Gels doi: 10.3390/gels10030207
Authors: Zaid Dahma Carlos Torrado-Salmerón Covadonga Álvarez-Álvarez Víctor Guarnizo-Herrero Borja Martínez-Alonso Guillermo Torrado Santiago Torrado-Santiago Paloma Marina de la Torre-Iglesias
Meloxicam (MX) is a poorly water-soluble drug with severe gastrointestinal side effects. Topical hydrogel of hydroxypropyl guar (HPG) was formulated using a solid dispersion (SD) of MX with hydroxypropyl cellulose (LHPC) as an alternative to oral administration. The development of a solid dispersion with an adequate MX:LHPC ratio could increase the topical delivery of meloxicam. Solid dispersions showed high MX solubility values and were related to an increase in hydrophilicity. The drug/polymer and polymer/polymer interactions of solid dispersions within the HPG hydrogels were evaluated by SEM, DSC, FTIR, and viscosity studies. A porous structure was observed in the solid dispersion hydrogel MX:LHPC (1:2.5) and its higher viscosity was related to a high increase in hydrogen bonds among the –OH groups from LHPC and HPG with water molecules. In vitro drug release studies showed increases of 3.20 and 3.97-fold for hydrogels with MX:LHPC ratios of (1:1) and (1:2.5), respectively, at 2 h compared to hydrogel with pure MX. Finally, a fitting transition from zero to first-order model was observed for these hydrogels containing solid dispersions, while the n value of Korsmeyer–Peppas model indicated that release mechanism is governed by diffusion through an important relaxation of the polymer.
]]>Gels doi: 10.3390/gels10030206
Authors: Tetsuya Adachi Yoshiro Tahara Kenta Yamamoto Toshiro Yamamoto Narisato Kanamura Kazunari Akiyoshi Osam Mazda
Novel functional biomaterials are expected to bring about breakthroughs in developing immunotherapy and regenerative medicine through their application as drug delivery systems and scaffolds. Nanogels are defined as nanoparticles with a particle size of 100 nm or less and as having a gel structure. Nanogels have a three-dimensional network structure of cross-linked polymer chains, which have a high water content, a volume phase transition much faster than that of a macrogel, and a quick response to external stimuli. As it is possible to transmit substances according to the three-dimensional mesh size of the gel, a major feature is that relatively large substances, such as proteins and nucleic acids, can be taken into the gel. Furthermore, by organizing nanogels as a building block, they can be applied as a scaffold material for tissue regeneration. This review provides a brief overview of the current developments in nanogels in general, especially drug delivery, therapeutic applications, and tissue engineering. In particular, polysaccharide-based nanogels are interesting because they have excellent complexation properties and are highly biocompatible.
]]>Gels doi: 10.3390/gels10030204
Authors: Zhuying Wang Zhenhai Yu Shuanghe Ren Jun Liu Jing Xu Zengwang Guo Zhongjiang Wang
In this study, the purpose was to investigate the effects with different concentrations of carrageenan (CG, 0–0.30%) on the gel properties and freeze–thaw stability of soy protein isolate (SPI, 8%) cold-set gels. LF-NMR, MRI, and rheology revealed that CG promoted the formation of SPI-CG cold-set gel dense three-dimensional network structures and increased gel network cross-linking sites. As visually demonstrated by microstructure observations, CG contributed to the formation of stable SPI-CG cold-set gels with uniform and compact network structures. The dense gel network formation was caused when the proportion of disulfide bonds in the intermolecular interaction of SPI-CG cold-set gels increased, and the particle size and zeta potential of SPI-CG aggregates increased. SG20 (0.20% CG) had the densest gel network in all samples. It effectively hindered the migration and flow of water, which decreased the damage of freezing to the gel network. Therefore, SG20 exhibited excellent gel strength, water holding capacity, freeze–thaw stability, and steaming stability. This was beneficial for the gel having a good quality after freeze–thaw, which provided a valuable reference for the development of freeze–thaw-resistant SPI cold-set gel products.
]]>Gels doi: 10.3390/gels10030205
Authors: Saira Mansha Amna Sajjad Aneeqa Zarbab Tahmina Afzal Zakia Kanwal Muhammad Javaid Iqbal Mohsin Ali Raza Sharafat Ali
Drug delivery techniques based on polymers have been investigated for their potential to improve drug solubility, reduce systemic side effects, and controlled and targeted administration at infection site. In this study, we developed a co-polymeric hydrogel composed of graphene sheets (GNS), polyvinyl alcohol (PVA), and chitosan (CS) that is loaded with methotrexate (MTX) for in vitro liver cancer treatment. Fourier transform infrared spectroscopy (FTIR) and atomic force microscopy (AFM) was employed to check the structural properties and surface morphology. Moreover, tests were conducted on the cytotoxicity, hemolytic activity, release kinetics, swelling behaviour and degradation of hydrogels. A controlled release of drug from hydrogel in PBS at pH 7.4 was examined using release kinetics. Maximal drug release in six hours was 97.34%. The prepared hydrogels did not encourage the HepG2 growth and were non-hemolytic. The current study highlights the potential of GNS-based hydrogel loaded with MTX as an encouraging therapy for hepatocellular carcinoma. HepG2 cell viability of MTX-loaded CS-PVA-GNS hydrogel was (IC50 5.87 µg/200 mL) in comparison to free MTX (IC50 5.03 µg/200 mL). These outcomes recommend that hydrogels with GNS ensure improved drug delivery in cancer microenvironment while lessening adverse consequences on healthy cells.
]]>Gels doi: 10.3390/gels10030203
Authors: Ana M. Diaz-Lasprilla Meagan McKee Andrea C. Jimenez-Vergara Swathisri Ravi Devon Bellamy Wendy Ortega Cody O. Crosby Jennifer Steele Germán Plascencia-Villa George Perry Dany J. Munoz-Pinto
Multicomponent interpenetrating polymer network (mIPN) hydrogels are promising tissue-engineering scaffolds that could closely resemble key characteristics of native tissues. The mechanical and biochemical properties of mIPNs can be finely controlled to mimic key features of target cellular microenvironments, regulating cell-matrix interactions. In this work, we fabricated hydrogels made of collagen type I (Col I), fibrin, hyaluronic acid (HA), and poly (ethylene glycol) diacrylate (PEGDA) using a network-by-network fabrication approach. With these mIPNs, we aimed to develop a biomaterial platform that supports the in vitro culture of human astrocytes and potentially serves to assess the effects of the abnormal deposition of fibrin in cortex tissue and simulate key aspects in the progression of neuroinflammation typically found in human pathologies such as Alzheimer’s disease (AD), Parkinson’s disease (PD), and tissue trauma. Our resulting hydrogels closely resembled the complex modulus of AD human brain cortex tissue (~7.35 kPa), promoting cell spreading while allowing for the modulation of fibrin and hyaluronic acid levels. The individual networks and their microarchitecture were evaluated using confocal laser scanning microscopy (CLSM) and scanning electron microscopy (SEM). Human astrocytes were encapsulated in mIPNs, and negligible cytotoxicity was observed 24 h after the cell encapsulation.
]]>Gels doi: 10.3390/gels10030202
Authors: Tianjiao Zeng Huajian Chen Toru Yoshitomi Naoki Kawazoe Yingnan Yang Guoping Chen
Chemotherapy is one of the most common strategies for cancer treatment, whereas drug resistance reduces the efficiency of chemotherapy and leads to treatment failure. The mechanism of emerging chemoresistance is complex and the effect of extracellular matrix (ECM) surrounding cells may contribute to drug resistance. Although it is well known that ECM plays an important role in orchestrating cell functions, it remains exclusive how ECM stiffness affects drug resistance. In this study, we prepared agarose hydrogels of different stiffnesses to investigate the effect of hydrogel stiffness on the chemoresistance of breast cancer cells to doxorubicin (DOX). Agarose hydrogels with a stiffness range of 1.5 kPa to 112.3 kPa were prepared and used to encapsulate breast cancer cells for a three-dimensional culture with different concentrations of DOX. The viability of the cells cultured in the hydrogels was dependent on both DOX concentration and hydrogel stiffness. Cell viability decreased with DOX concentration when the cells were cultured in the same stiffness hydrogels. When DOX concentration was the same, breast cancer cells showed higher viability in high-stiffness hydrogels than they did in low-stiffness hydrogels. Furthermore, the expression of P-glycoprotein mRNA in high-stiffness hydrogels was higher than that in low-stiffness hydrogels. The results suggested that hydrogel stiffness could affect the resistance of breast cancer cells to DOX by regulating the expression of chemoresistance-related genes.
]]>Gels doi: 10.3390/gels10030201
Authors: Maja Benković Izvorka Laljak Davor Valinger Tamara Jurina Tea Sokač Cvetnić Jasenka Gajdoš Kljusurić Ana Jurinjak Tušek
The aim of this work was to analyze and compare the adsorption and desorption processes of carbohydrates (glucose as a model molecule), polyphenols (gallic acid as a model molecule), and proteins (bovine serum albumin, BSA as a model molecule) on alginate microcapsules. The adsorption and desorption processes were described by mathematical models (pseudo-first-order, pseudo-second-order, and Weber–Morris intraparticle diffusion model for adsorption, and first-order, Korsmeyer–Peppas, and the Higuchi model for desorption) in order to determine the dominant mechanisms responsible for both processes. By comparing the values of adsorption rate (k2) and initial adsorption rate (h0) based on the pseudo-first-order model, the lowest values were recorded for BSA (k1 = 0.124 ± 0.030 min−1), followed by glucose (k1 = 0.203 ± 0.041 min−1), while the model-obtained values for gallic acid were not considered significant at p < 0.05. For glucose and gallic acid, the limiting step of the adsorption process is the chemical sorption of substances, and the rate of adsorption does not depend on the adsorbate concentration, but depends on the capacity of the hydrogel adsorbent. Based on the desorption rates determined by the Korsmeyer–Peppas model (k), the highest values were recorded for gallic acid (k = 3.66236 ± 0.20776 g beads/mg gallic acid per min), followed by glucose (k = 2.55760 ± 0.16960 g beads/mg glucose per min) and BSA (k = 0.78881 ± 0.11872 g beads/mg BSA per min). The desorption process from alginate hydrogel microcapsules is characterized by the pseudo Fickian diffusion mechanism.
]]>Gels doi: 10.3390/gels10030200
Authors: Seung Hyeon Weon Yuhyeon Na Jiwoo Han Jeong Woo Lee Hyung Joo Kim Saerom Park Sang Hyun Lee
In this study, cellulose/Fe3O4 hydrogel microbeads were prepared through the sol–gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (TBAH) and 40% tetrabutylphosphonium hydroxide (TBPH) dissolved cellulose at room temperature and effectively dispersed Fe3O4, forming cellulose/Fe3O4 microbeads with an average diameter of ~15 µm. Additionally, these solvents co-dissolved cellulose and silk, allowing for the manufacture of cellulose/silk/Fe3O4 hydrogel microbeads with altered surface characteristics. Owing to the negatively charged surface characteristics, the adsorption capacity of the cellulose/silk/Fe3O4 microbeads for the cationic dye crystal violet was >10 times higher than that of the cellulose/Fe3O4 microbeads. When prepared with TBAH, the initial adsorption rate of bovine serum albumin (BSA) on the cellulose/silk/Fe3O4 microbeads was 18.1 times higher than that on the cellulose/Fe3O4 microbeads. When preparing TBPH, the equilibrium adsorption capacity of the cellulose/silk/Fe3O4 microbeads for BSA (1.6 g/g) was 8.5 times higher than that of the cellulose/Fe3O4 microbeads. The pH-dependent BSA release from the cellulose/silk/Fe3O4 microbeads prepared with TBPH revealed 6.1-fold slower initial desorption rates and 5.2-fold lower desorption amounts at pH 2.2 than those at pH 7.4. Cytotoxicity tests on the cellulose and cellulose/silk composites regenerated with TBAH and TBPH yielded nontoxic results. Therefore, cellulose/silk/Fe3O4 microbeads are considered suitable pH-responsive supports for orally administered protein pharmaceuticals.
]]>Gels doi: 10.3390/gels10030199
Authors: Xinghua Liang Xueli Shi Lingxiao Lan Yunmei Qing Bing Zhang Zhijie Fang Yujiang Wang
Gel electrolytes for lithium-ion batteries continue to replace the organic liquid electrolytes in conventional batteries due to their advantages of being less prone to leakage and non-explosive and possessing a high modulus of elasticity. However, the development of gel electrolytes has been hindered by their generally low ionic conductivity at room temperature and high interfacial impedance with electrodes. In this paper, a poly (vinylidene fluoride)-hexafluoropropylene copolymer (PVdF-HFP) with a flexible structure, Li6PS5Cl (LPSCl) powder of the sulfur–silver–germanium ore type, and lithium perchlorate salt (LiClO4) were prepared into sulfide gel composite electrolyte films (GCEs) via a thermosetting process. The experimental results showed that the gel composite electrolyte with 1% LPSCl in the PVdF-HFP matrix exhibited an ionic conductivity as high as 1.27 × 10−3 S·cm−1 at 25 °C and a lithium ion transference number of 0.63. The assembled LiFePO4||GCEs||Li batteries have excellent rate (130 mAh·g−1 at 1 C and 54 mAh·g−1 at 5 C) and cycling (capacity retention was 93% after 100 cycles at 0.1 C and 80% after 150 cycles at 0.2 C) performance. This work provides new methods and strategies for the design and fabrication of solid-state batteries with high ionic conductivity and high specific energy.
]]>Gels doi: 10.3390/gels10030198
Authors: João Ribeiro Marco Â. Luís Bruno Rodrigues Fátima Milhano Santos Joana Mesquita Renato Boto Cândida Teixeira Tomaz
The increasing demand for highly pure biopharmaceuticals has put significant pressure on the biotechnological industry to innovate in production and purification processes. Nucleic acid purification, crucial for gene therapy and vaccine production, presents challenges due to the unique physical and chemical properties of these molecules. Meeting regulatory standards necessitates large quantities of biotherapeutic agents of high purity. While conventional chromatography offers versatility and efficiency, it suffers from drawbacks like low flow rates and binding capacity, as well as high mass transfer resistance. Recent advancements in continuous beds, including monoliths and cryogel-based systems, have emerged as promising solutions to overcome these limitations. This review explores and evaluates the latest progress in chromatography utilizing monolithic and cryogenic supports for nucleic acid purification.
]]>Gels doi: 10.3390/gels10030197
Authors: Shakila Parveen Asrafali Thirukumaran Periyasamy Gazi A. K. M. Rafiqul Bari Seong-Cheol Kim
Polybenzoxazines (Pbzs) are advanced forms of phenolic resins that possess many attractive properties, including thermal-induced self-curing polymerization, void-free polymeric products and absence of by-product formation. They also possess high Tg (glass transition temperature) and thermal stability. But the produced materials are brittle in nature. In this paper, we present our attempt to decrease the brittleness of Pbz by blending it with polyvinylalcohol (PVA). Benzoxazine monomer (Eu-Ed-Bzo) was synthesized by following a simple Mannich condensation reaction. The formation of a benzoxazine ring was confirmed by FT-IR and NMR spectroscopic analyses. The synthesized benzoxazine monomer was blended with PVA in order to produce composite films, PVA/Pbz, by varying the amount of benzoxazine monomer (1, 3 and 5 wt. % of PVA). The property of the composite films was studied using various characterization techniques, including DSC, TGA, water contact angle analysis (WCA) and SEM. WCA analysis proved that the hydrophobic nature of Pbz (value) was transformed to hydrophilic (WCA of PVA/Pbz5 is 35.5°). These composite films could play the same role as flexible electrolytes in supercapacitor applications. For this purpose, the composite films were immersed in a 1 M KOH solution for 12 h in order to analyze their swelling properties. Moreover, by using this swelled gel, a symmetric supercapacitor, AC//PVA/Pbz5//AC, was constructed, exhibiting a specific capacitance of 170 F g−1.
]]>Gels doi: 10.3390/gels10030196
Authors: Ilenia Motta Michelina Soccio Giulia Guidotti Nadia Lotti Gianandrea Pasquinelli
Cardiovascular disease (CVD), the leading cause of death globally, affects the heart and arteries with a variety of clinical manifestations, the most dramatic of which are myocardial infarction (MI), abdominal aortic aneurysm (AAA), and intracranial aneurysm (IA) rupture. In MI, necrosis of the myocardium, scar formation, and loss of cardiomyocytes result from insufficient blood supply due to coronary artery occlusion. Beyond stenosis, the arteries that are structurally and functionally connected to the cardiac tissue can undergo pathological dilation, i.e., aneurysmal dilation, with high risk of rupture. Aneurysms of the intracranial arteries (IAs) are more commonly seen in young adults, whereas those of the abdominal aorta (AAA) are predominantly seen in the elderly. IAs, unpredictably, can undergo rupture and cause life-threatening hemorrhage, while AAAs can result in rupture, internal bleeding and high mortality rate. In this clinical context, hydrogels, three-dimensional networks of water-seizing polymers, have emerged as promising biomaterials for cardiovascular tissue repair or protection due to their biocompatibility, tunable properties, and ability to encapsulate and release bioactive molecules. This review provides an overview of the current state of research on the use of hydrogels as an innovative platform to promote cardiovascular-specific tissue repair in MI and functional recovery or protection in aneurysmal dilation.
]]>Gels doi: 10.3390/gels10030195
Authors: Dafni Dimakopoulou-Papazoglou Konstantina Zampouni Prodromos Prodromidis Thomas Moschakis Eugenios Katsanidis
The utilization of natural waxes to form oleogels has emerged as a new and efficient technique for structuring liquid edible oil into solid-like structures for diverse food applications. The objective of this study was to investigate the interaction between sunflower wax (SW) and monoglycerides (MGs) in olive oil oleogels and assess their physical characteristics and storage stability. To achieve this, pure SW and a combination of SW with MGs in a 1:1 ratio were examined within a total concentration range of 6–12% w/w. The formed oleogels were characterized based on their microstructure, melting and crystallization properties, textural characteristics, and oxidative stability during storage. All the oleogels were self-standing, and, as the concentration increased, the hardness of the oleogels also increased. The crystals of SW oleogels were long needle-like, while the combination of SW and MGs led to the formation of crystal aggregates and rosette-like crystals. Differential scanning calorimetry and FTIR showed that the addition of MGs led to different crystal structures. The oxidation results revealed that oleogels had low peroxide and TBARS values throughout the 28-day storage period. These results provide useful insights about the utilization of SW and MGs oleogels for potential applications in the food industry.
]]>Gels doi: 10.3390/gels10030194
Authors: Sorina Ropciuc Florina Dranca Mircea Adrian Oroian Ana Leahu Ancuţa Elena Prisacaru Mariana Spinei Georgiana Gabriela Codină
Five varieties of vegetable oil underwent oleogelation with two types of wax as follows: beeswax (BW) and rice bran wax (RW). The oleogels were analyzed for their physicochemical, thermal, and textural characteristics. The oleogels were used in the bun dough recipe at a percentage level of 5%, and the textural and rheological properties of the oleogel doughs were analyzed using dynamic and empirical rheology devices such as the Haake rheometer, the Rheofermentometer, and Mixolab. The thermal properties of beeswax oleogels showed a melting peak at a lower temperature for all the oils used compared with that of the oleogels containing rice bran wax. Texturally, for both waxes, as the percentage of wax increased, the firmness of the oleogels increased proportionally, which indicates better technological characteristics for the food industry. The effect of the addition of oleogels on the viscoelastic properties of the dough was measured as a function of temperature. All dough samples showed higher values for G′ (storage modulus) than those of G″ (loss modulus) in the temperature range of 20–90 °C, suggesting a solid, elastic-like behavior of all dough samples with the addition of oleogels. The influence of the beeswax and rice bran oleogels based on different types of vegetable oils on the thermo-mechanical properties of wheat flour dough indicated that the addition of oleogels in dough recipes generally led to higher dough stability and lower values for the dough development time and those related to the dough’s starch characteristics. Therefore, the addition of oleogels in dough recipes inhibits the starch gelatinization process and increases the shelf life of bakery products.
]]>Gels doi: 10.3390/gels10030193
Authors: Fabrizio Villapiano Teresa Silvestri Camilla Lo Gatto Danilo Aleo Virginia Campani Sossio Fabio Graziano Concetta Giancola Federica D’Aria Giuseppe De Rosa Marco Biondi Laura Mayol
This study endeavored to overcome the physiological barriers hindering optimal bioavailability in ophthalmic therapeutics by devising drug delivery platforms that allow therapeutically effective drug concentrations in ocular tissues for prolonged times. Thermosensitive drug delivery platforms were formulated by blending poloxamers (F68 and F127) with low-molecular-weight hyaluronic acid (HA) in various concentrations and loaded with hydrocortisone (HC). Among the formulations examined, only three were deemed suitable based on their desirable gelling properties at a temperature close to the eye’s surface conditions while also ensuring minimal gelation time for swift ocular application. Rheological analyses unveiled the ability of the formulations to develop gels at suitable temperatures, elucidating the gel-like characteristics around the physiological temperature essential for sustained drug release. The differential scanning calorimetry findings elucidated intricate hydrogel–water interactions, indicating that HA affects the water–polymer interactions within the gel by increasing the platform hydrophilicity. Also, in vitro drug release studies demonstrated significant hydrocortisone release within 8 h, governed by an anomalous transport mechanism, prompting further investigation for optimized release kinetics. The produced platforms offer promising prospects for efficacious ocular drug delivery, addressing pivotal challenges in ocular therapeutics and heralding future advancements in the domain.
]]>Gels doi: 10.3390/gels10030192
Authors: João P. Vareda Pedro M. C. Matias José A. Paixão Dina Murtinho Artur J. M. Valente Luisa Durães
A chitosan–silica hybrid aerogel was synthesized and presented as a potential adsorbent for the purification of cupric ion-contaminated media. The combination of the organic polymer (chitosan), which can be obtained from fishery wastes, with silica produced a mostly macroporous material with an average pore diameter of 33 µm. The obtained aerogel was extremely light (56 kg m−3), porous (96% porosity, 17 cm3 g−1 pore volume), and presented a Brunauer–Emmett–Teller surface area (SBET) of 2.05 m2 g−1. The effects of solution pH, aerogel and Cu(II) concentration, contact time, and counterion on cupric removal with the aerogel were studied. Results showed that the initial pH of the cation-containing aqueous solution had very little influence on the removal performance of this aerogel. According to Langmuir isotherm, this material can remove a maximum amount of ca. 40 mg of cupric ions per gram and the kinetic data showed that the surface reaction was the rate-limiting step and equilibrium was quickly reached (in less than one hour). Thus, the approach developed in this study enabled the recovery of waste for the preparation of a novel material, which can be efficiently reused in a new application, namely water remediation.
]]>Gels doi: 10.3390/gels10030191
Authors: Cong Cheng Wenhua Ma Rui Chen Yeting Zhu Lizhen Zheng Wei Li Daodao Hu
In the ancient Chinese recipe for composite mortar used in the construction of ground layers for architectural painting, the mixture of porcine blood and lime water is one of the constituent materials. Herein, according to the traditional recipe, the interaction between porcine blood and lime water was systematically and deeply investigated. The experimental investigation demonstrated that porcine blood mixed with lime water at the ratio found in the recipe can form a hydrogel with a hydrophobic surface. During air-drying, the lime water in porcine blood hydrogel can react with CO2 to form calcium carbonate. The crystal morphology of the formed calcium carbonate depends on the surrounding micro-environment of calcium ions in the porcine blood hydrogel. The formed morphology of calcium carbonate includes small calcite crystallites, small graininess calcite crystals with round features, calcite aggregates with layered ladder-like structures, and amorphous calcium carbonate (ACC). Interestingly, the calcium carbonate formed in the inner part of the porcine blood hydrogel exhibits lamellar distribution due to a Liesegang pattern formation. Based on the findings that the porcine blood hydrogel has surface hydrophobicity and brittleness, it can be predicted that in the preparation process of composite mortar for ancient building color painting base course, porcine blood used in the form of a hydrogel is not only easier to be dispersed in hydrophobic tung oil than in liquid porcine blood but also the affinity between porcine blood gel and tung oil is enhanced. As constituent material dispersed in the composite mortar, the layered distribution of calcium carbonate in the porcine blood hydrogel may presumably be beneficial to reduce the internal stress of the composite mortar material.
]]>Gels doi: 10.3390/gels10030190
Authors: Gladys Arline Politrón-Zepeda Gabriela Fletes-Vargas Rogelio Rodríguez-Rodríguez
The repair of nervous tissue is a critical research field in tissue engineering because of the degenerative process in the injured nervous system. In this review, we summarize the progress of injectable hydrogels using in vitro and in vivo studies for the regeneration and repair of nervous tissue. Traditional treatments have not been favorable for patients, as they are invasive and inefficient; therefore, injectable hydrogels are promising for the treatment of damaged tissue. This review will contribute to a better understanding of injectable hydrogels as potential scaffolds and drug delivery system for neural tissue engineering applications.
]]>Gels doi: 10.3390/gels10030189
Authors: Sofia Milenkova Rita Ambrus Mahwash Mukhtar Bissera Pilicheva Maria Marudova
Chitosan, being a biocompatible and mucoadhesive polysaccharide, is one of the most preferred hydrogel-forming materials for drug delivery. The objectives of the present study are to obtain spray-dried microparticles based on low-molecular-weight chitosan and study their potential application as cargo systems for the orally active drug benzydamine hydrochloride. Three types of particles are obtained: raw chitosan particles (at three different concentrations), cross-linked with sodium tripolyphosphate (NaTPP) particles (at three different chitosan:NaTPP ratios), and particles coated with mannitol (at three different chitosan:mannitol ratios), all of them in the size range between 1 and 10 µm. Based on the loading efficiency and the yields of the formulated hydrogel particles, one model of each type is chosen for further investigation of the effect of the cross-linker or the excipient on the properties of the gel structures. The morphology of both empty and benzydamine hydrochloride-loaded chitosan particles was examined by scanning electron microscopy, and it was quite regular and spherical. Interactions and composition in the samples are investigated by Fourier-transformed infrared spectroscopy. The thermal stability and phase state of the drug and drug-containing polymer matrixes were tested by differential scanning calorimetry and X-ray powdered diffraction, revealing that the drug underwent a phase transition. A drug release kinetics study of the chosen gel-based structures in simulated saliva buffer (pH = 6.8) and mathematical modeling of the process were performed, indicating the Weibull model as the most appropriate one.
]]>Gels doi: 10.3390/gels10030188
Authors: Mariana Ribeiro Marco Simões Carla Vitorino Filipa Mascarenhas-Melo
Hydrogels are polymeric materials that possess a set of characteristics meeting various requirements of an ideal wound dressing, making them promising for wound care. These features include, among others, the ability to absorb and retain large amounts of water and the capacity to closely mimic native structures, such as the extracellular matrix, facilitating various cellular processes like proliferation and differentiation. The polymers used in hydrogel formulations exhibit a broad spectrum of properties, allowing them to be classified into two main categories: natural polymers like collagen and chitosan, and synthetic polymers such as polyurethane and polyethylene glycol. This review offers a comprehensive overview and critical analysis of the key polymers that can constitute hydrogels, beginning with a brief contextualization of the polymers. It delves into their function, origin, and chemical structure, highlighting key sources of extraction and obtaining. Additionally, this review encompasses the main intrinsic properties of these polymers and their roles in the wound healing process, accompanied, whenever available, by explanations of the underlying mechanisms of action. It also addresses limitations and describes some studies on the effectiveness of isolated polymers in promoting skin regeneration and wound healing. Subsequently, we briefly discuss some application strategies of hydrogels derived from their intrinsic potential to promote the wound healing process. This can be achieved due to their role in the stimulation of angiogenesis, for example, or through the incorporation of substances like growth factors or drugs, such as antimicrobials, imparting new properties to the hydrogels. In addition to substance incorporation, the potential of hydrogels is also related to their ability to serve as a three-dimensional matrix for cell culture, whether it involves loading cells into the hydrogel or recruiting cells to the wound site, where they proliferate on the scaffold to form new tissue. The latter strategy presupposes the incorporation of biosensors into the hydrogel for real-time monitoring of wound conditions, such as temperature and pH. Future prospects are then ultimately addressed. As far as we are aware, this manuscript represents the first comprehensive approach that brings together and critically analyzes fundamental aspects of both natural and synthetic polymers constituting hydrogels in the context of cutaneous wound healing. It will serve as a foundational point for future studies, aiming to contribute to the development of an effective and environmentally friendly dressing for wounds.
]]>Gels doi: 10.3390/gels10030187
Authors: Suhail Ayoub Khan Hamza Ahmad Guoyin Zhu Huan Pang Yizhou Zhang
The remarkable flexibility and heightened sensitivity of flexible sensors have drawn significant attention, setting them apart from traditional sensor technology. Within this domain, hydrogels—3D crosslinked networks of hydrophilic polymers—emerge as a leading material for the new generation of flexible sensors, thanks to their unique material properties. These include structural versatility, which imparts traits like adhesiveness and self-healing capabilities. Traditional templating-based methods fall short of tailor-made applications in crafting flexible sensors. In contrast, 3D printing technology stands out with its superior fabrication precision, cost-effectiveness, and satisfactory production efficiency, making it a more suitable approach than templating-based strategies. This review spotlights the latest hydrogel-based flexible sensors developed through 3D printing. It begins by categorizing hydrogels and outlining various 3D-printing techniques. It then focuses on a range of flexible sensors—including those for strain, pressure, pH, temperature, and biosensors—detailing their fabrication methods and applications. Furthermore, it explores the sensing mechanisms and concludes with an analysis of existing challenges and prospects for future research breakthroughs in this field.
]]>Gels doi: 10.3390/gels10030186
Authors: Shadi Shahriari P. Ravi Selvaganapathy
Sepsis, a life-threatening condition resulting from a failing host response to infection, causes millions of deaths annually, necessitating rapid and simple prognostic assessments. A variety of genomic and proteomic biomarkers have been developed for sepsis. For example, it has been shown that the level of plasma cell-free DNA (cfDNA) and circulating histones increases considerably during sepsis, and they are linked with sepsis severity and mortality. Developing a diagnostic tool that is capable of assessing such diverse biomarkers is challenging as the detection methodology is quite different for each. Here, a fully integrated microfluidic device capable of detecting a genomic biomarker (cfDNA) and a proteomic biomarker (total circulating histones) using a common detection platform has been demonstrated. The microfluidic device utilizes dehydrated agarose gates loaded with pH-specific agarose to electrophoretically trap cfDNA and histones at their respective isoelectric points. It also incorporates fluorescent dyes within the device, eliminating the need for off-chip sample preparation and allowing the direct testing of plasma samples without the need for labeling DNA and histones with fluorescent dyes beforehand. Xurography, which is a low-cost and rapid method for fabrication of microfluidics, is used in all the fabrication steps. Experimental results demonstrate the effective accumulation and separation of cfDNA and histones in the agarose gates in a total processing time of 20 min, employing 10 and 30 Volts for cfDNA and histone accumulation and detection, respectively. The device can potentially be used to distinguish between the survivors and non-survivors of sepsis. The integration of the detection of both biomarkers into a single device and dye immobilization enhances its clinical utility for rapid point-of-care assessment of sepsis prognosis.
]]>Gels doi: 10.3390/gels10030185
Authors: Oscar Valdes Daniel Bustos Luis Guzmán Marcelo Muñoz-Vera Gabriela Urra Ricardo I. Castro Luis Morales-Quintana
The integration of abscisic acid (ABA) into a chitosan–alginate gel blend unveils crucial insights into the formation and stability of these two substances. ABA, a key phytohormone in plant growth and stress responses, is strategically targeted for controlled release within these complexes. This study investigates the design and characterization of this novel controlled-release system, showcasing the potential of alginate–chitosan gel blends in ABA delivery. Computational methods, including molecular dynamics simulations, are employed to analyze the structural effects of microencapsulation, offering valuable insights into complex behavior under varying conditions. This paper focuses on the controlled release of ABA from these complexes, highlighting its strategic importance in drug delivery systems and beyond. This controlled release enables targeted and regulated ABA delivery, with far-reaching implications for pharmaceuticals, agriculture, and plant stress response studies. While acknowledging context dependency, the paper suggests that the liberation or controlled release of ABA holds promise in applications, urging further research and experimentation to validate its utility across diverse fields. Overall, this work significantly contributes to understanding the characteristics and potential applications of chitosan–alginate complexes, marking a noteworthy advancement in the field of controlled-release systems.
]]>Gels doi: 10.3390/gels10030184
Authors: Anandhu Mohan Madhappan Santhamoorthy Thi Tuong Vy Phan Seong-Cheol Kim
The regulated and targeted administration of hydrophobic and hydrophilic drugs is both promising and challenging in the field of drug delivery. Developing a hydrogel which is responsive to dual stimuli is considered a promising and exciting research area of study. In this work, melamine functionalized poly-N-isopropyl acrylamide-co-glycidyl methacrylate copolymer has been developed by copolymerizing glycidyl methacrylate (GMA) monomer with N-isopropyl acrylamide (NIPAm) and further functionalized with melamine units (pNIPAm-co-pGMA-Mela). The prepared pNIPAm-co-pGMA-Mela copolymer hydrogel was characterized using various characterization techniques, including 1H NMR, FTIR, SEM, zeta potential, and particle size analysis. A hydrophobic drug (ibuprofen, Ibu) and hydrophilic drug (5-fluorouracil, 5-Fu) were selected as model drugs. Dual pH and temperature stimuli-responsive drug release behavior of the pNIPAm-co-pGMA-Mela hydrogel was evaluated under different pH (pH 7.4 and 4.0) and temperature (25 °C, 37 °C, and 45 °C) conditions. Furthermore, the in vitro biocompatibility of the developed pNIPAm-co-pGMA-Mela copolymer hydrogel was determined on MDA-MB-231 cells. The pH and temperature-responsive drug delivery study results reveal that the pNIPAm-co-pGMA-Mela hydrogel system is responsive to both pH and temperature stimuli and exhibits about ~100% of Ibu and 5-Fu, respectively, released at pH 4.0/45 °C. Moreover, the MTT assay and hemocompatibility analysis results proved that the pNIPAm-co-pGMA-Mela hydrogel system is biocompatible and hemocompatible, suggesting that that it could be used for drug delivery applications. The experimental results suggest that the proposed pNIPAm-co-pGMA-Mela hydrogel system is responsive to dual pH and temperature stimuli, and could be a promising drug carrier system for both hydrophilic and hydrophobic drug delivery applications.
]]>Gels doi: 10.3390/gels10030183
Authors: Raghad Abdl Aali Shayma Al-Sahlany
Gellan gum (GG) is a linear, negatively charged exopolysaccharide that is biodegradable and non-toxic. When metallic ions are present, a hard and transparent gel is produced, which remains stable at a low pH. It exhibits high water solubility, can be easily bio-fabricated, demonstrates excellent film/hydrogel formation, is biodegradable, and shows biocompatibility. These characteristics render GG a suitable option for use in food, biomedical, and cosmetic fields. Thus, this review paper offers a concise summary of microbial polysaccharides. Moreover, an in-depth investigation of trends in different facets of GG, such as biosynthesis, chemical composition, and physical and chemical properties, is emphasized. In addition, this paper highlights the process of extracting and purifying GG. Furthermore, an in-depth discussion of the advantages and disadvantages of GG concerning other polysaccharides is presented. Moreover, the utilization of GG across different industries, such as food, medicine, pharmaceuticals, cosmetics, etc., is thoroughly examined and will greatly benefit individuals involved in this field who are seeking fresh opportunities for innovative projects in the future.
]]>Gels doi: 10.3390/gels10030182
Authors: Svenja Wein Carina Schemmer Miriam Aischa Al Enezy-Ulbrich Shannon Anna Jung Stephan Rütten Mark Kühnel Danny Jonigk Wilhelm Jahnen-Dechent Andrij Pich Sabine Neuss
This study focuses on enhancing controllable fibrin-based hydrogels for tissue engineering, addressing existing weaknesses. By integrating a novel copolymer, we improved the foundation for cell-based angiogenesis with adaptable structural features. Tissue engineering often faces challenges like waste disposal and nutrient supply beyond the 200 µm diffusion limit. Angiogenesis breaks through this limitation, allowing the construction of larger constructs. Our innovative scaffold combination significantly boosts angiogenesis, resulting in longer branches and more capillary network junctions. The copolymer attached to fibrin fibers enables precise adjustment of hydrogel mechanical dynamic properties for specific applications. Our material proves effective for angiogenesis, even under suppression factors like suramin. In our study, we prepared fibrin-based hydrogels with and without the copolymer PVP12400-co-GMA10mol%. Using a co-culture system of human umbilical vein endothelial cells (HUVEC) and mesenchymal stem cells (MSC), we analyzed angiogenetic behavior on and within the modified hydrogels. Capillary-like structures were reproducibly formed on different surfaces, demonstrating the general feasibility of three-dimensional endothelial cell networks in fibrin-based hydrogels. This highlights the biomaterial’s suitability for in vitro pre-vascularization of biohybrid implants.
]]>Gels doi: 10.3390/gels10030181
Authors: Martina Romeo Elisabetta Mazzotta Francesca Lovati Michele Porto Cesare Oliviero Rossi Rita Muzzalupo
Background: This study aims to evaluate the percutaneous permeation profiles of caffeic acid (CA) from the cubic and hexagonal liquid crystalline phases of Pluronic P123/water mixtures. Method: The resulting drug-loaded mesophases were subjected to characterisation through deuterium nuclear magnetic resonance spectroscopy and polarised optical microscopy observations. These analyses aimed to evaluate the structural changes that occurred in the mesophases loading with CA. Additionally, steady and dynamic rheology studies were conducted to further explore their mechanical properties and correlate them to the supramolecular structure. Finally, CA release experiments were carried out at two different temperatures to examine the behaviour of the structured systems in a physiological or hyperthermic state. Results: As the concentration of the polymer increases, an increase in the viscosity of the gel is noted; however, the addition of caffeic acid increases microstructure fluidity. It is observed that the temperature effect conforms to expectations. The increase in temperature causes a decrease in viscosity and, consequently, an increase in the rate of permeation of caffeic acid. Conclusions: The CA permeation profile from the prepared formulations is mostly dependent on the structural organisation and temperature. Cubic mesophase LLC 30/CA showed greater skin permeation with good accumulation in the skin at both tested temperatures.
]]>Gels doi: 10.3390/gels10030180
Authors: Marina González-Barriuso Mario Sánchez-Suárez Judith González-Lavín Ana Arenillas Natalia Rey-Raap
Carbonaceous materials used in most electrochemical applications require high specific surface area, adequate pore size distribution, and high electrical conductivity to ensure good interaction with the electrolyte and fast electron transport. The development of transition metal doped graphene aerogels is a possible solution, since their structure, morphology, and electrical properties can be controlled during the synthesis process. This work aims to synthesize Ni-doped graphene aerogels to study the role of different nickel salts in the sol-gel reaction and their final properties. The characterization data show that, regardless of the nature of the Ni salts, the surface area, volume of micropores, and enveloped density decrease, while the porosity and electrical conductivity increase. However, differences in morphology, mesopore size distribution, degree of order of the carbon structure, and electrical conductivity were observed depending on the type of Ni salt. It was found that nickel nitrate results in a material with a broader mesopore distribution, higher electrical conductivity, and hence, higher electrochemical surface area, demonstrating that graphene aerogels can be easily synthesized with tailored properties to fit the requirements of specific electrochemical applications.
]]>Gels doi: 10.3390/gels10030179
Authors: Xuanan Lu Jianguo Luo Lingxiao Lan Bing Zhang Zhikun Chen Yujiang Wang Xinghua Liang Qinglie Mo
Gel polymer electrolytes (GPEs) have high safety and excellent electrochemical performance, so applying GPEs in lithium batteries has received much attention. However, their poor lithium ion transfer number, cycling stability, and low room temperature ionic conductivity seriously affect the utilization of gel polymer electrolytes. This paper successfully synthesized flexible poly (vinylidene fluoride-hexafluoropropylene)–lithium titanium aluminum phosphate (PVDF-HFP-LATP) gel polymer electrolytes using the immersion precipitation method. The resulting GPE has a porous honeycomb structure, which ensures that the GPE has sufficient space to store the liquid electrolyte. The GPE has a high ionic conductivity of 1.03 ×10−3 S cm−1 at room temperature (25 °C). The GPE was applied to LiFePO4/GPE/Li batteries with good rate performance at room temperature. The discharge specific capacity of 1C was as high as 121.5 mAh/g, and the capacity retention rate was 94.0% after 300 cycles. These results indicate that PVDF-HFP-LATP-based GPEs have the advantage of simplifying the production process and can improve the utility of gel polymer lithium metal batteries.
]]>Gels doi: 10.3390/gels10030178
Authors: Yao Dai Fuwei Lu Yuhua Tang Yuanyuan Wang Xinyi He Tengfei Wang Juan Wu
To enhance the performance and reduce the amount of ester-based lubricants used in weak gel drilling fluids, a shear dynamics simulation under extreme pressure conditions was employed to refine the formulation of the base oil and pressure additives. The simulation results were validated using fatty acid methyl, ethyl, and butyl esters. Fatty acid methyl ester demonstrated the lowest temperature increase and the highest load-bearing capacity post-shear. The four-ball friction test revealed that methyl oleate had a coefficient of friction of 0.0018, approximately a third of that for butyl oleate, confirming the simulation’s accuracy. By using methyl oleate as the base oil and oleamide as the pressure-resistant component, the optimal shear stress was achieved with a 10% addition of oleamide. A lubricant composed of 90% methyl oleate and 10% oleamide was tested and showed a coefficient of friction of 0.03 when 0.5% was added to bentonite slurry, indicating a strong lubricating film. Adding 1% of this lubricant to a low gel drilling fluid system did not affect its rheological properties, and the gel structure remained stable after seven days of aging. Field tests at the Fu86-3 well in the Jiangsu Oilfield of Sinopec confirmed that adding 1% of the ester-based lubricant to the drilling fluid significantly improved drilling efficiency, reduced drag by an average of 33%, and increased the drilling rate to 22.12 m/h. This innovation effectively prevents drilling complications and successfully achieves the objectives of enhancing efficiency.
]]>Gels doi: 10.3390/gels10030177
Authors: Wei Wang Qi-Tong He Yin-Feng Chen Bai-Hui Wang Wen-Ying Xu Qing-Lei Liu Hui-Min Liu
Ethylhexyl methoxycinnamate (EHMC) is frequently employed as a photoprotective agent in sunscreen formulations. EHMC has been found to potentially contribute to health complications as a result of its propensity to produce irritation and permeate the skin. A microgel carrier, consisting of poly(ethylene glycol dimethacrylate) (pEDGMA), was synthesized using interfacial polymerization with the aim of reducing the irritation and penetration of EHMC. The thermogravimetric analysis (TGA) indicated that the EHMC content accounted for 75.72% of the total composition. Additionally, the scanning electron microscopy (SEM) images depicted the microgel as exhibiting a spherical morphology. In this study, the loading of EHMC was demonstrated through FTIR and contact angle tests. The UV resistance, penetration, and skin irritation of the EHMC-pEDGMA microgel were additionally assessed. The investigation revealed that the novel sunscreen compound, characterized by limited dermal absorption, had no irritant effects and offered sufficient protection against ultraviolet radiation.
]]>Gels doi: 10.3390/gels10030176
Authors: Mine Altunbek Mert Gezek Maria Eduarda Torres Gouveia Gulden Camci-Unal
Hydrogel-based dressings can effectively heal wounds by providing multiple functions, such as antibacterial, anti-inflammatory, and preangiogenic bioactivities. The ability to spray the dressing is important for the rapid and effective coverage of the wound surface. In this study, we developed a sprayable hydrogel-based wound dressing using naturally derived materials: hyaluronic acid and gelatin. We introduced methacrylate groups (HAMA and GelMA) to these materials to enable controllable photocrosslinking and form a stable hydrogel on the wound surface. To achieve sprayability, we evaluated the concentration of GelMA within a range of 5–15% (w/v) and then incorporated 1% (w/v) HAMA. Additionally, we incorporated calcium peroxide into the hydrogel at concentrations ranging from 0 to 12 mg/mL to provide self-oxygenation and antibacterial properties. The results showed that the composite hydrogels were sprayable and could provide oxygen for up to two weeks. The released oxygen relieved metabolic stress in fibroblasts and reduced cell death under hypoxia in in vitro culture. Furthermore, calcium peroxide added antibacterial properties to the wound dressing. In conclusion, the developed sprayable hydrogel dressing has the potential to be advantageous for wound healing due to its practical and conformable application, as well as its self-oxygenating and antibacterial functions.
]]>Gels doi: 10.3390/gels10030175
Authors: Wei Guo Xiaoyue Ding Han Zhang Zhenzhong Liu Yanting Han Qianqian Wei Oseweuba Valentine Okoro Amin Shavandi Lei Nie
The management of wound healing represents a significant clinical challenge due to the complicated processes involved. Chitosan has remarkable properties that effectively prevent certain microorganisms from entering the body and positively influence both red blood cell aggregation and platelet adhesion and aggregation in the bloodstream, resulting in a favorable hemostatic outcome. In recent years, chitosan-based hydrogels have been widely used as wound dressings due to their biodegradability, biocompatibility, safety, non-toxicity, bioadhesiveness, and soft texture resembling the extracellular matrix. This article first summarizes an overview of the main chemical modifications of chitosan for wound dressings and then reviews the desired properties of chitosan-based hydrogel dressings. The applications of chitosan-based hydrogels in wound healing, including burn wounds, surgical wounds, infected wounds, and diabetic wounds are then discussed. Finally, future prospects for chitosan-based hydrogels as wound dressings are discussed. It is anticipated that this review will form a basis for the development of a range of chitosan-based hydrogel dressings for clinical treatment.
]]>Gels doi: 10.3390/gels10030174
Authors: Hossein Omidian Arnavaz Akhzarmehr Sumana Dey Chowdhury
The development of superabsorbent hydrogels is experiencing a transformative era across industries. While traditional synthetic hydrogels have found broad utility, their non-biodegradable nature has raised environmental concerns, driving the search for eco-friendlier alternatives. Cellulose-based superabsorbents, derived from sustainable sources, are gaining prominence. Innovations include biodegradable polymer hydrogels, natural cellulose-chitosan variants, and cassava starch-based alternatives. These materials are reshaping agriculture by enhancing soil fertility and water retention, serving as potent hemostatic agents in medicine, contributing to pollution control, and providing eco-friendly construction materials. Cellulose-based hydrogels also offer promise in drug delivery and hygiene products. Advanced characterization techniques aid in optimizing their properties, while the shift towards circular economy practices further highlights sustainability. This manuscript provides a comprehensive overview of these advancements, highlighting their diverse applications and environmental benefits.
]]>Gels doi: 10.3390/gels10030173
Authors: Felix Ellwanger Melanie Fuhrmann Heike P. Karbstein Gabriela Itziar Saavedra Isusi
High-moisture extrusion of plant proteins to create meat-like structures is a process that has met with increasing attention in the recent past. In the process, the proteins are thermomechanically stressed in the screw section of the extruder, and the resulting protein gel is structured in the attached cooling die. Various protein sources, notably soy protein isolate (SPI) and wheat gluten, are used to form gels with different networks: SPI creates a physical, non-covalent network, while gluten forms a chemical, covalent one. The food industry frequently adds weak acids to modify taste and shelf life. However, it is known that a change in pH affects the gelation behavior of proteins because the repulsive forces within and between the proteins change. The research reported here was carried out to investigate for the two proteins mentioned the influence of pH modification by the addition of citric acid and acetic acid on gel formation and the meat-like structures produced. For this purpose, materials and parameters were screened using a closed cavity rheometer, followed by extrusion trials at pH 7.36–4.14 for SPI and pH 5.83–3.37 for gluten. The resulting extrudates were analyzed optically and mechanically, and protein solubility was tested in a reducing buffer. For both protein systems, the addition of acid results in less pronounced meat-like structures. At decreasing pH, the complex viscosity of SPI increases (from 11,970 Pa·s to 40,480 Pa·s at 100 °C), the generated gel becomes stronger (strain decreased from 0.62 to 0.48 at 4.5 × 105 Pa), and the cross-linking density grows. For gluten, a decreasing pH results in altered reaction kinetics, a more deformable resulting gel (strain increased from 0.7 to 0.95 at 4.5 × 105 Pa), and a decreased cross-linking density. Solubility tests show that no additional covalent bonds are formed with SPI. With gluten, however, the polymerization reaction is inhibited, and fewer disulfide bonds are formed.
]]>Gels doi: 10.3390/gels10030172
Authors: Silvia Locarno Paolo Arosio Francesca Curtoni Marco Piazzoni Emanuele Pignoli Salvatore Gallo
In recent decades, hydrogels have emerged as innovative soft materials with widespread applications in the medical and biomedical fields, including drug delivery, tissue engineering, and gel dosimetry. In this work, a comprehensive study of the macroscopic and microscopic properties of hydrogel matrices based on Poly(vinyl-alcohol) (PVA) chemically crosslinked with Glutaraldehyde (GTA) was reported. Five different kinds of PVAs differing in molecular weight and degree of hydrolysis were considered. The local microscopic organization of the hydrogels was studied through the use of the 1H nuclear magnetic resonance relaxometry technique. Various macroscopic properties (gel fraction, water loss, contact angle, swelling degree, viscosity, and Young’s Modulus) were investigated with the aim of finding a correlation between them and the features of the hydrogel matrix. Additionally, an optical characterization was performed on all the hydrogels loaded with Fricke solution to assess their dosimetric behavior. The results obtained indicate that the degree of PVA hydrolysis is a crucial parameter influencing the structure of the hydrogel matrix. This factor should be considered for ensuring stability over time, a vital property in the context of potential biomedical applications where hydrogels act as radiological tissue-equivalent materials.
]]>Gels doi: 10.3390/gels10030171
Authors: Jingyuan Xu James A. Kenar
As a soluble fiber, inulin is present in many plants and has many applications in food and non-food products. In this work, we investigated the rheological properties of inulin dispersions at seven concentrations. The linear viscoelastic properties of inulin were determined using a conventional mechanical rheometer. At 25 wt%, inulin exhibited fluid-like viscoelastic liquid behavior. However, when concentrations were ≥27.5 wt%, inulin exhibited gel-like viscoelastic properties. The viscoelastic properties (moduli and viscosities) increased with increasing inulin concentration. The high-frequency linear rheological properties of inulin were also investigated using the modern light scattering technique, diffusion wave spectroscopy (DWS). The diffusion wave spectroscopy (DWS) measurements showed the amplitude of complex moduli (|G*(ω)|) of inulin gels (≥27.5 wt%) to be proportional to ½ power law of the frequency, which suggests inulin gels behave similarly to flexible polymers. The non-linear steady shear experiments demonstrated that inulin exhibited shear-thinning behavior that was well fitted by a power law constitutive model. The trend of the power law exponent from the experiments indicated that the shear-thinning extent for inulin was greater as the inulin concentration increased. The results of this work indicated that the properties of inulin gel can be manipulated by altering its concentration. Therefore, the desired inulin product can be designed accordingly. These results can be used to direct further food and non-food applications, such as wound healing materials for inulin gels.
]]>Gels doi: 10.3390/gels10030170
Authors: Youssef Hafidi Hicham El Hatka Dominik Schmitz Manuel Krauss Jürgen Pettrak Markus Biel Najim Ittobane
Drought and water shortage are serious problems in many arid and semi-arid regions. This problem is getting worse and even continues in temperate climatic regions due to climate change. To address this problem, the use of biodegradable hydrogels is increasingly important for the application as water-retaining additives in soil. Furthermore, efficient (micro-)nutrient supply can be provided by the use of tailored hydrogels. Biodegradable polyaspartic acid (PASP) hydrogels with different available (1,6-hexamethylene diamine (HMD) and L-lysine (LYS)) and newly developed crosslinkers based on diesters of glycine (GLY) and (di-)ethylene glycol (DEG and EG, respectively) were synthesized and characterized using Fourier transform infrared (FTIR) spectroscopy and scanning electron microscopy (SEM) and regarding their swelling properties (kinetic, absorbency under load (AUL)) as well as biodegradability of PASP hydrogel. Copper (II) and zinc (II), respectively, were loaded as micronutrients in two different approaches: in situ with crosslinking and subsequent loading of prepared hydrogels. The results showed successful syntheses of di-glycine-ester-based crosslinkers. Hydrogels with good water-absorbing properties were formed. Moreover, the developed crosslinking agents in combination with the specific reaction conditions resulted in higher water absorbency with increased crosslinker content used in synthesis (10% vs. 20%). The prepared hydrogels are candidates for water-storing soil additives due to the biodegradability of PASP, which is shown in an exemple. The incorporation of Cu(II) and Zn(II) ions can provide these micronutrients for plant growth.
]]>Gels doi: 10.3390/gels10030169
Authors: Joanna Harasym Karol Banaś
This manuscript analyzes the research considering the exploitation of lecithin in oleogelation. The main objective of the work was to gather, analyze, and extract from the existing research data the information that enables us to identify lecithin-dependent roles. Oleogelation is still under research, while using various oleogelators and structurants provides changes on different physico-chemical levels. Multivariable formulations do not facilitate the elucidation of the specific role of any of them. Lecithin, due to its complex structure, big molecule, and amphiphilic nature, can provide different functionalities in complex matrices like oleogels. Therefore, this review identifies and categorizes the functionality of lecithin in oleogelation into four main roles: 1. oleogelation facilitator; 2. structure-forming impact; 3. texturing agent; and 4. functionality provider. Also, the origin and structure-forming characteristics of lecithin, as well as a short summary of the oleogelation process itself, are presented. Our critical analysis allowed us to identify the roles of lecithin in the oleogelation process and categorized them as follows: oleogelator, emulsifier, structural organization facilitator, structural modifier, crystal characteristics modifier, self-assembly promoter, thermal behavior changer, hydrogen-bonded networks promoter, hydrogel structure modifier, texture and structural modifier, gel-like state promoter, oil capacity enhancer, functionality provider, shelf life extender, and bioavailability and bioaccessibility enhancer. Lecithin came out as an important and multifunctional compound whose applications in oleogelation need to be thoroughly pre-considered. It is crucial to grasp all the possible roles of used compounds to be able to predict the final functionality and characteristics of formed oleogel matrices.
]]>Gels doi: 10.3390/gels10030168
Authors: Jorge Domínguez-Martínez Jesús López-Sánchez Federico García-Galván Aída Serrano Violeta Barranco Juan Carlos Galván Óscar Rodríguez de la Fuente Noemí Carmona
The latest advances in technology and materials science have catalyzed a transformative shift towards the adoption of environmentally conscious and lightweight materials across key sectors such as aeronautics, biomedical, and automotive industries. Noteworthy among these innovations are the magnesium-aluminum (Mg-Al) alloys employed in aeronautical applications, contributing to the overall reduction in aircraft weight and subsequently diminishing fuel consumption and mitigating atmospheric emissions. The present work delves into a study of the anti-corrosive properties inherent in various sol-gel coatings, leveraging a range of environmentally friendly corrosion inhibitors, specifically tailored for samples of the AZ61 alloy. Methodologically, the work involves the synthesis and application of sol-gel coatings on AZ61 alloy containing eco-friendly inhibitors: L-cysteine, N-acetyl-cysteine, curcumin and methylene blue. Subsequently, an accelerated corrosion test in a simulated saline environment is performed. Through microstructural and compositional analyses, the best inhibitors responses are achieved with inhibitors containing S, N heteroatoms and conjugated double bonds in their structure, probably due to the creation of a continuous MgCl2 layer. This research contributes to the ongoing discourse on protective eco-coatings, aligning with the broader paradigm shift towards sustainable and lightweight materials in key industries.
]]>Gels doi: 10.3390/gels10030167
Authors: Tess De Maeseneer Lana Van Damme Merve Kübra Aktan Annabel Braem Paula Moldenaers Sandra Van Vlierberghe Ruth Cardinaels
The tissue engineering field is currently advancing towards minimally invasive procedures to reconstruct soft tissue defects. In this regard, injectable hydrogels are viewed as excellent scaffold candidates to support and promote the growth of encapsulated cells. Cross-linked gelatin methacryloyl (GelMA) gels have received substantial attention due to their extracellular matrix-mimicking properties. In particular, GelMA microgels were recently identified as interesting scaffold materials since the pores in between the microgel particles allow good cell movement and nutrient diffusion. The current work reports on a novel microgel preparation procedure in which a bulk GelMA hydrogel is ground into powder particles. These particles can be easily transformed into a microgel by swelling them in a suitable solvent. The rheological properties of the microgel are independent of the particle size and remain stable at body temperature, with only a minor reversible reduction in elastic modulus correlated to the unfolding of physical cross-links at elevated temperatures. Salts reduce the elastic modulus of the microgel network due to a deswelling of the particles, in addition to triple helix denaturation. The microgels are suited for clinical use, as proven by their excellent cytocompatibility. The latter is confirmed by the superior proliferation of encapsulated adipose tissue-derived stem cells in the microgel compared to the bulk hydrogel. Moreover, microgels made from the smallest particles are easily injected through a 20G needle, allowing a minimally invasive delivery. Hence, the current work reveals that powdered cross-linked GelMA is an excellent candidate to serve as an injectable hydrogel for adipose tissue engineering.
]]>Gels doi: 10.3390/gels10030166
Authors: Sónia Oliveira Isabel Sousa Anabela Raymundo Carlos Bengoechea
Seaweeds, rich in high-value polysaccharides with thickening/gelling properties (e.g., agar, carrageenan, and alginate), are extensively used in the food industry for texture customization and enhancement. However, conventional extraction methods for these hydrocolloids often involve potentially hazardous chemicals and long extraction times. In this study, three red seaweed species (Chondrus crispus, Gelidium Corneum, and Gracilaria gracilis) commercialized as food ingredients by local companies were chosen for their native gelling biopolymers, which were extracted using water-based methodologies (i.e., (1) hydration at room temperature; (2) stirring at 90 °C; and (3) centrifugation at 40 °C) for production of sustainable food gels. The potential use of these extracts as bioinks was assessed employing an extrusion-based 3D printer. The present work aimed to study the gelation process, taken place during printing, and assess the effectiveness of the selected green extraction method in producing gels. To improve the definition of the printed gel, two critical printing parameters were investigated: the addition of locust bean gum (LBG) at different concentrations (0, 0.5, 1, 1.5, 2, and 2.5%) and printing temperature (30, 40, 60, and 80 °C). Rheological results from a controlled-stress rheometer indicated that gels derived from G. corneum and G. gracilis exhibited a lower gel strength (lower G′ and G″) and excessive material spreading during deposition (lower viscosity) than C. crispus. Thus, G′ was around 5 and 70 times higher for C. crispus gels than for G. corneum and G. gracilis, respectively. When increasing LBG concentration (0.5 to 2.5% w/w) and lowering the printing temperature (80 to 30 °C), an enhanced gel matrix definition for G. corneum and G. gracilis gels was found. In contrast, gels from C. crispus demonstrated greater stability and were less influenced by these parameters, showcasing the potential of the seaweed to develop sustainable clean label food gels. Eventually, these results highlight the feasibility of using algal-based extracts obtained through a green procedure as bioinks where LBG was employed as a synergic ingredient.
]]>Gels doi: 10.3390/gels10030165
Authors: Ivelina Ivanova Marta Slavkova Teodora Popova Borislav Tzankov Denitsa Stefanova Virginia Tzankova Diana Tzankova Ivanka Spassova Daniela Kovacheva Christina Voycheva
Agar, a naturally occurring polysaccharide, has been modified by grafting it with acrylic (AcA) and methacrylic (McA) acid monomers, resulting in acrylic or methacrylic acid grafted polymer (AA-g-AcA or AA-g-McA) with pH-sensitive swelling behavior. Different ratios between agar, monomers, and initiator were applied. The synthesized grades of both new polymer series were characterized using FTIR spectroscopy, NMR, TGA, DSC, and XRD to ascertain the intended grafting. The percentage of grafting (% G), grafting efficiency (% GE), and % conversion (% C) were calculated, and models with optimal characteristics were further characterized. The swelling behavior of the newly synthesized polymers was studied over time and in solutions with different pH. These polymers were subsequently crosslinked with varying amounts of glutaraldehyde to obtain 5-fluorouracil-loaded nanogels. The optimal ratios of polymer, drug, and crosslinker resulted in nearly 80% loading efficiency. The performed physicochemical characterization (TEM and DLS) showed spherical nanogels with nanometer sizes (105.7–250 nm), negative zeta potentials, and narrow size distributions. According to FTIR analysis, 5-fluorouracil was physically incorporated. The swelling and release behavior of the prepared nanogels was pH-sensitive, favoring the delivery of the chemotherapeutic to tumor cells. The biocompatibility of the proposed nanocarrier was proven using an in vitro hemolysis assay.
]]>Gels doi: 10.3390/gels10030164
Authors: Umu S. Jalloh Arielle Gsell Kirstene A. Gultian James MacAulay Abigail Madden Jillian Smith Luke Siri Sebastián L. Vega
Hydrogels are a class of soft biomaterials and the material of choice for a myriad of biomedical applications due to their biocompatibility and highly tunable mechanical and biochemical properties. Specifically, light-mediated thiol-norbornene click reactions between norbornene-modified macromers and di-thiolated crosslinkers can be used to form base hydrogels amenable to spatial biochemical modifications via subsequent light reactions between pendant norbornenes in the hydrogel network and thiolated peptides. Macromers derived from natural sources (e.g., hyaluronic acid, gelatin, alginate) can cause off-target cell signaling, and this has motivated the use of synthetic macromers such as poly(ethylene glycol) (PEG). In this study, commercially available 8-arm norbornene-modified PEG (PEG-Nor) macromers were reacted with di-thiolated crosslinkers (dithiothreitol, DTT) to form synthetic hydrogels. By varying the PEG-Nor weight percent or DTT concentration, hydrogels with a stiffness range of 3.3 kPa–31.3 kPa were formed. Pendant norbornene groups in these hydrogels were used for secondary reactions to either increase hydrogel stiffness (by reacting with DTT) or to tether mono-thiolated peptides to the hydrogel network. Peptide functionalization has no effect on bulk hydrogel mechanics, and this confirms that mechanical and biochemical signals can be independently controlled. Using photomasks, thiolated peptides can also be photopatterned onto base hydrogels, and mesenchymal stem cells (MSCs) attach and spread on RGD-functionalized PEG-Nor hydrogels. MSCs encapsulated in PEG-Nor hydrogels are also highly viable, demonstrating the ability of this platform to form biocompatible hydrogels for 2D and 3D cell culture with user-defined mechanical and biochemical properties.
]]>Gels doi: 10.3390/gels10030163
Authors: Giuseppe Proietto Salanitri Enrica Luzzi Daniele Caretti Tommaso Mecca Sabrina C. Carroccio Andrea A. Scamporrino
The investigation of the mechanical, thermal, and adsorption properties of hydroxyethyl methacrylate (HEMA) cryogels as a function of a reactant ratio is herein reported to better address materials for specific applications. To this aim, cryogels have been synthesized using different monomer/crosslinker (N,N′-methylene-bisacrylamide–MBAA) ratios. The study of SEM images made it possible to identify the trend in the material’s macroporosity. As would be expected, the average measured pore width decreased as the amount of MBAA increased while the number of pores grew. Swelling capacity ranges from 8.7 gW/ggel (grams of water per gram of gel) to 9.3 gW/ggel. These values are strictly connected with the pore’s size and distribution, revealing that the water uptake for the most crosslinked sample is inferior to other samples. The equilibrium-adsorption capacity (Qe) towards the methylene violet (MV) was also assessed, revealing no remarkable differences after 24 h of a batch test. As expected, thermogravimetric analysis (TGA) also showed no significant changes in stability that ranged from a maximum weight loss temperature (T Max) of 420 °C to 425 °C, which increased as a function of crosslinker content. Conversely, compression strength measurements showed a notable difference of about 50% in modulus (Ec), moving from the higher to the lower HEMA/MBAA ratio. These new comparative results indicate how slight variations in the reactant’s ratio can steadily improve the mechanical properties of the HEMA cryogel without affecting its adsorption efficiency. This can be helpful in the design of materials for water and energy purposes. Since swelling properties are needed in the case of biomedical applications, the HEMA/MBAA ratio should be tuned versus high values.
]]>Gels doi: 10.3390/gels10030162
Authors: Shutong Du Xiaohu Zhou Bo Zheng
Extracellular vesicles (EVs), especially exosomes, have shown great therapeutic potential in the treatment of diseases, as they can target cells or tissues. However, the therapeutic effect of EVs is limited due to the susceptibility of EVs to immune system clearance during transport in vivo. Hydrogels have become an ideal delivery platform for EVs due to their good biocompatibility and porous structure. This article reviews the preparation and application of EVs-loaded hydrogels as a cell-free therapy strategy in the treatment of diseases. The article also discusses the challenges and future outlook of EVs-loaded hydrogels.
]]>Gels doi: 10.3390/gels10030161
Authors: Monika Jokubaite Mindaugas Marksa Kristina Ramanauskiene
In situ poloxamer-based gels are increasingly being explored as ocular drug delivery carriers to extend the release of active substances, thereby enhancing bioavailability. The objective of this study was to develop thermally stable in situ gels incorporating balsam poplar bud extract, propolis extract, and p-coumaric acid solution and to evaluate the physicochemical parameters of these gelified eye drops. This research assessed the compatibility of poloxamer-based eye drops with active components, their physicochemical properties, stability post-sterilization and during storage, and the release profiles of the active compounds. Fifteen eye drop formulations were prepared and categorized into three groups based on active components. One of the active components was propolis extract. As an alternative to propolis, eye drops containing the plant precursor, balsam poplar bud extract, were developed. The third group’s active component was p-coumaric acid, a dominant phenolic acid in propolis and balsam poplar bud extracts. The study reported phenolic contents of 76.63 CAE mg/g for propolis and 83.25 CAE mg/g for balsam poplar bud aqueous extracts, with balsam poplar bud extracts showing higher SPF values (14.0) compared to propolis (12.7), while p-coumaric acid solution exhibited the highest SPF values (25.5). All eye drops were transparent, with pH values meeting the requirements for ocular drops. Formulations containing 8–10% poloxamer 407 met the criteria for in situ gels. All formulations remained stable for 90 days. Conclusion: The study results indicate that the formulated gels possess suitable physicochemical properties, are resistant to applied autoclaving conditions, and exhibit an extended release of active compounds with an increase in poloxamer content.
]]>Gels doi: 10.3390/gels10030160
Authors: Rui Sun Qiang Xia Yufeng Sun
The objective of the present study was to develop and evaluate NLC–chitosan hydrogel beads for topical administration. The feasibility of the preparation technology was verified by investigating various formulation factors and the impact of chitosan hydrogel beads on the NLC. The encapsulation efficiency of NLC–chitosan hydrogel beads was above 95% in optimized process conditions. The physical characterization of the NLC–chitosan hydrogel beads showed that the NLC was distributed within the network of the chitosan hydrogel beads. Furthermore, the incorporation of NLC into the chitosan hydrogel beads was related to the electrostatic interaction between the surface of the NLC and chitosan, which influenced the lipid ordering degree of the NLC and contributed to the stability. The stability studies showed that the retention rate of quercetin in the NLC–chitosan hydrogel beads was 88.63 ± 2.57% after 10 months of storage under natural daylight. An in vitro permeation study showed that NLC–chitosan hydrogel beads exhibited superior ability in enhancing skin permeation by hydrophobic active ingredients compared to the NLC and significantly increased skin accumulation. These studies demonstrated that the use of NLC–chitosan hydrogel beads might be a promising strategy for the delivery of hydrophobic active ingredients in topical administration.
]]>Gels doi: 10.3390/gels10030159
Authors: Magdalena Blachnio Malgorzata Zienkiewicz-Strzalka
In this work, novel chitosan–silica hydrogels were synthesized and investigated by various complementary techniques. The hydrogels were obtained via the immobilization of chitosan (Ch) on the surface of mesoporous cellular foams (MCFs). The latter silica materials were obtained by a sol–gel process, varying the composition of the reaction mixture (copolymer Pluronic 9400 or Pluronic 10500) and the ageing temperature conditions (80 °C or 100 °C). The role of the silica phase in the hydrogels was the formation of a scaffold for the biopolymeric chitosan component and providing chemical, mechanical, and thermal stability. In turn, the chitosan phase enabled the binding of anionic pollutions from aqueous solutions based on electrostatic interaction mechanisms and hydrogen bonds. To provide information on structural, morphological, and surface properties of the chitosan–silica hydrogels, analyses such as the low-temperature adsorption/desorption of nitrogen, small-angle X-ray scattering (SAXS), scanning electron microscopy (SEM), atomic force microscopy (AFM), and Fourier-transform infrared spectroscopy (FTIR) were performed. Moreover, the verification of the utility of the chitosan–silica hydrogels as adsorbents for water and wastewater treatment was carried out based on kinetic and equilibrium studies of the Acid Red 88 (AR88) adsorption. Adsorption data were analyzed by applying various equations and discussed in terms of the adsorption on heterogeneous solid-surfaces theory. The adsorption mechanism for the AR88 dye–chitosan–silica hydrogel systems was proposed.
]]>Gels doi: 10.3390/gels10030158
Authors: Chengzhi Zhang Jiale Wang Hao Wu Wenhui Fan Siyu Li Dong Wei Zongming Song Ye Tao
Age-related macular degeneration (AMD) is an ocular disease that leads to progressive photoreceptor death and visual impairment. Currently, the most common therapeutic strategy is to deliver anti-vascular endothelial growth factor (anti-VEGF) agents into the eyes of patients with wet AMD. However, this treatment method requires repeated injections, which potentially results in surgical complications and unwanted side effects for patients. An effective therapeutic approach for dry AMD also remains elusive. Therefore, there is a surge of enthusiasm for the developing the biodegradable drug delivery systems with sustained release capability and develop a promising therapeutic strategy. Notably, the strides made in hydrogels which possess intricate three-dimensional polymer networks have profoundly facilitated the treatments of AMD. Researchers have established diverse hydrogel-based delivery systems with marvelous biocompatibility and efficacy. Advantageously, these hydrogel-based transplantation therapies provide promising opportunities for vision restoration. Herein, we provide an overview of the properties and potential of hydrogels for ocular delivery. We introduce recent advances in the utilization of hydrogels for the delivery of anti-VEGF and in cell implantation. Further refinements of these findings would lay the basis for developing more rational and curative therapies for AMD.
]]>Gels doi: 10.3390/gels10030157
Authors: Igor D. Zlotnikov Alexander A. Ezhov Natalia V. Dobryakova Elena V. Kudryashova
We have developed a micellar formulation of anticancer drugs based on chitosan and heparin grafted with lipoic and oleic acids that can release the cytotoxic cargo (doxorubicin) in response to external stimuli, such as increased glutathione concentration—a hallmark of cancer. Natural polysaccharides (heparin and chitosan) provide the pH sensitivity of the nanocarrier: the release of doxorubicin (Dox) is enhanced in a slightly acidic environment (tumor microenvironment). Fatty acid residues are necessary for the formation of nanoparticles (micelles) and solubilization of cytostatics in a hydrophobic core. Lipoic acid residues provide the formation of a labile S-S cross-linking between polymer chains (the first variant) or covalently attached doxorubicin molecules through glutathione-sensitive S-S bridges (the second variant)—both determine Redox sensitivity of the anticancer drugs carriers stable in blood circulation and disintegrate after intracellular uptake in the tumor cells. The release of doxorubicin from micelles occurs slowly (20%/6 h) in an environment with a pH of 7.4 and the absence of glutathione, while in a slightly acidic environment and in the presence of 10 mM glutathione, the rate increases up to 6 times, with an increase in the effective concentration up to 5 times after 7 h. The permeability of doxorubicin in micellar formulations (covalent S-S cross-linked and not) into Raji, K562, and A875 cancer cells was studied using FTIR, fluorescence spectroscopy and confocal laser scanning microscopy (CLSM). We have shown dramatically improved accumulation, decreased efflux, and increased cytotoxicity compared to doxorubicin control with three tumor cell lines: Raji, K562, and A875. At the same time, cytotoxicity and permeability for non-tumor cells (HEK293T) are significantly lower, increasing the selectivity index against tumor cells by several times.
]]>Gels doi: 10.3390/gels10030156
Authors: Katya Kamenova Anna Prancheva Stiliyana Stoyanova Lyubomira Radeva Ivanka Pencheva-El Tibi Krassimira Yoncheva Martin A. Ravutsov Maya K. Marinova Svilen P. Simeonov Simona Mitova Rumyana Eneva Maya M. Zaharieva Hristo Najdenski Petar D. Petrov
Hydrogels are superior wound dressings because they can provide protection and hydration of the wound, as well as the controlled release of therapeutic substances to aid tissue regeneration and the healing process. Hydrogels obtained from natural precursors are preferred because of their low cost, biocompatibility, and biodegradability. We describe the synthesis of novel functional hydrogels based on two natural products—citric acid (CA) and pentane-1,2,5-triol (PT, a product from lignocellulose processing) and poly(ethylene glycol) (PEG-600)—via an environment friendly approach. The hydrogels were prepared via monomer crosslinking through a polycondensation reaction at an elevated temperature in the absence of any solvent. The reagents were blended at three different compositions with molar ratios of hydroxyl (from PT and PEG) to carboxyl (from CA) groups of 1:1, 1:1.4, and 1.4:1, respectively. The effect of the composition on the physicomechanical properties of materials was investigated. All hydrogels exhibited pH-sensitive behavior, while the swelling degree and elastic modulus were dependent on the composition of the polymer network. The proteolytic enzyme serratiopeptidase (SER) was loaded into a hydrogel via physical absorption as a model drug. The release profile of SER and the effects of the enzyme on healthy skin cells were assessed. The results showed that the hydrogel carrier could provide the complete release of the loaded enzyme.
]]>Gels doi: 10.3390/gels10030155
Authors: Badr Bahloul Enis Ben Bnina Assia Hamdi Luis Castillo Henríquez Dhaou Baccar Nesrine Kalboussi Aïmen Abbassi Nathalie Mignet Guido Flamini José Roberto Vega-Baudrit
This study explores a nanoemulsion (NE)-based gel incorporating Tunisian Pituranthos tortuosus essential oil, with a focus on its wound-healing potential. The essential oil, extracted via hydrodistillation, underwent GC-MS analysis for compositional verification. The physicochemical characterization included dynamic light scattering (DLS), transmission electron microscopy (TEM), zeta potential measurement, pH, and viscosity. The gelification of the NE facilitated topical application. The results revealed an average extraction yield of 0.45% and identified 38 compounds in the essential oil. The NE exhibited a particle size of 27 ± 0.4 nm, a polydispersity index (PDI) of 0.3, and a zeta potential of −22.8 ± 1.4 mV. The stability of the gelified preparation was confirmed through thermodynamic stability studies, TEM observations, and zeta and size results. In vivo experiments confirmed significant wound-healing effects, highlighting the promising role of the NE-based gel in healthcare advancements. This research underscores the potential of novel phyto-based delivery systems in wound care.
]]>Gels doi: 10.3390/gels10030154
Authors: Gabrijela Horvat Uroš Maver
Aerogels are unique solid materials that consist mainly of air and have an extremely low density, large open pores, and a large internal surface area [...]
]]>Gels doi: 10.3390/gels10020153
Authors: Alexander Trifonov Ahmer Shehzad Fariza Mukasheva Muhammad Moazzam Dana Akilbekova
Terminology is pivotal for facilitating clear communication and minimizing ambiguity, especially in specialized fields such as chemistry. In materials science, a subset of chemistry, the term “pore” is traditionally linked to the International Union of Pure and Applied Chemistry (IUPAC) nomenclature, which categorizes pores into “micro”, “meso”, and “macro” based on size. However, applying this terminology in closely-related areas, such as 3D bioprinting, often leads to confusion owing to the lack of consensus on specific definitions and classifications tailored to each field. This review article critically examines the current use of pore terminology in the context of 3D bioprinting, highlighting the need for reassessment to avoid potential misunderstandings. We propose an alternative classification that aligns more closely with the specific requirements of bioprinting, suggesting a tentative size-based division of interconnected pores into ‘parvo’-(d < 25 µm), ‘medio’-(25 < d < 100 µm), and ‘magno’-(d > 100 µm) pores, relying on the current understanding of the pore size role in tissue formation. The introduction of field-specific terminology for pore sizes in 3D bioprinting is essential to enhance the clarity and precision of research communication. This represents a step toward a more cohesive and specialized lexicon that aligns with the unique aspects of bioprinting and tissue engineering.
]]>Gels doi: 10.3390/gels10020152
Authors: Jeong Yeon Choi Yong-Joon Joo Ri Jin Kang Hee Kyung Jeon Gyeong Sik Hong
Immediate burn wound care is a critical factor influencing the outcomes of burn treatment. In this study, we developed a spray-type alginate hydrogel dressing that promotes wound healing, reduces pain, and increases the convenience of use in a burn treatment emergency. We investigated the efficiency of newly developed spray-type alginate hydrogel dressing on the wound healing process. We investigated the efficacy of the alginate hydrogel dressing for wound healing in 30 Sprague Dawley rats. Four deep, round second-degree burn wounds (diameter, 1.5 cm) were created bilaterally on the dorsum of the rat’s trunk; the rats were divided into four groups, in which different dressing materials were applied as follows: group A, gauze (control); group B, Mepilex™ (control); group C, 2.25% alginate hydrogel; and group D, 2.5% alginate hydrogel. The gross findings of each group were compared by tracing the remaining wound and performing visual and histological observations and biochemical analysis for proteins associated with wound healing at each time period. In burn wounds, groups C and D showed significantly higher contraction, epithelialization, and healing rates. Histologically, groups C and D showed an improved arrangement of collagen fibers and a thick epithelial layer 14 days after initial wound formation. Group C showed higher CD31, TGF-β, and fibronectin expression in Western blot analyses after day 14. This study suggests that the spray-type alginate hydrogel dressing is an effective material for initial burn wound care.
]]>Gels doi: 10.3390/gels10020151
Authors: Rongjun Ye Lei Wang Wenjun Xu Jianpeng Zhang Zhengbang Chen
To address the issue of ineffective injection resulting from the consistent channeling of injected water through highly permeable channels in ultra-deep, high-temperature, high-salinity, and strongly heterogeneous reservoirs during the production process, a gel particle profile control agent suitable for high-temperature and high-salinity conditions was chosen. With the help of the glass etching visual microscopic model and the heterogeneous long core model, the formation mechanism of a water flooding channeling path and the distribution law of the remaining oil were explored, the microscopic profile control mechanism of the different parameters was clarified, and the profile control effect of macroscopic core displacement was analyzed. The research shows that the formation mechanism of a water flooding channeling path is dominated by the distribution law of the permeability section and the connection mode between different penetration zones. The remaining oil types after water flooding are mainly contiguous block, parallel throats, and multi-branch clusters. The profile control effect of gel particles on reservoir vertical heterogeneity is better than that of reservoir lateral heterogeneity. It was found that 10 wt% submicron particles with a median diameter of 600 nm play a good role in profiling and plugging pores of 5–20 μm. In addition, 10 wt% micron-sized particles with a median diameter of 2.63 μm mainly play a strong plugging role in the pores of 20–30 μm, and 5 wt% micron-sized particles with a median diameter of 2.63 μm mainly form a weak plugging effect on the pores of 10–20 μm. The overall profile control effect of 10 wt% submicro particles is the best, and changes in concentration parameters have a more significant effect on the profile control effect. In the macroscopic core profile control, enhanced oil recovery (EOR) can reach 16%, and the gel particles show plugging, deformation migration, and re-plugging. The research results provide theoretical guidance for tapping the potential of the remaining oil in strong heterogeneous reservoirs. To date, the gel particles have been applied in the Tahe oilfield and have produced an obvious profile control effect; the oil production has risen to the highest value of 26.4 t/d, and the comprehensive water content has fallen to the lowest percentage of 32.1%.
]]>Gels doi: 10.3390/gels10020150
Authors: Erica Sonaglia Emily Schifano Mohammad Sharbaf Daniela Uccelletti Anna Candida Felici Maria Laura Santarelli
Cultural heritage stone materials frequently experience significant discoloration induced by copper corrosion products, especially calcareous stones associated with bronze or copper statues and architectural elements. This alteration originates from the corrosion of unprotected copper, resulting in the formation of various Cu minerals and the migration of soluble ions to adjacent stone materials. Traditional cleaning methods involve mechanical, chemical, and laser techniques, which are generally time-consuming, costly, not ecological, or can possibly damage original materials. The loading of highly effective chelating agents, such as ethylenediaminetetraacetic acid (EDTA), into hydrogels has recently been exploited. However, the preference for synthetic hydrogels has been prominent until now, although they lack renewability and biodegradability and require high costs. This study explores for the first time the potential to clean copper corrosion with bacterial nanocellulose (BC) loaded with EDTA as a biologically based, sustainable, and biodegradable hydrogel. The BC hydrogel was characterised by field emission–scanning electron microscopy (FE–SEM), X-ray diffraction analysis (XRD), attenuated total reflectance–Fourier transform infrared spectroscopy (ATR–FTIR), simultaneous thermal analysis (TG-DSC), and tensile testing. It revealed a nano-fibrous structure with high crystallinity and purity and mechanical properties suitable for cultural heritage applications. The EDTA-loaded hydrogel effectively removed copper stains from marble after 120 min of application. Micro-Raman and colorimetric analyses assessed the cleaning efficacy. The study introduces bacterial nanocellulose as a green and effective alternative for heritage conservation, aligning with sustainable methodologies in stone conservation.
]]>Gels doi: 10.3390/gels10020149
Authors: Camila Folle Natalia Díaz-Garrido Mireia Mallandrich Joaquim Suñer-Carbó Elena Sánchez-López Lyda Halbaut Ana M. Marqués Marta Espina Josefa Badia Laura Baldoma Ana Cristina Calpena Maria Luisa García
Thyme oil (THO) possesses excellent antibacterial and antioxidant properties which are suitable for skin inflammatory disorders such as acne vulgaris. However, THO is insoluble in water and its components are highly volatile. Therefore, these drawbacks may be overcome by its encapsulation in biodegradable PLGA nanoparticles (THO-NPs) that had been functionalized using several strategies. Moreover, cell viability was studied in HaCat cells, confirming their safety. In order to assess therapeutic efficacy against acne, bacterial reduction capacity and antioxidant properties were assessed. Moreover, the anti-inflammatory and wound-healing abilities of THO-NPs were also confirmed. Additionally, ex vivo antioxidant assessment was carried out using pig skin, demonstrating the suitable antioxidant properties of THO-NPs. Moreover, THO and THO-NPs were dispersed in a gelling system, and stability, rheological properties, and extensibility were assessed. Finally, the biomechanical properties of THO-hydrogel and THO-NP-hydrogel were studied in human volunteers, confirming the suitable activity for the treatment of acne. As a conclusion, THO has been encapsulated into PLGA NPs, and in vitro, ex vivo, and in vivo assessments had been carried out, demonstrating excellent properties for the treatment of inflammatory skin disorders.
]]>Gels doi: 10.3390/gels10020148
Authors: Xuyang Shi Shuzhao Chen Qiang Wang Yijun Lu Shisong Ren Jiandong Huang
As an environmentally responsible alternative to conventional concrete, geopolymer concrete recycles previously used resources to prepare the cementitious component of the product. The challenging issue with employing geopolymer concrete in the building business is the absence of a standard mix design. According to the chemical composition of its components, this work proposes a thorough system or framework for estimating the compressive strength of fly ash-based geopolymer concrete (FAGC). It could be possible to construct a system for predicting the compressive strength of FAGC using soft computing methods, thereby avoiding the requirement for time-consuming and expensive experimental tests. A complete database of 162 compressive strength datasets was gathered from the research papers that were published between the years 2000 and 2020 and prepared to develop proposed models. To address the relationships between inputs and output variables, long short-term memory networks were deployed. Notably, the proposed model was examined using several soft computing methods. The modeling process incorporated 17 variables that affect the CSFAG, such as percentage of SiO2 (SiO2), percentage of Na2O (Na2O), percentage of CaO (CaO), percentage of Al2O3 (Al2O3), percentage of Fe2O3 (Fe2O3), fly ash (FA), coarse aggregate (CAgg), fine aggregate (FAgg), Sodium Hydroxide solution (SH), Sodium Silicate solution (SS), extra water (EW), superplasticizer (SP), SH concentration, percentage of SiO2 in SS, percentage of Na2O in SS, curing time, curing temperature that the proposed model was examined to several soft computing methods such as multi-layer perception neural network (MLPNN), Bayesian regularized neural network (BRNN), generalized feed-forward neural networks (GFNN), support vector regression (SVR), decision tree (DT), random forest (RF), and LSTM. Three main innovations of this study are using the LSTM model for predicting FAGC, optimizing the LSTM model by a new evolutionary algorithm called the marine predators algorithm (MPA), and considering the six new inputs in the modeling process, such as aggregate to total mass ratio, fine aggregate to total aggregate mass ratio, FASiO2:Al2O3 molar ratio, FA SiO2:Fe2O3 molar ratio, AA Na2O:SiO2 molar ratio, and the sum of SiO2, Al2O3, and Fe2O3 percent in FA. The performance capacity of LSTM-MPA was evaluated with other artificial intelligence models. The results indicate that the R2 and RMSE values for the proposed LSTM-MPA model were as follows: MLPNN (R2 = 0.896, RMSE = 3.745), BRNN (R2 = 0.931, RMSE = 2.785), GFFNN (R2 = 0.926, RMSE = 2.926), SVR-L (R2 = 0.921, RMSE = 3.017), SVR-P (R2 = 0.920, RMSE = 3.291), SVR-S (R2 = 0.934, RMSE = 2.823), SVR-RBF (R2 = 0.916, RMSE = 3.114), DT (R2 = 0.934, RMSE = 2.711), RF (R2 = 0.938, RMSE = 2.892), LSTM (R2 = 0.9725, RMSE = 1.7816), LSTM-MPA (R2 = 0.9940, RMSE = 0.8332), and LSTM-PSO (R2 = 0.9804, RMSE = 1.5221). Therefore, the proposed LSTM-MPA model can be employed as a reliable and accurate model for predicting CSFAG. Noteworthy, the results demonstrated the significance and influence of fly ash and sodium silicate solution chemical compositions on the compressive strength of FAGC. These variables could adequately present variations in the best mix designs discovered in earlier investigations. The suggested approach may also save time and money by accurately estimating the compressive strength of FAGC with low calcium content.
]]>Gels doi: 10.3390/gels10020147
Authors: Olga Kammona Evgenia Tsanaktsidou Costas Kiparissides
Wound healing is a physiological process occurring after the onset of a skin lesion aiming to reconstruct the dermal barrier between the external environment and the body. Depending on the nature and duration of the healing process, wounds are classified as acute (e.g., trauma, surgical wounds) and chronic (e.g., diabetic ulcers) wounds. The latter take several months to heal or do not heal (non-healing chronic wounds), are usually prone to microbial infection and represent an important source of morbidity since they affect millions of people worldwide. Typical wound treatments comprise surgical (e.g., debridement, skin grafts/flaps) and non-surgical (e.g., topical formulations, wound dressings) methods. Modern experimental approaches include among others three dimensional (3D)-(bio)printed wound dressings. The present paper reviews recently developed 3D (bio)printed hydrogels for wound healing applications, especially focusing on the results of their in vitro and in vivo assessment. The advanced hydrogel constructs were printed using different types of bioinks (e.g., natural and/or synthetic polymers and their mixtures with biological materials) and printing methods (e.g., extrusion, digital light processing, coaxial microfluidic bioprinting, etc.) and incorporated various bioactive agents (e.g., growth factors, antibiotics, antibacterial agents, nanoparticles, etc.) and/or cells (e.g., dermal fibroblasts, keratinocytes, mesenchymal stem cells, endothelial cells, etc.).
]]>Gels doi: 10.3390/gels10020146
Authors: Minsik Lee Seonyeong Noh Jun-Bong Shin Jungwon Kwak Chiyoung Jeong
Accurate dosimetric verification is becoming increasingly important in radiotherapy. Although polymer gel dosimetry may be useful for verifying complex 3D dose distributions, it has limitations for clinical application due to its strong reactivity with oxygen and other contaminants. Therefore, it is important that the material of the gel storage container blocks reaction with external contaminants. In this study, we tested the effect of air and the chemical permeability of various polymer-based 3D printing materials that can be used as gel containers. A methacrylic acid, gelatin, and tetrakis (hydroxymethyl) phosphonium chloride gel was used. Five types of printing materials that can be applied to the fused deposition modeling (FDM)-type 3D printer were compared: acrylonitrile butadiene styrene (ABS), co-polyester (CPE), polycarbonate (PC), polylactic acid (PLA), and polypropylene (PP) (reference: glass vial). The map of R2 (1/T2) relaxation rates for each material, obtained from magnetic resonance imaging scans, was analyzed. Additionally, response histograms and dose calibration curves from the R2 map were evaluated. The R2 distribution showed that CPE had sharper boundaries than the other materials, and the profile gradient of CPE was also closest to the reference vial. Histograms and dose calibration showed that CPE provided the most homogeneous and the highest relative response of 83.5%, with 8.6% root mean square error, compared with the reference vial. These results indicate that CPE is a reasonable material for the FDM-type 3D printing gel container.
]]>Gels doi: 10.3390/gels10020145
Authors: Preetham Yerra Mario Migliario Sarah Gino Maurizio Sabbatini Monica Bignotto Marco Invernizzi Filippo Renò
Background: Gelatin–xanthan gum (Gel–Xnt) hydrogel has been previously modified to improve its printability; now, to increase its ability for use as cell-laden 3D scaffolds (bioink), polydopamine (PDA), a biocompatible, antibacterial, adhesive, and antioxidant mussel-inspired biopolymer, has been added (1–3% v/v) to hydrogel. Methods: Control (CT) and PDA-blended hydrogels were used to print 1 cm2 grids. The hydrogels’ printability, moisture, swelling, hydrolysis, and porosity were tested after glutaraldehyde (GTA) crosslinking, while biocompatibility was tested using primary human-derived skin fibroblasts and spontaneously immortalized human keratinocytes (HaCaT). Keratinocyte or fibroblast suspension (100 µL, 2.5 × 105 cells) was combined with an uncrosslinked CT and PDA blended hydrogel to fabricate cylinders (0.5 cm high, 1 cm wide). These cylinders were then cross-linked and incubated for 1, 3, 7, 14, and 21 days. The presence of cells within various hydrogels was assessed using optical microscopy. Results and discussion: PDA blending did not modify the hydrogel printability or physiochemical characteristics, suggesting that PDA did not interfere with GTA crosslinking. On the other hand, PDA presence strongly accelerated and increased both fibroblast and keratinocyte growth inside. This effect seemed to be linked to the adhesive abilities of PDA, which improve cell adhesion and, in turn, proliferation. Conclusions: The simple PDA blending method described could help in obtaining a new bioink for the development of innovative 3D-printed wound dressings.
]]>Gels doi: 10.3390/gels10020144
Authors: Juan Cao Bo Wu Ping Yuan Yeqi Liu Cheng Hu
Conductive hydrogels, characterized by their excellent conductivity and flexibility, have attracted widespread attention and research in the field of flexible wearable sensors. This paper reviews the application progress, related challenges, and future prospects of conductive hydrogels in flexible wearable sensors. Initially, the basic properties and classifications of conductive hydrogels are introduced. Subsequently, this paper discusses in detail the specific applications of conductive hydrogels in different sensor applications, such as motion detection, medical diagnostics, electronic skin, and human–computer interactions. Finally, the application prospects and challenges are summarized. Overall, the exceptional performance and multifunctionality of conductive hydrogels make them one of the most important materials for future wearable technologies. However, further research and innovation are needed to overcome the challenges faced and to realize the wider application of conductive hydrogels in flexible sensors.
]]>Gels doi: 10.3390/gels10020143
Authors: Ezgi Altınay Fatma Zehra Köse Sezen Canım Ateş Kadriye Kızılbey
In contrast to conventional drug delivery systems, controlled drug release systems employ distinct methodologies. These systems facilitate the release of active substances in predetermined quantities and for specified durations. Polymer hydrogels have gained prominence in controlled drug delivery because of their unique swelling–shrinkage behavior and ability to regulate drug release. In this investigation, films with a hydrogel structure were crafted using polyvinyl alcohol, a biocompatible polymer, and silver nanoparticles. Following characterization, ibuprofen was loaded into the hydrogels to evaluate their drug release capacity. The particle sizes of silver nanoparticles synthesized using a green approach were determined. This study comprehensively examined the structural properties, morphological features, mechanical strength, and cumulative release patterns of the prepared films. In vitro cytotoxicity analysis was employed to assess the cell viability of drug-loaded hydrogel films, and their antibacterial effects were examined. The results indicated that hydrogel films containing 5% and 10% polyvinyl alcohol released 89% and 97% of the loaded drug, respectively, by day 14. The release kinetics fits the Korsmeyer–Peppas model. This study, which describes nanoparticle-enhanced polyvinyl alcohol hydrogel systems prepared through a cost-effective and environmentally friendly approach, is anticipated to contribute to the existing literature and serve as a foundational study for future research.
]]>Gels doi: 10.3390/gels10020142
Authors: Xiaochun Yin Pei Xu Huiyao Wang
The presence of organic dyes and heavy metal ions in water sources poses a significant threat to human health and the ecosystem. In this study, hydrogel adsorbents for water pollution remediation were synthesized using Guipi residue (GP), a cellulose material from Chinese herbal medicine, and chitosan (CTS) through radical polymerization with acrylamide (AM) and acrylic acid (AA). The characteristics of the hydrogels were analyzed from a physicochemical perspective, and their ability to adsorb was tested using model pollutants such as Pb2+, Cd2+, Rhodamine B (RhB), and methyl orange (MO). The outcomes revealed that GP/CTS/AA-co-AM, which has improved mechanical attributes, effectively eliminated these pollutants. At a pH of 4.0, a contact duration of 120 min, and an initial concentration of 600 mg/L for Pb2+ and 500 mg/L for Cd2+, the highest adsorption capabilities were 314.6 mg/g for Pb2+ and 289.1 mg/g for Cd2+. Regarding the dyes, the GP/CTS/AA-co-AM hydrogel displayed adsorption capacities of 106.4 mg/g for RhB and 94.8 mg/g for MO, maintaining a stable adsorption capacity at different pHs. Compared with other competitive pollutants, GP/CTS/AA-co-AM demonstrated a higher absorption capability, mainly targeted toward Pb2+. The adsorption processes for the pollutants conformed to pseudo-second-order kinetics models and adhered to the Langmuir models. Even after undergoing five consecutive adsorption and desorption cycles, the adsorption capacities for heavy metals and dyes remained above 70% and 80%. In summary, this study effectively suggested the potential of the innovative GP/CTS/AA-co-AM hydrogel as a practical and feasible approach for eliminating heavy metals and dyes from water solutions.
]]>Gels doi: 10.3390/gels10020141
Authors: Ju-Qi Ruan Kai-Yue Xie Jun-Nan Wan Qing-Yuan Chen Xiaoqing Zuo Xiaodong Li Xiaodong Wu Chunlong Fei Shanshan Yao
Cellulose aerogels have great prospects for noise reduction applications due to their sustainable value and superior 3D interconnected porous structures. The drying principle is a crucial factor in the preparation process for developing high-performance aerogels, particularly with respect to achieving high acoustic absorption properties. In this study, multifunctional cellulose nanocrystal (CNC) aerogels were conveniently prepared using two distinct freeze-drying principles: refrigerator conventional freezing (RCF) and liquid nitrogen unidirectional freezing (LnUF). The results indicate that the rapid RCF process resulted in a denser CNC aerogel structure with disordered larger pores, causing a stronger compressive performance (Young’s modulus of 40 kPa). On the contrary, the LnUF process constructed ordered structures of CNC aerogels with a lower bulk density (0.03 g/cm3) and smaller apertures, resulting in better thermal stability, higher diffuse reflection across visible light, and especially increased acoustic absorption performance at low–mid frequencies (600–3000 Hz). Moreover, the dissipation mechanism of sound energy in the fabricated CNC aerogels is predicted by a designed porous media model. This work not only paves the way for optimizing the performance of aerogels through structure control, but also provides a new perspective for developing sustainable and efficient acoustic absorptive materials for a wide range of applications.
]]>Gels doi: 10.3390/gels10020140
Authors: Mehdi Salar Amoli Resmi Anand Mostafa EzEldeen Liesbet Geris Reinhilde Jacobs Veerle Bloemen
While available treatments have addressed a variety of complications in the dentoalveolar region, associated challenges have resulted in exploration of tissue engineering techniques. Often, scaffold biomaterials with specific properties are required for such strategies to be successful, development of which is an active area of research. This study focuses on the development of a copolymer of poly (N-isopropylacrylamide) (pNIPAM) and chitosan, used for 3D printing of scaffolds for dentoalveolar regeneration. The synthesized material was characterized by Fourier transform infrared spectroscopy, and the possibility of printing was evaluated through various printability tests. The rate of degradation and swelling was analyzed through gravimetry, and surface morphology was characterized by scanning electron microscopy. Viability of dental pulp stem cells seeded on the scaffolds was evaluated by live/dead analysis and DNA quantification. The results demonstrated successful copolymerization, and three formulations among various synthesized formulations were successfully 3D printed. Up to 35% degradability was confirmed within 7 days, and a maximum swelling of approximately 1200% was achieved. Furthermore, initial assessment of cell viability demonstrated biocompatibility of the developed scaffolds. While further studies are required to achieve the tissue engineering goals, the present results tend to indicate that the proposed hydrogel might be a valid candidate for scaffold fabrication serving dentoalveolar tissue engineering through 3D printing.
]]>Gels doi: 10.3390/gels10020139
Authors: Yuichi Ohya Yasuyuki Yoshida Taiki Kumagae Akinori Kuzuya
Biodegradable injectable polymer (IP) systems that form hydrogels in situ when injected into the body have considerable potential as medical materials. In this paper, we report a new two-solution mixed biodegradable IP system that utilizes the stereocomplex (SC) formation of poly(l-lactide) (PLLA) and poly(d-lactide) (PDLA). We synthesized triblock copolymers of PLLA and poly(ethylene glycol), PLLA-b-PEG-b-PLLA (tri-L), and a graft copolymer of dextran (Dex) attached to a PDLA-b-PEG diblock copolymer, Dex-g-(PDLA-b-PEG) (gb-D). We found that a hydrogel can be obtained by mixing gb-D solution and tri-L solution via SC formation. Although it is already known that graft copolymers attached to enantiomeric PLLA and PDLA chains can form an SC hydrogel upon mixing, we revealed that hydrogels can also be formed by a combination of graft and triblock copolymers. In this system (graft vs. triblock), the gelation time was shorter, within 1 min, and the physical strength of the resulting hydrogel (G′ > 100 Pa) was higher than when graft copolymers were mixed. Triblock copolymers form micelles (16 nm in diameter) in aqueous solutions and hydrophobic drugs can be easily encapsulated in micelles. In contrast, graft copolymers have the advantage that their molecular weight can be set high, contributing to improved mechanical strength of the obtained hydrogel. Various biologically active polymers can be used as the main chains of graft copolymers, and chemical modification using the remaining functional side chain groups is also easy. Therefore, the developed mixing system with a graft vs. triblock combination can be applied to medical materials as a highly convenient, physically cross-linked IP system.
]]>Gels doi: 10.3390/gels10020138
Authors: Long Quan Xueqian Shi Jie Zhang Zhuju Shu Liang Zhou
A novel lignocellulosic aerogel, MT-LCA, was successfully prepared from MT by undergoing partial dissolution in an ionic liquid, coagulation in water, freezing in liquid nitrogen, and subsequent freeze-drying. The MT-LCA preserves its original honeycomb-like porous structure, and the newly formed micropores contribute to increased porosity and specific surface area. FT-IR analysis reveals that MT, after dissolution and coagulation, experiences no chemical reactions. However, a change in the crystalline structure of cellulose is observed, transitioning from cellulose I to cellulose II. Both MT and MT-LCA demonstrate a quasi-second-order kinetic process during methylene blue adsorption, indicative of chemical adsorption. The Langmuir model proves to be more appropriate for characterizing the methylene blue adsorption process. Both adsorbents exhibit monolayer adsorption, and their effective adsorption sites are uniformly distributed. The higher porosity, nanoscale micropores, and larger pore size in MT-LCA enhance its capillary force, providing efficient directional transport performance. Consequently, the prepared MT-LCA displays exceptional compressive performance and efficient directional transport capabilities, making it well-suited for applications requiring high compressive performance and selective directional transport.
]]>Gels doi: 10.3390/gels10020137
Authors: Francesco La Monica Simona Campora Giulio Ghersi
Chronic wounds, commonly known as ulcers, represent a significant challenge to public health, impacting millions of individuals every year and imposing a significant financial burden on the global health system. Chronic wounds result from the interruption of the natural wound-healing process due to internal and/or external factors, resulting in slow or nonexistent recovery. Conventional medical approaches are often inadequate to deal with chronic wounds, necessitating the exploration of new methods to facilitate rapid and effective healing. In recent years, regenerative medicine and tissue engineering have emerged as promising avenues to encourage tissue regeneration. These approaches aim to achieve anatomical and functional restoration of the affected area through polymeric components, such as scaffolds or hydrogels. This review explores collagen-based biomaterials as potential therapeutic interventions for skin chronic wounds, specifically focusing on infective and diabetic ulcers. Hence, the different approaches described are classified on an action-mechanism basis. Understanding the issues preventing chronic wound healing and identifying effective therapeutic alternatives could indicate the best way to optimize therapeutic units and to promote more direct and efficient healing.
]]>Gels doi: 10.3390/gels10020136
Authors: Jumana Rashid Mohammed Haroub Alshehhi Nisal Wanasingha Rajkamal Balu Jitendra Mata Kalpit Shah Naba K. Dutta Namita Roy Choudhury
Bioplastic films comprising both plant- and animal-derived proteins have the potential to integrate the optimal characteristics inherent to the specific domain, which offers enormous potential to develop polymer alternatives to petroleum-based plastic. Herein, we present a facile strategy to develop hybrid films comprised of both wheat gluten and wool keratin proteins for the first time, employing a ruthenium-based photocrosslinking strategy. This approach addresses the demand for sustainable materials, reducing the environmental impact by using proteins from renewable and biodegradable sources. Gluten film was fabricated from an alcohol–water mixture soluble fraction, largely comprised of gliadin proteins. Co-crosslinking hydrolyzed low-molecular-weight keratin with gluten enhanced its hydrophilic properties and enabled the tuning of its physicochemical properties. Furthermore, the hierarchical structure of the fabricated films was studied using neutron scattering techniques, which revealed the presence of both hydrophobic and hydrophilic nanodomains, gliadin nanoclusters, and interconnected micropores in the matrix. The films exhibited a largely (>40%) β-sheet secondary structure, with diminishing gliadin aggregate intensity and increasing micropore size (from 1.2 to 2.2 µm) with an increase in keratin content. The hybrid films displayed improved molecular chain mobility, as evidenced by the decrease in the glass-transition temperature from ~179.7 °C to ~173.5 °C. Amongst the fabricated films, the G14K6 hybrid sample showed superior water uptake (6.80% after 30 days) compared to the pristine G20 sample (1.04%). The suitability of the developed system for multilayer 3D printing has also been demonstrated, with the 10-layer 3D-printed film exhibiting >92% accuracy, which has the potential for use in packaging, agricultural, and biomedical applications.
]]>Gels doi: 10.3390/gels10020135
Authors: Tatjana Paulauskiene Egle Sirtaute Arturas Tadzijevas Jochen Uebe
Aerogels are an excellent alternative to traditional oil absorbents and are designed to remove oil or organic solvents from water. Cellulose-based aerogels can be distinguished as polymers that are non-toxic, environmentally friendly, and biodegradable. The compression measurement properties of aerogels are often evaluated using dry samples. Here, oil-soaked, hydrophobized cellulose aerogel samples were examined in comparison to dry samples with and without additional hemp fibers and various levels of starch for crosslinking. The samples were characterized by compression measurement properties and filmed to evaluate the regeneration of the sorbent with repeated use. Overall, the measurements of the mechanical properties for the dry samples showed good reproducibility. The Young’s modulus of samples with additional hemp fibers is significantly increased and also shows higher strength than samples without hemp fibers. However, samples without hemp fibers showed slightly better relaxation after compression. Oil acts as a weak plasticizer for all aerogel samples. However, it is important to note that the oil does not cause the samples to decompose in the way unmodified cellulose aerogels do in water. Therefore, using hydrophobized cellulose aerogels as sorbents for oil in a sea or harbor with swell means that they can be collected in their entirety even after use.
]]>Gels doi: 10.3390/gels10020134
Authors: Toshiaki Dobashi
Most industrial gels are prepared as apparently isotropic and homogeneous materials through a preparation process encompassing alterations in temperature, application of isotropic mechanical stress, exposure to high-energy electromagnetic waves, and mixing with cross-linkers (gelators) [...]
]]>Gels doi: 10.3390/gels10020133
Authors: Tatyana Kouznetsova Andrei Ivanets Vladimir Prozorovich Polina Shornikova Lizaveta Kapysh Qiang Tian László Péter László Trif László Almásy
Mesoporous materials containing heteroelements have a huge potential for use as catalysts, exchangers, and adsorbents due to their tunable nanometer-sized pores and exceptionally large internal surfaces accessible to bulky organic molecules. In the present work, ordered mesoporous silica containing Ni atoms as active sites was synthesized by a new low-temperature method of condensation of silica precursors on a micellar template from aqueous solutions in the presence of nickel salt. The homogeneity of the resulting product was achieved by introducing ammonia and ammonium salt as a buffer to maintain a constant pH value. The obtained materials were characterized by nitrogen sorption, X-ray and neutron diffraction, scanning electron microscopy, infrared spectroscopy, and thermal analysis. Their morphology consists of polydisperse spherical particles 50–300 nm in size, with a hexagonally ordered channel structure, high specific surface area (ABET = 900–1200 m2/g), large pore volume (Vp = 0.70–0.90 cm3/g), average mesopore diameter of about 3 nm, and narrow pore size distribution. Adsorption tests for methylene blue show sorption capacities reaching 39–42 mg/g at alkaline pH. The advantages of producing nickel silicates by this method, in contrast to precipitation from silicon alkoxides, are the low cost of reagents, fire safety, room-temperature processing, and the absence of specific problems associated with the use of ethanol as a solvent, as well as the absence of the inevitable capture of organic matter in the precipitation process.
]]>Gels doi: 10.3390/gels10020132
Authors: Flavia Bartoli Leonora Corradi Zohreh Hosseini Antonella Privitera Martina Zuena Alma Kumbaric Valerio Graziani Luca Tortora Armida Sodo Giulia Caneva
The study explores the application of natural biocides (oregano essential oil and eugenol, directly applied in solutions or encapsulated within silica nanocapsules) for safeguarding stone cultural heritage from biodeterioration, using green algae (Chlorococcum sp.) and cyanobacteria (Leptolyngbya sp.) as common pioneer biodeteriogens. Core-shell nanocontainers were built for a controlled release of microbicidal agents, a safe application of chemicals and a prolonged efficacy. The qualitative and quantitative evaluations of biocide efficiency at different doses were periodically performed in vitro, after six scheduled intervals of time (until 100 days). The release kinetics of composite biocide-embedding silica nanocapsules were characterized by the UV-Vis spectroscopy technique. Data showed both promising potential and some limitations. The comparative tests of different biocidal systems shed light on their variable efficacy against microorganisms, highlighting how encapsulation influences the release dynamics and the overall effectiveness. Both the essential oils showed a potential efficacy in protective antifouling coatings for stone artifacts. Ensuring compatibility with materials, understanding their differences in biocidal activity and their release rates becomes essential in tailoring gel, microemulsion or coating products for direct on-site application.
]]>Gels doi: 10.3390/gels10020131
Authors: Luyan Zhang Huifang Ge Jing Zhao Changqi Liu Yaosong Wang
L-theanine (L-Th), a non-protein amino acid naturally found in teas and certain plant leaves, has garnered considerable attention due to its health benefits and potential to modify proteins such as ginkgo seed proteins, which have poor gelling properties, thereby expanding their applications in the food industry. The objective of this study was to investigate the impact of varying concentrations of L-Th (0.0%, 0.5%, 1.0%, and 2.0%) on the gelling properties of ginkgo seed protein isolate (GSPI) at various pH levels (5.0, 6.0, and 7.0). The GSPI gels exhibited the highest strength at a pH of 5.0 (132.1 ± 5.6 g), followed by a pH of 6.0 (95.9 ± 3.9 g), while a weak gel was formed at a pH of 7.0 (29.5 ± 0.2 g). The incorporation of L-Th increased the hardness (58.5–231.6%) and springiness (3.0–9.5%) of the GSPI gels at a pH of 7.0 in a concentration-dependent manner. However, L-Th did not enhance the gel strength or water holding capacity at a pH of 5.0. The rheological characteristics of the GSPI sols were found to be closely related to the textural properties of L-Th-incorporated gels. To understand the underlying mechanism of L-Th’s effects, the physicochemical properties of the sols were analyzed. Specifically, L-Th promoted GSPI solubilization (up to 7.3%), reduced their hydrophobicity (up to 16.2%), reduced the particle size (up to 40.9%), and increased the ζ potential (up to 21%) of the sols. Overall, our findings suggest that L-Th holds promise as a functional ingredient for improving gel products.
]]>Gels doi: 10.3390/gels10020130
Authors: Daline Mbitta Akoa Ludovic Sicard Christophe Hélary Coralie Torrens Brigitte Baroukh Anne Poliard Thibaud Coradin
Since their first description nearly 20 years ago, dense collagen hydrogels obtained by plastic compression have become popular scaffolds in tissue engineering. In particular, when seeded with dental pulp stem cells, they have demonstrated a great in vivo potential in cranial bone repair. Here, we investigated how physico-chemical and cell-seeding conditions could influence the formation and in vitro mineralization of these cellularized scaffolds. A qualitative assessment demonstrated that the gel stability before and after compression was highly sensitive to the conditions of fibrillogenesis, especially initial acid acetic and buffer concentrations. Gels with similar rheological properties but different fibrillar structures that exhibited different stabilities when used for the 3D culture of Stem cells from Human Exfoliated Deciduous teeth (SHEDs) could be prepared. Finally, in our optimal physico-chemical conditions, mineralization could be achieved only using human dental pulp stem cells (hDPSCs) at a high cell density. These results highlight the key role of fibrillogenic conditions and cell type/density on the bone repair potential of cell-laden plastically compressed collagen hydrogels.
]]>Gels doi: 10.3390/gels10020129
Authors: Gabriela Petcu Elena Maria Anghel Irina Atkinson Daniela C. Culita Nicoleta G. Apostol Andrei Kuncser Florica Papa Adriana Baran Jean-Luc Blin Viorica Parvulescu
Ti-aluminosilicate gels were used as supports for the immobilization of Fe, Co, and Ni oxides (5%) by impregnation and synthesis of efficient photocatalysts for the degradation of β-lactam antibiotics from water. Titanium oxide (1 and 2%) was incorporated into the zeolite network by modifying the gel during the zeolitization process. The formation of the zeolite Y structure and its microporous structure were evidenced by X-ray diffraction and N2 physisorption. The structure, composition, reduction, and optical properties were studied by X-ray diffraction, H2-TPR, XPS, Raman, photoluminescence, and UV–Vis spectroscopy. The obtained results indicated a zeolite Y structure for all photocatalysts with tetracoordinated Ti4+ sites. The second transitional metals supported by the post-synthesis method were obtained in various forms, such as oxides and/or in the metallic state. A red shift of the absorption edge was observed in the UV–Vis spectra of photocatalysts upon the addition of Fe, Co, or Ni species. The photocatalytic performances were evaluated for the degradation of cefuroxime in water under visible light irradiation. The best results were obtained for iron-immobilized photocatalysts. Scavenger experiments explained the photocatalytic results and their mechanisms. A different contribution of the active species to the photocatalytic reactions was evidenced.
]]>Gels doi: 10.3390/gels10020128
Authors: Lidia Ciołek Ewa Zaczyńska Małgorzata Krok-Borkowicz Monika Biernat Elżbieta Pamuła
The aim of the study was to produce biocomposites based on chitosan and sodium hyaluronate hydrogels supplemented with bioglasses obtained under different conditions (temperature, time) and to perform an in vitro evaluation of their cytocompatibility using both indirect and direct methods. Furthermore, the release of ions from the composites and the microstructure of the biocomposites before and after incubation in simulated body fluid were assessed. Tests on extracts from bioglasses and hydrogel biocomposites were performed on A549 epithelial cells, while MG63 osteoblast-like cells were tested in direct contact with the developed biomaterials. The immune response induced by the biomaterials was also evaluated. The experiments were carried out on both unstimulated and lipopolysaccharide (LPS) endotoxin-stimulated human peripheral blood cells in the presence of extracts of the biocomposites and their components. Extracts of the materials produced do not exhibit toxic effects on A549 cells, and do not increase the production of proinflammatory cytokines tumour necrosis factor alpha (TNF-α) and interleukin (IL-6) by blood cells in vitro. In direct contact with MG63 osteoblast-like cells, biocomposites containing the reference bioglass and those containing SrO are more cytocompatible than biocomposites with ZnO-doped bioglass. Using two testing approaches, the effects both of the potentially toxic agents released and of the surface of the tested materials on the cell condition were assessed. The results pave the way for the development of highly porous hydrogel–bioglass composite scaffolds for bone tissue engineering.
]]>Gels doi: 10.3390/gels10020127
Authors: Lianfeng Zhang Yanhua Liu Zhengxin Wang Hao Li Yuheng Zhao Yinuo Pan Yang Liu Weifeng Yuan Jirui Hou
The Henan Oilfield’s medium-permeability blocks face challenges such as high temperatures and severe heterogeneity, making conventional flooding systems less effective. The starch gel system is an efficient approach for deep profile control in high-temperature reservoirs, while the nano-MoS2 system is a promising enhanced oil recovery (EOR) technology for high-temperature low-permeability reservoirs. Combining these two may achieve the dual effects of profile control and oil displacement, significantly enhancing oil recovery in high-temperature heterogeneous reservoirs. The basic performance evaluation of the combination system was carried out under reservoir temperature. Displacement experiments were conducted in target blocks under different permeabilities and extreme disparity core flooding to evaluate the combination system’s oil displacement effect. Additionally, the displacement effects and mechanisms of the starch gel and nano-MoS2 combination system in heterogeneous reservoirs were evaluated by simulating interlayer and intralayer heterogeneity models. The results show that the single nano-MoS2 system’s efficiency decreases with increased core permeability, and its effectiveness is limited in triple and quintuple disparity parallel experiments. After injecting the starch gel–nano-MoS2 combination system, the enhanced oil recovery effect was significant. The interlayer and intralayer heterogeneous models demonstrated that the primary water flooding mainly affected the high-permeability layers, while the starch gel effectively blocked the dominant channels, forcing the nano-MoS2 oil displacement system towards unswept areas. This coordination significantly enhanced oil displacement, with the combination system improving recovery by 15.33 and 12.20 percentage points, respectively. This research indicates that the starch gel and nano-MoS2 combination flooding technique holds promise for enhancing oil recovery in high-temperature heterogeneous reservoirs of Henan Oilfield, providing foundational support for field applications.
]]>Gels doi: 10.3390/gels10020126
Authors: Ane García-García Leyre Pérez-Álvarez Leire Ruiz-Rubio Asier Larrea-Sebal Cesar Martin José Luis Vilas-Vilela
Photocuring of chitosan has shown great promise in the extrusion-based 3D printing of scaffolds for advanced biomedical and tissue engineering applications. However, the poor mechanical stability of methacrylated chitosan photocuring ink restricts its applicability. The inclusion of co-networks by means of simultaneous polycomplex formation is an effective method by which to solve this drawback, but the formed hydrogel inks are not printable. This work aims to develop new photocurable chitosan inks based on the simultaneous photocrosslinking of methacrylated chitosan (CHIMe) with N,N′-methylenebisacrylamide, polyethylene glycol diacrylate, and acrylic acid to be applied in extrusion 3D printing. Interestingly, the polycomplex co-network corresponding to the acrylic-acid-based ink could be successfully printed by the here-presented simultaneous photocuring strategy. Further, the conversion of photocrosslinking was studied via photo-DSC analyses that revealed a clear dependence on the chemical structure of the employed crosslinking agents (from 40 to ~100%). In addition, the mechanical and rheological properties of the photocured hydrogels were comparatively studied, as well as the printing quality of the extruded scaffolds. The newly developed chitosan photocurable inks demonstrated extrusion printability (squareness ~0.90; uniformity factor ~0.95) and tunable mechanical properties (Young modulus 14–1068 Pa) by means of different crosslinking approaches according to the chemical architecture of the reactive molecules employed. This work shows the great potential of photocrosslinkable chitosan inks.
]]>Gels doi: 10.3390/gels10020125
Authors: Jing Li Yanwei Lv Zheng Chen Jiulong Zhao Shige Wang
In recent years, the incidence of chronic pancreatitis has increased significantly. Pancreatic calculi obstruct the pancreatic duct and induce abdominal pain in the patients. Pancreatic duct stenting is the major treatment option for chronic pancreatitis with calculi. In this study, a new kind of drug-eluting stent, a pancreatic stent coated by methacrylated gelatin (GelMA) hydrogel loaded with citric acid (CA), was designed for the interventional treatment of pancreatic duct calculi. The CA loading capacity reached up to 0.7 g CA/g hydrogel-coated stent. The GelMA hydrogel coating has higher mechanical strength and lower swelling performance after loading with CA. The in vitro experiments of stents exhibited good performance in CA sustained release and the calculi can be dissolved in almost 3 days. The stents also showed good blood compatibility and cell compatibility. This research has important clinical value in the treatment of chronic pancreatitis with pancreatic calculi.
]]>Gels doi: 10.3390/gels10020124
Authors: Dong-Heon Song Na-Eun Yang Youn-Kyung Ham Hyun-Wook Kim
The physicochemical properties of the mixed gelatin gels with soy and whey proteins were investigated to develop the gel base with a soft texture and abundant essential amino acids for the elderly. Gelatin-only gel (control) was prepared at 6% (w/v), and mixed gelatin gels were formulated by replacing gelatin with soy protein isolate and whey protein concentrate at different mixing ratios [gelatin (G):soy protein isolate (S):whey protein concentrate (W)]. Results showed that replacing gelatin with the globular proteins in gelatin gels increased the pH value and processing yield (p < 0.05). Moreover, the mixed gelatin gels, particularly the G2:S1:W3 treatment, showed significantly higher essential amino acids than the gelatin-only control. The partial replacement of gelatin with the globular proteins could decrease the hardness of gelatin gel (p < 0.05), but there was no difference in hardness between the G2:G3:W1, G2:S2:W2, and G2:S1:W3 treatments (p > 0.05). The results of protein pattern, x-ray diffraction, and microstructure had no clear evidence for specific protein–protein interaction in the mixed gelatin gels. Therefore, this study indicates that mixed gelatin gels with the globular proteins at specific mixing ratios could be a practical approach to providing a soft texture and high-level essential amino acids to the elderly.
]]>Gels doi: 10.3390/gels10020123
Authors: Regina C. Carvalho Carlos J. Durán-Valle Marta Adame-Pereira
This study deals with the preparation of adsorbents from a commercial xerogel by chemically modifying its surface with concentrated mineral acids and alkali metal chlorides, their physicochemical characterization, and their use as adsorbents for gallic acid in aqueous solution. Although there are publications on the use of carbon xerogels as adsorbents, we propose and study simple modifications that can change their chemical properties and, therefore, their performance as adsorbents. The adsorbate of choice is gallic acid and, to our knowledge, there is no history of its adsorption with carbon xerogels. The prepared adsorbents have a high specific surface area (347–563 m2 g−1), better pore development for samples treated with alkali metal chlorides than with mineral acids, and are more acidic than the initial xerogel (p.z.c range 2.49–6.87 vs. 7.20). The adsorption equilibrium is reached in <16 h with a kinetic constant between 0.018 and 0.035 h−1 for the pseudo-second-order model. The adsorption capacity, according to the Langmuir model, reaches 62.89 to 83.33 mg g−1. The adsorption properties of the commercial xerogel improved over a wide range of pH values and temperatures. The experimental results indicate that the adsorption process is thermodynamically favored.
]]>Gels doi: 10.3390/gels10020122
Authors: Aditya Narayan Singh Abhishek Meena Kyung-Wan Nam
Gels are attracting materials for energy storage technologies. The strategic development of hydrogels with enhanced physicochemical properties, such as superior mechanical strength, flexibility, and charge transport capabilities, introduces novel prospects for advancing next-generation batteries, fuel cells, and supercapacitors. Through a refined comprehension of gelation chemistry, researchers have achieved notable progress in fabricating hydrogels endowed with stimuli-responsive, self-healing, and highly stretchable characteristics. This mini-review delineates the integration of hydrogels into batteries, fuel cells, and supercapacitors, showcasing compelling instances that underscore the versatility of hydrogels, including tailorable architectures, conductive nanostructures, 3D frameworks, and multifunctionalities. The ongoing application of creative and combinatorial approaches in functional hydrogel design is poised to yield materials with immense potential within the domain of energy storage.
]]>Gels doi: 10.3390/gels10020120
Authors: Jun Yang Tengfei Dong Jingtian Yi Guancheng Jiang
This study addresses the performance challenges of Synthetic-Based Drilling Fluids (SBDF) in deep wells and high-temperature environments by engineering a novel multiple hydrogen-bonded crosslinked polymer, MBAH/nano-SiO2. Synthesized using methyl methacrylate (MMA), butyl methacrylate (BMA), acrylic acid (AA), N-hydroxyethyl acrylamide (HEAA), and nano-silica (nano-SiO2), the polymer improved crosslinking density, thermal properties, particle size distribution, and colloidal stability. The development of a ‘weak gel’ structure in W/O emulsions improved rheology and electrical stability (ES), with ES values reaching up to 775 V after aging at 180 °C. Moreover, the polymer’s amphiphilic structure and the synergistic effect of nano-SiO2 increased emulsion film thickness and strength, further augmenting stability. The high-temperature and high-pressure filtration loss of SBDF was considerably reduced to 7.6 mL, benefiting well wall stability and reservoir damage control. This study provides crucial insights into optimizing multiple hydrogen-bonded crosslinked strategies and polymers in SBDF applications.
]]>Gels doi: 10.3390/gels10020121
Authors: Shu-Liang Li Yu-Tao Wang Shi-Jun Zhang Ming-Ze Sun Jie Li Li-Qiu Chu Chen-Xi Hu Yi-Lun Huang Da-Li Gao David A. Schiraldi
Aerogels prepared using freeze-drying methods have the potential to be insulation materials or absorbents in the fields of industry, architecture, agriculture, etc., for their low heat conductivity, high specific area, low density, degradability, and low cost. However, their native, poor water resistance caused by the hydrophilicity of their polymer matrix limits their practical application. In this work, a novel, controllable, and efficient templating method was utilized to construct a highly hydrophobic surface for freeze-drying aerogels. The influence of templates on the macroscopic morphology and hydrophobic properties of materials was investigated in detail. This method provided the economical and rapid preparation of a water-resistant aerogel made from polyvinyl alcohol (PVA) and montmorillonite (MMT), putting forward a new direction for the research and development of new, environmentally friendly materials.
]]>Gels doi: 10.3390/gels10020119
Authors: Nilanchala Sahu Perwez Alam Asad Ali Neeraj Kumar Rama Tyagi Swati Madan Ramanpreet Walia Shikha Saxena
The goal of this investigation is to improve the topical delivery of medicine by preparing and maximizing the potential of a nanotransferosome gel infused with Solanum xanthocarpum methanolic extract (SXE) to provide localized and regulated distribution. Thin-film hydration was used to create SXE-infused nanotransferosomes (SXE-NTFs), and a Box–Behnken design was used to improve them. Phospholipon 90G (X1), cholesterol (X2) and sodium cholate (X3) were chosen as the independent variables, and their effects on vesicle size (Y1), polydispersity index (PDI) (Y2) and the percentage of entrapment efficiency (EE) (Y3) were observed both individually and in combination. For the SXE-NTFs, the vesicle size was 146.3 nm, the PDI was 0.2594, the EE was 82.24 ± 2.64%, the drug-loading capacity was 8.367 ± 0.07% and the drug release rate was 78.86 ± 5.24%. Comparing the antioxidant activity to conventional ascorbic acid, it was determined to be 83.51 ± 3.27%. Ex vivo permeation tests revealed that the SXE-NTF gel (82.86 ± 2.38%) considerably outperformed the SXE gel (35.28 ± 1.62%) in terms of permeation. In addition, it seemed from the confocal laser scanning microscopy (CLSM) picture of the Wistar rat’s skin that the rhodamine-B-loaded SXE-NTF gel had a higher penetration capability than the control. Dermatokinetic studies showed that the SXE-NTF gel had a better retention capability than the SXE gel. According to the experimental results, the SXE-NTF gel is a promising and successful topical delivery formulation.
]]>Gels doi: 10.3390/gels10020118
Authors: Zhi Li Shengjie Yao Guichao Wang Xi Deng Fang Zhou Xiaoxu Wu Qiong Liu
The propensity of foamed concrete to absorb water results in a consequential degradation of its performance attributes. Addressing this issue, the integration of aerogels presents a viable solution; however, their direct incorporation has been observed to compromise mechanical properties, attributable to the effects of the interface transition zone. This study explores the incorporation of MTES-based aerogels into foamed cement via an impregnation technique, examining variations in water–cement ratios. A comprehensive analysis was conducted, evaluating the influences of MTES-based aerogels on the thermal conductivity, compressive strength, density, chemical composition, and microstructure of the resultant composites across different water–cement ratios. Our findings elucidate that an increment in the water–cement ratio engenders a gradual regularization of the pore structure in foamed concrete, culminating in augmented porosity and diminished density. Notably, aerogel-enhanced foamed concrete (AEFC) exhibited a significant reduction in water absorption, quantified at 86% lower than its conventional foamed concrete (FC) counterpart. Furthermore, the softening coefficient of AEFC was observed to surpass 0.75, with peak values reaching approximately 0.9. These results substantiate that the impregnation of MTES-based aerogels into cementitious materials not only circumvents the decline in strength but also bolsters their hydrophobicity and water resistance, indirectly enhancing the serviceability and longevity of foamed concrete. In light of these findings, the impregnation method manifests promising potential for broadening the applications of aerogels in cement-based materials.
]]>Gels doi: 10.3390/gels10020116
Authors: Clara F. López-León Ramon Planet Jordi Soriano
Three-dimensional (3D) neuronal cultures grown in hydrogels are promising platforms to design brain-like neuronal networks in vitro. However, the optimal properties of such cultures must be tuned to ensure a hydrogel matrix sufficiently porous to promote healthy development but also sufficiently rigid for structural support. Such an optimization is difficult since it implies the exploration of different hydrogel compositions and, at the same time, a functional analysis to validate neuronal culture viability. To advance in this quest, here we present a combination of a rheological protocol and a network-based functional analysis to investigate PEGylated fibrin hydrogel networks with gradually higher stiffness, achieved by increasing the concentration of thrombin. We observed that moderate thrombin concentrations of 10% and 25% in volume shaped healthy networks, although the functional traits depended on the hydrogel stiffness, which was much higher for the latter concentration. Thrombin concentrations of 65% or higher led to networks that did not survive. Our results illustrate the difficulties and limitations in preparing 3D neuronal networks, and stress the importance of combining a mechano-structural characterization of a biomaterial with a functional one.
]]>Gels doi: 10.3390/gels10020117
Authors: Lyubov Magadova Mikhail Silin Vladimir Gubanov Svetlana Aksenova
Today, a significant part of production wells’ stock has a high water cut percentage of 90% and above. Obviously, for this reason, the need to develop new and improved existing technologies for water shut-off in wells increases every year. Physico-chemical methods of water shut-off are based on the application of special reagents and compositions that plug the pathways of water inflow to the well. Depending on the mechanism and specific features of water barrier formation, isolation methods are divided into selective and non-selective. This article investigates the possibility of using hydrolyzed polyacrylonitrile as a gel-forming and precipitation-forming reagent for water shut-off technologies in production wells. A surfactant–polymer composition for the isolation of water inflow in production wells in objects with high salinity in formation water, possessing physical and chemical selectivity and providing permeability reduction only in water-saturated intervals, is proposed. The developed composition is the invert emulsion, which makes it possible to carry out treatment at a distance from the well and solve the problem of possible premature gel formation directly in the wellbore. The lowest effective concentration of HPAN in an aqueous solution for use as a gel-forming and sedimentation reagent was determined experimentally (5.0 wt% and more). The interaction of the polymer solution with a chromium crosslinker allows obtaining structured gels in the whole volume of the system. The structure of the gels was evaluated using the Sydansk classifier with the assignment of a letter code from A to J. It was experimentally proved that the structure of the obtained gels depends on the temperature and content of the crosslinking agent in the system; the more crosslinking agent in the composition of the system, the stronger the structure of the resulting gel. The optimal ratio of polymer and crosslinking agent to obtain a strong gel was obtained, which amounted to 5:1 by weight of dry polymer powder. For the HPAN concentration of 5 wt% according to the Sydansk classifier, the gel structure had the code “H”—slightly deformable non-flowing gel. The dependence of the volume of gel sediment obtained because of the interaction with mineralized water on the polymer concentration was studied. It was proved that an increase in the concentration of hydrolyzed polyacrylonitrile in the solution, as well as an increase in the concentration of calcium ions in mineralized water, leads to a larger volume of the resulting gel or precipitate and to the strengthening of the gel structure. The results of rheological studies of the developed composition, as well as experiments on thermal stability, are presented. The results of filtration tests on bulk reservoir models demonstrated the selectivity of the developed composition. The obtained value of the residual resistance factor for the oil-saturated low-permeability model was 1.49 units; the value of the residual resistance factor for the water-saturated high-permeability model was 18.04 units. The ratio of the obtained values of the residual resistance factor, equal to 0.08 (much less than 1), can characterize the developed composition as a selective material for water shut-off in producing wells. Existing technologies for water shut-off based on HPAN do not allow for making a treatment at a distance from the well and require the use of technological solutions to prevent premature gel sedimentation in the well. The developed composition makes it possible to solve the problem of premature gelation. In addition, the composition can form a blocking screen in highly permeable water-saturated zones. The development can be useful for deposits with difficult conditions (high mineralization in reservoir waters, boreholes with a horizontal end, elevated temperatures up to 80 °C).
]]>Gels doi: 10.3390/gels10020114
Authors: Zhuxing Zhou Jiajie Wang Chaoqian Jiang Kaiwang Xu Tengjing Xu Xinning Yu Jinghua Fang Yanyu Yang Xuesong Dai
Meniscus tissue engineering (MTE) has emerged as a promising strategy for meniscus repair and regeneration. As versatile platforms, hydrogels have gained significant attention in this field, as they possess tunable properties that allow them to mimic native extracellular matrices and provide a suitable microenvironment. Additionally, hydrogels can be minimally invasively injected and can be adjusted to match the shape of the implant site. They can conveniently and effectively deliver bioactive additives and demonstrate good compatibility with other functional materials. These inherent qualities have made hydrogel a promising candidate for therapeutic approaches in meniscus repair and regeneration. This article provides a comprehensive review of the advancements made in the research on hydrogel application for meniscus tissue engineering. Firstly, the biomaterials and crosslinking strategies used in the formation of hydrogels are summarized and analyzed. Subsequently, the role of therapeutic additives, including cells, growth factors, and other active products, in facilitating meniscus repair and regeneration is thoroughly discussed. Furthermore, we summarize the key issues for designing hydrogels used in MTE. Finally, we conclude with the current challenges encountered by hydrogel applications and suggest potential solutions for addressing these challenges in the field of MTE. We hope this review provides a resource for researchers and practitioners interested in this field, thereby facilitating the exploration of new design possibilities.
]]>Gels doi: 10.3390/gels10020115
Authors: Madelyn Reynolds Lindsay M. Stoy Jindi Sun Prince Emmanuel Opoku Amponsah Lin Li Misael Soto Shang Song
Conductive hydrogels are highly attractive for biomedical applications due to their ability to mimic the electrophysiological environment of biological tissues. Although conducting polymer polythiophene-poly-(3,4-ethylenedioxythiophene) (PEDOT) and polystyrene sulfonate (PSS) alone exhibit high conductivity, the addition of other chemical compositions could further improve the electrical and mechanical properties of PEDOT:PSS, providing a more promising interface with biological tissues. Here we study the effects of incorporating crosslinking additives, such as glycerol and sodium trimetaphosphate (STMP), in developing interpenetrating PEDOT:PSS-based conductive hydrogels. The addition of glycerol at a low concentration maintained the PEDOT:PSS conductivity with enhanced wettability but decreased the mechanical stiffness. Increasing the concentration of STMP allowed sufficient physical crosslinking with PEDOT:PSS, resulting in improved hydrogel conductivity, wettability, and rheological properties without glycerol. The STMP-based PEDOT:PSS conductive hydrogels also exhibited shear-thinning behaviors, which are potentially favorable for extrusion-based 3D bioprinting applications. We demonstrate an interpenetrating conducting polymer hydrogel with tunable electrical and mechanical properties for cellular interactions and future tissue engineering applications.
]]>Gels doi: 10.3390/gels10020113
Authors: Aurel Diacon Florin Albota Alexandra Mocanu Oana Brincoveanu Alice Ionela Podaru Traian Rotariu Ahmad A. Ahmad Edina Rusen Gabriela Toader
This study describes the development of a fast and cost-effective method for the detection and removal of Hg2+ ions from aqueous media, consisting of hydrogels incorporating chelating agents and a rhodamine derivative (to afford a qualitative evaluation of the heavy metal entrapment inside the 3D polymeric matrix). These hydrogels, designed for the simultaneous detection and entrapment of mercury, were obtained through the photopolymerization of 2-acrylamido-2-methyl-1-propanesulfonic acid (AMPSA) and N-vinyl-2-pyrrolidone (NVP), utilizing N,N′-methylenebisacrylamide (MBA) as crosslinker, in the presence of polyvinyl alcohol (PVA), a rhodamine B derivative, and one of the following chelating agents: phytic acid, 1,3-diamino-2-hydroxypropane-tetraacetic acid, triethylenetetramine-hexaacetic acid, or ethylenediaminetetraacetic acid disodium salt. The rhodamine derivative had a dual purpose in this study: firstly, it was incorporated into the hydrogel to allow the qualitative evaluation of mercury entrapment through its fluorogenic switch-off abilities when sensing Hg2+ ions; secondly, it was used to quantitatively evaluate the level of residual mercury from the decontaminated aqueous solutions, via the UV-Vis technique. The ICP-MS analysis of the hydrogels also confirmed the successful entrapment of mercury inside the hydrogels and a good correlation with the UV-Vis method.
]]>Gels doi: 10.3390/gels10020112
Authors: Quanyang Wang Chenghua Zhou Honghu Zhang Xue Zhang Xinxin Wen Jiexin Bai Hui Mao
Deep wells and ultra-deep wells often encounter cracks, karst caves, and other developed strata, which can lead to leakage during drilling. Conventional bridge slurry plugging technology is prone to leaking due to the poor plugging effect of the plugging agent. The gel plugging agent possesses characteristics of flexible plugging and adaptive matching of formation leakage channels. It can fill cracks or caves and enhance the pressure-bearing capacity of the formation. A controllable crosslinking plugging agent based on low-molecular-weight polyacrylamide was studied. Polyacrylamide with different molecular weights is synthesized from acrylamide and an initiator. A crosslinking time-controllable polymer is synthesized from low-molecular-weight polyacrylamide by adding crosslinking agent and retarder. The low-molecular-weight polyacrylamide plugging agent has low viscosity before gelation and good fluidity in the wellbore. After being configured on the ground, it is transported by pipeline and sent underground to reach the thickening condition. The gel solution rapidly solidifies, and its strength improves after high-temperature crosslinking. The synthesis conditions of the polymer were as follows: a monomer concentration of 9%, initiator 3.5%, synthesis temperature of 65 °C, and hydrogen peroxide initiator. The optimal formula of the gel plugging agent is as follows: a polymer concentration of 6%, a crosslinking agent concentration of 1%, and a retarder concentration of 8%. The generated polymer molecular structure contains amide groups. This crosslinking time-controllable plugging agent based on low-molecular-weight polyacrylamide has stable rheology, and its temperature resistance can reach 150 °C. At 150 °C, the gelation time can be controlled by adjusting the concentration of retarder, and the longest can reach 4 h. The plugging efficiency of the gel plugging agent is more than 95%. With the increase in seam width, the pressure of the gel plugging agent gradually decreases.
]]>Gels doi: 10.3390/gels10020111
Authors: Lai Wei Yuqing Ren Lu Huang Xinnan Ye He Li Jian Li Jinnuo Cao Xinqi Liu
Composite emulsion gel can effectively mimic animal adipose tissue. In this study, composite emulsion gels composed of soy protein isolates and konjac glucomannan (KGM) were prepared as plant-based cubic fat substitutes (CFS). The effects of CFS on the quality and structure of pork patties were investigated in terms of the proximate composition, lipid oxidation stability, technological characteristics, color, sensory attributes, texture, thermo-rheological behavior, and microstructure. CFS samples composed of various ratios of KGM were added to lean meat patties to ascertain the optimal CFS composition for its potential replacement of pork back fat in patties. The addition of CFS containing 7.0% KGM was found to decrease the hardness of the lean meat patties by 71.98% while simultaneously improving their sensory quality. The replacement of pork back fat with CFS also reduced the fat content of the patties to as little as 3.65%. Furthermore, the addition of CFS enhanced the technological characteristics, lipid oxidation stability, and surface color of the fat-replaced patties, with no significant impact on their overall acceptability. The gel network of the patties was shown to be fine and remained compact as the fat replacement ratio increased to 75%, while the texture parameters, storage modulus, and fractal dimension all increased. Quality and structure improvements may allow the composite emulsion gels to replace fat in pork patties to support a healthy diet. This study may be beneficial for the application and development of plant-based cubic fat substitutes.
]]>Gels doi: 10.3390/gels10020110
Authors: Emira D’Amico Silvia Di Lodovico Tania Vanessa Pierfelice Domenico Tripodi Adriano Piattelli Giovanna Iezzi Morena Petrini Simonetta D’Ercole
This study aimed to evaluate the ability of photodynamic therapy, based on the use of a gel containing 5% delta aminolaevulinic acid (ALAD) for 45′ followed by irradiation with 630 nm LED (PDT) for 7′, to eradicate Candida albicans strains without damaging the gingiva. C. albicans oral strains and gingival fibroblasts (hGFs) were used to achieve these goals. The potential antifungal effects on a clinical resistant C. albicans S5 strain were evaluated in terms of biofilm biomass, colony forming units (CFU/mL) count, cell viability by live/dead analysis, and fluidity membrane changes. Concerning the hGFs, viability assays, morphological analysis (optical, scanning electronic (SEM), and confocal laser scanning (CLSM) microscopes), and assays for reactive oxygen species (ROS) and collagen production were performed. ALAD-mediated aPDT (ALAD-aPDT) treatment showed significant anti-biofilm activity against C. albicans S5, as confirmed by a reduction in both the biofilm biomass and CFUs/mL. The cell viability was strongly affected by the treatment, while on the contrary, the fluidity of the membrane remained unchanged. The results for the hGFs showed an absence of cytotoxicity and no morphological differences in cells subjected to ALAD-aPDT expected for CLSM results that exhibited an increase in the thickening of actin filaments. ROS production was augmented only at 0 h and 3 h, while the collagen appeared enhanced 7 days after the treatment.
]]>Gels doi: 10.3390/gels10020109
Authors: Ying Sun Jiayi Wang Duanxin Li Feng Cheng
Cellulose-based antibacterial hydrogel has good biocompatibility, antibacterial performance, biodegradability, and other characteristics. It can be very compatible with human tissues and degradation, while its good water absorption and moisturizing properties can effectively absorb wound exudates, keep the wound moist, and promote wound healing. In this paper, the structural properties, and physical and chemical cross-linking preparation methods of cellulose-based antibacterial hydrogels were discussed in detail, and the application of cellulose-based hydrogels in the antibacterial field was deeply studied. In general, cellulose-based antibacterial hydrogels, as a new type of biomaterial, have shown good potential in antimicrobial properties and have been widely used. However, there are still some challenges, such as optimizing the preparation process and performance parameters, improving the antibacterial and physical properties, broadening the application range, and evaluating safety. However, with the deepening of research and technological progress, it is believed that cellulose-based antibacterial hydrogels will be applied and developed in more fields in the future.
]]>Gels doi: 10.3390/gels10020108
Authors: Yixuan Yuan Caleb Tyson Annika Szyniec Samuel Agro Tara N. Tavakol Alexander Harmon DessaRae Lampkins Lauran Pearson Jerald E. Dumas Lakeshia J. Taite
Polyurethanes (PUs) are a highly adaptable class of biomaterials that are among some of the most researched materials for various biomedical applications. However, engineered tissue scaffolds composed of PU have not found their way into clinical application, mainly due to the difficulty of balancing the control of material properties with the desired cellular response. A simple method for the synthesis of tunable bioactive poly(ethylene glycol) diacrylate (PEGDA) hydrogels containing photocurable PU is described. These hydrogels may be modified with PEGylated peptides or proteins to impart variable biological functions, and the mechanical properties of the hydrogels can be tuned based on the ratios of PU and PEGDA. Studies with human cells revealed that PU–PEG blended hydrogels support cell adhesion and viability when cell adhesion peptides are crosslinked within the hydrogel matrix. These hydrogels represent a unique and highly tailorable system for synthesizing PU-based synthetic extracellular matrices for tissue engineering applications.
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