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Gels, Volume 8, Issue 1 (January 2022) – 63 articles

Cover Story (view full-size image): Mechanically tough polymer composite hydrogels have attracted widespread interest from both scientific and industrial points of view because of their potential applications in various fields. Hydrogels composed of biocompatible polymers are of particular interest. In this study, we found that composite hydrogels composed of chitosan nanofiber (ChsNF), positively charged alumina-coated silica nanoparticles (ac-SiO2), carboxylated poly (vinyl alcohol) (cPVA), and borax were highly stretchable and robust. The network was formed by multiple crosslinking, such as the complexation between borate and cPVA, the ionic complexation between ac-SiO2 and cPVA, and the hydrogen bond between ChsNF and cPVA. This study showed that the combined use of bio-nanofiber and inorganic nanoparticles as reinforcing agents is effective to fabricate robust and highly stretchable composite hydrogels. View this paper
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13 pages, 2710 KiB  
Article
Sodium Alginate and Chitosan as Components Modifying the Properties of Inulin Hydrogels
by Anna Florowska, Adonis Hilal, Tomasz Florowski, Paulina Mrozek and Małgorzata Wroniak
Gels 2022, 8(1), 63; https://doi.org/10.3390/gels8010063 - 17 Jan 2022
Cited by 8 | Viewed by 2953
Abstract
The aim of the study was to investigate the influence of addition of sodium alginate (SA) and chitosan (CH) on the properties of inulin hydrogels. Inulin hydrogels (20 g/100 g) containing various additions (0.0, 0.1, 0.3, and 0.5 g/100 g) of SA and [...] Read more.
The aim of the study was to investigate the influence of addition of sodium alginate (SA) and chitosan (CH) on the properties of inulin hydrogels. Inulin hydrogels (20 g/100 g) containing various additions (0.0, 0.1, 0.3, and 0.5 g/100 g) of SA and CH were produced. The hydrogels’ properties were assessed based on the volumetric gel index, microstructure, yield stress, texture, stability, and color parameters. According to the findings, the inclusion of these polysaccharides had no influence on the gelation ability of the inulin solution. The physical properties of the hydrogels containing SA or CH differed from hydrogels containing only inulin (INU). The obtained microstructural pictures revealed that the addition of SA and CH resulted in the formation of hydrogels with a more compact, smooth, and cohesive structure. Consequently, they had higher yield stress, strength, and spreadability values than INU hydrogels. The addition of chitosan in comparison with sodium alginate also had a greater effect in strengthening the structure of hydrogels, especially at the level of 0.5 g/100 g. For example, the addition of this amount of SA increased the yield stress on average from 195.0 Pa (INU) to 493.6 Pa, while the addition of CH increased it to 745.3 Pa. In the case of the strength parameter, the addition of SA increased the force from 0.24 N (INU) to 0.42 N and the addition of CH increased it to 1.29 N. In the case of spreadability this increase was from 2.89 N * s (INU) to 3.44 N * s (SA) and to 6.16 N * s (CH). Chitosan also caused an increase in the stability of inulin hydrogels, whereas such an effect was not observed with the addition of sodium alginate. The gels with the addition of SA and CH also had significantly different values of color parameters. Inulin–alginate hydrogels were characterized by higher values of the color parameter a *, lower values of the color parameter b *, and in most concentrations higher values of the color parameter L * compared to inulin–chitosan hydrogels. Based on the collected data, it can therefore be concluded that through the addition of sodium alginate and chitosan, there is a possibility to modify the properties of inulin hydrogels and, consequently, to better adapt them to the characteristics of the pro-health food products in which they will be used. Full article
(This article belongs to the Special Issue Application of Hydrocolloids in Human Health and Nutrition)
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14 pages, 1654 KiB  
Article
Influences of NaCl and Na2SO4 on the Micellization Behavior of the Mixture of Cetylpyridinium Chloride + Polyvinyl Pyrrolidone at Several Temperatures
by Md. Farid Ahmed, Malik Abdul Rub, Md. Tuhinur R. Joy, Mohammad Robel Molla, Naved Azum and Md. Anamul Hoque
Gels 2022, 8(1), 62; https://doi.org/10.3390/gels8010062 - 16 Jan 2022
Cited by 9 | Viewed by 2797
Abstract
Herein, the conductivity measurement technique is used to determine the interactions that may occur between polyvinyl pyrrolidone (PVP) polymer and cetylpyridinium chloride (CPC) surfactant in the presence of NaCl and Na2SO4 of fixed concentration at variable temperatures (298.15–323.15 K) with [...] Read more.
Herein, the conductivity measurement technique is used to determine the interactions that may occur between polyvinyl pyrrolidone (PVP) polymer and cetylpyridinium chloride (CPC) surfactant in the presence of NaCl and Na2SO4 of fixed concentration at variable temperatures (298.15–323.15 K) with an interval of 5 K. In the absence or presence of salts, we observed three critical micelle concentrations (CMC) for the CPC + PVP mixture. In all situations, CMC1 values of CPC + PVP system were found to be higher in water than in attendance of salts (NaCl and Na2SO4). Temperature and additives have the tendency to affect counterion binding values. Various physico-chemical parameters were analyzed and demonstrated smoothly, including free energy (ΔG0m), enthalpy (ΔH0m) and entropy change (ΔS0m). The micellization process is achieved to be spontaneous based on the obtained negative ΔG0m values. The linearity of the ΔHmo and ΔSmo values is excellent. The intrinsic enthalpy gain (ΔH0*m) and compensation temperature (Tc) were calculated and discussed with logical points. Interactions of polymer hydrophobic chains or the polymer + surfactant associated with amphiphilic surface-active drugs can employ a strong impact on the behavior of the gels. Full article
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13 pages, 3260 KiB  
Article
Enhanced Antioxidant Activity of Fresh Fruits through Salicylic Acid/β-CD Hydroalcoholic Gels
by Zujin Yang, Youliang Guan and Hongbing Ji
Gels 2022, 8(1), 61; https://doi.org/10.3390/gels8010061 - 15 Jan 2022
Viewed by 2114
Abstract
Oxidation is an important cause of fruit spoilage, and therefore improving the antioxidant capacity of fresh fruits is beneficial to their preservation. Herein, fresh-cut bananas were used as a type of fresh fruit and soaked in 75% hydroalcoholic gels containing salicylic acid (SA) [...] Read more.
Oxidation is an important cause of fruit spoilage, and therefore improving the antioxidant capacity of fresh fruits is beneficial to their preservation. Herein, fresh-cut bananas were used as a type of fresh fruit and soaked in 75% hydroalcoholic gels containing salicylic acid (SA) or SA/β-CD inclusion complex (SA/β-CD). After treatment, they were placed in an atmosphere at 85% relative humidity at 20 °C for 12 days. A significant reduction in spoilage in bananas treated with the hydroalcoholic gels in the presence of SA/β-CD was observed, compared with those treated with gels in the presence or absence of SA. The free-radical-scavenging performances of SA and its complex were investigated using the DPPH (1,1-diphenyl-2-picryl-hydrazil) method. Based on the results, the significant increase in antioxidant activity was attributed to the fact that the inclusion complex could break the intramolecular hydrogen bonding of SA, thus efficiently eliminating ROS in the fruits. The formation of the inclusion complex was confirmed by experiments and theoretical calculations. Our findings indicate that treatment with SA/β-CD can provide an efficient method of maintaining postharvest quality and extending the shelf life of bananas. Full article
(This article belongs to the Special Issue Recent Advances on Gels for Food Industry)
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12 pages, 1350 KiB  
Article
The Role of Cations in Resorcinol–Formaldehyde Gel Textural Characteristics
by Stewart J. Taylor, Liu Yang and Ashleigh J. Fletcher
Gels 2022, 8(1), 60; https://doi.org/10.3390/gels8010060 - 15 Jan 2022
Viewed by 2307
Abstract
The production of resorcinol–formaldehyde xerogels has yielded insight into the gelation processes underpinning their structures. In this work, the role of the cation species from the catalyst is probed by studying the simultaneous addition of sodium carbonate and calcium carbonate to a resorcinol–formaldehyde [...] Read more.
The production of resorcinol–formaldehyde xerogels has yielded insight into the gelation processes underpinning their structures. In this work, the role of the cation species from the catalyst is probed by studying the simultaneous addition of sodium carbonate and calcium carbonate to a resorcinol–formaldehyde mixture. Twenty-eight xerogels were prepared by varying the solids content, catalyst concentration, and catalyst composition, and each was analysed for its textural properties, including the surface area and average pore diameter. The results indicate that the role of the cation is linked to the stabilisation of the clusters formed within the system, and that the Group II catalyst causes the salting out of the oligomers, resulting in fewer, larger clusters, hence, an increase in pore size and a broadening of the pore size distribution. The results provide insight into how these systems can be further controlled to create tailored porous materials for a range of applications. Full article
(This article belongs to the Collection Feature Papers in Gel Materials)
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19 pages, 8942 KiB  
Article
Curcuminoid Co-Loading Platinum Heparin-Poloxamer P403 Nanogel Increasing Effectiveness in Antitumor Activity
by Ngoc The Nguyen, Quynh Anh Bui, Hoang Huong Nhu Nguyen, Tien Thanh Nguyen, Khanh Linh Ly, Ha Le Bao Tran, Vu Nguyen Doan, Tran Thi Yen Nhi, Ngoc Hoa Nguyen, Ngoc Hao Nguyen, Ngoc Quyen Tran and Dinh Trung Nguyen
Gels 2022, 8(1), 59; https://doi.org/10.3390/gels8010059 - 14 Jan 2022
Cited by 15 | Viewed by 3140
Abstract
Nanosized multi-drug delivery systems provide synergistic effects between drugs and bioactive compounds, resulting in increased overall efficiency and restricted side effects compared to conventional single-drug chemotherapy. In this study, we develop an amphiphilic heparin-poloxamer P403 (HP403) nanogel that could effectively co-load curcuminoid (Cur) [...] Read more.
Nanosized multi-drug delivery systems provide synergistic effects between drugs and bioactive compounds, resulting in increased overall efficiency and restricted side effects compared to conventional single-drug chemotherapy. In this study, we develop an amphiphilic heparin-poloxamer P403 (HP403) nanogel that could effectively co-load curcuminoid (Cur) and cisplatin hydrate (CisOH) (HP403@CisOH@Cur) via two loading mechanisms. The HP403 nanogels and HP403@CisOH@Cur nanogels were closely analyzed with 1H-NMR spectroscopy, FT-IR spectroscopy, TEM, and DLS, exhibiting high stability in spherical forms. In drug release profiles, accelerated behavior of Cur and CisOH at pH 5.5 compared with neutral pH was observed, suggesting effective delivery of the compounds in tumor sites. In vitro studies showed high antitumor activity of HP403@CisOH@Cur nanogels, while in vivo assays showed that the dual-drug platform prolonged the survival time of mice and prevented tail necrosis. In summary, HP403@CisOH@Cur offers an intriguing strategy to achieve the cisplatin and curcumin synergistic effect in a well-designed delivery platform that increases antitumor effectiveness and overcomes undesired consequences caused by cisplatin in breast cancer treatment. Full article
(This article belongs to the Special Issue Cancer Cell Biology in Biological Hydrogel)
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23 pages, 49355 KiB  
Article
Self-Gelling Solid Lipid Nanoparticle Hydrogel Containing Simvastatin as Suitable Wound Dressing: An Investigative Study
by Bhumika Gupta, Garima Sharma, Pratibha Sharma, Simarjot Kaur Sandhu and Indu Pal Kaur
Gels 2022, 8(1), 58; https://doi.org/10.3390/gels8010058 - 13 Jan 2022
Cited by 10 | Viewed by 2627
Abstract
Hydrogels, an advanced interactive system, is finding use as wound dressings, however, they exhibit restricted mechanical properties, macroscopic nature, and may not manage high exudate wounds or incorporate lipophilic actives. In this study, we developed a self-gelling solid lipid nanoparticle (SLNs) dressing to [...] Read more.
Hydrogels, an advanced interactive system, is finding use as wound dressings, however, they exhibit restricted mechanical properties, macroscopic nature, and may not manage high exudate wounds or incorporate lipophilic actives. In this study, we developed a self-gelling solid lipid nanoparticle (SLNs) dressing to incorporate simvastatin (SIM), a lipophilic, potential wound-healing agent, clinically limited due to poor solubility (0.03 mg/mL) and absorption. The study explores unconventional and novel application of SIM. The idea was to incorporate a significant amount of SIM in a soluble form and release it slowly over a prolonged time. Further, a suitable polymeric surfactant was selected that assigned a self-gelling property to SLNs (SLN-hydrogel) so as to be used as a novel wound dressing. SLNs assign porosity, elasticity, and occlusivity to the dressing to keep the wound area moist. It will also provide better tolerance and sensory properties to the hydrogel. SIM loaded SLN-hydrogel was prepared employing an industry amenable high-pressure homogenization technique. The unique hydrogel dressing was characterized for particle size, zeta potential, Fourier transform infra-red spectroscopy, powder X-ray diffraction, differential scanning calorimetry, rheology, and texture. Significant loading of SIM (10% w/w) was achieved in spherical nanoparticule hydrogel (0.3 nm (nanoparticles) to 2 µm (gelled-matrix)) that exhibited good spreadability and mechanical properties and slow release up to 72 h. SLN-hydrogel was safe as per the organization for economic co-operation and development (OECD-404) guidelines, with no signs of irritation. Complete healing of excision wound observed in rats within 11 days was 10 times better than marketed povidone-iodine product. The presented work is novel both in terms of classifying a per se SLN-hydrogel and employing SIM. Further, it was established to be a safe, effective, and industry amenable invention. Full article
(This article belongs to the Collection Hydrogel in Tissue Engineering and Regenerative Medicine)
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13 pages, 3724 KiB  
Article
Mechanically Strong and Tailorable Polyimide Aerogels Prepared with Novel Silicone Polymer Crosslinkers
by Zhongxin Zhang, Yurui Deng, Zhiyi Lun, Xiao Zhang, Mingyuan Yan, Pan He, Caihong Li and Yuelei Pan
Gels 2022, 8(1), 57; https://doi.org/10.3390/gels8010057 - 12 Jan 2022
Cited by 2 | Viewed by 2683
Abstract
Polyimide (PI) aerogels were prepared using self-designed silicone polymer cross-linkers with multi-amino from low-cost silane coupling agents to replace conventional small-molecule cross-linkers. The long-chain structure of silicone polymers provides more crosslinking points than small-molecule cross-linkers, thus improving the mechanical properties of polyimide. To [...] Read more.
Polyimide (PI) aerogels were prepared using self-designed silicone polymer cross-linkers with multi-amino from low-cost silane coupling agents to replace conventional small-molecule cross-linkers. The long-chain structure of silicone polymers provides more crosslinking points than small-molecule cross-linkers, thus improving the mechanical properties of polyimide. To investigate the effects of amino content and degree of polymerization on the properties of silicone polymers, the different silicone polymers and their cross-linked PI aerogels were prepared. The obtained PI aerogels exhibit densities as low as 0.106 g/cm3 and specific surface areas as high as 314 m2/g, and the maximum Young’s modulus of aerogel is up to 20.9 MPa when using (T-20) as cross-linkers. The cross-linkers were an alternative to expensive small molecule cross-linkers, which can improve the mechanical properties and reduce the cost of PI aerogels. Full article
(This article belongs to the Special Issue Preparation and Application of Aerogel and its Composite Materials)
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19 pages, 59469 KiB  
Article
GOx/Hb Cascade Oxidized Crosslinking of Silk Fibroin for Tissue-Responsive Wound Repair
by Hongdou Shen, Pei Wang, Xiaoke Han, Mengli Ma, Yinghui Shang, Ye Ju, Saiji Shen, Feng Yin and Qigang Wang
Gels 2022, 8(1), 56; https://doi.org/10.3390/gels8010056 - 12 Jan 2022
Cited by 4 | Viewed by 3028
Abstract
Promising wound dressings can achieve rapid soft-tissue filling while refactoring the biochemical and biophysical microenvironment to recruit endogenous cells, facilitating tissue healing, integration, and regeneration. In this study, a tissue biomolecule-responsive hydrogel matrix, employing natural silk fibroin (SF) as a functional biopolymer and [...] Read more.
Promising wound dressings can achieve rapid soft-tissue filling while refactoring the biochemical and biophysical microenvironment to recruit endogenous cells, facilitating tissue healing, integration, and regeneration. In this study, a tissue biomolecule-responsive hydrogel matrix, employing natural silk fibroin (SF) as a functional biopolymer and haemoglobin (Hb) as a peroxidase-like biocatalyst, was fabricated through cascade enzymatic crosslinking. The hydrogels possessed mechanical tunability and displayed adjustable gelation times. A tyrosine unit on SF stabilised the structure of Hb during the cascade oxidation process; thus, the immobilized Hb in SF hydrogels exhibited higher biocatalytic efficiency than the free enzyme system, which provided a continuously antioxidative system. The regulation of the dual enzyme ratio endowed the hydrogels with favourable biocompatibility, biodegradability, and adhesion strength. These multifunctional hydrogels provided a three-dimensional porous extracellular matrix-like microenvironment for promoting cell adhesion and proliferation. A rat model with a full-thickness skin defect revealed accelerated wound regeneration via collagen deposition, re-epithelialisation and revascularisation. Enzyme-loaded hydrogels are an attractive and high-safety biofilling material with the potential for wound healing, tissue regeneration, and haemostasis. Full article
(This article belongs to the Special Issue Supramolecular/Supramolecular Hybrid Hydrogel)
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25 pages, 3992 KiB  
Article
Synthesis and Characterization of Carboxymethyl Chitosan Nanosponges with Cyclodextrin Blends for Drug Solubility Improvement
by Syeda Sadia Batool Rizvi, Naveed Akhtar, Muhammad Usman Minhas, Arshad Mahmood and Kifayat Ullah Khan
Gels 2022, 8(1), 55; https://doi.org/10.3390/gels8010055 - 12 Jan 2022
Cited by 16 | Viewed by 3836
Abstract
This study aimed to enhance the solubility and release characteristics of docetaxel by synthesizing highly porous and stimuli responsive nanosponges, a nano-version of hydrogels with the additional qualities of both hydrogels and nano-systems. Nanosponges were prepared by the free radical polymerization technique and [...] Read more.
This study aimed to enhance the solubility and release characteristics of docetaxel by synthesizing highly porous and stimuli responsive nanosponges, a nano-version of hydrogels with the additional qualities of both hydrogels and nano-systems. Nanosponges were prepared by the free radical polymerization technique and characterized by their solubilization efficiency, swelling studies, sol-gel studies, percentage entrapment efficiency, drug loading, FTIR, PXRD, TGA, DSC, SEM, zeta sizer and in vitro dissolution studies. In vivo toxicity study was conducted to assess the safety of the oral administration of prepared nanosponges. FTIR, TGA and DSC studies confirmed the successful grafting of components into the stable nano-polymeric network. A porous and sponge-like structure was visualized through SEM images. The particle size of the optimized formulation was observed in the range of 195 ± 3 nm. The fabricated nanosponges noticeably enhanced the drug loading and solubilization efficiency of docetaxel in aqueous media. The drug release of fabricated nanosponges was significantly higher at pH 6.8 as compared to pH 1.2 and 4.5. An acute oral toxicity study endorsed the safety of the system. Due to an efficient preparation technique, as well as its enhanced solubility, excellent physicochemical properties, improved dissolution and non-toxic nature, nanosponges could be an efficient and a promising approach for the oral delivery of poorly soluble drugs. Full article
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15 pages, 4583 KiB  
Article
Zinc- and Copper-Loaded Nanosponges from Cellulose Nanofibers Hydrogels: New Heterogeneous Catalysts for the Synthesis of Aromatic Acetals
by Laura Riva, Angelo Davide Lotito, Carlo Punta and Alessandro Sacchetti
Gels 2022, 8(1), 54; https://doi.org/10.3390/gels8010054 - 12 Jan 2022
Cited by 14 | Viewed by 2530
Abstract
Herein we report the synthesis of cellulose-based metal-loaded nano-sponges and their application as heterogeneous catalysts in organic synthesis. First, the combination in water solution of TEMPO-oxidized cellulose nanofibers (TOCNF) with branched polyethyleneimine (bPEI) and citric acid (CA), and the thermal treatment of the [...] Read more.
Herein we report the synthesis of cellulose-based metal-loaded nano-sponges and their application as heterogeneous catalysts in organic synthesis. First, the combination in water solution of TEMPO-oxidized cellulose nanofibers (TOCNF) with branched polyethyleneimine (bPEI) and citric acid (CA), and the thermal treatment of the resulting hydrogel, leads to the synthesis of an eco-safe micro- and nano-porous cellulose nano-sponge (CNS). Subsequently, by exploiting the metal chelation characteristics of CNS, already extensively investigated in the field of environmental decontamination, this material is successfully loaded with Cu (II) or Zn (II) metal ions. Efficiency and homogeneity of metal-loading is confirmed by scanning electron microscopy (SEM) analysis with an energy dispersive X-ray spectroscopy (EDS) detector and by inductively coupled plasma-optical emission spectrometry (ICP-OES) analysis. The resulting materials perform superbly as heterogeneous catalysts for promoting the reaction between aromatic aldehydes and alcohols in the synthesis of aromatic acetals, which play a fundamental role as intermediates in organic synthesis. Optimized conditions allow one to obtain conversions higher than 90% and almost complete selectivity toward acetal products, minimizing, and in some cases eliminating, the formation of carboxylic acid by-products. ICP-OES analysis of the reaction medium allows one to exclude any possible metal-ion release, confirming that catalysis undergoes under heterogeneous conditions. The new metal-loaded CNS can be re-used and recycled five times without losing their catalytic activity. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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24 pages, 8129 KiB  
Article
Effects of Sulfate and Sulfuric Acid on Efficiency of Geopolymers as Concrete Repair Materials
by Rayed Alyousef, Ahmed Abdel Khalek Ebid, Ghasan Fahim Huseien, Hossein Mohammadhosseini, Hisham Alabduljabbar, Shek Poi Ngian and Abdeliazim Mustafa Mohamed
Gels 2022, 8(1), 53; https://doi.org/10.3390/gels8010053 - 12 Jan 2022
Cited by 10 | Viewed by 2940
Abstract
Various geopolymer mortars (GPMs) as concrete repairing materials have become effective owing to their eco-friendly properties. Geopolymer binders designed from agricultural and industrial wastes display interesting and useful mechanical performance. Based on this fact, this research (experimental) focuses on the feasibility of achieving [...] Read more.
Various geopolymer mortars (GPMs) as concrete repairing materials have become effective owing to their eco-friendly properties. Geopolymer binders designed from agricultural and industrial wastes display interesting and useful mechanical performance. Based on this fact, this research (experimental) focuses on the feasibility of achieving a new GPM with improved mechanical properties and enhanced durability performance against the aggressive sulfuric acid and sulfate attacks. This new ternary blend of GPMs can be achieved by combining waste ceramic tiles (WCT), fly ash (FA) and ground blast furnace slag (GBFS) with appropriate proportions. These GPMs were designed from a high volume of WCT, FA, and GBFS to repair the damaged concretes existing in the construction sectors. Flexural strength, slant shear bond strength, and compatibility of the obtained GPMs were compared with the base or normal concrete (NC) before and after exposure to the aggressive environments. Tests including flexural four-point loading and thermal expansion coefficient were performed. These GPMs were prepared using a low concentration of alkaline activator solution with increasing levels of GBFS and FA replaced by WCT. The results showed that substitution of GBFS and FA by WCT in the GPMs could enhance their bond strength, mechanical characteristics, and durability performance when exposed to aggressive environments. In addition, with the increase in WCT contents from 50 to 70%, the bond strength performance of the GPMs was considerably enhanced under sulfuric acid and sulfate attack. The achieved GPMs were shown to be highly compatible with the concrete substrate and excellent binders for various civil engineering construction applications. It is affirmed that the proposed GPMs can efficiently be used as high-performance materials to repair damaged concrete surfaces. Full article
(This article belongs to the Special Issue Geopolymer Gels for Next-Generation Construction)
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14 pages, 4906 KiB  
Article
Fast Gelation of Poly(ionic liquid)-Based Injectable Antibacterial Hydrogels
by Che Zhao, Chengju Sheng and Chao Zhou
Gels 2022, 8(1), 52; https://doi.org/10.3390/gels8010052 - 12 Jan 2022
Cited by 7 | Viewed by 2537
Abstract
Traditional antibacterial hydrogels have a broad-spectrum bactericidal effect and are widely used as wound dressings. However, the biological toxicity and drug resistance of these antibacterial hydrogels cannot meet the requirements of long-term clinical application. Imidazolium poly(ionic liquids) (PILs) are polymeric antibacterial agents exhibiting [...] Read more.
Traditional antibacterial hydrogels have a broad-spectrum bactericidal effect and are widely used as wound dressings. However, the biological toxicity and drug resistance of these antibacterial hydrogels cannot meet the requirements of long-term clinical application. Imidazolium poly(ionic liquids) (PILs) are polymeric antibacterial agents exhibiting strong antibacterial properties, as they contain a strong positive charge. In this study, two imidazolium PILs, namely poly(N-butylimidazolium propiolic acid sodium) (PBP) and poly(N-(3,6-dioxaoctane) imidazolium propiolic acid sodium) (PDP), as high efficiency antibacterial agents, were synthesized by polycondensation reaction. Then, the PILs were compounded with polyethylene glycol (PEG) by a thiol-yne click reaction to prepare injectable antibacterial hydrogels. An in vitro assay showed that the injectable antibacterial hydrogels could not only quickly kill Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), but also had low toxicity for human skin fibroblasts cells (HSFs) and human umbilical vein endothelial cells (HUVECs), respectively. Additionally, the lipopolysaccharide (LPS) inflammation model revealed that the injectable antibacterial hydrogels also had anti-inflammatory effects, which would be advantageous to accelerate wound healing. Full article
(This article belongs to the Special Issue Recent Advances on Functional Stimuli-Responsive Hydrogels)
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16 pages, 39820 KiB  
Article
Effect of Tricarboxylic Acids on the Formation of Hydrogels with Melem or Melamine: Morphological, Structural and Rheological Investigations
by Pradip Kumar Sukul, Puspendu Das, Gopal Lal Dhakar, Lalmohan Das and Sudip Malik
Gels 2022, 8(1), 51; https://doi.org/10.3390/gels8010051 - 10 Jan 2022
Cited by 3 | Viewed by 2247
Abstract
Herein, aggregation behaviors of melem or melamine in the presence of three symmetric carboxylic acids (1,3,5-tris(4-carboxyphenyl)benzene (TPCA), 1,3,5-benzene-tri-carboxylic acid (BTA) and 1,3,5-cyclohexane-tri-carboxylic acid (CHTA)) have been performed to check the influence of acid on the formation of aggregated structures which have been investigated [...] Read more.
Herein, aggregation behaviors of melem or melamine in the presence of three symmetric carboxylic acids (1,3,5-tris(4-carboxyphenyl)benzene (TPCA), 1,3,5-benzene-tri-carboxylic acid (BTA) and 1,3,5-cyclohexane-tri-carboxylic acid (CHTA)) have been performed to check the influence of acid on the formation of aggregated structures which have been investigated by optical microscopy, FESEM, FTIR, XRD and viscoelastic properties have been explored with rheological studies. Interestingly, melem, that has limited solubility in aqueous medium, forms aggregation that leads to the formation of hydrogels with TPCA. More significantly, hydrogel is formed here by matching the size selectivity. Melem forms hydrogel with only large tricarboxylic acid, whereas melamine produces hydrogel with any kind of its counterpart from small to large tricarboxylic acid derivatives. Present investigations and results provide the strategy of design of organic self-assembled materials having two component systems. Full article
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13 pages, 1491 KiB  
Article
Ingestion of Carbohydrate Solutions and Mouth Rinse on Mood and Perceptual Responses during Exercise in Triathletes
by María Martínez-Olcina, Laura Miralles-Amorós, Nuria Asencio-Mas, Manuel Vicente-Martínez, Rodrigo Yáñez-Sepúlveda and Alejandro Martínez-Rodríguez
Gels 2022, 8(1), 50; https://doi.org/10.3390/gels8010050 - 09 Jan 2022
Viewed by 2338
Abstract
Triathlons are endurance events that include swimming, running, and cycling. Triathletes need to eat optimally during training and competitions to maximize their potential for success. The presence of carbohydrates in the mouth could activate regions in the brain to enhance athletic performance in [...] Read more.
Triathlons are endurance events that include swimming, running, and cycling. Triathletes need to eat optimally during training and competitions to maximize their potential for success. The presence of carbohydrates in the mouth could activate regions in the brain to enhance athletic performance in exercise. Methods: This study examined the effects of glucose and mouthwash in ten male triathletes (age: 26.0 ± 8.7 years, height: 173.6 ± 10.4 cm, BMI 22.0 ± 1.7 kg/m2). The four oral test solutions included (A) Rinse with placebo, (B) Water + gel with placebo, (C) Rinse with 15% CH concentration, and (D) Water + gel with 15% CH concentration (25 g gel in 165 mL water). The Rate of Perceived Exertion (RPE), Sensation Scale (FS), Felt Arousal Scale (FAS), Profile of Mood States (POMS), blood glucose, sprints, and dietary habits were assessed in each subject. All preceded ingestion of the oral-based test solution during workouts. Results: RPE showed no significant differences for subjective perceptions. The same was observed for FS and sprints. FAS scores increased over time (p = 0.039) in all groups. POMS score increased significantly in group D (p = 0.041). There was no effect of time on plasma glucose levels (p = 0.737). As for correlations, positive correlations were observed between sprint and FAS variables (p = 0.011). Conclusions: It appears that CH intake correlates positively with mood, but in all other variables, there are no differences depending on the product. Full article
(This article belongs to the Special Issue Recent Advances on Gels for Food Industry)
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12 pages, 6369 KiB  
Article
Evaluating the Biocompatibility of an Injectable Wound Matrix in a Murine Model
by Hatem Alnojeidi, Ruhangiz Taghi Kilani and Aziz Ghahary
Gels 2022, 8(1), 49; https://doi.org/10.3390/gels8010049 - 09 Jan 2022
Cited by 4 | Viewed by 1775
Abstract
(1) Background: Developing a high-quality, injectable biomaterial that is labor-saving, cost-efficient, and patient-ready is highly desirable. Our research group has previously developed a collagen-based injectable scaffold for the treatment of a variety of wounds including wounds with deep and irregular beds. Here, we [...] Read more.
(1) Background: Developing a high-quality, injectable biomaterial that is labor-saving, cost-efficient, and patient-ready is highly desirable. Our research group has previously developed a collagen-based injectable scaffold for the treatment of a variety of wounds including wounds with deep and irregular beds. Here, we investigated the biocompatibility of our liquid scaffold in mice and compared the results to a commercially available injectable granular collagen-based product. (2) Methods: Scaffolds were applied in sub-dermal pockets on the dorsum of mice. To examine the interaction between the scaffolds and the host tissue, samples were harvested after 1 and 2 weeks and stained for collagen content using Masson’s Trichrome staining. Immunofluorescence staining and quantification were performed to assess the type and number of cells infiltrating each scaffold. (3) Results: Histological evaluation after 1 and 2 weeks demonstrated early and efficient integration of our liquid scaffold with no evident adverse foreign body reaction. This rapid incorporation was accompanied by significant cellular infiltration of stromal and immune cells into the scaffold when compared to the commercial product (p < 0.01) and the control group (p < 0.05). Contrarily, the commercial scaffold induced a foreign body reaction as it was surrounded by a capsule-like, dense cellular layer during the 2-week period, resulting in delayed integration and hampered cellular infiltration. (4) Conclusion: Results obtained from this study demonstrate the potential use of our liquid scaffold as an advanced injectable wound matrix for the management of skin wounds with complex geometries. Full article
(This article belongs to the Special Issue Application of Hydrogels in Therapeutics and Theranostics Delivery)
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17 pages, 3360 KiB  
Article
The Influence of Edible Oils’ Composition on the Properties of Beeswax-Based Oleogels
by Yuliya Frolova, Varuzhan Sarkisyan, Roman Sobolev, Mariia Makarenko, Michael Semin and Alla Kochetkova
Gels 2022, 8(1), 48; https://doi.org/10.3390/gels8010048 - 09 Jan 2022
Cited by 33 | Viewed by 3358
Abstract
This study aimed to find relationships between the properties of beeswax-based oleogels and the type of oil used. The influence of linseed, sunflower, olive, and fish oils was studied. For these oils, the fatty acid composition, the content of total polar components, and [...] Read more.
This study aimed to find relationships between the properties of beeswax-based oleogels and the type of oil used. The influence of linseed, sunflower, olive, and fish oils was studied. For these oils, the fatty acid composition, the content of total polar components, and the iodine value were characterized. Textural and thermodynamic properties were determined for oleogels, the oil-binding capacity was estimated, and the morphology of crystals was studied. The concentration of beeswax in all oleogels was 6.0% w/w. It was shown that the type of oil has a significant influence on all characteristics of the oleogels. The use of different oils at the same technological treatment leads to the formation of crystals of diverse morphology—from platelets to spherulites. At the same time, it was revealed that some characteristics of oils have a varying contribution to the properties of oleogels. The content of total polar materials in oils is associated with a decrease in strength parameters (yield value and elastic modulus) and the oil-binding capacity of oleogels. In its turn, the iodine value of oils has a close positive correlation with the melting and crystallization temperatures of oleogels. The results obtained in this article indicate that the properties of beeswax-based oleogels can be directed by changing the oil composition. Full article
(This article belongs to the Special Issue Advances in Oil Structuring)
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18 pages, 3497 KiB  
Article
Synthesis and Characterization of Acrylamide/Acrylic Acid Co-Polymers and Glutaraldehyde Crosslinked pH-Sensitive Hydrogels
by Munir Ahmad Khan, Abul Kalam Azad, Muhammad Safdar, Asif Nawaz, Muhammad Akhlaq, Pijush Paul, Md. Kamal Hossain, Md. Habibur Rahman, Roua S. Baty, Attalla F. El-kott, Mohamed Kamel, Simona G. Bungau and Mohamed M. Abdel-Daim
Gels 2022, 8(1), 47; https://doi.org/10.3390/gels8010047 - 09 Jan 2022
Cited by 17 | Viewed by 4020
Abstract
This project aims to synthesize and characterize the pH-sensitive controlled release of 5-fluorouracil (5-FU) loaded hydrogels (5-FULH) by polymerization of acrylamide (AM) and acrylic acid (AA) in the presence of glutaraldehyde (GA) as a crosslinker with ammonium persulphate as an initiator. The formulation’s [...] Read more.
This project aims to synthesize and characterize the pH-sensitive controlled release of 5-fluorouracil (5-FU) loaded hydrogels (5-FULH) by polymerization of acrylamide (AM) and acrylic acid (AA) in the presence of glutaraldehyde (GA) as a crosslinker with ammonium persulphate as an initiator. The formulation’s code is named according to acrylamide (A1, A2, A3), acrylic acid (B1, B2, B3) and glutaraldehyde (C1, C2, C3). The optimized formulations were exposed to various physicochemical tests, namely swelling, diffusion, porosity, sol gel analysis, and attenuated total reflection-Fourier transform infrared (ATR-FTIR). These 5-FULH were subjected to kinetic models for drug release data. The 5-FU were shown to be soluble in distilled water and phosphate buffer media at pH 7.4, and sparingly soluble in an acidic media at pH 1.2. The ATR-FTIR data confirmed that the 5-FU have no interaction with other ingredients. The lowest dynamic (0.98 ± 0.04% to 1.90 ± 0.03%; 1.65 ± 0.01% to 6.88 ± 0.03%) and equilibrium swelling (1.85 ± 0.01% to 6.68 ± 0.03%; 10.12 ± 0.02% to 27.89 ± 0.03%) of formulations was observed at pH 1.2, whereas the higher dynamic (4.33 ± 0.04% to 10.21 ± 0.01%) and equilibrium swelling (22.25 ± 0.03% to 55.48 ± 0.04%) was recorded at pH 7.4. These findings clearly indicated that the synthesized 5-FULH have potential swelling characteristics in pH 6.8 that will enhance the drug’s release in the same pH medium. The porosity values of formulated 5-FULH range from 34% to 62% with different weight ratios of AM, AA, and GA. The gel fractions data showed variations ranging from 74 ± 0.4% (A1) to 94 ± 0.2% (B3). However, formulation A1 reported the highest 24 ± 0.1% and B3 the lowest 09 ± 0.3% sol fractions rate among the formulations. Around 20% drug release from the 5-FULH was found at 1 h in an acidic media (pH1.2), whereas >65% of drug release (pH7.4) was observed at around 25 h. These findings concluded that GA crosslinked 5-FU loaded AM and AA based hydrogels would be a potential pH-sensitive oral controlled colon drug delivery carrier. Full article
(This article belongs to the Special Issue Recent Advances on Nanogel Engineering for Drug Delivery)
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34 pages, 9541 KiB  
Review
Recent Advances in Zwitterionic Hydrogels: Preparation, Property, and Biomedical Application
by Sihang Liu, Jingyi Tang, Fangqin Ji, Weifeng Lin and Shengfu Chen
Gels 2022, 8(1), 46; https://doi.org/10.3390/gels8010046 - 07 Jan 2022
Cited by 50 | Viewed by 7421
Abstract
Nonspecific protein adsorption impedes the sustainability of materials in biologically related applications. Such adsorption activates the immune system by quick identification of allogeneic materials and triggers a rejection, resulting in the rapid failure of implant materials and drugs. Antifouling materials have been rapidly [...] Read more.
Nonspecific protein adsorption impedes the sustainability of materials in biologically related applications. Such adsorption activates the immune system by quick identification of allogeneic materials and triggers a rejection, resulting in the rapid failure of implant materials and drugs. Antifouling materials have been rapidly developed in the past 20 years, from natural polysaccharides (such as dextran) to synthetic polymers (such as polyethylene glycol, PEG). However, recent studies have shown that traditional antifouling materials, including PEG, still fail to overcome the challenges of a complex human environment. Zwitterionic materials are a class of materials that contain both cationic and anionic groups, with their overall charge being neutral. Compared with PEG materials, zwitterionic materials have much stronger hydration, which is considered the most important factor for antifouling. Among zwitterionic materials, zwitterionic hydrogels have excellent structural stability and controllable regulation capabilities for various biomedical scenarios. Here, we first describe the mechanism and structure of zwitterionic materials. Following the preparation and property of zwitterionic hydrogels, recent advances in zwitterionic hydrogels in various biomedical applications are reviewed. Full article
(This article belongs to the Special Issue Gels Horizons: From Science to Smart Materials)
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17 pages, 2039 KiB  
Review
Drug Delivery Based on Stimuli-Responsive Injectable Hydrogels for Breast Cancer Therapy: A Review
by Hai Xin and Sina Naficy
Gels 2022, 8(1), 45; https://doi.org/10.3390/gels8010045 - 07 Jan 2022
Cited by 28 | Viewed by 4497
Abstract
Breast cancer is the most common and biggest health threat for women. There is an urgent need to develop novel breast cancer therapies to overcome the shortcomings of conventional surgery and chemotherapy, which include poor drug efficiency, damage to normal tissues, and increased [...] Read more.
Breast cancer is the most common and biggest health threat for women. There is an urgent need to develop novel breast cancer therapies to overcome the shortcomings of conventional surgery and chemotherapy, which include poor drug efficiency, damage to normal tissues, and increased side effects. Drug delivery systems based on injectable hydrogels have recently gained remarkable attention, as they offer encouraging solutions for localized, targeted, and controlled drug release to the tumor site. Such systems have great potential for improving drug efficiency and reducing the side effects caused by long-term exposure to chemotherapy. The present review aims to provide a critical analysis of the latest developments in the application of drug delivery systems using stimuli-responsive injectable hydrogels for breast cancer treatment. The focus is on discussing how such hydrogel systems enhance treatment efficacy and incorporate multiple breast cancer therapies into one system, in response to multiple stimuli, including temperature, pH, photo-, magnetic field, and glutathione. The present work also features a brief outline of the recent progress in the use of tough hydrogels. As the breast undergoes significant physical stress and movement during sporting and daily activities, it is important for drug delivery hydrogels to have sufficient mechanical toughness to maintain structural integrity for a desired period of time. Full article
(This article belongs to the Special Issue Tough Hydrogels for Biomedical Applications 2.0)
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16 pages, 2177 KiB  
Article
Chitosan/Pluronic F127 Thermosensitive Hydrogel as an Injectable Dexamethasone Delivery Carrier
by Jomarien García-Couce, Miriela Tomás, Gastón Fuentes, Ivo Que, Amisel Almirall and Luis J. Cruz
Gels 2022, 8(1), 44; https://doi.org/10.3390/gels8010044 - 07 Jan 2022
Cited by 40 | Viewed by 6716
Abstract
Intra-articular administration of anti-inflammatory drugs is a strategy that allows localized action on damaged articular cartilage and reduces the side effects associated with systemic drug administration. The objective of this work is to prepare injectable thermosensitive hydrogels for the long-term application of dexamethasone. [...] Read more.
Intra-articular administration of anti-inflammatory drugs is a strategy that allows localized action on damaged articular cartilage and reduces the side effects associated with systemic drug administration. The objective of this work is to prepare injectable thermosensitive hydrogels for the long-term application of dexamethasone. The hydrogels were prepared by mixing chitosan (CS) and Pluronic-F127 (PF) physically. In addition, tripolyphosphate (TPP) was used as a crosslinking agent. Chitosan added to the mix increased the gel time compared to the pluronic gel alone. The incorporation of TPP into the material modified the morphology of the hydrogels formed. Subsequently, MTS and Live/Dead® experiments were performed to investigate the toxicity of hydrogels against human chondrocytes. The in vitro releases of dexamethasone (DMT) from CS-PF and CS-PF-TPP gels had an initial burst and took more time than that from the PF hydrogel. In vivo studies showed that hydrogels retained the fluorescent compound longer in the joint than when administered in PBS alone. These results suggest that the CS-PF and CS-PF-TPP hydrogels loaded with DMT could be a promising drug delivery platform for the treatment of osteoarthritis. Full article
(This article belongs to the Special Issue Advanced Hydrogels for the Repair of Cartilage Defects)
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11 pages, 1170 KiB  
Article
A Ponceau S Staining-Based Dot Blot Assay for Rapid Protein Quantification of Biological Samples
by Dario Lucas Helbing, Leopold Böhm, Nova Oraha, Leonie Karoline Stabenow and Yan Cui
Gels 2022, 8(1), 43; https://doi.org/10.3390/gels8010043 - 07 Jan 2022
Cited by 6 | Viewed by 5515
Abstract
Despite the availability of a wide range of commercial kits, protein quantification is often unreliable, especially for tissue-derived samples, leading to uneven loading in subsequent experiments. Here we show that the widely used Bicinchoninic Acid (BCA) assay tends to underestimate protein concentrations of [...] Read more.
Despite the availability of a wide range of commercial kits, protein quantification is often unreliable, especially for tissue-derived samples, leading to uneven loading in subsequent experiments. Here we show that the widely used Bicinchoninic Acid (BCA) assay tends to underestimate protein concentrations of tissue samples. We present a Ponceau S staining-based dot-blot assay as an alternative for protein quantification. This method is simple, rapid, more reliable than the BCA assay, compatible with biological samples lysed in RIPA or 2x SDS gel-loading buffer, and also inexpensive. Full article
(This article belongs to the Special Issue Advance in Composite Gels)
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17 pages, 9728 KiB  
Article
Preparation and Evaluation of Polymer-Based Ultrasound Gel and Its Application in Ultrasonography
by Sadia Afzal, Muhammad Zahid, Zulfiqar Ahmad Rehan, H. M. Fayzan Shakir, Hamza Javed, Meshari M. H. Aljohani, Syed Khalid Mustafa, Maqsood Ahmad and Montaser M. Hassan
Gels 2022, 8(1), 42; https://doi.org/10.3390/gels8010042 - 06 Jan 2022
Cited by 11 | Viewed by 10608
Abstract
Ultrasound imaging is a widely used technique in every health care center and hospital. Ultrasound gel is used as a coupling medium in all ultrasound procedures to replace air between the transducer and the patient’s skin, as ultrasound waves have trouble in traveling [...] Read more.
Ultrasound imaging is a widely used technique in every health care center and hospital. Ultrasound gel is used as a coupling medium in all ultrasound procedures to replace air between the transducer and the patient’s skin, as ultrasound waves have trouble in traveling through air. This research was performed to formulate an inexpensive alternative to commercially available ultrasound gel as it is expensive and imported from other countries. Different formulations with different concentrations of carbopol 980 (CAR 980) and methylparaben were prepared with natural ingredients such as aloe vera gel and certain available chemicals that have no harmful effects on the skin. To justify the efficiency of the formulations; necessary physicochemical characteristics such as visual clarity, homogeneity, transparency, skin irritation, antibacterial activity, pH, stability, spreadability, conductivity, acoustic impedance, viscosity, and cost were evaluated. Moreover, a comparison study was also conducted with commercially available ultrasound gel that was utilized as a control. All samples showed excellent transparency and no microbial growth. S1 was the only formulation that met all of the requirements for commercial ultrasound gel and produced images that were similar to those produced by commercial ultrasound gel. So, this formulation could be used as an alternative to expensive commercial ultrasound gel for taking images in hospitals and medical centers. Full article
(This article belongs to the Special Issue Dynamics of Gels and Its Applications)
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14 pages, 2443 KiB  
Review
Application of Hybrid Electrically Conductive Hydrogels Promotes Peripheral Nerve Regeneration
by Fengshi Zhang, Meng Zhang, Songyang Liu, Ci Li, Zhentao Ding, Teng Wan and Peixun Zhang
Gels 2022, 8(1), 41; https://doi.org/10.3390/gels8010041 - 06 Jan 2022
Cited by 8 | Viewed by 3047
Abstract
Peripheral nerve injury (PNI) occurs frequently, and the prognosis is unsatisfactory. As the gold standard of treatment, autologous nerve grafting has several disadvantages, such as lack of donors and complications. The use of functional biomaterials to simulate the natural microenvironment of the nervous [...] Read more.
Peripheral nerve injury (PNI) occurs frequently, and the prognosis is unsatisfactory. As the gold standard of treatment, autologous nerve grafting has several disadvantages, such as lack of donors and complications. The use of functional biomaterials to simulate the natural microenvironment of the nervous system and the combination of different biomaterials are considered to be encouraging alternative methods for effective tissue regeneration and functional restoration of injured nerves. Considering the inherent presence of an electric field in the nervous system, electrically conductive biomaterials have been used to promote nerve regeneration. Due to their singular physical properties, hydrogels can provide a three-dimensional hydrated network that can be integrated into diverse sizes and shapes and stimulate the natural functions of nerve tissue. Therefore, conductive hydrogels have become the most effective biological material to simulate human nervous tissue’s biological and electrical characteristics. The principal merits of conductive hydrogels include their physical properties and their electrical peculiarities sufficient to effectively transmit electrical signals to cells. This review summarizes the recent applications of conductive hydrogels to enhance peripheral nerve regeneration. Full article
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14 pages, 3125 KiB  
Article
Soft-Tissue-Mimicking Using Hydrogels for the Development of Phantoms
by Aitor Tejo-Otero, Felip Fenollosa-Artés, Isabel Achaerandio, Sergi Rey-Vinolas, Irene Buj-Corral, Miguel Ángel Mateos-Timoneda and Elisabeth Engel
Gels 2022, 8(1), 40; https://doi.org/10.3390/gels8010040 - 06 Jan 2022
Cited by 30 | Viewed by 5345
Abstract
With the currently available materials and technologies it is difficult to mimic the mechanical properties of soft living tissues. Additionally, another significant problem is the lack of information about the mechanical properties of these tissues. Alternatively, the use of phantoms offers a promising [...] Read more.
With the currently available materials and technologies it is difficult to mimic the mechanical properties of soft living tissues. Additionally, another significant problem is the lack of information about the mechanical properties of these tissues. Alternatively, the use of phantoms offers a promising solution to simulate biological bodies. For this reason, to advance in the state-of-the-art a wide range of organs (e.g., liver, heart, kidney as well as brain) and hydrogels (e.g., agarose, polyvinyl alcohol –PVA–, Phytagel –PHY– and methacrylate gelatine –GelMA–) were tested regarding their mechanical properties. For that, viscoelastic behavior, hardness, as well as a non-linear elastic mechanical response were measured. It was seen that there was a significant difference among the results for the different mentioned soft tissues. Some of them appear to be more elastic than viscous as well as being softer or harder. With all this information in mind, a correlation between the mechanical properties of the organs and the different materials was performed. The next conclusions were drawn: (1) to mimic the liver, the best material is 1% wt agarose; (2) to mimic the heart, the best material is 2% wt agarose; (3) to mimic the kidney, the best material is 4% wt GelMA; and (4) to mimic the brain, the best materials are 4% wt GelMA and 1% wt agarose. Neither PVA nor PHY was selected to mimic any of the studied tissues. Full article
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12 pages, 23556 KiB  
Article
A Study of the Quantitative Relationship between Yield Strength and Crystal Size Distribution of Beeswax Oleogels
by Varuzhan Sarkisyan, Roman Sobolev, Yuliya Frolova, Irina Vorobiova and Alla Kochetkova
Gels 2022, 8(1), 39; https://doi.org/10.3390/gels8010039 - 05 Jan 2022
Cited by 6 | Viewed by 1665
Abstract
Beeswax and beeswax hydrocarbon-based oleogels were studied to evaluate the quantitative relationship between their yield strength and crystal size distribution. With this aim, oleogels were prepared using four different cooling regimes to obtain different crystal size distributions. The microstructure was evaluated by polarized [...] Read more.
Beeswax and beeswax hydrocarbon-based oleogels were studied to evaluate the quantitative relationship between their yield strength and crystal size distribution. With this aim, oleogels were prepared using four different cooling regimes to obtain different crystal size distributions. The microstructure was evaluated by polarized light microscopy. The yield strength is measured by the cone penetration test. Oleogels were characterized by average grain size, microstructure entropy, grain boundary energy per unit volume, and microstructure temperature. We have provided the theoretical basis for interpreting the microstructure and evaluating the microstructure-based hardening of oleogels. It is shown that the microstructure entropy might be used to predict the yield strength of oleogels by the Hall-Petch relationship. Full article
(This article belongs to the Special Issue Advances in Oil Structuring)
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22 pages, 6588 KiB  
Article
Clozapine-Encapsulated Binary Mixed Micelles in Thermosensitive Sol–Gels for Intranasal Administration
by Madeleine S. A. Tan, Preeti Pandey, James R. Falconer, Dan J. Siskind, Alexandra Balmanno and Harendra S. Parekh
Gels 2022, 8(1), 38; https://doi.org/10.3390/gels8010038 - 05 Jan 2022
Cited by 9 | Viewed by 2485
Abstract
(1) Background: Clozapine is the most effective antipsychotic. It is, however, associated with many adverse drug reactions. Nose-to-brain (N2B) delivery offers a promising approach. This study aims to develop clozapine-encapsulated thermosensitive sol–gels for N2B delivery. (2) Methods: Poloxamer 407 and hydroxypropyl methylcellulose were [...] Read more.
(1) Background: Clozapine is the most effective antipsychotic. It is, however, associated with many adverse drug reactions. Nose-to-brain (N2B) delivery offers a promising approach. This study aims to develop clozapine-encapsulated thermosensitive sol–gels for N2B delivery. (2) Methods: Poloxamer 407 and hydroxypropyl methylcellulose were mixed and hydrated with water. Glycerin and carbopol solutions were added to the mixture and stirred overnight at 2–8 °C. Clozapine 0.1% w/w was stirred with polysorbate 20 (PS20) or polysorbate 80 (PS80) at RT (25 °C) before being added to the polymer solution. The final formulation was made to 10 g with water, stirred overnight at 2–8 °C and then adjusted to pH 5.5. (3) Results: Formulations F3 (3% PS20) and F4 (3% PS80) were selected for further evaluation, as their gelation temperatures were near 28 °C. The hydrodynamic particle diameter of clozapine was 18.7 ± 0.2 nm in F3 and 20.0 ± 0.4 nm in F4. The results show a crystallinity change in clozapine to amorphous. Drug release studies showed a 59.1 ± 3.0% (F3) and 53.1 ± 2.7% (F4) clozapine release after 72 h. Clozapine permeated after 8 h was 20.8 ± 3.0% (F3) and 17.8 ± 3.1% (F4). The drug deposition was higher with F4 (144.8 ± 1.4 µg/g) than F3 (110.7 ± 2.7 µg/g). Both sol–gels showed no phase separation after 3 months. (4) Conclusions: Binary PS80-P407 mixed micelles were more thermodynamically stable and rigid due to the higher synergism of both surfactants. However, binary mixed PS20-P407 micelles showed better drug permeation across the nasal mucosa tissue and may be a preferable carrier system for the intranasal administration of clozapine. Full article
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15 pages, 2510 KiB  
Article
Gelation Behavior and Stability of Multicomponent Sterol-Based Oleogels
by Artur J. Martins, Fátima Cerqueira, António A. Vicente, Rosiane L. Cunha, Lorenzo M. Pastrana and Miguel A. Cerqueira
Gels 2022, 8(1), 37; https://doi.org/10.3390/gels8010037 - 05 Jan 2022
Cited by 9 | Viewed by 2453
Abstract
Novel fat mimetic materials, such as oleogels, are advancing the personalization of healthier food products and can be developed from low molecular weight compounds such as γ-oryzanol and β-sitosterol. Following molecular assembly, the formation of a tubular system ensues, which seems to be [...] Read more.
Novel fat mimetic materials, such as oleogels, are advancing the personalization of healthier food products and can be developed from low molecular weight compounds such as γ-oryzanol and β-sitosterol. Following molecular assembly, the formation of a tubular system ensues, which seems to be influenced by elements such as the oleogelators’ concentration and ratio, cooling rates, and storage periods. Sterol-based oleogels were formulated under distinct environmental conditions, and a comprehensive study aimed to assess the effects of the mentioned factors on oleogel formation and stability, through visual observation and by using techniques such as small-angle X-ray scattering, X-ray diffraction, confocal Raman spectroscopy, rheology, and polarized microscopy. The long, rod-like conformations, identified by small-angle X-ray scattering, showed that different cooling rates influence oleogels’ texture. Raman spectra showed that the stabilization time is associated with the interfibrillar aggregation, which occurred differently for 8 and 10 wt%, with a proven relationship between ferulic acid and the tubular formation. This report gives fundamental insight into the critical point of gelation, referring to the time scale of the molecular stabilization. Our results verify that understanding the structuring mechanisms of oleogelation is decisive for the processing and manufacturing of novel foods which integrate oleogels in their structure. Full article
(This article belongs to the Collection Feature Papers in Gel Materials)
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15 pages, 3755 KiB  
Article
Influence of the Mixtures of Vegetable Oil and Vitamin E over the Microstructure and Rheology of Organogels
by Renata Miliani Martinez, Pedro Leonidas Oseliero Filho, Barbara Bianca Gerbelli, Wagner Vidal Magalhães, Maria Valéria Robles Velasco, Suzana Caetano da Silva Lannes, Cristiano Luis Pinto de Oliveira, Catarina Rosado and André Rolim Baby
Gels 2022, 8(1), 36; https://doi.org/10.3390/gels8010036 - 05 Jan 2022
Cited by 4 | Viewed by 2090
Abstract
Candelilla wax (CW) and 12-hydroxystearic acid (12HSA) are classic solid-fiber-matrix organogelators. Despite the high number of studies using those ingredients in oily systems, there is scarce literature using a mixture of oil and antioxidants. Vitamin E (VE) is an important candidate for its [...] Read more.
Candelilla wax (CW) and 12-hydroxystearic acid (12HSA) are classic solid-fiber-matrix organogelators. Despite the high number of studies using those ingredients in oily systems, there is scarce literature using a mixture of oil and antioxidants. Vitamin E (VE) is an important candidate for its lipophilicity and several applications on pharmaceutical, cosmetics, and food industries. In this work, we investigated the influences of mixtures between vegetable oil (VO) and VE on the microstructures and rheological properties of CW and 12HSA organogels. A weak gel (G′′/G′ > 0.1) with a shear-thinning behavior was observed for all samples. The presence of VE impacted the gel strength and the phase transition temperatures in a dose-dependent pattern. Larger and denser packed crystals were seen for 12HSA samples, while smaller and more dispersed structures were obtained for CW organogels. The results obtained in this work allowed the correlation of the structural and mechanical properties of the organogels, which plays an important role in the physical-chemical characteristics of these materials. Full article
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13 pages, 1196 KiB  
Article
Influence of Bile Acids in Hydrogel Pharmaceutical Formulations on Dissolution Rate and Permeation of Clindamycin Hydrochloride
by Nebojša Pavlović, Isidora Anastasija Bogićević, Dragana Zaklan, Maja Đanić, Svetlana Goločorbin-Kon, Hani Al-Salami and Momir Mikov
Gels 2022, 8(1), 35; https://doi.org/10.3390/gels8010035 - 05 Jan 2022
Cited by 5 | Viewed by 2581
Abstract
Clindamycin hydrochloride is a widely used antibiotic for topical use, but its main disadvantage is poor skin penetration. Therefore, new approaches in the development of clindamycin topical formulations are of great importance. We aimed to investigate the effects of the type of gelling [...] Read more.
Clindamycin hydrochloride is a widely used antibiotic for topical use, but its main disadvantage is poor skin penetration. Therefore, new approaches in the development of clindamycin topical formulations are of great importance. We aimed to investigate the effects of the type of gelling agent (carbomer and sodium carmellose), and the type and concentration of bile acids as penetration enhancers (0.1% and 0.5% of cholic and deoxycholic acid), on clindamycin release rate and permeation in a cellulose membrane in vitro model. Eight clindamycin hydrogel formulations were prepared using a 23 full factorial design, and they were evaluated for physical appearance, pH, drug content, drug release, and permeability parameters. Although formulations with carbomer as the gelling agent exerted optimal sensory properties, carmellose sodium hydrogels had significantly higher release rates and permeation of clindamycin hydrochloride. The bile acid enhancement factors were higher in carbomer gels, and cholic acid exerted more pronounced permeation-enhancing effects. Since the differences in the permeation parameters of hydrogels containing cholic acid in different concentrations were insignificant, its addition in a lower concentration is more favorable. The hydrogel containing carmellose sodium as a gelling agent and 0.1% cholic acid as a penetration enhancer can be considered as the formulation of choice. Full article
(This article belongs to the Special Issue Application of Hydrogels in Therapeutics and Theranostics Delivery)
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12 pages, 2122 KiB  
Article
Hybrid Sol-Gel Coatings Doped with Non-Toxic Corrosion Inhibitors for Corrosion Protection on AZ61 Magnesium Alloy
by Luis Rodríguez-Alonso, Jesús López-Sánchez, Aida Serrano, Oscar Rodríguez de la Fuente, Juan Carlos Galván and Noemí Carmona
Gels 2022, 8(1), 34; https://doi.org/10.3390/gels8010034 - 05 Jan 2022
Cited by 10 | Viewed by 1953
Abstract
Physiological human fluid is a natural corrosive environment and can lead to serious corrosion and mechanical damages to light Mg–Al alloys used in prosthetics for biomedical applications. In this work, organic–inorganic hybrid coatings doped with various environmentally friendly and non-toxic corrosion inhibitors have [...] Read more.
Physiological human fluid is a natural corrosive environment and can lead to serious corrosion and mechanical damages to light Mg–Al alloys used in prosthetics for biomedical applications. In this work, organic–inorganic hybrid coatings doped with various environmentally friendly and non-toxic corrosion inhibitors have been prepared by the sol-gel process for the corrosion protection of AZ61 magnesium alloys. Effectiveness has been evaluated by pH measurements, optical microscopy, and SEM during a standard corrosion test in a Hanks’ Balanced Salt Solution. The results showed that the addition of an inhibitor to the sol-gel coating can improve significantly the corrosion performance, being an excellent barrier for the L-cysteine-doped hybrid sol-gel films. The incorporation of TiO2 nanoparticles, 2-Aminopyridine and quinine organic molecules slowed down the corrosion rate of the Mg–Al alloy. Graphene oxide seemed to have the same response to corrosion as the hybrid sol-gel coating without inhibitors. Full article
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