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Gels, Volume 7, Issue 3 (September 2021) – 70 articles

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Review
3D Bioprinting of Hydrogels for Cartilage Tissue Engineering
Gels 2021, 7(3), 144; https://doi.org/10.3390/gels7030144 (registering DOI) - 16 Sep 2021
Abstract
Three-dimensional (3D) bioprinting is an emerging technology based on 3D digital imaging technology and multi-level continuous printing. The precise positioning of biological materials, seed cells, and biological factors, known as “additive biomanufacturing”, can provide personalized therapy strategies in regenerative medicine. Over the last [...] Read more.
Three-dimensional (3D) bioprinting is an emerging technology based on 3D digital imaging technology and multi-level continuous printing. The precise positioning of biological materials, seed cells, and biological factors, known as “additive biomanufacturing”, can provide personalized therapy strategies in regenerative medicine. Over the last two decades, 3D bioprinting hydrogels have significantly advanced the field of cartilage and bone tissue engineering. This article reviews the development of 3D bioprinting and its application in cartilage tissue engineering, followed by a discussion of the current challenges and prospects for 3D bioprinting. This review presents foundational information on the future optimization of the design and manufacturing process of 3D additive biomanufacturing. Full article
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Article
Silica Xerogel Doped with Iron(III) as Sensor Material for Salicylhydroxamic Acid Determination in Urine
Gels 2021, 7(3), 143; https://doi.org/10.3390/gels7030143 (registering DOI) - 16 Sep 2021
Abstract
Salicylhydroxamic acid (SHA) is used as antimicrobic medicine and its concentration has to be monitored in urine. For the first time, silica xerogels doped with iron(III) have been proposed as sensor materials for SHA determination in biological samples. Three xerogels with iron(III) content [...] Read more.
Salicylhydroxamic acid (SHA) is used as antimicrobic medicine and its concentration has to be monitored in urine. For the first time, silica xerogels doped with iron(III) have been proposed as sensor materials for SHA determination in biological samples. Three xerogels with iron(III) content in the range of 0.04–1.74% wt have been synthesized. BET surface area of these xerogels has varied in the range of 696–529 m2/g and total pore volume has varied in the range of 0.92–0.23 cm3/g. Complex formation between immobilized iron(III) and salicylhydroxamic acid has been investigated with solid phase spectrophotometry and IR spectroscopy. Orange-brown iron(III)-SHA complex with 1:1 stoichiometry is formed at pH 1–4 with half-reaction time of 17 min. Silica xerogel doped with 0.33% wt iron(III)) has been used as sensor material for SHA solid phase spectrophotometric determination (LOD 1.4 mg/L (n = 3), analytical range 4–230 mg/L). Proposed sensor material has been applied for SHA determination in biological samples of synthetic and human urine. The proposed procedure is characterized by a good level of accuracy (recovery values 97–120%) and precision (RSD values 4–9%) and can be recommended for pharmacokinetic–pharmacodynamic studies of hydroxamic acid-based medications. Full article
(This article belongs to the Special Issue Advances in Xerogels)
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Article
Investigating the Role of the Catalyst within Resorcinol–Formaldehyde Gel Synthesis
Gels 2021, 7(3), 142; https://doi.org/10.3390/gels7030142 - 15 Sep 2021
Viewed by 140
Abstract
Resorcinol–formaldehyde (RF) gels are porous materials synthesized via a sol–gel reaction and subsequently dried, producing structures with high surface areas and low densities—properties that are highly attractive for use in various applications. The RF gel reaction takes place in the presence of a [...] Read more.
Resorcinol–formaldehyde (RF) gels are porous materials synthesized via a sol–gel reaction and subsequently dried, producing structures with high surface areas and low densities—properties that are highly attractive for use in various applications. The RF gel reaction takes place in the presence of a catalyst, either acidic or basic in nature, the concentration of which significantly impacts final gel properties. The full extent of the catalyst’s role, however, has been subject to debate, with the general consensus within the field being that it is simply a pH-adjuster. The work presented here explores this theory, in addition to other theories postulated in the literature, through the synthesis and analysis of RF gels catalysed by mixtures of relevant compounds with varying concentrations. The relationship between catalyst concentration and initial solution pH is decoupled, and the individual roles of both the cation and the anion within the catalyst are investigated. The results presented here point towards the significance of the metal cation within the RF gel reaction, with similar structural properties observed for gels synthesized at constant Na+ concentrations, regardless of the initial solution pH. Furthermore, through the use of alternative cations and anions within catalyst compounds, the potential effects of ions on the stabilization of macromolecules in solution are explored, the results of which suggest a ‘Hofmeister-like’ series could be applicable within the catalysis of RF gel reactions. Full article
(This article belongs to the Special Issue Advances in Xerogels)
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Article
Chemically Crosslinked Methylcellulose Substrates for Cell Sheet Engineering
Gels 2021, 7(3), 141; https://doi.org/10.3390/gels7030141 - 14 Sep 2021
Viewed by 152
Abstract
Methylcellulose (MC) hydrogels have been successfully proposed in the field of cell sheet engineering (CSE), allowing cell detachment from their surface by lowering the temperature below their transition temperature (Tt). Among the main limitations of pristine MC hydrogels, low physical stability [...] Read more.
Methylcellulose (MC) hydrogels have been successfully proposed in the field of cell sheet engineering (CSE), allowing cell detachment from their surface by lowering the temperature below their transition temperature (Tt). Among the main limitations of pristine MC hydrogels, low physical stability and mechanical performances limit the breadth of their potential applications. In this study, a crosslinking strategy based on citric acid (CA) was used to prepare thermoresponsive MC hydrogels, with different degrees of crosslinking, to exploit their possible use as substrates in CSE. The investigated amounts of CA did not cause any cytotoxic effect while improving the mechanical performance of the hydrogels (+11-fold increase in E, compared to control MC). The possibility to obtain cell sheets (CSs) was then demonstrated using murine fibroblast cell line (L929 cells). Cells adhered on crosslinked MC hydrogels’ surface in standard culture conditions and then were harvested at selected time points as single CSs. CS detachment was achieved simply by lowering the external temperature below the Tt of MC. The detached CSs displayed adhesive and proliferative activity when transferred to new plastic culture surfaces, indicating a high potential for regenerative purposes. Full article
(This article belongs to the Special Issue Hydrogel in Tissue Engineering and Regenerative Medicine)
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Article
Thermally Tunable Acoustic Beam Splitter Based on Poly(vinyl alcohol) Poly(N-isopropylacrylamide) Hydrogel
Gels 2021, 7(3), 140; https://doi.org/10.3390/gels7030140 - 13 Sep 2021
Viewed by 141
Abstract
In this study, we demonstrated a thermally tunable acoustic beam splitter using a poly(vinyl alcohol) poly(N-isopropylacrylamide) hydrogel (PVA-pNIPAM). The nature of PVA-pNIPAM hydrogel offers exceptional temperature-dependent physical properties due to its phase transition around its lower critical solution temperature. The acoustic impedance of [...] Read more.
In this study, we demonstrated a thermally tunable acoustic beam splitter using a poly(vinyl alcohol) poly(N-isopropylacrylamide) hydrogel (PVA-pNIPAM). The nature of PVA-pNIPAM hydrogel offers exceptional temperature-dependent physical properties due to its phase transition around its lower critical solution temperature. The acoustic impedance of the hydrogel can be tuned below, above, or matched to that of water by changing the environmental temperature. An acoustic wave propagating in water can be split into transmitted and reflected components by the PVA-pNIPAM hydrogel slab on varying its angle of incidence. The intensity ratio between the reflected and the transmitted componence can be adjusted by tuning the temperature of the medium. The acoustic beam can be entirely reflected at a temperature corresponding to the matched impedance between hydrogel and water. The beam-splitting behavior was observed for acoustic waves from both a monochromatic wave and broadband pulse source. In addition, the phase of beam split pulses can be reversed by selecting the hydrogel’s operating temperature. Full article
(This article belongs to the Special Issue Polymer Gels)
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Article
Comparative Physicochemical Analysis among 1,4-Butanediol Diglycidyl Ether Cross-Linked Hyaluronic Acid Dermal Fillers
Gels 2021, 7(3), 139; https://doi.org/10.3390/gels7030139 - 11 Sep 2021
Viewed by 219
Abstract
(1) Background: Injectable hyaluronic acid (HA) dermal fillers are used in several chirurgical practices and in aesthetic medicine. HA filler stability can be enhanced through different cross-linking technologies; one of the most frequently cross-linker used is 1,4-butanediol diglycidyl ether (BDDE), also present in [...] Read more.
(1) Background: Injectable hyaluronic acid (HA) dermal fillers are used in several chirurgical practices and in aesthetic medicine. HA filler stability can be enhanced through different cross-linking technologies; one of the most frequently cross-linker used is 1,4-butanediol diglycidyl ether (BDDE), also present in the HA-BDDE dermal filler family of the company Matex Lab S.p.A. (Brindisi, Italy). Our overview is focused on their characterization, drawing a correlation between matrix structure, rheological and physicochemical properties related to their cross-linking technologies. (2) Methods: Four different injectable HA hydrogels were characterized through optical microscopic examination and rheological behavior investigation. (3) Results: The cross-linked HA dermal fillers showed a fibrous “spiderweb-like” matrix structure and an elastic and solid-like profile. (4) Conclusions: The comparative analysis represents a preliminary characterization of these injectable medical devices in order to identify their best field of application. Full article
(This article belongs to the Special Issue Gels Horizons: From Science to Smart Materials)
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Article
Ovarian Cell Encapsulation in an Enzymatically Crosslinked Silk-Based Hydrogel with Tunable Mechanical Properties
Gels 2021, 7(3), 138; https://doi.org/10.3390/gels7030138 - 10 Sep 2021
Viewed by 239
Abstract
An artificial ovary is a promising approach for preserving fertility in prepubertal girls and women who cannot undergo current cryopreservation strategies. However, this approach is in its infancy, due to the possible challenges of creating a suitable 3D matrix for encapsulating ovarian follicles [...] Read more.
An artificial ovary is a promising approach for preserving fertility in prepubertal girls and women who cannot undergo current cryopreservation strategies. However, this approach is in its infancy, due to the possible challenges of creating a suitable 3D matrix for encapsulating ovarian follicles and stromal cells. To maintain the ovarian stromal cell viability and proliferation, as a first step towards developing an artificial ovary, in this study, a double network hydrogel with a high water swelling capacity (swelling index 15–19) was developed, based on phenol conjugated chitosan (Cs-Ph) and silk fibroin (SF) through an enzymatic crosslinking method using horseradish peroxidase. The addition of SF (1%) to Cs (1%) decreased the storage modulus (G’) from 3500 Pa (Cs1) to 1600 Pa (Cs-SF1), and the hydrogels with a rapid gelation kinetic produced a spatially homogeneous distribution of ovarian cells that demonstrated 167% proliferation after 7 days. This new Cs-SF hydrogel benefits from the toughness and flexibility of SF, and phenolic chemistry could provide the potential microstructure for encapsulating human ovarian stromal cells. Full article
(This article belongs to the Collection Feature Papers in Gel Materials)
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Article
Effect of Addition of Chokeberry Juice Concentrate and Foaming Agent on the Physical Properties of Agar Gel
Gels 2021, 7(3), 137; https://doi.org/10.3390/gels7030137 - 10 Sep 2021
Viewed by 158
Abstract
This study aimed to determine the effect of the addition of chokeberry juice concentrate (CJC) and foaming agent (egg albumin) with different percentages on the selected physical properties of agar gel. The agar gels with the addition of 5, 10, and 20% concentrations [...] Read more.
This study aimed to determine the effect of the addition of chokeberry juice concentrate (CJC) and foaming agent (egg albumin) with different percentages on the selected physical properties of agar gel. The agar gels with the addition of 5, 10, and 20% concentrations of chokeberry juice concentrate and with fructose addition were prepared. In addition, the foamed gels with different concentrations of egg albumin (in the range 0.5–2.0%) and CJC were produced. The water content, colour, density, hold-up and some mechanical and TPA (Texture Profile Analysis) descriptors as well some structural and acoustic emission parameters of non-aerated and foamed gels were analysed. The addition of CJC changed the colour of agar gel with fructose, the attractive appearance of the aerated gel was also linked with the addition of concentrate. The addition of 20% of CJC and foaming agent created samples with very low hardness, cohesiveness, and gumminess, and the structure of the aerated samples was characterised by the larger bubble diameter and the wider distribution of their size. The more promising texture and structure properties were obtained for samples with aerated gels with 5 and 10% addition of chokeberry juice concentrate. Full article
(This article belongs to the Special Issue Advanced Research in Food Gels)
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Review
Marine Biopolymer Dynamics, Gel Formation, and Carbon Cycling in the Ocean
Gels 2021, 7(3), 136; https://doi.org/10.3390/gels7030136 - 09 Sep 2021
Viewed by 174
Abstract
Much like our own body, our planet is a macroscale dynamic system equipped with a complex set of compartmentalized controls that have made life and evolution possible on earth. Many of these global autoregulatory functions take place in the ocean; paramount among those [...] Read more.
Much like our own body, our planet is a macroscale dynamic system equipped with a complex set of compartmentalized controls that have made life and evolution possible on earth. Many of these global autoregulatory functions take place in the ocean; paramount among those is its role in global carbon cycling. Understanding the dynamics of organic carbon transport in the ocean remains among the most critical, urgent, and least acknowledged challenges to modern society. Dissolved in seawater is one of the earth’s largest reservoirs of reduced organic carbon, reaching ~700 billion tons. It is composed of a polydisperse collection of marine biopolymers (MBP), that remain in reversible assembled↔dissolved equilibrium forming hydrated networks of marine gels (MG). MGs are among the least understood aspects of marine carbon dynamics. Despite the polymer nature of this gigantic pool of material, polymer physics theory has only recently been applied to study MBP dynamics and gel formation in the ocean. There is a great deal of descriptive phenomenology, rich in classifications, and significant correlations. Still missing, however, is the guide of robust physical theory to figure out the fundamental nature of the supramolecular interactions taking place in seawater that turn out to be critical to understanding carbon transport in the ocean. Full article
(This article belongs to the Special Issue Marine Gels)
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Article
Improved Gel Properties of Whey Protein-Stabilized Emulsions by Ultrasound and Enzymatic Cross-Linking
Gels 2021, 7(3), 135; https://doi.org/10.3390/gels7030135 - 09 Sep 2021
Viewed by 203
Abstract
This study investigated the effects of high-intensity ultrasound (HUS) and transglutaminase pretreatment on the gelation behavior of whey protein soluble aggregate (WPISA) emulsions. HUS pretreatment and TGase-mediated cross-linking delayed the onset of gelation but significantly increased (p < 0.05) the gel firmness [...] Read more.
This study investigated the effects of high-intensity ultrasound (HUS) and transglutaminase pretreatment on the gelation behavior of whey protein soluble aggregate (WPISA) emulsions. HUS pretreatment and TGase-mediated cross-linking delayed the onset of gelation but significantly increased (p < 0.05) the gel firmness (G′) both after gel formation at 25 °C and during storage at 4 °C. The frequency sweep test indicated that all gels had a similar frequency dependence at 4 and 25 °C, and the elasticity and viscosity of the WPISA-stabilized emulsion gel were significantly enhanced by HUS pretreatment and TGase-mediated cross-linking (p < 0.05). HUS and TGase-mediated cross-linking greatly improved the textural properties of WPISA-stabilized emulsion gels, as revealed by their increases in gel hardness, cohesiveness, resilience, and chewiness. HUS pretreatment and TGase-mediated cross-linking significantly increased the water-holding capacity but decreased the swelling ratios of the gels (p < 0.05). Interactive force analysis confirmed that noncovalent interactions, disulfide bonds, and TGase-induced covalent cross-links were all involved in the formation of gel networks. In conclusion, the combination of HUS and TGase-mediated cross-linking were beneficial for improving the gelation properties of WPISA-stabilized emulsion as a controlled release vehicle for potential food industrial applications. Full article
(This article belongs to the Special Issue Polymer Gels)
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Article
Fine-Tuning of Molecular Structures to Generate Carbohydrate Based Super Gelators and Their Applications for Drug Delivery and Dye Absorption
Gels 2021, 7(3), 134; https://doi.org/10.3390/gels7030134 - 07 Sep 2021
Viewed by 214
Abstract
Carbohydrate-based low molecular weight gelators (LMWGs) exhibit many desirable properties making them useful in various fields including applications as drug delivery carriers. In order to further understand the structural connection to gelation properties, especially the influence of halide substitutions, we have designed and [...] Read more.
Carbohydrate-based low molecular weight gelators (LMWGs) exhibit many desirable properties making them useful in various fields including applications as drug delivery carriers. In order to further understand the structural connection to gelation properties, especially the influence of halide substitutions, we have designed and synthesized a series of para-chlorobenzylidene acetal protected D-glucosamine amide derivatives. Fifteen different amides were synthesized, and their self-assembling properties were assessed in multiple organic solvents, as well as mixtures of organic solvents with water. All derivatives were found to be gelators for at least one solvent and majority formed gels in multiple solvents at concentrations lower than 2 wt%. A few derivatives rendered remarkably stable gels in aqueous solutions at concentrations below 0.1 wt%. The benzamide 13 formed gels in water and in EtOH/H2O (v/v 1:2) at 0.36 mg/mL. The gels were characterized using optical microscopy and atomic force microscopy, and the self-assembly mechanism was probed using variable temperature 1H-NMR spectroscopy. Gel extrusion studies using H2O/DMSO gels successfully printed lines of gels on glass slides, which retained viscoelasticity based on rheology. Gels formed by the benzamide 13 were used for encapsulation and the controlled release of chloramphenicol and naproxen, as well as for dye removal for toluidine blue aqueous solutions. Full article
(This article belongs to the Special Issue Gels Horizons: From Science to Smart Materials)
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Article
Effect of Biodegradable Hydrophilic and Hydrophobic Emulsifiers on the Oleogels Containing Sunflower Wax and Sunflower Oil
Gels 2021, 7(3), 133; https://doi.org/10.3390/gels7030133 - 07 Sep 2021
Viewed by 233
Abstract
The use of an appropriate oleogelator in the structuring of vegetable oil is a crucial point of consideration. Sunflower wax (SFW) is used as an oleogelator and displays an excellent potential to bind vegetable oils. The current study aimed to look for the [...] Read more.
The use of an appropriate oleogelator in the structuring of vegetable oil is a crucial point of consideration. Sunflower wax (SFW) is used as an oleogelator and displays an excellent potential to bind vegetable oils. The current study aimed to look for the effects of hydrophobic (SPAN-80) and hydrophilic (TWEEN-80) emulsifiers on the oleogels prepared using SFW and sunflower oil (SO). The biodegradability and all formulations showed globular crystals on their surface that varied in size and number. Wax ester, being the most abundant component of SFW, was found to produce fibrous and needle-like entanglements capable of binding more than 99% of SO. The formulations containing 3 mg of liquid emulsifiers in 20 g of oleogels showed better mechanical properties such as spreadability and lower firmness than the other tested concentrations. Although the FTIR spectra of all the formulations were similar, which indicated not much variation in the molecular interactions, XRD diffractograms confirmed the presence of β′ form of fat crystals. Further, the mentioned formulations also showed larger average crystallite sizes, which was supported by slow gelation kinetics. A characteristic melting point (Tm~60 °C) of triglyceride was visualized through DSC thermograms. However, a higher melting point in the case of few formulations suggests the possibility of even a stable β polymorph. The formed oleogels indicated the significant contribution of diffusion for curcumin release. Altogether, the use of SFW and SO oleogels with modified properties using biodegradable emulsifiers can be beneficial in replacing saturated fats and fat-derived products. Full article
(This article belongs to the Special Issue Oleogels and Organogels: A Promising Tool for New Functionalities 2.0)
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Article
In Vivo Evaluation of a Pectin-Honey Hydrogel Coating on Polypropylene Mesh in a Rat Model of Acute Hernia
Gels 2021, 7(3), 132; https://doi.org/10.3390/gels7030132 - 31 Aug 2021
Viewed by 271
Abstract
Investigations about ventral hernia repair are focused on improving the quality, resistance, and biocompatibility of mesh. This study compared plain polypropylene mesh with a pectin-honey hydrogel-coated polypropylene mesh in an acute hernia model in rats. Forty Wistar rats, randomly assigned to two groups, [...] Read more.
Investigations about ventral hernia repair are focused on improving the quality, resistance, and biocompatibility of mesh. This study compared plain polypropylene mesh with a pectin-honey hydrogel-coated polypropylene mesh in an acute hernia model in rats. Forty Wistar rats, randomly assigned to two groups, were submitted to laparotomy, and a 1 cm × 2 cm fascial defect was created, centered on the midline. Uncoated (group C) or coated mesh (group T) was inserted in an inlay fashion to repair the defect. After 30 days, the rats were euthanized, and the presence of adhesions to the mesh was macroscopically evaluated. Histology and measurement of COX-2 as tissue inflammation markers were used to assess fascia tissue healing. Grades of adhesion were not different between groups. Histological score and COX-2 expression were not significantly different between groups, except for the higher inflammatory response demonstrated in group T. The pectin-hydrogel coated mesh could not reduce adhesion formation compared to uncoated polypropylene mesh but improved peritoneal regeneration and tissue healing. Full article
(This article belongs to the Special Issue Gels Horizons: From Science to Smart Materials)
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Article
Polypeptide Composition and Topology Affect Hydrogelation of Star-Shaped Poly(L-lysine)-Based Amphiphilic Copolypeptides
Gels 2021, 7(3), 131; https://doi.org/10.3390/gels7030131 - 30 Aug 2021
Viewed by 220
Abstract
In this research, we studied the effect of polypeptide composition and topology on the hydrogelation of star-shaped block copolypeptides based on hydrophilic, coil poly(L-lysine)20 (s-PLL20) tethered with a hydrophobic, sheet-like polypeptide segment, which is poly(L [...] Read more.
In this research, we studied the effect of polypeptide composition and topology on the hydrogelation of star-shaped block copolypeptides based on hydrophilic, coil poly(L-lysine)20 (s-PLL20) tethered with a hydrophobic, sheet-like polypeptide segment, which is poly(L-phenylalanine) (PPhe), poly(L-leucine) (PLeu), poly(L-valine) (PVal) or poly(L-alanine) (PAla) with a degree of polymerization (DP) about 5. We found that the PPhe, PLeu, and PVal segments are good hydrogelators to promote hydrogelation. The hydrogelation and hydrogel mechanical properties depend on the arm number and hydrophobic polypeptide segment, which are dictated by the amphiphilic balance between polypeptide blocks and the hydrophobic interactions/hydrogen bonding exerted by the hydrophobic polypeptide segment. The star-shaped topology could facilitate their hydrogelation due to the branching chains serving as multiple interacting depots between hydrophobic polypeptide segments. The 6-armed diblock copolypeptides have better hydrogelation ability than 3-armed ones and s-PLL-b-PPhe exhibits better hydrogelation ability than s-PLL-b-PVal and s-PLL-b-PLeu due to the additional cation–π and π–π interactions. This study highlights that polypeptide composition and topology could be additional parameters to manipulate polypeptide hydrogelation. Full article
(This article belongs to the Special Issue Supramolecular/Supramolecular Hybrid Hydrogel)
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Review
Gel-Based Materials for Ophthalmic Drug Delivery
Gels 2021, 7(3), 130; https://doi.org/10.3390/gels7030130 - 29 Aug 2021
Viewed by 253
Abstract
The most common route of administration of ophthalmic drugs is the topical route because it is convenient, non-invasive, and accessible to all patients. Unfortunately, drugs administered topically are not able to reach effective concentrations. Moreover, their bioavailability must be improved to decrease the [...] Read more.
The most common route of administration of ophthalmic drugs is the topical route because it is convenient, non-invasive, and accessible to all patients. Unfortunately, drugs administered topically are not able to reach effective concentrations. Moreover, their bioavailability must be improved to decrease the frequency of administrations and their side effects, and to increase their therapeutic efficiency. For this purpose, in recent decades, particular attention has been given to the possibility of developing prolonged-release forms that are able to increase the precorneal residence time and decrease the loss of the drug due to tearing. Among these forms, gel-based materials have been studied as an ideal delivery system because they are an extremely versatile class with numerous prospective applications in ophthalmology. These materials are used in gel eye drops, in situ gelling formulations, intravitreal injections, and therapeutic contact lenses. This review is intended to describe gel-based materials and their main applications in ophthalmology. Full article
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Article
Molecular Simulation and Theoretical Analysis of Slide-Ring Gels under Biaxial Deformation
Gels 2021, 7(3), 129; https://doi.org/10.3390/gels7030129 - 29 Aug 2021
Viewed by 258
Abstract
Slide-ring (SR) gels, a new type of gels that have cross-links moving along the chains, are known to have unique mechanical characteristics. In the case of biaxial deformations, it has been experimentally shown that the stress–strain (S–S) relationships of SR gels can be [...] Read more.
Slide-ring (SR) gels, a new type of gels that have cross-links moving along the chains, are known to have unique mechanical characteristics. In the case of biaxial deformations, it has been experimentally shown that the stress–strain (S–S) relationships of SR gels can be well described by the neo-Hookean (NH) model. This behavior is quite different from that of conventional chemical gels, where the S–S curves deviate from the NH model. To understand the molecular mechanism of such peculiar elastic properties of SR gels, we studied the effects of movable cross-links by using molecular simulations and theoretical analysis. We calculate the S–S relationships in biaxial deformation for two types of models: slip model, where the cross-links can slide along chains representing SR gels, and non-slip model, which corresponds to conventional chemical gels. In the theoretical analysis, we calculate the S–S relationships by using the models with the Gaussian and the Langevin chains to investigate the nonlinear stretching effect of the chain in the slip and non-slip models. As a result, we found that the peculiar elastic behaviors of SR gels in biaxial deformations are well explained by the effect of movable cross-links suppressing the nonlinear stretching of the chain. Full article
(This article belongs to the Special Issue Physicochemical and Mechanical Properties of Polymer Gels)
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Review
Dissolved Organic Matter in the Global Ocean: A Primer
Gels 2021, 7(3), 128; https://doi.org/10.3390/gels7030128 - 28 Aug 2021
Viewed by 475
Abstract
Marine dissolved organic matter (DOM) holds ~660 billion metric tons of carbon, making it one of Earth’s major carbon reservoirs that is exchangeable with the atmosphere on annual to millennial time scales. The global ocean scale dynamics of the pool have become better [...] Read more.
Marine dissolved organic matter (DOM) holds ~660 billion metric tons of carbon, making it one of Earth’s major carbon reservoirs that is exchangeable with the atmosphere on annual to millennial time scales. The global ocean scale dynamics of the pool have become better illuminated over the past few decades, and those are very briefly described here. What is still far from understood is the dynamical control on this pool at the molecular level; in the case of this Special Issue, the role of microgels is poorly known. This manuscript provides the global context of a large pool of marine DOM upon which those missing insights can be built. Full article
(This article belongs to the Special Issue Marine Gels)
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Article
Chondroitin Sulfate-Based Cryogels for Biomedical Applications
Gels 2021, 7(3), 127; https://doi.org/10.3390/gels7030127 - 26 Aug 2021
Viewed by 306
Abstract
Cryogels attained from natural materials offer exceptional properties in applications such as tissue engineering. Moreover, Halloysite Nanotubes (HNT) at 1:0.5 weight ratio were embedded into CS cryogels to render additional biomedical properties. The hemolysis index of CS cryogel and CS:HNT cryogels was calculated [...] Read more.
Cryogels attained from natural materials offer exceptional properties in applications such as tissue engineering. Moreover, Halloysite Nanotubes (HNT) at 1:0.5 weight ratio were embedded into CS cryogels to render additional biomedical properties. The hemolysis index of CS cryogel and CS:HNT cryogels was calculated as 0.77 ± 0.41 and 0.81 ± 0.24 and defined as non-hemolytic materials. However, the blood coagulation indices of CS cryogel and CS:HNT cryogels were determined as 76 ± 2% and 68 ± 3%, suggesting a mild blood clotting capability. The maximum% swelling capacity of CS cryogel was measured as 3587 ± 186%, 4014 ± 184%, and 3984 ± 113%, at pH 1.0, pH 7.4 and pH 9.0, respectively, which were reduced to 1961 ± 288%, 2816 ± 192, 2405 ± 73%, respectively, for CS:HNT cryogel. It was found that CS cryogels can hydrolytically be degraded 41 ± 1% (by wt) in 16-day incubation, whereas the CS:HNT cryogels degraded by 30 ± 1 wt %. There is no chelation for HNT and 67.5 ± 1% Cu(II) chelation for linear CS was measured. On the other hand, the CS cryogel and CS:HNT cryogel revealed Cu(II) chelating capabilities of 60.1 ± 12.5%, and 43.2 ± 17.5%, respectively, from 0.1 mg/mL Cu(II) ion stock solution. Additionally, at 0.5 mg/mL CS, CS:HNT, and HNT, the Fe(II) chelation capacity of 99.7 ± 0.6, 86.2 ± 4.7% and only 11.9 ± 4.5% were measured, respectively, while no Fe(II) was chelated by linear CS chelated Fe(II). As the adjustable and controllable swelling properties of cryogels are important parameters in biomedical applications, the swelling properties of CS cryogels, at different solution pHs, e.g., at the solution pHs of 1.0, 7.4 and 9.0, were measured as 3587 ± 186%, 4014 ± 184%, and 3984 ± 113%, respectively, and the maximum selling% values of CS:HNT cryogels were determined as 1961 ± 288%, 2816 ± 192, 2405 ± 73%, respectively, at the same conditions. Alpha glucosidase enzyme interactions were investigated and found that CS-based cryogels can stimulate this enzyme at any CS formulation. Full article
(This article belongs to the Special Issue Advances in Cryogels)
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Communication
Clinical Application of Antibacterial Hydrogel and Coating in Orthopaedic and Traumatology Surgery
Gels 2021, 7(3), 126; https://doi.org/10.3390/gels7030126 (registering DOI) - 25 Aug 2021
Viewed by 273
Abstract
Implant related infection is one of the most frequent complications in orthopaedic and trauma surgery. Local antibiotic treatment strategies are becoming part of the prevention and treatment methodology for this fearful complication. To date, there are two coatings available on the market, both [...] Read more.
Implant related infection is one of the most frequent complications in orthopaedic and trauma surgery. Local antibiotic treatment strategies are becoming part of the prevention and treatment methodology for this fearful complication. To date, there are two coatings available on the market, both with a polylactic acid base. Current evidence supports the use of these types of coatings in the prophylaxis of periprosthetic infections and fracture-related infections. However, their therapeutic use has been less investigated. The purpose of this article is to summarise recent evidence relating to the clinical application of antibacterial hydrogels and coatings in orthopaedic and traumatology surgery and indicating which future applications may benefit from it. Full article
(This article belongs to the Special Issue Gels Horizons: From Science to Smart Materials)
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Article
Effective Removal of Calcium and Magnesium Ions from Water by a Novel Alginate–Citrate Composite Aerogel
Gels 2021, 7(3), 125; https://doi.org/10.3390/gels7030125 - 25 Aug 2021
Viewed by 267
Abstract
In this work, a novel alginate/citrate composite aerogel (CA–SC) was synthesized by chemical grafting technology combined with vacuum freeze-drying method, and CA–SC was used for removing calcium (Ca2+) and magnesium (Mg2+) ions from water. The experimental results indicate that [...] Read more.
In this work, a novel alginate/citrate composite aerogel (CA–SC) was synthesized by chemical grafting technology combined with vacuum freeze-drying method, and CA–SC was used for removing calcium (Ca2+) and magnesium (Mg2+) ions from water. The experimental results indicate that the as-prepared CA–SC has a high affinity for Ca2+ and Mg2+ and can remove 96.5% of Ca2+ (or 96.8% of Mg2+) from the corresponding solution. The maximum adsorption capacities of CA–SC for Ca2+ and Mg2+ are 62.38 and 36.23 mg/g, respectively. These values are higher than those of the most reported Ca2+-sorbents and Mg2+-sorbents. The CA–SC adsorbent can be regenerated through a simple pickling step, and its adsorption performance keeps stable after repeated use. Analysis of the adsorption mechanism shows that the CA–SC combines Ca2+ and Mg2+ in water mainly through coordination effect. Full article
(This article belongs to the Special Issue Aerogels 2021)
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Article
Photoinduced Porcine Gelatin Cross-Linking by Homobi- and Homotrifunctional Tetrazoles
Gels 2021, 7(3), 124; https://doi.org/10.3390/gels7030124 - 20 Aug 2021
Viewed by 237
Abstract
Gelatin is a costless polypeptide material of natural origin, able to form hydrogels that are potentially useful in biomaterial scaffold design for drug delivery, cell cultures, and tissue engineering. However, gelatin hydrogels are unstable at physiological conditions, losing their features only after a [...] Read more.
Gelatin is a costless polypeptide material of natural origin, able to form hydrogels that are potentially useful in biomaterial scaffold design for drug delivery, cell cultures, and tissue engineering. However, gelatin hydrogels are unstable at physiological conditions, losing their features only after a few minutes at 37 °C. Accordingly, treatments to address this issue are of great interest. In the present work, we propose for the first time the use of bi- and trifunctional tetrazoles, most of them unknown to date, for photoinduced gelatin cross-linking towards the production of physiologically stable hydrogels. Indeed, after UV-B irradiation, aryl tetrazoles generate a nitrilimine intermediate that is reactive towards different functionalities, some of them constitutively present in the amino acid side chains of gelatin. The efficacy of the treatment strictly depends on the structure of the cross-linking agent used, and substantial improved stability was observed by switching from bifunctional to trifunctional cross-linkers. Full article
(This article belongs to the Special Issue Gels Horizons: From Science to Smart Materials)
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Article
Microstructured Hyaluronic Acid Hydrogel for Tooth Germ Bioengineering
Gels 2021, 7(3), 123; https://doi.org/10.3390/gels7030123 - 18 Aug 2021
Viewed by 511
Abstract
Tooth loss has been found to adversely affect not just masticatory and speech functions, but also psychological health and quality of life. Currently, teeth replacement options include dentures, bridges, and implants. However, these artificial replacement options remain inferior to biological replacements due to [...] Read more.
Tooth loss has been found to adversely affect not just masticatory and speech functions, but also psychological health and quality of life. Currently, teeth replacement options include dentures, bridges, and implants. However, these artificial replacement options remain inferior to biological replacements due to their reduced efficiency, the need for replacements, and the risk of immunological rejection. To this end, there has been a heightened interest in the bioengineering of teeth in recent years. While there have been reports of successfully regenerated teeth, controlling the size and shape of bioengineered teeth remains a challenge. In this study, methacrylated hyaluronic acid (MeHA) was synthesized and microstructured in a hydrogel microwell array using soft lithography. The resulting MeHA hydrogel microwell scaffold resembles the shape of a naturally developing human tooth germ. To facilitate the epithelial–mesenchymal interactions, human adult low calcium high temperature (HaCaT) cells were seeded on the surface of the hydrogels and dental pulp stem cells (DPSCs) were encapsulated inside the hydrogels. It was found that hydrogel scaffolds were able to preserve the viability of both types of cells and they appeared to favor signaling between epithelial and mesenchymal cells, which is necessary in the promotion of cell proliferation. As such, the hydrogel scaffolds offer a promising system for the bioengineering of human tooth germs in vitro. Full article
(This article belongs to the Special Issue Hydrogel in Tissue Engineering and Regenerative Medicine)
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Article
Alumina-Doped Silica Aerogels for High-Temperature Thermal Insulation
Gels 2021, 7(3), 122; https://doi.org/10.3390/gels7030122 - 14 Aug 2021
Viewed by 397
Abstract
In this study, we used two methods to prepare alumina-doped silica aerogels with the aim of increasing the thermal stability of silica aerogels. The first method was physical doping of α-Al2O3 nano powders, and the second method was to create [...] Read more.
In this study, we used two methods to prepare alumina-doped silica aerogels with the aim of increasing the thermal stability of silica aerogels. The first method was physical doping of α-Al2O3 nano powders, and the second method was to create a chemical compound via the co-precursor of TEOS and AlCl3·6H2O in different proportions. The shrinkage, chemical composition, and specific surface area (SSA) of samples after heating at different temperatures were analyzed. Our results show that the silicon hydroxyl groups of samples derived from AlCl3·6H2O gradually decreased and nearly disappeared after heating at 800 °C, which indicates the complete dehydration of the silicon hydroxyl. Thus, the samples exhibited a large linear shrinkage and decreased SSA after high-temperature heat treatment. By contrast, samples doped with α-Al2O3 powders retained abundant silicon hydroxyl groups, and the 6.1 wt.% α-Al2O3-doped sample exhibited the lowest linear shrinkage of 11% and the highest SSA of 1056 m2/g after heat treatment at 800 °C. The alumina-doped silica aerogels prepared using a simple and low-price synthesized method pave the way for the low-cost and large-scale production of high-temperature thermal insulation. Full article
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Communication
Poly (Amidehydrazide) Hydrogel Particles for Removal of Cu2+ and Cd2+ Ions from Water
Gels 2021, 7(3), 121; https://doi.org/10.3390/gels7030121 - 12 Aug 2021
Viewed by 374
Abstract
Poly(amidoamine)s (PAMAM) are very effective in the removal of heavy metal ions from water due to their abundant amine and amide functional groups, which have a high binding ability to heavy metal ions. We synthesized a new class of hyperbranched poly(amidehydrazide) (PAMH) hydrogel [...] Read more.
Poly(amidoamine)s (PAMAM) are very effective in the removal of heavy metal ions from water due to their abundant amine and amide functional groups, which have a high binding ability to heavy metal ions. We synthesized a new class of hyperbranched poly(amidehydrazide) (PAMH) hydrogel particles from dihydrazides and N,N′-methylenebisacrylamide (MBA) monomer by using the A2 + B4 polycondensation reaction in an inverse suspension polymerization process. In Cd2+ and Cu2+ ion sorption tests, the synthesized dihydrazide-based PAMH hydrogel particles exhibited sorption capacities of 85 mg/g for copper and 47 mg/g for cadmium. Interestingly, the PAMH showed only a 10% decrease in sorption ability in an acidic condition (pH = 4) compared to the diamine-based hyperbranched PAMAM, which showed a ~90% decrease in sorption ability at pH of 4. In addition, PAMH hydrogel particles remove trace amounts of copper (0.67 ppm) and cadmium (0.5 ppm) in water, below the detection limit. Full article
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Article
Emulgels Containing Propolis and Curcumin: The Effect of Type of Vegetable Oil, Poly(Acrylic Acid) and Bioactive Agent on Physicochemical Stability, Mechanical and Rheological Properties
Gels 2021, 7(3), 120; https://doi.org/10.3390/gels7030120 - 12 Aug 2021
Viewed by 435
Abstract
Emulgels are obtained by the entrapment of an organic phase within a three-dimensional network built by hydrophilic molecules. Polymers based on cross-linked poly(acrylic acid) have been utilized as gel matrices, improving adhesiveness, rheological and mechanical performance. Propolis (PRP) produced by Apis mellifera L. [...] Read more.
Emulgels are obtained by the entrapment of an organic phase within a three-dimensional network built by hydrophilic molecules. Polymers based on cross-linked poly(acrylic acid) have been utilized as gel matrices, improving adhesiveness, rheological and mechanical performance. Propolis (PRP) produced by Apis mellifera L. bees displays a wide range of biological activities. Together with curcumin (CUR), they may show synergic anti-inflammatory, antioxidant and antimicrobial action on skin disorders. This work investigated the effect of vegetable oils (sweet almond, andiroba, and passion fruit) with regard to the physicochemical properties of emulgels composed of Carbopol 934P®, Carbopol 974P®, or polycarbophil aiming the CUR and PRP delivery. Physicochemical stability enabled the selection of systems containing passion fruit or andiroba oil. Mechanical and rheological characteristics provided rational comprehension of how vegetable oils and bioactive agents affect the structure of emulsion gels. All formulations exhibited high physiochemical stability and properties dependent on the polymer type, oil, and bioactive agent. Formulations displayed pseudoplastic, thixotropic and viscoelastic properties. Emulgels containing andiroba oil were the most stable systems. Carbopol 934P® or polycarbophil presence resulted in formulations with improved smoothness and mechanical properties. Systems containing andiroba oil and one of these two polymers are promising for further investigations as topical delivery systems of CUR and/or PRP on the skin and mucous membranes. Full article
(This article belongs to the Special Issue Polymer Gels)
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Article
Acidic and Electrosurface Properties of Binary TiO2-SiO2 Xerogels Using EPR of pH-Sensitive Nitroxides
Gels 2021, 7(3), 119; https://doi.org/10.3390/gels7030119 - 11 Aug 2021
Viewed by 282
Abstract
The binary xerogels TiO2-SiO2 are widely used as catalysts and their carriers in organic synthesis. Characterization and adjustment of the electrostatic properties of the surface and the local acidity inside the pores, are necessary for the further development of TiO [...] Read more.
The binary xerogels TiO2-SiO2 are widely used as catalysts and their carriers in organic synthesis. Characterization and adjustment of the electrostatic properties of the surface and the local acidity inside the pores, are necessary for the further development of TiO2-SiO2 xerogels applications. This research investigates acid–base equilibria in the pores, and the surface electrostatic potential (SEP) of binary TiO2-SiO2 xerogels, by the EPR of stable pH-sensitive nitroxide radicals. These radicals are small enough to penetrate directly into the pores, and to be adsorbed onto the surface of the material under study. This makes it possible to obtain valuable information on the acidic and electrosurface properties of the studied system. The highest negative surface electrical charge associated with surface electrical potential (SEP) was equal to −196 ± 6 mV. It was induced by the surface of the sample with a 7% TiO2 content. The local acidity inside the pores of this sample was found to be higher, by approximately 1.49 pH units, as compared to that in the external bulk solution. Full article
(This article belongs to the Special Issue Advances in Xerogels)
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Article
Tuning the Mechanical and Thermal Properties of Hydroxypropyl Methylcellulose Cryogels with the Aid of Surfactants
Gels 2021, 7(3), 118; https://doi.org/10.3390/gels7030118 - 11 Aug 2021
Viewed by 309
Abstract
The mechanical and thermal properties of cryogels depend on their microstructure. In this study, the microstructure of hydroxypropyl methylcellulose (HPMC) cryogels was modified by the addition of ionic (bis (2-ethylhexyl) sodium sulfosuccinate, AOT) and non-ionic (Kolliphor® EL) surfactants to the precursor hydrogels [...] Read more.
The mechanical and thermal properties of cryogels depend on their microstructure. In this study, the microstructure of hydroxypropyl methylcellulose (HPMC) cryogels was modified by the addition of ionic (bis (2-ethylhexyl) sodium sulfosuccinate, AOT) and non-ionic (Kolliphor® EL) surfactants to the precursor hydrogels (30 g/L). The surfactant concentrations varied from 0.2 mmol/L to 3.0 mmol/L. All of the hydrogels presented viscous behavior (G″ > G′). Hydrogels containing AOT (c > 2.0 mmol/L) led to cryogels with the lowest compressive modulus (13 ± 1 kPa), the highest specific surface area (2.31 m2/g), the lowest thermal conductivity (0.030 W/(m·°C)), and less hygroscopic walls. The addition of Kolliphor® EL to the hydrogels yielded the stiffest cryogels (320 ± 32 kPa) with the lowest specific surface area (1.11 m2/g) and the highest thermal conductivity (0.055 W/(m·°C)). Density functional theory (DFT) calculations indicated an interaction energy of −31.8 kcal/mol due to the interaction between the AOT sulfonate group and the HPMC hydroxyl group and the hydrogen bond between the AOT carbonyl group and the HPMC hydroxyl group. The interaction energy between the HPMC hydroxyl group and the Kolliphor® EL hydroxyl group was calculated as −7.91 kcal/mol. A model was proposed to describe the effects of AOT or Kolliphor® EL on the microstructures and the mechanical/thermal properties of HPMC cryogels. Full article
(This article belongs to the Special Issue Advances in Cryogels)
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Article
The Effect of Different Additives on the Hydration and Gelation Properties of Composite Dental Gypsum
Gels 2021, 7(3), 117; https://doi.org/10.3390/gels7030117 - 11 Aug 2021
Viewed by 375
Abstract
Dental mold gypsum materials require fine powder, appropriate liquidity, fast curing, and easy-to-perform clinical operations. They require low linear expansion coefficient and high strength, reflecting the master model and facilitating demolding. In this article, the suitable accelerators and reinforcing agents were selected as [...] Read more.
Dental mold gypsum materials require fine powder, appropriate liquidity, fast curing, and easy-to-perform clinical operations. They require low linear expansion coefficient and high strength, reflecting the master model and facilitating demolding. In this article, the suitable accelerators and reinforcing agents were selected as additives to modify dental gypsum. The main experimental methods used were to compare the trends of linear expansion coefficients of several commercially available dental gypsum products over 72 h and to observe the cross-sectional microstructure of cured bodies before and after dental gypsum modification using scanning electron microscopy. By adjusting the application of additives, the linear expansion coefficient of dental gypsum decreased from 0.26% to 0.06%, while the flexural strength increased from 6.7 MPa to 7.4 MPa at 2 h. Formulated samples showed good stability and gelation properties with linear expansion completed within 12 h. It is indicated that the performance of dental gypsum materials can be improved by adding additives and nanomaterials, which provided a good reference for clinical preparation of high-precision dental prosthesis. Full article
(This article belongs to the Special Issue Advance in Composite Gels)
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Article
Homopolymer and ABC Triblock Copolymer Mixtures for Thermoresponsive Gel Formulations
Gels 2021, 7(3), 116; https://doi.org/10.3390/gels7030116 - 09 Aug 2021
Viewed by 362
Abstract
Our group has recently invented a novel series of thermoresponsive ABC triblock terpolymers based on oligo(ethylene glycol) methyl ether methacrylate with average Mn 300 g mol−1 (OEGMA300, A unit), n-butyl methacrylate (BuMA, B unit) and di(ethylene glycol) methyl ether methacrylate [...] Read more.
Our group has recently invented a novel series of thermoresponsive ABC triblock terpolymers based on oligo(ethylene glycol) methyl ether methacrylate with average Mn 300 g mol−1 (OEGMA300, A unit), n-butyl methacrylate (BuMA, B unit) and di(ethylene glycol) methyl ether methacrylate (DEGMA, C unit) with excellent thermogelling properties. In this study, we investigate how the addition of OEGMA300x homopolymers of varying molar mass (MM) affects the gelation characteristics of the best performing ABC triblock terpolymer. Interestingly, the gelation is not disrupted by the addition of the homopolymers, with the gelation temperature (Tgel) remaining stable at around 30 °C, depending on the MM and content in OEGMA300x homopolymer. Moreover, stronger gels are formed when higher MM OEGMA300x homopolymers are added, presumably due to the homopolymer chains acting as bridges between the micelles formed by the triblock terpolymer, thus, favouring gelation. In summary, novel formulations based on mixtures of triblock copolymer and homopolymers are presented, which can provide a cost-effective alternative for use in biomedical applications, compared to the use of the triblock copolymer only. Full article
(This article belongs to the Special Issue Polymer Gels)
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Article
Design and Fabrication of Sodium Alginate/Carboxymethyl Cellulose Sodium Blend Hydrogel for Artificial Skin
Gels 2021, 7(3), 115; https://doi.org/10.3390/gels7030115 - 09 Aug 2021
Viewed by 458
Abstract
Tissue-engineered skin grafts have long been considered to be the most effective treatment for large skin defects. Especially with the advent of 3D printing technology, the manufacture of artificial skin scaffold with complex shape and structure is becoming more convenient. However, the matrix [...] Read more.
Tissue-engineered skin grafts have long been considered to be the most effective treatment for large skin defects. Especially with the advent of 3D printing technology, the manufacture of artificial skin scaffold with complex shape and structure is becoming more convenient. However, the matrix material used as the bio-ink for 3D printing artificial skin is still a challenge. To address this issue, sodium alginate (SA)/carboxymethyl cellulose (CMC-Na) blend hydrogel was proposed to be the bio-ink for artificial skin fabrication, and SA/CMC-Na (SC) composite hydrogels at different compositions were investigated in terms of morphology, thermal properties, mechanical properties, and biological properties, so as to screen out the optimal composition ratio of SC for 3D printing artificial skin. Moreover, the designed SC composite hydrogel skin membranes were used for rabbit wound defeat repairing to evaluate the repair effect. Results show that SC4:1 blend hydrogel possesses the best mechanical properties, good moisturizing ability, proper degradation rate, and good biocompatibility, which is most suitable for 3D printing artificial skin. This research provides a process guidance for the design and fabrication of SA/CMC-Na composite artificial skin. Full article
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