering scaffolds, where improved mechanical properties and bioactivity are critical. In dentistry, hydrogels are utilized for drug delivery systems targeting oral diseases, dental adhesives, and periodontal therapies due to their ability to adhere to the mucosa, provide localized treatment, and support tissue regeneration. Their unique properties, such as mucoadhesion, controlled drug release, and stimuli responsiveness, make them ideal candidates for treating oral conditions. This review highlights both experimental breakthroughs and theoretical insights into the structure–property relationships within hydrogel composites, aiming to guide future developments in the design and application of these multifunctional materials in dentistry. Ultimately, hydrogel composites represent a promising frontier for advancing materials science with far-reaching implications in healthcare, environmental technology, and beyond. Full article
(This article belongs to the Special Issue Properties of Hydrogels, Aerogels, and Cryogels Composites (2nd Edition))
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