Gels | February 2023 - Browse Articles

13 pages, 6164 KiB

Open AccessArticle

Directional-Freezing-Assisted In Situ Sol–Gel Strategy to Synthesize High-Strength, Fire-Resistant, and Hydrophobic Wood-Based Composite Aerogels for Thermal Insulation

by Yan Hou, Junyong Chen, Defang Pan and Lu Zhao

Gels 2023, 9(2), 170; https://doi.org/10.3390/gels9020170 - 20 Feb 2023

Cited by 2 | Viewed by 1924

Abstract

The undesirable inherent natural characteristics of wood, such as low mechanical strength, flammability, and hygroscopicity, limit its potential applications in the thermal insulation industry. Overcoming these disadvantages can greatly expand the application scope of wood. A new attempt at wood modification, the directional-freezing-assisted [...] Read more.

The undesirable inherent natural characteristics of wood, such as low mechanical strength, flammability, and hygroscopicity, limit its potential applications in the thermal insulation industry. Overcoming these disadvantages can greatly expand the application scope of wood. A new attempt at wood modification, the directional-freezing-assisted in situ sol–gel strategy, was used to obtain wood–silica composite aerogels with the unique multi-level ordered porous structure of wood. This method enables silica nanoparticles to successfully replace lignin and facilitates the formation of strong hydrogen bonds between the silica and cellulose molecules. This results in improved mechanical properties for the composite with a density similar to that of natural wood but a mechanical strength that can be up to five times greater. The thermal conductivity coefficient is also reduced to 0.032 W (m·K)⁻¹ compared to 0.066 W (m·K)⁻¹ for natural wood. This aerogel composite exhibits improved fire resistance and hygroscopicity, with a decomposition temperature increase of approximately 45 °C compared to natural wood. Additionally, the composite demonstrates self-extinguishing behavior, with the structure remaining intact after combustion, and thus enhanced fire resistance. Simultaneously, the enhanced aerogel composite hydrophobicity, with water contact angle of up to 120°, is beneficial to a prominent thermal insulation performance in a high-humidity environment. The successful synthesis of wood-based composite aerogels provides a new and innovative approach for the utilization of wood resources in the thermal insulation industry. Full article

(This article belongs to the Special Issue Advances in Biopolymer Aerogels and Their Composites)

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12 pages, 1786 KiB

Open AccessArticle

Hydrogel Encapsulation of Genome-Engineered Stem Cells for Long-Term Self-Regulating Anti-Cytokine Therapy

by Kelsey H. Collins, Lara Pferdehirt, Leila S. Saleh, Alireza Savadipour, Luke E. Springer, Kristin L. Lenz, Dominic M. Thompson, Jr., Sara J. Oswald, Christine T. N. Pham and Farshid Guilak

Gels 2023, 9(2), 169; https://doi.org/10.3390/gels9020169 - 20 Feb 2023

Cited by 4 | Viewed by 3712

Abstract

Biologic therapies have revolutionized treatment options for rheumatoid arthritis (RA) but their continuous administration at high doses may lead to adverse events. Thus, the development of improved drug delivery systems that can sense and respond commensurately to disease flares represents an unmet medical [...] Read more.

Biologic therapies have revolutionized treatment options for rheumatoid arthritis (RA) but their continuous administration at high doses may lead to adverse events. Thus, the development of improved drug delivery systems that can sense and respond commensurately to disease flares represents an unmet medical need. Toward this end, we generated induced pluripotent stem cells (iPSCs) that express interleukin-1 receptor antagonist (IL-1Ra, an inhibitor of IL-1) in a feedback-controlled manner driven by the macrophage chemoattractant protein-1 (Ccl2) promoter. Cells were seeded in agarose hydrogel constructs made from 3D printed molds that can be injected subcutaneously via a blunt needle, thus simplifying implantation of the constructs, and the translational potential. We demonstrated that the subcutaneously injected agarose hydrogels containing genome-edited Ccl2-IL1Ra iPSCs showed significant therapeutic efficacy in the K/BxN model of inflammatory arthritis, with nearly complete abolishment of disease severity in the front paws. These implants also exhibited improved implant longevity as compared to the previous studies using 3D woven scaffolds, which require surgical implantation. This minimally invasive cell-based drug delivery strategy may be adapted for the treatment of other autoimmune or chronic diseases, potentially accelerating translation to the clinic. Full article

(This article belongs to the Special Issue Bioprinting Hydrogels)

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16 pages, 4387 KiB

Open AccessArticle

Study on the Low-Temperature Rheology of Polar Drilling Fluid and Its Regulation Method

by Ning Huang, Kaihe Lv, Jinsheng Sun, Jingping Liu, Jintang Wang and Zonglun Wang

Gels 2023, 9(2), 168; https://doi.org/10.3390/gels9020168 - 20 Feb 2023

Viewed by 1722

Abstract

Drilling fluid is the blood of drilling engineering. In the polar drilling process, the ultra-low temperature environment puts high demands on the rheological performance of drilling fluids. In this paper, the effects of temperature, ice debris concentration and weighting agent on the rheological [...] Read more.

Drilling fluid is the blood of drilling engineering. In the polar drilling process, the ultra-low temperature environment puts high demands on the rheological performance of drilling fluids. In this paper, the effects of temperature, ice debris concentration and weighting agent on the rheological properties of drilling fluids were studied. It was found that the lower the temperature and the higher the ice debris concentration, the higher the drilling fluid viscosity, but when the ice debris concentration was below 2%, the drilling fluid rheology hardly changed. Secondly, the low temperature rheological properties of drilling fluid were adjusted by three different methods: base fluid ratio, organoclay, and polymers (dimer acid, polymethacrylate, ethylene propylene copolymer, and vinyl resin). The results showed that the base fluid rheological performance was optimal when the base fluid ratio was 7:3. Compared with polymers, organoclay has the most significant improvement on the low temperature rheological performance of drilling fluid. The main reason is that organoclay can transform the drilling fluid from Newtonian to non-Newtonian fluid, which exhibits excellent shear dilution of drilling fluid. The organoclay is also more uniformly dispersed in the oil, forming a denser weak gel mesh structure, so it is more effective in improving the cuttings carrying and suspension properties of drilling fluids. However, the drilling fluid containing polymer additives is still a Newtonian fluid, which cannot form a strong mesh structure at ultra-low temperatures, and thus cannot effectively improve the low-temperature rheological performance of drilling fluid. In addition, when the amount of organoclay is 2%, the improvement rate of the yield point reaches 250% at −55 °C, which can effectively improve the cuttings carrying and suspension performance of drilling fluid at ultra-low temperature. Full article

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11 pages, 4249 KiB

Open AccessArticle

Conductive and Adhesive Granular Alginate Hydrogels for On-Tissue Writable Bioelectronics

by Sumin Kim, Heewon Choi, Donghee Son and Mikyung Shin

Gels 2023, 9(2), 167; https://doi.org/10.3390/gels9020167 - 19 Feb 2023

Cited by 8 | Viewed by 2676

Abstract

Conductive hydrogels are promising materials in bioelectronics that ensure a tissue-like soft modulus and re-enact the electrophysiological function of damaged tissues. However, recent approaches to fabricating conductive hydrogels have proved difficult: fixing of the conductive hydrogels on the target tissues hydrogels requires the [...] Read more.

Conductive hydrogels are promising materials in bioelectronics that ensure a tissue-like soft modulus and re-enact the electrophysiological function of damaged tissues. However, recent approaches to fabricating conductive hydrogels have proved difficult: fixing of the conductive hydrogels on the target tissues hydrogels requires the aids from other medical glues because of their weak tissue-adhesiveness. In this study, an intrinsically conductive and tissue-adhesive granular hydrogel consisting of a PEDOT:PSS conducting polymer and an adhesive catechol-conjugated alginate polymer was fabricated via an electrohydrodynamic spraying method. Because alginate-based polymers can be crosslinked by calcium ions, alginate-catechol polymers mixed with PEDOT:PSS granular hydrogels (ACP) were easily fabricated. The fabricated ACP exhibited not only adhesive and shear-thinning properties but also conductivity similar to that of muscle tissue. Additionally, the granular structure makes the hydrogel injectable through a syringe, enabling on-tissue printing. This multifunctional granular hydrogel can be applied to soft and flexible electronics to connect humans and machines. Full article

(This article belongs to the Special Issue Recent Advances in Designing Hydrogels for Flexible Electronics and Devices)

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33 pages, 7268 KiB

Open AccessEditor’s ChoiceArticle

Bioengineered Water-Responsive Carboxymethyl Cellulose/Poly(vinyl alcohol) Hydrogel Hybrids for Wound Dressing and Skin Tissue Engineering Applications

by Nádia Sueli Vieira Capanema, Alexandra Ancelmo Piscitelli Mansur, Isadora Cota Carvalho, Sandhra Maria Carvalho and Herman Sander Mansur

Gels 2023, 9(2), 166; https://doi.org/10.3390/gels9020166 - 18 Feb 2023

Cited by 8 | Viewed by 2800

Abstract

The burden of chronic wounds is growing due to the increasing incidence of trauma, aging, and diabetes, resulting in therapeutic problems and increased medical costs. Thus, this study reports the synthesis and comprehensive characterization of water-responsive hybrid hydrogels based on carboxymethyl cellulose (CMC) [...] Read more.

The burden of chronic wounds is growing due to the increasing incidence of trauma, aging, and diabetes, resulting in therapeutic problems and increased medical costs. Thus, this study reports the synthesis and comprehensive characterization of water-responsive hybrid hydrogels based on carboxymethyl cellulose (CMC) and poly(vinyl alcohol) (PVA) using citric acid (CA) as the chemical crosslinking agent, with tunable physicochemical properties suitable to be applied as a wound dressing for soft tissue engineering applications. They were produced through an eco-friendly process under mild conditions. The hydrogels were designed and produced with flexible swelling degree properties through the selection of CMC molecular mass (Mw = 250 and 700 kDa) and degree of functionalization (DS = 0.81), degree of hydrolysis of PVA (DH > 99%, Mw = 84–150 kDa) associated with synthesis parameters, CMC/PVA ratio and extension of chemical crosslinking (CA/CMC:PVA ratio), for building engineered hybrid networks. The results demonstrated that highly absorbent hydrogels were produced with swelling degrees ranging from 100% to 5000%, and gel fraction from 40% to 80%, which significantly depended on the concentration of CA crosslinker and the presence of PVA as the CMC-based network modifier. The characterizations indicated that the crosslinking mechanism was mostly associated with the chemical reaction of CA carboxylic groups with hydroxyl groups of CMC and PVA polymers forming ester bonds, rendering a hybrid polymeric network. These hybrid hydrogels also presented hydrophilicity, permeability, and structural features dependent on the degree of crosslinking and composition. The hydrogels were cytocompatible with in vitro cell viability responses of over 90% towards model cell lines. Hence, it is envisioned that this research provides a simple strategy for producing biocompatible hydrogels with tailored properties as wound dressings for assisting chronic wound healing and skin tissue engineering applications. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels (2nd Edition))

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19 pages, 2635 KiB

Open AccessArticle

Calcitermin-Loaded Smart Gels Activity against Candida albicans: A Preliminary In Vitro Study

by Denise Bellotti, Maria D’Accolti, Walter Pula, Nicolas Huang, Fanny Simeliere, Elisabetta Caselli, Elisabetta Esposito and Maurizio Remelli

Gels 2023, 9(2), 165; https://doi.org/10.3390/gels9020165 - 18 Feb 2023

Cited by 4 | Viewed by 1484

Abstract

Calcitermin is an antimicrobial peptide of 15 amino acids found in human nasal fluid characterized by antifungal and antibacterial properties. Candida albicans is the most common human fungal pathogen affecting many tissues, such as vaginal mucosa. In this study a formulation suitable for [...] Read more.

Calcitermin is an antimicrobial peptide of 15 amino acids found in human nasal fluid characterized by antifungal and antibacterial properties. Candida albicans is the most common human fungal pathogen affecting many tissues, such as vaginal mucosa. In this study a formulation suitable for calcitermin administration on vaginal mucosa was developed for the treatment of fungal infections. To favor topical application, mucosal adhesion, and permanence, gels based on poloxamer 407 and xanthan gum were designed and compared with regard to their rheological behavior, erosion, and leakage. The selected gel was loaded with calcitermin, whose release kinetic was evaluated in vitro by Franz cells. An antifungal activity assay was conducted to assess the calcitermin anticandidal potential and the effect of its inclusion in the selected gel. The rheological study revealed the elastic and viscous moduli behavior as a function of poloxamer 407 and xanthan gum concentration. Xanthan gum presence decreased the transition temperature of the gel, while prolonging its erosion and leakage. Particularly, poloxamer 407, 18% and xanthan gum 0.4% were chosen. The calcitermin loading in the selected gel resulted in a transparent and homogeneous formulation and in a 4-fold decrease of the release rate with respect to the calcitermin solution, as evidenced by Franz cell study. The anticandidal activity tests demonstrated that calcitermin-loaded gel was more active against Candida albicans with respect to the peptide solution. Full article

(This article belongs to the Special Issue Advanced Gels for Drug Delivery Systems Based on Sustainable Development Goals (SDGs))

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10 pages, 1925 KiB

Open AccessArticle

Spatial Control over Catalyst Positioning for Increased Micromotor Efficiency

by Shauni Keller, Serena P. Teora, Arif Keskin, Luuk J. C. Daris, Norman A. P. E. Samuels, Moussa Boujemaa and Daniela A. Wilson

Gels 2023, 9(2), 164; https://doi.org/10.3390/gels9020164 - 18 Feb 2023

Cited by 1 | Viewed by 1591

Abstract

Motion is influenced by many different aspects of a micromotor’s design, such as shape, roughness and the type of materials used. When designing a motor, asymmetry is the main requirement to take into account, either in shape or in catalyst distribution. It influences [...] Read more.

Motion is influenced by many different aspects of a micromotor’s design, such as shape, roughness and the type of materials used. When designing a motor, asymmetry is the main requirement to take into account, either in shape or in catalyst distribution. It influences both speed and directionality since it dictates the location of propulsion force. Here, we combine asymmetry in shape and asymmetry in catalyst distribution to study the motion of soft micromotors. A microfluidic method is utilized to generate aqueous double emulsions, which upon UV-exposure form asymmetric microgels. Taking advantage of the flexibility of this method, we fabricated micromotors with homogeneous catalyst distribution throughout the microbead and micromotors with different degrees of catalyst localization within the active site. Spatial control over catalyst positioning is advantageous since less enzyme is needed for the same propulsion speed as the homogeneous system and it provides further confinement and compartmentalization of the catalyst. This proof-of-concept of our new design will make the use of enzymes as driving forces for motors more accessible, as well as providing a new route for compartmentalizing enzymes at interfaces without the need for catalyst-specific functionalization. Full article

(This article belongs to the Special Issue Hydrogels, Microgels, and Nanogels: From Fundamentals to Applications)

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14 pages, 2033 KiB

Open AccessArticle

Development of a Polyherbal Topical Gel for the Treatment of Acne

by Benedict Jose Chellathurai, Ramyadevi Anburose, Mohammad H. Alyami, Mohan Sellappan, Mohammad F. Bayan, Balakumar Chandrasekaran, Kumarappan Chidambaram and Mohamed Rahamathulla

Gels 2023, 9(2), 163; https://doi.org/10.3390/gels9020163 - 17 Feb 2023

Cited by 6 | Viewed by 3463

Abstract

The present work aimed to formulate and evaluate a polyherbal gel using Aloe barbadensis and extract of Vigna radiata for the treatment of acne, a disorder of the skin in which hair follicles and sebaceous glands are blocked, causing inflammation and redness of [...] Read more.

The present work aimed to formulate and evaluate a polyherbal gel using Aloe barbadensis and extract of Vigna radiata for the treatment of acne, a disorder of the skin in which hair follicles and sebaceous glands are blocked, causing inflammation and redness of the skin. Aloe barbadensis pulp was collected and mixed with the extract of Vigna radiata and formulated into a gel using Carbopol 940, triethanolamine, and propylene glycol as the gelling agent, viscosity modifier, and pH modifier, respectively. The gel was evaluated for its antimicrobial properties against Staphylococcus aureus, Escherichia coli, and Candida albicans. Antimicrobial agents, such as gentamycin and fluconazole, were used as the standards. The developed formulation showed promising zone of inhibition. The gel was further evaluated for its physicochemical properties. The formulation showed a promising effect on acne together with the additive effect of Aloe barbadensis on skin. Full article

(This article belongs to the Special Issue Advanced Gels for Drug Delivery Systems Based on Sustainable Development Goals (SDGs))

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15 pages, 6814 KiB

Open AccessArticle

Ultrasensitive and Self-Powered Multiparameter Pressure–Temperature–Humidity Sensor Based on Ultra-Flexible Conductive Silica Aerogel

by Song He, Chunhua Du, Hongliang Sheng, Chunxiang He, Xinyu Liu, Xin Jin, Qilin Chen and Fuliang Tian

Gels 2023, 9(2), 162; https://doi.org/10.3390/gels9020162 - 17 Feb 2023

Cited by 2 | Viewed by 1317

Abstract

The application of silica aerogel has been limited because of its poor mechanical properties. In order to expand the application scope of silica aerogel, this study fabricated an ultra-flexible conductive silica aerogel as a multiparameter sensor. The sample is fabricated by introducing poly [...] Read more.

The application of silica aerogel has been limited because of its poor mechanical properties. In order to expand the application scope of silica aerogel, this study fabricated an ultra-flexible conductive silica aerogel as a multiparameter sensor. The sample is fabricated by introducing poly (3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) on a base of ultra-flexible silica aerogel, which was prepared by a diene synthesis reaction at atmospheric pressure. The pressure, temperature, and humidity can be converted into electrical signals. The pressure sensitivity can reach up to 54.88 kPa⁻¹, and the detection limit is as low as 5 Pa. The temperature resolution is up to 0.1 K, and the response time of humidity is within 4 s. More importantly, the developed multiparameter sensor can be self-powered to realize multiparameter sensing of pressure, temperature, and humidity. The ultra-flexible conductive silica aerogel is a promising candidate for monitoring human activities and fire-affected areas. Full article

(This article belongs to the Special Issue Aerogels: Synthesis and Applications)

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27 pages, 4370 KiB

Open AccessEditor’s ChoiceReview

Polymer Gels: Classification and Recent Developments in Biomedical Applications

by Mariana Chelu and Adina Magdalena Musuc

Gels 2023, 9(2), 161; https://doi.org/10.3390/gels9020161 - 17 Feb 2023

Cited by 24 | Viewed by 7292

Abstract

Polymer gels are a valuable class of polymeric materials that have recently attracted significant interest due to the exceptional properties such as versatility, soft-structure, flexibility and stimuli-responsive, biodegradability, and biocompatibility. Based on their properties, polymer gels can be used in a wide range [...] Read more.

Polymer gels are a valuable class of polymeric materials that have recently attracted significant interest due to the exceptional properties such as versatility, soft-structure, flexibility and stimuli-responsive, biodegradability, and biocompatibility. Based on their properties, polymer gels can be used in a wide range of applications: food industry, agriculture, biomedical, and biosensors. The utilization of polymer gels in different medical and industrial applications requires a better understanding of the formation process, the factors which affect the gel’s stability, and the structure-rheological properties relationship. The present review aims to give an overview of the polymer gels, the classification of polymer gels’ materials to highlight their important features, and the recent development in biomedical applications. Several perspectives on future advancement of polymer hydrogel are offered. Full article

(This article belongs to the Section Gel Analysis and Characterization)

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24 pages, 5498 KiB

Open AccessArticle

Origin of the Springback Effect in Ambient-Pressure-Dried Silica Aerogels: The Effect of Surface Silylation

by Fabian Zemke, Julien Gonthier, Ernesto Scoppola, Ulla Simon, Maged F. Bekheet, Wolfgang Wagermaier and Aleksander Gurlo

Gels 2023, 9(2), 160; https://doi.org/10.3390/gels9020160 - 16 Feb 2023

Cited by 5 | Viewed by 1807

Abstract

Ambient pressure drying (APD) can prospectively reduce the costs of aerogel fabrication and processing. APD relies solely on preventing shrinkage or making it reversible. The latter, i.e., the aerogel re-expansion after drying (so-called springback effect—SBE), needs to be controlled for reproducible aerogel fabrication [...] Read more.

Ambient pressure drying (APD) can prospectively reduce the costs of aerogel fabrication and processing. APD relies solely on preventing shrinkage or making it reversible. The latter, i.e., the aerogel re-expansion after drying (so-called springback effect—SBE), needs to be controlled for reproducible aerogel fabrication by APD. This can be achieved by an appropriate surface functionalization of aerogel materials (e.g., SiO₂). This work addresses the fabrication of monolithic SiO₂ aerogels and xerogels by APD. The effect of several silylation agents, i.e., trimethylchlorosilane, triethylchlorosilane, and hexamethyldisilazane on the SBE is studied in detail, applying several complementary experimental techniques, allowing the evaluation of the macroscopic and microscopic morphology as well as the composition of SiO₂ aerogels. Here, we show that some physical properties, e.g., the bulk density, the macroscopic structure, and pore sizes/volumes, were significantly affected by the re-expansion. However, silylation did not necessarily lead to full re-expansion. Therefore, similarities in the molecular composition could not be equated to similarities in the SBE. The influences of steric hindrance and reactivity are discussed. The impact of silylation is crucial in tailoring the SBE and, as a result, the APD of monolithic aerogels. Full article

(This article belongs to the Special Issue Recent Advances in Aerogels)

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13 pages, 4965 KiB

Open AccessArticle

Synthesis and Characterization of Gamma Radiation Induced Diallyldimethylammonium Chloride-Acrylic Acid-(3-Acrylamidopropyl) Trimethylammonium Chloride Superabsorbent Hydrogel

by Md Murshed Bhuyan and Jae-Ho Jeong

Gels 2023, 9(2), 159; https://doi.org/10.3390/gels9020159 - 16 Feb 2023

Cited by 3 | Viewed by 1464

Abstract

The gamma radiation technique is simple and time-saving for the synthesis of pure hydrogels. The present work focuses on synthesizing and characterizing Diallyldimethylammonium Chloride-Acrylic acid-(3-Acrylamidopropyl) trimethylammonium Chloride (DADMAC-AAc-APTAC) superabsorbent hydrogels. The hydrogels were synthesized by applying gamma radiation of different doses (2 kGy [...] Read more.

The gamma radiation technique is simple and time-saving for the synthesis of pure hydrogels. The present work focuses on synthesizing and characterizing Diallyldimethylammonium Chloride-Acrylic acid-(3-Acrylamidopropyl) trimethylammonium Chloride (DADMAC-AAc-APTAC) superabsorbent hydrogels. The hydrogels were synthesized by applying gamma radiation of different doses (2 kGy to 30 kGy) to two different compositions of monomers. The equilibrium swelling was found to be 33483.48% of dried gel for a 1:0.5:1 composition ratio of monomers at a 2 kGy radiation dose. Therefore, on the basis of equilibrium swelling, 2 kGy is the optimum radiation dose for synthesizing the hydrogel. Fourier transform infrared (FTIR), nuclear magnetic resonance (NMR) spectroscopy, and X-ray diffraction (XRD) characterization techniques were used to analyze and confirm the structure of the hydrogel. Thermogravimetric analysis (TGA) and Scanning electron microscopy (SEM) equipped with energy dispersive spectroscopy (EDS) clearly showed the thermal stability and surface morphology of the gel. Therefore, it can be concluded that hydrogels can be used in metal adsorption, drug delivery, and other fields of study. Full article

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13 pages, 3833 KiB

Open AccessArticle

Enhanced Rupture Force in a Cut-Dispersed Double-Network Hydrogel

by Shilei Zhu, Dongdong Yan, Lin Chen, Yan Wang, Fengbo Zhu, Yanan Ye, Yong Zheng, Wenwen Yu and Qiang Zheng

Gels 2023, 9(2), 158; https://doi.org/10.3390/gels9020158 - 16 Feb 2023

Cited by 1 | Viewed by 1350

Abstract

The Kirigami approach is an effective way to realize controllable deformation of intelligent materials via introducing cuts into bulk materials. For materials ranging from ordinary stiff materials such as glass, ceramics, and metals to soft materials, including ordinary hydrogels and elastomers, all of [...] Read more.

The Kirigami approach is an effective way to realize controllable deformation of intelligent materials via introducing cuts into bulk materials. For materials ranging from ordinary stiff materials such as glass, ceramics, and metals to soft materials, including ordinary hydrogels and elastomers, all of them are all sensitive to the presence of cuts, which usually act as defects to deteriorate mechanical properties. Herein, we study the influence of the cuts on the mechanical properties by introducing “dispersed macro-scale cuts” into a model tough double network (DN) hydrogel (named D-cut gel), which consists of a rigid and brittle first network and a ductile stretchable second network. For comparison, DN gels with “continuous cuts” having the same number of interconnected cuts (named C-cut gel) were chosen. The fracture tests of D-cut gel and C-cut gel with different cut patterns were performed. The fracture observation revealed that crack blunting occurred at each cut tip, and a large wrinkle-like zone was formed where the wrinkles were parallel to the propagation direction of the cut. By utilizing homemade circular polarizing optical systems, we found that introducing dispersed cuts increases the rupture force by homogenizing the stress around the crack tip surrounding every cut, which reduces stress concentration in one certain cut. We believe this work reveals the fracture mechanism of tough soft materials with a kirigami cut structure, which should guide the design of advanced soft and tough materials along this line. Full article

(This article belongs to the Special Issue Properties and Structure of Hydrogel-Related Materials)

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14 pages, 1927 KiB

Open AccessArticle

Detection of Gel-Forming Polymers via Calcium Crosslinking, Applied to the Screening of Extracellular Polymeric Substances Extracted from Biological Aggregates

by Abdo Bou-Sarkis, Etienne Paul, Elisabeth Girbal-Neuhauser, Nicolas Derlon and Yolaine Bessiere

Gels 2023, 9(2), 157; https://doi.org/10.3390/gels9020157 - 16 Feb 2023

Cited by 1 | Viewed by 1680

Abstract

The valorization of biological aggregates through the extraction of hydrogel-forming polymers can enhance the economics and sustainability of various processes in which bacteria are involved in organic waste transformation, such as wastewater treatment. Achieving these goals requires the development of a method capable [...] Read more.

The valorization of biological aggregates through the extraction of hydrogel-forming polymers can enhance the economics and sustainability of various processes in which bacteria are involved in organic waste transformation, such as wastewater treatment. Achieving these goals requires the development of a method capable of detecting the presence of gel-forming polymers in complex mixtures containing biopolymers that are most often unknown and uncharacterized. A miniaturized screening method capable of detecting gelation via ionic crosslinking using only 1 to 3 mg of the tested samples (commercial molecules or extracellular polymeric substances, EPSs) is proposed. The method consists of calculating a percentage of reactivity (%R) through UV-vis spectra and determining the percentage of gel volume (%Vg) formed after the addition of calcium. Both factors were combined to give a gelling factor (GF), and the test was applied to pure commercial molecules (BSA, DNA, alginate (ALV), and a mixture of them), allowing the classification of the following solutions according to their gel-forming capacity: GF_(ALV) > GF_(ALV+DNA) > GF_{(BSA+ALV+DNA)} > GF_(BSA+ALV) > GF_(DNA) > GF_(BSA+DNA) > GF_(BSA). As a relevant tool for screening hydrogel-forming solutions, the method was applied to the EPS extracted from aerobic granular sludge. The EPS (0.5% w/v) had a GF of 0.16 ± 0.03, equivalent to approximately half of the GF of ALV (0.38 ± 0.02 at 0.5% w/v). The developed test pushes the limits of the existing gel-detection techniques because it allows for quicker, less consuming, and more informative gelation detection through the use of simple methods that do not require sophisticated equipment. Full article

(This article belongs to the Special Issue Preparation, Properties and Applications of Functional Hydrogels)

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18 pages, 4815 KiB

Open AccessArticle

Preparation and Performance Evaluation of a Self-Crosslinking Emulsion-Type Fracturing Fluid for Quasi-Dry CO₂ Fracturing

by Jiani Hu, Meilong Fu, Minxuan Li, Yan Zheng, Guojun Li and Baofeng Hou

Gels 2023, 9(2), 156; https://doi.org/10.3390/gels9020156 - 15 Feb 2023

Cited by 2 | Viewed by 1472

Abstract

Quasi-dry CO₂ fracturing technology is a new CO₂ fracturing technology that combines liquid CO₂ fracturing (dry CO₂ fracturing) and water-based fracturing. It uses a liquid CO₂ system containing a small amount of water-based fracturing fluid to carry sand, [...] Read more.

Quasi-dry CO₂ fracturing technology is a new CO₂ fracturing technology that combines liquid CO₂ fracturing (dry CO₂ fracturing) and water-based fracturing. It uses a liquid CO₂ system containing a small amount of water-based fracturing fluid to carry sand, and it is characterized by sand blending at normal pressure, convenient preparation, the integrated application of resistance reduction and sand carrying, and no dedicated closed sand blender requirement. We developed a self-crosslinking emulsion-type water-based fracturing fluid (ZJL-1), which contained ionic bonds, hydrogen bonds, van der Waals forces, and hydrophobic associations, for quasi-dry CO₂ fracturing, and the comprehensive properties of the ZJL-1 fracturing fluid were evaluated. The results showed that the ZJL-1 fracturing fluid had obvious viscoelastic characteristics, a heat loss rate of less than 10% at 200 °C, a good thermal stability, sufficient rheology under high temperature and high shear conditions, and a good thermal stability. The resistance reduction rate reached 70%, which demonstrates a good resistance reduction performance. Compared with conventional guar fracturing fluid, ZJL-1 can carry more sand and has a lower core damage rate. The on-site use of quasi-dry fracturing showed that optimizing the mixing ratio of liquid CO₂ fracturing fluid and ZJL-1 fracturing fluid effectively enhanced oil and gas recovery. This can be used to optimize quasi-dry fracturing and can be used as a reference. Full article

(This article belongs to the Special Issue Recent Advances in Polymeric Gel for Geo-Energy Recovery)

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15 pages, 6223 KiB

Open AccessArticle

Enhancing Conductivity and Self-Healing Properties of PVA/GEL/OSA Composite Hydrogels by GO/SWNTs for Electronic Skin

by Xiaohu Chen, Haonan Zhang, Jiashu Cui, Yanen Wang, Mingyang Li, Juan Zhang, Changgeng Wang, Zhisheng Liu and Qinghua Wei

Gels 2023, 9(2), 155; https://doi.org/10.3390/gels9020155 - 15 Feb 2023

Cited by 3 | Viewed by 1660

Abstract

The use of flexible, self-healing conductive hydrogels as a type of typical electronic skin with the function of transmitting sensory signals has attracted wide attention in the field of biomaterials. In this study, composite hydrogels based on polyvinyl alcohol (PVA), gelatin (GEL), oxidized [...] Read more.

The use of flexible, self-healing conductive hydrogels as a type of typical electronic skin with the function of transmitting sensory signals has attracted wide attention in the field of biomaterials. In this study, composite hydrogels based on polyvinyl alcohol (PVA), gelatin (GEL), oxidized sodium alginate (OSA), graphene oxide (GO), and single-walled carbon nanotubes (SWNTs) were successfully prepared. The hydrogen and imine bonding of the composite hydrogels gives them excellent self-healing properties. Their self-healing properties restore 68% of their breaking strength and over 95% of their electrical conductivity. The addition of GO and SWNTs enables the PGO-GS hydrogels to achieve a compressive modulus and conductivity of 42.2 kPa and 29.6 mS/m, which is 8.2 times and 1.5 times that of pure PGO, respectively. Furthermore, the PGO-GS hydrogels can produce profound feedback signals in response to deformation caused by external forces and human movements such as finger flexion and speech. In addition, the PGO-GS hydrogels exhibit superior biocompatibility compared to PGO. All of these results indicate that the PGO-GS hydrogels have great potential with respect to future applications in the field of electronic skin. Full article

(This article belongs to the Special Issue Modification of Hydrogels and Their Applications in Biomedical Engineering)

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16 pages, 2772 KiB

Open AccessArticle

Amino-Functionalized Cellulose Nanofiber/Lignosulfonate New Aerogel Adsorbent for the Removal of Dyes and Heavy Metals from Wastewater

by Islam Elsayed, Gregory T. Schueneman, Emad M. El-Giar and El Barbary Hassan

Gels 2023, 9(2), 154; https://doi.org/10.3390/gels9020154 - 14 Feb 2023

Cited by 15 | Viewed by 2470

Abstract

Due to the increasingly widespread water pollutants and the high cost of treatment methods, there is a demand for new, inexpensive, renewable, and biodegradable adsorbent materials for the purification of wastewater contaminants. In this study, a new biocomposite aerogel (Amf-CNF/LS) was prepared using [...] Read more.

Due to the increasingly widespread water pollutants and the high cost of treatment methods, there is a demand for new, inexpensive, renewable, and biodegradable adsorbent materials for the purification of wastewater contaminants. In this study, a new biocomposite aerogel (Amf-CNF/LS) was prepared using a chemically cross-linking method between the amino-functionalized cellulose nanofibers (Amf-CNF) and lignosulfonates (LS). The physical and chemical properties of the prepared aerogel were investigated using several techniques including elemental analysis, scanning electron microscopy (SEM-EDS), Fourier transform infrared spectroscopy (FTIR), thermal gravimetric analysis (TGA), and N₂ adsorption-desorption analysis. The Amf-CNF/LS aerogel was then applied for the removal of methylene blue (MB), rhodamine B dye (RhB), and the heavy metal cadmium ion (Cd²⁺) from synthetic wastewater solutions. The adsorption parameters controlling the adsorption process including the pH, contact time, adsorbent dosage, and adsorbate concen-tration were optimized. High adsorption kinetics and isotherms were observed, with the adsorption isotherms of the Amf-CNF/LS aerogel fitting the Langmuir model with maximum adsorption capacities of 170.94, 147.28, and 129.87 mg/g for MB, RhB, and Cd²⁺, respectively. These results show that Amf-CNF/LS aerogel is a promising green and inexpensive adsorbent for MB, RhB, and Cd²⁺ removal from wastewater. Full article

(This article belongs to the Special Issue Recent Advances in Aerogel-Based Composites)

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41 pages, 6482 KiB

Open AccessReview

Nanocomposite Hydrogels as Functional Extracellular Matrices

by Stijn Jooken, Olivier Deschaume and Carmen Bartic

Gels 2023, 9(2), 153; https://doi.org/10.3390/gels9020153 - 13 Feb 2023

Cited by 4 | Viewed by 2135

Abstract

Over recent years, nano-engineered materials have become an important component of artificial extracellular matrices. On one hand, these materials enable static enhancement of the bulk properties of cell scaffolds, for instance, they can alter mechanical properties or electrical conductivity, in order to better [...] Read more.

Over recent years, nano-engineered materials have become an important component of artificial extracellular matrices. On one hand, these materials enable static enhancement of the bulk properties of cell scaffolds, for instance, they can alter mechanical properties or electrical conductivity, in order to better mimic the in vivo cell environment. Yet, many nanomaterials also exhibit dynamic, remotely tunable optical, electrical, magnetic, or acoustic properties, and therefore, can be used to non-invasively deliver localized, dynamic stimuli to cells cultured in artificial ECMs in three dimensions. Vice versa, the same, functional nanomaterials, can also report changing environmental conditions—whether or not, as a result of a dynamically applied stimulus—and as such provide means for wireless, long-term monitoring of the cell status inside the culture. In this review article, we present an overview of the technological advances regarding the incorporation of functional nanomaterials in artificial extracellular matrices, highlighting both passive and dynamically tunable nano-engineered components. Full article

(This article belongs to the Section Gel Chemistry and Physics)

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37 pages, 17529 KiB

Open AccessArticle

Phosphonation of Alginate–Polyethyleneimine Beads for the Enhanced Removal of Cs(I) and Sr(II) from Aqueous Solutions

by Khalid A. M. Salih, Kanggen Zhou, Mohammed F. Hamza, Hamed Mira, Yuezhou Wei, Shunyan Ning, Eric Guibal and Waheed M. Salem

Gels 2023, 9(2), 152; https://doi.org/10.3390/gels9020152 - 11 Feb 2023

Cited by 4 | Viewed by 2056

Abstract

Although Cs(I) and Sr(II) are not strategic and hazardous metal ions, their recovery from aqueous solutions is of great concern for the nuclear industry. The objective of this work consists of designing a new sorbent for the simultaneous recovery of these metals with [...] Read more.

Although Cs(I) and Sr(II) are not strategic and hazardous metal ions, their recovery from aqueous solutions is of great concern for the nuclear industry. The objective of this work consists of designing a new sorbent for the simultaneous recovery of these metals with selectivity against other metals. The strategy is based on the functionalization of algal/polyethyleneimine hydrogel beads by phosphonation. The materials are characterized by textural, thermo-degradation, FTIR, elemental, titration, and SEM-EDX analyses to confirm the chemical modification. To evaluate the validity of this modification, the sorption of Cs(I) and Sr(II) is compared with pristine support under different operating conditions: the pH effect, kinetics, and isotherms are investigated in mono-component and binary solutions, before investigating the selectivity (against competitor metals) and the possibility to reuse the sorbent. The functionalized sorbent shows a preference for Sr(II), enhanced sorption capacities, a higher stability at recycling, and greater selectivity against alkali, alkaline-earth, and heavy metal ions. Finally, the sorption properties are compared for Cs(I) and Sr(II) removal in a complex solution (seawater sample). The combination of these results confirms the superiority of phosphonated sorbent over pristine support with promising performances to be further evaluated with effluents containing radionuclides. Full article

(This article belongs to the Special Issue Innovative Biopolymer-Based Hydrogels)

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19 pages, 8417 KiB

Open AccessArticle

Rheological Performance of High-Temperature-Resistant, Salt-Resistant Fracturing Fluid Gel Based on Organic-Zirconium-Crosslinked HPAM

by Hui Xin, Bo Fang, Luyao Yu, Yongjun Lu, Ke Xu and Kejing Li

Gels 2023, 9(2), 151; https://doi.org/10.3390/gels9020151 - 11 Feb 2023

Cited by 5 | Viewed by 1706

Abstract

Development of low-cost, high-temperature-resistant and salt-resistant fracturing fluids is a hot and difficult issue in reservoir fluids modification. In this study, an organic zirconium crosslinker that was synthesized and crosslinked with partially hydrolyzed polyacrylamide (HPAM) was employed as a cost-effective polymer thickener to [...] Read more.

Development of low-cost, high-temperature-resistant and salt-resistant fracturing fluids is a hot and difficult issue in reservoir fluids modification. In this study, an organic zirconium crosslinker that was synthesized and crosslinked with partially hydrolyzed polyacrylamide (HPAM) was employed as a cost-effective polymer thickener to synthesize a high-temperature-resistant and salt-resistant fracturing fluid. The rheological properties of HPAM in tap water solutions and 2 × 10⁴ mg/L salt solutions were analyzed. The results demonstrated that addition of salt reduced viscosity and viscoelasticity of HPAM solutions. Molecular dynamics (MD) simulation results indicated that, due to electrostatic interaction, the carboxylate ions of HPAM formed an ionic bridge with metal cations, curling the conformation, decreasing the radius of rotation and thus decreasing viscosity. However, optimizing fracturing fluids formulation can mitigate the detrimental effects of salt on HPAM. The rheological characteristics of the HPAM fracturing fluid crosslinking process were analyzed and a crosslinking rheological kinetic equation was established under small-amplitude oscillatory shear (SAOS) test. The results of a large-amplitude oscillation shear (LAOS) test indicate that the heating effect on crosslinking is stronger than the shear effect on crosslinking. High-temperature-resistant and shear-resistant experiments demonstrated good performance of fracturing fluids of tap water and salt solution at 200 °C and 180 °C. Full article

(This article belongs to the Special Issue Advanced Gels for Oil Recovery)

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17 pages, 1893 KiB

Open AccessArticle

Organogel of Acai Oil in Cosmetics: Microstructure, Stability, Rheology and Mechanical Properties

by Suellen Christtine da Costa Sanches, Maria Inês Ré, José Otávio Carréra Silva-Júnior and Roseane Maria Ribeiro-Costa

Gels 2023, 9(2), 150; https://doi.org/10.3390/gels9020150 - 10 Feb 2023

Cited by 4 | Viewed by 1662

Abstract

Organogel (OG) is a semi-solid material composed of gelling molecules organized in the presence of an appropriate organic solvent, through physical or chemical interactions, in a continuous net. This investigation aimed at preparing and characterizing an organogel from acai oil with hyaluronic acid [...] Read more.

Organogel (OG) is a semi-solid material composed of gelling molecules organized in the presence of an appropriate organic solvent, through physical or chemical interactions, in a continuous net. This investigation aimed at preparing and characterizing an organogel from acai oil with hyaluronic acid (HA) structured by 12-hydroxystearic acid (12-HSA), aiming at topical anti-aging application. Organogels containing or not containing HA were analyzed by Fourier-transform Infrared Spectroscopy, polarized light optical microscopy, thermal analysis, texture analysis, rheology, HA quantification and oxidative stability. The organogel containing hyaluronic acid (OG + HA) has a spherulitic texture morphology with a net-like structure and absorption bands that evidenced the presence of HA in the three-dimensional net of organogel. The thermal analysis confirmed the gelation and the insertion of HA, as well as a good thermal stability, which is also confirmed by the study of oxidative stability carried out under different temperature conditions for 90 days. The texture and rheology studies indicated a viscoelastic behavior. HA quantification shows the efficiency of the HA cross-linking process in the three-dimensional net of organogel with 11.22 µg/mL for cross-linked HA. Thus, it is concluded that OG + HA shows potentially promising physicochemical characteristics for the development of a cosmetic system. Full article

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11 pages, 1509 KiB

Open AccessTechnical Note

Crosslinking of Bovine Gelatin Gels by Genipin Revisited Using Ferrule-Top Micro-Indentation

by Vincent Ball

Gels 2023, 9(2), 149; https://doi.org/10.3390/gels9020149 - 10 Feb 2023

Viewed by 1124

Abstract

(1) Background: Gelatin is widely used in food science, bioengineering, and as a sealant. However, for most of those applications, the mechanical properties of gelatin gels need to be improved by means of physical or chemical crosslinking. Among the used chemical agents, genipin [...] Read more.

(1) Background: Gelatin is widely used in food science, bioengineering, and as a sealant. However, for most of those applications, the mechanical properties of gelatin gels need to be improved by means of physical or chemical crosslinking. Among the used chemical agents, genipin allows low cytotoxicity in addition to improved Young’s modulus. However, the mechanical properties of gelatin–genipin gels have only been investigated at the macroscale, and there is no knowledge of the influence of the genipin concentration on the surface homogeneity of Young’s modulus. (2) Methods: To this aim, the influence of genipin concentration on Young’s modulus of gelatin gels was investigated by means of ferrule-top micro-indentation. The data were compared with storage moduli obtained by shear rheology data. (3) Results: Ferrule-top indentation measurements allowed us to show that Young’s moduli of gelatin–genipin gels increase up to a plateau value after approximately 12 mg/mL in genipin and 4 h of crosslinking. Young’s moduli distribute with high homogeneity over 80 µm × 80 µm surface areas and are consistent with the storage moduli obtained by shear rheology. (4) Conclusions: It has been shown that ferrule-top indentation data fitted with the Hertz model yield Young’s moduli of gelatin–genipin gels which are consistent with the storage moduli obtained by characterization at the macroscale using shear rheometry. In addition, Young’s moduli are homogenously distributed (with some irregularities at the highest genipin concentrations) and can be increased by two orders of magnitude with respect to the uncrosslinked gel. Full article

(This article belongs to the Special Issue Structured Gels: Mechanics, Responsivity and Applications)

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11 pages, 1668 KiB

Open AccessArticle

Stiffness-Modulation of Collagen Gels by Genipin-Crosslinking for Cell Culture

by Seiichiro Ishihara, Haruna Kurosawa and Hisashi Haga

Gels 2023, 9(2), 148; https://doi.org/10.3390/gels9020148 - 10 Feb 2023

Cited by 5 | Viewed by 2686

Abstract

The stiffness of extracellular matrices (ECMs) is critical for cellular functions. Therefore, modulating the stiffness of ECMs in vitro is necessary to investigate the role of stiffness in cellular phenomena. Collagen gels are widely used for cell culture matrices in vitro. However, modulation [...] Read more.

The stiffness of extracellular matrices (ECMs) is critical for cellular functions. Therefore, modulating the stiffness of ECMs in vitro is necessary to investigate the role of stiffness in cellular phenomena. Collagen gels are widely used for cell culture matrices in vitro. However, modulation of the stiffness in collagen gels for cell culture is challenging owing to the limited knowledge of the method to increase the stiffness while maintaining low cytotoxicity. Here, we established a novel method to modulate collagen gel stiffness from 0.0292 to 12.5 kPa with low cytotoxicity. We prepared collagens with genipin, a low-cytotoxic crosslinker of amines, at different concentrations and successfully modulated the stiffness of the gels. In addition, on 10 mM genipin-mixed collagen gels (approximately 12.5 kPa), H1299 human lung cancer cells showed spreading morphology and nuclear localization of yes-associated protein (YAP), typical phenomena of cells on stiff ECMs. Mouse mesenchymal stromal cells on 10 mM genipin-mixed collagen gels differentiated to vascular smooth muscle cells. On the other hand, the cells on 0 mM genipin-mixed collagen gels (approximately 0.0292 kPa) differentiated to visceral smooth muscle cells. Our new method provides a novel way to prepare stiffness-modulated collagen gels with low cytotoxicity in cell culture. Full article

(This article belongs to the Special Issue Hydrogels with Appropriate/Tunable Properties for Biomedical Applications)

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29 pages, 5462 KiB

Open AccessArticle

Preparation, Characterization, and Evaluation of Cytotoxicity of Fast Dissolving Hydrogel Based Oral Thin Films Containing Pregabalin and Methylcobalamin

by Emrah Özakar, Rukiye Sevinç-Özakar and Bilal Yılmaz

Gels 2023, 9(2), 147; https://doi.org/10.3390/gels9020147 - 09 Feb 2023

Cited by 3 | Viewed by 3590

Abstract

The oral availability of many drugs is problematic due to the pH of the stomach, enzymes, and first-pass effects through the liver. However, especially geriatric, pediatric, bedridden, or mentally handicapped patients and those with dysphagia have difficulty swallowing or chewing solid dosage forms. [...] Read more.

The oral availability of many drugs is problematic due to the pH of the stomach, enzymes, and first-pass effects through the liver. However, especially geriatric, pediatric, bedridden, or mentally handicapped patients and those with dysphagia have difficulty swallowing or chewing solid dosage forms. Oral Thin Films (OTFs) are one of the new drug delivery systems that can solve these problems. Pregabalin (PG) and Methylcobalamin (MC), which are frequently preferred for pain originating in the central nervous system, were brought together for the first time using OTF technology in this study. In this study, a quantification method for PG and MC was developed and validated simultaneously. Optimum formulations were selected with organoleptic and morphological controls, moisture absorption capacity, swelling capacity, percent elongation, foldability, pH, weight variability, thickness, disintegration time, and transparency tests on OTFs prepared by the solvent pouring method. Content uniformity, dissolution rate, determination of release kinetics, SEM, XRD, FT-IR, DSC, long-term stability, and cytotoxicity studies on the tongue epithelial cell line (SCC-9) were performed on selected OTFs. As a result, OTFs containing PG-MC, which are non-toxic, highly flexible, transparent, compatible with intraoral pH, with fast disintegration time (<30 s), and acceptable in taste and appearance, have been developed successfully. Full article

(This article belongs to the Special Issue The Role of Mucus Gel Layer in Drug and Nutraceutical Delivery)

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30 pages, 3803 KiB

Open AccessReview

Applications of Hydrogels in Drug Delivery for Oral and Maxillofacial Diseases

by Lijia Liu, Dan Wu, Heng Tu, Mengjiao Cao, Mengxin Li, Li Peng and Jing Yang

Gels 2023, 9(2), 146; https://doi.org/10.3390/gels9020146 - 09 Feb 2023

Cited by 6 | Viewed by 3508

Abstract

Oral and maxillofacial diseases have an important impact on local function, facial appearance, and general health. As a multifunctional platform, hydrogels are widely used in the biomedical field due to their excellent physicochemical properties. In recent years, a large number of studies have [...] Read more.

Oral and maxillofacial diseases have an important impact on local function, facial appearance, and general health. As a multifunctional platform, hydrogels are widely used in the biomedical field due to their excellent physicochemical properties. In recent years, a large number of studies have been conducted to adapt hydrogels to the complex oral and maxillofacial environment by modulating their pore size, swelling, degradability, stimulus-response properties, etc. Meanwhile, many studies have attempted to use hydrogels as drug delivery carriers to load drugs, cytokines, and stem cells for antibacterial, anticancer, and tissue regeneration applications in oral and maxillofacial regions. This paper reviews the application and research progress of hydrogel-based drug delivery systems in the treatment of oral and maxillofacial diseases such as caries, endodontic diseases, periodontal diseases, maxillofacial bone diseases, mucosal diseases, oral cancer, etc. The characteristics and applications of hydrogels and drug-delivery systems employed for the treatment of different diseases are discussed in order to provide a reference for further research on hydrogel drug-delivery systems in the future. Full article

(This article belongs to the Special Issue Gels: Applications in Drug Delivery and Tissue Engineering)

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19 pages, 5877 KiB

Open AccessArticle

Metal-Coordinated Dynamics and Viscoelastic Properties of Double-Network Hydrogels

by Shilei Zhu, Yan Wang, Zhe Wang, Lin Chen, Fengbo Zhu, Yanan Ye, Yong Zheng, Wenwen Yu and Qiang Zheng

Gels 2023, 9(2), 145; https://doi.org/10.3390/gels9020145 - 09 Feb 2023

Cited by 2 | Viewed by 1543

Abstract

Biological soft tissues are intrinsically viscoelastic materials which play a significant role in affecting the activity of cells. As potential artificial alternatives, double-network (DN) gels, however, are pure elastic and mechanically time independent. The viscoelasticization of DN gels is an urgent challenge in [...] Read more.

Biological soft tissues are intrinsically viscoelastic materials which play a significant role in affecting the activity of cells. As potential artificial alternatives, double-network (DN) gels, however, are pure elastic and mechanically time independent. The viscoelasticization of DN gels is an urgent challenge in enabling DN gels to be used for advanced development of biomaterial applications. Herein, we demonstrate a simple approach to regulate the viscoelasticity of tough double-network (DN) hydrogels by forming sulfonate–metal coordination. Owing to the dynamic nature of the coordination bonds, the resultant hydrogels possess highly viscoelastic, mechanical time-dependent, and self-recovery properties. Rheological measurements are performed to investigate the linear dynamic mechanical behavior at small strains. The tensile tests and cyclic tensile tests are also systematically performed to evaluate the rate-dependent large deformation mechanical behaviors and energy dissipation behaviors of various ion-loaded DN hydrogels. It has been revealed based on the systematic analysis that robust strong sulfonate–Zr⁴⁺ coordination interactions not only serve as dynamic crosslinks imparting viscoelastic rate-dependent mechanical performances, but also strongly affect the relative strength of the first PAMPS network, thereby increasing the yielding stress σ_y and the fracture stress at break σ_b and reducing the stretch ratio at break λ_b. It is envisioned that the viscoelasticization of DN gels enables versatile applications in the biomedical and engineering fields. Full article

(This article belongs to the Special Issue Properties and Structure of Hydrogel-Related Materials)

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18 pages, 6973 KiB

Open AccessReview

Recent Progress in Hydrogel-Based Synthetic Cartilage: Focus on Lubrication and Load-Bearing Capacities

by Fei Qiu, Xiaopeng Fan, Wen Chen, Chunming Xu, Yumei Li and Renjian Xie

Gels 2023, 9(2), 144; https://doi.org/10.3390/gels9020144 - 08 Feb 2023

Cited by 3 | Viewed by 2979

Abstract

Articular cartilage (AC), which covers the ends of bones in joints, particularly the knee joints, provides a robust interface to maintain frictionless movement during daily life due to its remarkable lubricating and load-bearing capacities. However, osteoarthritis (OA), characterized by the progressive degradation of [...] Read more.

Articular cartilage (AC), which covers the ends of bones in joints, particularly the knee joints, provides a robust interface to maintain frictionless movement during daily life due to its remarkable lubricating and load-bearing capacities. However, osteoarthritis (OA), characterized by the progressive degradation of AC, compromises the properties of AC and thus leads to frayed and rough interfaces between the bones, which subsequently accelerates the progression of OA. Hydrogels, composed of highly hydrated and interconnected polymer chains, are potential candidates for AC replacement due to their physical and chemical properties being similar to those of AC. In this review, we summarize the recent progress of hydrogel-based synthetic cartilage, or cartilage-like hydrogels, with a particular focus on their lubrication and load-bearing properties. The different formulations, current limitations, and challenges of such hydrogels are also discussed. Moreover, we discuss the future directions of hydrogel-based synthetic cartilage to repair and even regenerate the damaged AC. Full article

(This article belongs to the Special Issue Advanced Hydrogels for Regenerative Medicine and Tissue Engineering)

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15 pages, 2123 KiB

Open AccessArticle

Pluronics-Based Drug Delivery Systems for Flavonoids Anticancer Treatment

by Sylwia Ronka, Aleksandra Kowalczyk, Dagmara Baczyńska and Anna K. Żołnierczyk

Gels 2023, 9(2), 143; https://doi.org/10.3390/gels9020143 - 08 Feb 2023

Cited by 4 | Viewed by 1755

Abstract

This research concerns the investigation of the preparation of polymeric nanocarriers containing a flavonoid—naringenin, xanthohumol or isoxanthohumol—based on Pluronics by the thin-film formation method. The size of the formed micelles and their stability upon dilution were evaluated using Dynamic light scattering (DLS) analysis; [...] Read more.

This research concerns the investigation of the preparation of polymeric nanocarriers containing a flavonoid—naringenin, xanthohumol or isoxanthohumol—based on Pluronics by the thin-film formation method. The size of the formed micelles and their stability upon dilution were evaluated using Dynamic light scattering (DLS) analysis; the high values of the drug loading and the encapsulation efficiency confirmed that the proposed systems of flavonoids delivery consisting of Pluronic P123 and F127 nanomicelles could effectively distribute the drug into tumour tissues, which makes these nanocarriers ideal candidates for passive targeting of cancer cells by the enhanced permeation and retention (EPR) effect. The in vitro cytotoxicity of proposed flavonoids in the Pluronic formulations was investigated by the SRB assay with human colon cancer cells. We designed mixed polymeric micelles, which was a successful drug delivery system for the case of naringenin not being able to enhance the bioavailability and cytotoxic activity of xanthohumol and isoxanthohumol. Furthermore, it was observed that the higher amount of polymer in the formulation achieved better cytotoxic activity. Full article

(This article belongs to the Special Issue Nanosized Gel as a Drug Delivery System)

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15 pages, 8157 KiB

Open AccessArticle

Effect of Storage Time and Temperature on Digestibility, Thermal, and Rheological Properties of Retrograded Rice

by Ishita Chakraborty, Indira Govindaraju, Steffi Kunnel, Vishwanath Managuli and Nirmal Mazumder

Gels 2023, 9(2), 142; https://doi.org/10.3390/gels9020142 - 08 Feb 2023

Cited by 8 | Viewed by 4080

Abstract

Retrogradation is defined as the recrystallization or realignment of amylose and amylopectin chains upon cooling of gelatinization starch gels. The storage conditions such as the storage time and temperature are crucial factors that influence and govern the degree of retrogradation and in turn, [...] Read more.

Retrogradation is defined as the recrystallization or realignment of amylose and amylopectin chains upon cooling of gelatinization starch gels. The storage conditions such as the storage time and temperature are crucial factors that influence and govern the degree of retrogradation and in turn, affect the formation of resistant starch and alteration of thermal and rheological properties. This article investigates the effect of storage time and temperature on the properties of retrograded rice starch. Rice kernels of five different indigenous varieties, namely Diasang lahi, Khaju lahi, Dhusuri bao, Omkar, and Bili rajamudi were cooked by boiling in water and stored at 4 °C and −20 °C for 6 and 12 h, respectively. Differential scanning calorimetry (DSC) studies revealed in raw form that Bili rajamudi exhibited the highest peak gelatinization temperature (T_p, °C) at 79.05 °C whereas Diasang lahi showed the least T_p at 56.12 °C. Further, it was indicated that the T_p and degree of retrogradation (DR%) also increase with increasing time and decreasing temperature of storage. All samples stored at −20 °C for 12 h exhibited the highest degree of retrogradation DR%. Amongst all five varieties stored at −20 °C for 12 h, Omkar exhibited the highest %DR, followed by Bili rajamudi, Khaju lahi, Dhusuri bao, and Diasang lahi. A negative correlation was also established between T_p and resistant starch content (RS%). It was also observed that the resistant starch (RS%) content increased with the increasing time and decreasing temperature of storage. A strong negative correlation was observed between RS% and non-resistant starch (NRS%). Further, rheological studies indicated that retrogradation also affects the viscosity and dynamic rheological properties of starch. In this study, it was evident that extending storage duration from 6 to 12 h and lowering temperature from 4 to −20 °C impact retrogradation of rice starch, which in turn affects the starch’s gelatinization, digestibility, and rheology. Rice starch retrograded at lower temperatures for a longer period could prove to be extremely beneficial for development of food products with better textural properties and high RS content or low glycemic index. Full article

(This article belongs to the Section Gel Analysis and Characterization)

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13 pages, 7739 KiB

Open AccessArticle

Construction of Engineered Muscle Tissue Consisting of Myotube Bundles in a Collagen Gel Matrix

by Kazuya Furusawa, Yuuki Kawahana and Ryoya Miyashita

Gels 2023, 9(2), 141; https://doi.org/10.3390/gels9020141 - 08 Feb 2023

Viewed by 2004

Abstract

Tissue engineering methods that aim to mimic the hierarchical structure of skeletal muscle tissue have been widely developed due to utilities in various fields of biology, including regenerative medicine, food technology, and soft robotics. Most methods have aimed to reproduce the microscopical morphology [...] Read more.

Tissue engineering methods that aim to mimic the hierarchical structure of skeletal muscle tissue have been widely developed due to utilities in various fields of biology, including regenerative medicine, food technology, and soft robotics. Most methods have aimed to reproduce the microscopical morphology of skeletal muscles, such as the orientation of myotubes and the sarcomere structure, and there is still a need to develop a method to reproduce the macroscopical morphology. Therefore, in this study, we aim to establish a method to reproduce the macroscopic morphology of skeletal muscle by constructing an engineered muscle tissue (EMT) by culturing embryonic chicken myoblast-like cells that are unidirectionally aligned in collagen hydrogels with micro-channels (i.e., MCCG). Whole mount fluorescent imaging of the EMT showed that the myotubes were unidirectionally aligned and that they were bundled in the collagen gel matrix. The myotubes contracted in response to periodic electrostimulations with a frequency range of 0.5–2.0 Hz, but not at 5.0 Hz. Compression tests of the EMT showed that the EMT had anisotropic elasticity. In addition, by measuring the relaxation moduli of the EMTs, an anisotropy of relaxation strengths was observed. The observed anisotropies could be attributed to differences in maturation and connectivity of myotubes in the directions perpendicular and parallel to the long axis of the micro-channels of the MCCG. Full article

(This article belongs to the Special Issue Shaping and Structuring of Polymer Gels)

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