Editor’s Choice Articles

Editor’s Choice articles are based on recommendations by the scientific editors of MDPI journals from around the world. Editors select a small number of articles recently published in the journal that they believe will be particularly interesting to readers, or important in the respective research area. The aim is to provide a snapshot of some of the most exciting work published in the various research areas of the journal.

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26 pages, 4543 KiB  
Review
Bio-Based Aerogels in Energy Storage Systems
by Vilko Mandić, Arijeta Bafti, Ivana Panžić and Floren Radovanović-Perić
Gels 2024, 10(7), 438; https://doi.org/10.3390/gels10070438 - 30 Jun 2024
Cited by 1 | Viewed by 1299
Abstract
Bio-aerogels have emerged as promising materials for energy storage, providing a sustainable alternative to conventional aerogels. This review addresses their syntheses, properties, and characterization challenges for use in energy storage devices such as rechargeable batteries, supercapacitors, and fuel cells. Derived from renewable sources [...] Read more.
Bio-aerogels have emerged as promising materials for energy storage, providing a sustainable alternative to conventional aerogels. This review addresses their syntheses, properties, and characterization challenges for use in energy storage devices such as rechargeable batteries, supercapacitors, and fuel cells. Derived from renewable sources (such as cellulose, lignin, and chitosan), bio-based aerogels exhibit mesoporosity, high specific surface area, biocompatibility, and biodegradability, making them advantageous for environmental sustainability. Bio-based aerogels serve as electrodes and separators in energy storage systems, offering desirable properties such as high specific surface area, porosity, and good electrical conductivity, enhancing the energy density, power density, and cycle life of devices. Recent advancements highlight their potential as anode materials for lithium-ion batteries, replacing non-renewable carbon materials. Studies have shown excellent cycling stability and rate performance for bio-aerogels in supercapacitors and fuel cells. The yield properties of these materials, primarily porosity and transport phenomena, demand advanced characterization methods, and their synthesis and processing methods significantly influence their production, e.g., sol–gel and advanced drying. Bio-aerogels represent a sustainable solution for advancing energy storage technologies, despite challenges such as scalability, standardization, and cost-effectiveness. Future research aims to improve synthesis methods and explore novel applications. Bio-aerogels, in general, provide a healthier path to technological progress. Full article
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19 pages, 10524 KiB  
Article
Antimicrobial Hydrogels Based on Cationic Curdlan Derivatives for Biomedical Applications
by Dana M. Suflet, Irina Popescu, Magdalena-Cristina Stanciu and Cristina Mihaela Rimbu
Gels 2024, 10(7), 424; https://doi.org/10.3390/gels10070424 - 27 Jun 2024
Viewed by 904
Abstract
Hydrogels based on biocompatible polysaccharides with biological activity that can slowly release an active principle at the wound site represent promising alternatives to traditional wound dressing materials. In this respect, new hydrogels based on curdlan derivative with 2-hydroxypropyl dimethyl octyl ammonium groups (QCurd) [...] Read more.
Hydrogels based on biocompatible polysaccharides with biological activity that can slowly release an active principle at the wound site represent promising alternatives to traditional wound dressing materials. In this respect, new hydrogels based on curdlan derivative with 2-hydroxypropyl dimethyl octyl ammonium groups (QCurd) and native curdlan (Curd) were obtained at room temperature by covalent cross-linking using a diepoxy cross-linking agent. The chemical structure of the QCurd/Curd hydrogels was investigated by Fourier transform infrared spectroscopy (FTIR) spectroscopy. Scanning electron microscopy (SEM) revealed well-defined regulated pores with an average diameter between 50 and 75 μm, and hydrophobic micro-domains of about 5 μm on the pore walls. The high swelling rate (21–24 gwater/ghydrogel) and low elastic modulus values (7–14 kPa) make them ideal for medical applications as wound dressings. To evaluate the possible use of the curdlan-based hydrogels as active dressings, the loading capacity and release kinetics of diclofenac, taken as a model drug, were studied under simulated physiological skin conditions. Several mathematical models have been applied to evaluate drug transport processes and to calculate the diffusion coefficients. The prepared QCurd/Curd hydrogels were found to have good antibacterial properties, showing a bacteriostatic effect after 48 h against S. aureus, MRSA, E. coli, and P. aeruginosa. The retarded drug delivery and antimicrobial properties of the new hydrogels support our hypothesis that they are candidates for the manufacture of wound dressings. Full article
(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels (2nd Edition))
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22 pages, 7021 KiB  
Article
Impact of Fibrin Gel Architecture on Hepatocyte Growth Factor Release and Its Role in Modulating Cell Behavior for Tissue Regeneration
by Svenja Wein, Shannon Anna Jung, Miriam Aischa Al Enezy-Ulbrich, Luca Reicher, Stephan Rütten, Mark Kühnel, Danny Jonigk, Wilhelm Jahnen-Dechent, Andrij Pich and Sabine Neuss
Gels 2024, 10(6), 402; https://doi.org/10.3390/gels10060402 - 16 Jun 2024
Viewed by 919
Abstract
A novel scaffold design has been created to enhance tissue engineering and regenerative medicine by optimizing the controlled, prolonged release of Hepatocyte Growth Factor (HGF), a powerful chemoattractant for endogenous mesenchymal stem cells. We present a new stacked scaffold that is made up [...] Read more.
A novel scaffold design has been created to enhance tissue engineering and regenerative medicine by optimizing the controlled, prolonged release of Hepatocyte Growth Factor (HGF), a powerful chemoattractant for endogenous mesenchymal stem cells. We present a new stacked scaffold that is made up of three different fibrin gel layers, each of which has HGF integrated into the matrix. The design attempts to preserve HGF’s regenerative properties for long periods of time, which is necessary for complex tissue regeneration. These multi-layered fibrin gels have been mechanically evaluated using rheometry, and their degradation behavior has been studied using D-Dimer ELISA. Understanding the kinetics of HGF release from this novel scaffold configuration is essential for understanding HGF’s long-term sustained bioactivity. A range of cell-based tests were carried out to verify the functionality of HGF following extended incorporation. These tests included 2-photon microscopy using phalloidin staining to examine cellular morphology, SEM analysis for scaffold–cell interactions, and scratch and scatter assays to assess migration and motility. The analyses show that the novel stacking scaffold promotes vital cellular processes for tissue regeneration in addition to supporting HGF’s bioactivity. This scaffold design was developed for in situ tissue engineering. Using the body as a bioreactor, the scaffold should recruit mesenchymal stem cells from their niche, thus combining the regenerative abilities of HGF and MSCs to promote tissue remodeling and wound repair. Full article
(This article belongs to the Special Issue Hydrogel for Tissue Regeneration)
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22 pages, 551 KiB  
Article
Dipole Theory of Polyzwitterion Microgels and Gels
by Murugappan Muthukumar
Gels 2024, 10(6), 393; https://doi.org/10.3390/gels10060393 - 11 Jun 2024
Cited by 1 | Viewed by 969
Abstract
The behavior of polyzwitterions, constituted by dipole-like zwitterionic monomers, is significantly different from that of uniformly charged polyelectrolytes. The origin of this difference lies in the intrinsic capacity of polyzwitterions to self-associate intramolecularly and associate with interpenetrating chains driven by dominant dipolar interactions. [...] Read more.
The behavior of polyzwitterions, constituted by dipole-like zwitterionic monomers, is significantly different from that of uniformly charged polyelectrolytes. The origin of this difference lies in the intrinsic capacity of polyzwitterions to self-associate intramolecularly and associate with interpenetrating chains driven by dominant dipolar interactions. Earlier attempts to treat polyzwitterions implicitly assume that the dipoles of zwitterion monomers are randomly oriented. At ambient temperatures, the dipolar zwitterion monomers can readily align with each other generating quadrupoles and other multipoles and thus generating heterogeneous structures even in homogeneous solutions. Towards an attempt to understand the role of such dipolar associations, we present a mean field theory of solutions of polyzwitterions. Generally, we delineate a high-temperature regime where the zwitterion dipoles are randomly oriented from a low-temperature regime where quadrupole formation is significantly prevalent. We present closed-form formulas for: (1) Coil-globule transition in the low-temperature regime, the anti-polyelectrolyte effect of chain expansion upon addition of low molar mass salt, and chain relaxation times in dilute solutions. (2) Spontaneous formation of a mesomorphic state at the borderline between the high-temperature and low-temperature regimes and its characteristics. A universal law is presented for the radius of gyration of the microgel, as a proportionality to one-sixth power of the polymer concentration. (3) Swelling equilibrium of chemically cross-linked polyzwitterion gels in both the high temperature and low-temperature regimes. Addressing the hierarchical internal dynamics of polyzwitterion gels, we present a general stretched exponential law for the time-correlation function of gel displacement vector, that can be measured in dynamic light scattering experiments. The present theory is of direct experimental relevance and additional theoretical developments to all polyzwitterion systems, and generally to biological macromolecular systems such as intrinsically disordered proteins. Full article
(This article belongs to the Special Issue Recent Advances in Thermoreversible Gelation)
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28 pages, 6758 KiB  
Review
Recent Insights into Glucose-Responsive Concanavalin A-Based Smart Hydrogels for Controlled Insulin Delivery
by Maria Bercea and Alexandra Lupu
Gels 2024, 10(4), 260; https://doi.org/10.3390/gels10040260 - 11 Apr 2024
Cited by 2 | Viewed by 2588
Abstract
Many efforts are continuously undertaken to develop glucose-sensitive biomaterials able of controlling glucose levels in the body and self-regulating insulin delivery. Hydrogels that swell or shrink as a function of the environmental free glucose content are suitable systems for monitoring blood glucose, delivering [...] Read more.
Many efforts are continuously undertaken to develop glucose-sensitive biomaterials able of controlling glucose levels in the body and self-regulating insulin delivery. Hydrogels that swell or shrink as a function of the environmental free glucose content are suitable systems for monitoring blood glucose, delivering insulin doses adapted to the glucose concentration. In this context, the development of sensors based on reversible binding to glucose molecules represents a continuous challenge. Concanavalin A (Con A) is a bioactive protein isolated from sword bean plants (Canavalia ensiformis) and contains four sugar-binding sites. The high affinity for reversibly and specifically binding glucose and mannose makes Con A as a suitable natural receptor for the development of smart glucose-responsive materials. During the last few years, Con A was used to develop smart materials, such as hydrogels, microgels, nanoparticles and films, for producing glucose biosensors or drug delivery devices. This review is focused on Con A-based materials suitable in the diagnosis and therapeutics of diabetes. A brief outlook on glucose-derived theranostics of cancer is also presented. Full article
(This article belongs to the Special Issue Recent Advances in Protein Gels)
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17 pages, 3531 KiB  
Article
Functionalized Gelatin/Polysaccharide Hydrogels for Encapsulation of Hepatocytes
by Christian Willems, Fangdi Qi, Marie-Luise Trutschel and Thomas Groth
Gels 2024, 10(4), 231; https://doi.org/10.3390/gels10040231 - 28 Mar 2024
Viewed by 1658
Abstract
Liver diseases represent a considerable burden to patients and healthcare systems. Hydrogels play an important role in the engineering of soft tissues and may be useful for embedding hepatocytes for different therapeutic interventions or the development of in vitro models to study the [...] Read more.
Liver diseases represent a considerable burden to patients and healthcare systems. Hydrogels play an important role in the engineering of soft tissues and may be useful for embedding hepatocytes for different therapeutic interventions or the development of in vitro models to study the pathogenesis of liver diseases or testing of drugs. Here, we developed two types of hydrogels by crosslinking hydrazide-functionalized gelatin with either oxidized dialdehyde hyaluronan or alginate through the formation of hydrazone bonds. Gel formulations were studied through texture analysis and rheometry, showing mechanical properties comparable to those of liver tissue while also demonstrating long-term stability. The biocompatibility of hydrogels and their ability to host hepatocytes was studied in vitro in comparison to pure gelatin hydrogels crosslinked by transglutaminase using the hepatocellular line HepG2. It was found that HepG2 cells could be successfully embedded in the hydrogels, showing no signs of gel toxicity and proliferating in a 3D environment comparable to pure transglutaminase cross-linked gelatin hydrogels used as control. Altogether, hydrazide gelatin in combination with oxidized polysaccharides makes stable in situ gelling systems for the incorporation of hepatocytes, which may pave the way for use in liver tissue engineering and drug testing. Full article
(This article belongs to the Special Issue Advances in Hydrogels for Tissue Engineering)
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20 pages, 3726 KiB  
Article
The Influence of Gamma Radiation on Different Gelatin Nanofibers and Gelatins
by Carmen Gaidau, Maria Râpă, Gabriela Ionita, Ioana Rodica Stanculescu, Traian Zaharescu, Rodica-Roxana Constantinescu, Andrada Lazea-Stoyanova and Maria Stanca
Gels 2024, 10(4), 226; https://doi.org/10.3390/gels10040226 - 26 Mar 2024
Cited by 2 | Viewed by 1379
Abstract
Gelatin nanofibers are known as wound-healing biomaterials due to their high biocompatible, biodegradable, and non-antigenic properties compared to synthetic-polymer-fabricated nanofibers. The influence of gamma radiation doses on the structure of gelatin nanofiber dressings compared to gelatin of their origin is little known, although [...] Read more.
Gelatin nanofibers are known as wound-healing biomaterials due to their high biocompatible, biodegradable, and non-antigenic properties compared to synthetic-polymer-fabricated nanofibers. The influence of gamma radiation doses on the structure of gelatin nanofiber dressings compared to gelatin of their origin is little known, although it is very important for the production of stable bioactive products. Different-origin gelatins were extracted from bovine and donkey hides, rabbit skins, and fish scales and used for fabrication of nanofibers through electrospinning of gelatin solutions in acetic acid. Nanofibers with sizes ranging from 73.50 nm to 230.46 nm were successfully prepared, thus showing the potential of different-origin gelatin by-products valorization as a lower-cost alternative to native collagen. The gelatin nanofibers together with their origin gelatins were treated with 10, 20, and 25 kGy gamma radiation doses and investigated for their structural stability through chemiluminescence and FTIR spectroscopy. Chemiluminescence analysis showed a stable behavior of gelatin nanofibers and gelatins up to 200 °C and increased chemiluminescent emission intensities for nanofibers treated with gamma radiation, at temperatures above 200 °C, compared to irradiated gelatins and non-irradiated nanofibers and gelatins. The electron paramagnetic (EPR) signals of DMPO adduct allowed for the identification of long-life HO radicals only for bovine and donkey gelatin nanofibers treated with a 20 kGy gamma radiation dose. Microbial contamination with aerobic microorganisms, yeasts, filamentous fungi, Staphylococcus aureus, Escherichia coli, and Candida albicans of gelatin nanofibers treated with 10 kGy gamma radiation was under the limits required for pharmaceutical and topic formulations. Minor shifts of FTIR bands were observed at irradiation, indicating the preservation of secondary structure and stable properties of different-origin gelatin nanofibers. Full article
(This article belongs to the Special Issue Gel-Based Novel Wound Dressing)
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26 pages, 5328 KiB  
Article
Chitosan–Oxidized Pullulan Hydrogels Loaded with Essential Clove Oil: Synthesis, Characterization, Antioxidant and Antimicrobial Properties
by Dana Mihaela Suflet, Marieta Constantin, Irina Mihaela Pelin, Irina Popescu, Cristina M. Rimbu, Cristina Elena Horhogea and Gheorghe Fundueanu
Gels 2024, 10(4), 227; https://doi.org/10.3390/gels10040227 - 26 Mar 2024
Cited by 4 | Viewed by 1798
Abstract
Emulsion hydrogels are promising materials for encapsulating and stabilizing high amounts of hydrophobic essential oils in hydrophilic matrices. In this work, clove oil-loaded hydrogels (CS/OP-C) are synthesized by combining covalent and physical cross-linking approaches. First, clove oil (CO) was emulsified and stabilized in [...] Read more.
Emulsion hydrogels are promising materials for encapsulating and stabilizing high amounts of hydrophobic essential oils in hydrophilic matrices. In this work, clove oil-loaded hydrogels (CS/OP-C) are synthesized by combining covalent and physical cross-linking approaches. First, clove oil (CO) was emulsified and stabilized in a chitosan (CS) solution, which was further hardened by Schiff base covalent cross-linking with oxidized pullulan (OP). Second, the hydrogels were subjected to freeze–thaw cycles and, as a result, the clove oil was stabilized in physically cross-linked polymeric walls. Moreover, due to cryogelation, the obtained hydrogels exhibited sponge-like porous interconnected morphology (160–250 µm). By varying the clove oil content in the starting emulsion and the degree of cross-linking, the hydrogels displayed a high water retention capacity (swelling ratios between 1300 and 2000%), excellent elastic properties with fast shape recovery (20 s) after 70% compression, and controlled in vitro clove oil release in simulated skin conditions for 360 h. Furthermore, the prepared clove oil-loaded hydrogels had a strong scavenging activity of 83% and antibacterial and antifungal properties, showing a bacteriostatic effect after 48 and 72 h against S. aureus and E. coli. Our results recommend the new clove oil-embedded emulsion hydrogels as promising future materials for application as wound dressings. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization (2nd Edition))
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33 pages, 3926 KiB  
Review
Three-Dimensional Printing Strategies for Enhanced Hydrogel Applications
by Hossein Omidian and Kwadwo Mfoafo
Gels 2024, 10(4), 220; https://doi.org/10.3390/gels10040220 - 25 Mar 2024
Viewed by 2224
Abstract
This study explores the dynamic field of 3D-printed hydrogels, emphasizing advancements and challenges in customization, fabrication, and functionalization for applications in biomedical engineering, soft robotics, and tissue engineering. It delves into the significance of tailored biomedical scaffolds for tissue regeneration, the enhancement in [...] Read more.
This study explores the dynamic field of 3D-printed hydrogels, emphasizing advancements and challenges in customization, fabrication, and functionalization for applications in biomedical engineering, soft robotics, and tissue engineering. It delves into the significance of tailored biomedical scaffolds for tissue regeneration, the enhancement in bioinks for realistic tissue replication, and the development of bioinspired actuators. Additionally, this paper addresses fabrication issues in soft robotics, aiming to mimic biological structures through high-resolution, multimaterial printing. In tissue engineering, it highlights efforts to create environments conducive to cell migration and functional tissue development. This research also extends to drug delivery systems, focusing on controlled release and biocompatibility, and examines the integration of hydrogels with electronic components for bioelectronic applications. The interdisciplinary nature of these efforts highlights a commitment to overcoming material limitations and optimizing fabrication techniques to realize the full potential of 3D-printed hydrogels in improving health and well-being. Full article
(This article belongs to the Special Issue 3D Printing of Gels: Applications and Properties)
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15 pages, 6848 KiB  
Article
A Comparative Study between Beeswax and Glycerol Monostearate for Food-Grade Oleogels
by Francesca Malvano, Donatella Albanese, Luciano Cinquanta, Sara Liparoti and Francesco Marra
Gels 2024, 10(4), 214; https://doi.org/10.3390/gels10040214 - 22 Mar 2024
Cited by 3 | Viewed by 1834
Abstract
With the aim to produce solid fats with a high percentage of unsaturated fatty acids, oleogels based on olive and peanut oil with different concentrations of beeswax (BW) and glycerol monostearate (GMS) as oleogelators were studied and compared. The critical oleogelator concentration for [...] Read more.
With the aim to produce solid fats with a high percentage of unsaturated fatty acids, oleogels based on olive and peanut oil with different concentrations of beeswax (BW) and glycerol monostearate (GMS) as oleogelators were studied and compared. The critical oleogelator concentration for both BW and GMS was 3%. Thermal properties of the developed GMS-based oleogels pointed to a polymorphic structure, confirmed by the presence of two exothermic and endothermic peaks. All developed oleogels released less than 4% of oil, highlighting their high oil binding capacity. A morphology evaluation of oleogels showed platelet-like crystals, characterized by a cross-sectional length of 50 μm in BW-based oleogels and irregular clusters of needle-like crystals with a higher diameter in GMS-based oleogels. BW-based oleogels showed a solid fat content ranging from 1.16% to 2.27%, and no solid fat content was found at 37 °C. GMS-based oleogels reached slightly higher values of SFC that ranged from 1.58% to 2.97% at 25 °C and from 1.00% to 1.75% at 37 °C. Olive oil-based oleogels with GMS showed higher firmness compared with BW-based ones. The stronger structure network in olive oil/GMS-based oleogels provided a real physical barrier to oxidants, showing a high oxidation stability. Full article
(This article belongs to the Special Issue Recent Advances in Food Gels)
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50 pages, 9695 KiB  
Review
Evolution of Hybrid Hydrogels: Next-Generation Biomaterials for Drug Delivery and Tissue Engineering
by Md Mohosin Rana and Hector De la Hoz Siegler
Gels 2024, 10(4), 216; https://doi.org/10.3390/gels10040216 - 22 Mar 2024
Cited by 16 | Viewed by 4021
Abstract
Hydrogels, being hydrophilic polymer networks capable of absorbing and retaining aqueous fluids, hold significant promise in biomedical applications owing to their high water content, permeability, and structural similarity to the extracellular matrix. Recent chemical advancements have bolstered their versatility, facilitating the integration of [...] Read more.
Hydrogels, being hydrophilic polymer networks capable of absorbing and retaining aqueous fluids, hold significant promise in biomedical applications owing to their high water content, permeability, and structural similarity to the extracellular matrix. Recent chemical advancements have bolstered their versatility, facilitating the integration of the molecules guiding cellular activities and enabling their controlled activation under time constraints. However, conventional synthetic hydrogels suffer from inherent weaknesses such as heterogeneity and network imperfections, which adversely affect their mechanical properties, diffusion rates, and biological activity. In response to these challenges, hybrid hydrogels have emerged, aiming to enhance their strength, drug release efficiency, and therapeutic effectiveness. These hybrid hydrogels, featuring improved formulations, are tailored for controlled drug release and tissue regeneration across both soft and hard tissues. The scientific community has increasingly recognized the versatile characteristics of hybrid hydrogels, particularly in the biomedical sector. This comprehensive review delves into recent advancements in hybrid hydrogel systems, covering the diverse types, modification strategies, and the integration of nano/microstructures. The discussion includes innovative fabrication techniques such as click reactions, 3D printing, and photopatterning alongside the elucidation of the release mechanisms of bioactive molecules. By addressing challenges, the review underscores diverse biomedical applications and envisages a promising future for hybrid hydrogels across various domains in the biomedical field. Full article
(This article belongs to the Special Issue Hydrogel for Tissue Regeneration)
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17 pages, 9594 KiB  
Article
Exploring the Impact of the Synthesis Variables Involved in the Polyurethane Aerogels-like Materials Design
by Esther Pinilla-Peñalver, Darío Cantero, Amaya Romero and Luz Sánchez-Silva
Gels 2024, 10(3), 209; https://doi.org/10.3390/gels10030209 - 20 Mar 2024
Cited by 4 | Viewed by 1837
Abstract
This research presents a novel approach to synthesising polyurethane (PUR)-based aerogels at the pilot scale, optimizing synthesis variables such as the gelation solvent, solids content, chain extender/isocyanate ratio, and dispersion mode. The solids content (2–11 wt.%) is the parameter with the most influence [...] Read more.
This research presents a novel approach to synthesising polyurethane (PUR)-based aerogels at the pilot scale, optimizing synthesis variables such as the gelation solvent, solids content, chain extender/isocyanate ratio, and dispersion mode. The solids content (2–11 wt.%) is the parameter with the most influence on the density of the aerogels, with a clear decrease in this property as the solids content decreases. On the other hand, it was demonstrated that minimizing the excess of ethylenediamine (used as chain extender) in relation to the isocyanate is a valuable consideration to improve the thermal conductivity of the aerogel. Related to the chain extender/isocyanate ratio, a compromise situation where the initial isocyanate reacts almost completely is crucial. Fourier-transform infrared spectroscopy was used to conduct such monitoring during the reaction. Once the conditions were optimised, the aerogel showing improved properties was synthesised using ethyl acetate as the gelling solvent, a 3.7 wt.% solids content, an ethylenediamine/isocyanate ratio of 0.20, and sonication as the dispersion mode, attaining a thermal conductivity of 0.030 W m−1 K−1 and a density of 0.046 g cm−3. Therefore, the synthesized aerogel emerges as a promising candidate for use in the construction and automotive industries. Full article
(This article belongs to the Special Issue Synthesis and Application of Aerogel)
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17 pages, 4240 KiB  
Article
Fabrication and Characterization of Quad-Component Bioinspired Hydrogels to Model Elevated Fibrin Levels in Central Nervous Tissue Scaffolds
by Ana M. Diaz-Lasprilla, Meagan McKee, Andrea C. Jimenez-Vergara, Swathisri Ravi, Devon Bellamy, Wendy Ortega, Cody O. Crosby, Jennifer Steele, Germán Plascencia-Villa, George Perry and Dany J. Munoz-Pinto
Gels 2024, 10(3), 203; https://doi.org/10.3390/gels10030203 - 17 Mar 2024
Viewed by 1863
Abstract
Multicomponent interpenetrating polymer network (mIPN) hydrogels are promising tissue-engineering scaffolds that could closely resemble key characteristics of native tissues. The mechanical and biochemical properties of mIPNs can be finely controlled to mimic key features of target cellular microenvironments, regulating cell-matrix interactions. In this [...] Read more.
Multicomponent interpenetrating polymer network (mIPN) hydrogels are promising tissue-engineering scaffolds that could closely resemble key characteristics of native tissues. The mechanical and biochemical properties of mIPNs can be finely controlled to mimic key features of target cellular microenvironments, regulating cell-matrix interactions. In this work, we fabricated hydrogels made of collagen type I (Col I), fibrin, hyaluronic acid (HA), and poly (ethylene glycol) diacrylate (PEGDA) using a network-by-network fabrication approach. With these mIPNs, we aimed to develop a biomaterial platform that supports the in vitro culture of human astrocytes and potentially serves to assess the effects of the abnormal deposition of fibrin in cortex tissue and simulate key aspects in the progression of neuroinflammation typically found in human pathologies such as Alzheimer’s disease (AD), Parkinson’s disease (PD), and tissue trauma. Our resulting hydrogels closely resembled the complex modulus of AD human brain cortex tissue (~7.35 kPa), promoting cell spreading while allowing for the modulation of fibrin and hyaluronic acid levels. The individual networks and their microarchitecture were evaluated using confocal laser scanning microscopy (CLSM) and scanning electron microscopy (SEM). Human astrocytes were encapsulated in mIPNs, and negligible cytotoxicity was observed 24 h after the cell encapsulation. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization (2nd Edition))
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20 pages, 4786 KiB  
Article
pH-Responsive Cellulose/Silk/Fe3O4 Hydrogel Microbeads Designed for Biomedical Applications
by Seung Hyeon Weon, Yuhyeon Na, Jiwoo Han, Jeong Woo Lee, Hyung Joo Kim, Saerom Park and Sang Hyun Lee
Gels 2024, 10(3), 200; https://doi.org/10.3390/gels10030200 - 16 Mar 2024
Cited by 1 | Viewed by 1857
Abstract
In this study, cellulose/Fe3O4 hydrogel microbeads were prepared through the sol–gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (TBAH) and 40% tetrabutylphosphonium hydroxide (TBPH) dissolved cellulose at room temperature [...] Read more.
In this study, cellulose/Fe3O4 hydrogel microbeads were prepared through the sol–gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (TBAH) and 40% tetrabutylphosphonium hydroxide (TBPH) dissolved cellulose at room temperature and effectively dispersed Fe3O4, forming cellulose/Fe3O4 microbeads with an average diameter of ~15 µm. Additionally, these solvents co-dissolved cellulose and silk, allowing for the manufacture of cellulose/silk/Fe3O4 hydrogel microbeads with altered surface characteristics. Owing to the negatively charged surface characteristics, the adsorption capacity of the cellulose/silk/Fe3O4 microbeads for the cationic dye crystal violet was >10 times higher than that of the cellulose/Fe3O4 microbeads. When prepared with TBAH, the initial adsorption rate of bovine serum albumin (BSA) on the cellulose/silk/Fe3O4 microbeads was 18.1 times higher than that on the cellulose/Fe3O4 microbeads. When preparing TBPH, the equilibrium adsorption capacity of the cellulose/silk/Fe3O4 microbeads for BSA (1.6 g/g) was 8.5 times higher than that of the cellulose/Fe3O4 microbeads. The pH-dependent BSA release from the cellulose/silk/Fe3O4 microbeads prepared with TBPH revealed 6.1-fold slower initial desorption rates and 5.2-fold lower desorption amounts at pH 2.2 than those at pH 7.4. Cytotoxicity tests on the cellulose and cellulose/silk composites regenerated with TBAH and TBPH yielded nontoxic results. Therefore, cellulose/silk/Fe3O4 microbeads are considered suitable pH-responsive supports for orally administered protein pharmaceuticals. Full article
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17 pages, 13462 KiB  
Article
Microstructure, Physical Properties, and Oxidative Stability of Olive Oil Oleogels Composed of Sunflower Wax and Monoglycerides
by Dafni Dimakopoulou-Papazoglou, Konstantina Zampouni, Prodromos Prodromidis, Thomas Moschakis and Eugenios Katsanidis
Gels 2024, 10(3), 195; https://doi.org/10.3390/gels10030195 - 13 Mar 2024
Cited by 1 | Viewed by 2154
Abstract
The utilization of natural waxes to form oleogels has emerged as a new and efficient technique for structuring liquid edible oil into solid-like structures for diverse food applications. The objective of this study was to investigate the interaction between sunflower wax (SW) and [...] Read more.
The utilization of natural waxes to form oleogels has emerged as a new and efficient technique for structuring liquid edible oil into solid-like structures for diverse food applications. The objective of this study was to investigate the interaction between sunflower wax (SW) and monoglycerides (MGs) in olive oil oleogels and assess their physical characteristics and storage stability. To achieve this, pure SW and a combination of SW with MGs in a 1:1 ratio were examined within a total concentration range of 6–12% w/w. The formed oleogels were characterized based on their microstructure, melting and crystallization properties, textural characteristics, and oxidative stability during storage. All the oleogels were self-standing, and, as the concentration increased, the hardness of the oleogels also increased. The crystals of SW oleogels were long needle-like, while the combination of SW and MGs led to the formation of crystal aggregates and rosette-like crystals. Differential scanning calorimetry and FTIR showed that the addition of MGs led to different crystal structures. The oxidation results revealed that oleogels had low peroxide and TBARS values throughout the 28-day storage period. These results provide useful insights about the utilization of SW and MGs oleogels for potential applications in the food industry. Full article
(This article belongs to the Special Issue Functionality of Oleogels and Bigels in Foods)
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13 pages, 2136 KiB  
Article
Thermosensitive In Situ Gelling Poloxamers/Hyaluronic Acid Gels for Hydrocortisone Ocular Delivery
by Fabrizio Villapiano, Teresa Silvestri, Camilla Lo Gatto, Danilo Aleo, Virginia Campani, Sossio Fabio Graziano, Concetta Giancola, Federica D’Aria, Giuseppe De Rosa, Marco Biondi and Laura Mayol
Gels 2024, 10(3), 193; https://doi.org/10.3390/gels10030193 - 12 Mar 2024
Viewed by 2097
Abstract
This study endeavored to overcome the physiological barriers hindering optimal bioavailability in ophthalmic therapeutics by devising drug delivery platforms that allow therapeutically effective drug concentrations in ocular tissues for prolonged times. Thermosensitive drug delivery platforms were formulated by blending poloxamers (F68 and F127) [...] Read more.
This study endeavored to overcome the physiological barriers hindering optimal bioavailability in ophthalmic therapeutics by devising drug delivery platforms that allow therapeutically effective drug concentrations in ocular tissues for prolonged times. Thermosensitive drug delivery platforms were formulated by blending poloxamers (F68 and F127) with low-molecular-weight hyaluronic acid (HA) in various concentrations and loaded with hydrocortisone (HC). Among the formulations examined, only three were deemed suitable based on their desirable gelling properties at a temperature close to the eye’s surface conditions while also ensuring minimal gelation time for swift ocular application. Rheological analyses unveiled the ability of the formulations to develop gels at suitable temperatures, elucidating the gel-like characteristics around the physiological temperature essential for sustained drug release. The differential scanning calorimetry findings elucidated intricate hydrogel–water interactions, indicating that HA affects the water–polymer interactions within the gel by increasing the platform hydrophilicity. Also, in vitro drug release studies demonstrated significant hydrocortisone release within 8 h, governed by an anomalous transport mechanism, prompting further investigation for optimized release kinetics. The produced platforms offer promising prospects for efficacious ocular drug delivery, addressing pivotal challenges in ocular therapeutics and heralding future advancements in the domain. Full article
(This article belongs to the Special Issue Gels in Medicine and Pharmacological Therapies (2nd Edition))
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46 pages, 5115 KiB  
Review
Hydrogels in Cutaneous Wound Healing: Insights into Characterization, Properties, Formulation and Therapeutic Potential
by Mariana Ribeiro, Marco Simões, Carla Vitorino and Filipa Mascarenhas-Melo
Gels 2024, 10(3), 188; https://doi.org/10.3390/gels10030188 - 8 Mar 2024
Cited by 9 | Viewed by 4791
Abstract
Hydrogels are polymeric materials that possess a set of characteristics meeting various requirements of an ideal wound dressing, making them promising for wound care. These features include, among others, the ability to absorb and retain large amounts of water and the capacity to [...] Read more.
Hydrogels are polymeric materials that possess a set of characteristics meeting various requirements of an ideal wound dressing, making them promising for wound care. These features include, among others, the ability to absorb and retain large amounts of water and the capacity to closely mimic native structures, such as the extracellular matrix, facilitating various cellular processes like proliferation and differentiation. The polymers used in hydrogel formulations exhibit a broad spectrum of properties, allowing them to be classified into two main categories: natural polymers like collagen and chitosan, and synthetic polymers such as polyurethane and polyethylene glycol. This review offers a comprehensive overview and critical analysis of the key polymers that can constitute hydrogels, beginning with a brief contextualization of the polymers. It delves into their function, origin, and chemical structure, highlighting key sources of extraction and obtaining. Additionally, this review encompasses the main intrinsic properties of these polymers and their roles in the wound healing process, accompanied, whenever available, by explanations of the underlying mechanisms of action. It also addresses limitations and describes some studies on the effectiveness of isolated polymers in promoting skin regeneration and wound healing. Subsequently, we briefly discuss some application strategies of hydrogels derived from their intrinsic potential to promote the wound healing process. This can be achieved due to their role in the stimulation of angiogenesis, for example, or through the incorporation of substances like growth factors or drugs, such as antimicrobials, imparting new properties to the hydrogels. In addition to substance incorporation, the potential of hydrogels is also related to their ability to serve as a three-dimensional matrix for cell culture, whether it involves loading cells into the hydrogel or recruiting cells to the wound site, where they proliferate on the scaffold to form new tissue. The latter strategy presupposes the incorporation of biosensors into the hydrogel for real-time monitoring of wound conditions, such as temperature and pH. Future prospects are then ultimately addressed. As far as we are aware, this manuscript represents the first comprehensive approach that brings together and critically analyzes fundamental aspects of both natural and synthetic polymers constituting hydrogels in the context of cutaneous wound healing. It will serve as a foundational point for future studies, aiming to contribute to the development of an effective and environmentally friendly dressing for wounds. Full article
(This article belongs to the Special Issue Hydrogel-Based Novel Biomaterials: Achievements and Prospects)
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16 pages, 4654 KiB  
Article
Fibrin-Based Hydrogels with Reactive Amphiphilic Copolymers for Mechanical Adjustments Allow for Capillary Formation in 2D and 3D Environments
by Svenja Wein, Carina Schemmer, Miriam Aischa Al Enezy-Ulbrich, Shannon Anna Jung, Stephan Rütten, Mark Kühnel, Danny Jonigk, Wilhelm Jahnen-Dechent, Andrij Pich and Sabine Neuss
Gels 2024, 10(3), 182; https://doi.org/10.3390/gels10030182 - 6 Mar 2024
Cited by 1 | Viewed by 2552
Abstract
This study focuses on enhancing controllable fibrin-based hydrogels for tissue engineering, addressing existing weaknesses. By integrating a novel copolymer, we improved the foundation for cell-based angiogenesis with adaptable structural features. Tissue engineering often faces challenges like waste disposal and nutrient supply beyond the [...] Read more.
This study focuses on enhancing controllable fibrin-based hydrogels for tissue engineering, addressing existing weaknesses. By integrating a novel copolymer, we improved the foundation for cell-based angiogenesis with adaptable structural features. Tissue engineering often faces challenges like waste disposal and nutrient supply beyond the 200 µm diffusion limit. Angiogenesis breaks through this limitation, allowing the construction of larger constructs. Our innovative scaffold combination significantly boosts angiogenesis, resulting in longer branches and more capillary network junctions. The copolymer attached to fibrin fibers enables precise adjustment of hydrogel mechanical dynamic properties for specific applications. Our material proves effective for angiogenesis, even under suppression factors like suramin. In our study, we prepared fibrin-based hydrogels with and without the copolymer PVP12400-co-GMA10mol%. Using a co-culture system of human umbilical vein endothelial cells (HUVEC) and mesenchymal stem cells (MSC), we analyzed angiogenetic behavior on and within the modified hydrogels. Capillary-like structures were reproducibly formed on different surfaces, demonstrating the general feasibility of three-dimensional endothelial cell networks in fibrin-based hydrogels. This highlights the biomaterial’s suitability for in vitro pre-vascularization of biohybrid implants. Full article
(This article belongs to the Special Issue Biopolymer-Based Gels for Drug Delivery and Tissue Engineering)
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11 pages, 2116 KiB  
Article
Synthesis of Ni-Doped Graphene Aerogels for Electrochemical Applications
by Marina González-Barriuso, Mario Sánchez-Suárez, Judith González-Lavín, Ana Arenillas and Natalia Rey-Raap
Gels 2024, 10(3), 180; https://doi.org/10.3390/gels10030180 - 4 Mar 2024
Viewed by 2511
Abstract
Carbonaceous materials used in most electrochemical applications require high specific surface area, adequate pore size distribution, and high electrical conductivity to ensure good interaction with the electrolyte and fast electron transport. The development of transition metal doped graphene aerogels is a possible solution, [...] Read more.
Carbonaceous materials used in most electrochemical applications require high specific surface area, adequate pore size distribution, and high electrical conductivity to ensure good interaction with the electrolyte and fast electron transport. The development of transition metal doped graphene aerogels is a possible solution, since their structure, morphology, and electrical properties can be controlled during the synthesis process. This work aims to synthesize Ni-doped graphene aerogels to study the role of different nickel salts in the sol-gel reaction and their final properties. The characterization data show that, regardless of the nature of the Ni salts, the surface area, volume of micropores, and enveloped density decrease, while the porosity and electrical conductivity increase. However, differences in morphology, mesopore size distribution, degree of order of the carbon structure, and electrical conductivity were observed depending on the type of Ni salt. It was found that nickel nitrate results in a material with a broader mesopore distribution, higher electrical conductivity, and hence, higher electrochemical surface area, demonstrating that graphene aerogels can be easily synthesized with tailored properties to fit the requirements of specific electrochemical applications. Full article
(This article belongs to the Special Issue Advances in Xerogels: From Design to Applications (2nd Edition))
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18 pages, 3755 KiB  
Article
Development of a Sprayable Hydrogel-Based Wound Dressing: An In Vitro Model
by Mine Altunbek, Mert Gezek, Maria Eduarda Torres Gouveia and Gulden Camci-Unal
Gels 2024, 10(3), 176; https://doi.org/10.3390/gels10030176 - 1 Mar 2024
Cited by 1 | Viewed by 3633
Abstract
Hydrogel-based dressings can effectively heal wounds by providing multiple functions, such as antibacterial, anti-inflammatory, and preangiogenic bioactivities. The ability to spray the dressing is important for the rapid and effective coverage of the wound surface. In this study, we developed a sprayable hydrogel-based [...] Read more.
Hydrogel-based dressings can effectively heal wounds by providing multiple functions, such as antibacterial, anti-inflammatory, and preangiogenic bioactivities. The ability to spray the dressing is important for the rapid and effective coverage of the wound surface. In this study, we developed a sprayable hydrogel-based wound dressing using naturally derived materials: hyaluronic acid and gelatin. We introduced methacrylate groups (HAMA and GelMA) to these materials to enable controllable photocrosslinking and form a stable hydrogel on the wound surface. To achieve sprayability, we evaluated the concentration of GelMA within a range of 5–15% (w/v) and then incorporated 1% (w/v) HAMA. Additionally, we incorporated calcium peroxide into the hydrogel at concentrations ranging from 0 to 12 mg/mL to provide self-oxygenation and antibacterial properties. The results showed that the composite hydrogels were sprayable and could provide oxygen for up to two weeks. The released oxygen relieved metabolic stress in fibroblasts and reduced cell death under hypoxia in in vitro culture. Furthermore, calcium peroxide added antibacterial properties to the wound dressing. In conclusion, the developed sprayable hydrogel dressing has the potential to be advantageous for wound healing due to its practical and conformable application, as well as its self-oxygenating and antibacterial functions. Full article
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29 pages, 2617 KiB  
Review
Advancements in Cellulose-Based Superabsorbent Hydrogels: Sustainable Solutions across Industries
by Hossein Omidian, Arnavaz Akhzarmehr and Sumana Dey Chowdhury
Gels 2024, 10(3), 174; https://doi.org/10.3390/gels10030174 - 29 Feb 2024
Cited by 6 | Viewed by 3555
Abstract
The development of superabsorbent hydrogels is experiencing a transformative era across industries. While traditional synthetic hydrogels have found broad utility, their non-biodegradable nature has raised environmental concerns, driving the search for eco-friendlier alternatives. Cellulose-based superabsorbents, derived from sustainable sources, are gaining prominence. Innovations [...] Read more.
The development of superabsorbent hydrogels is experiencing a transformative era across industries. While traditional synthetic hydrogels have found broad utility, their non-biodegradable nature has raised environmental concerns, driving the search for eco-friendlier alternatives. Cellulose-based superabsorbents, derived from sustainable sources, are gaining prominence. Innovations include biodegradable polymer hydrogels, natural cellulose-chitosan variants, and cassava starch-based alternatives. These materials are reshaping agriculture by enhancing soil fertility and water retention, serving as potent hemostatic agents in medicine, contributing to pollution control, and providing eco-friendly construction materials. Cellulose-based hydrogels also offer promise in drug delivery and hygiene products. Advanced characterization techniques aid in optimizing their properties, while the shift towards circular economy practices further highlights sustainability. This manuscript provides a comprehensive overview of these advancements, highlighting their diverse applications and environmental benefits. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization (2nd Edition))
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22 pages, 5082 KiB  
Article
Efficient and Selective Removal of Heavy Metals and Dyes from Aqueous Solutions Using Guipi Residue-Based Hydrogel
by Xiaochun Yin, Pei Xu and Huiyao Wang
Gels 2024, 10(2), 142; https://doi.org/10.3390/gels10020142 - 13 Feb 2024
Cited by 3 | Viewed by 2076
Abstract
The presence of organic dyes and heavy metal ions in water sources poses a significant threat to human health and the ecosystem. In this study, hydrogel adsorbents for water pollution remediation were synthesized using Guipi residue (GP), a cellulose material from Chinese herbal [...] Read more.
The presence of organic dyes and heavy metal ions in water sources poses a significant threat to human health and the ecosystem. In this study, hydrogel adsorbents for water pollution remediation were synthesized using Guipi residue (GP), a cellulose material from Chinese herbal medicine, and chitosan (CTS) through radical polymerization with acrylamide (AM) and acrylic acid (AA). The characteristics of the hydrogels were analyzed from a physicochemical perspective, and their ability to adsorb was tested using model pollutants such as Pb2+, Cd2+, Rhodamine B (RhB), and methyl orange (MO). The outcomes revealed that GP/CTS/AA-co-AM, which has improved mechanical attributes, effectively eliminated these pollutants. At a pH of 4.0, a contact duration of 120 min, and an initial concentration of 600 mg/L for Pb2+ and 500 mg/L for Cd2+, the highest adsorption capabilities were 314.6 mg/g for Pb2+ and 289.1 mg/g for Cd2+. Regarding the dyes, the GP/CTS/AA-co-AM hydrogel displayed adsorption capacities of 106.4 mg/g for RhB and 94.8 mg/g for MO, maintaining a stable adsorption capacity at different pHs. Compared with other competitive pollutants, GP/CTS/AA-co-AM demonstrated a higher absorption capability, mainly targeted toward Pb2+. The adsorption processes for the pollutants conformed to pseudo-second-order kinetics models and adhered to the Langmuir models. Even after undergoing five consecutive adsorption and desorption cycles, the adsorption capacities for heavy metals and dyes remained above 70% and 80%. In summary, this study effectively suggested the potential of the innovative GP/CTS/AA-co-AM hydrogel as a practical and feasible approach for eliminating heavy metals and dyes from water solutions. Full article
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13 pages, 2070 KiB  
Article
Factors That Influence Base-Catalyzed Thiol-Ene Hydrogel Synthesis
by Nolan Morrison and Brandon M. Vogel
Gels 2023, 9(11), 917; https://doi.org/10.3390/gels9110917 - 20 Nov 2023
Cited by 1 | Viewed by 2746
Abstract
Injectable, localized drug delivery using hydrogels made from ethoxylated trimethylolpropane tri-3-mercaptopropionate (ETTMP) and poly(ethylene glycol) diacrylate (PEGDA) has shown great potential due to these hydrogels’ ability to exhibit non-swelling behavior and tunable drug release properties. However, current synthesis methods in the literature suffer [...] Read more.
Injectable, localized drug delivery using hydrogels made from ethoxylated trimethylolpropane tri-3-mercaptopropionate (ETTMP) and poly(ethylene glycol) diacrylate (PEGDA) has shown great potential due to these hydrogels’ ability to exhibit non-swelling behavior and tunable drug release properties. However, current synthesis methods in the literature suffer from poor ETTMP solubility in water, slow gelation times exceeding 20 min, and a lack of reproducibility. To address these limitations, we have developed a reliable synthesis procedure and conducted a sensitivity analysis of key variables. This has enabled us to synthesize ETTMP-PEGDA hydrogels in a polymer concentration range of 15 to 90 wt% with gelation times of less than 2 min and moduli ranging from 3.5 to 190 kPa. We overcame two synthesis limitations by identifying the impact of residual mercaptopropionic acid and alumina purification column height on gelation time and by premixing ETTMP and PEGDA to overcome low ETTMP solubility in water. Our ETTMP-PEGDA mixture can be stored at −20 °C for up to 2 months without crosslinking, allowing easy storage and shipment. These and previous results demonstrate the potential of ETTMP-PEGDA hydrogels as promising candidates for injectable, localized drug delivery with tunable drug release properties. Full article
(This article belongs to the Special Issue Advances in Chemistry and Physics of Hydrogels)
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22 pages, 3289 KiB  
Review
Exploring the Potential of Artificial Intelligence for Hydrogel Development—A Short Review
by Irina Negut and Bogdan Bita
Gels 2023, 9(11), 845; https://doi.org/10.3390/gels9110845 - 25 Oct 2023
Cited by 5 | Viewed by 3633
Abstract
AI and ML have emerged as transformative tools in various scientific domains, including hydrogel design. This work explores the integration of AI and ML techniques in the realm of hydrogel development, highlighting their significance in enhancing the design, characterisation, and optimisation of hydrogels [...] Read more.
AI and ML have emerged as transformative tools in various scientific domains, including hydrogel design. This work explores the integration of AI and ML techniques in the realm of hydrogel development, highlighting their significance in enhancing the design, characterisation, and optimisation of hydrogels for diverse applications. We introduced the concept of AI train hydrogel design, underscoring its potential to decode intricate relationships between hydrogel compositions, structures, and properties from complex data sets. In this work, we outlined classical physical and chemical techniques in hydrogel design, setting the stage for AI/ML advancements. These methods provide a foundational understanding for the subsequent AI-driven innovations. Numerical and analytical methods empowered by AI/ML were also included. These computational tools enable predictive simulations of hydrogel behaviour under varying conditions, aiding in property customisation. We also emphasised AI’s impact, elucidating its role in rapid material discovery, precise property predictions, and optimal design. ML techniques like neural networks and support vector machines that expedite pattern recognition and predictive modelling using vast datasets, advancing hydrogel formulation discovery are also presented. AI and ML’s have a transformative influence on hydrogel design. AI and ML have revolutionised hydrogel design by expediting material discovery, optimising properties, reducing costs, and enabling precise customisation. These technologies have the potential to address pressing healthcare and biomedical challenges, offering innovative solutions for drug delivery, tissue engineering, wound healing, and more. By harmonising computational insights with classical techniques, researchers can unlock unprecedented hydrogel potentials, tailoring solutions for diverse applications. Full article
(This article belongs to the Special Issue Design of Polymeric Hydrogels Biomaterials)
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13 pages, 1537 KiB  
Review
Compendium of Safety Regulatory for Safe Applications of Aerogels
by Antonella Caterina Boccia, Alfio Pulvirenti, Carlos A. García-González, Fabia Grisi and Monica Neagu
Gels 2023, 9(11), 842; https://doi.org/10.3390/gels9110842 - 24 Oct 2023
Cited by 5 | Viewed by 2608
Abstract
An increasing number of aerogels as nanostructured highly porous materials are entering the market in every day products, with an attractive portfolio of properties for emerging applications ranging from health care and leisure to electronics, cosmetics, energy, agriculture, food and environmental. However, the [...] Read more.
An increasing number of aerogels as nanostructured highly porous materials are entering the market in every day products, with an attractive portfolio of properties for emerging applications ranging from health care and leisure to electronics, cosmetics, energy, agriculture, food and environmental. However, the novelty in properties and forms of aerogels makes the development of a legislative framework particularly challenging for ensuring the safe development and use of nano-enabled products. The presented safety regulatory Compendium intends to share knowledge with the international aerogels community, as well as end-users and stakeholders, on the regulatory and safe handling procedures, as best safety practices, to be followed during the production process, handling, transport and end-use of aerogel-based formulations to mitigate human and environmental risks considering lack of data availability for this purpose in general. Full article
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23 pages, 945 KiB  
Review
Current Advances in Stimuli-Responsive Hydrogels as Smart Drug Delivery Carriers
by Yulong Zhang and Benjamin M. Wu
Gels 2023, 9(10), 838; https://doi.org/10.3390/gels9100838 - 22 Oct 2023
Cited by 15 | Viewed by 5122
Abstract
In recent years, significant advancements in the field of advanced materials and hydrogel engineering have enabled the design and fabrication of smart hydrogels and nanogels that exhibit sensitivity to specific signals or pathological conditions, leading to a wide range of applications in drug [...] Read more.
In recent years, significant advancements in the field of advanced materials and hydrogel engineering have enabled the design and fabrication of smart hydrogels and nanogels that exhibit sensitivity to specific signals or pathological conditions, leading to a wide range of applications in drug delivery and disease treatment. This comprehensive review aims to provide an in-depth analysis of the stimuli-responsive principles exhibited by smart hydrogels in response to various triggers, such as pH levels, temperature fluctuations, light exposure, redox conditions, or the presence of specific biomolecules. The functionality and performance characteristics of these hydrogels are highly influenced by both their constituent components and fabrication processes. Key design principles, their applications in disease treatments, challenges, and future prospects were also discussed. Overall, this review aims to contribute to the current understanding of gel-based drug delivery systems and stimulate further research in this rapidly evolving field. Full article
(This article belongs to the Special Issue Recent Advances in Gels Engineering for Drug Delivery)
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13 pages, 2330 KiB  
Article
Forward Light Scattering of First to Third Generation Vitreous Body Replacement Hydrogels after Surgical Application Compared to Conventional Silicone Oils and Vitreous Body
by Maximilian Hammer, Jonathan Herth, Marcel Muuss, Sonja Schickhardt, Alexander Scheuerle, Ramin Khoramnia, Grzegorz Łabuz, Philipp Uhl and Gerd Uwe Auffarth
Gels 2023, 9(10), 837; https://doi.org/10.3390/gels9100837 - 21 Oct 2023
Cited by 5 | Viewed by 1781
Abstract
To treat certain vitreoretinal diseases, the vitreous body, a hydrogel composed of mostly collagen and hyaluronic acid, must be removed. After vitrectomy surgery, the vitreous cavity is filled with an endotamponade. Previously, pre-clinical hydrogel-based vitreous body substitutes either made from uncrosslinked monomers (1st [...] Read more.
To treat certain vitreoretinal diseases, the vitreous body, a hydrogel composed of mostly collagen and hyaluronic acid, must be removed. After vitrectomy surgery, the vitreous cavity is filled with an endotamponade. Previously, pre-clinical hydrogel-based vitreous body substitutes either made from uncrosslinked monomers (1st generation), preformed crosslinked polymers (2nd generation), or in situ gelating polymers (3rd generation) have been developed. Forward light scattering is a measure of Stray light induced by optical media, when increased, causing visual disturbance and glare. During pinhole surgery, the hydrogels are injected into the vitreous cavity through a small 23G-cannula. The aim of this study was to assess if and to what extent forward light scattering is induced by vitreous body replacement hydrogels and if Stray light differs between different generations of vitreous body hydrogel replacements due to the different gelation mechanisms and fragmentation during injection. A modified C-Quant setup was used to objectively determine forward light scattering. In this study, we found that the 1st and 3rd generation vitreous body replacements show very low stray light levels even after injection (2.8 +/− 0.4 deg2/sr and 0.2 +/− 0.2 deg2/sr, respectively) as gel fragmentation and generation of interfaces is circumvented. The 2nd generation preformed hydrogels showed a permanent increase in stray light after injection that will most likely lead to symptoms such as glare when used in patients (11.9 +/− 0.9 deg2/sr). Stray light of the 2nd generation hydrogels was 3- and 2-fold increased compared to juvenile and aged vitreous bodies, respectively. In conclusion, this significant downside in the forward light scattering of the 2nd generation hydrogels should be kept in mind when developing vitreous body replacement strategies, as any source of stray light should be minimized in patients with retinal comorbidities. Full article
(This article belongs to the Special Issue Advances in Functional Gel)
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20 pages, 1903 KiB  
Review
Engineered Vesicles and Hydrogel Technologies for Myocardial Regeneration
by Kaitlyn Ghassemi, Keiko Inouye, Tatevik Takhmazyan, Victor Bonavida, Jia-Wei Yang, Natan Roberto de Barros and Finosh G. Thankam
Gels 2023, 9(10), 824; https://doi.org/10.3390/gels9100824 - 18 Oct 2023
Cited by 2 | Viewed by 2000
Abstract
Increased prevalence of cardiovascular disease and potentially life-threatening complications of myocardial infarction (MI) has led to emerging therapeutic approaches focusing on myocardial regeneration and restoration of physiologic function following infarction. Extracellular vesicle (EV) technology has gained attention owing to the biological potential to [...] Read more.
Increased prevalence of cardiovascular disease and potentially life-threatening complications of myocardial infarction (MI) has led to emerging therapeutic approaches focusing on myocardial regeneration and restoration of physiologic function following infarction. Extracellular vesicle (EV) technology has gained attention owing to the biological potential to modulate cellular immune responses and promote the repair of damaged tissue. Also, EVs are involved in local and distant cellular communication following damage and play an important role in initiating the repair process. Vesicles derived from stem cells and cardiomyocytes (CM) are of particular interest due to their ability to promote cell growth, proliferation, and angiogenesis following MI. Although a promising candidate for myocardial repair, EV technology is limited by the short retention time of vesicles and rapid elimination by the body. There have been several successful attempts to address this shortcoming, which includes hydrogel technology for the sustained bioavailability of EVs. This review discusses and summarizes current understanding regarding EV technology in the context of myocardial repair. Full article
(This article belongs to the Special Issue Recent Advances in Crosslinked Gels)
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28 pages, 2649 KiB  
Review
Advances in the Development of Nano-Engineered Mechanically Robust Hydrogels for Minimally Invasive Treatment of Bone Defects
by Kulwinder Kaur and Ciara M. Murphy
Gels 2023, 9(10), 809; https://doi.org/10.3390/gels9100809 - 10 Oct 2023
Cited by 3 | Viewed by 2263
Abstract
Injectable hydrogels were discovered as attractive materials for bone tissue engineering applications given their outstanding biocompatibility, high water content, and versatile fabrication platforms into materials with different physiochemical properties. However, traditional hydrogels suffer from weak mechanical strength, limiting their use in heavy load-bearing [...] Read more.
Injectable hydrogels were discovered as attractive materials for bone tissue engineering applications given their outstanding biocompatibility, high water content, and versatile fabrication platforms into materials with different physiochemical properties. However, traditional hydrogels suffer from weak mechanical strength, limiting their use in heavy load-bearing areas. Thus, the fabrication of mechanically robust injectable hydrogels that are suitable for load-bearing environments is of great interest. Successful material design for bone tissue engineering requires an understanding of the composition and structure of the material chosen, as well as the appropriate selection of biomimetic natural or synthetic materials. This review focuses on recent advancements in materials–design considerations and approaches to prepare mechanically robust injectable hydrogels for bone tissue engineering applications. We outline the materials–design approaches through a selection of materials and fabrication methods. Finally, we discuss unmet needs and current challenges in the development of ideal materials for bone tissue regeneration and highlight emerging strategies in the field. Full article
(This article belongs to the Special Issue Biosoursed and Bioinspired Gels for Biomedical Applications)
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15 pages, 1521 KiB  
Article
The Development of a Novel Sodium Alginate-Based Edible Active Hydrogel Coating and Its Application on Traditional Greek Spreadable Cheese
by Aris E. Giannakas, Konstantinos Zaharioudakis, Eleni Kollia, Anna Kopsacheili, Learda Avdylaj, Stavros Georgopoulos, Areti Leontiou, Vassilios K. Karabagias, George Kehayias, Efthymia Ragkava, Charalampos Proestos and Constantinos E. Salmas
Gels 2023, 9(10), 807; https://doi.org/10.3390/gels9100807 - 7 Oct 2023
Cited by 4 | Viewed by 2882
Abstract
The necessity of reducing the greenhouse effect by decreasing the carbon dioxide fingerprint directed the food packaging technology to use biobased raw materials. Alginates, which are derived from brown algae species, are one of the most promising biobased biopolymers for the development of [...] Read more.
The necessity of reducing the greenhouse effect by decreasing the carbon dioxide fingerprint directed the food packaging technology to use biobased raw materials. Alginates, which are derived from brown algae species, are one of the most promising biobased biopolymers for the development of edible active coatings capable of protecting food from oxidation/bacterial spoilage. In this study, sodium alginate, which was plasticized with glycerol and mixed with a biobased thymol/natural halloysite nanohybrid, was used to develop novel edible active coatings. Nanocomposite coatings were also developed in this project by mixing pure halloysite with sodium alginate/glycerol matrix and were used as reference material for comparison reasons. Instrumental analysis indicated a higher compatibility of a thymol/halloysite nanohybrid with a sodium alginate/glycerol matrix compared to pure halloysite with a sodium alginate/glycerol matrix. Increased compatibility resulted in improved tensile properties, water/oxygen barrier properties, and total antioxidant activity. These edible active coatings were applied to traditional Greek spread cheese and showed a reduction in the mesophilic microbial population over one log10 unit (cfu/g) compared to uncoated cheese. Moreover, the reduction in the mesophilic microbial population increased with the increase in halloysite and thymol content, indicating such sodium alginate/glycerol/thymol/halloysite hydrogels as promising edible active coatings for dairy products. Full article
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22 pages, 2129 KiB  
Review
Stimuli-Responsive Hydrogels for Protein Delivery
by Rafaela Malta, Ana Camila Marques, Paulo Cardoso da Costa and Maria Helena Amaral
Gels 2023, 9(10), 802; https://doi.org/10.3390/gels9100802 - 6 Oct 2023
Cited by 6 | Viewed by 2840
Abstract
Proteins and peptides are potential therapeutic agents, but their physiochemical properties make their use as drug substances challenging. Hydrogels are hydrophilic polymeric networks that can swell and retain high amounts of water or biological fluids without being dissolved. Due to their biocompatibility, their [...] Read more.
Proteins and peptides are potential therapeutic agents, but their physiochemical properties make their use as drug substances challenging. Hydrogels are hydrophilic polymeric networks that can swell and retain high amounts of water or biological fluids without being dissolved. Due to their biocompatibility, their porous structure, which enables the transport of various peptides and proteins, and their protective effect against degradation, hydrogels have gained prominence as ideal carriers for these molecules’ delivery. Particularly, stimuli-responsive hydrogels exhibit physicochemical transitions in response to subtle modifications in the surrounding environment, leading to the controlled release of entrapped proteins or peptides. This review is focused on the application of these hydrogels in protein and peptide delivery, including a brief overview of therapeutic proteins and types of stimuli-responsive polymers. Full article
(This article belongs to the Special Issue Advances in Functional Gel)
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38 pages, 5898 KiB  
Review
Emerging Advances in Microfluidic Hydrogel Droplets for Tissue Engineering and STEM Cell Mechanobiology
by Mohamad Orabi and Joe F. Lo
Gels 2023, 9(10), 790; https://doi.org/10.3390/gels9100790 - 1 Oct 2023
Cited by 5 | Viewed by 3736
Abstract
Hydrogel droplets are biodegradable and biocompatible materials with promising applications in tissue engineering, cell encapsulation, and clinical treatments. They represent a well-controlled microstructure to bridge the spatial divide between two-dimensional cell cultures and three-dimensional tissues, toward the recreation of entire organs. The applications [...] Read more.
Hydrogel droplets are biodegradable and biocompatible materials with promising applications in tissue engineering, cell encapsulation, and clinical treatments. They represent a well-controlled microstructure to bridge the spatial divide between two-dimensional cell cultures and three-dimensional tissues, toward the recreation of entire organs. The applications of hydrogel droplets in regenerative medicine require a thorough understanding of microfluidic techniques, the biocompatibility of hydrogel materials, and droplet production and manipulation mechanisms. Although hydrogel droplets were well studied, several emerging advances promise to extend current applications to tissue engineering and beyond. Hydrogel droplets can be designed with high surface-to-volume ratios and a variety of matrix microstructures. Microfluidics provides precise control of the flow patterns required for droplet generation, leading to tight distributions of particle size, shape, matrix, and mechanical properties in the resultant microparticles. This review focuses on recent advances in microfluidic hydrogel droplet generation. First, the theoretical principles of microfluidics, materials used in fabrication, and new 3D fabrication techniques were discussed. Then, the hydrogels used in droplet generation and their cell and tissue engineering applications were reviewed. Finally, droplet generation mechanisms were addressed, such as droplet production, droplet manipulation, and surfactants used to prevent coalescence. Lastly, we propose that microfluidic hydrogel droplets can enable novel shear-related tissue engineering and regeneration studies. Full article
(This article belongs to the Special Issue Hydrogel for Tissue Regeneration)
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40 pages, 1970 KiB  
Review
Aerogel-Based Materials in Bone and Cartilage Tissue Engineering—A Review with Future Implications
by István Lázár, Ladislav Čelko and Melita Menelaou
Gels 2023, 9(9), 746; https://doi.org/10.3390/gels9090746 - 13 Sep 2023
Cited by 8 | Viewed by 3117
Abstract
Aerogels are fascinating solid materials known for their highly porous nanostructure and exceptional physical, chemical, and mechanical properties. They show great promise in various technological and biomedical applications, including tissue engineering, and bone and cartilage substitution. To evaluate the bioactivity of bone substitutes, [...] Read more.
Aerogels are fascinating solid materials known for their highly porous nanostructure and exceptional physical, chemical, and mechanical properties. They show great promise in various technological and biomedical applications, including tissue engineering, and bone and cartilage substitution. To evaluate the bioactivity of bone substitutes, researchers typically conduct in vitro tests using simulated body fluids and specific cell lines, while in vivo testing involves the study of materials in different animal species. In this context, our primary focus is to investigate the applications of different types of aerogels, considering their specific materials, microstructure, and porosity in the field of bone and cartilage tissue engineering. From clinically approved materials to experimental aerogels, we present a comprehensive list and summary of various aerogel building blocks and their biological activities. Additionally, we explore how the complexity of aerogel scaffolds influences their in vivo performance, ranging from simple single-component or hybrid aerogels to more intricate and organized structures. We also discuss commonly used formulation and drying methods in aerogel chemistry, including molding, freeze casting, supercritical foaming, freeze drying, subcritical, and supercritical drying techniques. These techniques play a crucial role in shaping aerogels for specific applications. Alongside the progress made, we acknowledge the challenges ahead and assess the near and far future of aerogel-based hard tissue engineering materials, as well as their potential connection with emerging healing techniques. Full article
(This article belongs to the Special Issue Aerogel Hybrids and Nanocomposites)
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19 pages, 10628 KiB  
Article
Self-Healing of Pluronic® F127 Hydrogels in the Presence of Various Polysaccharides
by Alexandra Lupu, Luiza Madalina Gradinaru, Daniela Rusu and Maria Bercea
Gels 2023, 9(9), 719; https://doi.org/10.3390/gels9090719 - 5 Sep 2023
Cited by 8 | Viewed by 3500
Abstract
Thermoresponsive Pluronic® F127 (PL) gels in water were investigated through rheological tests in different shear conditions. The gel strength was tuned with the addition of 1% polysaccharide solution. In the presence of xanthan gum (XG), the viscoelastic behavior of PL-based hydrogels was improved [...] Read more.
Thermoresponsive Pluronic® F127 (PL) gels in water were investigated through rheological tests in different shear conditions. The gel strength was tuned with the addition of 1% polysaccharide solution. In the presence of xanthan gum (XG), the viscoelastic behavior of PL-based hydrogels was improved in aqueous environment, but the rheological behavior was less changed with the addition of XG in PBS solutions, whereas in the presence of 0.1 M NaCl, the viscoelastic parameters decreased. PL micellar networks exhibited a self-healing ability, recovering their initial structure after applying cycles of high strain. The rheological characteristics of the PL hydrogel changed with the addition of 1% polysaccharides (xanthan gum, alginate, κ-carrageenan, gellan, or chitosan). PL/polysaccharide systems form temperature-responsive hydrogels with shear thinning behavior, yield stress, and self-healing ability, being considered a versatile platform for injectable biomaterials or bioinks. Thus, in the presence of xanthan gum in aqueous medium, the gel strength was improved after applying a high strain (the values of elastic modulus increased). The other investigated natural polymers induced specific self-healing behaviors. Good performances were observed with the addition of gellan gum, alginate, and κ-carrageenan, but for high values of strain, the ability to recover the initial structure decreased. A modest self-healing behavior was observed in the presence of chitosan and xanthan gum dissolved in NaCl solution. Full article
(This article belongs to the Special Issue Hydrogel-Based Novel Biomaterials: Achievements and Prospects)
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20 pages, 10831 KiB  
Article
Composite Hydrogels with Embedded Silver Nanoparticles and Ibuprofen as Wound Dressing
by Irina Popescu, Marieta Constantin, Gheorghe Solcan, Daniela Luminita Ichim, Delia Mihaela Rata, Loredana Horodincu and Carmen Solcan
Gels 2023, 9(8), 654; https://doi.org/10.3390/gels9080654 - 14 Aug 2023
Cited by 9 | Viewed by 2505
Abstract
The wound healing process is often slowed down as a result of complications from bacterial infections and inflammatory reactions. Therefore, it is necessary to develop dressings with fast antibacterial and anti-inflammatory activity that shorten the wound healing period by promoting cell migration and [...] Read more.
The wound healing process is often slowed down as a result of complications from bacterial infections and inflammatory reactions. Therefore, it is necessary to develop dressings with fast antibacterial and anti-inflammatory activity that shorten the wound healing period by promoting cell migration and proliferation. Chitosan (CS)-based hydrogels have been widely studied for their antibacterial and wound healing capabilities. Herein, we developed a composite hydrogel based on CS and PVA embedding silver nanoparticles (AgNPs) with antibacterial properties and ibuprofen (Ib) as an anti-inflammatory agent. The hydrogel prepared by double physical cross-linking, with oxalic acid and by freeze–thawing, loaded with 0.225 wt.% AgNPs and 0.264 wt.% Ib, displayed good mechanical properties (compressive modulus = 132 kPa), a high swelling degree and sustained drug delivery (in simulated skin conditions). Moreover, the hydrogel showed strong antibacterial activity against S. aureus and K. pneumoniae due to the embedded AgNPs. In vivo, this hydrogel accelerated the wound regeneration process through the enhanced expression of TNF alpha IP8, by activating downstream cascades and supporting the healing process of inflammation; Cox2, which enhances the migration and proliferation of cells involved in re-epithelization and angiogenesis; MHCII, which promotes immune cooperation between local cells, eliminating dead tissue and controlling infection; the intense expression of Col I as a major marker in the tissue granulation process; and αSMA, which marks the presence of myofibroblasts involved in wound closure and indicates ongoing re-epithelization. The results reveal the potential healing effect of CS/PVA/AgNPs/Ib hydrogels and suggest their potential use as wound dressings. Full article
(This article belongs to the Special Issue Recent Advances in Hydrogels for Wound Healing)
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18 pages, 4531 KiB  
Article
Development of Blended Biopolymer-Based Photocatalytic Hydrogel Beads for Adsorption and Photodegradation of Dyes
by Seung Hyeon Weon, Jiwoo Han, Yong-Keun Choi, Saerom Park and Sang Hyun Lee
Gels 2023, 9(8), 630; https://doi.org/10.3390/gels9080630 - 5 Aug 2023
Cited by 7 | Viewed by 1962
Abstract
Blended biopolymer-based photocatalytic hydrogel beads were synthesized by dissolving the biopolymers in 1-ethyl-3-methylimidazolium acetate ([Emim][Ac]), adding TiO2, and reconstituting the beads with ethanol. The incorporation of modifying biopolymer significantly enhanced the adsorption capacity of the cellulose/TiO2 beads. Cellulose/carrageenan/TiO2 beads [...] Read more.
Blended biopolymer-based photocatalytic hydrogel beads were synthesized by dissolving the biopolymers in 1-ethyl-3-methylimidazolium acetate ([Emim][Ac]), adding TiO2, and reconstituting the beads with ethanol. The incorporation of modifying biopolymer significantly enhanced the adsorption capacity of the cellulose/TiO2 beads. Cellulose/carrageenan/TiO2 beads exhibited a 7.0-fold increase in adsorption capacity for methylene blue (MB). In contrast, cellulose/chitosan/TiO2 beads showed a 4.8-fold increase in adsorption capacity for methyl orange (MO) compared with cellulose/TiO2 beads. In addition, cellulose/TiO2 microbeads were prepared through the sol–gel transition of the [Emim][Ac]-in-oil emulsion to enhance photodegradation activity. These microbeads displayed a 4.6-fold higher adsorption capacity and 2.8-fold higher photodegradation activity for MB than the millimeter-sized beads. Furthermore, they exhibited superior dye removal efficiencies for various dyes such as Congo red, MO, MB, crystal violet, and rhodamine B, surpassing the performance of larger beads. To expand the industrial applicability of the microbeads, biopolymer/TiO2 magnetic microbeads were developed by incorporating Fe2O3. These magnetic microbeads outperformed millimeter-sized beads regarding the efficiency and time required for MB removal from aqueous solutions. Furthermore, the physicochemical properties of magnetic microbeads can be easily controlled by adjusting the type of biopolymer modifier, the TiO2 and magnetic particle content, and the ratio of each component based on the target molecule. Therefore, biopolymer-based photocatalytic magnetic microbeads have great potential not only in environmental fields but also in biomedical fields. Full article
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20 pages, 1202 KiB  
Review
Unraveling the New Perspectives on Antimicrobial Hydrogels: State-of-the-Art and Translational Applications
by Miguel A. Ortega, Diego De Leon-Oliva, Diego Liviu Boaru, Oscar Fraile-Martinez, Cielo García-Montero, Raul Diaz, Santiago Coca, Silvestra Barrena-Blázquez, Julia Bujan, Natalio García-Honduvilla, Miguel A. Saez, Melchor Álvarez-Mon and Jose V. Saz
Gels 2023, 9(8), 617; https://doi.org/10.3390/gels9080617 - 29 Jul 2023
Cited by 5 | Viewed by 2106
Abstract
The growing impact of infections and the rapid emergence of antibiotic resistance represent a public health concern worldwide. The exponential development in the field of biomaterials and its multiple applications can offer a solution to the problems that derive from these situations. In [...] Read more.
The growing impact of infections and the rapid emergence of antibiotic resistance represent a public health concern worldwide. The exponential development in the field of biomaterials and its multiple applications can offer a solution to the problems that derive from these situations. In this sense, antimicrobial hydrogels represent a promising opportunity with multiple translational expectations in the medical management of infectious diseases due to their unique physicochemical and biological properties as well as for drug delivery in specific areas. Hydrogels are three-dimensional cross-linked networks of hydrophilic polymers that can absorb and retain large amounts of water or biological fluids. Moreover, antimicrobial hydrogels (AMH) present good biocompatibility, low toxicity, availability, viscoelasticity, biodegradability, and antimicrobial properties. In the present review, we collect and discuss the most promising strategies in the development of AMH, which are divided into hydrogels with inherent antimicrobial activity and antimicrobial agent-loaded hydrogels based on their composition. Then, we present an overview of the main translational applications: wound healing, tissue engineering and regeneration, drug delivery systems, contact lenses, 3D printing, biosensing, and water purification. Full article
(This article belongs to the Special Issue Antibacterial Gels)
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15 pages, 903 KiB  
Review
Injectable Poloxamer Hydrogels for Local Cancer Therapy
by Ana Camila Marques, Paulo Cardoso Costa, Sérgia Velho and Maria Helena Amaral
Gels 2023, 9(7), 593; https://doi.org/10.3390/gels9070593 - 24 Jul 2023
Cited by 12 | Viewed by 3677
Abstract
The widespread push to invest in local cancer therapies comes from the need to overcome the limitations of systemic treatment options. In contrast to intravenous administration, local treatments using intratumoral or peritumoral injections are independent of tumor vasculature and allow high concentrations of [...] Read more.
The widespread push to invest in local cancer therapies comes from the need to overcome the limitations of systemic treatment options. In contrast to intravenous administration, local treatments using intratumoral or peritumoral injections are independent of tumor vasculature and allow high concentrations of therapeutic agents to reach the tumor site with minimal systemic toxicity. Injectable biodegradable hydrogels offer a clear advantage over other delivery systems because the former requires no surgical procedures and promotes drug retention at the tumor site. More precisely, in situ gelling systems based on poloxamers have garnered considerable attention due to their thermoresponsive behavior, biocompatibility, ease of preparation, and possible incorporation of different anticancer agents. Therefore, this review focuses on the use of injectable thermoresponsive hydrogels based on poloxamers and their physicochemical and biological characterization. It also includes a summary of these hydrogel applications in local cancer therapies using chemotherapy, phototherapy, immunotherapy, and gene therapy. Full article
(This article belongs to the Special Issue Hydrogel-Based Novel Biomaterials: Achievements and Prospects)
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17 pages, 5165 KiB  
Article
Functional Hydrogels for Agricultural Application
by Romana Kratochvílová, Milan Kráčalík, Marcela Smilková, Petr Sedláček, Miloslav Pekař, Elke Bradt, Jiří Smilek, Petra Závodská and Martina Klučáková
Gels 2023, 9(7), 590; https://doi.org/10.3390/gels9070590 - 22 Jul 2023
Cited by 4 | Viewed by 1953
Abstract
Ten different hydrogels were prepared and analyzed from the point of view of their use in soil. FT-IR spectra, morphology, swelling ability, and rheological properties were determined for their characterization and appraisal of their stability. The aim was to characterize prepared materials containing [...] Read more.
Ten different hydrogels were prepared and analyzed from the point of view of their use in soil. FT-IR spectra, morphology, swelling ability, and rheological properties were determined for their characterization and appraisal of their stability. The aim was to characterize prepared materials containing different amounts of NPK as mineral fertilizer, lignohumate as a source of organic carbon, and its combination. This study of stability was focused on utility properties in their application in soil—repeated drying/re-swelling cycles and possible freezing in winter. Lignohumate supported the water absorbency, while the addition of NPK caused a negative effect. Pore sizes decreased with NPK addition. Lignohumate incorporated into polymers resulted in a much miscellaneous structure, rich in different pores and voids of with a wide range of sizes. NPK fertilizer supported the elastic character of prepared materials, while the addition of lignohumate shifted their rheological behavior to more liquid. Both dynamic moduli decreased in time. The most stable samples appeared to contain only one fertilizer constituent (NPK or lignohumate). Repeated re-swelling resulted in an increase in elastic character, which was connected with the gradual release of fertilizers. A similar effect was observed with samples that were frozen and defrosted, except samples containing a higher amount of NPK without lignohumate. A positive effect of acrylamide on superabsorbent properties was not confirmed. Full article
(This article belongs to the Special Issue Advances in Smart and Tough Hydrogels)
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28 pages, 2738 KiB  
Review
High-Performing Conductive Hydrogels for Wearable Applications
by Hossein Omidian and Sumana Dey Chowdhury
Gels 2023, 9(7), 549; https://doi.org/10.3390/gels9070549 - 6 Jul 2023
Cited by 9 | Viewed by 3384
Abstract
Conductive hydrogels have gained significant attention for their extensive applications in healthcare monitoring, wearable sensors, electronic devices, soft robotics, energy storage, and human–machine interfaces. To address the limitations of conductive hydrogels, researchers are focused on enhancing properties such as sensitivity, mechanical strength, electrical [...] Read more.
Conductive hydrogels have gained significant attention for their extensive applications in healthcare monitoring, wearable sensors, electronic devices, soft robotics, energy storage, and human–machine interfaces. To address the limitations of conductive hydrogels, researchers are focused on enhancing properties such as sensitivity, mechanical strength, electrical performance at low temperatures, stability, antibacterial properties, and conductivity. Composite materials, including nanoparticles, nanowires, polymers, and ionic liquids, are incorporated to improve the conductivity and mechanical strength. Biocompatibility and biosafety are emphasized for safe integration with biological tissues. Conductive hydrogels exhibit unique properties such as stretchability, self-healing, wet adhesion, anti-freezing, transparency, UV-shielding, and adjustable mechanical properties, making them suitable for specific applications. Researchers aim to develop multifunctional hydrogels with antibacterial characteristics, self-healing capabilities, transparency, UV-shielding, gas-sensing, and strain-sensitivity. Full article
(This article belongs to the Special Issue Gels for Flexible Electronics and Energy Devices)
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30 pages, 9896 KiB  
Review
Aloe vera-Based Hydrogels for Wound Healing: Properties and Therapeutic Effects
by Mariana Chelu, Adina Magdalena Musuc, Monica Popa and Jose Calderon Moreno
Gels 2023, 9(7), 539; https://doi.org/10.3390/gels9070539 - 3 Jul 2023
Cited by 25 | Viewed by 18534
Abstract
Aloe vera-based hydrogels have emerged as promising platforms for the delivery of therapeutic agents in wound dressings due to their biocompatibility and unique wound-healing properties. The present study provides a comprehensive overview of recent advances in the application of Aloe vera-based [...] Read more.
Aloe vera-based hydrogels have emerged as promising platforms for the delivery of therapeutic agents in wound dressings due to their biocompatibility and unique wound-healing properties. The present study provides a comprehensive overview of recent advances in the application of Aloe vera-based hydrogels for wound healing. The synthesis methods, structural characteristics, and properties of Aloe vera-based hydrogels are discussed. Mechanisms of therapeutic agents released from Aloe vera-based hydrogels, including diffusion, swelling, and degradation, are also analyzed. In addition, the therapeutic effects of Aloe vera-based hydrogels on wound healing, as well as the reduction of inflammation, antimicrobial activity, and tissue regeneration, are highlighted. The incorporation of various therapeutic agents, such as antimicrobial and anti-inflammatory ones, into Aloe vera-based hydrogels is reviewed in detail. Furthermore, challenges and future prospects of Aloe vera-based hydrogels for wound dressing applications are considered. This review provides valuable information on the current status of Aloe vera-based hydrogels for the delivery of therapeutic agents in wound dressings and highlights their potential to improve wound healing outcomes. Full article
(This article belongs to the Special Issue Hydrogel for Sustained Delivery of Therapeutic Agents)
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13 pages, 3756 KiB  
Article
Dual pH- and Thermo-Sensitive Poly(N-isopropylacrylamide-co-allylamine) Nanogels for Curcumin Delivery: Swelling–Deswelling Behavior and Phase Transition Mechanism
by Madhappan Santhamoorthy and Seong-Cheol Kim
Gels 2023, 9(7), 536; https://doi.org/10.3390/gels9070536 - 1 Jul 2023
Cited by 4 | Viewed by 2207
Abstract
Curcumin (Cur) is a beneficial ingredient with numerous bioactivities. However, due to its low solubility and poor bioavailability, its therapeutic application is limited. In this work, we prepared poly-N-isopropylacrylamide p(NIPAm) and polyallylamine p(Am)-based nanogel (p(NIPAm-co-Am)) NG for a dual pH- and temperature-sensitive copolymer [...] Read more.
Curcumin (Cur) is a beneficial ingredient with numerous bioactivities. However, due to its low solubility and poor bioavailability, its therapeutic application is limited. In this work, we prepared poly-N-isopropylacrylamide p(NIPAm) and polyallylamine p(Am)-based nanogel (p(NIPAm-co-Am)) NG for a dual pH- and temperature-sensitive copolymer system for drug delivery application. In this copolymer system, the p(NIPAm) segment was incorporated to introduce thermoresponsive behavior and the p(Am) segment was incorporated to introduce drug binding sites (amine groups) in the resulting (p(NIPAm-co-Am)) NG system. Various instrumental characterizations including 1H nuclear magnetic resonance (1H NMR) spectroscopy, Fourier transform infrared (FT-IR) analysis, scanning electron microscopy (SEM), zeta potential, and particle size analysis were performed to confirm the copolymer synthesis. Curcumin (Cur), an anticancer bioactive substance, was employed to assess the in vitro drug loading and release performance of the resulting copolymer nanogels system at varied pH levels (pH 7.2, 6.5, and 4.0) and temperatures (25 °C, 37 °C, and 42 °C). The cytocompatibility of the p(NIPAm-co-Am) NG sample was also tested on MDA-MB-231 cells at various sample concentrations. All the study results indicate that the p(NIPAm-co-Am) NG produced might be effective for drug loading and release under pH and temperature dual-stimuli conditions. As a result, the p(NIPAm-co-Am) NG system has the potential to be beneficial in the use of drug delivery applications in cancer therapy. Full article
(This article belongs to the Special Issue Recent Advances in Gels Engineering for Drug Delivery)
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21 pages, 3893 KiB  
Review
Essential Guide to Hydrogel Rheology in Extrusion 3D Printing: How to Measure It and Why It Matters?
by Helena Herrada-Manchón, Manuel Alejandro Fernández and Enrique Aguilar
Gels 2023, 9(7), 517; https://doi.org/10.3390/gels9070517 - 26 Jun 2023
Cited by 38 | Viewed by 8444
Abstract
Rheology plays a crucial role in the field of extrusion-based three-dimensional (3D) printing, particularly in the context of hydrogels. Hydrogels have gained popularity in 3D printing due to their potential applications in tissue engineering, regenerative medicine, and drug delivery. The rheological properties of [...] Read more.
Rheology plays a crucial role in the field of extrusion-based three-dimensional (3D) printing, particularly in the context of hydrogels. Hydrogels have gained popularity in 3D printing due to their potential applications in tissue engineering, regenerative medicine, and drug delivery. The rheological properties of the printing material have a significant impact on its behaviour throughout the 3D printing process, including its extrudability, shape retention, and response to stress and strain. Thus, understanding the rheological characteristics of hydrogels, such as shear thinning behaviour, thixotropy, viscoelasticity, and gelling mechanisms, is essential for optimising the printing process and achieving desired product quality and accuracy. This review discusses the theoretical foundations of rheology, explores different types of fluid and their properties, and discusses the essential rheological tests necessary for characterising hydrogels. The paper emphasises the importance of terminology, concepts, and the correct interpretation of results in evaluating hydrogel formulations. By presenting a detailed understanding of rheology in the context of 3D printing, this review paper aims to assist researchers, engineers, and practitioners in the field of hydrogel-based 3D printing in optimizing their printing processes and achieving desired product outcomes. Full article
(This article belongs to the Special Issue Hydrogels for 3D Printing)
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14 pages, 1404 KiB  
Article
Dielectric Study on Supramolecular Gels by Fiber Structure Formation from Low-Molecular-Weight Gelator/Water Mixtures
by Kenta Shimizu, Fumiya Abe, Yasuhiro Kishi, Rio Kita, Naoki Shinyashiki and Shin Yagihara
Gels 2023, 9(5), 408; https://doi.org/10.3390/gels9050408 - 12 May 2023
Cited by 2 | Viewed by 1744
Abstract
There are various types of gel materials used in a wide range of fields, and their gelation mechanisms are extremely diverse. Furthermore, in the case of hydrogels, there exist some difficulties in understanding complicated molecular mechanisms especially with water molecules interacting through hydrogen [...] Read more.
There are various types of gel materials used in a wide range of fields, and their gelation mechanisms are extremely diverse. Furthermore, in the case of hydrogels, there exist some difficulties in understanding complicated molecular mechanisms especially with water molecules interacting through hydrogen bonding as solvents. In the present work, the molecular mechanism of the structural formation of fibrous super-molecular gel by the low molecular weight gelator, N-oleyl lactobionamide/water mixture was elucidated using the broadband dielectric spectroscopy (BDS) method. The dynamic behaviors observed for the solute and water molecules indicated hierarchical structure formation processes in various time scales. The relaxation curves obtained at various temperatures in the cooling and heating processes showed relaxation processes respectively reflecting the dynamic behaviors of water molecules in the 10 GHz frequency region, solute molecules interacting with water in MHz region, and ion-reflecting structures of the sample and electrode in kHz region. These relaxation processes, characterized by the relaxation parameters, showed remarkable changes around the sol–gel transition temperature, 37.8 °C, determined by the falling ball method and over the temperature range, around 53 °C. The latter change suggested a structure formation of rod micelles appearing as precursors before cross-linking into the three-dimensional network of the supramolecular gels. These results clearly demonstrate how effective relaxation parameter analysis is for understanding the gelation mechanism in detail. Full article
(This article belongs to the Special Issue Shaping and Structuring of Polymer Gels)
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16 pages, 2717 KiB  
Article
Effects of Steam Sterilization on the Properties of Stimuli-Responsive Polymer-Based Hydrogels
by Inês Ferreira, Ana Camila Marques, Paulo Cardoso Costa and Maria Helena Amaral
Gels 2023, 9(5), 385; https://doi.org/10.3390/gels9050385 - 6 May 2023
Cited by 3 | Viewed by 2759
Abstract
Hydrogels based on stimuli-responsive polymers can change their characteristics in response to small variations in environmental conditions, such as temperature, pH, and ionic strength, among others. In the case of some routes of administration, such as ophthalmic and parenteral, the formulations must meet [...] Read more.
Hydrogels based on stimuli-responsive polymers can change their characteristics in response to small variations in environmental conditions, such as temperature, pH, and ionic strength, among others. In the case of some routes of administration, such as ophthalmic and parenteral, the formulations must meet specific requirements, namely sterility. Therefore, it is essential to study the effect of the sterilization method on the integrity of smart gel systems. Thus, this work aimed to study the effect of steam sterilization (121 °C, 15 min) on the properties of hydrogels based on the following stimuli-responsive polymers: Carbopol® 940, Pluronic® F-127, and sodium alginate. The properties of the prepared hydrogels—pH, texture, rheological behavior, and sol-gel phase transition—were evaluated to compare and identify the differences between sterilized and non-sterilized hydrogels. The influence of steam sterilization on physicochemical stability was also investigated by Fourier-transform infrared spectroscopy and differential scanning calorimetry. The results of this study showed that the Carbopol® 940 hydrogel was the one that suffered fewer changes in the studied properties after sterilization. By contrast, sterilization was found to cause slight changes in the Pluronic® F-127 hydrogel regarding gelation temperature/time, as well as a considerable decrease in the viscosity of the sodium alginate hydrogel. There were no considerable differences in the chemical and physical characteristics of the hydrogels after steam sterilization. It is possible to conclude that steam sterilization is suitable for Carbopol® 940 hydrogels. Contrarily, this technique does not seem adequate for the sterilization of alginate or Pluronic® F-127 hydrogels, as it could considerably alter their properties. Full article
(This article belongs to the Special Issue Advances in Functional Gel)
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20 pages, 6671 KiB  
Article
Chitosan-Silica Hybrid Biomaterials for Bone Tissue Engineering: A Comparative Study of Xerogels and Aerogels
by Antonio Pérez-Moreno, Manuel Piñero, Rafael Fernández-Montesinos, Gonzalo Pinaglia-Tobaruela, María V. Reyes-Peces, María del Mar Mesa-Díaz, José Ignacio Vilches-Pérez, Luis Esquivias, Nicolás de la Rosa-Fox and Mercedes Salido
Gels 2023, 9(5), 383; https://doi.org/10.3390/gels9050383 - 5 May 2023
Cited by 12 | Viewed by 2027
Abstract
Chitosan (CS) is a natural biopolymer that shows promise as a biomaterial for bone-tissue regeneration. However, because of their limited ability to induce cell differentiation and high degradation rate, among other drawbacks associated with its use, the creation of CS-based biomaterials remains a [...] Read more.
Chitosan (CS) is a natural biopolymer that shows promise as a biomaterial for bone-tissue regeneration. However, because of their limited ability to induce cell differentiation and high degradation rate, among other drawbacks associated with its use, the creation of CS-based biomaterials remains a problem in bone tissue engineering research. Here we aimed to reduce these disadvantages while retaining the benefits of potential CS biomaterial by combining it with silica to provide sufficient additional structural support for bone regeneration. In this work, CS-silica xerogel and aerogel hybrids with 8 wt.% CS content, designated SCS8X and SCS8A, respectively, were prepared by sol-gel method, either by direct solvent evaporation at the atmospheric pressure or by supercritical drying in CO2, respectively. As reported in previous studies, it was confirmed that both types of mesoporous materials exhibited large surface areas (821 m2g−1–858 m2g−1) and outstanding bioactivity, as well as osteoconductive properties. In addition to silica and chitosan, the inclusion of 10 wt.% of tricalcium phosphate (TCP), designated SCS8T10X, was also considered, which stimulates a fast bioactive response of the xerogel surface. The results here obtained also demonstrate that xerogels induced earlier cell differentiation than the aerogels with identical composition. In conclusion, our study shows that the sol-gel synthesis of CS-silica xerogels and aerogels enhances not only their bioactive response, but also osteoconduction and cell differentiation properties. Therefore, these new biomaterials should provide adequate secretion of the osteoid for a fast bone regeneration. Full article
(This article belongs to the Special Issue Aerogel Hybrids and Nanocomposites)
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48 pages, 9421 KiB  
Review
Diversity of Bioinspired Hydrogels: From Structure to Applications
by Alexandra Lupu, Luiza Madalina Gradinaru, Vasile Robert Gradinaru and Maria Bercea
Gels 2023, 9(5), 376; https://doi.org/10.3390/gels9050376 - 2 May 2023
Cited by 13 | Viewed by 3222
Abstract
Hydrogels are three-dimensional networks with a variety of structures and functions that have a remarkable ability to absorb huge amounts of water or biological fluids. They can incorporate active compounds and release them in a controlled manner. Hydrogels can also be designed to [...] Read more.
Hydrogels are three-dimensional networks with a variety of structures and functions that have a remarkable ability to absorb huge amounts of water or biological fluids. They can incorporate active compounds and release them in a controlled manner. Hydrogels can also be designed to be sensitive to external stimuli: temperature, pH, ionic strength, electrical or magnetic stimuli, specific molecules, etc. Alternative methods for the development of various hydrogels have been outlined in the literature over time. Some hydrogels are toxic and therefore are avoided when obtaining biomaterials, pharmaceuticals, or therapeutic products. Nature is a permanent source of inspiration for new structures and new functionalities of more and more competitive materials. Natural compounds present a series of physico-chemical and biological characteristics suitable for biomaterials, such as biocompatibility, antimicrobial properties, biodegradability, and nontoxicity. Thus, they can generate microenvironments comparable to the intracellular or extracellular matrices in the human body. This paper discusses the main advantages of the presence of biomolecules (polysaccharides, proteins, and polypeptides) in hydrogels. Structural aspects induced by natural compounds and their specific properties are emphasized. The most suitable applications will be highlighted, including drug delivery, self-healing materials for regenerative medicine, cell culture, wound dressings, 3D bioprinting, foods, etc. Full article
(This article belongs to the Special Issue Structured Gels: Mechanics, Responsivity and Applications)
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19 pages, 4402 KiB  
Article
New Methacrylated Biopolymer-Based Hydrogels as Localized Drug Delivery Systems in Skin Cancer Therapy
by Andreea Luca, Isabella Nacu, Sabina Tanasache, Cătălina Anişoara Peptu, Maria Butnaru and Liliana Verestiuc
Gels 2023, 9(5), 371; https://doi.org/10.3390/gels9050371 - 1 May 2023
Cited by 7 | Viewed by 2626
Abstract
The aim of the present work was to obtain drug-loaded hydrogels based on combinations of dextran, chitosan/gelatin/xanthan, and poly (acrylamide) as a sustained and controlled release vehicle of Doxorubicin, a drug used in skin cancer therapy that is associated with severe side effects. [...] Read more.
The aim of the present work was to obtain drug-loaded hydrogels based on combinations of dextran, chitosan/gelatin/xanthan, and poly (acrylamide) as a sustained and controlled release vehicle of Doxorubicin, a drug used in skin cancer therapy that is associated with severe side effects. Hydrogels for use as 3D hydrophilic networks with good manipulation characteristics were produced using methacrylated biopolymer derivatives and the methacrylate group’s polymerization with synthetic monomers in the presence of a photo-initiator, under UV light stimulation (365 nm). Transformed infrared spectroscopy analysis (FT-IR) confirmed the hydrogels’ network structure (natural–synthetic composition and photocrosslinking), while scanning electron microscopy (SEM) analysis confirmed the microporous morphology. The hydrogels are swellable in simulated biological fluids and the material’s morphology regulates the swelling properties: the maximum swelling degree was obtained for dextran–chitosan-based hydrogels because of their higher porosity and pore distribution. The hydrogels are bioadhesive on a biological simulating membrane, and values for the force of detachment and work of adhesion are recommended for applications on skin tissue. The Doxorubicin was loaded into the hydrogels and the drug was released by diffusion for all the resulting hydrogels, with small contributions from the hydrogel networks’ relaxation. Doxorubicin-loaded hydrogels are efficient on keratinocytes tumor cells, the sustained released drug interrupting the cells’ division and inducing cell apoptosis; we recommend the obtained materials for the topical treatment of cutaneous squamous cell carcinoma. Full article
(This article belongs to the Special Issue Smart Hydrogels: From Rational Design to Applications)
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14 pages, 5050 KiB  
Article
Tissue Adhesive, Biocompatible, Antioxidant, and Antibacterial Hydrogels Based on Tannic Acid and Fungal-Derived Carboxymethyl Chitosan for Wound-Dressing Applications
by Kummara Madhusudana Rao, Uluvangada Thammaiah Uthappa, Hyeon Jin Kim and Sung Soo Han
Gels 2023, 9(5), 354; https://doi.org/10.3390/gels9050354 - 22 Apr 2023
Cited by 12 | Viewed by 2378
Abstract
This study aimed to develop hydrogels for tissue adhesion that are biocompatible, antioxidant, and antibacterial. We achieved this by using tannic acid (TA) and fungal-derived carboxymethyl chitosan (FCMCS) incorporated in a polyacrylamide (PAM) network using free-radical polymerization. The concentration of TA greatly influenced [...] Read more.
This study aimed to develop hydrogels for tissue adhesion that are biocompatible, antioxidant, and antibacterial. We achieved this by using tannic acid (TA) and fungal-derived carboxymethyl chitosan (FCMCS) incorporated in a polyacrylamide (PAM) network using free-radical polymerization. The concentration of TA greatly influenced the physicochemical and biological properties of the hydrogels. Scanning electron microscopy showed that the nanoporous structure of the FCMCS hydrogel was retained with the addition of TA, resulting in a nanoporous surface structure. Equilibrium-swelling experiments revealed that increasing the concentration of TA significantly improved water uptake capacity. Antioxidant radical-scavenging assays and porcine skin adhesion tests confirmed the excellent adhesive properties of the hydrogels, with adhesion strengths of up to 39.8 ± 1.2 kPa for 1.0TA-FCMCS due to the presence of abundant phenolic groups on TA. The hydrogels were also found to be biocompatible with skin fibroblast cells. Furthermore, the presence of TA significantly enhanced the antibacterial properties of the hydrogels against both Gram-positive (Staphylococcus aureus) and Gram-negative (Escherichia coli) bacteria. Therefore, the developed drug-free antibacterial and tissue-adhesive hydrogels can potentially be used as wound dressings for infected wounds. Full article
(This article belongs to the Special Issue Recent Developments in Chitosan Hydrogels)
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15 pages, 6503 KiB  
Article
Dehydrofluorination Process of Poly(vinylidene difluoride) PVdF-Based Gel Polymer Electrolytes and Its Effect on Lithium-Sulfur Batteries
by Julen Castillo, Adrián Robles-Fernandez, Rosalía Cid, José Antonio González-Marcos, Michel Armand, Daniel Carriazo, Heng Zhang and Alexander Santiago
Gels 2023, 9(4), 336; https://doi.org/10.3390/gels9040336 - 14 Apr 2023
Cited by 10 | Viewed by 3430
Abstract
Gel polymer electrolytes (GPEs) are emerging as suitable candidates for high-performing lithium-sulfur batteries (LSBs) due to their excellent performance and improved safety. Within them, poly(vinylidene difluoride) (PVdF) and its derivatives have been widely used as polymer hosts due to their ideal mechanical and [...] Read more.
Gel polymer electrolytes (GPEs) are emerging as suitable candidates for high-performing lithium-sulfur batteries (LSBs) due to their excellent performance and improved safety. Within them, poly(vinylidene difluoride) (PVdF) and its derivatives have been widely used as polymer hosts due to their ideal mechanical and electrochemical properties. However, their poor stability with lithium metal (Li0) anode has been identified as their main drawback. Here, the stability of two PVdF-based GPEs with Li0 and their application in LSBs is studied. PVdF-based GPEs undergo a dehydrofluorination process upon contact with the Li0. This process results in the formation of a LiF-rich solid electrolyte interphase that provides high stability during galvanostatic cycling. Nevertheless, despite their outstanding initial discharge, both GPEs show an unsuitable battery performance characterized by a capacity drop, ascribed to the loss of the lithium polysulfides and their interaction with the dehydrofluorinated polymer host. Through the introduction of an intriguing lithium salt (lithium nitrate) in the electrolyte, a significant improvement is achieved delivering higher capacity retention. Apart from providing a detailed study of the hitherto poorly characterized interaction process between PVdF-based GPEs and the Li0, this study demonstrates the need for an anode protection process to use this type of electrolytes in LSBs. Full article
(This article belongs to the Special Issue Gel-Based Electrolytes for Solid-State Electrochemical Devices)
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