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Gels, Volume 8, Issue 11 (November 2022) – 73 articles

Cover Story (view full-size image): Composites involving reduced graphene oxide (rGO) aerogels supporting Pt/TiO2 nanoparticles were fabricated using a one-pot supercritical CO2 gelling and drying method. Electron microscopy images and N2 adsorption–desorption isotherms indicated the formation of 3D monolithic aerogels with a meso/macroporous morphology. A comprehensive evaluation of the synthesized photocatalyst was carried out with a focus on the target application: the photocatalytic production of H2 from methanol in aqueous media. The reaction conditions, together with the aerogel composition and architecture, were varied to optimize the process. In the most favorable conditions, using rGO aerogels as the catalyst support, remarkably high values of H2 production rate were obtained. View this paper
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18 pages, 3318 KiB  
Article
Cr(III) Ion-Imprinted Hydrogel Membrane for Chromium Speciation Analysis in Water Samples
by Ivanka Dakova, Penka Vasileva and Irina Karadjova
Gels 2022, 8(11), 757; https://doi.org/10.3390/gels8110757 - 21 Nov 2022
Cited by 6 | Viewed by 2155
Abstract
Novel Cr(III)-imprinted poly(vinyl alcohol)/sodium alginate/AuNPs hydrogel membranes (Cr(III)-IIMs) were obtained and characterized and further applied as a sorbent for chromium speciation in waters. Cr(III)-IIMs were prepared via solution blending method using blends of poly(vinyl alcohol) and sodium alginate as film-forming materials, poly(ethylene glycol) [...] Read more.
Novel Cr(III)-imprinted poly(vinyl alcohol)/sodium alginate/AuNPs hydrogel membranes (Cr(III)-IIMs) were obtained and characterized and further applied as a sorbent for chromium speciation in waters. Cr(III)-IIMs were prepared via solution blending method using blends of poly(vinyl alcohol) and sodium alginate as film-forming materials, poly(ethylene glycol) as a porogen agent, sodium alginate stabilized gold nanoparticles (SA-AuNPs) as a crosslinking and mechanically stabilizing component, and Cr(III) ions as a template species. The physicochemical characteristics of pre-synthesized AuNPs and obtained hydrogel membranes Cr(III)-IIM were studied by UV-vis and FTIR spectroscopy, TEM and SEM observations, N2 adsorption–desorption measurements, and XRD analysis. The mechanism of the adsorption process toward Cr(III) was best described by pseudo-first-order kinetic and Langmuir models. Experiments performed showed that quantitative retention of Cr(III) is attained in 20 h at pH 6 and temperature 40 °C. Under the same conditions, the adsorption of Cr(VI) is below 5%. A simple and sensitive analytical procedure was developed for the speciation of Cr in an aquatic environment using dispersive solid phase extraction of Cr(III) by Cr(III)-IIM prior to selective Cr(VI) measurement by ETAAS in the supernatants. The detection limits and reproducibility achieved for the Cr speciation analysis fulfill the requirements for their monitoring in waters under the demand of the Water Framework Directive. Full article
(This article belongs to the Special Issue Gels for Removal and Adsorption)
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<p>Schematic representation of the hydrogel Cr(III)-IIMs preparation.</p>
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<p>UV-vis absorption spectra of SA-AuNPs in: aqueous dispersion (red line) and PVA/PEG/SA hydrogel matrix solution (black line); inset: optical photo of SA-AuNPs aqueous dispersion.</p>
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<p>(<b>a</b>) TEM and (<b>b</b>) HRTEM micrographs of SA-AuNPs.</p>
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<p>TEM micrographs at different magnifications (<b>a</b>,<b>b</b>) of Cr(III)-IIM.</p>
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<p>SEM images at different magnifications of (<b>a</b>,<b>b</b>) NIIM and (<b>c</b>,<b>d</b>) Cr(III)-IIM.</p>
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<p>Effect of contact time on the degree of sorption <span class="html-italic">D</span><sub>s</sub> of Cr(III) onto Cr(III)-IIM at initial concentration 5 mg/L, pH 6, temperature 40 °C, and adsorbent dose (one membrane) 0.140 g.</p>
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<p>Dependence of the degree of sorption (<span class="html-italic">D</span><sub>S</sub>, %) of Cr(III) ions onto Cr(III)-IIM on pH and temperature.</p>
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<p>Effect of the initial concentration of Cr(III) on the adsorption capacity of Cr(III)-IIM and NIIM (pH 6; contact time 20 h; temperature 40 °C).</p>
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14 pages, 1892 KiB  
Article
The Use of Biopolymers as a Natural Matrix for Incorporation of Essential Oils of Medicinal Plants
by Roxana Gheorghita Puscaselu, Andrei Lobiuc, Ioan Ovidiu Sirbu and Mihai Covasa
Gels 2022, 8(11), 756; https://doi.org/10.3390/gels8110756 - 21 Nov 2022
Cited by 7 | Viewed by 2450
Abstract
The benefits of using biopolymers for the development of films and coatings are well known. The enrichment of these material properties through various natural additions has led to their applicability in various fields. Essential oils, which are well-known for their beneficial properties, are [...] Read more.
The benefits of using biopolymers for the development of films and coatings are well known. The enrichment of these material properties through various natural additions has led to their applicability in various fields. Essential oils, which are well-known for their beneficial properties, are widely used as encapsulating agents in films based on biopolymers. In this study, we developed biopolymer-based films and tested their properties following the addition of 7.5% and 15% (w/v) essential oils of lemon, orange, grapefruit, cinnamon, clove, chamomile, ginger, eucalyptus or mint. The samples were tested immediately after development and after one year of storage in order to examine possible long-term property changes. All films showed reductions in mass, thickness and microstructure, as well as mechanical properties. The most considerable variations in physical properties were observed in the 7.5% lemon oil sample and the 15% grapefruit oil sample, with the largest reductions in mass (23.13%), thickness (from 109.67 µm to 81.67 µm) and density (from 0.75 g/cm3 to 0.43 g/cm3). However, the microstructure of the sample was considerably improved. Although the addition of lemon essential oil prevented the reduction in mass during the storage period, it favored the degradation of the microstructure and the loss of elasticity (from 16.7% to 1.51% for the sample with 7.5% lemon EO and from 18.28% to 1.91% for the sample with 15% lemon EO). Although the addition of essential oils of mint and ginger resulted in films with a more homogeneous microstructure, the increase in concentration favored the appearance of pores and modifications of color parameters. With the exception of films with added orange, cinnamon and clove EOs, the antioxidant capacity of the films decreased during storage. The most obvious variations were identified in the samples with lemon, mint and clove EOs. The most unstable samples were those with added ginger (95.01%), lemon (92%) and mint (90.22%). Full article
(This article belongs to the Special Issue Bioactive Gel Films and Coatings Applied in Active Food Packaging)
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Figure 1
<p>Mass of biopolymeric films.</p>
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<p>Sample thickness after one year of storage. T0, light brown bars; T1, blue bars.</p>
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<p>Transmittance values of samples (t0).</p>
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<p>The transmittance values of samples after one year of storage (t1).</p>
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<p>Sample tensile strength.</p>
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<p>Sample elongation.</p>
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<p>Graphical representation of DPPH radical scavenging activity of biopolymeric films before (red) and after storage (turquoise).</p>
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16 pages, 5626 KiB  
Article
Preparation of Bio-Based Aerogel and Its Adsorption Properties for Organic Dyes
by Penghui Li, Chi Yang, Xuewen Xu, Chen Miao, Tianjiao He, Bo Jiang and Wenjuan Wu
Gels 2022, 8(11), 755; https://doi.org/10.3390/gels8110755 - 21 Nov 2022
Cited by 20 | Viewed by 3594
Abstract
The effective utilization of biomass and the purification of dye wastewater are urgent problems. In this study, a biomass aerogel (CaCO3@starch/polyacrylamide/TEMPO-oxidized nanocellulose, CaCO3@STA/PAM/TOCN) was prepared by combining nanocellulose with starch and introducing calcium carbonate nanoparticles, which exhibited a rich [...] Read more.
The effective utilization of biomass and the purification of dye wastewater are urgent problems. In this study, a biomass aerogel (CaCO3@starch/polyacrylamide/TEMPO-oxidized nanocellulose, CaCO3@STA/PAM/TOCN) was prepared by combining nanocellulose with starch and introducing calcium carbonate nanoparticles, which exhibited a rich three-dimensional layered porous structure with a very light mass. Starch and nanocellulose can be grafted onto the molecular chain of acrylamide, while calcium carbonate nanopores can make the gel pore size uniform and have excellent swelling properties. Here, various factors affecting the adsorption behavior of this aerogel, such as pH, contact time, ambient temperature, and initial concentration, are investigated. From the kinetic data, it can be obtained that the adsorption process fits well with the pseudo-second-order. The Langmuir isotherm model can fit the equilibrium data well. The thermodynamic data also demonstrated the spontaneous and heat-absorbing properties of anionic and cationic dyes on CaCO3@STA/PAM/TOCN aerogels. The adsorption capacity of Congo red (CR) and methylene blue (MB) by CaCO3@STA/PAM/TOCN was 277.76 mg/g and 101.01 mg/g, respectively. Therefore, cellulose and starch-based aerogels can be considered promising adsorbents for the treatment of dye wastewater. Full article
(This article belongs to the Special Issue Recent Advances in Aerogels)
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<p>Digital photos of the (<b>a</b>) CaCO<sub>3</sub>@STA/PAM/TOCN aerogel; (<b>b</b>) CaCO<sub>3</sub>@STA/PAM/TOCN aerogel after adsorption of methylene blue; (<b>c</b>) CaCO<sub>3</sub>@STA/PAM/TOCN aerogel after adsorption of Congo red; SEM images of the (<b>d</b>,<b>e</b>) CaCO<sub>3</sub>@STA/PAM/TOCN aerogel; (<b>f</b>) CaCO<sub>3</sub>@STA/PAM/TOCN aerogel after adsorption of methylene blue; (<b>g</b>) CaCO<sub>3</sub>@STA/PAM/TOCN aerogel after adsorption of Congo red; (<b>h</b>) EDX mapping images of the CaCO<sub>3</sub>@STA/PAM/TOCN.</p>
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<p>(<b>a</b>) Nitrogen adsorption–desorption isotherms of CaCO<sub>3</sub>@STA/PAM/TOCN aerogels; (<b>b</b>) TGA results of CaCO<sub>3</sub>@STA/PAM/TOCN aerogels; (<b>c</b>) XRD patterns of CaCO<sub>3</sub>@STA/PAM/TOCN aerogels; (<b>d</b>) FITR of CaCO<sub>3</sub>@STA/PAM/TOCN aerogels.</p>
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<p>Effects of initial pH on the MB and CR adsorption capacity (adsorption time t = 6 h, ambient temperature T = 20 °C).</p>
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<p>Effects of the adsorption time on the MB and CR adsorption capacity (pH value pH = 7, ambient temperature T = 20 °C).</p>
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<p>Effects of ambient temperature on the MB and CR adsorption capacity (pH value pH = 7, adsorption time t = 6 h).</p>
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<p>Pseudo-first-order and pseudo-second-order kinetic models for the adsorption of CR (<b>a</b>,<b>c</b>) and MB (<b>b</b>,<b>d</b>) on the aerogel.</p>
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<p>The linear dependence of q<sub>t</sub> on t<sup>0.5</sup> based on the intra-particle diffusion, MB (<b>a</b>) and CR (<b>b</b>).</p>
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<p>Langmuir and Freundlich isotherms for the adsorption of CR (<b>a</b>,<b>c</b>) and MB (<b>b</b>,<b>d</b>) on the aerogel (m = 10 mg, V = 50 mL, t = 6 h).</p>
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<p>Plots of lnk against 1/T for the adsorption of CR (<b>a</b>) and MB (<b>b</b>) onto aerogel.</p>
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<p>Cyclic adsorption of CaCO<sub>3</sub>@STA/PAM/TOCN aerogels (reusability experiments were performed at pH 7.0 with a dose of 10 mg of CaCO<sub>3</sub>@STA/PAM/TOCN, an elution volume of 25 mL at 20 °C, an initial CR dye concentration of 100 mg/L, an initial MB dye concentration 4 mg/L. After each elution, the aerogels were freeze-dried at −40 °C).</p>
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<p>Schematic illustration of the preparation of CaCO<sub>3</sub>@STA/PAM/TOCN aerogel.</p>
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16 pages, 9342 KiB  
Article
In Situ Biosynthesis of Photothermal Parasite for Fluorescence Imaging-Guided Photothermal Therapy of Tumors
by Yaqiong Wang, Haiyan Pan, Zhaowei Meng and Cai Zhang
Gels 2022, 8(11), 754; https://doi.org/10.3390/gels8110754 - 21 Nov 2022
Cited by 2 | Viewed by 2045
Abstract
Photothermal therapy (PTT) has been widely known as a promising therapeutic strategy for cancer treatment in recent decades. However, some organic and inorganic photothermal agents exhibit shortcomings including potential long-term toxicity and lack of biodegradability. Biocompatible extracts from plants and animals provide several [...] Read more.
Photothermal therapy (PTT) has been widely known as a promising therapeutic strategy for cancer treatment in recent decades. However, some organic and inorganic photothermal agents exhibit shortcomings including potential long-term toxicity and lack of biodegradability. Biocompatible extracts from plants and animals provide several alternatives for the reformation of photothermal agents. Bio-inspired products still have inherent problems such as low accumulation in tumors, easy diffusion, and fast elimination. Herein, we aim to develop a biocompatible photothermal agent with tumor enrichment. Enlightened by “parasitized snails”, in situ biosynthesis of photothermal agents and fluorescence imaging-guided PTT are achieved with the assistance of alginate–calcium–genipin (ACG) hydrogel. ACG hydrogel is a mixture of alginate (ALG), calcium (Ca), and genipin (GP). Given that the crosslinking product of GP and protein displays fluorescent/photothermal features, the constructed ACG hydrogel can gradually react with the tumor and then “light up” and “ignite” the tumor under specific light excitation. The ACG hydrogel can be seen as a photothermal parasite, eventually leading to the death of tumor. The photothermal therapeutic effects of ACG hydrogel reacting with tumors are successfully proven in vivo. The naturally derived GP and ALG ensure the biosafety of the ACG hydrogel-based bio-application. This work is another successful practice of nature-inspired methodological strategy for in situ biosynthesis of the photothermal agent. Full article
(This article belongs to the Special Issue Biofunctional Gels)
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<p>Characterization of the ACG hydrogel. (<b>A</b>) The tilted ALG–Ca hydrogel (left) and ACG hydrogel (right). (<b>B</b>) The photograph of ACG hydrogel (upright and inverted). (<b>C</b>) The pattern of “ALG–Ca–GP” is coherently formed by the ACG hydrogel with a 1 mL syringe. SEM image of ALG–Ca hydrogel (<b>D</b>) and ACG hydrogel (<b>E</b>), Scale bar: 20 μm. (<b>F</b>) UV–vis–NIR absorption spectra of ACG + BSA (10 mg/mL) hydrogel, ACG hydrogel, ALG–Ca hydrogel, GP and CaCl<sub>2</sub> after fourfold dilution.</p>
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<p>In vitro evaluation of the properties of ACG hydrogel in a simulated protein-rich environment. Digital photos of the upright (<b>A</b>) and tilted (<b>B</b>) ACG + BSA hydrogel with different concentrations of BSA (0, 5, 10, 20, 50 mg/mL). Infrared thermal photos (<b>C</b>) and photothermal heating curves (<b>D</b>) of ACG + BSA hydrogel (0, 10, and 50 mg BSA/mL) and water under 808 nm laser irradiation (2 W/cm<sup>2</sup>, 10 min). The fluorescence imaging (<b>E</b>) and the fluorescent counts of the region of interest (ROI) (<b>F</b>) of ACG + BSA hydrogel (0, 10, and 50 mg BSA/mL).</p>
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<p>The cytological experiment of ACG hydrogel in vitro. (<b>A</b>) The fluorescent images of the 4T1 cells incubated with ACG hydrogel (0, 50, 75, and 100 μg GP/mL) for 0 h, 3 h, 6 h, 12 h, and 24 h, <span class="html-italic">n</span> = 3. (<b>B</b>) The quantitative analysis of fluorescent counts in each well of (<b>A</b>), shown as means ± SD, <span class="html-italic">n</span> = 3. (<b>C</b>) The infrared thermal photos of 4T1 cells incubated with ACG hydrogel (0, 50, 75, and 100 μg GP/mL) under 808 nm laser irradiation (4 or 6 W/cm<sup>2</sup>, 10 min). (<b>D</b>) The quantitative analysis of temperature change of different treatments, shown as means ± SD, <span class="html-italic">n</span> = 3, was evaluated by two-way ANOVA tests, *** <span class="html-italic">p</span> &lt; 0.001. (<b>E</b>) Cell viabilities of 4T1 cells incubated with ACG hydrogel (0, 50, 75, and 100 μg GP/mL) under 808 nm laser irradiation (0, 4, and 6 W/cm<sup>2</sup>, 10 min), shown as means ± SD, evaluated by two-way ANOVA tests, *** <span class="html-italic">p</span> &lt; 0.001. (<b>F</b>) The dual staining of living/dead cells with Calcein AM and PI is shown as green and red, respectively. Scale bar: 200 μm.</p>
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<p>Time optimization of intratumoral injection of ACG hydrogel in mice. (<b>A</b>) Digital photographs of tumor color change derived from the reaction of ACG hydrogel with tumor during 12 h. (<b>B</b>) In vivo imaging of tumor fluorescence signal change derived from the reaction of ACG hydrogel with tumor during 12 h. (<b>C</b>) The quantitative analysis of fluorescent counts of tumor sites in (<b>B</b>) is shown as means ± SD, <span class="html-italic">n</span> = 5. (<b>D</b>) Blue tumors exfoliated at 12 h after intratumoral injection of ACG hydrogel. Up: color digital photograph. Middle: fluorescence photo. Down: overlay of grey photo and fluorescence photo.</p>
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<p>In vivo PTT assisted by the “parasitism” of ACG hydrogel in the tumor. (<b>A</b>) Infrared thermal photos of tumor-bearing mice during 808 nm laser irradiation, <span class="html-italic">n</span> = 5. (<b>B</b>) The average temperature change curves of mice’s tumor surface during 808 nm laser irradiation, shown as means ± SD, complied with the normal distribution and evaluated by one-way ANOVA tests, ** <span class="html-italic">p</span> &lt; 0.01, *** <span class="html-italic">p</span> &lt; 0.001. (<b>C</b>) The average relative tumor volume (V/V<sub>0</sub>) change of mice in each group, shown as means ± SD, complied with the normal distribution and evaluated by one-way ANOVA tests, * <span class="html-italic">p</span> &lt; 0.05, ** <span class="html-italic">p</span> &lt; 0.01. (<b>D</b>) The digital photographs of tumor-bearing mice at different time points (Origin, 0, 3, 9, and 15 d) in each group, <span class="html-italic">n</span> = 5. (<b>E</b>) The ratio of tumor weight to body weight of mice in each group, shown as means ± SD, not complied with the normal distribution and evaluated by nonparametric Kruskal–Wallis tests, * <span class="html-italic">p</span> &lt; 0.05, ** <span class="html-italic">p</span> &lt; 0.01. (<b>F</b>) Photo of tumor masses excised from tumor-bearing mice after different treatments. ACG: intratumoral injection of 50 μL ACG hydrogel. L: 808 nm laser irradiation (2 W/cm<sup>2</sup>, 10 min). ACG (0 h) + L: intratumoral injection of 50 μL ACG hydrogel followed by immediate laser irradiation (2 W/cm<sup>2</sup>, 10 min). ACG (12 h) + L: intratumoral injection of 50 μL ACG hydrogel followed by 12 h delayed laser irradiation (2 W/cm<sup>2</sup>, 10 min). TW: Tumor Weight. BW: Body Weight.</p>
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<p>The representative hematoxylin and eosin (H&amp;E) stained tissue sections of mice’s major organs, including heart, liver, spleen, lung, and kidney, after different treatments. Scale bar: 200 μm. ACG: intratumoral injection of 50 μL ACG hydrogel. L: 808 nm laser irradiation (2 W/cm<sup>2</sup>, 10 min). ACG (0 h) + L: intratumoral injection of 50 μL ACG hydrogel followed by immediate laser irradiation (2 W/cm<sup>2</sup>, 10 min). ACG (12 h) + L: intratumoral injection of 50 μL ACG hydrogel followed by 12 h delayed laser irradiation (2 W/cm<sup>2</sup>, 10 min).</p>
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<p>The biochemical analysis of mice with different treatments. (<b>A</b>) TBIL. (<b>B</b>) ALT. (<b>C</b>) AST. (<b>D</b>) ALP. (<b>E</b>) TP. (<b>F</b>) ALB. (<b>G</b>) CREA. (<b>H</b>) UA. (<b>I</b>) UERA. Data shown as means ± SD, <span class="html-italic">n</span> = 3. Control: blood sample collection of tumor-bearing mice without other interference. ACG 0.5 d: blood sample collection at 0.5 d after intratumoral injection of 50 μL ACG hydrogel. ACG 7 d: blood sample collection at 7 d after intratumoral injection of 50 μL ACG hydrogel.</p>
Full article ">Scheme 1
<p>The schematic illustration of “photothermal parasite” practice: ACG hydrogel-assisted in situ biosynthesis of the tumor–GP complex for fluorescence imaging-guided PTT.</p>
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18 pages, 2689 KiB  
Article
Spontaneous and Electrically Induced Anisotropy of Composite Agarose Gels
by Alexandar M. Zhivkov and Svetlana H. Hristova
Gels 2022, 8(11), 753; https://doi.org/10.3390/gels8110753 - 21 Nov 2022
Viewed by 1730
Abstract
Agarose gels containing and not bacteriorhodopsin purple membranes (incorporated before gelling) manifest spontaneous optical anisotropy. The dependencies of the anisotropy on the agarose concentration and time have been studied. The rise in the anisotropy is explained by the predominant orientation of the agarose [...] Read more.
Agarose gels containing and not bacteriorhodopsin purple membranes (incorporated before gelling) manifest spontaneous optical anisotropy. The dependencies of the anisotropy on the agarose concentration and time have been studied. The rise in the anisotropy is explained by the predominant orientation of the agarose fibers during the gelling and subsequent deformation of the gel net. In the electric field, additional optical anisotropy rises, which is caused by the orientation of the membranes. A procedure has been developed to separate electrically induced and spontaneous anisotropy in composite gels. The isoelectric points and surface electric potential of bacteriorhodopsin trimer and purple membranes are calculated by the method of protein electrostatics to explain their electric asymmetry, which leads to perpendicular orientation in the direct electric field and longitudinal in the kilohertz sinusoidal field. The results allow for an increase in the separation capability of composite gels of electrophoresis for macromolecules with different sizes by applying an appropriate electric field to modulate the effective pore size. Full article
(This article belongs to the Special Issue Physical and Mechanical Properties of Polymer Gels)
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Figure 1
<p>pH-dependences of the net charge <span class="html-italic">nz</span> of the polypeptide chain of bacteriorhodopsin trimer (3bR) in folded (curve 1) and unfolded (curve 2) conformation, and <span class="html-italic">nz</span> of purple membrane (PM, curve 3). <span class="html-italic">Insert</span>: Molecular model of single bR macromolecule horizontally oriented with the cytoplasmic side on the left. The colors correspond to the sign (red—negative and blue—positive) and the value of the electrostatic potential on the intramembrane surface of the bR monomer in the range of −7 <span class="html-italic">kT</span>/<span class="html-italic">e</span> to +7 <span class="html-italic">kT</span>/<span class="html-italic">e</span>, where <span class="html-italic">e</span>—the elementary charge, <span class="html-italic">k</span>—Boltzmann constant, and <span class="html-italic">T</span>—absolute temperature; <span class="html-italic">kT</span>/<span class="html-italic">e</span> = 25.26 mV at 20 °C.</p>
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<p>Molecular models of bacteriorhodopsin trimer (3bR) with adjoining 30 lipid molecules (the upper two pictures) and a part of the purple membrane (the lower two pictures). The left two pictures show the intracellular (cytoplasmic) surface of bR and PM and the right two pictures show the extracellular surface. The colors correspond to the sign and value of the electrostatic potential at pH 6.0: Negative (red) and positive (blue) in the range of −11 <span class="html-italic">kT</span>/<span class="html-italic">e</span> to +11 <span class="html-italic">kT</span>/<span class="html-italic">e</span>. The red points around the bR trimer represent the oxygen atoms in the heads of the lipid molecules.</p>
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<p>Dependence of the intensity <span class="html-italic">I</span><sub>φ</sub> of the transmitted light with a wavelength of 650 nm on the angle of decrossing φ (degrees) in the aqueous suspension of PM and in composite agarose gels with incorporated PM in equal concentrations: 1—PM in bidistilled water; 2—PM in fresh 0.3% gel; 3—PM in fresh 0.4% gel; and 4—PM in fresh 0.6% gel.</p>
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<p>Dependence of the steady-state optical anisotropy Δ<span class="html-italic">n</span> on the squared strength <span class="html-italic">E</span> of the sinusoidal electric field with a frequency of 1 kHz at a wavelength λ<sub>0</sub> = 650 nm: 1—PM-water suspension; 2—PM in 0.3% gel, 5 h old; 3—PM in 0.4% gel, 3 h old; and 4—PM in 0.6% gel, 3 h old. The PM concentration in all samples is equal.</p>
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<p>Time dependence of the growth of the spontaneous optical anisotropy Δ<span class="html-italic">n</span><sub>0</sub> at λ<sub>0</sub> = 650 nm in 0.6% pure agarose gel.</p>
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<p>Imaginary picture of the composite agarose gel with incorporated PM, which are shown schematically as rods (diametrical cross section of the membrane plane) oriented chaotically (the left picture), perpendicularly to the direct electric field (the medium picture) and along the field direction in the kilohertz sinusoidal electric field (the right picture).</p>
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<p>Schematic diagram of the set-up used for electric birefringence: L—halogenous lamp 12 V, 100 W; LPS—low-voltage power supply unit; M—prism monochromator; CL—cylindrical lens; P—polarizer; EOC—electrooptical cell; A—analyzer; PhM—photomultiplier; HPS—high-voltage power supply unit; O—digital oscilloscope; G—functional generator; PA—wide band power amplifier. The coloured components are: lamp (yellow); light beam (green), metal electrodes (two thick red lines in EOC); electric impulses (red lines); electrooptical signal (blue line), low- and high-voltage direct current (brown lines).</p>
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12 pages, 1302 KiB  
Article
Gelling Power Alteration on Kappa-Carrageenan Dispersion through Esterification Method with Different Fatty Acid Saturation
by Yoga W. Wardhana, Nuur Aanisah, Iyan Sopyan, Rini Hendriani and Anis Y. Chaerunisaa
Gels 2022, 8(11), 752; https://doi.org/10.3390/gels8110752 - 21 Nov 2022
Cited by 14 | Viewed by 3138
Abstract
The physicochemical properties of κ-carrageenan gels and their ester forms derived from different fatty-acid saturations were characterized and compared with those of native κ-carrageenan. Furthermore, stearic and oleic acids were used as the saturated and unsaturated fatty acids, respectively. Fourier-transform infrared (FTIR) spectra [...] Read more.
The physicochemical properties of κ-carrageenan gels and their ester forms derived from different fatty-acid saturations were characterized and compared with those of native κ-carrageenan. Furthermore, stearic and oleic acids were used as the saturated and unsaturated fatty acids, respectively. Fourier-transform infrared (FTIR) spectra confirmed the introduction of the ester into the κ-carrageenan backbone. The thermogravimetric analysis showed that thermal stability increased along with the level of unsaturation, but there was a decrease in viscosity, hardness, and syneresis, which caused the consistency of the product to become more elastic. The results also showed that the ester form still has a swelling ability that is almost the same as that of κ-carrageenan. After being formulated into a gel dosage form, the product was successfully produced from the ester with unsaturated fatty acids, and it was more elastic than native κ-carrageenan and had good physical properties with spreadability that meets the requirements for topical preparations. Full article
(This article belongs to the Special Issue Gel Formation and Processing Technologies for Material Applications)
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<p>FTIR spectra of pyridine, κ-carrageenan, and its ester derivatives.</p>
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<p>TGA thermogram of κ-carrageenan and its ester derivatives.</p>
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<p>The pH (<b>A</b>), viscosity (<b>B</b>), gel hardness and strength (<b>C</b>), swelling ratio (<b>D</b>), water-binding capacity (<b>E</b>), and syneresis (<b>F</b>) of κ-carrageenan gel in comparison with its ester derivatives (means ± SD, n = 3).</p>
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10 pages, 2454 KiB  
Article
A Polyvinyl Alcohol–Tannic Acid Gel with Exceptional Mechanical Properties and Ultraviolet Resistance
by Chunqing Si, Xintong Tian, Yan Wang, Zhigang Wang, Xinfang Wang, Dongjun Lv, Aili Wang, Fang Wang, Longlong Geng, Jing Zhao, Ruofei Hu and Qingzeng Zhu
Gels 2022, 8(11), 751; https://doi.org/10.3390/gels8110751 - 20 Nov 2022
Cited by 9 | Viewed by 4874
Abstract
Design and preparation of gels with excellent mechanical properties has garnered wide interest at present. In this paper, preparation of polyvinyl alcohol (PVA)–tannic acid (TA) gels with exceptional properties is documented. The crystallization zone and hydrogen bonding acted as physical crosslinkages fabricated by [...] Read more.
Design and preparation of gels with excellent mechanical properties has garnered wide interest at present. In this paper, preparation of polyvinyl alcohol (PVA)–tannic acid (TA) gels with exceptional properties is documented. The crystallization zone and hydrogen bonding acted as physical crosslinkages fabricated by a combination of freeze–thaw treatment and a tannic acid compound. The effect of tannic acid on mechanical properties of prepared PVA–TA gels was investigated and analyzed. When the mass fraction of PVA was 20.0 wt% and soaking time was 12 h in tannic acid aqueous solution, tensile strength and the elongation at break of PVA–TA gel reached 5.97 MPa and 1450%, respectively. This PVA–TA gel was far superior to a pure 20.0 wt% PVA hydrogel treated only with the freeze–thaw process, as well as most previously reported PVA–TA gels. The toughness of a PVA–TA gel is about 14 times that of a pure PVA gel. In addition, transparent PVA–TA gels can effectively prevent ultraviolet-light-induced degradation. This study provides a novel strategy and reference for design and preparation of high-performance gels that are promising for practical application. Full article
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<p>Diagram showing preparation of PVA–TA gel (third row, from left to right: PVA solution, freeze–thawed PVA gel, and PVA–TA gel).</p>
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<p>(<b>a</b>) FTIR spectra of pure PVA hydrogel and 15.0 wt% PVA–TA gel. (<b>b</b>) TG curves of pure 15.0 wt% PVA hydrogel and 15.0 wt% PVA–TA gel.</p>
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<p>(<b>a</b>) XRD patterns of pure 15.0 wt% PVA gel and 15.0 wt% PVA–TA gel; (<b>b</b>,<b>c</b>) SEM image of 15.0 wt% PVA–TA24 gel.</p>
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<p>Images of 20.0 wt% PVA–TA24 gel mechanical properties: (<b>a</b>) bending, (<b>b</b>) stretching, and (<b>c</b>,<b>d</b>) holding a weight of 200 g and 4.80 kg.</p>
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<p>For 10.0 wt% PVA–TA gel: stress–strain curves (<b>a</b>), corresponding rupture stress–strain (<b>b</b>) and toughness values (<b>c</b>). For 15.0 wt% PVA–TA gel: stress–strain curves (<b>d</b>), corresponding rupture stress–strain (<b>e</b>) and toughness values (<b>f</b>). For 20.0 wt% PVA–TA gel: stress–strain curves (<b>g</b>), corresponding rupture stress/strain (<b>h</b>) and toughness values (<b>i</b>).</p>
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<p>UV-radiation shielding of 15.0 wt% PVA–TA gel: (<b>a</b>) pure PVA gel under natural light (two images on the left) and ultraviolet light (two images on the right; wavelength of ultraviolet lamps was 365 nm). (<b>b</b>) Samples of 15.0 wt% PVA–TA24 gel (thickness: 0.12 cm) under natural light (two images on the left) and ultraviolet light (two images on the right). (<b>c</b>) Schematics illustrating the UV filtration process of gel derived from TA molecules. (<b>d</b>) Transmittance spectra of 15.0 wt% PVA–TA24 gel in the visible wavelength range (during 200–800 nm).</p>
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19 pages, 3571 KiB  
Article
Development of Thermoresponsive-Gel-Matrix-Embedded Amoxicillin Trihydrate-Loaded Bovine Serum Albumin Nanoparticles for Local Intranasal Therapy
by Sandra Aulia Mardikasari, Mária Budai-Szűcs, László Orosz, Katalin Burián, Ildikó Csóka and Gábor Katona
Gels 2022, 8(11), 750; https://doi.org/10.3390/gels8110750 - 19 Nov 2022
Cited by 10 | Viewed by 2568
Abstract
A high dose of amoxicillin is recommended as the first-line therapy for acute bacterial rhinosinusitis (ABR). However, oral administration of amoxicillin is connected to many adverse reactions coupled with moderate bioavailability (~60%). Therefore, this study aimed to develop a topical nasal preparation of [...] Read more.
A high dose of amoxicillin is recommended as the first-line therapy for acute bacterial rhinosinusitis (ABR). However, oral administration of amoxicillin is connected to many adverse reactions coupled with moderate bioavailability (~60%). Therefore, this study aimed to develop a topical nasal preparation of amoxicillin, employing a thermoresponsive nanogel system to increase nasal residence time and prolong drug release. Rheological investigations revealed that formulations containing 21–23% w/w Poloxamer 407 (P407) were in accordance with the requirement of nasal administration (gelling temperature ~35 °C). The average hydrodynamic diameter (<200 nm), pH (6.7–6.9), and hypertonic osmolality (611–663 mOsmol/L) of the in situ gelling nasal nanogel appeared as suitable characteristics for local rhinosinusitis treatment. Moreover, taking into account the mucoadhesive strength and drug release studies, the 21% w/w P407 could be considered as an optimized concentration for effective nasal delivery. Antibacterial activity studies showed that the ability of amoxicillin-loaded in situ gelling nasal nanogel to inhibit bacterial growth (five common ABR pathogens) preserved its effectiveness in comparison to 1 mg/mL amoxicillin aqueous solution as a positive control. Altogether, the developed amoxicillin-loaded in situ gelling thermoresponsive nasal nanogel can be a potential candidate for local antibiotic therapy in the nasal cavity. Full article
(This article belongs to the Special Issue Drug-Loaded Hydrogel Biomaterials)
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<p>Response surface plots showing the effect of independent variables: AMT–ethanol (<b>a</b>), PW–ethanol (<b>b</b>), and AMT–PW (<b>c</b>) on Z-average.</p>
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<p>In situ gelling properties of nasal formulations with different P407 concentrations on gelling temperature (<b>a</b>) and gelling time at 35 °C (<b>b</b>). Data are presented as means ± SD, <span class="html-italic">n</span> = 3.</p>
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<p>Effect of P407 concentration on gel strength (<b>a</b>) and mucoadhesive strength (<b>b</b>) in comparison to 0.5% <span class="html-italic">w</span>/<span class="html-italic">v</span> NaHA solution. Data are presented as means ± SD, <span class="html-italic">n</span> = 3.</p>
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<p>pH of optimized in situ gelling nasal formulations. Data are presented as means ± SD, <span class="html-italic">n</span> = 3.</p>
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<p>Raman chemical mapping of AMT-BSA in the in situ gelling matrices with different concentrations of P407: 21 (<b>a</b>), 22 (<b>b</b>), and 23% <span class="html-italic">w</span>/<span class="html-italic">v</span> (<b>c</b>).</p>
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<p>In vitro drug release profile of AMT-loaded in situ gelling thermosensitive nasal formulations (21, 22, and 23% <span class="html-italic">w</span>/<span class="html-italic">v</span>) in comparison to initial AMT. Data are presented as means ± SD, <span class="html-italic">n</span> = 3.</p>
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<p>Disk diffusion test zone of AMT-free BSA-P407, as negative control (NC); 1 mg/mL AMT aqueous solution, as positive control (PC); and in situ gelling AMT-BSA nasal gel formulations (containing 21, 22, and 23% <span class="html-italic">w</span>/<span class="html-italic">v</span> of P407). (<b>a</b>) Diameter of the inhibitory zone formed against five investigated bacteria (<span class="html-italic">S. aureus; H. influenzae; M. catarrhalis; S. pyogenes;</span> and <span class="html-italic">S. pneumoniae</span>). (<b>b</b>) Data are presented as means ± SD, <span class="html-italic">n</span> = 5.</p>
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<p>Change of AMT content in the in situ gelling nasal preparation for 4 weeks storage at room temperature (RT) and cold place (4 °C). Data are presented as means ± SD, <span class="html-italic">n</span> = 3.</p>
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<p>Preparation of AMT-loaded in situ gelling thermoresponsive nasal gel formulation. Illustration was created using BioRender (<a href="https://biorender.com/" target="_blank">https://biorender.com/</a>), accessed on 13 November 2022.</p>
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17 pages, 7712 KiB  
Article
The Feasibility of Shellac Wax Emulsion Oleogels as Low-Fat Spreads Analyzed by Means of Multidimensional Statistical Analysis
by Andreea Puşcaş and Vlad Mureşan
Gels 2022, 8(11), 749; https://doi.org/10.3390/gels8110749 - 18 Nov 2022
Cited by 8 | Viewed by 2336
Abstract
Shellac wax-based oleogel emulsions were studied with a three level two factorial design in order to find an optimal formulation for a spread formulation. Rheological, textural, colorimetry, and stability analysis were conducted to assess the performance of oleogel emulsions. FTIR spectra were also [...] Read more.
Shellac wax-based oleogel emulsions were studied with a three level two factorial design in order to find an optimal formulation for a spread formulation. Rheological, textural, colorimetry, and stability analysis were conducted to assess the performance of oleogel emulsions. FTIR spectra were also compared. The similarities between the samples were studied using cluster analysis. Analysis of variance (ANOVA) demonstrates that (i) the texture is influenced by the wax concentration, (ii) the rheology and stability by both the considered numeric factors (wax and water concentration) and their interaction, and (iii) the color by both factors. The emulsions containing 7% (m/m) shellac oleogels behaved like the strongest systems, (G′ & GLVR > 30,000 Pa) and exhibited the highest value of the G′-G″ cross-over. The lowest oil binding capacity (OBC) was 99.88% for the sample with 3% (m/m) shellac and 20% (m/m) water. The whiteness index (Windex) varied between 58.12 and 78.50. The optimization process indicated that a formulation based on 4.29% (m/m) shellac wax and 24.13% (m/m) water was suitable as a low-fat spread. Full article
(This article belongs to the Special Issue Recent Progress on Oleogels and Organogels)
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<p>Effects of wax and water concentration on the hardness of shellac wax oleogel emulsions.</p>
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<p>Effects of wax and water concentration on the adhesive force of shellac wax oleogel emulsions.</p>
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<p>Effects of wax and water concentration on the determined G’<sub>LVR</sub> of shellac wax oleogel emulsions.</p>
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<p>Appearance and macroscopic properties of the emulsions obtained from shellac wax-based oleogels.</p>
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<p>Effects of wax and water concentration on the determined G<sub>crossover</sub> point of shellac wax oleogel emulsions.</p>
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<p>Effects of wax and water concentration on Stability of shellac wax-based oleogel emulsions.</p>
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<p>Effects of wax and water concentration on the calculated Whiteness index of shellac wax oleogel emulsions.</p>
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<p>The calculated concentration (<span class="html-fig-inline" id="gels-08-00749-i019"><img alt="Gels 08 00749 i019" src="/gels/gels-08-00749/article_deploy/html/images/gels-08-00749-i019.png"/></span>) of water (A) and shellac wax (B) and the responses (<span class="html-fig-inline" id="gels-08-00749-i020"><img alt="Gels 08 00749 i020" src="/gels/gels-08-00749/article_deploy/html/images/gels-08-00749-i020.png"/></span>) of shellac wax-based oleogel emulsion suitable as low-fat margarine replacer, as given by Design Expert Software in the optimization test.</p>
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<p>The dendrogram of shellac wax emulsion oleogels (1–9) and the margarine formulation (10), based on the structural analysis (Cluster 1 <b><span style="color:red">–</span></b>, Cluster 2 <b><span style="color:#92D050">–</span></b>, Cluster 3 <b><span style="color:#FFC000">–</span></b>, Cluster 4 <b><span style="color:#2F5496">–</span></b>, Cluster 5 <b><span style="color:#E020AE">–</span></b>)</p>
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<p>FTIR spectra of shellac wax-based emulsion oleogels, containing (<b>a</b>) 7% shellac wax and various water concentrations (20–60%), (<b>b</b>) 60% water and various shellac concentration (3–7%), (<b>c</b>) 5% shellac wax and various water concentration (20–60%), (<b>d</b>) 40% water and various shellac concentration (3–7%), (<b>e</b>) 3% Shellac wax and various water concentration (20–60%), and (<b>f</b>) 20% water and various shellac concentration (3–7%).</p>
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<p>FTIR spectra of shellac wax-based emulsion oleogels, containing (<b>a</b>) 7% shellac wax and various water concentrations (20–60%), (<b>b</b>) 60% water and various shellac concentration (3–7%), (<b>c</b>) 5% shellac wax and various water concentration (20–60%), (<b>d</b>) 40% water and various shellac concentration (3–7%), (<b>e</b>) 3% Shellac wax and various water concentration (20–60%), and (<b>f</b>) 20% water and various shellac concentration (3–7%).</p>
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29 pages, 6125 KiB  
Review
Natural Materials for 3D Printing and Their Applications
by Chunyu Su, Yutong Chen, Shujing Tian, Chunxiu Lu and Qizhuang Lv
Gels 2022, 8(11), 748; https://doi.org/10.3390/gels8110748 - 17 Nov 2022
Cited by 23 | Viewed by 5754
Abstract
In recent years, 3D printing has gradually become a well-known new topic and a research hotspot. At the same time, the advent of 3D printing is inseparable from the preparation of bio-ink. Natural materials have the advantages of low toxicity or even non-toxicity, [...] Read more.
In recent years, 3D printing has gradually become a well-known new topic and a research hotspot. At the same time, the advent of 3D printing is inseparable from the preparation of bio-ink. Natural materials have the advantages of low toxicity or even non-toxicity, there being abundant raw materials, easy processing and modification, excellent mechanical properties, good biocompatibility, and high cell activity, making them very suitable for the preparation of bio-ink. With the help of 3D printing technology, the prepared materials and scaffolds can be widely used in tissue engineering and other fields. Firstly, we introduce the natural materials and their properties for 3D printing and summarize the physical and chemical properties of these natural materials and their applications in tissue engineering after modification. Secondly, we discuss the modification methods used for 3D printing materials, including physical, chemical, and protein self-assembly methods. We also discuss the method of 3D printing. Then, we summarize the application of natural materials for 3D printing in tissue engineering, skin tissue, cartilage tissue, bone tissue, and vascular tissue. Finally, we also express some views on the research and application of these natural materials. Full article
(This article belongs to the Special Issue 3D Printing of Gel-Based Materials)
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<p>Schematic diagram of the preparation of some protein bioscaffolds and bio-inks. (<b>A</b>) Schematic representation of the 3D printed Col–chitosan scaffold [<a href="#B15-gels-08-00748" class="html-bibr">15</a>]. (<b>B</b>) Schematic diagram of the preparation of CNF/GelMA bio-inks and their use for 3D printing into scaffolds [<a href="#B16-gels-08-00748" class="html-bibr">16</a>]. (<b>C</b>) Schematic diagram of the preparation of the SF–chitosan composite scaffold [<a href="#B17-gels-08-00748" class="html-bibr">17</a>]. (<b>D</b>) Schematic diagram of the preparation of the BSA–MA hydrogel [<a href="#B18-gels-08-00748" class="html-bibr">18</a>].</p>
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<p>Schematic diagram of the preparation of biocomposite scaffolds and bio-inks using proteinaceous natural materials. (<b>A</b>) Schematic diagram of the preparation of the Col/SF/CaO-SiO<sub>2</sub> composite fibers [<a href="#B31-gels-08-00748" class="html-bibr">31</a>]. (<b>B</b>) Schematic diagram of the preparation of the PCL/elastin composite scaffold [<a href="#B32-gels-08-00748" class="html-bibr">32</a>]. (<b>C</b>) Schematic diagram of the preparation of the KEMA bio-ink [<a href="#B33-gels-08-00748" class="html-bibr">33</a>]. (<b>D</b>) Schematic diagram of the preparation of the GF/LAgel composite scaffold [<a href="#B34-gels-08-00748" class="html-bibr">34</a>].</p>
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<p>Schematic diagram for the preparation of bio-scaffolds, composites, and hydrogels using polysaccharides. (<b>A</b>) Schematic diagram of the preparation of the chitosan–agarose membrane as a skin surrogate [<a href="#B47-gels-08-00748" class="html-bibr">47</a>]. (<b>B</b>) Schematic diagram of the water-based light-cured PU/HA scaffolds preparation [<a href="#B48-gels-08-00748" class="html-bibr">48</a>]. (<b>C</b>) Schematic diagram of the preparation of the gelatin/chitosan/PVA/nHAp (GCPH) composite scaffold [<a href="#B49-gels-08-00748" class="html-bibr">49</a>]. (<b>D</b>) Schematic diagram of the preparation of the TCS-A-PEG-N porous hydrogel network [<a href="#B50-gels-08-00748" class="html-bibr">50</a>].</p>
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<p>Schematic diagram of the preparation of related polysaccharide bio-inks and bioscaffolds. (<b>A</b>) Bioprinting of MA-k-CA bio-ink [<a href="#B70-gels-08-00748" class="html-bibr">70</a>]. (<b>B</b>) Schematic diagram of preparation of PVA-XG hydrogel [<a href="#B71-gels-08-00748" class="html-bibr">71</a>]. (<b>C</b>) Schematic diagram of preparation of Dex-G glucose-sensitive hydrogel [<a href="#B72-gels-08-00748" class="html-bibr">72</a>]. (<b>D</b>) Schematic diagram of preparation of a double-layer tubular biological scaffold modified by heparin [<a href="#B73-gels-08-00748" class="html-bibr">73</a>].</p>
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<p>Schematic diagram of the preparation of a composite scaffold and hydrogel using polysaccharides and ECM. (<b>A</b>) Schematic diagram of preparation of chitosan–nHA–Fu biocomposite scaffold [<a href="#B86-gels-08-00748" class="html-bibr">86</a>]. (<b>B</b>) Schematic diagram of preparation of guar gum–-MA hydrogel [<a href="#B87-gels-08-00748" class="html-bibr">87</a>]. (<b>C</b>) Schematic diagram of preparation of pectin hydrogel nanofiber holders [<a href="#B88-gels-08-00748" class="html-bibr">88</a>]. (<b>D</b>) Schematic diagram of the preparation of chitosan–SA–ECM scaffold material [<a href="#B89-gels-08-00748" class="html-bibr">89</a>].</p>
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<p>Processing and modification of natural biological materials. (<b>A</b>) Schematic diagram of HBSAC hydrogel scaffold prepared via Ca<sup>2+</sup> modification [<a href="#B113-gels-08-00748" class="html-bibr">113</a>]. (<b>B</b>) Schematic diagram of the preparation of CMCS-TA hydrogels under HRP operation [<a href="#B114-gels-08-00748" class="html-bibr">114</a>]. (<b>C</b>) Schematic diagram of the protein self-assembly of silk fibroin in aqueous solution [<a href="#B115-gels-08-00748" class="html-bibr">115</a>].</p>
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<p>Schematic diagram of 3D printing methods and principles. (<b>A</b>) Extrusion and coaxial extrusion [<a href="#B122-gels-08-00748" class="html-bibr">122</a>]. (<b>B</b>) Basic principle of continuous inkjet [<a href="#B123-gels-08-00748" class="html-bibr">123</a>]. (<b>C</b>) Schematic diagram of an on-demand inkjet printer [<a href="#B123-gels-08-00748" class="html-bibr">123</a>]. (<b>D</b>) Schematic diagram of 3D printing mechanism of molten deposition modeling [<a href="#B124-gels-08-00748" class="html-bibr">124</a>].</p>
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<p>Schematic diagram of hydrogels, bio-scaffolds, and bio-inks prepared from related natural materials and used for 3D printing. (<b>A</b>) Schematic diagram of the preparation of GelMA/pectin-g-PCL hydrogels [<a href="#B143-gels-08-00748" class="html-bibr">143</a>]. (<b>B</b>) Preparation of CS–RHCMA bio-ink and its use for 3D printing [<a href="#B144-gels-08-00748" class="html-bibr">144</a>]. (<b>C</b>) Schematic diagram of the preparation of 3D printed GelMA/HA-NB/LAP hydrogel [<a href="#B145-gels-08-00748" class="html-bibr">145</a>]. (<b>D</b>) Schematic diagram of the preparation of PO/OD bio-scaffold [<a href="#B146-gels-08-00748" class="html-bibr">146</a>].</p>
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<p>Schematic diagram of biomodification and preparation of bio-scaffolds using related natural materials. (<b>A</b>) Schematic diagram of the modification of ALMA using alginate [<a href="#B158-gels-08-00748" class="html-bibr">158</a>]. (<b>B</b>) Schematic diagram of the preparation of SF/OCP/PDA scaffold [<a href="#B159-gels-08-00748" class="html-bibr">159</a>]. (<b>C</b>) Schematic diagram of the preparation of SA–Chitosan–Col–GO composite scaffold [<a href="#B160-gels-08-00748" class="html-bibr">160</a>].</p>
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<p>Schematic representation of the preparation of bio-scaffolds, nanofibers, and hydrogels using related natural materials. (<b>A</b>) Schematic diagram of SF scaffold prepared via 3D printing technology [<a href="#B166-gels-08-00748" class="html-bibr">166</a>]. (<b>B</b>) Schematic representation of the preparation of CS–gelatin–PCL composite nanofibers [<a href="#B167-gels-08-00748" class="html-bibr">167</a>]. (<b>C</b>) Schematic diagram of a hydrogel printed using HAMA/pECM bio-ink [<a href="#B168-gels-08-00748" class="html-bibr">168</a>].</p>
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14 pages, 2049 KiB  
Article
Effect of Composite Chitosan/Sodium Alginate Gel Coatings on the Quality of Fresh-Cut Purple-Flesh Sweet Potato
by Chit-Swe Chit, Ibukunoluwa Fola Olawuyi, Jong Jin Park and Won Young Lee
Gels 2022, 8(11), 747; https://doi.org/10.3390/gels8110747 - 17 Nov 2022
Cited by 5 | Viewed by 2543
Abstract
In this study, single-layer coating using chitosan (Ch) and sodium alginate (SA) solutions and their gel coating (ChCSA) formed by layer-by-layer (LbL) electrostatic deposition using calcium chloride (C) as a cross linking agent were prepared to improve storage qualities and shelf-life of fresh-cut [...] Read more.
In this study, single-layer coating using chitosan (Ch) and sodium alginate (SA) solutions and their gel coating (ChCSA) formed by layer-by-layer (LbL) electrostatic deposition using calcium chloride (C) as a cross linking agent were prepared to improve storage qualities and shelf-life of fresh-cut purple-flesh sweet potatoes (PFSP). The preservative effects of single-layer coating in comparison with LbL on the quality parameters of fresh-cut PFSP, including color change, weight loss, firmness, microbial analysis, CO2 production, pH, solid content, total anthocyanin content (TAC), and total phenolic content (TPC) were evaluated during 16 days of storage at 5 °C. Uncoated samples were applicable as a control. The result established the effectiveness of coating in reducing microbial proliferation (~2 times), color changes (~3 times), and weight loss (~4 times) with negligible firmness losses after the storage period. In addition, TAC and TPC were better retained in the coated samples than in the uncoated samples. In contrast, quality deterioration was observed in the uncoated fresh cuts, which progressed with storage time. Relatively, gel-coating ChCSA showed superior effects in preserving the quality of fresh-cut PFSP and could be suggested as a commercial method for preserving fresh-cut purple-flesh sweet potato and other similar roots. Full article
(This article belongs to the Special Issue Bioactive Gel Films and Coatings Applied in Active Food Packaging)
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<p>The effect of single-layer and gel coatings on the changes in total color difference value (ΔE) of fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of single-layer and gel coatings on the percentage of weight loss of fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of single-layer and gel coatings on the flesh firmness of fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of single-layer and gel coatings on the aerobic bacteria on fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of single-layer and gel coatings on the yeast and mold on fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of layer-by-layer and single-layer coatings on the percentage of carbon dioxide gas emission on fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of layer-by-layer and single-layer coatings on the percentage of <sup>o</sup>Brix of fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of single-layer and gel coatings on the pH on fresh-cut purple sweet potato potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of single-layer and gel coatings on the anthocyanin content on fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>The effect of single-layer and gel coatings on the total phenolic content on fresh-cut purple sweet potatoes. Vertical bars represent means and standard deviation. Bars with different alphabets within the same storage day (lower case) or same treatment group at different storage days (upper case) are significantly different (Tukey’s HSD Test, <span class="html-italic">p ≤</span> 0.05).</p>
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<p>Illustration of coating procedure for fresh-cut purple flesh sweet potatoes.</p>
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20 pages, 5550 KiB  
Article
In Vitro and Ex Vivo Evaluation of Fluocinolone Acetonide–Acitretin-Coloaded Nanostructured Lipid Carriers for Topical Treatment of Psoriasis
by Hassan Raza, Shefaat Ullah Shah, Zakir Ali, Atif Ullah Khan, Irfa Basharat Rajput, Arshad Farid, Mohammed Al Mohaini, Abdulkhaliq J. Alsalman, Maitham A. Al Hawaj, Saima Mahmood, Abid Hussain and Kifayat Ullah Shah
Gels 2022, 8(11), 746; https://doi.org/10.3390/gels8110746 - 17 Nov 2022
Cited by 13 | Viewed by 2976
Abstract
Psoriasis is chronic autoimmune disease that affects 2–5% of the global population. Fluocinolone acetonide (FLU) and acitretin (ACT) are widely used antipsoriatic drugs that belong to BCS classes II and IV, respectively. FLU exhibits side effects, such as skin irritation and a burning [...] Read more.
Psoriasis is chronic autoimmune disease that affects 2–5% of the global population. Fluocinolone acetonide (FLU) and acitretin (ACT) are widely used antipsoriatic drugs that belong to BCS classes II and IV, respectively. FLU exhibits side effects, such as skin irritation and a burning sensation. ACT also shows adverse effects, such as gingivitis, teratogenic effects and xerophthalmia. In the present study, topical nanostructured lipid carriers (NLCs) were fabricated to reduce the side effects and enhance the therapeutic efficacy. FLU–ACT-coloaded NLCs were prepared by the modified microemulsion method and optimized by the Box–Behnken model of Design Expert® version 12. The optimization was based on the particle size (PS), zeta potential (ZP) and percentage of encapsulation efficiency (%EE). The physicochemical analyses were performed by TEM, FTIR, XRD and DSC to assess the morphology, chemical interactions between excipients, crystallinity and thermal behavior of the optimized FLU–ACT-coloaded NLCs. The FLU–ACT-coloaded NLCs were successfully loaded into gel and characterized appropriately. The dialysis bag method and Franz diffusion cells were used for the in vitro release and ex vivo permeation studies, respectively. The optimized FLU–ACT-coloaded NLCs had the desired particle size of 288.2 ± 2.3 nm, ZP of −34.2 ± 1.0 mV and %EE values of 81.6 ± 1.1% for ACT and 75 ± 1.3% for FLU. The TEM results confirmed the spherical morphology, while the FTIR results showed the absence of chemical interactions of any type among the ingredients of the FLU–ACT-coloaded NLCs. The XRD and DSC analyses confirmed the amorphous nature and thermal behavior. The in vitro study showed the sustained release of the FLU and ACT from the optimized FLU–ACT-coloaded NLCs and FLU–ACT-coloaded NLC gel compared with the FLU–ACT suspension and conventional gel. The ex vivo study confirmed the minimal permeation of both drugs from the FLU–ACT-coloaded NLC gel. Full article
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<p>Desirability and point prediction data provided by Design Expert<sup>®</sup> for the selection of the optimized formulation.</p>
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<p>3D response surface graphs: effects of lipids, surfactants and drugs on particle size (<b>a</b>–<b>c</b>); zeta potential (<b>d</b>–<b>f</b>): % entrapment efficiency of acitretin (<b>g</b>–<b>i</b>): % entrapment efficiency of fluocinolone (<b>j</b>–<b>l</b>).</p>
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<p>3D response surface graphs: effects of lipids, surfactants and drugs on particle size (<b>a</b>–<b>c</b>); zeta potential (<b>d</b>–<b>f</b>): % entrapment efficiency of acitretin (<b>g</b>–<b>i</b>): % entrapment efficiency of fluocinolone (<b>j</b>–<b>l</b>).</p>
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<p>Particle characterization: (<b>a</b>) particle size and PDI analysis; (<b>b</b>) zeta potential analysis; (<b>c</b>) TEM analysis.</p>
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<p>Particle characterization: (<b>a</b>) particle size and PDI analysis; (<b>b</b>) zeta potential analysis; (<b>c</b>) TEM analysis.</p>
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<p>XRD analysis of acitretin, fluocinolone, stearic acid and lyophilized optimized FLU–ACT-coloaded NLCs.</p>
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<p>DSC analyses of fluocinolone, acitretin and optimized FLU–ACT-coloaded NLCs.</p>
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<p>FTIR analysis of fluocinolone, acitretin, stearic acid, oleic acid and lyophilized FLU–ACT-coloaded NLCs.</p>
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<p>Histopathological analysis of: (<b>a</b>) positive control; (<b>b</b>) FLU–ACT–coloaded NLC treatment; (<b>c</b>) negative control.</p>
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<p>In vitro release profiles of fluocinolone at (<b>a</b>) pH of 5.5 and (<b>b</b>) pH of 7.4, and acitretin at (<b>c</b>) pH of 5.5 and (<b>d</b>) pH of 7.4.</p>
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<p>Ex vivo permeability data of FLU–ACT-coloaded NLC gel and FLU–ACT conventional gel.</p>
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13 pages, 4375 KiB  
Article
Facile Construction of Hybrid Hydrogels with High Strength and Biocompatibility for Cranial Bone Regeneration
by Shuai Chang, Jiedong Wang, Nanfang Xu, Shaobo Wang, Hong Cai, Zhongjun Liu and Xing Wang
Gels 2022, 8(11), 745; https://doi.org/10.3390/gels8110745 - 17 Nov 2022
Cited by 6 | Viewed by 2470
Abstract
The significant efforts being made towards the utilization of artificial soft materials holds considerable promise for developing tissue engineering scaffolds for bone-related diseases in clinics. However, most of these biomaterials cannot simultaneously satisfy the multiple requirements of high mechanics, good compatibility, and biological [...] Read more.
The significant efforts being made towards the utilization of artificial soft materials holds considerable promise for developing tissue engineering scaffolds for bone-related diseases in clinics. However, most of these biomaterials cannot simultaneously satisfy the multiple requirements of high mechanics, good compatibility, and biological osteogenesis. In this study, an osteogenic hybrid hydrogel between the amine-functionalized bioactive glass (ABG) and 4-armed poly(ethylene glycol) succinimidyl glutarate-gelatin network (SGgel) is introduced to flexibly adhere onto the defective tissue and to subsequently guide bone regeneration. Relying on the rapid ammonolysis reaction between amine groups (-NH2) of gelatin and ABG components and N-hydroxysuccinimide (NHS)-ester of tetra-PEG-SG polymer, the hydrogel networks were formed within seconds, offering a multifunctional performance, including easy injection, favorable biocompatibility, biological and mechanical properties (compressive strength: 4.2 MPa; storage modulus: 104 kPa; adhesive strength: 56 kPa), which could facilitate the stem cell viability, proliferation, migration and differentiation into osteocytes. In addition, the integration between the SGgel network and ABG moieties within a nano-scale level enabled the hybrid hydrogel to form adhesion to tissue, maintain the durable osteogenesis and accelerate bone regeneration. Therefore, a robust approach to the simultaneously satisfying tough adhesion onto the tissue defects and high efficiency for bone regeneration on a mouse skull was achieved, which may represent a promising strategy to design therapeutic scaffolds for tissue engineering in clinical applications. Full article
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<p>Schematic illustration of the fabrication procedures of SGgel@ABG composite hydrogel for calvaria bone defects repair.</p>
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<p>Structure and property characterizations. (<b>A</b>) Synthesis route of modified polymers and amine-functionalized ABG. (<b>B</b>) <sup>1</sup>H NMR spectrum of the tetra-PEG-SG polymer. (<b>C</b>–<b>F</b>) SEM images, compressive, rheology and adhesive profiles of (<b>a</b>) SGgel and (<b>b</b>) SGgel@ABG hydrogels. Red arrows represent the similar inner pores.</p>
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<p>Cell cytotoxicity of SGgel and SGgel@ABG hybrid scaffolds in vitro. (<b>A</b>) Live/dead staining of BMSCs. Wherein, the green cells are the living BMSCs, and the red cells are the dead BMSCs. (<b>B</b>) Cell viability and (<b>C</b>) Cell proliferation of SGgel and SGgel@ABG hybrid scaffolds after the cultivation for the appointed time. NS, not significant.</p>
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<p>In vitro osteogenic differentiation of SGgel@ABG hydrogel. (<b>A</b>–<b>C</b>) ALP (14 d) and ARS staining (21 d) revealing the enhanced osteogenic differentiation of BMSCs. (<b>D</b>,<b>E</b>) Western blotting analysis and (<b>F</b>) qPCR quantification showing the highest osteogenic expression markers (OCN, ALP, Osterix and RUNX2) in the hydrogels. Statistically significant differences in comparison with untreated cells (control), SGgel hydrogel and SGgel@ABG hydrogel. ** <span class="html-italic">p</span> &lt; 0.01.</p>
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<p>(<b>A</b>) 3D reconstruction of Micro-CT images of regenerated bone formation in rat cranium after the hydrogel implantation for 8 weeks with control group, SGgel group and SGgel@ABG group. (<b>B</b>–<b>D</b>) Quantitative analysis of BV, BV/TV and BMD of newly formed bone tissue. (<b>E</b>) H&amp;E and Masson’s trichrome staining. (<b>F</b>,<b>G</b>) Woven bone and cartilage areas were analyzed in defect bone region. ** <span class="html-italic">p</span> &lt; 0.01.</p>
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13 pages, 7214 KiB  
Article
Preparation and Properties of Highly Transparent SiO2 Aerogels for Thermal Insulation
by Baolu Shi, Long Xie, Bin Ma, Zhiliang Zhou, Baosheng Xu and Lijie Qu
Gels 2022, 8(11), 744; https://doi.org/10.3390/gels8110744 - 16 Nov 2022
Cited by 26 | Viewed by 5196
Abstract
SiO2 aerogels have attracted extensive attention due to their unique structural characteristics, which exhibit many special properties, especially good optical transparency. As far as we know, the sol-gel stage during the synthesis of aerogel plays an important role in the construction of [...] Read more.
SiO2 aerogels have attracted extensive attention due to their unique structural characteristics, which exhibit many special properties, especially good optical transparency. As far as we know, the sol-gel stage during the synthesis of aerogel plays an important role in the construction of the gel skeleton. In this study, we adjusted the amount of silicon source and catalyst to explore the best scheme for preparing highly transparent SiO2 aerogels, and further clarify the effects of both on the properties of SiO2 aerogels. Results indicated that the pore size distribution was between 10 and 20 nm, the thermal conductivity was between 0.0135 and 0.021 W/(m·K), and the transmittance reached 97.78% at 800 nm of the aerogels, better than most studies. Therefore, it has the potential to be used in aerogel glass for thermal insulation. Full article
(This article belongs to the Special Issue Gels as High-Performance Thermal Insulation Materials)
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<p>FTIR spectrum of SiO<sub>2</sub> aerogels.</p>
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<p>SEM of SiO<sub>2</sub> aerogels: the concentration of NH<sub>4</sub>OH solution was 0.75 mol/L and the mass fractions of TMOS were (<b>a</b>) 15 wt.%; (<b>b</b>) 25 wt.%; (<b>c</b>) 35 wt.%; (<b>d</b>) 45 wt.%.</p>
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<p>SEM of SiO<sub>2</sub> aerogels: the mass fraction of TMOS was 45 wt.% and the concentration of NH<sub>4</sub>OH solutions were (<b>a</b>) 0.15 mol/L; (<b>b</b>) 0.30 mol/L; (<b>c</b>) 0.45 mol/L; (<b>d</b>) 0.60 mol/L; (<b>e</b>) 0.75 mol/L.</p>
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<p>(<b>a</b>) N<sub>2</sub> adsorption-desorption isotherm curves of SiO<sub>2</sub> aerogels; (<b>b</b>) pore size distribution curves of SiO<sub>2</sub> aerogels.</p>
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<p>(<b>a</b>) The heat transfer modes in aerogels; (<b>b</b>) thermal conductivity curves of SiO<sub>2</sub> aerogels.</p>
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<p>The infrared thermal imaging of the SiO<sub>2</sub> aerogel.</p>
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<p>The propagation paths of light in SiO<sub>2</sub> aerogels.</p>
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<p>Transmittance curves of SiO<sub>2</sub> aerogels with different TMOS mass fractions: (<b>a</b>) 15 wt.%; (<b>b</b>) 25 wt.%; (<b>c</b>) 35 wt.%; (<b>d</b>) 45 wt.%; (<b>e</b>) the highest transmittance among the TMOS mass fractions of 15–45 wt.% and its (<b>f</b>) local magnification of wavelengths from 750 nm to 850 nm.</p>
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<p>Schematic of preparation process of highly transparent SiO<sub>2</sub> aerogels.</p>
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<p>(<b>a</b>) Hydrolysis reaction of TMOS; (<b>b</b>) condensation reaction of TMOS after hydrolysis; (<b>c</b>) further cross-linking by condensation reaction to form a 3D network.</p>
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<p>Pictures of SiO<sub>2</sub> aerogels with difference transparency: (<b>a</b>) sample 12 and (<b>b</b>) sample 20.</p>
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19 pages, 6743 KiB  
Article
Influence of Copper-Strontium Co-Doping on Bioactivity, Cytotoxicity and Antibacterial Activity of Mesoporous Bioactive Glass
by Akrity Anand, Susanta Sengupta, Hana Kaňková, Anna Švančárková, Ana M. Beltrán, Dušan Galusek, Aldo R. Boccaccini and Dagmar Galusková
Gels 2022, 8(11), 743; https://doi.org/10.3390/gels8110743 - 16 Nov 2022
Cited by 22 | Viewed by 2906
Abstract
Mesoporous bioactive glass (MBG) is an extensively studied biomaterial used for the healing of bone defects. Its biological applications can be tailored by introducing metallic ions, such as strontium (Sr) and copper (Cu), which can enhance its functionalities, including osteogenetic, angiogenetic and antibacterial [...] Read more.
Mesoporous bioactive glass (MBG) is an extensively studied biomaterial used for the healing of bone defects. Its biological applications can be tailored by introducing metallic ions, such as strontium (Sr) and copper (Cu), which can enhance its functionalities, including osteogenetic, angiogenetic and antibacterial functionalities. In this study, Cu and Sr ions were co-doped (ratio 1:1) with x = 0.5, 1 and 2 mol% each in glass with an intended nominal composition of 80SiO2-(15-2x)CaO-5P2O5-xCuO-xSrO and synthesized with an evaporation-induced self-assembly (EISA)-based sol-gel technique. XRD confirmed the amorphous nature of the glass, while compositional analysis using ICP-OES confirmed the presence of dopant ions with the required amounts. A TEM study of the MBG powders showed fringes that corresponded to the formation of a highly ordered mesoporous structure. The Cu-Sr-doped MBG showed a positive effect on apatite formation when immersed in SBF, although the release of Cu and Sr ions was relatively slow for 1 mol% of each co-dopant, which signified a stable network structure in the glass. The impact of the Cu and Sr ions on the osteoblast-like cell line MG-63 was assessed. At the particle concentrations of 1 wt./vol.% or lower, the cell viability was above 50%. An antibacterial test was conducted against Gram-negative E. coli and Gram-positive S. aureus bacteria. With a sequential increase in the co-doped ion content in the glass, the zone of inhibition for bacteria increased. The results suggest that the doping of MBG with Cu and Sr ions at up to 2 mol% can result in tailored sustained release of ions to enhance the applicability of the studied glass as a functional biomaterial for bone regeneration applications. Full article
(This article belongs to the Special Issue High-Surface Area Advanced Materials and Their Applications)
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<p>DTA (<b>a</b>) and TGA (<b>b</b>) plots of as-prepared base glass (80G) and co-doped CS-MBG (1CS, 2CS, 4CS) powders.</p>
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<p>Represents the XRD patterns of the base and CS-MBG powders calcined at 700 °C.</p>
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<p>N<sub>2</sub> adsorption–desorption isotherm plots of base glass and co-doped MBG.</p>
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<p>TEM images with EDX analysis of MBG powders. (<b>a</b>) 80G, (<b>b</b>) 1CS, (<b>c</b>) 2CS and (<b>d</b>) 4CS2.2. In vitro Bioactivity Assessment.</p>
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<p>Release profile Si, Ca, P, Cu and Sr ions (mg/L) in SBF and pH measurements for base glass (80G) and co-doped MBG (1CS, 2CS and 4CS).</p>
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<p>XRD patterns of SBF soaked MBG powders after (<b>a</b>) 24 h, (<b>b</b>) 7 days, and (<b>c</b>) 14 days; (red star marks indicate possible formation of a new hydroxyapatite (HAp) phase.</p>
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<p>FTIR spectra of all MBG powders before and after 0 h, 4 h, 8 h, 24 h, 7 d and 14 d of immersion in SBF.</p>
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<p>FESEM images of bare MBG powders and after SBF soaked (7 and 14 days) MBG powders.</p>
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<p>Relative cell viability percentage of MG-63 cells cultured with 0.1, 1, 5 and 10 wt./vol.% extract of MBG (n = 9, PC = positive control, NC = Negative control, samples in triplicate, * <span class="html-italic">p</span> &lt; 0.05).</p>
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<p>H&amp;E-stained images of MG-63 cells cultured with 0.1 and 1 wt./vol.% extract of MBG along with positive control (PC) and negative control (NC).</p>
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<p>Photographic images of MBG pellets treated with Gram-negative (<span class="html-italic">E. coli</span>) and Gram-positive (<span class="html-italic">S. aureus</span>) bacteria using the agar disk diffusion method.</p>
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16 pages, 2298 KiB  
Article
A Top-Down Procedure for Synthesizing Calcium Carbonate-Enriched Chitosan from Shrimp Shell Wastes
by Andreea Miron, Andrei Sarbu, Anamaria Zaharia, Teodor Sandu, Horia Iovu, Radu Claudiu Fierascu, Ana-Lorena Neagu, Anita-Laura Chiriac and Tanta-Verona Iordache
Gels 2022, 8(11), 742; https://doi.org/10.3390/gels8110742 - 15 Nov 2022
Cited by 16 | Viewed by 4119
Abstract
Chitosan is used in medicine, pharmaceuticals, cosmetics, agriculture, water treatment, and food due to its superior biocompatibility and biodegradability. Nevertheless, the complex and relatively expensive extraction costs hamper its exploitation and, implicitly, the recycling of marine waste, the most abundant source of chitosan. [...] Read more.
Chitosan is used in medicine, pharmaceuticals, cosmetics, agriculture, water treatment, and food due to its superior biocompatibility and biodegradability. Nevertheless, the complex and relatively expensive extraction costs hamper its exploitation and, implicitly, the recycling of marine waste, the most abundant source of chitosan. In the spirit of developing environmental-friendly and cost-effective procedures, the present study describes one method worth consideration to deliver calcium-carbonate-enriched chitosan from shrimp shell waste, which proposes to maintain the native minerals in the structure of chitin in order to improve the thermal stability and processability of chitosan. Therefore, a synthesis protocol was developed starting from an optimized deacetylation procedure using commercial chitin. The ultimate chitosan product from shrimp shells, containing native calcium carbonate, was further compared to commercial chitosan and chitosan synthesized from commercial chitin. Finally, the collected data during the study pointed out that the prospected method succeeded in delivering calcium-carbonate-enriched chitosan with high deacetylation degree (approximately 75%), low molecular weight (Mn ≈ 10.000 g/ mol), a crystallinity above 59 calculated in the (020) plane, high thermal stability (maximum decomposition temperature over 300 °C), and constant viscosity on a wide range of share rates (quasi-Newtonian behavior), becoming a viable candidate for future chitosan-based materials that can expand the application horizon. Full article
(This article belongs to the Special Issue Chitosan Functional Hydrogels: Synthesis and Applications)
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<p>FTIR spectra of the obtained commercial chitin-derived chitosan samples at different deacetylation times.</p>
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<p>FTIR spectra of the SH, CHSH, and CHC (<b>a</b>) and of CC, CCHC6, and CCHSH (<b>b</b>) samples.</p>
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<p>XRD patterns for the SH, CHSH, and CHC (<b>a</b>) and CC, CCHC6, and CCHSH (<b>b</b>) series.</p>
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<p>TGA (<b>a</b>) and DTG (<b>b</b>) curves for SH, CHSH, and CHC samples; TGA (<b>c</b>) and DTG (<b>d</b>) curves for CC, CCHC6, and CCHSH samples.</p>
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<p>N<sub>2</sub> adsorption/desorption isotherms of (<b>a</b>) SH, (<b>b</b>) CHSH, (<b>c</b>) CHC, (<b>d</b>) CC, (<b>e</b>) CCHC6, and (<b>f</b>) CCHSH materials. Inset: Pore distribution diagram (0–40 nm range).</p>
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<p>Viscosity (<b>a</b>) and stress (<b>b</b>) analysis of commercial chitosan (CC), chitosan obtained from commercial chitin (CCHC6), and chitosan obtained from shrimp shells (CCHSH).</p>
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<p>Preparation process of calcium-carbonate-enriched chitosan from shrimp shells waste.</p>
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24 pages, 3797 KiB  
Review
Developments on the Smart Hydrogel-Based Drug Delivery System for Oral Tumor Therapy
by Yiwen Zhao, Bei Ran, Xi Xie, Wanrong Gu, Xiuwen Ye and Jinfeng Liao
Gels 2022, 8(11), 741; https://doi.org/10.3390/gels8110741 - 15 Nov 2022
Cited by 20 | Viewed by 4863
Abstract
At present, an oral tumor is usually treated by surgery combined with preoperative or postoperative radiotherapies and chemotherapies. However, traditional chemotherapies frequently result in substantial toxic side effects, including bone marrow suppression, malfunction of the liver and kidneys, and neurotoxicity. As a new [...] Read more.
At present, an oral tumor is usually treated by surgery combined with preoperative or postoperative radiotherapies and chemotherapies. However, traditional chemotherapies frequently result in substantial toxic side effects, including bone marrow suppression, malfunction of the liver and kidneys, and neurotoxicity. As a new local drug delivery system, the smart drug delivery system based on hydrogel can control drug release in time and space, and effectively alleviate or avoid these problems. Environmentally responsive hydrogels for smart drug delivery could be triggered by temperature, photoelectricity, enzyme, and pH. An overview of the most recent research on smart hydrogels and their controlled-release drug delivery systems for the treatment of oral cancer is given in this review. It is anticipated that the local drug release method and environment-responsive benefits of smart hydrogels will offer a novel technique for the low-toxicity and highly effective treatment of oral malignancy. Full article
(This article belongs to the Special Issue Gels: Applications in Drug Delivery and Tissue Engineering)
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<p>The smart hydrogel-based drug delivery system for oral cancer therapy.</p>
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<p>Drug release mechanism of the photosensitive hydrogel. (<b>a</b>) The photosensitive hydrogel containing photothermal agent; (<b>b</b>) Introducing photosensitive groups onto the chain of the gel polymer.</p>
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<p>Schematic illustration of Dox/Cel/MOFs@Gel as novel injectable metal–organic frameworks@thermosensitive hydrogel local dual drug delivery for oral cancer therapy. Reprinted with permission [<a href="#B109-gels-08-00741" class="html-bibr">109</a>].</p>
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<p>Schematic diagram of the in situ thermosensitive hydrogel containing GA micelles for improving anti-tumor immunity against OSCC. The GA micelle-encapsulated PLEL sol was locally injected into the tumor, formed hydrogel at body temperature, and continually released GA in situ, thus exerting the chemotherapeutic effect and anti-tumor immune activation. Reprinted with permission [<a href="#B128-gels-08-00741" class="html-bibr">128</a>].</p>
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<p>(<b>a</b>) The preparation of NIR-responsive MC/IR820-MSNs/DOX and (<b>b</b>) its use in the localized synergistic photochemotherapy of OSCC. Reprinted with permission [<a href="#B143-gels-08-00741" class="html-bibr">143</a>].</p>
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<p>Schematic illustration of the formation of (<b>A</b>,<b>B</b>) the pH-responsive peptide hydrogel and (<b>C</b>) the anti-tumor mechanism of the pH-responsive peptide hydrogel at the tumor site. Reprinted with permission [<a href="#B152-gels-08-00741" class="html-bibr">152</a>].</p>
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<p>Schematic illustration of GO−Fe<sub>3</sub>O<sub>4</sub>/PNIPAM-AAm/alginate nanocomposite hydrogel microcapsules for controlled drug release. (<b>a</b>) Schematic diagram of the fabrication of GO−Fe<sub>3</sub>O<sub>4</sub>/PNIPAM-AAm/alginate NCH microcapsules based on the centrifugal microfluidic method. (<b>b</b>) GO−Fe<sub>3</sub>O<sub>4</sub>/PNIPAM-AAm/alginate NCH microcapsules for NIR light-, magneto-, and pH-responsive drug release. Reprinted with permission [<a href="#B176-gels-08-00741" class="html-bibr">176</a>].</p>
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15 pages, 6055 KiB  
Article
Stress and Strain Characteristics under the Large Deformation of Surimi Gel during Penetration and Extension Tests Using Digital Image Correlation and the Numerical Simulation Method
by Hwabin Jung, Timilehin Martins Oyinloye and Won Byong Yoon
Gels 2022, 8(11), 740; https://doi.org/10.3390/gels8110740 - 15 Nov 2022
Cited by 2 | Viewed by 2107
Abstract
The stress and strain properties of surimi gels (72.49% moisture content) under large deformation were analyzed during penetration (cylindrical, conical, and spherical puncture) and extension (ring tensile) tests. Mechanical measurements were compared and validated using digital image correlation (DIC) and numerical simulations. The [...] Read more.
The stress and strain properties of surimi gels (72.49% moisture content) under large deformation were analyzed during penetration (cylindrical, conical, and spherical puncture) and extension (ring tensile) tests. Mechanical measurements were compared and validated using digital image correlation (DIC) and numerical simulations. The DIC and the finite element method reflected the influence of the probe shape and the surface area in contact with the gel during the measurements. In puncture tests, a larger probe surface increased the strain concentration at the puncture point. In the extension test, the strain distribution was symmetrical. The strain values observed during penetration tests were comparable in both the DIC and numerical simulation. The tensile failure characteristics observed in DIC and numerical simulations are similar to those found in the experiment. The study demonstrated that the extension method with the ring tensile device did not show a stress concentration during the measurement, and DIC and numerical simulation can be effective tools in analyzing the textural properties of surimi gel during the puncture and ring tensile tests. Full article
(This article belongs to the Special Issue Recent Advance in Food Gels)
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<p>Mechanical properties of surimi gel; (<b>a</b>) Force-time curve from the penetration test, (<b>b</b>) Normalized penetration force per unit area, and (<b>c</b>) Force-time curve from ring tensile until the failure.</p>
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<p>Contour plots of the strain component of surimi gel during a penetration test using (<b>a</b>) a cylindrical probe, (<b>b</b>) a spherical probe, and (<b>c</b>) a conical probe.</p>
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<p>Contour plot of surimi gel displacement during a penetration test using (<b>a</b>) a cylindrical probe, (<b>b</b>) a spherical probe, and (<b>c</b>) a conical probe.</p>
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<p>Contour plots of the strain component for surimi gel during the ring tensile test to the failure point.</p>
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<p>Contour plots of surimi gel displacement during the ring tensile test to the failure point.</p>
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<p>Curve of surimi gel true stress vs. plastic strain.</p>
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<p>Stress curve of various penetration probes during puncture analysis for surimi gel; (<b>a</b>,<b>b</b>) quantitative stress value and (<b>c</b>) contour description of the stress distribution in a puncture gel at a depth of 20 mm.</p>
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<p>Strain curve of various penetration probes during puncture analysis for surimi gel; (<b>a</b>,<b>b</b>) quantitative strain value and (<b>c</b>) contour description of the strain distribution in a puncture gel at a depth of 20 mm.</p>
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<p>Stress distribution in surimi gel during the ring tensile test; (<b>a</b>) quantitative stress value and (<b>b</b>) contour description of the stress concentration region.</p>
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<p>Strain distribution in surimi gel during the ring tensile test; (<b>a</b>) quantitative strain value and (<b>b</b>) contour description of the strain concentration region.</p>
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<p>Schematic representation of the ring tensile test system (<b>a</b>), stainless steel stamp for the preparation of ring-shaped surimi gel (<b>b</b>), and the cylindrical and ring sample for the penetration and ring tensile test (<b>c</b>).</p>
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<p>Schematic diagram of an image acquisition system for (<b>a</b>) penetration test, and (<b>b</b>) ring tensile test.</p>
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<p>Geometry description of surimi gel during numerical analysis (<b>a</b>), and mesh model (<b>b</b>).</p>
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14 pages, 2124 KiB  
Article
Sodium Alginate-Quaternary Polymethacrylate Composites: Characterization of Dispersions and Calcium Ion Cross-Linked Gel Beads
by Wanwisa Khunawattanakul, Napaphak Jaipakdee, Thitiphorn Rongthong, Narin Chansri, Pathomthat Srisuk, Padungkwan Chitropas and Thaned Pongjanyakul
Gels 2022, 8(11), 739; https://doi.org/10.3390/gels8110739 - 15 Nov 2022
Cited by 5 | Viewed by 1896
Abstract
The objective of this work was to examine the effect of quaternary polymethacrylate (QPM), a water-insoluble polymer with a positive charge, on the characteristics of the sodium alginate (SA) dispersions and the calcium alginate (CA) gel beads containing propranolol HCl (PPN). The SA-QPM [...] Read more.
The objective of this work was to examine the effect of quaternary polymethacrylate (QPM), a water-insoluble polymer with a positive charge, on the characteristics of the sodium alginate (SA) dispersions and the calcium alginate (CA) gel beads containing propranolol HCl (PPN). The SA-QPM composite dispersions presented the formation of flocculates with a negative charge due to the electrostatic interaction of both substances. The QPM addition did not affect the SA dispersions’ Newtonian flow, but the composite dispersions’ viscosity enhancement was found. The PPN-loaded CA-QPM gel beads had more spherical than the PPN-loaded CA gel beads. The incorporation of QPM caused a bigger particle size, higher drug entrapment efficiency, and greater particle strength of the gel beads. Despite the similar water uptake property, the PPN-loaded CA-QPM gel beads displayed lower burst release and slower drug release rate than the PPN-loaded CA gel beads. However, the drug release from the PPN-loaded CA-QPM gel beads involved drug diffusion and matrix swelling mechanisms. This study demonstrated that adding QPM into the SA dispersions leads to a viscosity synergism. The CA-QPM gel beads display a good potential for use as a bioactive compound delivery system. Full article
(This article belongs to the Special Issue Physically Cross-Linked Gels and Their Applications)
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<p>Appearance of SA and SA-QPM dispersions after preparation (<bold>a</bold>) and storing at room temperature for 24 h (<bold>b</bold>).</p>
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<p>Microscopic morphology of QPM particles in QPM dispersion (<bold>a</bold>), and SA-QPM dispersions at the ratios of 1:0.5 (<bold>b</bold>), 1:1 (<bold>c</bold>), and 1:2 (<bold>d</bold>).</p>
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<p>Particle size (<bold>a</bold>) and zeta potential (<bold>b</bold>) of dispersed phase in QPM, SA, and SA-QPM dispersions. Each value is the mean ± S.D., <italic>n</italic> = 3.</p>
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<p>Rheograms of SA and SA-QPM dispersions. Each value is the mean ± S.D., <italic>n</italic> = 3.</p>
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<p>Particle morphology of PPN-loaded CA gel bead (<bold>a</bold>) and PPN-loaded CA-QPM gel bead at the SA:QPM ratios of 1:2 (<bold>b</bold>).</p>
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<p>Mechanical property of PPN-loaded CA-QPM gel beads at different SA:QPM ratios. Each value is the mean ± S.D., <italic>n</italic> = 10.</p>
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<p>Water uptake of PPN-loaded CA-QPM gel beads at different SA:QPM ratios. Each value is the mean ± S.D., <italic>n</italic> = 3.</p>
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<p>PPN release profiles of PPN-loaded CA-QPM gel beads at different SA:QPM ratios. Each value is the mean ± S.D., <italic>n</italic> = 3.</p>
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15 pages, 2585 KiB  
Article
The Rheological Properties and Texture of Agar Gels with Canola Oil—Effect of Mixing Rate and Addition of Lecithin
by Ewa Jakubczyk, Anna Kamińska-Dwórznicka and Anna Kot
Gels 2022, 8(11), 738; https://doi.org/10.3390/gels8110738 - 15 Nov 2022
Cited by 10 | Viewed by 3971
Abstract
This study aimed to determine the effect of different mixing rates and the addition of lecithin on the rheological mechanical, and acoustic properties of agar gels with the addition of canola oil. The mixing rate of the agar–oil mixture was changed from 10,000 [...] Read more.
This study aimed to determine the effect of different mixing rates and the addition of lecithin on the rheological mechanical, and acoustic properties of agar gels with the addition of canola oil. The mixing rate of the agar–oil mixture was changed from 10,000 to 13,000 rpm. Additionally, agar gels with the addition of lecithin from 1 to 5% were prepared. The frequency sweep test was used (at 4 and 50 °C) within the linear viscoelastic region (LVR) in oscillatory measurement. The agar–oil mixture was cooled from 80 to 10 °C, enabling the obtainment of the gelling temperature. Texture profile analysis (TPA) and compression tests, as well as the acoustic emission method, were applied to analyse the texture of the gels. The syneresis and stability of gels during storage were also measure. The increase in mixing rate in the case of agar gel with canola oil causes an increase in the elastic component of materials as well hardness and gumminess. Also, samples prepared with the higher mixing rate have more uniform and stable structures, with small bubbles. The increase in the concentration of lecithin is ineffective due to the formation of gels with a weak matrix and low hardness, gumminess, and stability during storage. Full article
(This article belongs to the Special Issue Novel Gels for Food Product Development)
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<p>Frequency sweep curves of agar gel obtained with different mixing velocity at temperatures of 4 (<b>a</b>) and 50 °C (<b>b</b>).</p>
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<p>Frequency sweep curves of agar gel with different concentration of lecithin at temperatures of 4 (<b>a</b>) and 50 °C (<b>b</b>).</p>
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<p>Tan (δ) as a function of temperature for agar during cooling of sample from 80 to 10 °C.</p>
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<p>The variation of the delta backscattering of agar gel (<b>a</b>) and gel with oil and 1% of lecithin (<b>b</b>).</p>
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<p>Structure of agar gel with oil prepared with different mixing rate: (<b>a</b>) 10,000, (<b>b</b>) 11,000, (<b>c</b>) 13,000 rpm.</p>
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20 pages, 3710 KiB  
Article
Ginger Extract-Loaded Sesame Oil-Based Niosomal Emulgel: Quality by Design to Ameliorate Anti-Inflammatory Activity
by Marwa H. Abdallah, Hanaa A. Elghamry, Nasrin E. Khalifa, Weam M. A. Khojali, El-Sayed Khafagy, Amr S. Abu Lila, Hemat El-Sayed El-Horany and Shaimaa El-Housiny
Gels 2022, 8(11), 737; https://doi.org/10.3390/gels8110737 - 14 Nov 2022
Cited by 15 | Viewed by 3471
Abstract
Ginger, a natural plant belonging to the Zingeberaceae family, has been reported to have reasonable anti-inflammatory effects. The current study aimed to examine ginger extract transdermal delivery by generating niosomal vesicles as a promising nano-carrier incorporated into emulgel prepared with sesame oil. Particle [...] Read more.
Ginger, a natural plant belonging to the Zingeberaceae family, has been reported to have reasonable anti-inflammatory effects. The current study aimed to examine ginger extract transdermal delivery by generating niosomal vesicles as a promising nano-carrier incorporated into emulgel prepared with sesame oil. Particle size, viscosity, in vitro release, and ex vivo drug penetration experiments were performed on the produced formulations (ginger extract loaded gel, ginger extract loaded emulgel, ginger extract niosomal gel, and ginger extract niosomal emulgel). Carrageenan-induced edema in rat hind paw was employed to estimate the in vivo anti-inflammatory activity. The generated ginger extract formulations showed good viscosity and particle size. The in vitro release of ginger extract from niosomal formulation surpassed other formulations. In addition, the niosomal emulgel formulation showed improved transdermal flux and increased drug permeability through rabbit skin compared to other preparations. Most importantly, carrageenan-induced rat hind paw edema test confirmed the potential anti-inflammatory efficacy of ginger extract niosomal emulgel, compared to other formulations, as manifested by a significant decrease in paw edema with a superior edema inhibition potency. Overall, our findings suggest that incorporating a niosomal formulation within sesame oil-based emulgel might represent a plausible strategy for effective transdermal delivery of anti-inflammatory drugs like ginger extract. Full article
(This article belongs to the Special Issue Liposomal and Ethosomal Gels: From Design to Application)
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<p>Vesicular size and size distribution curve of ginger extract-loaded niosomes.</p>
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<p>Outline of stability study for ginger extract-loaded niosomal formulation for 1 and 3 months at 4 °C and 25 °C in terms of (<b>a</b>) Particle size (nm); (<b>b</b>) PDI; (<b>c</b>) EE% in comparison to freshly prepared niosomes.</p>
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<p>Solubility of ginger extract in different surfactants and co-surfactants.</p>
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<p>Study of pseudoternary phase diagrams using sesame oil, Tween 80, and PEG 400 at different S<sub>mix</sub> ratios of (<b>a</b>) 1:1, (<b>b</b>) 1:2, (<b>c</b>) 1:3, (<b>d</b>) 2:1, (<b>e</b>) 3:1.</p>
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<p>3D response surface plots (<b>a</b>) and corresponding contour plots (<b>b</b>) showing the effects of the independent variables on viscosity (Y<sub>1</sub>). Two independent variables are considered at a time, while the third one remains constant.</p>
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<p>3D response surface plots (<b>a</b>) and corresponding contour plots (<b>b</b>) showing the effects of the independent variables on the percent of in vitro drug release (Y<sub>2</sub>). Two independent variables are considered at a time, while the third one remains constant.</p>
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<p>3D response surface plots (<b>a</b>) and corresponding contour plots (<b>b</b>) showing the effects of the independent variables on the percent of drug content (Y<sub>3</sub>). Two independent variables are considered at a time, while the third one remains constant.</p>
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<p>In vitro release study of ginger extract from different formulations compared to ginger extract suspension in phosphate buffer pH 7.4 at 37 °C. Results are expressed as the mean ± SD of three experiments. * <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract suspension; # <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract gel; ■ <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract emulgel and <span>$</span> <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract niosomal gel.</p>
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<p>Permeation study of ginger extract from different formulations through excised rabbit skin compared to ginger extract suspension (control). Results are expressed as mean ± SD (<span class="html-italic">n</span> = 3). * <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract suspension; # <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract gel; ■ <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract emulgel and <span>$</span> <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract niosomal gel.</p>
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<p>Effects of ginger extract prepared in various formulations on mean hind paw edema (<b>a</b>) and percentage of edema inhibition of carrageenan-induced paw edema rats (<b>b</b>). Results are expressed as mean with the bar showing SD (<span class="html-italic">n</span> = 5). * <span class="html-italic">p</span> &lt; 0.05 compared to plain niosomal gel; # <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract orally and ■ <span class="html-italic">p</span> &lt; 0.05 compared to ginger extract niosomal gel.</p>
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11 pages, 1139 KiB  
Article
Herbal Fennel Essential Oil Nanogel: Formulation, Characterization and Antibacterial Activity against Staphylococcus aureus
by Aftab Alam, Ahmed I. Foudah, Mohammad Ayman Salkini, Mohammad Raish and Jyotiram Sawale
Gels 2022, 8(11), 736; https://doi.org/10.3390/gels8110736 - 12 Nov 2022
Cited by 12 | Viewed by 3081
Abstract
Antimicrobial resistance (AMR) is one of the greatest threats to humanity in the world. Antibiotic-resistant bacteria spread easily in communities and hospitals. Staphylococcus aureus (S. aureus) is a serious human infectious agent with threatening broad-spectrum resistance to many commonly used antibiotics. [...] Read more.
Antimicrobial resistance (AMR) is one of the greatest threats to humanity in the world. Antibiotic-resistant bacteria spread easily in communities and hospitals. Staphylococcus aureus (S. aureus) is a serious human infectious agent with threatening broad-spectrum resistance to many commonly used antibiotics. To prevent the spread of pathogenic microorganisms, alternative strategies based on nature have been developed. Essential oils (EOs) are derived from numerous plant parts and have been described as antibacterial agents against S. aureus. Fennel essential oils were selected as antibacterial agents encapsulated in nanoparticles of polylactic acid and glycolic acid (PLGA). The optimum size of the formulation after loading with the active ingredient was 123.19 ± 6.1595 nm with a zeta potential of 0.051 ± 0.002 (23 ± 1.15 mV). The results of the encapsulation efficiency analysis showed high encapsulation of EOs, i.e., 66.4 ± 3.127. To obtain promising carrier materials for the delivery of fennel EOs, they were incorporated in the form of nanogels. The newly developed fennel oils in PLGANPs nanogels have good drug release and MIC against S. aureus. These results indicate the potential of this novel delivery system for antimicrobial therapy. Full article
(This article belongs to the Special Issue Recent Advances in Antimicrobial Hydrogels)
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<p>Physicochemical analysis: (<b>a</b>) FE-SEM image of gel prepared from FEO–PLGANPs; (<b>b</b>) TEM image of prepared gel; (<b>c</b>) measurements of particle size, polydispersity index and zeta potential of gel prepared from FEO–PLGANPs before and after drug loading.</p>
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<p>Comparative in vitro drug release study of FEO, FEO–PLGANPs and FEO–PLGANPs in a buffer solution of pH 6.8.</p>
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<p>(<b>a</b>) Comparative in vitro cell viability assay of FEO–PLGANPs gel and FEO–PLGANPs; (<b>b</b>) Time-kill assay of the control, FEO–PLGANPs gel and FEO–PLGANPs.</p>
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15 pages, 2872 KiB  
Article
New Zwitterionic Polymer as a Highly Effective Salt- and Calcium-Resistant Fluid Loss Reducer in Water-Based Drilling Fluids
by Luman Liu, Jinsheng Sun, Ren Wang, Fan Liu, Shifeng Gao, Jie Yang, Han Ren, Yuanzhi Qu, Rongchao Cheng, Yuan Geng and Zhenbo Feng
Gels 2022, 8(11), 735; https://doi.org/10.3390/gels8110735 - 11 Nov 2022
Cited by 17 | Viewed by 2888
Abstract
To control the filtration loss of drilling fluids in salt–gypsum formations, a novel type of zwitterionic polymer gel (DNDAP) was synthesized by free radical polymerization, which was used as a salt- and calcium-resistant fluid loss reducer for water-based drilling fluids (WBDF). DNDAP was [...] Read more.
To control the filtration loss of drilling fluids in salt–gypsum formations, a novel type of zwitterionic polymer gel (DNDAP) was synthesized by free radical polymerization, which was used as a salt- and calcium-resistant fluid loss reducer for water-based drilling fluids (WBDF). DNDAP was prepared with N, N-dimethylacrylamide (DMAA), N-vinylpyrrolidone (NVP), Diallyl dimethyl ammonium chloride (DMDAAC), 2-acrylamide-2-methylpropaneonic acid (AMPS), and isopentenol polyether (TPEG) as raw materials. Fourier transform infrared spectroscopy (FT-IR) and proton nuclear magnetic resonance (1H-NMR) were used to characterize the composition and structure of the DNDAP copolymer. The thermal stability of DNDAP was evaluated by the use of thermogravimetric analysis (TGA). WBDF with DNDAP was analyzed for zeta potential and particle size and the corresponding filter cake underwent energy dispersive spectrum (EDS) analysis and scanning electron microscope (SEM) analysis. The results showed that the thermal decomposition of DNDAP mainly occurred above 303 °C. DNDAP exhibits excellent rheological and filtration properties in water-based drilling fluids, even under high-temperature aging (up to 200 °C) and high salinity (20 wt% NaCl or 5 wt% CaCl2) environments. The strong adsorption effect of DNDAP makes the particle size of bentonite reasonably distributed to form a dense mud cake that reduces filtration losses. Full article
(This article belongs to the Special Issue Gels for Oil Drilling and Enhanced Recovery)
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<p>FTIR spectrum of DNDAP.</p>
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<p><sup>1</sup>H NMR spectrum of DNDAP.</p>
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<p>TGA-DSC analysis of DNDAP.</p>
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<p>Filtration performance of DNDAP in the WBDF. (<b>a</b>) WBDF containing various concentrations of DNDAP and its filtration loss before and after aging at 200 °C for 16 h. (<b>b</b>) Filtration performance of the WBDF supplemented with 2 wt% DNDAP at various temperatures. (<b>c</b>) The filter loss of DNDAP in Na-WBDF at different concentrations after aging at 200 °C for 16 h. (<b>d</b>) The filter loss of DNDAP in Ca-WBDF at different concentrations after aging at 200 °C for 16 h.</p>
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<p>Rheological parameters of different concentrations of DNDAP before (BHR) and after (AHR) aging in the WBDF (<b>a</b>–<b>c</b>).</p>
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<p>Rheological parameters of DNDAP before and after aging in WBDF with different salt and calcium concentrations (<b>a</b>–<b>f</b>).</p>
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<p>(<b>a</b>−<b>f</b>) SEM of filter cakes; (<b>a1</b>−<b>f1</b>) digital images of filter cakes; (<b>a</b>,<b>a1</b>) WBDF; (<b>b</b>,<b>b1</b>) 20Na -WBDF; (<b>c</b>,<b>c1</b>) 5Ca-WBDF; (<b>d</b>,<b>d1</b>) DNDAP/WBDF; (<b>e</b>,<b>e1</b>) DNDAP/20Na -WBDF; (<b>f</b>,<b>f1</b>) DNDAP/5Ca-WBDF.</p>
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<p>EDS element analysis of filter cakes.</p>
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<p>Size distribution of the WBDF under different conditions after aging at 200 °C for 16 h.</p>
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<p>Zeta potential value of WBDF.</p>
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<p>The synthesis procedure of the DNDAP copolymer.</p>
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16 pages, 3230 KiB  
Article
Encapsulation of Grape (Vitis vinifera L.) Pomace Polyphenols in Soybean Extract-Based Hydrogel Beads as Carriers of Polyphenols and pH-Monitoring Devices
by Gianluca Viscusi, Elena Lamberti, Carmela Gerardi, Giovanna Giovinazzo and Giuliana Gorrasi
Gels 2022, 8(11), 734; https://doi.org/10.3390/gels8110734 - 11 Nov 2022
Cited by 10 | Viewed by 2455
Abstract
In this work, novel bio-based hydrogel beads were fabricated by using soybean extract as raw waste material loaded with Lambrusco extract, an Italian grape cultivar. The phenolic profile and the total amount of anthocyanins from the Lambrusco extract were evaluated before encapsulating it [...] Read more.
In this work, novel bio-based hydrogel beads were fabricated by using soybean extract as raw waste material loaded with Lambrusco extract, an Italian grape cultivar. The phenolic profile and the total amount of anthocyanins from the Lambrusco extract were evaluated before encapsulating it in soybean extract-based hydrogels produced through an ionotropic gelation technique. The physical properties of the produced hydrogel beads were then studied in terms of their morphological and spectroscopic properties. Swelling degree was evaluated in media with different pH levels. The release kinetics of Lambrusco extract were then studied over time as a function of pH of the release medium, corroborating that the acidity/basicity could affect the release rate of encapsulated molecules, as well as their counter-diffusion. The pH-sensitive properties of wine extract were studied through UV-Vis spectroscopy while the colorimetric responses of loaded hydrogel beads were investigated in acidic and basic solutions. Finally, in the framework of circular economy and sustainability, the obtained data open routes to the design and fabrication of active materials as pH-indicator devices from food industry by-products. Full article
(This article belongs to the Special Issue Hydrogels as Controlled Drug Delivery Systems)
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<p>SEM micrographs of SBs (<b>a</b>) and LSBs (<b>b</b>). Appearance of SB and LSB (<b>c</b>). Surface plot profiles for SBs (<b>d</b>) and LSBs (<b>e</b>). Diameter distributions of SBs (<b>f</b>) and LSBs (<b>g</b>).</p>
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<p>EDX maps of Lambrusco polyphenol-loaded beads (LSBs).</p>
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<p>FTIR spectra of Lambrusco extract and soybean extract-based beads.</p>
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<p>Swelling data for SBs (<b>a</b>) and LSBs (<b>b</b>) as function of pH level.</p>
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<p>Release kinetics of Lambrusco polyphenol-loaded soybean-based beads.</p>
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<p>Release data fitted through Korsmeyer–Peppas (<b>a</b>), first-order (<b>b</b>), Higuchi (<b>c</b>) and modified Weibull (<b>d</b>) models.</p>
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<p>Color variations of Lambrusco GP-derived anthocyanins in different buffer solutions of different pH (2–12).</p>
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<p>Colorimetric responses of LSBs at pH = 2 and pH = 12. Below: pictures of LSBs in different buffer pH solutions after 24 h.</p>
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<p>Reversibility of Lambrusco anthocyanin-encapsulated beads.</p>
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<p>Schematization of ionotropic gelation and production of soybean extract-based beads.</p>
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24 pages, 8457 KiB  
Article
A Pharmaco-Technical Investigation of Thymoquinone and Peat-Sourced Fulvic Acid Nanoemulgel: A Combination Therapy
by Rahmuddin Khan, Mohd Aamir Mirza, Mohd Aqil, Nazia Hassan, Foziyah Zakir, Mohammad Javed Ansari and Zeenat Iqbal
Gels 2022, 8(11), 733; https://doi.org/10.3390/gels8110733 - 10 Nov 2022
Cited by 14 | Viewed by 2828
Abstract
Thymoquinone has a multitude of pharmacological effects and has been researched for a wide variety of indications, but with limited clinical success. It is associated with pharmaco-technical caveats such as hydrophobicity, high degradation, and a low oral bioavailability. A prudent approach warrants its [...] Read more.
Thymoquinone has a multitude of pharmacological effects and has been researched for a wide variety of indications, but with limited clinical success. It is associated with pharmaco-technical caveats such as hydrophobicity, high degradation, and a low oral bioavailability. A prudent approach warrants its usage through an alternative dermal route in combination with functional excipients to harness its potential for treating dermal afflictions, such as psoriasis. Henceforth, the present study explores a nanoformulation approach for designing a fulvic acid (peat-sourced)-based thymoquinone nanoemulsion gel (FTQ-NEG) for an enhanced solubility and improved absorption. The excipients, surfactant/co-surfactant, and oil selected for the o/w nanoemulsion (FTQ-NE) are Tween 80/Transcutol-P and kalonji oil. The formulation methodology includes high-energy ultrasonication complemented with a three-dimensional/factorial Box–Behnken design for guided optimization. The surface morphology assessment through scanning/transmission electron microscopy and fluorescence microscopy revealed a 100 nm spherical, globule-like structure of the prepared nanoemulsion. Furthermore, the optimized FTQ-NE had a zeta potential of −2.83 ± 0.14 Mv, refractive index of 1.415 ± 0.036, viscosity of 138.5 ± 3.08 mp, and pH of 5.8 ± 0.16, respectively. The optimized FTQ-NE was then formulated as a gel using Carbopol 971® (1%). The in vitro release analysis of the optimized FTQ-NEG showed a diffusion-dominant drug release (Higuchi model) for 48 h. The drug permeation flux observed for FTQ-NEG (3.64 μg/cm2/h) was much higher compared to that of the pure drug (1.77 mg/cm2/h). The results were further confirmed by confocal microscopy studies, which proved the improved penetration of thymoquinone through mice skin. Long-term stability studies of the purported formulation were also conducted and yielded satisfactory results. Full article
(This article belongs to the Special Issue Advance in Supramolecular Gels)
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<p>TQ solubility in various surfactants, co-surfactants, and oils.</p>
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<p>Pseudo-ternary phase diagrams for various Smix ratios.</p>
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<p>3D response surface depicting the interaction effect of the independent variables like oil, smix, sonication time on (<b>a</b>–<b>c</b>) particle size, (<b>d</b>–<b>f</b>) PDI, and(<b>g</b>–<b>i</b>) %transmittance.</p>
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<p>(<b>A</b>) Dilution test, (<b>B</b>) filter paper test, and (<b>C</b>) cobalt chloride test.</p>
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<p>Particle size, polydispersity index (<b>A</b>) (PDI), and zeta potential (<b>B</b>) of FTQ-NE.</p>
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<p>Overlay of differential scanning calorimetry (DSC) (<b>A</b>) (thymoquinone), (<b>B</b>) (fulvic acid), (<b>C</b>) (mannitol), and (<b>D</b>) (FTQ-NE).</p>
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<p>Overlay spectra showing the FTIR of (<b>A</b>) TQ, (<b>B</b>) FA, (<b>C</b>) mannitol, and (<b>D</b>) FTQ-NE.</p>
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<p>Overlay of X-ray diffractograms.</p>
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<p>(<b>A</b>) SEM, (<b>B</b>) TEM, and (<b>C</b>) fluorescent microscopy of the optimized FTQ-NE.</p>
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<p>Texture analysis of the FTQ-NEG formulation (<b>A</b>) and placebo gel (<b>B</b>).</p>
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<p>(<b>A</b>) In vitro drug release of TQ, FTQ-NE, and FTQ-NEG. (<b>B</b>) The ex vivo skin permeation release of the free drug TQ, FTQ-NEG, and FTQ-NE.</p>
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<p>Confocal microscopic studies of mouse skin treated with (<b>A</b>) Rhodamine B hydroalcoholic solution, (<b>B</b>) drug solution with rhodamine dye, and (<b>C</b>) FTQ-NEG with rhodamine.</p>
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20 pages, 5551 KiB  
Article
X-ray Tomography Coupled with Finite Elements, A Fast Method to Design Aerogel Composites and Prove Their Superinsulation Experimentally
by Genevieve Foray, Jaona Harifidy Randrianalisoa, Jerome Adrien and Eric Maire
Gels 2022, 8(11), 732; https://doi.org/10.3390/gels8110732 - 10 Nov 2022
Cited by 1 | Viewed by 1938
Abstract
Composite aerogels can include fibers, opacifiers and binders but are rarely designed and optimized to achieve the best thermal/mechanical efficiency. This paper proposes a three-dimensional X-ray tomography-based method for designing composites. Two types of models are considered: classical and inexpensive homogenization models and [...] Read more.
Composite aerogels can include fibers, opacifiers and binders but are rarely designed and optimized to achieve the best thermal/mechanical efficiency. This paper proposes a three-dimensional X-ray tomography-based method for designing composites. Two types of models are considered: classical and inexpensive homogenization models and more refined finite element models. XrFE is based on the material’s real three-dimensional microstructure and/or its twin numerical microstructure, and calculates the effective conductivity of the material. First, the three-dimensional sample is meshed and labeled. Then, a finite element method is used to calculate the heat flow in the samples. The entire three-dimensional microstructure of a real or fictitious sample is thus associated with a heat flow and an effective conductivity. Parametric studies were performed to understand the relationship between microstructure and thermal efficiency. They highlighted how quickly a low volume fraction addition can improve or ruin thermal conductivity. A reduced set of three formulations was developed and fully characterized. The mechanical behavior was higher than 50 KPa, with thermal efficiencies ranging from 14 to 15 mW·m·K1. Full article
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<p>Tomography cross-section of aerogel composite. (<b>a</b>) Monomodal pile-up medium size grain IP = 36%; (<b>b</b>) bimodal aerogel pile up IP = 42%; (<b>c</b>) organic binder and bimodal pile-up IP = 19%; (<b>d</b>) defect simulation, binder band perpendicular to the heat flux.</p>
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<p>Pore size distribution determined by X-ray tomography, compaction, combining grain size, binding, and binding with SiC addition contribute to decreasing pore size.</p>
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<p>(<b>a</b>) Full cross-section of a segmented prismatic sample X binder, (pores and SAP are black), showing that on the bottom the volume fraction of binder is higher and the thickness of the binder is greater,(green squares locate zoom shown in (<b>b</b>,<b>c</b>)); (<b>b</b>) 200 µm × 200 µm bottom zoom (green square in (<b>a</b>)) showing SAP sealed by a thick continuous binder skin near the sample edge; (<b>c</b>) 200 µm × 200 µm top zoom (green interrupted line square in (<b>a</b>)) showing a thin and disrupted binder skin of a few microns thick, far from the sample edge. (<b>b</b>,<b>c</b>) the binder is white, SAP is light gray, and the IP is dark.</p>
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<p>Homogenization simulated thermal conductivity values compared to experimental measurements (issued from [<a href="#B45-gels-08-00732" class="html-bibr">45</a>]) as a function of inter-aerogel particle porosity (IP determined with X-ray tomograms). An insert zooms on data within the superinsulation range. Input values: <math display="inline"><semantics> <mrow> <mo> </mo> <msubsup> <mi>λ</mi> <mrow> <mi>S</mi> <mi>A</mi> <mi>P</mi> </mrow> <mo>*</mo> </msubsup> <mo>=</mo> </mrow> </semantics></math> <math display="inline"><semantics> <mrow> <mn>14</mn> <mo> </mo> <mi>mW</mi> <mo>·</mo> <mi mathvariant="normal">m</mi> <mo>·</mo> <msup> <mi mathvariant="normal">K</mi> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> <mo>,</mo> <mo> </mo> <msubsup> <mi>λ</mi> <mrow> <mi>a</mi> <mi>i</mi> <mi>r</mi> </mrow> <mo>*</mo> </msubsup> <mo>=</mo> </mrow> </semantics></math> <math display="inline"><semantics> <mrow> <mn>25</mn> <mo> </mo> <mi>mW</mi> <mo>·</mo> <mi mathvariant="normal">m</mi> <mo>·</mo> <msup> <mi mathvariant="normal">K</mi> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> </mrow> </semantics></math>.</p>
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<p>3D reconstructed X-ray tomogram illustrating the post-treatments performed: (<b>a</b>) segmentation and medium filter applied, with view of SAP only; (<b>b</b>) watershed applied, contacts between grains only viewed. The dark 2D square in the image illustrates a possible cross-section. (reprinted with permission from [<a href="#B46-gels-08-00732" class="html-bibr">46</a>]).</p>
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<p>Parametric study on an aerogel composite with the XrFE model. (<b>a</b>) <math display="inline"><semantics> <mrow> <mi>V</mi> <msub> <mi>f</mi> <mrow/> </msub> </mrow> </semantics></math> of aerogel, (increasing compacity causes a sharp decrease in conductivity); (<b>b</b>) the thermal conductivity of the contacts,(including contacts in mesh, is neutral); (<b>c</b>) oganic binder, (filling pores with binder causes a huge increase in conductivity); (<b>d</b>) aerogel price and efficiency, (when using lower-priced, lower thermal intrinsic conductivity aerogel, XrFE and experimental conductivity are equal).</p>
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<p>Tomography cross-section of aerogel composite. (<b>a</b>) SBA T composite <math display="inline"><semantics> <mrow> <mi>V</mi> <msub> <mi>f</mi> <mrow> <mi>b</mi> <mi>i</mi> <mi>n</mi> <mi>d</mi> <mi>e</mi> <mi>r</mi> </mrow> </msub> </mrow> </semantics></math> 2% IP = 17%; (<b>b</b>) SBA X <math display="inline"><semantics> <mrow> <mi>V</mi> <msub> <mi>f</mi> <mrow> <mi>b</mi> <mi>i</mi> <mi>n</mi> <mi>d</mi> <mi>e</mi> <mi>r</mi> </mrow> </msub> </mrow> </semantics></math> 2.0% IP = 12%; (<b>c</b>) SBA X SiC <math display="inline"><semantics> <mrow> <mi>V</mi> <msub> <mi>f</mi> <mrow> <mi>b</mi> <mi>i</mi> <mi>n</mi> <mi>d</mi> <mi>e</mi> <mi>r</mi> </mrow> </msub> </mrow> </semantics></math> 2% IP = 6%, please not the micron size isolated SiC particles paving space in white; (<b>d</b>) hydraulic binder, no quantitative analysis; (<b>e</b>) experimental values (flexural stress versus density and thermal conductivity measured given on graph in (<math display="inline"><semantics> <mrow> <mi>mW</mi> <mo>·</mo> <mi mathvariant="normal">m</mi> <mo>·</mo> <msup> <mi mathvariant="normal">K</mi> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> </mrow> </semantics></math>) issued from ref. [<a href="#B45-gels-08-00732" class="html-bibr">45</a>,<a href="#B48-gels-08-00732" class="html-bibr">48</a>]).</p>
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<p>200 × 200 cross-section in the X-ray tomogram, microstructure details. (<b>a</b>) organic binder wrapping aerogel particles without binder intrusion inside aerogel particle cracks and fracture lines; (<b>b</b>) mineral binder filling space between aerogel particles, and also filling aerogel particle cracks and fracture lines; (<b>c</b>) organic binder T, ESRF, low thickness binder skin, and adhesive contact between particles; (<b>d</b>) organic binder X,— few medium thickness binder skins, including aligned air bubbles. (<b>e</b>) organic binder X,— numerous large thickness binder skins and regular thickness skins showing disrupted adhesion to particles and large air gaps in between. White arrows show crack openings, and red double arrows measure binder thickness perpendicular to aerogel particles.</p>
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<p>Cross-sections within the 3D reconstructed X-ray tomogram to illustrate the post-treatments performed: (<b>a</b>) raw monomodal SAP pileup; (<b>b</b>) segmentation and medium filter applied, two phases only viewed: air in pores and SAP; (<b>c</b>) watershed applied, contacts between SAP only viewed; (<b>d</b>) all phases (pores, SAP and contact between SAP (color code black, gray, white)).</p>
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<p>Composite aerogel with binder, and 3D-reconstructed ESRF X-ray tomogram to illustrate the post-treatments performed; (<b>a</b>) raw 3D volumes showing the three phases, (the binder, SAP, and IP); (<b>b</b>) cross-section resulting from (<b>a</b>) showing in white the binder has a discrete element in IP (outside SAP); (<b>c</b>) zoom in (<b>b</b>) (shown as a blue perimeter) showing that the organic binder either wraps SAP or connects SAP with fibrils; (<b>d</b>) after segmentation to separate the binder phase, (3D crop to show the connectivity of the binder phase).</p>
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<p>Meshed volumes based on 3D-reconstructed X-ray tomogram: (<b>a</b>) monomodal SAP composite recombined or not; (<b>b</b>) nodal temperature view within a bound bimodal composite.</p>
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19 pages, 5806 KiB  
Article
The Effect of Hydrogels with Different Chemical Compositions on the Behavior of Alkali-Activated Slag Pastes
by Joshua Prabahar, Babak Vafaei and Ali Ghahremaninezhad
Gels 2022, 8(11), 731; https://doi.org/10.3390/gels8110731 - 10 Nov 2022
Cited by 8 | Viewed by 1940
Abstract
The effect of in-house synthesized hydrogels with different chemical compositions on the properties of alkali-activated slag pastes was examined. It was found that the teabag test and modified teabag test as a direct method and the flow test as an indirect method showed [...] Read more.
The effect of in-house synthesized hydrogels with different chemical compositions on the properties of alkali-activated slag pastes was examined. It was found that the teabag test and modified teabag test as a direct method and the flow test as an indirect method showed a similar trend in hydrogel absorption; however, the absorption values differ noticeably between the direct and indirect methods. The alkali-activated slag pastes with hydrogels demonstrated a significant reduction in autogenous shrinkage compared to the pastes without hydrogels. The creation of macrovoids by the hydrogels and change in pore structure resulted in a decrease in compressive strength and electrical resistivity of the pastes with hydrogels. The absorption and desorption of hydrogels in the pastes were tracked using X-ray microcomputed tomography (micro-CT), and it was shown that the onset of hydrogel desorption approximately coincided with the final setting time of the pastes. Full article
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<p>Absorption of different hydrogels in (<b>a</b>) activator solution and (<b>b</b>) slag and activator solution mixture.</p>
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<p>Heat flow of the pastes with and without hydrogels.</p>
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<p>Autogenous shrinkage of the pastes with and without hydrogels.</p>
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<p>Compressive strength of the pastes with and without hydrogels after 28 days of curing.</p>
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<p>Electrical resistivity of the pastes with and without hydrogels at different ages of curing.</p>
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<p>TGA and DTG curves of the paste without hydrogel and the pastes with select hydrogels after 28 days of curing.</p>
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<p>FTIR spectra of the paste without hydrogel and the pastes with select hydrogels after 28 days of curing.</p>
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<p>Two-dimensional images of a cross section of AAS-H-a at (<b>a</b>) 4 h, (<b>b</b>) 8 h, (<b>c</b>) 24 h, and (<b>d</b>) 72 h obtained from micro-CT.</p>
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<p>Total volume fraction of hydrogels in AAS-H-a and AAS-H-b at different times of curing.</p>
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<p>Desorption of hydrogels in AAS-H-a and AAS-H-b at different times of curing.</p>
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<p>Size of hydrogels in AAS-H-a and AAS-H-b at different times of curing.</p>
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<p>SEM image showing the particle size and morphology of H-d.</p>
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15 pages, 1488 KiB  
Review
Hydrogels for Salivary Gland Tissue Engineering
by Sangeeth Pillai, Jose G. Munguia-Lopez and Simon D. Tran
Gels 2022, 8(11), 730; https://doi.org/10.3390/gels8110730 - 10 Nov 2022
Cited by 5 | Viewed by 4741
Abstract
Mimicking the complex architecture of salivary glands (SGs) outside their native niche is challenging due their multicellular and highly branched organization. However, significant progress has been made to recapitulate the gland structure and function using several in vitro and ex vivo models. Hydrogels [...] Read more.
Mimicking the complex architecture of salivary glands (SGs) outside their native niche is challenging due their multicellular and highly branched organization. However, significant progress has been made to recapitulate the gland structure and function using several in vitro and ex vivo models. Hydrogels are polymers with the potential to retain a large volume of water inside their three-dimensional structure, thus simulating extracellular matrix properties that are essential for the cell and tissue integrity. Hydrogel-based culture of SG cells has seen a tremendous success in terms of developing platforms for cell expansion, building an artificial gland, and for use in transplantation to rescue loss of SG function. Both natural and synthetic hydrogels have been used widely in SG tissue engineering applications owing to their properties that support the proliferation, reorganization, and polarization of SG epithelial cells. While recent improvements in hydrogel properties are essential to establish more sophisticated models, the emphasis should still be made towards supporting factors such as mechanotransduction and associated signaling cues. In this concise review, we discuss considerations of an ideal hydrogel-based biomaterial for SG engineering and their associated signaling pathways. We also discuss the current advances made in natural and synthetic hydrogels for SG tissue engineering applications. Full article
(This article belongs to the Special Issue Engineering Hydrogel for Biomedical Applications)
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<p>Schematic diagram of a salivary gland structure showing the secretory end pieces made of mucous and serous acini, supported by overlying myoepithelial cells. The secretory units extend to form the intercalated, striated, and excretory ducts through which saliva passes into the oral cavity.</p>
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<p>Schematic illustration of different types of SG cells within a hydrogel matrix describing the key hydrogel properties to be considered to adequately regulate cell functions for SG tissue engineering applications.</p>
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<p>Schematic map of the key signaling pathways to be considered while designing hydrogel properties (binding sites, stiffness, pore size, architecture, etc.) for SG tissue engineering and their association with the cell fate and function [<a href="#B70-gels-08-00730" class="html-bibr">70</a>,<a href="#B71-gels-08-00730" class="html-bibr">71</a>,<a href="#B72-gels-08-00730" class="html-bibr">72</a>,<a href="#B73-gels-08-00730" class="html-bibr">73</a>,<a href="#B74-gels-08-00730" class="html-bibr">74</a>].</p>
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16 pages, 4418 KiB  
Article
From Macro to Micro: Comparison of Imaging Techniques to Detect Vascular Network Formation in Left Ventricle Decellularized Extracellular Matrix Hydrogels
by Meng Zhang, Vasilena E. Getova, Francisco Drusso Martinez-Garcia, Theo Borghuis, Janette K. Burgess and Martin C. Harmsen
Gels 2022, 8(11), 729; https://doi.org/10.3390/gels8110729 - 10 Nov 2022
Cited by 6 | Viewed by 2343
Abstract
Background: Angiogenesis is a crucial process in physiological maintenance and tissue regeneration. To understand the contribution of angiogenesis, it is essential to replicate this process in an environment that reproduces the biochemical and physical properties which are largely governed by the extracellular matrix [...] Read more.
Background: Angiogenesis is a crucial process in physiological maintenance and tissue regeneration. To understand the contribution of angiogenesis, it is essential to replicate this process in an environment that reproduces the biochemical and physical properties which are largely governed by the extracellular matrix (ECM). We investigated vascularization in cardiac left ventricular ECM hydrogels to mimic post-myocardial repair. We set out to assess and compare different destructive and non-destructive methods, optical as well as non-optical, to visualize angiogenesis and associated matrix remodeling in myocardial ECM hydrogels. Methods: A total of 100,000, 300,000, and 600,000 Human Pulmonary Microvascular Endothelial Cells (HPMEC) were seeded in left ventricular cardiac ECM hydrogel in 48-well plates. After 1, 7, and 14 days of culture, the HPMEC were imaged by inverted fluorescence microscopy and 3D confocal laser scanning microscopy (Zeiss Cell Discoverer 7). In addition, cell-seeded ECM hydrogels were scanned by optical coherence tomography (OCT). Fixed and paraffin-embedded gels were thin-sectioned and assessed for ECM components via H&E, picrosirius red histochemical staining, and immunostaining for collagen type I. ImageJ-based densitometry was used to quantify vascular-like networks and GraphPad was used for statistical analyses. Results: Qualitative analyses were realized through fluoromicrographs obtained by the confocal laser scanning microscope which allowed us to visualize the extensive vascular-like networks that readily appeared at all seeding densities. Quantification of networks was only possible using fluoromicrographs from inverted microscopy. These showed that, after three days, the number of master junctions was seeding density-dependent. The resolution of optical coherence tomography was too low to distinguish between signals caused by the ECM and cells or networks, yet it did show that gels, irrespective of cells, were heterogeneous. Interestingly, (immuno)histochemistry could clearly distinguish between the cast cardiac-derived matrix and newly deposited ECM in the hydrogels. The H&E staining corroborated the presence of vascular-like network structures, albeit that sectioning inevitably led to the loss of 3D structure. Conclusions: Except for OCT, all methods had complementary merit and generated qualitative and quantitative data that allowed us to understand vascular network formation in organ-derived ECM hydrogels. Full article
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<p>Vascular network formation (VNF) by HPMEC detected by fluorescent microscopy imaging; 100 k, 300 k, and 600 k HPMEC in LV ECM hydrogel were examined after 1, 7, and 14 days. As control, HPMEC were seeded directly on culture plastic. Scale bars represent 400 µm.</p>
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<p>Quantitative analyses of VNF by HPMEC in LV ECM hydrogels. (<b>A</b>): comparison of the number of nodes based on ImageJ quantification among 100 k, 300 k, and 600 k HPMEC at three time points (1 d, 7 d, and 14 d). (<b>B</b>): comparison of the number of master junctions based on ImageJ quantification among 100 k, 300 k, and 600 k HPMEC at three time points (1 d, 7 d, and 14 d). (<b>C</b>): comparison of the number of branches based on ImageJ quantification among 100 k, 300 k, and 600 k HPMEC at three time points (1 d, 7 d, and 14 d). (<b>D</b>): comparison of total branching length based on ImageJ quantification among 100 k, 300 k, and 600 k HPMEC at three time points (1 d, 7 d, and 14 d). * <span class="html-italic">p</span> &lt; 0.05, ** <span class="html-italic">p</span> &lt; 0.01, **** <span class="html-italic">p</span> &lt;&lt;0.0001.</p>
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<p>OCT analyses: HPMEC engaged in VNF in LV ECM hydrogels; 100 k, 300 k, and 600 k HPMEC seeded in LV ECM hydrogel examined after 1 day, 7 days, and 14 days. As control, hydrogels without HPMEC were used. Scale bars represent 1 mm (landscape view) and 0.2 mm (insets).</p>
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<p>Densitrometric analyses of OCT imaging. HPMEC seeded in LV ECM hydrogels were compared at d1 (<b>A</b>), d7 (<b>B</b>), and d14 (<b>C</b>). Measurements were obtained from three pullbacks over each gel (<span class="html-italic">n</span> = 5, one way ANOVA comparing gel, *** <span class="html-italic">p</span> &lt; 0.001).</p>
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<p>Histochemical analyses of VNF by HPMEC seeded in LV ECM hydrogels and stained by H&amp;E. (<b>A</b>): 100 k, 300 k, and 600 k HPMEC seeded in LV ECM hydrogel were examined at days 1, 7, and 14 of culturing (original magnification was 40×) after H&amp;E staining of thin sections. Bare hydrogels served as controls. Control hydrogels show the fiber-like meshwork of the LV ECM hydrogels. Cell-seeded hydrogels show clusters of cells (purple with dark-stained nuclei), often arranged as tubular structures. Insets show the entire section as scanned by the Hamamatsu image scanner. Scale bars represent 100 µm. (<b>B</b>): quantification of the number of tubes (visible as cell clusters with a lumen) at days 7 and 14 (<span class="html-italic">n</span> = 3, one way ANOVA comparing gel).</p>
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<p>Influence on collagen organization of the VNF of HPMEC seeded in LV ECM hydrogels as examined by picrosirius red staining. Picrosirius red-stained sections of 100 k, 300 k, and 600 k HPMEC in LV ECM hydrogel at days 1, 7, and 14. As a control, bare LV ECM hydrogels were used. Staining intensity was markedly increased in the vicinity of cell clusters and tube-like structures in a seeding density-dependent fashion, while more distal of cells staining was weaker. The original magnification used for scan slides (insets) in Hamamatsu imaging was 20×. Scale bars represent 100 µm.</p>
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<p>Quantitative analyses of picrosirius red staining imaging. Densitrometric data acquired using ImageJ for days 1 (<b>A</b>), 7 (<b>B</b>), and 14 (<b>C</b>) were compared with regard to seeding density (100 k, 300 k, 600 k, and control (no cells)). Three ROI are depicted: 1—close to cells, 2—at an intermediate distance from cells, and 3—cell-free area. Data represent <span class="html-italic">n</span> = 3 independent experiments assessed with two-way ANOVA multiple comparisons tests. * <span class="html-italic">p</span> &lt; 0.05, ** <span class="html-italic">p</span> &lt; 0.01.</p>
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<p>Immunohistochemical staining for the presence of collagen type I. LV ECM hydrogels were seeded with 600 k HPMEC and assessed at days 1, 7, and 14 for collagen type I. Bare hydrogels served as controls. Micrographs shown are areas with representative VNF taken from scans by Hamamatsu imaging at 20× magnification (insets). Collagen fibers are visible as a fibrous meshwork, while cells are white with a blue nucleus.</p>
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<p>Schematic representation of the methodology. HPMEC were mixed with pregel (<b>A</b>) and cast in 48-well plates at 37 °C (<b>B</b>). Visualization of cells was performed via inverted fluorescence microscopy (<b>C</b>), the use of a live cell confocal imaging system (<b>D</b>), and OCT (<b>E</b>). After culture, the gels were fixed with paraformaldehyde, embedded into the paraffin, and thin-sectioned (<b>F</b>). The sections were subjected to different (immuno)histochemical staining (<b>G</b>) and imaged by microscopy (<b>H</b>). [Image partially made with BioRender.] [<a href="#B23-gels-08-00729" class="html-bibr">23</a>].</p>
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12 pages, 4512 KiB  
Article
A Modified Sol–Gel Synthesis of Anatase {001}-TiO2/Au Hybrid Nanocomposites for Enhanced Photodegradation of Organic Contaminants
by Abubakar Katsina Usman, Diana-Luciana Cursaru, Gheorghe Brănoiu, Raluca Şomoghi, Ana-Maria Manta, Dănuţa Matei and Sonia Mihai
Gels 2022, 8(11), 728; https://doi.org/10.3390/gels8110728 - 10 Nov 2022
Cited by 8 | Viewed by 2292
Abstract
A sol–gel synthesis technique was employed for the preparation of anatase phase {001}-TiO2/Au hybrid nanocomposites (NCs). The scalable, schematic, and cost-efficient method was successfully modified using HF and NH4OH capping agents. The photocatalytic activity of the as-synthesized {001}-TiO2 [...] Read more.
A sol–gel synthesis technique was employed for the preparation of anatase phase {001}-TiO2/Au hybrid nanocomposites (NCs). The scalable, schematic, and cost-efficient method was successfully modified using HF and NH4OH capping agents. The photocatalytic activity of the as-synthesized {001}-TiO2/Au NCs were tested over 2-cycle degradation of methylene blue (MB) dye and pharmaceutical active compounds (PhACs) of ibuprofen and naproxen under direct sunlight illumination at 35 °C and 44,000 lx. Transmission electron microscopy (TEM), high resolution transmission electron microscopy (HR-TEM), fast Fourier transform (FFT), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDS), and ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS) were employed for the characterization of the as-prepared sample. The characterization results from the TEM, XPS, and XRD studies established both the distribution of Au colloids on the surface of TiO2 material, and the presence of the highly crystalline structure of anatase {001}-TiO2/Au NCs. Photodegradation results from the visible light irradiation of MB indicate an enhanced photocatalytic performance of Au/TiO2 NCs over TiO2. The results from the photocatalytic activity test performed under direct sunlight exposure exhibited promising photodegradation efficiencies. In the first cycle, the sol–gel synthesized material exhibited relatively better efficiencies (91%) with the MB dye and ibuprofen, while the highest degradation efficiency for the second cycle was 79% for the MB dye. Pseudo first-order photodegradation rates from the first cycle were determined to be comparatively slower than those from the second degradation cycle. Full article
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<p>(<b>a</b>) Ibuprofen; (<b>b</b>) Naproxen; (<b>c</b>) Methylene blue dye.</p>
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<p>X-ray diffraction (XRD) patterns of the hybrid Au/TiO<sub>2</sub> nanosheets.</p>
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<p>X-ray photoemission spectroscopy (XPS) peaks of (<b>a</b>) convoluted spectra of Ti 2p, O 1s, and Au 4f; (<b>b</b>) deconvoluted Ti 2p spectra; (<b>c</b>) deconvoluted Au 4f spectra; and (<b>d</b>) deconvoluted O1s spectra.</p>
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<p>(<b>a</b>) TEM image of TiO<sub>2</sub> NSs; (<b>b</b>,<b>c</b>) HR-TEM images obtained from a small portion of (<b>a</b>); insert HR-TEM corresponding FFT image.</p>
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<p>(<b>a</b>) TEM image of TiO<sub>2</sub> NSs; (<b>b</b>,<b>c</b>) HR-TEM images obtained from a small portion of (<b>a</b>); insert HR-TEM corresponding FFT image.</p>
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<p>Magnified lattice fringes for d-spacing calculation in (<b>a</b>) (004), (<b>b</b>) (101), and (<b>c</b>) (105) peaks.</p>
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<p>Energy dispersive X-ray (EDX) image for the as-synthesized TiO<sub>2</sub>/Au NSs.</p>
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<p>(<b>a</b>) UV–Vis diffuse absorption spectra of TiO<sub>2</sub>/Au; and (<b>b</b>) Additional peak shoulder in the visible region; and (<b>c</b>) Tauc plot for band gap determination of TiO<sub>2</sub>/Au NSs.</p>
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<p>Photocatalytic degradation of methylene blue (MB) dye, ibuprofen, and naproxen for (<b>a</b>) cycle 1 and (<b>b</b>) cycle 2 under direct solar irradiation; (<b>c</b>) degradation of MB under controlled visible light irradiation; and UV–visible spectra of (<b>d</b>) TiO<sub>2</sub> and (<b>e</b>) Au/TiO<sub>2</sub> NCs for MB degradation.</p>
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<p>Photocatalytic degradation of methylene blue (MB) dye, ibuprofen, and naproxen for (<b>a</b>) cycle 1 and (<b>b</b>) cycle 2 under direct solar irradiation; (<b>c</b>) degradation of MB under controlled visible light irradiation; and UV–visible spectra of (<b>d</b>) TiO<sub>2</sub> and (<b>e</b>) Au/TiO<sub>2</sub> NCs for MB degradation.</p>
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<p>Pseudo-first order kinetics of (MB) dye, ibuprofen, and naproxen for (<b>a</b>) cycle 1 and (<b>b</b>) cycle 2 under direct sunlight exposure; and (<b>c</b>) MB under controlled visible light irradiation.</p>
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