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Gels
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Innovative Biopolymer-Based Hydrogels
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Innovative Biopolymer-Based Hydrogels

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

Deadline for manuscript submissions: closed (24 July 2023) | Viewed by 22047

Special Issue Editors

Dr. Diana Elena Ciolacu

E-Mail Website
Guest Editor
Laboratory of Polymer Physical Chemistry, “Petru Poni” Institute of Macromolecular Chemistry, Iasi, Romania
Interests: cellulose; hydrogel; cross-linking; nanocellulose; lignin; polyssacharides; drug release
Special Issues, Collections and Topics in MDPI journals
Dr. Florin Ciolacu

E-Mail Website
Guest Editor
Department of Natural and Synthetic Polymers, “Gheorghe Asachi” Technical University of Iasi, Iasi, Romania
Interests: biopolymers; cellulose; hemicelluloses; lignin; chitosan; nanocelluloses; nanopaper; nanomaterials; paper technology and wet-end chemistry; deinking technology; physics of fibrous structures; paper rheology; polymer-based conservation materials; polymer-based papermaking additives; paper-based microfluidics; active and smart paper-based packaging
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Hydrogels are extremely versatile materials with the potential for wide use in various fields. Their exceptional physicochemical characteristics allow them to be applied from environmental and agricultural applications to pharmaceutical and biomedical areas. Research efforts to upgrade hydrogels into ever-more sophisticated materials with ever-more complex structures and properties require extensive interdisciplinary collaboration (chemistry, biology, and material science) in order to accomplish highly specific and complex biological tasks and to effectively mimic their bio-counterpart.

This Special Issue aims to focus attention on the cutting-edge knowledge related to biopolymer-based hydrogels, to highlight the progress of them in multidisciplinary fields, and to emphasize the new challenges and opportunities, respectively.

We welcome original research articles and review papers related to new strategies in the design of the chemical compositions, functionalities, and properties of hydrogels, as well as the tailoring of the hydrogel performances in controlled drug delivery, wound dressings, tissue engineering and regenerative medicine, gene therapy, cell immobilization, hygiene products, and many others.

Dr. Diana Elena Ciolacu
Dr. Florin Ciolacu
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 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.

Keywords

  • biopolymers
  • hydrogels
  • biomaterials
  • stimuli-responsive
  • drug delivery
  • wound healing
  • tissue engineering
  • regenerative medicine

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Published Papers (10 papers)

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Research

Jump to: Review

17 pages, 4270 KiB  
Article
Degradation Kinetics of Disulfide Cross-Linked Microgels: Real-Time Monitoring by Confocal Microscopy
by Iris G. Mercer, Angelina N. Italiano, Irina G. Gazaryan, Aaron B. Steiner and Sergey V. Kazakov
Gels 2023, 9(10), 782; https://doi.org/10.3390/gels9100782 - 25 Sep 2023
Viewed by 1142
Abstract
Although biodegradable microgels represent a useful drug delivery system, questions remain regarding the kinetics of gel degradation and subsequent drug release. Spherical microgels (~Ø10–300 µm) were synthesized using an inverse suspension polymerization method. Specifically, acrylamide and acrylonitrile monomers were thermally co-polymerized with N [...] Read more.
Although biodegradable microgels represent a useful drug delivery system, questions remain regarding the kinetics of gel degradation and subsequent drug release. Spherical microgels (~Ø10–300 µm) were synthesized using an inverse suspension polymerization method. Specifically, acrylamide and acrylonitrile monomers were thermally co-polymerized with N,N’-bis(acryloyl)cystamine as a cross-linker with disulfide bridges. The kinetics and mechanism of degradation of these cross-linked, degradable, fluorescently labeled microgels (PAAm-AN-BAC-FA) were quantitatively studied under confocal microscopy at various concentrations of glutathione (reducing agent) ranging from 0.06 to 91.8 mM. It was found that polymer network degradation via the cleavage of disulfide bonds was accompanied by two overlapping processes: diffusion-driven swelling and dissolution-driven erosion. A slow increase in microgel size (swelling) resulted from partial de-cross-linking in the bulk of the microgel, whereas a faster decrease in fluorescence intensity (erosion) resulted from the complete cleavage of disulfide bonds and the release of uncleaved polymeric chains from the microgel immediate surface into the solution. Swelling and erosion exhibited distinct kinetics and characteristic times. Importantly, the dependence of kinetics on glutathione concentration for both swelling and erosion suggests that degradation would occur faster in cancer cells (higher concentration of reductants) than in normal cells (lower concentration of reductants), such that drug release profiles would be correspondingly different. A greater comprehension of microgel degradation kinetics would help in (i) predicting the drug release profiles for novel multifunctional drug delivery systems and (ii) using redox-sensitive degradable hydrogel particles to determine the concentrations of reducing agents either in vitro or in vivo. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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20 pages, 7987 KiB  
Article
Remote Positioning of Spherical Alginate Ferrogels in a Fluid Flow by a Magnetic Field: Experimental and Computer Simulation
by Felix Blyakhman, Alexander Safronov, Ilya Starodumov, Darya Kuznetsova and Galina Kurlyandskaya
Gels 2023, 9(9), 711; https://doi.org/10.3390/gels9090711 - 01 Sep 2023
Cited by 2 | Viewed by 941
Abstract
This work belongs to the development of mechanical force-responsive drug delivery systems based on remote stimulation by an external magnetic field at the first stage, assisting the positioning of a ferrogel-based targeted delivery platform in a fluid flow. Magnetically active biopolymer beads were [...] Read more.
This work belongs to the development of mechanical force-responsive drug delivery systems based on remote stimulation by an external magnetic field at the first stage, assisting the positioning of a ferrogel-based targeted delivery platform in a fluid flow. Magnetically active biopolymer beads were considered a prototype implant for the needs of replacement therapy and regenerative medicine. Spherical calcium alginate ferrogels (FGs)~2.4 mm in diameter, filled with a 12.6% weight fraction of magnetite particles of 200–300 nm in diameter, were synthesized. A detailed characterization of the physicochemical and magnetic properties of FGs was carried out, as were direct measurements of the field dependence of the attractive force for FG-beads. The hydrodynamic effects of the positioning of FG-beads in a fluid flow by a magnetic field were studied experimentally in a model vessel with a fluid stream. Experimental results were compared with the results of mathematical and computer modeling, showing reasonable agreement. The contributions of the hydrodynamic and magnetic forces acting on the FG-bead in a fluid flow were discussed. Obtained forces for a single ferrogel implant were as high as 0 to 10−4 N for the external field range of 0 to 35 kA/m, perfectly in the range of mechanical force stimuli in biological systems. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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18 pages, 4407 KiB  
Article
Evaluation of Poly(vinyl alcohol)–Xanthan Gum Hydrogels Loaded with Neomycin Sulfate as Systems for Drug Delivery
by Diana Serbezeanu, Manuela Maria Iftime, Gabriela-Liliana Ailiesei, Alina-Mirela Ipate, Alexandra Bargan, Tǎchiţǎ Vlad-Bubulac and Cristina Mihaela Rîmbu
Gels 2023, 9(8), 655; https://doi.org/10.3390/gels9080655 - 14 Aug 2023
Cited by 2 | Viewed by 1236
Abstract
In recent years, multidrug-resistant bacteria have developed the ability to resist multiple antibiotics, limiting the available options for effective treatment. Raising awareness and providing education on the appropriate use of antibiotics, as well as improving infection control measures in healthcare facilities, are crucial [...] Read more.
In recent years, multidrug-resistant bacteria have developed the ability to resist multiple antibiotics, limiting the available options for effective treatment. Raising awareness and providing education on the appropriate use of antibiotics, as well as improving infection control measures in healthcare facilities, are crucial steps to address the healthcare crisis. Further, innovative approaches must be adopted to develop novel drug delivery systems using polymeric matrices as carriers and support to efficiently combat such multidrug-resistant bacteria and thus promote wound healing. In this context, the current work describes the use of two biocompatible and non-toxic polymers, poly(vinyl alcohol) (PVA) and xanthan gum (XG), to achieve hydrogel networks through cross-linking by oxalic acid following the freezing/thawing procedure. PVA/XG-80/20 hydrogels were loaded with different quantities of neomycin sulfate to create promising low-class topical antibacterial formulations with enhanced antimicrobial effects. The inclusion of neomycin sulfate in the hydrogels is intended to impart them with powerful antimicrobial properties, thereby facilitating the development of exceptionally efficient topical antibacterial formulations. Thus, incorporating higher quantities of neomycin sulfate in the PVA/XG-80/20-2 and PVA/XG-80/20-3 formulations yielded promising cycling characteristics. These formulations exhibited outstanding removal efficiency, exceeding 80% even after five cycles, indicating remarkable and consistent adsorption performance with repeated use. Furthermore, both PVA/XG-80/20-2 and PVA/XG-80/20-3 formulations outperformed the drug-free sample, PVA/XG-80/20, demonstrating a significant enhancement in maximum compressive stress. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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13 pages, 3474 KiB  
Article
Autoclaving-Triggered Hydrogelation of Chitosan-Gluconic acid Conjugate Aqueous Solution for Wound Healing
by Yusuke Yamashita, Yoshihiro Ohzuno, Yoichi Saito, Yukio Fujiwara, Masahiro Yoshida and Takayuki Takei
Gels 2023, 9(4), 280; https://doi.org/10.3390/gels9040280 - 29 Mar 2023
Cited by 7 | Viewed by 1318
Abstract
Moist wound healing is known to heal wounds faster than dry wound healing. Hydrogel wound dressings are suitable for moist wound healing because of their hyperhydrous structure. Chitosan, a natural polymer, promotes wound healing by stimulating inflammatory cells and releasing bioactive compounds. Therefore, [...] Read more.
Moist wound healing is known to heal wounds faster than dry wound healing. Hydrogel wound dressings are suitable for moist wound healing because of their hyperhydrous structure. Chitosan, a natural polymer, promotes wound healing by stimulating inflammatory cells and releasing bioactive compounds. Therefore, chitosan hydrogel has great potential as a wound dressing. In our previous study, physically crosslinked chitosan hydrogels were successfully prepared solely by freeze-thawing of chitosan-gluconic acid conjugate (CG) aqueous solution without using any toxic additives. Furthermore, the CG hydrogels could be sterilized by autoclaving (steam sterilization). In this study, we showed that autoclaving (121 °C, 20 min) of a CG aqueous solution simultaneously achieved gelation of the solution and sterilization of the hydrogel. Hydrogelation of CG aqueous solution by autoclaving is also physically crosslinking without any toxic additives. Further, we showed that the CG hydrogels retained favorable biological properties of the CG hydrogels prepared by freeze-thawing and subsequent autoclaving. These results indicated that CG hydrogels prepared by autoclaving were promising as wound dressings. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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37 pages, 17529 KiB  
Article
Phosphonation of Alginate–Polyethyleneimine Beads for the Enhanced Removal of Cs(I) and Sr(II) from Aqueous Solutions
by Khalid A. M. Salih, Kanggen Zhou, Mohammed F. Hamza, Hamed Mira, Yuezhou Wei, Shunyan Ning, Eric Guibal and Waheed M. Salem
Gels 2023, 9(2), 152; https://doi.org/10.3390/gels9020152 - 11 Feb 2023
Cited by 4 | Viewed by 2056
Abstract
Although Cs(I) and Sr(II) are not strategic and hazardous metal ions, their recovery from aqueous solutions is of great concern for the nuclear industry. The objective of this work consists of designing a new sorbent for the simultaneous recovery of these metals with [...] Read more.
Although Cs(I) and Sr(II) are not strategic and hazardous metal ions, their recovery from aqueous solutions is of great concern for the nuclear industry. The objective of this work consists of designing a new sorbent for the simultaneous recovery of these metals with selectivity against other metals. The strategy is based on the functionalization of algal/polyethyleneimine hydrogel beads by phosphonation. The materials are characterized by textural, thermo-degradation, FTIR, elemental, titration, and SEM-EDX analyses to confirm the chemical modification. To evaluate the validity of this modification, the sorption of Cs(I) and Sr(II) is compared with pristine support under different operating conditions: the pH effect, kinetics, and isotherms are investigated in mono-component and binary solutions, before investigating the selectivity (against competitor metals) and the possibility to reuse the sorbent. The functionalized sorbent shows a preference for Sr(II), enhanced sorption capacities, a higher stability at recycling, and greater selectivity against alkali, alkaline-earth, and heavy metal ions. Finally, the sorption properties are compared for Cs(I) and Sr(II) removal in a complex solution (seawater sample). The combination of these results confirms the superiority of phosphonated sorbent over pristine support with promising performances to be further evaluated with effluents containing radionuclides. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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16 pages, 7576 KiB  
Article
Characterization of a Bioink Combining Extracellular Matrix-like Hydrogel with Osteosarcoma Cells: Preliminary Results
by Giada Loi, Gaia Stucchi, Franca Scocozza, Laura Cansolino, Francesca Cadamuro, Elena Delgrosso, Federica Riva, Cinzia Ferrari, Laura Russo and Michele Conti
Gels 2023, 9(2), 129; https://doi.org/10.3390/gels9020129 - 03 Feb 2023
Cited by 9 | Viewed by 2316
Abstract
Three-dimensional (3D) bioprinting allows the production of artificial 3D cellular microenvironments thanks to the controlled spatial deposition of bioinks. Proper bioink characterization is required to achieve the essential characteristics of printability and biocompatibility for 3D bioprinting. In this work, a protocol to standardize [...] Read more.
Three-dimensional (3D) bioprinting allows the production of artificial 3D cellular microenvironments thanks to the controlled spatial deposition of bioinks. Proper bioink characterization is required to achieve the essential characteristics of printability and biocompatibility for 3D bioprinting. In this work, a protocol to standardize the experimental characterization of a new bioink is proposed. A functionalized hydrogel based on gelatin and chitosan was used. The protocol was divided into three steps: pre-printing, 3D bioprinting, and post-printing. For the pre-printing step, the hydrogel formulation and its repeatability were evaluated. For the 3D-bioprinting step, the hydrogel-printability performance was assessed through qualitative and quantitative tests. Finally, for the post-printing step, the hydrogel biocompatibility was investigated using UMR-106 cells. The hydrogel was suitable for printing grids with good resolution from 4 h after the cross-linker addition. To guarantee a constant printing pressure, it was necessary to set the extruder to 37 °C. Furthermore, the hydrogel was shown to be a valid biomaterial for the UMR-106 cells’ growth. However, fragmentation of the constructs appeared after 14 days, probably due to the negative osteosarcoma-cell interference. The protocol that we describe here denotes a strong approach to bioink characterization to improve standardization for future biomaterial screening and development. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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10 pages, 4630 KiB  
Communication
Effect of Grape Seed Extract on Gelatin-Based Edible 3D-Hydrogels for Cultured Meat Application
by Kummara Madhusudana Rao, Hyeon Jin Kim, Soyeon Won, Soon Mo Choi and Sung Soo Han
Gels 2023, 9(1), 65; https://doi.org/10.3390/gels9010065 - 12 Jan 2023
Cited by 4 | Viewed by 2311
Abstract
Cell-cultured meat, which is artificial meat made by in vitro cultivation of animal-derived cells, has attracted a lot of interest as a potential source of protein in the future. Porous hydrogels are crucial components that can be used as an artificial extracellular matrix [...] Read more.
Cell-cultured meat, which is artificial meat made by in vitro cultivation of animal-derived cells, has attracted a lot of interest as a potential source of protein in the future. Porous hydrogels are crucial components that can be used as an artificial extracellular matrix (ECM) to provide cell growth for generating cultured meat. In this study, we highlight the effects of grape seed extract (proanthocyanidins, PC) on the physicochemical and biological functions (bovine satellite muscle cell (BSC) growth and adhesion) of an edible gelatin (GL)-based hydrogel. The freeze-dried hydrogels had good compressive characteristics with pore sizes ranging from 100 to 300 μm. BSCs were able to grow and attach to porous GL-PC hydrogels. These studies suggested that the developed hydrogels using edible materials and made by employing a low-cost method may serve in the cell growth of muscle cells for cultured meat applications. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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23 pages, 8595 KiB  
Article
Synthesis and Characterization of Zinc Oxide Nanoparticles Stabilized with Biopolymers for Application in Wound-Healing Mixed Gels
by Andrey V. Blinov, Maksim D. Kachanov, Alexey A. Gvozdenko, Andrey A. Nagdalian, Anastasiya A. Blinova, Zafar A. Rekhman, Alexey B. Golik, Dmitriy S. Vakalov, David G. Maglakelidze, Anzhela G. Nagapetova, Alexander D. Pokhilko and Irina V. Burkina
Gels 2023, 9(1), 57; https://doi.org/10.3390/gels9010057 - 11 Jan 2023
Cited by 16 | Viewed by 2483
Abstract
A method for the synthesis of ZnO nanoparticles (ZnO NPs) gels was developed. ZnO NPs were obtained through a sol–gel method with zinc acetate usage as a precursor. Optimization of the method of synthesis of ZnO NPs gel has been carried out. It [...] Read more.
A method for the synthesis of ZnO nanoparticles (ZnO NPs) gels was developed. ZnO NPs were obtained through a sol–gel method with zinc acetate usage as a precursor. Optimization of the method of synthesis of ZnO NPs gel has been carried out. It was observed that the most stable ZnO NPs gels are formed at room temperature, pH = 8 and molar concentration of zinc C(Zn2+) = 0.05–0.2 M. It was shown that the addition of polysaccharide significantly affects the rheological properties and microstructure of ZnO NPs gels. We found that the optimal polysaccharide for the synthesis of ZnO NPs gels is hydroxyethyl cellulose. It is shown that the microstructure of a gel of ZnO NPs stabilized with hydroxyethyl cellulose is represented by irregularly shaped particles that are assembled into aggregates, with sizes ranging from 150 to 1400 nm. A significant hysteresis region is observed in a gel of ZnO NPs stabilized with hydroxyethyl cellulose. The process of interaction of ZnO NPs with polysaccharides was investigated. It was shown that the interaction of ZnO NPs with polysaccharides occurs through a charged hydroxyl group. In the experiment, a sample of a gel of ZnO NPs modified with hydroxyethyl cellulose was tested. It was shown that the gel of ZnO NPs modified with hydroxyethyl cellulose has a pronounced regenerative effect on burn wounds, which is significantly higher than that of the control group and the group treated with a gel of ZnO microparticles (MPs) and hydroxyethyl cellulose. It is also shown that the rate of healing of burn wounds in animals treated with gel of ZnO nanoparticles with hydroxyethyl cellulose (group 3) is 16.23% higher than in animals treated with gel of ZnO microparticles with hydroxyethyl cellulose (group 2), and 24.33% higher than in the control group treated with hydroxyethyl cellulose. The average rate of healing of burn wounds for the entire experimental period in experimental animals of group 3 is 1.26 and 1.54 times higher than in animals of group 2 and control group, respectively. An experimental study of a gel of ZnO NPs modified with hydroxyethyl cellulose has shown the effectiveness of its use in modeling the healing of skin wounds through primary tension. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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15 pages, 3635 KiB  
Article
One-Step Preparation of Carboxymethyl Cellulose—Phytic Acid Hydrogels with Potential for Biomedical Applications
by Alina Ghilan, Loredana Elena Nita, Daniela Pamfil, Natalia Simionescu, Nita Tudorachi, Daniela Rusu, Alina Gabriela Rusu, Maria Bercea, Irina Rosca, Diana Elena Ciolacu and Aurica P. Chiriac
Gels 2022, 8(10), 647; https://doi.org/10.3390/gels8100647 - 12 Oct 2022
Cited by 7 | Viewed by 2523
Abstract
Hydrogels based on natural, biodegradable materials have gained considerable interest in the medical field due to their improved drug delivery profiles and tissue-mimicking architecture. In this regard, this study was devoted to the preparation and characterization of new physically crosslinked hydrogels based on [...] Read more.
Hydrogels based on natural, biodegradable materials have gained considerable interest in the medical field due to their improved drug delivery profiles and tissue-mimicking architecture. In this regard, this study was devoted to the preparation and characterization of new physically crosslinked hydrogels based on carboxymethyl cellulose and an unconventional crosslinking agent, phytic acid. Phytic acid, in addition to its antioxidant and antibacterial effects, can improve the biological properties and stability of gels, without adding toxicity. Fourier transform infrared (FTIR) spectroscopy, rheological studies and thermal analysis confirmed the hydrogel formation. The influence of the ratio between the cellulose derivative and the crosslinker upon the morphological structure and water uptake was evidenced by scanning electron microscopy (SEM) and swelling measurements in simulated body fluids. Furthermore, procaine was entrapped within the hydrogels and used as a model drug for in vitro studies, which highlighted the dependence of the drug release on the phytic acid content of the matrix. The materials demonstrated antibacterial effects against Escherichia coli and Staphylococcus aureus bacteria. The biocompatibility was assessed on fibroblast cells, and according to our results, hydrogels can improve cell viability highlighting the potential of these systems as therapeutic scaffolds for skin tissue engineering. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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Review

Jump to: Research

45 pages, 3279 KiB  
Review
A Review of Patents and Innovative Biopolymer-Based Hydrogels
by Snežana Ilić-Stojanović, Ljubiša Nikolić and Suzana Cakić
Gels 2023, 9(7), 556; https://doi.org/10.3390/gels9070556 - 07 Jul 2023
Cited by 13 | Viewed by 4436
Abstract
Biopolymers represent a great resource for the development and utilization of new functional materials due to their particular advantages such as biocompatibility, biodegradability and non-toxicity. “Intelligent gels” sensitive to different stimuli (temperature, pH, ionic strength) have different applications in many industries (e.g., pharmacy, [...] Read more.
Biopolymers represent a great resource for the development and utilization of new functional materials due to their particular advantages such as biocompatibility, biodegradability and non-toxicity. “Intelligent gels” sensitive to different stimuli (temperature, pH, ionic strength) have different applications in many industries (e.g., pharmacy, biomedicine, food). This review summarizes the research efforts presented in the patent and non-patent literature. A discussion was conducted regarding biopolymer-based hydrogels such as natural proteins (i.e., fibrin, silk fibroin, collagen, keratin, gelatin) and polysaccharides (i.e., chitosan, hyaluronic acid, cellulose, carrageenan, alginate). In this analysis, the latest advances in the modification and characterization of advanced biopolymeric formulations and their state-of-the-art administration in drug delivery, wound healing, tissue engineering and regenerative medicine were addressed. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)
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