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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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39 pages, 1821 KB  
Review
Hydrogel Development, Processing and Applications in Agriculture: A Review
by Carmen Mª. Granados-Carrera, Victor M. Perez-Puyana, Mercedes Jiménez-Rosado and Alberto Romero
Gels 2026, 12(3), 259; https://doi.org/10.3390/gels12030259 - 20 Mar 2026
Cited by 1 | Viewed by 1950
Abstract
Hydrogels have emerged as promising functional materials for improving water management and nutrient delivery in agriculture, particularly under conditions of increasing water scarcity and declining soil fertility. However, most commercially available superabsorbent hydrogels are based on petroleum-derived polymers, raising concerns regarding their persistence [...] Read more.
Hydrogels have emerged as promising functional materials for improving water management and nutrient delivery in agriculture, particularly under conditions of increasing water scarcity and declining soil fertility. However, most commercially available superabsorbent hydrogels are based on petroleum-derived polymers, raising concerns regarding their persistence in soils, potential microplastic formation and long-term environmental impact. In response, significant research efforts are being directed toward the development of biodegradable hydrogels derived from renewable biopolymers. This review provides a critical overview of recent advances in hydrogel systems designed for agricultural applications, with a particular focus on biopolymer-based materials. First, the current landscape of hydrogel technologies used as soil conditioners and controlled-release systems for agrochemicals is contextualized, highlighting the limitations of conventional synthetic hydrogels. Subsequently, the main classes of natural polymers explored for hydrogel fabrication, including polysaccharides (e.g., chitosan, alginate, cellulose and starch) and proteins (e.g., gelatin, keratin and soy protein), are analyzed in terms of raw material sources, gelation mechanisms and structure–property relationships. Their performance in key agricultural functions, such as water retention, controlled nutrient release, soil conditioning and enhancement of plant growth, is also discussed. Finally, the review identifies major challenges that currently hinder large-scale implementation, including mechanical stability, degradation behavior in complex soil environments, nutrient release control and economic scalability. By integrating recent progress and outlining emerging research directions, this work aims to support the rational design of next-generation biodegradable hydrogels capable of contributing to sustainable agriculture and circular bioeconomy strategies. Full article
(This article belongs to the Special Issue Innovative Gels: Structure, Properties, and Emerging Applications)
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15 pages, 2687 KB  
Article
Interpretable Machine Learning Insights into Adhesion and Modulus of Biomedical HA–Dopamine Hydrogels
by Yuze Zhang, Yabei Xu, Yimin Shi and Daxin Liang
Gels 2026, 12(3), 206; https://doi.org/10.3390/gels12030206 - 28 Feb 2026
Viewed by 785
Abstract
Hyaluronic acid–dopamine (HA-Dopa) hydrogels have emerged as promising adhesive biomaterials for biomedical applications. However, the complex dependencies between formulation parameters and hydrogel performance pose challenges for rational material design. In this study, an interpretable machine learning framework was developed to investigate the structure–property [...] Read more.
Hyaluronic acid–dopamine (HA-Dopa) hydrogels have emerged as promising adhesive biomaterials for biomedical applications. However, the complex dependencies between formulation parameters and hydrogel performance pose challenges for rational material design. In this study, an interpretable machine learning framework was developed to investigate the structure–property relationships of HA-Dopa hydrogels. A dataset comprising 228 data points was collected from 37 peer-reviewed publications, representing heterogeneous experimental conditions across different research groups, and gradient boosting regression models were established to predict adhesion strength and elastic modulus, achieving test R2 of 0.99 and 0.94, respectively, with stable performance across cross-validation splits. SHAP analysis revealed that HA molecular weight and dopamine substitution degree are the dominant factors governing adhesion, while mechanical properties exhibit more distributed dependence on multiple formulation parameters. The identified synergistic interactions between key features provide potential guidance for targeted formulation optimization. This work demonstrates the utility of interpretable machine learning in elucidating structure–property relationships and accelerating the development of functional hydrogels for biomedical applications. Full article
(This article belongs to the Special Issue Recent Research on Medical Hydrogels (2nd Edition))
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22 pages, 8225 KB  
Article
Migration and Chondrogenesis of Cells from Minced Nasal Cartilage in Type I Collagen Hydrogel: A Workflow for One-Step Engineering of Injectable Grafts
by Alexander Gensch, Atharva Damle, Orhan Sonsöz, Diana Mock, Martin Haug, Davide Adamo, Ewelina M. Bartoszek, Gyözö Lehoczky, Ivan Martin and Andrea Barbero
Gels 2026, 12(3), 190; https://doi.org/10.3390/gels12030190 - 25 Feb 2026
Viewed by 1163
Abstract
Articular cartilage (AC) damage heals poorly and can progress to osteoarthritis. Implantation of AC fragments (Minced Cartilage Implantation, MCI) is a promising one-step repair technique but is constrained by the limited availability of healthy AC. In this study, we evaluated the feasibility of [...] Read more.
Articular cartilage (AC) damage heals poorly and can progress to osteoarthritis. Implantation of AC fragments (Minced Cartilage Implantation, MCI) is a promising one-step repair technique but is constrained by the limited availability of healthy AC. In this study, we evaluated the feasibility of MCI using nasal septal cartilage (NSC) as an alternative source of hyaline tissue with strong regenerative capacity. NSC obtained from rhinoplasties was decontaminated using a novel protocol, minced with or without Poloxamer 188 (P188), embedded in collagen I gel (0.5 mL per sample), and cultured for 42 days in platelet-rich plasma (PRP)-supplemented medium. The decontamination procedure with a combination of antibiotics was effective and did not impair cell viability. Histology of the resulting constructs confirmed robust cellular outgrowth and matrix deposition. Tissues produced from NSC and fragmented with P188 contained more cartilaginous matrix than those from NSC fragmented without P188 and those from AC fragmented with P188. NSC fragments embedded in a 1 mL hydrogel, sufficient for clinically relevant defect volumes, also demonstrated strong outgrowth and satisfactory matrix formation. Overall, the developed protocol supports the use of NSC as a viable tissue source in gel-based, injectable MCI grafts for focal cartilage repair. Full article
(This article belongs to the Special Issue Gel-Based Materials for Cartilage Regeneration)
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22 pages, 19658 KB  
Article
Mechanistic Investigation of Microdroplet Formation in High-Viscosity Shear-Thinning Hydrogel Bioinks
by Qiang Gao, Yanling Mi, Kaicheng Yu, Youyun Shang, Lihua Lu, Yongqiang Gao and Peng Zhang
Gels 2026, 12(2), 148; https://doi.org/10.3390/gels12020148 - 6 Feb 2026
Viewed by 571
Abstract
High-resolution biofabrication requires precise microscale deposition, yet drop-on-demand (DOD) inkjet bioprinting is constrained by a narrow printable viscosity window. Many biocompatible hydrogel precursors display high zero-shear viscosity and strong shear-thinning, so stable droplet ejection typically requires dilution or reformulation that can compromise the [...] Read more.
High-resolution biofabrication requires precise microscale deposition, yet drop-on-demand (DOD) inkjet bioprinting is constrained by a narrow printable viscosity window. Many biocompatible hydrogel precursors display high zero-shear viscosity and strong shear-thinning, so stable droplet ejection typically requires dilution or reformulation that can compromise the biochemical microenvironment. We present a transient shear-enabled jetting method that exploits intrinsic shear-thinning by using a high-frequency electromagnetic microvalve to deliver short, high-pressure pulses. The resulting localized shear dynamically lowers apparent viscosity in the nozzle region and promotes controlled nucleation, ligament formation, necking, and pinch-off. A coupled, rheology-informed modeling framework (axisymmetric transient CFD, valve dynamics, and electromagnetic FEM) links actuation parameters to droplet volume and stability and guides hardware optimization. Experiments with 2.5% (w/v) sodium alginate validate stable droplet generation and tunable droplet size via stroke length and driving conditions. These results define a practical process window for high-resolution droplet printing of high-viscosity shear-thinning hydrogel inks. Full article
(This article belongs to the Special Issue Biosoursed and Bioinspired Gels for Biomedical Applications (2nd Edition))
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14 pages, 2416 KB  
Article
Highly Porous Polyimide Gel for Use as a Battery Separator with Room-Temperature Ionic Liquid Electrolytes
by Rocco P. Viggiano, James Wu, Daniel A. Scheiman, Brianne DeMattia, Patricia Loyselle and Baochau N. Nguyen
Gels 2026, 12(2), 108; https://doi.org/10.3390/gels12020108 - 27 Jan 2026
Viewed by 501
Abstract
Advanced aerospace vehicle concepts demand concurrent advances in energy storage technologies that improve both specific energy and safety. Commercial lithium-ion batteries commonly employ polyolefin microporous separators and carbonate-based liquid electrolytes, which can deliver room-temperature ionic conductivities on the order of 10−3–10 [...] Read more.
Advanced aerospace vehicle concepts demand concurrent advances in energy storage technologies that improve both specific energy and safety. Commercial lithium-ion batteries commonly employ polyolefin microporous separators and carbonate-based liquid electrolytes, which can deliver room-temperature ionic conductivities on the order of 10−3–10−2 S/cm but rely on inherently flammable solvents. Room-temperature ionic liquids (RTILs) offer a nonvolatile, nonflammable alternative with a stable electrochemical window; however, many RTILs exhibit poor compatibility and wetting with polyolefin separators. Here, we evaluate highly porous, cross-linked polyimide (PI) gel separators based on 4,4′-oxydianiline (ODA) and biphenyl-3,3′,4,4′-tetracarboxylic dianhydride (BPDA), cross-linked with Desmodur N3300A, formulated with repeating unit lengths (n) of 30 and 60. These PI gel separators exhibit an open, fibrillar network with high porosity (typically >85%), high thermal stability (onset decomposition > 561 °C), and high char yield. Six imidazolium-based RTILs containing 10 wt% LiTFSI were screened, yielding nonflammable separator/electrolyte systems with room-temperature conductivities in the 10−3 S/cm range. Among the RTILs studied, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIM-TFSI) provided the best overall performance. Ionic conductivity and its retention after four months of storage at 75 °C were evaluated in the EMIM-TFSI/LiTFSI system, and the corresponding gel separator exhibited a tensile modulus of 26.66 MPa. Collectively, these results demonstrate that PI gel separators can enable carbonate-free, nonflammable RTIL electrolytes while maintaining the ionic conductivity suitable for lithium-based cells. Full article
(This article belongs to the Special Issue Gels for Energy Applications)
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37 pages, 5704 KB  
Review
β-Hairpin-Based Peptide Hydrogels: The Case of MAX1
by Mariantonietta Pizzella, Valéria Gomes, Enrico Gallo, Sérgio Veloso, Célio Fernandes, Antonella Accardo and Carlo Diaferia
Gels 2026, 12(2), 100; https://doi.org/10.3390/gels12020100 - 24 Jan 2026
Cited by 1 | Viewed by 1159
Abstract
This review explores the advancements and applications of β-hairpin peptide hydrogels, starting from the paradigmatic case of MAX1 and its highly versatile analogue MAX8. MAX1 (H-VKVKVKVKVDPPTKVKVKVKV-NH2) has been identified as the first synthetic β-hairpin peptide for the preparation of [...] Read more.
This review explores the advancements and applications of β-hairpin peptide hydrogels, starting from the paradigmatic case of MAX1 and its highly versatile analogue MAX8. MAX1 (H-VKVKVKVKVDPPTKVKVKVKV-NH2) has been identified as the first synthetic β-hairpin peptide for the preparation of stimuli-responsive peptide-based hydrogels. At low ionic strength or neutral pH, MAX1 remains unfolded and soluble. However, under physiological conditions, it folds into a β-hairpin structure, then producing a self-supporting matrix within minutes. The formed gel is shear-thinning and self-healing, making it suitable for injectable therapies. To explore MAX1 molecular space and enhance its practical clinical use, the primary sequence was engineered via chemical modification, with specific single amino acid substitution and relative net charge alteration. This approach generates MAX1 analogues, differing in gelation kinetics, mechanical response and biological performances. The β-hairpin peptide hydrogels are categorized into five different groups: MAX1, MAX1 analogues, MAX8, MAX8 analogues and non-MAX peptides sequences. Collectively, the review outcomes demonstrate the use of β-hairpin peptide matrices as tunable platforms for the development of predictable and stable biomaterials for advanced tissue engineering and drug delivery applications. Full article
(This article belongs to the Special Issue Innovations in Application of Biofunctional Hydrogels)
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17 pages, 5690 KB  
Review
Conductive Hydrogels in Biomedical Engineering: Recent Advances and a Comprehensive Review
by Chenyu Shen, Ying Wang, Peng Yuan, Jinhuan Wei, Jingyin Bao and Zhangkang Li
Gels 2026, 12(1), 69; https://doi.org/10.3390/gels12010069 - 13 Jan 2026
Cited by 9 | Viewed by 1668
Abstract
Conductive hydrogels have gained considerable interest in the biomedical field because they provide a soft, hydrated, and electrically active microenvironment that closely resembles native tissue. Their unique combination of electrical conductivity and biocompatibility enables monitoring and modulation of biological activities. With the rapid [...] Read more.
Conductive hydrogels have gained considerable interest in the biomedical field because they provide a soft, hydrated, and electrically active microenvironment that closely resembles native tissue. Their unique combination of electrical conductivity and biocompatibility enables monitoring and modulation of biological activities. With the rapid development of conductive hydrogel technologies in recent years, a comprehensive overview is needed to clarify their biological functions and the latest biomedical applications. This review first summarizes the fundamental design strategies, fabrication methods, and conductive mechanisms of conductive hydrogels. We then highlight their applications in wearable device, implanted bioelectronics, wound healing, neural regeneration and cell regulation, accompanied by discussions of the underlying biological and electroactive mechanisms. Potential challenges and future directions, including strategies to optimize fabrication methods, balance key material properties, and tailor conductive hydrogels for diverse biomedical applications, are also highlighted. Finally, we discuss the existing limitations and future perspectives of the biomedical applications of conductive hydrogels. We hope that this article may provide some useful insights to support their further development and potential biomedical applications. Full article
(This article belongs to the Special Issue Research on the Applications of Conductive Hydrogels)
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18 pages, 4997 KB  
Article
Towards Enhanced Battery Thermal Safety: A Lightweight and Mechanically Robust Aerogel with Superior Insulation
by Yin Chen, Ruinan Sheng and Mingyi Chen
Gels 2026, 12(1), 54; https://doi.org/10.3390/gels12010054 - 5 Jan 2026
Cited by 2 | Viewed by 1384
Abstract
With the continuous increase in energy density of lithium-ion batteries, thermal safety has become a critical constraint on their further development. To address the limitations of mechanical brittleness and high-temperature infrared transparency in SiO2 aerogels for thermal safety applications in lithium-ion batteries, [...] Read more.
With the continuous increase in energy density of lithium-ion batteries, thermal safety has become a critical constraint on their further development. To address the limitations of mechanical brittleness and high-temperature infrared transparency in SiO2 aerogels for thermal safety applications in lithium-ion batteries, this study developed a novel nanofiber aerogel composite by incorporating chitosan and MXene into a SiO2 aerogel matrix. This material retains the characteristics of being ultra-lightweight and highly elastic while significantly enhancing mechanical strength and high-temperature insulation performance. It exhibits a thermal conductivity of 0.034 W/m K at room temperature and 0.053 W/m K at 400 °C, alongside a compressive strength of 1.172 MPa. In battery thermal runaway propagation tests, the aerogel successfully prevented propagation in serially connected and electrically isolated systems, and delayed thermal runaway propagation by 35 s in a parallel system, demonstrating excellent thermal runaway suppression capability. This work provides an effective material solution for the practical application of high-performance thermal insulation aerogels in battery safety protection and offers inspiration for developing new insulating ceramic aerogels. Full article
(This article belongs to the Special Issue Recent Advances in Functionalized Aerogels: Preparation, Modification and Applications)
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14 pages, 5040 KB  
Article
Being a Target for Glycation by Methylglyoxal Contributes to Therapeutic Efficacy of Injectable Collagen Hydrogels Post-Myocardial Infarction
by Xixi Guo, Ramis Ileri, Marc Ruel, Emilio I. Alarcon and Erik J. Suuronen
Gels 2026, 12(1), 18; https://doi.org/10.3390/gels12010018 - 24 Dec 2025
Viewed by 1091
Abstract
Despite the advances in medical therapies for treating myocardial infarction (MI), morbidity and mortality rates remain high. Following MI, increased methylglyoxal (MG) production leads to the accumulation of advanced glycation end-products (AGEs), which contribute to adverse remodeling and to the deterioration of cardiac [...] Read more.
Despite the advances in medical therapies for treating myocardial infarction (MI), morbidity and mortality rates remain high. Following MI, increased methylglyoxal (MG) production leads to the accumulation of advanced glycation end-products (AGEs), which contribute to adverse remodeling and to the deterioration of cardiac function. We previously reported that an injectable collagen type I hydrogel improves the repair and function of mouse hearts post-MI. Notably, we observed that the injected hydrogel was a target for MG-AGE glycation, and that there were less MG-modified proteins in the myocardium. In this study, we further evaluated this protective mechanism by pre-glycating the hydrogels and assessing their therapeutic efficacy for treating MI. In vitro experiments showed that the viability of macrophages was reduced when cultured with the glycated hydrogel in the presence of MG. In vivo, female C57BL/6 mice were randomly assigned to receive intramyocardial injections of one of three treatments: phosphate-buffered saline, normal collagen hydrogel, or MG-glycated hydrogel. After 28 days, echocardiography was performed to evaluate cardiac function, and hearts were harvested for immunohistochemistry. Our results showed that the MG-glycated hydrogel had a reduced treatment effect (greater scar size, fewer wound-healing macrophages, less viable myocardium and decreased cardiac function) compared to mice that received the normal collagen hydrogel. In summary, this study demonstrates that the ability of the collagen hydrogel to act as a target for glycation and remove MG from the environment contributes to its therapeutic effect in treating the post-MI heart. Full article
(This article belongs to the Special Issue Synthesis, Characterization and Applications of Collagen-Based Gels)
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32 pages, 11529 KB  
Review
Flexible Polymer Hydrogel Materials for Next-Generation Wearable Energy Storage Technologies
by Thirukumaran Periyasamy, Shakila Parveen Asrafali and Jaewoong Lee
Gels 2025, 11(12), 999; https://doi.org/10.3390/gels11120999 - 11 Dec 2025
Viewed by 1743
Abstract
The rapid advancement of wearable technology has created an increasing demand for efficient, high-performance energy storage systems that also offer key characteristics such as flexibility, lightweight, and durability. Among the emerging materials, polymer hydrogels have garnered significant attention due to their unique combination [...] Read more.
The rapid advancement of wearable technology has created an increasing demand for efficient, high-performance energy storage systems that also offer key characteristics such as flexibility, lightweight, and durability. Among the emerging materials, polymer hydrogels have garnered significant attention due to their unique combination of viscoelasticity, low density, and tunable porous nanostructures. These materials exhibit adaptable surface and structural properties, making them promising candidates for next-generation flexible and wearable energy storage devices. This work provides an overview of recent progress and innovations in the application of polymer hydrogels for the development of flexible energy storage systems. The intrinsic three-dimensional architecture and porous morphology of these hydrogels offer a versatile platform for constructing high-performance supercapacitors, rechargeable batteries, and personal thermal management devices. Various types of polymer hydrogels and their principal fabrication methods are discussed in detail, along with the structural factors that influence their electrochemical and mechanical performance. Furthermore, recent advancements in integrating polymer hydrogel materials into wearable and flexible technologies—such as energy storage devices, thermal regulation systems, and multifunctional energy platforms—are comprehensively reviewed and analyzed. Full article
(This article belongs to the Special Issue Energy Storage and Conductive Gel Polymers)
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56 pages, 3092 KB  
Review
Hydrogels in the Immune Context: In Vivo Applications for Modulating Immune Responses in Cancer Therapy
by Mara R. Lanis, Sujin Kim and Jonathan P. Schneck
Gels 2025, 11(11), 889; https://doi.org/10.3390/gels11110889 - 4 Nov 2025
Cited by 13 | Viewed by 4018
Abstract
In response to growing clinical demands for more targeted and effective immunotherapies to treat cancer, biomaterial-based strategies have emerged as powerful tools for locally regulating immune responses. Among these, hydrogels, a class of biocompatible and tunable polymeric networks, are increasingly being leveraged for [...] Read more.
In response to growing clinical demands for more targeted and effective immunotherapies to treat cancer, biomaterial-based strategies have emerged as powerful tools for locally regulating immune responses. Among these, hydrogels, a class of biocompatible and tunable polymeric networks, are increasingly being leveraged for their high versatility and adaptability for creating tailored immune environments. By enabling controlled delivery of immune cues and direct cellular engineering, hydrogels utilized in vivo can precisely regulate both innate and adaptive immune responses while minimizing systemic toxicity. In this review, we outline essential hydrogel design features necessary for in vivo functionality including injectability, degradation kinetics, and immune-specific functionalization. Building on these principles, we explore how hydrogels have been employed to enhance T cell activation and dendritic cell maturation and guide macrophage reprogramming. Beyond cellular modulation, we further examine the use of hydrogels for cytokine and immunoregulatory agent delivery, tumor microenvironment remodeling, and the creation of tertiary-like lymphoid structures. Finally, we review recently completed and ongoing clinical trials of hydrogels in the cancer immunotherapy space. Together, these insights underscore the growing potential of in vivo hydrogel systems as immuno-interactive platforms capable of reshaping immune responses across diverse disease contexts. Full article
(This article belongs to the Special Issue Gel Biomaterials for Cancer Therapy and Biomedical Applications)
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24 pages, 4939 KB  
Article
Engineering Rare Earth-Assisted Cobalt Oxide Gels Toward Superior Energy Storage in Asymmetric Supercapacitors
by Pritam J. Morankar, Rutuja U. Amate, Aviraj M. Teli, Aditya A. Patil, Sonali A. Beknalkar and Chan-Wook Jeon
Gels 2025, 11(11), 867; https://doi.org/10.3390/gels11110867 - 29 Oct 2025
Cited by 6 | Viewed by 1402
Abstract
The rational design of transition metal oxides with tailored electronic structures and defect chemistries is critical for advancing high-performance supercapacitors. Herein, we report the engineering of cobalt oxide (Co3O4) gels through controlled sol–gel synthesis and rare earth (RE) incorporation [...] Read more.
The rational design of transition metal oxides with tailored electronic structures and defect chemistries is critical for advancing high-performance supercapacitors. Herein, we report the engineering of cobalt oxide (Co3O4) gels through controlled sol–gel synthesis and rare earth (RE) incorporation using neodymium (Nd), gadolinium (Gd), and dual neodymium/gadolinium (Nd/Gd) doping. X-ray diffraction (XRD) confirmed the preservation of the cubic spinel structure with systematic peak shifts and broadening, evidencing lattice strain, oxygen vacancy generation, and defect enrichment. Field-emission scanning electron microscopy (FE-SEM) analyses revealed distinct morphological evolution from compact nanoparticle assemblies in pristine Co3O4 to highly porous, interconnected frameworks in Nd/Gd–Co3O4 (Nd/Gd-Co). X-ray photoelectron spectroscopy (XPS) verified the stable incorporation of RE ions, accompanied by electronic interaction with the Co–O matrix and enhanced oxygen defect states. Electrochemical measurements demonstrated that the Nd/Gd–Co electrode achieved a remarkable areal capacitance of 25 F/cm2 at 8 mA/cm2, superior ionic diffusion coefficients, and the lowest equivalent series resistance (0.26 Ω) among all samples. Long-term cycling confirmed 84.35% capacitance retention with 94.46% coulombic efficiency after 12,000 cycles. Furthermore, the asymmetric pouch-type supercapacitor (APSD) constructed with Nd/Gd–Co as the positive electrode and activated carbon as the negative electrode delivered a wide operational window of 1.5 V, an areal capacitance of 140 mF/cm2, an energy density of 0.044 mWh/cm2, and 89.44% retention after 7000 cycles. These findings establish Nd/Gd-Co gels as robust and scalable electrode materials and demonstrate that RE co-doping is an effective strategy for bridging high energy density with long-term electrochemical stability in asymmetric supercapacitors. Full article
(This article belongs to the Special Issue Gel-Based Materials for Energy Storage)
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18 pages, 2376 KB  
Article
pH-Responsive Nanogels from Bioinspired Comb-like Polymers with Hydrophobic Grafts for Effective Oral Delivery
by Qinglong Liu, Dewei Ma, Haoze Cheng, Keke Yang, Bo Hou, Ziwen Heng, Yu Qian, Wei Liu and Siyuan Chen
Gels 2025, 11(10), 806; https://doi.org/10.3390/gels11100806 - 8 Oct 2025
Cited by 2 | Viewed by 1188
Abstract
Oral administration remains the most patient-friendly drug delivery route, yet its efficacy is limited by physiological barriers including gastric degradation and inefficient cellular uptake. pH-responsive nanogels have shown promise for gastrointestinal drug delivery, though their effectiveness is often constrained by poor membrane interaction. [...] Read more.
Oral administration remains the most patient-friendly drug delivery route, yet its efficacy is limited by physiological barriers including gastric degradation and inefficient cellular uptake. pH-responsive nanogels have shown promise for gastrointestinal drug delivery, though their effectiveness is often constrained by poor membrane interaction. Inspired by natural membrane-anchoring mechanisms, a series of comb-like anionic polymers were designed via grafting alkylamines of different chain lengths (C10, C14, C18) at varying densities (10–30%) onto a biodegradable poly(L-lysine isophthalamide) (PLP) backbone. These pH-responsive comb-like polymers self-assembled into nanogels for loading the hydrophobic chemotherapeutic agent camptothecin. The alkyl length and grafting density significantly influenced pH-responsive behavior, membrane disruption, and drug release profiles. The optimal formulation—the nanogel prepared with PLP grafted 30% C14—achieved a high drug-loading capacity, ideal particle size and stability, and offered superior protection in acidic conditions (only 7 ± 5% release at pH 1.2 over 24 h), while enabling rapid intestinal release (78 ± 2% at pH 7.4 within 24 h). The nanogels significantly enhanced cellular uptake, cytoplasmic delivery, and cytotoxicity against colorectal carcinoma cells. This study demonstrates the key role of hydrophobic modification in designing effective oral nanocarriers, providing a promising platform for the treatment of intestinal diseases. Full article
(This article belongs to the Special Issue Recent Advances in Hydrogel Materials)
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22 pages, 3236 KB  
Review
Nano Gel/Hydrogel-Based Components for Battery Technology: An Overview
by Md Murshed Bhuyan and Kyungjun Lee
Gels 2025, 11(9), 762; https://doi.org/10.3390/gels11090762 - 22 Sep 2025
Cited by 2 | Viewed by 2525
Abstract
Battery technology represents a cornerstone in the evolution of the energy sector, driven by the urgent need for sustainable and efficient energy storage systems. Various materials, including metals, non-metals, semiconductors, and polymeric gel conductors comprise batteries, and their size and composition can significantly [...] Read more.
Battery technology represents a cornerstone in the evolution of the energy sector, driven by the urgent need for sustainable and efficient energy storage systems. Various materials, including metals, non-metals, semiconductors, and polymeric gel conductors comprise batteries, and their size and composition can significantly affect battery performance. The essential components of a battery are electrolytes, electrodes, nanogelators, and membranes that can be built up by using nanogels. The nanogel components significantly enhance the efficiency and stability of redox-active flow batteries, which makes them cheaper and eco-friendly. Little research has been conducted on nanogel-based battery technology. This study mainly focuses on the nanogels used in the components of batteries. The review explains the functions of nanogels in different electrolytes, electrodes, nanogelators, and membranes. This review explicitly discusses the current status and literature background of nanogels and hydrogels in battery technology. For anyone interested in delving deeper into the realm of nanogel-based batteries, this review article serves as a valuable resource, offering a thorough exploration of their role in revolutionizing modern energy storage systems. Full article
(This article belongs to the Special Issue Recent Advances in Multi-Functional Hydrogels)
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67 pages, 37309 KB  
Review
Polymer Network-Based Nanogels and Microgels: Design, Classification, Synthesis, and Applications in Drug Delivery
by Sabuj Chandra Sutradhar, Nipa Banik, Gazi A. K. M. Rafiqul Bari and Jae-Ho Jeong
Gels 2025, 11(9), 761; https://doi.org/10.3390/gels11090761 - 22 Sep 2025
Cited by 5 | Viewed by 3673
Abstract
Polymer network-based nanogels (NGs) and microgels (MGs) have emerged as highly versatile platforms for advanced drug delivery, owing to their tunable architecture, biocompatibility, and responsiveness to diverse stimuli. This review presents a comprehensive and structured analysis of NG/MGs, encompassing their classification based on [...] Read more.
Polymer network-based nanogels (NGs) and microgels (MGs) have emerged as highly versatile platforms for advanced drug delivery, owing to their tunable architecture, biocompatibility, and responsiveness to diverse stimuli. This review presents a comprehensive and structured analysis of NG/MGs, encompassing their classification based on polymer origin, crosslinking mechanisms, composition, charge, stimuli-responsiveness, and structural architecture. We detail synthesis strategies—including inverse microemulsion and radiation-induced polymerization—and highlight key characterization techniques essential for evaluating physicochemical and functional properties. Emphasis is placed on the design-driven applications of NG/MGs in overcoming biological barriers and enabling targeted therapies, particularly in cancer, inflammation, diabetes, and viral infections. Multifunctional NGs integrating therapeutic and diagnostic capabilities (theranostics), as well as emerging platforms for immunotherapy and personalized medicine, are critically discussed. Finally, we address translational challenges and future directions, including scalable manufacturing, regulatory considerations, and integration with smart diagnostics. This review aims to serve as a foundational resource for researchers and clinicians developing next-generation NG/MG-based therapeutics. Full article
(This article belongs to the Special Issue Nanogels and Microgels: Fundamental Studies, Applications, and Emerging Trends)
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17 pages, 8259 KB  
Article
NMR/MRI Techniques to Characterize Alginate-Based Gel Rafts for the Treatment of Gastroesophageal Reflux Disease
by Ewelina Baran, Piotr Kulinowski, Marek Król and Przemysław Dorożyński
Gels 2025, 11(9), 749; https://doi.org/10.3390/gels11090749 - 17 Sep 2025
Cited by 1 | Viewed by 3516
Abstract
Gastroesophageal reflux disease (GERD) is associated with symptoms such as heartburn, resulting from gastric content reflux. Alginate-based raft-forming gel formulations represent a non-pharmacological strategy for GERD management by forming a floating gel barrier in the stomach. This study evaluated three commercial anti-reflux oral [...] Read more.
Gastroesophageal reflux disease (GERD) is associated with symptoms such as heartburn, resulting from gastric content reflux. Alginate-based raft-forming gel formulations represent a non-pharmacological strategy for GERD management by forming a floating gel barrier in the stomach. This study evaluated three commercial anti-reflux oral gel systems under simulated fed-state gastric conditions, using in vitro magnetic resonance relaxometry techniques. Magnetic resonance imaging (MRI) was performed in 0.01 M hydrochloric acid (HCl) to visualize gel raft formation, spatial structure, and spatial distribution of effective T2 relaxation time. Nuclear magnetic resonance (NMR) relaxometry in 0.01 M deuterium chloride (DCl) measured T1 and T2 relaxation times of the protons that were initially included in the preparation to assess its molecular mobility within the gel matrix. Two formulations formed floating, coherent gels, whereas the remaining one exhibited only polymer swelling without flotation. In one case, relaxometry data revealed a solid-like component that can be detected, indicating enhanced mechanical stability. The performance of each formulation was influenced by interactions among alginate, bicarbonates, and calcium ions, which determined gel consistency and flotation behavior. MRI and NMR relaxometry in vitro provide valuable non-invasive insights into the structural and functional behavior of alginate-based gel formulations. This approach supports the rational design of advanced gel-based therapies for GERD by linking molecular composition with in situ performance. Full article
(This article belongs to the Special Issue Polymeric Hydrogels for Biomedical Application (2nd Edition))
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58 pages, 16131 KB  
Review
Polymer Gel-Based Triboelectric Nanogenerators: Conductivity and Morphology Engineering for Advanced Sensing Applications
by Sabuj Chandra Sutradhar, Nipa Banik, Mohammad Mizanur Rahman Khan and Jae-Ho Jeong
Gels 2025, 11(9), 737; https://doi.org/10.3390/gels11090737 - 13 Sep 2025
Cited by 6 | Viewed by 2685
Abstract
Polymer gel-based triboelectric nanogenerators (TENGs) have emerged as versatile platforms for self-powered sensing due to their inherent softness, stretchability, and tunable conductivity. This review comprehensively explores the roles of polymer gels in TENG architecture, including their function as triboelectric layers, electrodes, and conductive [...] Read more.
Polymer gel-based triboelectric nanogenerators (TENGs) have emerged as versatile platforms for self-powered sensing due to their inherent softness, stretchability, and tunable conductivity. This review comprehensively explores the roles of polymer gels in TENG architecture, including their function as triboelectric layers, electrodes, and conductive matrices. We analyze four operational modes—vertical contact-separation, lateral-sliding, single-electrode, and freestanding configurations—alongside key performance metrics. Recent studies have reported output voltages of up to 545 V, short-circuit currents of 48.7 μA, and power densities exceeding 120 mW/m2, demonstrating the high efficiency of gel-based TENGs. Gel materials are classified by network structure (single-, double-, and multi-network), matrix composition (hydrogels, aerogels, and ionic gels), and dielectric medium. Strategies to enhance conductivity using ionic salts, conductive polymers, and nanomaterials are discussed in relation to triboelectric output and sensing sensitivity. Morphological features such as surface roughness, porosity, and micro/nano-patterning are examined for their impact on charge generation. Application-focused sections detail the integration of gel-based TENGs in health monitoring (e.g., sweat, glucose, respiratory, and tremor sensing), environmental sensing (e.g., humidity, fire, marine, and gas detection), and tactile interfaces (e.g., e-skin and wearable electronics). Finally, we address current challenges, including mechanical durability, dehydration, and system integration, and outline future directions involving self-healing gels, hybrid architectures, and AI-assisted sensing. This review expands the subject area by synthesizing recent advances and offering a strategic roadmap for developing intelligent, sustainable, and multifunctional TENG-based sensing technologies. Full article
(This article belongs to the Special Issue Gel-Based Materials for Intelligent Sensors and Self-Powered Nanogenerators)
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18 pages, 2955 KB  
Article
Exploring Mechanotransduction and Inflammation in Human Cartilaginous Endplate Cells in Blended Collagen–Agarose Hydrogels Under Cyclic Compression
by Katherine B. Crump, Chloé Chapallaz, Ahmad Alminnawi, Paola Bermudez-Lekerika, Liesbet Geris, Jérôme Noailly and Benjamin Gantenbein
Gels 2025, 11(9), 736; https://doi.org/10.3390/gels11090736 - 12 Sep 2025
Viewed by 1732
Abstract
Little is known about cartilaginous endplate (CEP) mechanobiology or how it changes in a catabolic microenvironment, partly due to difficulties in conducting mechanotransduction in vitro. Recent studies have found blended collagen–agarose hydrogels to offer improved mechanotransduction in chondrocytes compared to agarose alone. It [...] Read more.
Little is known about cartilaginous endplate (CEP) mechanobiology or how it changes in a catabolic microenvironment, partly due to difficulties in conducting mechanotransduction in vitro. Recent studies have found blended collagen–agarose hydrogels to offer improved mechanotransduction in chondrocytes compared to agarose alone. It was hypothesized that blended collagen–agarose hydrogels would be sufficient to improve the mechanobiological response in CEP cells relative to that in agarose alone, while maintaining the chondrocyte phenotype and ability to respond to pro-inflammatory stimulation. Thus, human CEP cells were seeded into blended 2% agarose and 2 mg/mL type I collagen hydrogels, followed by culture with dynamic compression up to 7% and stimulation with TNF. Results confirmed CEP cells retained a rounded phenotype and high cell viability during culture in blended collagen–agarose hydrogels. Additionally, TNF induced a catabolic response through downregulation of pericellular marker COL6A1 and anabolic markers ACAN and COL2A1. No significant changes were seen due to dynamic compression, suggesting addition of collagen to agarose was not sufficient to induce mechanotransduction in human CEP cells in this study. However, blended collagen–agarose hydrogels increased stiffness by 4× and gene expression of key cartilage marker SOX9 and physioosmotic mechanosensor TRPV4, offering an improvement on agarose alone. Full article
(This article belongs to the Special Issue Hydrogels for the Regeneration of Joints of the Musculoskeletal System in Orthopedics (2nd Edition))
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21 pages, 1668 KB  
Review
Hemicellulosic Biogels: A Fundamentally New Sustainable Platform Approach to Address Societal Grand Challenges
by Ali Ayoub and Lucian Lucia
Gels 2025, 11(9), 722; https://doi.org/10.3390/gels11090722 - 10 Sep 2025
Cited by 2 | Viewed by 1132
Abstract
The global issues of resource depletion and environmental pollution have led to increased interest in a circular bioeconomy focusing on converting renewable biomass into functional biomaterials. This article explores the transformative potential of hemicellulosic biogels as a sustainable platform to address critical societal [...] Read more.
The global issues of resource depletion and environmental pollution have led to increased interest in a circular bioeconomy focusing on converting renewable biomass into functional biomaterials. This article explores the transformative potential of hemicellulosic biogels as a sustainable platform to address critical societal challenges, such as water scarcity, food solutions and environmental pollution. Derived from hemicelluloses, an abundant and underutilized polysaccharide in lignocellulose biomass, these biogels offer a fundamentally new approach to developing high-performance, ecofriendly based materials. The review examines their development, characterization, and diverse applications in water treatment, food, agriculture, adhesive and coating systems. In water treatment, these gels exhibit exceptional performance, demonstrating a maximum NaCl uptake of 0.26 g/g and rapid pseudo-second-order adsorption kinetics for desalination. They also show high selectivity for heavy metal removal, with a remarkable binding capacity for lead if 2.9 mg/g at pH 5. For adhesive and coating applications, hemicellulose crosslinked with ammonium zirconium carbonate (AZC) forms water-resistant gels that significantly enhance paper properties, including gloss, smoothness, liquid resistance, and adhesive strength. Furthermore, hemicellulosics exhibit controlled biodegradation in physiological solutions while maintaining their mechanical integrity, underscoring their broad application promise. Overall, this review highlights how hemicellulose-based hydrogels can transform a low-value byproduct from biorefinery into high-performance solutions, contributing significantly to a sustainable economy. Full article
(This article belongs to the Special Issue Advanced Hydrogel for Water Treatment (2nd Edition))
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16 pages, 3927 KB  
Article
3D Printing of Polyacrylamide/Sodium Alginate/Ammonium Molybdate/Lithium Chloride Hydrogels for E-Skin and Information Encryption
by Qinglin Wang, Yinghao Zhao, Hao Zeng, Xiaohu Chen, Chunliang Chen, Jiashu Cui and Yanen Wang
Gels 2025, 11(9), 703; https://doi.org/10.3390/gels11090703 - 2 Sep 2025
Cited by 1 | Viewed by 1725
Abstract
With the rapid development of flexible electronic skin materials, the demand for ion-conductive hydrogels is constantly growing. Specifically, these ion-conductive hydrogels are required to simultaneously exhibit excellent mechanical properties, high conductivity, and multifunctionality. Moreover, this performance requirement needs to be met in complex [...] Read more.
With the rapid development of flexible electronic skin materials, the demand for ion-conductive hydrogels is constantly growing. Specifically, these ion-conductive hydrogels are required to simultaneously exhibit excellent mechanical properties, high conductivity, and multifunctionality. Moreover, this performance requirement needs to be met in complex environments. However, the rapid production of hydrogels that combine high conductivity and photochromic properties remains a major challenge. In this study, a simple one-pot method was employed to successfully prepare multifunctional photochromic hydrogels by incorporating ammonium molybdate (Mo7) and lithium chloride (LiCl) into a dual-network hydrogel composed of polyacrylamide (PAAm) and sodium alginate (SA). PAAm/SA/Mo7/LiCl (PSML) hydrogels exhibit excellent comprehensive performance, including superior conductivity (average value of 164 S/cm), rapid UV response time (<20 s), good color-changing reversibility, outstanding high stretchability (peak value of 2800%), and high transparency (>70%). The design ingeniously combines two types of synergistic effects: the synergistic effect of the dual-network structure and that of the multifunctional component functional additives (Mo7, LiCl). Specifically, the PSML hydrogel integrates photochromic properties, excellent mechanical properties, good anti-freezing properties, and 3D printability through this design. Due to these outstanding properties, the PSML hydrogel shows broad application prospects in fields such as flexible strain sensors, information storage, and encryption devices. Full article
(This article belongs to the Special Issue Gel-Based Materials for Intelligent Sensors and Self-Powered Nanogenerators)
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52 pages, 9728 KB  
Review
Hydrogel Network Architecture Design Space: Impact on Mechanical and Viscoelastic Properties
by Andres F. Roca-Arroyo, Jhonatan A. Gutierrez-Rivera, Logan D. Morton and David A. Castilla-Casadiego
Gels 2025, 11(8), 588; https://doi.org/10.3390/gels11080588 - 30 Jul 2025
Cited by 48 | Viewed by 7297
Abstract
This comprehensive review explores the expansive design space of network architectures and their significant impact on the mechanical and viscoelastic properties of hydrogel systems. By examining the intricate relationships between molecular structure, network connectivity, and resulting bulk properties, we provide critical insights into [...] Read more.
This comprehensive review explores the expansive design space of network architectures and their significant impact on the mechanical and viscoelastic properties of hydrogel systems. By examining the intricate relationships between molecular structure, network connectivity, and resulting bulk properties, we provide critical insights into rational design strategies for tailoring hydrogel mechanics for specific applications. Recent advances in sequence-defined crosslinkers, dynamic covalent chemistries, and biomimetic approaches have significantly expanded the toolbox for creating hydrogels with precisely controlled viscoelasticity, stiffness, and stress relaxation behavior—properties that are crucial for biomedical applications, particularly in tissue engineering and regenerative medicine. Full article
(This article belongs to the Special Issue State-of-the Art Gel Research in USA)
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28 pages, 6648 KB  
Review
Machine Learning in Gel-Based Additive Manufacturing: From Material Design to Process Optimization
by Zhizhou Zhang, Yaxin Wang and Weiguang Wang
Gels 2025, 11(8), 582; https://doi.org/10.3390/gels11080582 - 28 Jul 2025
Cited by 22 | Viewed by 5172
Abstract
Machine learning is reshaping gel-based additive manufacturing by enabling accelerated material design and predictive process optimization. This review provides a comprehensive overview of recent progress in applying machine learning across gel formulation development, printability prediction, and real-time process control. The integration of algorithms [...] Read more.
Machine learning is reshaping gel-based additive manufacturing by enabling accelerated material design and predictive process optimization. This review provides a comprehensive overview of recent progress in applying machine learning across gel formulation development, printability prediction, and real-time process control. The integration of algorithms such as neural networks, random forests, and support vector machines allows accurate modeling of gel properties, including rheology, elasticity, swelling, and viscoelasticity, from compositional and processing data. Advances in data-driven formulation and closed-loop robotics are moving gel printing from trial and error toward autonomous and efficient material discovery. Despite these advances, challenges remain regarding data sparsity, model robustness, and integration with commercial printing systems. The review results highlight the value of open-source datasets, standardized protocols, and robust validation practices to ensure reproducibility and reliability in both research and clinical environments. Looking ahead, combining multimodal sensing, generative design, and automated experimentation will further accelerate discoveries and enable new possibilities in tissue engineering, biomedical devices, soft robotics, and sustainable materials manufacturing. Full article
(This article belongs to the Section Gel Processing and Engineering)
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26 pages, 5763 KB  
Article
The Development and Optimization of Extrusion-Based 3D Food Printing Inks Using Composite Starch Gels Enriched with Various Proteins and Hydrocolloids
by Evgenia N. Nikolaou, Eftychios Apostolidis, Eirini K. Nikolidaki, Evangelia D. Karvela, Athena Stergiou, Thomas Kourtis and Vaios T. Karathanos
Gels 2025, 11(8), 574; https://doi.org/10.3390/gels11080574 - 23 Jul 2025
Cited by 13 | Viewed by 3197
Abstract
This study presents a comprehensive evaluation of starch-based gel formulations enriched with proteins and hydrocolloids for extrusion-based 3D food printing (3DFP). Food inks were prepared using corn or potato starch, protein concentrates (fava, whey, rice, pea and soya), and hydrocolloids (κ-carrageenan, arabic gum, [...] Read more.
This study presents a comprehensive evaluation of starch-based gel formulations enriched with proteins and hydrocolloids for extrusion-based 3D food printing (3DFP). Food inks were prepared using corn or potato starch, protein concentrates (fava, whey, rice, pea and soya), and hydrocolloids (κ-carrageenan, arabic gum, xanthan gum, and carboxy methylcellulose). Their rheological, mechanical, and textural properties were systematically analyzed to assess printability. Among all formulations, those containing κ-carrageenan consistently demonstrated superior viscoelastic behavior (G′ > 4000 Pa), optimal tan δ values (0.096–0.169), and yield stress conducive to stable extrusion. These inks also achieved high structural fidelity (93–96% accuracy) and favourable textural attributes such as increased hardness and chewiness. Computational Fluid Dynamics (CFD) simulations further validated the inks’ performances by linking pressure and velocity profiles with rheological parameters. FTIR analysis revealed that gel strengthening was primarily driven by non-covalent interactions, such as hydrogen bonding and electrostatic effects. The integration of empirical measurements and simulation provided a robust framework for evaluating and optimizing printable food gels. These findings contribute to the advancement of personalized and functional 3D-printed foods through data-driven formulation design. Full article
(This article belongs to the Special Issue Recent Advances in Food Gels (2nd Edition))
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26 pages, 8710 KB  
Article
MOFs—Combining Fully Synthetic Injectable Hydrogel Scaffolds Exhibiting Higher Skeletal Muscle Regenerative Efficiency than Matrigel
by Sobuj Shahidul Islam, Tatsuya Dode, Soma Kawashima, Myu Fukuoka, Takaaki Tsuruoka and Koji Nagahama
Gels 2025, 11(7), 514; https://doi.org/10.3390/gels11070514 - 2 Jul 2025
Cited by 3 | Viewed by 1767
Abstract
Due to its sarcoma-derived origin and the associated carcinogenic risks, as well as its lack of tissue-specific extracellular matrix biochemical cues, the use of the injectable gel scaffold Matrigel is generally restricted to research applications. Therefore, the development of new fully synthetic injectable [...] Read more.
Due to its sarcoma-derived origin and the associated carcinogenic risks, as well as its lack of tissue-specific extracellular matrix biochemical cues, the use of the injectable gel scaffold Matrigel is generally restricted to research applications. Therefore, the development of new fully synthetic injectable gel scaffolds that exhibit performance comparable to Matrigel is a high priority. In this study, we developed a novel fully synthetic injectable gel scaffold by combining a biodegradable PLGA-PEG-PLGA copolymer, clay nanoparticle LAPONITE®, and L-arginine-loaded metal–organic frameworks (NU-1000) at the nano level. An aqueous solution of the developed hybrid scaffold (PLGA-PEG-PLGA/LAPONITE®/L-Arg@NU-1000) exhibited rapid sol–gel transition at body temperature following simple injection and formed a continuous bulk-sized gel, demonstrating good injectability. Long-term sustained slow release of L-arginine from the resultant gels can be achieved because NU-1000 is a suitable reservoir for L-arginine. PLGA-PEG-PLGA/LAPONITE®/L-Arg@NU-1000 hybrid gels exhibited good compatibility with and promoted the growth of human skeletal muscle satellite cells. Importantly, in vivo experiments using skeletal muscle injury model mice demonstrated that the tissue regeneration efficiency of PLGA-PEG-PLGA/LAPONITE®/L-Arg@NU-1000 gels is higher than that of Matrigel. Specifically, we judged the higher tissue regeneration efficacy of our gels by histological analysis, including MYH3 immunofluorescent staining, H&E staining, and Masson’s trichrome staining. Taken together, these data suggest that novel hybrid hydrogels could serve as injectable hydrogel scaffolds for in vivo tissue engineering and ultimately replace Matrigel. Full article
(This article belongs to the Section Gel Applications)
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19 pages, 3763 KB  
Article
Elaboration of Conductive Hydrogels by 3D Printer for the Development of Strain Sensors
by Lucas Carravero Costa, Isabelle Pochard, Cédric C. Buron and Florian E. Jurin
Gels 2025, 11(7), 474; https://doi.org/10.3390/gels11070474 - 20 Jun 2025
Cited by 1 | Viewed by 1831
Abstract
The development of biocompatible, conductive hydrogels via direct ink writing (DIW) has gained increasing attention for strain sensor applications. In this work, a hydrogel matrix composed of polyvinyl alcohol (PVA) and κ-carrageenan (KC) was formulated and enhanced with polyvinylidene fluoride (PVDF) and silver [...] Read more.
The development of biocompatible, conductive hydrogels via direct ink writing (DIW) has gained increasing attention for strain sensor applications. In this work, a hydrogel matrix composed of polyvinyl alcohol (PVA) and κ-carrageenan (KC) was formulated and enhanced with polyvinylidene fluoride (PVDF) and silver nanoparticles (AgNPs) to impart piezoelectric properties. The ink formulation was optimized to achieve shear-thinning and thixotropic recovery behavior, ensuring printability through extrusion-based 3D printing. The resulting hydrogels exhibited high water uptake (~280–300%) and retained mechanical integrity. Rheological assessments showed that increasing PVDF content improved stiffness without compromising printability. Electrical characterization demonstrated that AgNPs were essential for generating piezoelectric signals under mechanical stress, as PVDF alone was insufficient. While AgNPs did not significantly alter the crystalline phase distribution of PVDF, they enhanced conductivity and signal responsiveness. XRD and SEM-EDX analyses confirmed the presence and uneven distribution of AgNPs within the hydrogel. The optimized ink formulation (5% PVA, 0.94% KC, 6% PVDF) enabled the successful fabrication of functional sensors, highlighting the material’s strong potential for use in wearable or biomedical strain-sensing applications. Full article
(This article belongs to the Special Issue Hydrogel-Based Flexible Electronics and Devices)
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18 pages, 664 KB  
Review
Hydrogels in Veterinary Vaccine Development: Types, Mechanisms, and Applications
by Peisen Zhao, Yuwei Yang, Lingxue Yu, Guoxin Li and Dandan Zhu
Gels 2025, 11(6), 468; https://doi.org/10.3390/gels11060468 - 18 Jun 2025
Cited by 6 | Viewed by 2679
Abstract
This review examines the potential and challenges of using hydrogel vaccine delivery systems in animal immunization. Traditional methods face issues like low immunogenicity, reliance on cold chains, and inefficient delivery, limiting their use in modern animal husbandry. Hydrogels offer a promising solution due [...] Read more.
This review examines the potential and challenges of using hydrogel vaccine delivery systems in animal immunization. Traditional methods face issues like low immunogenicity, reliance on cold chains, and inefficient delivery, limiting their use in modern animal husbandry. Hydrogels offer a promising solution due to their biocompatibility, controlled drug release, and immune regulation. This paper highlights hydrogels’ benefits, such as mimicking natural infection through sustained antigen release, boosting antigen-presenting cell activity, activating immune responses, and forming barriers at mucosal sites to prevent pathogen invasion. Additionally, innovative delivery methods like microneedle patches and nasal sprays show promise in enhancing convenience and compliance in animal vaccination. By combining interdisciplinary efforts and technological advancements, the hydrogel vaccine delivery system is anticipated to be crucial in preventing animal diseases, supporting sustainable animal husbandry, and ensuring global animal health and food safety. Full article
(This article belongs to the Special Issue Recent Advances in Multi-Functional Polymer-Based Hydrogels)
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23 pages, 8674 KB  
Article
Porous and Tough Polyacrylamide/Carboxymethyl Cellulose Gels Chemically Crosslinked via Cryo-UV Polymerization for Sustained Drug Release
by Duangkamon Viboonratanasri, Daniel Rudolf King, Tsuyoshi Okumura, Mohamad Alaa Terkawi, Yoshinori Katsuyama, Milena Lama, Tomoki Yasui and Takayuki Kurokawa
Gels 2025, 11(6), 453; https://doi.org/10.3390/gels11060453 - 13 Jun 2025
Cited by 5 | Viewed by 2889
Abstract
While carboxymethyl cellulose (CMC)—a biocompatible and water-soluble cellulose derivative—holds promise for biomedical applications, challenges remain in synthesizing CMC-based hydrogels with covalent crosslinking through free radical polymerization without requiring complex, multi-step processes. In this study, we introduce a facile one-pot strategy that combines CMC [...] Read more.
While carboxymethyl cellulose (CMC)—a biocompatible and water-soluble cellulose derivative—holds promise for biomedical applications, challenges remain in synthesizing CMC-based hydrogels with covalent crosslinking through free radical polymerization without requiring complex, multi-step processes. In this study, we introduce a facile one-pot strategy that combines CMC with acrylamide (AAm) under cryogelation and low-intensity UV irradiation to achieve covalent bonding and a high polymerization yield. The resulting polyacrylamide/carboxymethyl cellulose (PAAm/CMC) porous gels were systematically evaluated for their chemical, physical, thermal, and drug-release properties, with a focus on the effects of AAm concentration and polymerization temperature (frozen vs. room temperature). Notably, the cryogel synthesized with 2.5 M AAm (PC2.5) exhibited significantly enhanced mechanical properties—that is, an 8.4-fold increase in tensile modulus and a 26-fold increase in toughness—compared with the non-cryo gel. Moreover, PC2.5 demonstrated excellent cyclic compression stability in water and phosphate-buffered saline (PBS), with less than 10% reduction in modulus after 100 cycles. These increases in the mechanical properties of PC2.5 are attributed to the formation of macropores with high polymer density and high crosslinking density at the pore walls. PC2.5 also showed slower drug release in PBS and good cytocompatibility. This study presents a simplified and efficient route for fabricating mechanically robust, covalently crosslinked PAAm/CMC cryogels, highlighting their strong potential for biomedical applications in drug delivery systems. Full article
(This article belongs to the Section Gel Analysis and Characterization)
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28 pages, 2905 KB  
Review
Gel-Based Self-Powered Nanogenerators: Materials, Mechanisms, and Emerging Opportunities
by Aditya Narayan Singh and Kyung-Wan Nam
Gels 2025, 11(6), 451; https://doi.org/10.3390/gels11060451 - 12 Jun 2025
Cited by 6 | Viewed by 3147
Abstract
With the rapid rise in Internet of Things (IoT) and artificial intelligence (AI) technologies, there is an increasing need for portable, wearable, and self-powered flexible sensing devices. In such scenarios, self-powered nanogenerators have emerged as promising energy harvesters capable of converting ambient mechanical [...] Read more.
With the rapid rise in Internet of Things (IoT) and artificial intelligence (AI) technologies, there is an increasing need for portable, wearable, and self-powered flexible sensing devices. In such scenarios, self-powered nanogenerators have emerged as promising energy harvesters capable of converting ambient mechanical stimuli into electrical energy, enabling the development of autonomous flexible sensors and sustainable systems. This review highlights recent advances in nanogenerator technologies—particularly those based on piezoelectric and triboelectric effects—with a focus on soft, flexible, and gel-based polymer materials. Key mechanisms of energy conversion are discussed alongside strategies to enhance performance through material innovation, structural design, and device integration. Special attention is given to the role of gel-type composites, which offer unique advantages such as mechanical tunability, self-healing ability, and biocompatibility, making them highly suitable for next-generation wearable, biomedical, and environmental sensing applications. We also explore the evolving landscape of energy applications, from microscale sensors to large-area systems, and identify critical challenges and opportunities for future research. By synthesizing progress across materials, mechanisms, and application domains, this review aims to guide the rational design of high-performance, sustainable nanogenerators for the next era of energy technologies. Full article
(This article belongs to the Special Issue Gel-Based Materials for Intelligent Sensors and Self-Powered Nanogenerators)
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26 pages, 8645 KB  
Article
Effect of the Gel Drying Method on Properties of Semicrystalline Aerogels Prepared with Different Network Morphologies
by Glenn A. Spiering, Garrett F. Godshall and Robert B. Moore
Gels 2025, 11(6), 447; https://doi.org/10.3390/gels11060447 - 10 Jun 2025
Cited by 9 | Viewed by 3574
Abstract
The purpose of this study was to investigate the effect of different drying methods on the structure and properties of semicrystalline polymer aerogels. Aerogels, consisting of either globular or strut-like morphologies, were prepared from poly(ether ether ketone) (PEEK) or poly(phenylene sulfide) (PPS) and [...] Read more.
The purpose of this study was to investigate the effect of different drying methods on the structure and properties of semicrystalline polymer aerogels. Aerogels, consisting of either globular or strut-like morphologies, were prepared from poly(ether ether ketone) (PEEK) or poly(phenylene sulfide) (PPS) and dried using vacuum drying, freeze-drying, or supercritical CO2 extraction. Vacuum drying was found to result in aerogels with a higher shrinkage, smaller mesopores (with pore widths of 2–50 nm), and smaller surface areas compared to the use of supercritical extraction as the drying method. Freeze-dried aerogels tended to have properties between those of vacuum-dried aerogels and aerogels prepared with supercritical extraction. High network connectivity was found to lead to improved gel modulus, which increased the ability of aerogels to resist network deformation due to stresses induced during drying. The PEEK and PPS aerogel networks consisting of highly connected strut-like features were considerably stiffer than those composed of globular features, and thus shrank less under the forces induced by vacuum drying or freeze-drying. The aerogels prepared from PPS were found to have larger mesopores and smaller surface areas than the aerogels prepared from PEEK. The larger mesopores of the PPS aerogels induced lower capillary stresses on the aerogel network, and thus shrank less. This work demonstrates that preparing PEEK and PPS gels with strut-like features can allow aerogel processing with simpler evaporative drying methods rather than the more complex supercritical drying method. Full article
(This article belongs to the Special Issue Advances in Synthetic and Bio-Based Aerogels: Mechanical Properties, Thermal Insulation, and Environmental Remediation (2nd Edition))
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33 pages, 11543 KB  
Review
Recent Progress of Biomaterial-Based Hydrogels for Wearable and Implantable Bioelectronics
by Baojin Chen, Yan Zhu, Renjie Yu, Yunxiang Feng, Zhenpeng Han, Chang Liu, Pengcheng Zhu, Lijun Lu and Yanchao Mao
Gels 2025, 11(6), 442; https://doi.org/10.3390/gels11060442 - 9 Jun 2025
Cited by 12 | Viewed by 6519
Abstract
Bioelectronics for wearable and implantable biomedical devices has attracted significant attention due to its potential for continuous health monitoring, early disease diagnosis, and real-time therapeutic interventions. Among the various materials explored for bioelectronic applications, hydrogels derived from natural biopolymers have emerged as highly [...] Read more.
Bioelectronics for wearable and implantable biomedical devices has attracted significant attention due to its potential for continuous health monitoring, early disease diagnosis, and real-time therapeutic interventions. Among the various materials explored for bioelectronic applications, hydrogels derived from natural biopolymers have emerged as highly promising candidates, owing to their inherent biocompatibility, mechanical compliance akin to biological tissues, and tunable structural properties. This review provides a comprehensive overview of recent advancements in the design and application of protein-based hydrogels, including gelatin, collagen, silk fibroin, and gluten, as well as carbohydrate-based hydrogels such as chitosan, cellulose, alginate, and starch. Particular emphasis is placed on elucidating their intrinsic material characteristics, modification strategies to improve electrical and mechanical performance, and their applicability for bioelectronic interfaces. The review further explores their diverse applications in physiological and biochemical signal sensing, bioelectric signal recording, and electrical stimulation. Finally, current challenges and future perspectives are discussed to guide the ongoing innovation of hydrogel-based systems for next-generation bioelectronic technologies. Full article
(This article belongs to the Special Issue Stretchable Conductive Hydrogel Materials for Flexible Sensors and Bioelectronics)
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14 pages, 3406 KB  
Article
A Recyclable, Adhesive, and Self-Healing Ionogel Based on Zinc–Halogen Coordination Anion Crosslinked Poly(ionic Liquid)/Ionic Liquid Networks for High-Performance Microwave Absorption
by Lei Wang, Jie Liu, Meng Zong, Yi Liu and Jianfeng Zhu
Gels 2025, 11(6), 436; https://doi.org/10.3390/gels11060436 - 5 Jun 2025
Cited by 2 | Viewed by 2154
Abstract
In the past, powder-like microwave absorbers have made notable breakthroughs in performance enhancements, but complicated processes and undesirable properties have limited their practical application. Herein, a novel poly(ionic liquid) (PIL)-based ionic gel with excellent microwave absorption properties was prepared via a facile UV-initiated [...] Read more.
In the past, powder-like microwave absorbers have made notable breakthroughs in performance enhancements, but complicated processes and undesirable properties have limited their practical application. Herein, a novel poly(ionic liquid) (PIL)-based ionic gel with excellent microwave absorption properties was prepared via a facile UV-initiated polymerization method. By simply adjusting the mole ratio of the polymerizable ionic liquid (IL)monomer and the IL dispersion medium, the microwave absorption properties of the obtained ionic gels can be tuned. A maximum reflection loss (RLmax) of −45.7 dB and an effective absorption bandwidth (EAB) of 8.08 GHz were achieved, which was mainly ascribed to high ionic conduction loss induced by the high content of the dispersion medium. Furthermore, it displayed recyclable, adhesive, and self-healing properties, thus providing a new candidate for developing efficient microwave absorbers for practical applications. Full article
(This article belongs to the Section Gel Applications)
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23 pages, 2058 KB  
Review
Alginate Sphere-Based Soft Actuators
by Umme Salma Khanam, Hyeon Teak Jeong, Rahim Mutlu and Shazed Aziz
Gels 2025, 11(6), 432; https://doi.org/10.3390/gels11060432 - 5 Jun 2025
Cited by 1 | Viewed by 2491
Abstract
Alginate hydrogels offer distinct advantages as ionically crosslinked, biocompatible networks that can be shaped into spherical beads with high compositional flexibility. These spherical architectures provide isotropic geometry, modularity and the capacity for encapsulation, making them ideal platforms for scalable, stimuli-responsive actuation. Their ability [...] Read more.
Alginate hydrogels offer distinct advantages as ionically crosslinked, biocompatible networks that can be shaped into spherical beads with high compositional flexibility. These spherical architectures provide isotropic geometry, modularity and the capacity for encapsulation, making them ideal platforms for scalable, stimuli-responsive actuation. Their ability to respond to thermal, magnetic, electrical, optical and chemical stimuli has enabled applications in targeted delivery, artificial muscles, microrobotics and environmental interfaces. This review examines recent advances in alginate sphere-based actuators, focusing on fabrication methods such as droplet microfluidics, coaxial flow and functional surface patterning, and strategies for introducing multi-stimuli responsiveness using smart polymers, nanoparticles and biologically active components. Actuation behaviours are understood and correlated with physical mechanisms including swelling kinetics, photothermal effects and the field-induced torque, supported by analytical and multiphysics models. Their demonstrated functionalities include shape transformation, locomotion and mechano-optical feedback. The review concludes with an outlook on the existing limitations, such as the material stability, cyclic durability and integration complexity, and proposes future directions toward the development of autonomous, multifunctional soft systems. Full article
(This article belongs to the Special Issue Polysaccharide Gels for Biomedical and Environmental Applications)
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15 pages, 2578 KB  
Article
Surface Relief Gratings of Slide-Ring Hydrogels for Label-Free Biosensing
by Aitor Cubells-Gómez, María Isabel Lucío, María-José Bañuls and Ángel Maquieira
Gels 2025, 11(6), 415; https://doi.org/10.3390/gels11060415 - 30 May 2025
Viewed by 1600
Abstract
The creation of surface relief gratings using hydrogels for label-free biomolecule detection represents a significant advance in the development of versatile, cutting-edge biosensors. Central to this innovation is the formulation of materials with enhanced mechanical properties, especially for applications in soft, wearable technologies. [...] Read more.
The creation of surface relief gratings using hydrogels for label-free biomolecule detection represents a significant advance in the development of versatile, cutting-edge biosensors. Central to this innovation is the formulation of materials with enhanced mechanical properties, especially for applications in soft, wearable technologies. In this work, we have developed novel biofunctional hydrogels that incorporate slide-ring supramolecular structures into their network, enabling the production of surface relief gratings with superior mechanical characteristics for biomolecule detection without the need for labels. These hydrogels, functionalized with bovine serum albumin and goat anti-rabbit antibodies, demonstrated excellent selectivity and sensitivity toward anti-bovine serum albumin and rabbit IgGs in blood serum, evaluated using a label-free format. Remarkably, the new materials matched the analytical performance of conventional hydrogels based on static networks while offering dramatically improved toughness and elasticity, with a compressive modulus comparable to human skin. This demonstrates the potential of slide-ring hydrogels for fabricating robust, label-free biosensing platforms. Furthermore, the flexibility of this system allows for the incorporation of various recognition elements tailored to specific applications. Full article
(This article belongs to the Special Issue Recent Progress of Hydrogel Sensors and Biosensors (2nd Edition))
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18 pages, 5904 KB  
Article
Gellan Gum-Based In Situ Hydrogels for Nasal Delivery of Polymeric Micelles Loaded with Risperidone
by Bence Sipos, Mária Budai-Szűcs, Gábor Katona and Ildikó Csóka
Gels 2025, 11(6), 404; https://doi.org/10.3390/gels11060404 - 28 May 2025
Cited by 4 | Viewed by 2314
Abstract
Nasal drug delivery faces numerous challenges related to the ineffectiveness of most nasal formulations without a mucoadhesive nature, prolonging residence time on the nasal mucosa. Another challenge is the low administrable dosage strength, which can be solved via nano-encapsulation techniques, including the utilization [...] Read more.
Nasal drug delivery faces numerous challenges related to the ineffectiveness of most nasal formulations without a mucoadhesive nature, prolonging residence time on the nasal mucosa. Another challenge is the low administrable dosage strength, which can be solved via nano-encapsulation techniques, including the utilization of polymeric micelles. In this study, gellan gum–cellulose derivative complex in situ gelling matrices were formulated to test their effect on the colloidal characteristics of polymeric micelles, their respective rheological behavior, and nasal applicability. It has been proven that these complex matrices can form gels upon contact with nasal fluid without disrupting the micellar structure. Changes in the drug release and permeation profile have been shown in a concentration-dependent manner to hinder the burst-like drug release profile of polymeric micelles. Formulations show concentration- and composition-dependent mucoadhesive features under nasal conditions. Most of the hydrogels possess a soft gel characteristic, making them suitable for nasal administration. In conclusion, this descriptive study provides useful insights for conscious, nasal dosage form design. Full article
(This article belongs to the Special Issue Novel Polymer-Based Smart Hydrogels: Design, Properties and Applications)
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16 pages, 3996 KB  
Article
Exploring the Combination of Microgels and Nanostructured Fluids for the Cleaning of Works of Art
by Jacopo Vialetto, David Chelazzi, Marco Laurati and Giovanna Poggi
Gels 2025, 11(6), 382; https://doi.org/10.3390/gels11060382 - 23 May 2025
Cited by 3 | Viewed by 1512
Abstract
Cultural Heritage is a vital socioeconomic driver that must contend with works of art continuously exposed to degradation processes, which are further exacerbated by climate change. Aged coatings, varnishes, and soil can compromise the appearance of artworks, preventing their preservation and valorization. In [...] Read more.
Cultural Heritage is a vital socioeconomic driver that must contend with works of art continuously exposed to degradation processes, which are further exacerbated by climate change. Aged coatings, varnishes, and soil can compromise the appearance of artworks, preventing their preservation and valorization. In response, soft matter and colloidal systems, such as nanostructured cleaning fluids (NCFs), have proved to be valuable solutions for safely and effectively cleaning works of art. Here, a novel cleaning system is proposed, for the first time employing microgels of poly(N-isopropylacrylamide) (PNIPAM) with surface chains of oligoethylene glycol methyl ether methacrylate (OEGMA) to favor shear deformation by lubrication. These microgels are loaded with NCFs featuring “green” solvents and different kinds of bio-derived or petroleum-based surfactants (non-ionic, zwitterionic). Rheological characterization of the combined systems highlighted a sharp transition from solid to liquid-like state in the 21–24 °C range when the zwitterionic surfactant dodecyldimethylamine oxide was used; the system displays a solid-like behavior at rest but flows easily at intermediate strains. At slightly higher temperature (>24 °C), an inversion of the G′, G″ values was observed, leading to a system that behaves as a liquid. Such control of rheological behavior is significant for feasible and complete removal of soiled polymer coatings from textured ceramic surfaces, which are difficult to clean with conventional gels, without leaving residues. These results position the PNIPAM-OEGMA microgels as promising cleaning materials for the conservation of Cultural Heritage, with possible applications also in fields where gelled systems are of interest (pharmaceutics, cosmetics, detergency, etc.). Full article
(This article belongs to the Special Issue Gel Materials for Heritage Conservation)
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28 pages, 4902 KB  
Review
Advancements in the Field of Protein-Based Hydrogels: Main Types, Characteristics, and Their Applications
by Gábor Katona, Bence Sipos and Ildikó Csóka
Gels 2025, 11(5), 306; https://doi.org/10.3390/gels11050306 - 22 Apr 2025
Cited by 17 | Viewed by 4076
Abstract
Regenerative medicine is a challenging field in current research and development, whilst translating the findings of novel tissue regenerative agents into clinical application. Protein-based hydrogels are derived from various sources, with animal-derived products being primarily utilized to deliver cells and promote cell genesis [...] Read more.
Regenerative medicine is a challenging field in current research and development, whilst translating the findings of novel tissue regenerative agents into clinical application. Protein-based hydrogels are derived from various sources, with animal-derived products being primarily utilized to deliver cells and promote cell genesis and proliferation, thereby aiding in numerous indications, including bone tissue regeneration, cartilage regeneration, spinal cord injury, and wound healing. As biocompatible and biodegradable systems, they are tolerated by the human body, allowing them to exert their beneficial effects in many indications. In this review article, multiple types of animal-derived proteins (e.g., collagen, gelatin, serum albumin, fibrin) were described, and a selection of the recent literature was collected to support the claims behind these innovative systems. During the literature review, special indications were found when applying these hydrogels, including the therapeutic option to treat post-myocardial infarct sites, glaucoma, and others. Maintaining their structure and mechanical integrity is still challenging. It is usually solved by adding (semi)synthetic polymers or small molecules to strengthen or loosen the mechanical stress in the hydrogel’s structure. All in all, this review points out the potential application of value-added delivery systems in regenerative medicine. Full article
(This article belongs to the Special Issue Advances in Protein Gels and Their Applications)
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30 pages, 1375 KB  
Review
Post-Stroke Recovery: A Review of Hydrogel-Based Phytochemical Delivery Systems
by Irina Musa, Alexandra Daniela Rotaru-Zavaleanu, Veronica Sfredel, Madalina Aldea, Andrei Gresita and Daniela Gabriela Glavan
Gels 2025, 11(4), 260; https://doi.org/10.3390/gels11040260 - 1 Apr 2025
Cited by 10 | Viewed by 5686
Abstract
Stroke remains a leading cause of disability worldwide, underscoring the urgent need for novel and innovative therapeutic strategies to enhance neuroprotection, support regeneration, and improve functional recovery. Previous research has shown that phytochemicals such as curcumin, tannic acid, gallic acid, ginsenosides, resveratrol, and [...] Read more.
Stroke remains a leading cause of disability worldwide, underscoring the urgent need for novel and innovative therapeutic strategies to enhance neuroprotection, support regeneration, and improve functional recovery. Previous research has shown that phytochemicals such as curcumin, tannic acid, gallic acid, ginsenosides, resveratrol, and isorhamnetin display extensive neuroprotective properties, including antioxidant, anti-inflammatory, and anti-apoptotic effects. These natural compounds could also promote neurogenesis, angiogenesis, and the preservation of the blood–brain barrier. Despite their promising bioactivities, clinical application is often limited by poor solubility, bioavailability, and suboptimal pharmacokinetics. Hydrogels offer a promising solution by encapsulating and controlling the gradual release of these phytochemicals directly at the site of injury. Recent advancements in hydrogel formulations, constructed from biopolymers and functionalized using nanotechnological approaches, could significantly improve the solubility, stability, and targeted delivery of phytochemicals. Controlled release profiles from pH-sensitive and environment-responsive hydrogels could ensure that the compounds’ therapeutic effects are optimally timed with individual and critical stages of post-stroke repair. Moreover, hydrogel scaffolds with tailored material properties and biocompatibility can create a favorable microenvironment, reducing secondary inflammation, enhancing tissue regeneration, and potentially improving functional and cognitive outcomes following stroke. This review explores the potential of integrating phytochemicals within hydrogel-based delivery systems specifically designed for post-stroke recovery. The design and synthesis of biocompatible, biodegradable hydrogels functionalized especially with phytochemicals and their applications are also discussed. Lastly, we emphasize the need for additional robust and translatable preclinical studies. Full article
(This article belongs to the Special Issue Recent Advances in Gels Engineering for Drug Delivery (2nd Edition))
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31 pages, 10917 KB  
Article
Rheological Insight into the 3D Printability of Carboxymethyl Cellulose-Based Hydrogels
by Itziar Insua, Oliver Etzold, Itxaso Calafel, Robert Aguirresarobe, Marcelo Calderón and Mercedes Fernández
Gels 2025, 11(4), 259; https://doi.org/10.3390/gels11040259 - 1 Apr 2025
Cited by 13 | Viewed by 4922
Abstract
Direct Ink Writing (DIW) is an advanced additive manufacturing 3D-printing technique with significant potential for producing hydrogels in biomedical and engineering applications. This study presents a comprehensive rheological analysis of the yielding and recovery properties critical for ensuring the printability of carboxymethyl cellulose [...] Read more.
Direct Ink Writing (DIW) is an advanced additive manufacturing 3D-printing technique with significant potential for producing hydrogels in biomedical and engineering applications. This study presents a comprehensive rheological analysis of the yielding and recovery properties critical for ensuring the printability of carboxymethyl cellulose (CMC)-based hydrogels incorporating atenolol, an antihypertensive agent, as the active ingredient. The viscoelastic properties under shear conditions were examined using Large Amplitude Oscillatory Shear (LAOS) testing. To obtain both qualitative and quantitative insight into hydrogel dynamics, Lissajous-Bowditch plots and Fourier Transform (FT) coefficients were analyzed. The evaluation of stress signal anharmonicity and the decomposition of stress into its elastic and viscous components allowed for distinguishing structural evolution under flow among the tested hydrogels. Additionally, the analysis of the Sequence of Physical Processes (SPP) during each deformation cycle provided deeper insight into oscillatory yielding behavior, emphasizing the role of elastic strains in determining printability. Overall, the study offers valuable understanding of the nonlinear viscoelastic behavior of CMC-based hydrogels, providing a framework for optimizing hydrogel formulations in DIW applications. Full article
(This article belongs to the Special Issue Thixotropic Gels: Mechanisms, Functions and Applications)
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21 pages, 7897 KB  
Article
Urea Delays High-Temperature Crosslinking of Polyacrylamide for In Situ Preparation of an Organic/Inorganic Composite Gel
by Li Liang, Junlong Li, Dongxiang Li, Jie Xu, Bin Zheng and Jikuan Zhao
Gels 2025, 11(4), 256; https://doi.org/10.3390/gels11040256 - 31 Mar 2025
Cited by 4 | Viewed by 2411
Abstract
To address the rapid crosslinking reaction and short stability duration of polyacrylamide gel under high salinity and temperature conditions, this paper proposes utilizing urea to delay the nucleophilic substitution crosslinking reaction among polyacrylamide, hydroquinone, and formaldehyde. Additionally, urea regulates the precipitation of calcium [...] Read more.
To address the rapid crosslinking reaction and short stability duration of polyacrylamide gel under high salinity and temperature conditions, this paper proposes utilizing urea to delay the nucleophilic substitution crosslinking reaction among polyacrylamide, hydroquinone, and formaldehyde. Additionally, urea regulates the precipitation of calcium and magnesium ions, enabling the in situ preparation of an organic/inorganic composite gel consisting of crosslinked polyacrylamide and carbonate particles. With calcium and magnesium ion concentrations at 6817 mg/L and total salinity at 15 × 104 mg/L, the gelation time can be controlled to range from 6.6 to 14.1 days at 95 °C and from 2.9 to 6.5 days at 120 °C. The resulting composite gel can remain stable for up to 155 days at 95 °C and 135 days at 120 °C. The delayed gelation facilitates longer-distance diffusion of the gelling agent into the formation, while the enhancements in gel strength and stability provide a solid foundation for improving the effectiveness of profile control and water shut-off in oilfields. The urea-controlling method is novel and effective in extending the high-temperature cross-linking reaction time of polyacrylamide. By converting calcium and magnesium ions into inorganic particles, it enables the in situ preparation of organic/inorganic composite gels, enhancing their strength and stability. Full article
(This article belongs to the Special Issue Advanced Gels for Oil Recovery (2nd Edition))
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54 pages, 19999 KB  
Review
Hydrogel-Based Continuum Soft Robots
by Honghong Wang, Jingli Du and Yi Mao
Gels 2025, 11(4), 254; https://doi.org/10.3390/gels11040254 - 27 Mar 2025
Cited by 24 | Viewed by 9432
Abstract
This paper comprehensively reviews the latest advances in hydrogel-based continuum soft robots. Hydrogels exhibit exceptional flexibility and adaptability compared to traditional robots reliant on rigid structures, making them ideal as biomimetic robotic skins and platforms for constructing highly accurate, real-time responsive sensory interfaces. [...] Read more.
This paper comprehensively reviews the latest advances in hydrogel-based continuum soft robots. Hydrogels exhibit exceptional flexibility and adaptability compared to traditional robots reliant on rigid structures, making them ideal as biomimetic robotic skins and platforms for constructing highly accurate, real-time responsive sensory interfaces. The article systematically summarizes recent research developments across several key dimensions, including application domains, fabrication methods, actuator technologies, and sensing mechanisms. From an application perspective, developments span healthcare, manufacturing, and agriculture. Regarding fabrication techniques, the paper extensively explores crosslinking methods, additive manufacturing, microfluidics, and other related processes. Additionally, the article categorizes and thoroughly discusses various hydrogel-based actuators responsive to solute/solvent variations, pH, chemical reactions, temperature, light, magnetic fields, electric fields, hydraulic/electro-osmotic stimuli, and humidity. It also details the strategies for designing and implementing diverse sensors, including strain, pressure, humidity, conductive, magnetic, thermal, gas, optical, and multimodal sensors. Finally, the paper offers an in-depth discussion of the prospective applications of hydrogel-based continuum soft robots, particularly emphasizing their potential in medical and industrial fields. Concluding remarks include a forward-looking outlook highlighting future challenges and promising research directions. Full article
(This article belongs to the Special Issue Next-Generation Hydrogels: Bridging Biology and Engineering for Medical Breakthroughs)
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21 pages, 4111 KB  
Review
Magnetic Ionogel and Its Applications
by Sayan Ganguly and Shlomo Margel
Gels 2025, 11(4), 219; https://doi.org/10.3390/gels11040219 - 21 Mar 2025
Cited by 7 | Viewed by 3617
Abstract
Magnetic ionogels, a category of hybrid materials consisting of magnetic nanoparticles and ionic liquids, have garnered significant interest owing to their remarkable attributes, including tunability, flexibility, and reactivity to external magnetic fields. These materials provide a distinctive amalgamation of the benefits of both [...] Read more.
Magnetic ionogels, a category of hybrid materials consisting of magnetic nanoparticles and ionic liquids, have garnered significant interest owing to their remarkable attributes, including tunability, flexibility, and reactivity to external magnetic fields. These materials provide a distinctive amalgamation of the benefits of both magnetic nanoparticles and ionogels, resulting in improved efficacy across many applications. Magnetic ionogels may be readily controlled using magnetic fields, rendering them suitable for drug administration, biosensing, soft robotics, and actuators. The capacity to incorporate these materials into dynamic systems presents novel opportunities for the development of responsive, intelligent materials capable of real-time environmental adaptation. Nonetheless, despite the promising potential of magnetic ionogels, problems persist, including the optimization of the magnetic particle dispersion, the enhancement of the ionogel mechanical strength, and the improvement of the long-term stability. This review presents a comprehensive examination of the syntheses, characteristics, and uses of magnetic ionogels, emphasizing significant breakthroughs and persistent problems within the domain. We examine recent advancements and prospective research trajectories aimed at enhancing the design and efficacy of magnetic ionogels for practical applications across diverse fields, including biomedical uses, sensors, and next-generation actuators. This review seeks to elucidate the present status of magnetic ionogels and their prospective influence on materials science and engineering. Full article
(This article belongs to the Special Issue Biopolymer Gel-Assisted Synthesis of Particles for Biomedical Applications (2nd Edition))
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44 pages, 11931 KB  
Review
Eco-Friendly Conductive Hydrogels: Towards Green Wearable Electronics
by José María Calderón Moreno, Mariana Chelu and Monica Popa
Gels 2025, 11(4), 220; https://doi.org/10.3390/gels11040220 - 21 Mar 2025
Cited by 20 | Viewed by 6861
Abstract
The rapid advancement of wearable electronics has catalyzed the development of flexible, lightweight, and highly conductive materials. Among these, conductive hydrogels have emerged as promising candidates due to their tissue-like properties, which can minimize the mechanical mismatch between flexible devices and biological tissues [...] Read more.
The rapid advancement of wearable electronics has catalyzed the development of flexible, lightweight, and highly conductive materials. Among these, conductive hydrogels have emerged as promising candidates due to their tissue-like properties, which can minimize the mechanical mismatch between flexible devices and biological tissues and excellent electrical conductivity, stretchability and biocompatibility. However, the environmental impact of synthetic components and production processes in conventional conductive hydrogels poses significant challenges to their sustainable application. This review explores recent advances in eco-friendly conductive hydrogels used in healthcare, focusing on their design, fabrication, and applications in green wearable electronics. Emphasis is placed on the use of natural polymers, bio-based crosslinkers, and green synthesis methods to improve sustainability while maintaining high performance. We discuss the incorporation of conductive polymers and carbon-based nanomaterials into environmentally benign matrices. Additionally, the article highlights strategies for improving the biodegradability, recyclability, and energy efficiency of these materials. By addressing current limitations and future opportunities, this review aims to provide a comprehensive understanding of environmentally friendly conductive hydrogels as a basis for the next generation of sustainable wearable technologies. Full article
(This article belongs to the Special Issue Application of Smart Gel Material in Flexible and Wearable Electronic (2nd Edition))
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17 pages, 3765 KB  
Article
A Multifunctional γ-Polyglutamic Acid Hydrogel for Combined Tumor Photothermal and Chemotherapy
by Xiaoqing Jia and Shige Wang
Gels 2025, 11(3), 217; https://doi.org/10.3390/gels11030217 - 20 Mar 2025
Cited by 27 | Viewed by 2849
Abstract
Efficient and precise cancer therapy remains a challenge due to limitations in current treatment modalities. In this study, we developed a multifunctional hydrogel system that integrates photothermal therapy (PTT) and chemotherapy to achieve combined tumor treatment. The hydrogel, composed of γ-polyglutamic acid (γ-PGA), [...] Read more.
Efficient and precise cancer therapy remains a challenge due to limitations in current treatment modalities. In this study, we developed a multifunctional hydrogel system that integrates photothermal therapy (PTT) and chemotherapy to achieve combined tumor treatment. The hydrogel, composed of γ-polyglutamic acid (γ-PGA), fifth-generation polyamide-amine dendrimers (G5), and polydopamine (PDA) nanoparticles, exhibits high photothermal conversion efficiency and temperature-responsive drug release properties. The hydrogel exhibited a high photothermal conversion efficiency of 45.6% under 808 nm near-infrared (NIR) irradiation. Drug release studies demonstrated a cumulative hydrophilic anticancer drug doxorubicin DOX release of 79.27% within 72 h under mild hyperthermia conditions (50 °C). In vivo experiments revealed a significant tumor inhibition rate of 82.3% with minimal systemic toxicity. Comprehensive in vitro and in vivo evaluations reveal that the hydrogel demonstrates excellent biocompatibility, photothermal stability, and biodegradability. Unlike conventional hydrogel systems, our γ-PGA-based hydrogel uniquely integrates a biocompatible and biodegradable polymer with polydopamine (PDA) nanoparticles, providing a smart and responsive platform for precise cancer therapy. This multifunctional hydrogel system represents a promising platform that combines PTT precision and chemotherapy efficacy, providing a robust strategy for advanced and safer cancer treatment. Full article
(This article belongs to the Special Issue Hydrogels, Microgels, and Nanogels: From Fundamentals to Applications (2nd Edition))
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12 pages, 5422 KB  
Article
Revealing the Impact of Gel Electrolytes on the Performance of Organic Electrochemical Transistors
by Mancheng Li, Xiaoci Liang, Chuan Liu and Songjia Han
Gels 2025, 11(3), 202; https://doi.org/10.3390/gels11030202 - 14 Mar 2025
Cited by 6 | Viewed by 3471
Abstract
Gel electrolyte-gated organic electrochemical transistors (OECTs) are promising bioelectronic devices known for their high transconductance, low operating voltage, and integration with biological systems. Despite extensive research on the performance of OECTs, a precise model defining the dependence of OECT performance on gel electrolytes [...] Read more.
Gel electrolyte-gated organic electrochemical transistors (OECTs) are promising bioelectronic devices known for their high transconductance, low operating voltage, and integration with biological systems. Despite extensive research on the performance of OECTs, a precise model defining the dependence of OECT performance on gel electrolytes is still lacking. In this work, we refine the device model to comprehensively account for the electrical double layer (EDL)’s capacitance of the gel electrolyte. Both experimental data and theoretical calculations indicate that the maximum transconductance of the OECT is contingent upon ion concentration, drain voltage, and scan rate, highlighting a strong correlation between the transconductance and the hydrogel electrolyte. Overall, this model serves as a theoretical tool for improving the performance of OECTs, enabling the further development of bioelectronic devices. Full article
(This article belongs to the Special Issue Research on the Applications of Conductive Hydrogels)
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29 pages, 2414 KB  
Review
Current Status of Bioprinting Using Polymer Hydrogels for the Production of Vascular Grafts
by Jana Matějková, Denisa Kaňoková and Roman Matějka
Gels 2025, 11(1), 4; https://doi.org/10.3390/gels11010004 - 26 Dec 2024
Cited by 4 | Viewed by 4173
Abstract
Cardiovascular disease is one of the leading causes of death and serious illness in Europe and worldwide. Conventional treatment—replacing the damaged blood vessel with an autologous graft—is not always affordable for the patient, so alternative approaches are being sought. One such approach is [...] Read more.
Cardiovascular disease is one of the leading causes of death and serious illness in Europe and worldwide. Conventional treatment—replacing the damaged blood vessel with an autologous graft—is not always affordable for the patient, so alternative approaches are being sought. One such approach is patient-specific tissue bioprinting, which allows for precise distribution of cells, material, and biochemical signals. With further developmental support, a functional replacement tissue or vessel can be created. This review provides an overview of the current state of bioprinting for vascular graft manufacturing and summarizes the hydrogels used as bioinks, the material of carriers, and the current methods of fabrication used, especially for vessels smaller than 6 mm, which are the most challenging for cardiovascular replacements. The fabrication methods are divided into several sections—self-supporting grafts based on simple 3D bioprinting and bioprinting of bioinks on scaffolds made of decellularized or nanofibrous material. Full article
(This article belongs to the Special Issue Application of Hydrogels in 3D Bioprinting for Tissue Engineering)
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17 pages, 5375 KB  
Article
Tunable Alginate-Polyvinyl Alcohol Bioinks for 3D Printing in Cartilage Tissue Engineering
by Alexandra Hunter Aitchison, Nicholas B. Allen, Kishen Mitra, Bijan Abar, Conor N. O’Neill, Kian Bagheri, Albert T. Anastasio and Samuel B. Adams
Gels 2024, 10(12), 829; https://doi.org/10.3390/gels10120829 - 14 Dec 2024
Cited by 10 | Viewed by 2723
Abstract
This study investigates 3D extrusion bioinks for cartilage tissue engineering by characterizing the physical properties of 3D-printed scaffolds containing varying alginate and polyvinyl alcohol (PVA) concentrations. We systematically investigated the effects of increasing PVA and alginate concentrations on swelling, degradation, and the elastic [...] Read more.
This study investigates 3D extrusion bioinks for cartilage tissue engineering by characterizing the physical properties of 3D-printed scaffolds containing varying alginate and polyvinyl alcohol (PVA) concentrations. We systematically investigated the effects of increasing PVA and alginate concentrations on swelling, degradation, and the elastic modulus of printed hydrogels. Swelling decreased significantly with increased PVA concentrations, while degradation rates rose with higher PVA concentrations, underscoring the role of PVA in modulating hydrogel matrix stability. The highest elastic modulus value was achieved with a composite of 5% PVA and 20% alginate, reaching 0.22 MPa, which approaches that of native cartilage. These findings demonstrate that adjusting PVA and alginate concentrations enables the development of bioinks with tailored physical and mechanical properties, supporting their potential use in cartilage tissue engineering and other biomedical applications. Full article
(This article belongs to the Special Issue Hydrogel for Tissue Regeneration (2nd Edition))
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16 pages, 4724 KB  
Article
Various Hydrogel Types as a Potential In Vitro Angiogenesis Model
by Chloé Radermacher, Annika Rohde, Vytautas Kucikas, Eva Miriam Buhl, Svenja Wein, Danny Jonigk, Willi Jahnen-Dechent and Sabine Neuss
Gels 2024, 10(12), 820; https://doi.org/10.3390/gels10120820 - 12 Dec 2024
Cited by 8 | Viewed by 3569
Abstract
Angiogenesis, the formation of new blood vessels, is a fundamental process in both physiological repair mechanisms and pathological conditions, including cancer and chronic inflammation. Hydrogels are commonly used as in vitro models to mimic the extracellular matrix (ECM) and support endothelial cell behavior [...] Read more.
Angiogenesis, the formation of new blood vessels, is a fundamental process in both physiological repair mechanisms and pathological conditions, including cancer and chronic inflammation. Hydrogels are commonly used as in vitro models to mimic the extracellular matrix (ECM) and support endothelial cell behavior during angiogenesis. Mesenchymal stem cells further augment cell and tissue growth and are therefore widely used in regenerative medicine. Here we examined the combination of distinct hydrogel types—fibrin, collagen, and human platelet lysate (HPL)—on the formation of capillaries in a co-culture system containing human umbilical vein endothelial cells (HUVECs) and bone marrow-derived mesenchymal stem cells (BM-MSCs). The mechanical properties and structural changes of the hydrogels were characterized through scanning electron microscopy (SEM) and nanoindentation over 10 days. Fibrin and HPL gels sustained complex network formations, with HPL gels promoting even vascular tube formation of up to 10-fold capillary caliber. Collagen gels supported negligible angiogenesis. Our results suggest that HPL gels in combination with MSC-EC co-culture may be employed to obtain robust vascularization in tissue engineering. This study provides a comparative analysis of fibrin, collagen, and HPL hydrogels, focusing on their ability to support angiogenesis under identical conditions. Our findings demonstrate the superior performance of HPL gels in promoting robust vascular structures, highlighting their potential as a versatile tool for in vitro angiogenesis modeling. Full article
(This article belongs to the Special Issue Smart Polymer Hydrogels: Synthesis, Properties and Applications (2nd Edition))
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17 pages, 1606 KB  
Article
Swelling Behavior of Anionic Hydrogels: Experiments and Modeling
by Raffaella De Piano, Diego Caccavo, Anna Angela Barba and Gaetano Lamberti
Gels 2024, 10(12), 813; https://doi.org/10.3390/gels10120813 - 10 Dec 2024
Cited by 36 | Viewed by 6462
Abstract
Polyelectrolyte hydrogels are smart materials whose swelling behavior is governed by ionizable groups on their polymeric chains, making them sensitive to pH and ionic strength. This study combined experiments and modeling to characterize anionic hydrogels. Mechanical tests and gravimetric analyses were performed to [...] Read more.
Polyelectrolyte hydrogels are smart materials whose swelling behavior is governed by ionizable groups on their polymeric chains, making them sensitive to pH and ionic strength. This study combined experiments and modeling to characterize anionic hydrogels. Mechanical tests and gravimetric analyses were performed to track hydrogel mass over time and at a steady state under varying pH and salt concentrations. The swelling ratio exhibited a bell-shaped curve with pH, reaching 120 in pure water, and decreased with increasing salt concentrations. Transient regimes showed slower swelling (~40 h) under pH stimulation compared to faster deswelling (~20 h) induced by salt. A fully coupled model integrating mass transport and solid mechanics was developed, with solvent diffusivity as the sole adjustable parameter in transient simulations. In conclusion, this study combined experiments and modeling to uncover complex mechanisms in PE behavior under two external stimuli, providing insights essential for designing advanced hydrogels. Full article
(This article belongs to the Special Issue Mathematical Modeling in Gel Design and Applications)
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17 pages, 5910 KB  
Article
Silicon-Enhanced PVA Hydrogels in Flexible Sensors: Mechanism, Applications, and Recycling
by Xiaolei Guo, Hao Zhang, Manman Wu, Zhan Tian, Yanru Chen, Rui Bao, Jinghao Hao, Xiao Cheng and Chuanjian Zhou
Gels 2024, 10(12), 788; https://doi.org/10.3390/gels10120788 - 2 Dec 2024
Cited by 8 | Viewed by 2665
Abstract
Hydrogels, known for their outstanding water absorption, flexibility, and biocompatibility, have been widely utilized in various fields. Nevertheless, their application is still limited by their relatively low mechanical performance. This study has successfully developed a dual-network hydrogel with exceptional mechanical properties by embedding [...] Read more.
Hydrogels, known for their outstanding water absorption, flexibility, and biocompatibility, have been widely utilized in various fields. Nevertheless, their application is still limited by their relatively low mechanical performance. This study has successfully developed a dual-network hydrogel with exceptional mechanical properties by embedding amino-functionalized polysiloxane (APSi) networks into a polyvinyl alcohol (PVA) matrix. This hydrogel effectively dissipates energy through dense sacrificial bonds between the networks, allowing for precise control over its tensile strength (ranging from 0.07 to 1.46 MPa) and toughness (from 0.06 to 2.17 MJ/m3) by adjusting the degree of crosslinking in the polysiloxane network. Additionally, the hydrogel exhibits excellent conductivity (10.97 S/cm) and strain sensitivity (GF = 1.43), indicating its potential for use in wearable strain sensors. Moreover, at the end of its life (EOL), the sensor waste can be repurposed as an adsorbent material for metal ions in water treatment, achieving the recycling of hydrogel materials and maximizing resource utilization. Full article
(This article belongs to the Special Issue Flexible Gel Sensor: From Design to Application)
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14 pages, 3392 KB  
Article
Double Encapsulation of Resveratrol and Doxorubicin in Composite Nanogel—An Opportunity to Reduce Cardio- and Neurotoxicity of Doxorubicin
by Lyubomira Radeva, Yordan Yordanov, Ivanka Spassova, Daniela Kovacheva, Virginia Tzankova and Krassimira Yoncheva
Gels 2024, 10(11), 699; https://doi.org/10.3390/gels10110699 - 28 Oct 2024
Cited by 8 | Viewed by 3155
Abstract
The simultaneous encapsulation of drugs into nanosized delivery systems could be beneficial for cancer therapies since it could alleviate adverse reactions as well as provide synergistic effects. However, the encapsulation of hydrophobic drugs into hydrophilic nanoparticles, such as nanogels, could be challenging. Therefore, [...] Read more.
The simultaneous encapsulation of drugs into nanosized delivery systems could be beneficial for cancer therapies since it could alleviate adverse reactions as well as provide synergistic effects. However, the encapsulation of hydrophobic drugs into hydrophilic nanoparticles, such as nanogels, could be challenging. Therefore, innovative technological approaches are needed. In this research, a composite nanogel system was prepared from chitosan, albumin, and hydroxypropyl-β-cyclodextrin for co-delivery of the hydrophilic anticancer drug doxorubicin and hydrophobic antioxidant resveratrol. The nanoparticles were characterized using dynamic light scattering and found to have a hydrodynamic diameter of approx. 31 nm, narrow size distribution (PDI = 0.188), positive ƺ-potential (+51.23 mV), and pH-dependent release of the loaded drugs. FTIR and X-ray analyses proved the successful development of the composite nanogel. Moreover, the double-loaded system showed that the loading of resveratrol exerted protection against doxorubicin-induced toxicity in cardioblast H9c2 and neuroblast SH-SY5Y cells. The simultaneous loading did not influence the cytostatic effect of the antitumor agent in lymphoma L5178Y and L5178MDR cell lines. Full article
(This article belongs to the Special Issue Hydrogels, Oleogels and Bigels Used for Drug Delivery)
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