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Gels, Volume 10, Issue 3 (March 2024) – 59 articles

Cover Story (view full-size image): This is a study on the mechanical, thermal, and adsorption properties of hydroxyethyl methacrylate (HEMA) cryogels concerning varying monomer–crosslinker (N,N′-methylene-bisacrylamide–MBAA) ratios. Cryogels were synthesized with different ratios to assess their suitability for specific applications. An analysis of scanning-electron-microscopy images revealed a trend in macroporosity, with a decreasing average pore width and increasing pore number as the MBAA content increased. While swelling capacity correlates with pore size and distribution, stability increases with crosslinker content. Additionally, compression-strength measurements show an approximate 50% variation across different HEMA/MBAA ratios. These findings suggest that slight variations in reactant ratios can tune the properties of HEMA cryogels, offering insights for different material-design applications. View this paper
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15 pages, 3665 KiB  
Article
Tailoring Hydrogel Structures: Investigating the Effects of Multistep Cellulose Defibrillation on Polyvinyl Alcohol Composites
by Gabriel Goetten de Lima, Bruno Bernardi Aggio, Alessandra Cristina Pedro, Tielidy A. de M. de Lima and Washington Luiz Esteves Magalhães
Gels 2024, 10(3), 212; https://doi.org/10.3390/gels10030212 - 21 Mar 2024
Viewed by 1146
Abstract
Defibrillating cellulose through various grinding steps and incorporating it into hydrogels introduces unique properties that warrant thorough exploration. This study investigates cellulose defibrillation at different steps (15–120) using an ultra-fine friction grinder, blended with high-molecular-weight polyvinyl alcohol (PVA), and crosslinked via freeze–thawing. A [...] Read more.
Defibrillating cellulose through various grinding steps and incorporating it into hydrogels introduces unique properties that warrant thorough exploration. This study investigates cellulose defibrillation at different steps (15–120) using an ultra-fine friction grinder, blended with high-molecular-weight polyvinyl alcohol (PVA), and crosslinked via freeze–thawing. A critical discovery is the influence of defibrillation on the hydrogel structure, as evidenced by reduced crystallinity, thermal degradation, and the enhanced swelling of PVA chains. Despite an increased elastic modulus of up to 120 steps, the synthesized material maintains remarkable strength under hydrated conditions, holding significant promise in biomaterial applications. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels (3rd Edition))
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<p>Surface morphology performed by SEM for PVA hydrogels samples containing cellulose defibrillated at different steps: (<b>a</b>) 15, (<b>b</b>) 30, (<b>c</b>) 60, and (<b>d</b>) 120.</p>
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<p>Cross-section (<b>a</b>–<b>d</b>) and processed colourmap (<b>e</b>–<b>h</b>) images for samples studied of PVA hydrogels with cellulose defibrillated at 15 (<b>a</b>,<b>e</b>), 30 (<b>b</b>,<b>f</b>), 60 (<b>c</b>,<b>g</b>), and 120 (<b>d</b>,<b>h</b>) steps.</p>
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<p>FTIR of PVA hydrogels and also containing cellulose defibrillated at different steps: 30, 60, and 120. Regions were assigned as to the most different profiles seen; the numbers on each assigned band mean that there is a perceived difference for that specific condition.</p>
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<p>PM-IRRAS for the bulk signal of PVA hydrogels containing cellulose defibrillated at different steps, where (<b>a</b>) corresponds to the whole spectra region and purple circle indicates the region where a zoom with smoothing spectra was performed in (<b>b</b>).</p>
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<p>DMA tensile stress–strain mode for dried (<b>a</b>) and fully swollen (<b>c</b>) PVA+NFC hydrogels, containing cellulose defibrillated at different steps. (<b>b</b>,<b>d</b>) The elastic modulus calculated as the slope in stress–strain curves. (*) Statistically significant different by HSD Tukey test (<span class="html-italic">p</span> &lt; 0.05).</p>
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<p>(<b>a</b>) Thermogravimetric analysis and its derivative for pure NFC films defibrillated at different steps (<b>a</b>,<b>c</b>) and PVA hydrogel samples blended with cellulose defibrillated at different steps (<b>b</b>,<b>d</b>). Arrows indicate the direction in which the main peak is shifting at increased defibrillation steps.</p>
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<p>Swelling ratio of the studied PVA hydrogels containing defibrillated cellulose at different steps.</p>
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<p>Diagram to illustrate the hypothesis of this work in which cellulose bundles are defibrillated by the mechanical forces; depending on the degree of defibrillation, the interaction between PVA by physical crosslinking changes. A saturation fn the interaction occurs at 60 steps, and at 120 steps, PVA is aggregated around the overdefibrillated fibres.</p>
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44 pages, 7409 KiB  
Review
Hydrogels Based on Chitosan and Nanoparticles and Their Suitability for Dyes Adsorption from Aqueous Media: Assessment of the Last-Decade Progresses
by Cristina-Gabriela Grigoraș, Andrei-Ionuț Simion and Cătălin Drob
Gels 2024, 10(3), 211; https://doi.org/10.3390/gels10030211 - 21 Mar 2024
Cited by 1 | Viewed by 2112
Abstract
Water is one of the fundamental resources for the existence of humans and the environment. Throughout time, due to urbanization, expanding population, increased agricultural production, and intense industrialization, significant pollution with persistent contaminants has been noted, placing the water quality in danger. As [...] Read more.
Water is one of the fundamental resources for the existence of humans and the environment. Throughout time, due to urbanization, expanding population, increased agricultural production, and intense industrialization, significant pollution with persistent contaminants has been noted, placing the water quality in danger. As a consequence, different procedures and various technologies have been tested and used in order to ensure that water sources are safe for use. The adsorption process is often considered for wastewater treatment due to its straightforward design, low investment cost, availability, avoidance of additional chemicals, lack of undesirable byproducts, and demonstrated significant efficacious potential for treating and eliminating organic contaminants. To accomplish its application, the need to develop innovative materials has become an essential goal. In this context, an overview of recent advances in hydrogels based on chitosan and nanocomposites and their application for the depollution of wastewater contaminated with dyes is reported herein. The present review focuses on (i) the challenges raised by the synthesis process and characterization of the different hydrogels; (ii) the discussion of the impact of the main parameters affecting the adsorption process; (iii) the understanding of the adsorption isotherms, kinetics, and thermodynamic behavior; and (iv) the examination of the possibility of recycling and reusing the hydrogels. Full article
(This article belongs to the Special Issue Advances in Hydrogels and Hydrogel-Based Composites)
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<p>Search code used in Scopus database.</p>
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<p>Scopus descriptive analysis of 874 records—records by year.</p>
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<p>Scopus descriptive analysis of 874 records—records by year per source.</p>
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<p>Scopus descriptive analysis of 874 records—records by country/territory.</p>
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<p>Scopus descriptive analysis of 874 records—records by author.</p>
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<p>PRISMA diagram of the articles chosen for the study.</p>
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13 pages, 6355 KiB  
Article
Cellulose Diacetate Aerogels with Low Drying Shrinkage, High-Efficient Thermal Insulation, and Superior Mechanical Strength
by Sizhao Zhang, Kunming Lu, Yangbiao Hu, Guangyu Xu, Jing Wang, Yanrong Liao and Shuai Yu
Gels 2024, 10(3), 210; https://doi.org/10.3390/gels10030210 - 21 Mar 2024
Cited by 1 | Viewed by 1424
Abstract
The inherent characteristics of cellulose-derived aerogels, such as their natural abundance and environmental friendliness, make them highly interesting. However, its significant shrinkage before and after the supercritical drying procedure and low mechanical strength limit its potential application. Here, we propose a strategy to [...] Read more.
The inherent characteristics of cellulose-derived aerogels, such as their natural abundance and environmental friendliness, make them highly interesting. However, its significant shrinkage before and after the supercritical drying procedure and low mechanical strength limit its potential application. Here, we propose a strategy to prepare cellulose diacetate aerogels (CDAAs) with low drying shrinkage, exceptional thermal insulation, and superior mechanical strength. The low drying shrinkage (radial drying shrinkage of 1.4%) of CDAAs is attributed to their relative strong networking skeletons, which are greatly formed by tert-butanol solvent exchange in exerting the interaction of reducing the surface tension force. In this case, CDAAs are eventually endowed with the low bulk density of 0.069 g cm−3 as well. Additionally, as-prepared CDAAs possess an abundant three-dimensional networking structure whose pore size is concentrated in the diameter range of ~50 nm, and the result above is beneficial for improving the thermal insulation performance (thermal conductivity of 0.021 W m−1 K−1 at ambient environmental and pressure conditions). On the other hand, the optimal compressive stresses of CDAAs at 3% and 5% strain are 0.22 and 0.27 MPa respectively, indicating a mechanically well robustness. The above evidence demonstrates indeed the exceptional thermal insulation and superior compressive properties of CDAAs. This work may provide a new solution for developing a kind of high-performance cellulose-derived aerogel in the future. Full article
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<p>Photographs of the corresponding sol, initial gel, final gel, and aerogel in the CDAAs’ preparation processes: the respective stages for (<b>a</b>,<b>d</b>,<b>g</b>,<b>j</b>) CDAAs-T2P2, (<b>b</b>,<b>e</b>,<b>h</b>,<b>k</b>) CDAAs-T2P3, and (<b>c</b>,<b>f</b>,<b>i</b>,<b>l</b>) CDAAs-T2P4.</p>
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<p>Bulk density (<b>a</b>) and drying shrinkage (<b>b</b>) of CDAAs prepared with different catalyst contents.</p>
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<p>FESEM images of CDAAs showing the textural structure at different magnifications: (<b>a</b>–<b>c</b>) CDAAs-T2P2, (<b>d</b>–<b>f</b>) CDAAs-T2P3, (<b>g</b>–<b>i</b>) CDAAs-T2P4.</p>
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<p>N<sub>2</sub> adsorption–desorption isotherms and pore distributions of CDAAs: (<b>a</b>,<b>d</b>) CDAAs-T2P2, (<b>b</b>,<b>e</b>) CDAAs-T2P3, (<b>c</b>,<b>f</b>) CDAAs-T2P4.</p>
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<p>FTIR spectra of CDAAs (<b>a</b>) and XPS spectra of CDAAs: (<b>b</b>) CDAAs-T2P2, (<b>c</b>) CDAAs-T2P3, (<b>d</b>) CDAAs-T2P4.</p>
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<p>Chemical reaction process of CDAA formation.</p>
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<p>Monitoring temperature changes in the center of the cold surface of CDAAs-T2P4 on the heating plates at 50, 100, and 150 °C, respectively: CDAAs-T2P4 at (<b>a</b>–<b>c</b>) 50 °C, (<b>d</b>–<b>f</b>) 100 °C, and (<b>g</b>–<b>i</b>) 150 °C. Note: The red circle in the figure indicates the temperature measurement location.</p>
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<p>Compressive stress–strain curves of CDAAs: (<b>a</b>) CDAAs-T2P2, (<b>b</b>) CDAAs-T2P3, (<b>c</b>) CDAAs-T2P4.</p>
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<p>Thermal stability properties of CDAAs obtained by TG-DSC: (<b>a</b>) CDAAs-T2P2, (<b>b</b>) CDAAs-T2P3, (<b>c</b>) CDAAs-T2P4. Note: The solid line indicates the mass retention rate and the dashed line indicates the heat flow.</p>
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17 pages, 9594 KiB  
Article
Exploring the Impact of the Synthesis Variables Involved in the Polyurethane Aerogels-like Materials Design
by Esther Pinilla-Peñalver, Darío Cantero, Amaya Romero and Luz Sánchez-Silva
Gels 2024, 10(3), 209; https://doi.org/10.3390/gels10030209 - 20 Mar 2024
Cited by 3 | Viewed by 1781
Abstract
This research presents a novel approach to synthesising polyurethane (PUR)-based aerogels at the pilot scale, optimizing synthesis variables such as the gelation solvent, solids content, chain extender/isocyanate ratio, and dispersion mode. The solids content (2–11 wt.%) is the parameter with the most influence [...] Read more.
This research presents a novel approach to synthesising polyurethane (PUR)-based aerogels at the pilot scale, optimizing synthesis variables such as the gelation solvent, solids content, chain extender/isocyanate ratio, and dispersion mode. The solids content (2–11 wt.%) is the parameter with the most influence on the density of the aerogels, with a clear decrease in this property as the solids content decreases. On the other hand, it was demonstrated that minimizing the excess of ethylenediamine (used as chain extender) in relation to the isocyanate is a valuable consideration to improve the thermal conductivity of the aerogel. Related to the chain extender/isocyanate ratio, a compromise situation where the initial isocyanate reacts almost completely is crucial. Fourier-transform infrared spectroscopy was used to conduct such monitoring during the reaction. Once the conditions were optimised, the aerogel showing improved properties was synthesised using ethyl acetate as the gelling solvent, a 3.7 wt.% solids content, an ethylenediamine/isocyanate ratio of 0.20, and sonication as the dispersion mode, attaining a thermal conductivity of 0.030 W m−1 K−1 and a density of 0.046 g cm−3. Therefore, the synthesized aerogel emerges as a promising candidate for use in the construction and automotive industries. Full article
(This article belongs to the Special Issue Synthesis and Application of Aerogel)
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<p>Influence of the organic solvent on the density and thermal conductivity of WBPUR aerogels (synthesis conditions: 10.8 wt.% solids content).</p>
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<p>FT-IR spectra of pure isocyanate and WBPUR aerogels prepared using different gelation solvents.</p>
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<p>Influence of the solids content on the density and thermal conductivity of WBPUR aerogels.</p>
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<p>SEM micrographs of WBPUR aerogels prepared using EtOAc solvent with (<b>a</b>) 3.2, (<b>b</b>) 3.7, (<b>c</b>) 7.2, and (<b>d</b>) 10.8 wt.% solids content.</p>
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<p>Compressive stress–strain curves of WBPUR aerogel prepared with different solids contents.</p>
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<p>Shrinkage ratios corresponding to WBPUR aerogels obtained using different chain extender/isocyanate ratios (measured one month after their preparation).</p>
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<p>Physical appearance of WBPUR aerogels. WBPUR aerogels obtained using different chain extender/isocyanate ratios (freshly prepared and one month after their preparation).</p>
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<p>FT-IR profiles of the synthesized WBPUR aerogels obtained using different chain extender/isocyanate ratios. Inset: amplified region showing the -N=C=O groups.</p>
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<p>Influence of EDA/HMDI ratio in the density and thermal conductivity of WBPUR aerogels.</p>
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<p>DSC thermograms of the synthesized WBPUR aerogels obtained using different chain extender/isocyanate ratios.</p>
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<p>Thermal conductivity and density values found for the synthesized aerogels with different solids contents and dispersion modes (synthesis conditions: 0.33 EDA/HMDI ratio).</p>
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<p>SEM micrographs corresponding to the obtained WBPUR aerogels using (<b>a</b>,<b>b</b>) mechanical agitation and (<b>c</b>,<b>d</b>) sonication as dispersion mode (synthesis conditions: 10.8 wt.% solids content and 0.33 EDA/HMDI ratio).</p>
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<p>TGA (solid line) and DTGA (dotted line) curves of WBPUR aerogel (synthesis conditions: EtOAc, 3.7 wt.% solids content and 0.2 EDA/HMDI ratio).</p>
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<p>Schematic process of WBPUR aerogel design via stepwise polymerization and freeze-drying methods.</p>
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14 pages, 5619 KiB  
Article
Bimetallic Organic Gel for Effective Methyl Orange Dye Adsorption
by Hua Jin, Xinyuan Xu, Xiaoyang Yu, Shihua Yu, Shanshan Wang and Xiaoshu Qu
Gels 2024, 10(3), 208; https://doi.org/10.3390/gels10030208 - 19 Mar 2024
Cited by 2 | Viewed by 1376
Abstract
A bimetallic organic gel (MOG-Fe/Al) was synthesized through the solvothermal method. The gel state of the product obtained under optimized gel formation conditions is sufficient to carry 2 g of weight for a long time. Scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier [...] Read more.
A bimetallic organic gel (MOG-Fe/Al) was synthesized through the solvothermal method. The gel state of the product obtained under optimized gel formation conditions is sufficient to carry 2 g of weight for a long time. Scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, Brunauer–Emmett–Teller (BET) technique, and X-ray photoelectron spectroscopy (XPS) analysis confirmed the structures and morphologies of the synthesized materials. MOG-Fe/Al, with good stability, excellent durability, and wide applicability, exhibited efficient MO adsorption capacity as high as 335.88 mg/g at 25 °C. Adsorption-influencing factors including solution pH, contact time, and temperature were investigated. The adsorption performance of the bimetallic organic gel was better than that of the monometallic organic gels (MOG-Fe and MOG-Al), and its adsorption processes were in accordance with the pseudo-second-order kinetic and Langmuir isothermal models. The excellent adsorption capacity of the MOG-Fe/Al is due to its surface structure, pore volume, π-π interactions, hydrogen bonds, and electrostatic interactions. Full article
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<p>SEM images of MOG-Fe (<b>A</b>,<b>B</b>), MOG-Al (<b>C</b>,<b>D</b>), MOG-Fe/Al (<b>E</b>,<b>F</b>).</p>
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<p>The high-resolution survey (<b>A</b>), Fe 2p spectrum (<b>B</b>), Al 2p spectrum (<b>C</b>), C 1s spectrum (<b>D</b>), and O 1s spectrum (<b>E</b>) of MOG-Fe/Al.</p>
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<p>XRD spectra (<b>A</b>), FT-IR spectra (<b>B</b>), and BET results (<b>C</b>) of the three MOGs and pore size distribution of MOG-Fe/Al (<b>D</b>).</p>
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<p>Effect of the metal source on the adsorption properties, Adsorption capacity (<b>A</b>) (Inset: picture of the MOG-Fe/Al adsorption system before and after adsorption; <span class="html-italic">C</span><sub>0</sub>: 100 mg/L; adsorbent: 0.5 g/L; pH: deregulation; T: 298 K) and Adsorption efficiency (<b>B</b>).</p>
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<p>Effect of pH on the adsorption properties (<b>A</b>); effect of contact time (<b>B</b>) (<span class="html-italic">C</span><sub>0</sub>: 100 mg/L; MOG-Fe/Al: 0.5 g/L; pH: deregulation; T: 298 K).</p>
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<p>Kinetic fitting curves for MO by MOG-Fe/Al: pseudo-first-order (<b>A</b>), pseudo-second-order (<b>B</b>) (<span class="html-italic">C</span><sub>0</sub>: 100 mg/L; MOG-Fe/Al: 0.5 g/L; pH: deregulation; T: 298 K).</p>
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<p>Effect of initial MO concentration on adsorption (<b>A</b>) and the Langmuir (<b>B</b>), Freundlich (<b>C</b>), and Temkin isotherms (<b>D</b>) (MOG-Fe/Al: 0.5 g/L; pH: deregulation; T: 298 K).</p>
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<p>Effect of temperature on MO removal (<b>A</b>); Van’t Hoff plot for MO adsorption on MOG-Fe/Al (<b>B</b>) (<span class="html-italic">C</span><sub>0</sub>: 100 mg/L; MOG-Fe/Al: 0.5 g/L; pH: deregulation).</p>
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<p>Seven consecutive recycling experiments for MO adsorption by MOG-Fe/Al (<b>A</b>); the FT-IR spectra of MOG-Fe/Al before and after regeneration (<b>B</b>); adsorption of multiple dyes, i.e., CV, MB, MO, RhB, and EY (<span class="html-italic">C</span><sub>0</sub> of dye: 20 mg/L; MOG-Fe/Al: 0.5 g/L; pH: deregulation) (<b>C</b>).</p>
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<p>Schematic representation of the procedures for preparing MOGs.</p>
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20 pages, 3086 KiB  
Article
Topical Meloxicam Hydroxypropyl Guar Hydrogels Based on Low-Substituted Hydroxypropyl Cellulose Solid Dispersions
by Zaid Dahma, Carlos Torrado-Salmerón, Covadonga Álvarez-Álvarez, Víctor Guarnizo-Herrero, Borja Martínez-Alonso, Guillermo Torrado, Santiago Torrado-Santiago and Paloma Marina de la Torre-Iglesias
Gels 2024, 10(3), 207; https://doi.org/10.3390/gels10030207 - 18 Mar 2024
Cited by 1 | Viewed by 1151
Abstract
Meloxicam (MX) is a poorly water-soluble drug with severe gastrointestinal side effects. Topical hydrogel of hydroxypropyl guar (HPG) was formulated using a solid dispersion (SD) of MX with hydroxypropyl cellulose (LHPC) as an alternative to oral administration. The development of a solid dispersion [...] Read more.
Meloxicam (MX) is a poorly water-soluble drug with severe gastrointestinal side effects. Topical hydrogel of hydroxypropyl guar (HPG) was formulated using a solid dispersion (SD) of MX with hydroxypropyl cellulose (LHPC) as an alternative to oral administration. The development of a solid dispersion with an adequate MX:LHPC ratio could increase the topical delivery of meloxicam. Solid dispersions showed high MX solubility values and were related to an increase in hydrophilicity. The drug/polymer and polymer/polymer interactions of solid dispersions within the HPG hydrogels were evaluated by SEM, DSC, FTIR, and viscosity studies. A porous structure was observed in the solid dispersion hydrogel MX:LHPC (1:2.5) and its higher viscosity was related to a high increase in hydrogen bonds among the –OH groups from LHPC and HPG with water molecules. In vitro drug release studies showed increases of 3.20 and 3.97-fold for hydrogels with MX:LHPC ratios of (1:1) and (1:2.5), respectively, at 2 h compared to hydrogel with pure MX. Finally, a fitting transition from zero to first-order model was observed for these hydrogels containing solid dispersions, while the n value of Korsmeyer–Peppas model indicated that release mechanism is governed by diffusion through an important relaxation of the polymer. Full article
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<p>Solubility degree in phosphate buffer (pH 5.8) of MX raw material (MX − RM), physical mixture PM − MX:LHPC (1:2.5) and solid dispersions: SD − MX:LHPC (1:0), SD − MX:LHPC (1:1), SD − M:LHPC (1:2.5), SD − MX:LHPC (1:5), and SD − MX:LHPC (1:10).</p>
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<p>DSC thermograms of MX and LHPC raw materials (MX − RM and LHPC − RM), physical mixture PM − MX:LHPC (1:2.5) and solid dispersions: SD − MX:LHPC (1:1), SD − M:LHPC (1:2.5), SD − MX:LHPC (1:5), and SD − MX:LHPC (1:10).</p>
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<p>X-ray powder diffraction scans of MX and LHPC raw materials (MX − RM and LHPC − RM), physical mixture PM − MX:LHPC (1:2.5) and solid dispersions: SD − MX: LHPC (1:1), SD − M:LHPC (1:2.5), SD − MX:LHPC (1:5), and SD − MX:LHPC (1:10).</p>
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<p>FTIR spectra of MX raw material (MX − RM), physical mixture PM − MX:LHPC (1:2.5), and solid dispersions: SD − MX: LHPC (1:1) and SD − M:LHPC (1:2.5).</p>
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<p>Rheological behavior of the hydrogel formulations: H − Blank, HMX − RM, HPM − MX:LHPC (1:2.5), and HSD − MX:LHPC (1:2.5). Results are presented as mean values (<span class="html-italic">n</span> = 3) for each formulation.</p>
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<p>Scanning electron micrographs of freeze-dried formulations: (<b>A</b>) HPG hydrogel (H − Blank); (<b>B</b>) MX hydrogel (HMX − RM); (<b>C</b>) physical mixture hydrogel HPM − MX:LHPC (1:2.5); (<b>D</b>) solid dispersion hydrogel HSD − MX:LHPC: (1:2.5). Original magnification is 500× and the scale bar is equal to 50 μm.</p>
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<p>FTIR spectra of HPG hydrogel (H − Blank), MX hydrogel (HMX − RM), physical mixture hydrogel HPM − MX:LHPC (1:2.5), and solid dispersion hydrogel HSD − MX: LHPC (1:2.5).</p>
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<p>Release profiles at pH 5.8 for meloxicam hydrogels: HMX − RM, HPM − MX:LHPC (1:2.5), HSD − MX:LHPC (1:0), HSD − MX:LHPC (1:1), HSD − MX:LHPC (1:2.5), and HSD − MX:LHPC (1:5).</p>
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16 pages, 2389 KiB  
Review
Cholesterol-Bearing Polysaccharide-Based Nanogels for Development of Novel Immunotherapy and Regenerative Medicine
by Tetsuya Adachi, Yoshiro Tahara, Kenta Yamamoto, Toshiro Yamamoto, Narisato Kanamura, Kazunari Akiyoshi and Osam Mazda
Gels 2024, 10(3), 206; https://doi.org/10.3390/gels10030206 - 18 Mar 2024
Viewed by 1720
Abstract
Novel functional biomaterials are expected to bring about breakthroughs in developing immunotherapy and regenerative medicine through their application as drug delivery systems and scaffolds. Nanogels are defined as nanoparticles with a particle size of 100 nm or less and as having a gel [...] Read more.
Novel functional biomaterials are expected to bring about breakthroughs in developing immunotherapy and regenerative medicine through their application as drug delivery systems and scaffolds. Nanogels are defined as nanoparticles with a particle size of 100 nm or less and as having a gel structure. Nanogels have a three-dimensional network structure of cross-linked polymer chains, which have a high water content, a volume phase transition much faster than that of a macrogel, and a quick response to external stimuli. As it is possible to transmit substances according to the three-dimensional mesh size of the gel, a major feature is that relatively large substances, such as proteins and nucleic acids, can be taken into the gel. Furthermore, by organizing nanogels as a building block, they can be applied as a scaffold material for tissue regeneration. This review provides a brief overview of the current developments in nanogels in general, especially drug delivery, therapeutic applications, and tissue engineering. In particular, polysaccharide-based nanogels are interesting because they have excellent complexation properties and are highly biocompatible. Full article
(This article belongs to the Special Issue Development of Nanogels/Microgels for Regenerative Medicine)
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<p>Schematic illustration of this review. Cholesterol-substituted polysaccharides form self-assembled nanogels that are cross-linked to build a nanogel-cross-linked (NanoClik) gel. Nanogels are used in immunotherapy, delivering proteins and genes. NanoClik gels are used in regenerative medicine, delivering growth factors or adhering cells for tissue engineering.</p>
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<p>Observation of cells adhered on NanoCliP-FD gels by CLM. (<b>a</b>) Fibroblasts adhered to small-scale NanoCliP-FD gels prepared using a similar method described in a previous study [<a href="#B40-gels-10-00206" class="html-bibr">40</a>]. Blue (nucleus), green (F-actin), red (gel). (<b>b</b>) Fibroblasts adhered to large NanoCliP-FD gels. Blue (live cell), red (gel). (<b>c</b>) HepG2 cells adhered to NanoCliP-FD microspheres on a large scale. Blue (nucleus), green (F-actin), red (gel).</p>
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<p>Observation of biological apatite on a NanoCliP gel using electron microscopy. Transmission electron microscopy (TEM) and scanning electron microscopy (SEM) images are shown. Matrix vesicles (<b>a</b>), with a grain size of ~200 nm, are the starting points of calcification, calcified globules formed with the progress of calcification, and apatite crystals are observed inside the NanoCliP (<b>b</b>,<b>c</b>). Apatite crystals and collagen (arrow) are observed (<b>d</b>,<b>e</b>).</p>
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<p>Characters of the complex of each cell and NanoCliP-FD gel. Alizarin Red S staining of the complex of each cell and NanoCliP-FD gel (magnification 40×) (<b>a</b>). ALP mRNA expression of the complex of each cell and NanoCliP-FD gel (<b>b</b>). ** <span class="html-italic">p</span> &lt; 0.01 vs. HDFs. HDFs: human dermal fibroblasts, cOBs: chemical compound-mediated directly converted osteoblasts.</p>
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16 pages, 5275 KiB  
Article
Development of pH-Responsive, Thermosensitive, Antibacterial, and Anticancer CS/PVA/Graphene Blended Hydrogels for Controlled Drug Delivery
by Saira Mansha, Amna Sajjad, Aneeqa Zarbab, Tahmina Afzal, Zakia Kanwal, Muhammad Javaid Iqbal, Mohsin Ali Raza and Sharafat Ali
Gels 2024, 10(3), 205; https://doi.org/10.3390/gels10030205 - 18 Mar 2024
Viewed by 1676
Abstract
Drug delivery techniques based on polymers have been investigated for their potential to improve drug solubility, reduce systemic side effects, and controlled and targeted administration at infection site. In this study, we developed a co-polymeric hydrogel composed of graphene sheets (GNS), polyvinyl alcohol [...] Read more.
Drug delivery techniques based on polymers have been investigated for their potential to improve drug solubility, reduce systemic side effects, and controlled and targeted administration at infection site. In this study, we developed a co-polymeric hydrogel composed of graphene sheets (GNS), polyvinyl alcohol (PVA), and chitosan (CS) that is loaded with methotrexate (MTX) for in vitro liver cancer treatment. Fourier transform infrared spectroscopy (FTIR) and atomic force microscopy (AFM) was employed to check the structural properties and surface morphology. Moreover, tests were conducted on the cytotoxicity, hemolytic activity, release kinetics, swelling behaviour and degradation of hydrogels. A controlled release of drug from hydrogel in PBS at pH 7.4 was examined using release kinetics. Maximal drug release in six hours was 97.34%. The prepared hydrogels did not encourage the HepG2 growth and were non-hemolytic. The current study highlights the potential of GNS-based hydrogel loaded with MTX as an encouraging therapy for hepatocellular carcinoma. HepG2 cell viability of MTX-loaded CS-PVA-GNS hydrogel was (IC50 5.87 µg/200 mL) in comparison to free MTX (IC50 5.03 µg/200 mL). These outcomes recommend that hydrogels with GNS ensure improved drug delivery in cancer microenvironment while lessening adverse consequences on healthy cells. Full article
(This article belongs to the Special Issue Advanced Hydrogels in Drug Delivery and Wound Healing)
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<p>FTIR spectra of the prepared hydrogels indicating the presence of Si-O-Si linkage among OH and NH groups.</p>
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<p>AFM images of the prepared hydrogels (<b>a</b>,<b>b</b>) CP2b and (<b>c</b>,<b>d</b>) CP2b-GNS (<b>e</b>) GNS (<b>f</b>) height profile of GNS showing 1 nm thickness.</p>
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<p>Wetting analysis of the prepared hydrogels (<b>a</b>) CP2b and (<b>b</b>) CP2b-GNS.</p>
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<p>Time vs. Swelling % of CP1, CP2 and CP3 in (<b>a</b>) distilled water (<b>b</b>) PBS (<b>c</b>) acidic (HCl at pH 4) and basic (NaOH at pH 10) solutions (<b>d</b>,<b>e</b>) effect of temperature of the medium.</p>
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<p>Time vs. Swelling % of CP2a, CP2b, CP3c, and CP2b-GNS in (<b>a</b>) distilled water, (<b>b</b>) acid-base (HCl at pH 4 and NaOH at pH 10), and (<b>c</b>) at different temperatures.</p>
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<p>Degradation of CP2a, CP2b, CP2c and CP2b-GNS in PBS media for 7 days.</p>
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<p>(<b>a</b>) Hemolysis % of prepared hydrogels (<b>b</b>) Microscopic images of (<b>i</b>) +ve Control, (<b>ii</b>) CP2b, (<b>iii</b>) CP2b-GNS, (<b>iv</b>) −ve Control.</p>
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<p>(<b>a</b>) Antibacterial activity of CP2a, CP2b, CP2c and CP2GNS against Gram +ve <span class="html-italic">Staphylococcus aureus</span> (<span class="html-italic">S. aureus</span>) and Gram −ve <span class="html-italic">Escherichia coli</span> (<span class="html-italic">E. coli</span>), (<b>b</b>) Zone of inhibition of CP2b-GNS against Gram +ve <span class="html-italic">Staphylococcus aureus</span> (<span class="html-italic">S. aureus</span>), (<b>c</b>) Zone of inhibition of CP2b-GNS against Gram −ve <span class="html-italic">Escherichia coli</span> (<span class="html-italic">E. coli</span>).</p>
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<p>(<b>a</b>) Standard Curve of MTX at 321 nm (<b>b</b>) Cumulative drug release % of MTX from CP2b-GNS hydrogel.</p>
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<p>Release kinetics of drug loaded prepared hydrogel, (<b>a</b>) zero-order, (<b>b</b>) first-order, (<b>c</b>) Higuchi model and (<b>d</b>) Peppas model.</p>
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<p>Cytotoxic potential of Free MTX, CP2b-GNS, and CP2b-GNS + MTX against HepG2 cell line at different concentrations after 48 h of treatment.</p>
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<p>(<b>a</b>) Schematic illustration of the expected chemical bonding between chitosan, polyvinyl alcohol and GNS, (<b>b</b>) Possible scheme of interaction among CS, PVA, TEOS and GNS.</p>
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14 pages, 5686 KiB  
Article
Investigating Texture and Freeze–Thaw Stability of Cold-Set Gel Prepared by Soy Protein Isolate and Carrageenan Compounding
by Zhuying Wang, Zhenhai Yu, Shuanghe Ren, Jun Liu, Jing Xu, Zengwang Guo and Zhongjiang Wang
Gels 2024, 10(3), 204; https://doi.org/10.3390/gels10030204 - 18 Mar 2024
Cited by 1 | Viewed by 1462
Abstract
In this study, the purpose was to investigate the effects with different concentrations of carrageenan (CG, 0–0.30%) on the gel properties and freeze–thaw stability of soy protein isolate (SPI, 8%) cold-set gels. LF-NMR, MRI, and rheology revealed that CG promoted the formation of [...] Read more.
In this study, the purpose was to investigate the effects with different concentrations of carrageenan (CG, 0–0.30%) on the gel properties and freeze–thaw stability of soy protein isolate (SPI, 8%) cold-set gels. LF-NMR, MRI, and rheology revealed that CG promoted the formation of SPI-CG cold-set gel dense three-dimensional network structures and increased gel network cross-linking sites. As visually demonstrated by microstructure observations, CG contributed to the formation of stable SPI-CG cold-set gels with uniform and compact network structures. The dense gel network formation was caused when the proportion of disulfide bonds in the intermolecular interaction of SPI-CG cold-set gels increased, and the particle size and zeta potential of SPI-CG aggregates increased. SG20 (0.20% CG) had the densest gel network in all samples. It effectively hindered the migration and flow of water, which decreased the damage of freezing to the gel network. Therefore, SG20 exhibited excellent gel strength, water holding capacity, freeze–thaw stability, and steaming stability. This was beneficial for the gel having a good quality after freeze–thaw, which provided a valuable reference for the development of freeze–thaw-resistant SPI cold-set gel products. Full article
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<p>Plotting of (<b>A</b>) the curve of T<sub>2</sub> relaxation time; (<b>B</b>) magnetic resonance images; (<b>C</b>) storage modulus G′; (<b>D</b>) loss modulus G″ in the SPI-CG composite gels.</p>
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<p>The SEM pictures of SPI-CG cold-set gels. (<b>A</b>) SPI. (<b>B</b>) SG10. (<b>C</b>) SG15. (<b>D</b>) SG20. (<b>E</b>) SG25. (<b>F</b>) SG30.</p>
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<p>Plotting of (<b>A</b>) intermolecular forces of SPI-CG composite gels; (<b>B</b>) mean diameter of SPI-CG mixed solutions; (<b>C</b>) the particle size distribution of SPI-CG mixed solutions; (<b>D</b>) absolute value of Zeta potential of SPI-CG mixed solutions. Data with different letters in (<b>A</b>–<b>D</b>) are significantly different (<span class="html-italic">p</span> &lt; 0.05).</p>
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<p>Plotting of (<b>A</b>) gel strength; (<b>B</b>) WHC; (<b>C</b>) freeze–thaw stability; (<b>D</b>) steaming stability in SPI-CG composite gels. Data with different letters in (<b>A</b>–<b>D</b>) are significantly different (<span class="html-italic">p</span> &lt; 0.05).</p>
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17 pages, 4240 KiB  
Article
Fabrication and Characterization of Quad-Component Bioinspired Hydrogels to Model Elevated Fibrin Levels in Central Nervous Tissue Scaffolds
by Ana M. Diaz-Lasprilla, Meagan McKee, Andrea C. Jimenez-Vergara, Swathisri Ravi, Devon Bellamy, Wendy Ortega, Cody O. Crosby, Jennifer Steele, Germán Plascencia-Villa, George Perry and Dany J. Munoz-Pinto
Gels 2024, 10(3), 203; https://doi.org/10.3390/gels10030203 - 17 Mar 2024
Viewed by 1705
Abstract
Multicomponent interpenetrating polymer network (mIPN) hydrogels are promising tissue-engineering scaffolds that could closely resemble key characteristics of native tissues. The mechanical and biochemical properties of mIPNs can be finely controlled to mimic key features of target cellular microenvironments, regulating cell-matrix interactions. In this [...] Read more.
Multicomponent interpenetrating polymer network (mIPN) hydrogels are promising tissue-engineering scaffolds that could closely resemble key characteristics of native tissues. The mechanical and biochemical properties of mIPNs can be finely controlled to mimic key features of target cellular microenvironments, regulating cell-matrix interactions. In this work, we fabricated hydrogels made of collagen type I (Col I), fibrin, hyaluronic acid (HA), and poly (ethylene glycol) diacrylate (PEGDA) using a network-by-network fabrication approach. With these mIPNs, we aimed to develop a biomaterial platform that supports the in vitro culture of human astrocytes and potentially serves to assess the effects of the abnormal deposition of fibrin in cortex tissue and simulate key aspects in the progression of neuroinflammation typically found in human pathologies such as Alzheimer’s disease (AD), Parkinson’s disease (PD), and tissue trauma. Our resulting hydrogels closely resembled the complex modulus of AD human brain cortex tissue (~7.35 kPa), promoting cell spreading while allowing for the modulation of fibrin and hyaluronic acid levels. The individual networks and their microarchitecture were evaluated using confocal laser scanning microscopy (CLSM) and scanning electron microscopy (SEM). Human astrocytes were encapsulated in mIPNs, and negligible cytotoxicity was observed 24 h after the cell encapsulation. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization (2nd Edition))
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<p>The effect of increasing fibrin concentration on the complex modulus of Col I-fibrin IPNs; Col I levels were maintained consistently at 3.0 mg/mL across all formulations. *, significantly different from AD brain cortex, <span class="html-italic">p</span> &lt; 0.05; #, significantly different from mIPN 1, <span class="html-italic">p</span> &lt; 0.05, n = 4. ND, below the detection limit of the testing method.</p>
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<p>Representative confocal images of fibrin structure of mIPNs 5–8 at different fibrin concentrations (0.0–6.0 mg/mL); scale bar = 50 µm.</p>
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<p>Representative confocal images of mIPN containing Col I (3.0 mg/mL), HA (2.0 mg/mL), and fibrin (0.0 mg/mL and 6.0 mg/mL); scale bar = 50 µm.</p>
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<p>Representative SEM micrographs of scaffold microstructure. (<b>A</b>) Col I-HA (2.0 mg/mL)-PEGDA. (<b>B</b>) Col I-fibrin (6.0 mg/mL)-PEGDA (<b>C</b>) Col I-HA (2.0 mg/mL)-fibrin (6.0 mg/mL)-PEGDA; Scale bar = 2 µm; 10 kV and 7000× magnification. The red circles highlight denser areas or nodes associated with the introduction of fibrin.</p>
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<p>Cell viability of human astrocytes after 1 day of culture in mIPN 9 and mIPN 12. (<b>A</b>) Quantitative results using ImageJ software version 1.54f. (<b>B</b>) Representative laser scanning confocal microscopy images of Live/Dead staining, n = 7; scale bar = 100 µm.</p>
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<p>Representative 3D reconstructions of DAPI/phalloidin-stained human cortex astrocytes in mIPN 12 as a function of the spreading time before PEGDA infiltration. (<b>A</b>) Round control. (<b>B</b>) 4 h spreading time. (<b>C</b>) 24 h spreading time. The cell cytoskeleton is stained in red with rhodamine-phalloidin, and the cell nuclei are stained in blue with DAPI; scale bar = 100 µm.</p>
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<p>Schematic representation of mIPNs fabrication process.</p>
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13 pages, 4447 KiB  
Article
Effect of Hydrogel Stiffness on Chemoresistance of Breast Cancer Cells in 3D Culture
by Tianjiao Zeng, Huajian Chen, Toru Yoshitomi, Naoki Kawazoe, Yingnan Yang and Guoping Chen
Gels 2024, 10(3), 202; https://doi.org/10.3390/gels10030202 - 17 Mar 2024
Viewed by 1807
Abstract
Chemotherapy is one of the most common strategies for cancer treatment, whereas drug resistance reduces the efficiency of chemotherapy and leads to treatment failure. The mechanism of emerging chemoresistance is complex and the effect of extracellular matrix (ECM) surrounding cells may contribute to [...] Read more.
Chemotherapy is one of the most common strategies for cancer treatment, whereas drug resistance reduces the efficiency of chemotherapy and leads to treatment failure. The mechanism of emerging chemoresistance is complex and the effect of extracellular matrix (ECM) surrounding cells may contribute to drug resistance. Although it is well known that ECM plays an important role in orchestrating cell functions, it remains exclusive how ECM stiffness affects drug resistance. In this study, we prepared agarose hydrogels of different stiffnesses to investigate the effect of hydrogel stiffness on the chemoresistance of breast cancer cells to doxorubicin (DOX). Agarose hydrogels with a stiffness range of 1.5 kPa to 112.3 kPa were prepared and used to encapsulate breast cancer cells for a three-dimensional culture with different concentrations of DOX. The viability of the cells cultured in the hydrogels was dependent on both DOX concentration and hydrogel stiffness. Cell viability decreased with DOX concentration when the cells were cultured in the same stiffness hydrogels. When DOX concentration was the same, breast cancer cells showed higher viability in high-stiffness hydrogels than they did in low-stiffness hydrogels. Furthermore, the expression of P-glycoprotein mRNA in high-stiffness hydrogels was higher than that in low-stiffness hydrogels. The results suggested that hydrogel stiffness could affect the resistance of breast cancer cells to DOX by regulating the expression of chemoresistance-related genes. Full article
(This article belongs to the Special Issue Global Excellence in Bioactive Gels)
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<p>Usage of agarose hydrogels to mimic the ECM stiffness of breast cancers to investigate the effect of ECM stiffness on chemoresistance of breast cancer cells.</p>
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<p>Gross appearance (<b>a</b>) and SEM image of agarose hydrogels (<b>b</b>,<b>c</b>) prepared from 0.35%, 0.5%, 1%, 2%, 3% and 4% agarose aqueous solutions. Scale bar: 1 mm (<b>a</b>), 500 μm (<b>b</b>) and 100 μm (<b>c</b>).</p>
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<p>Young’s modulus of agarose hydrogels prepared from different concentrations of agarose. Data are the means ± S.D. (<span class="html-italic">n</span> = 5).</p>
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<p>Live/dead staining of breast cancer cells after 24 h culture in 0.35%, 0.5%, 1%, 2%, 3% and 4% agarose hydrogels without (<b>a</b>) or with different concentrations of DOX (<b>b</b>–<b>e</b>). A brief summary illustration of live/dead staining results (<b>f</b>). Scale bar: 200 μm. Green fluorescence: live cells; red fluorescence: dead cells.</p>
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<p>Quantified viability of breast cancer cells after 24 h culture in 0.35%, 0.5%, 1%, 2%, 3% and 4% agarose hydrogels with different DOX concentrations of 5 mg L<sup>−1</sup> (<b>a</b>), 10 mg L<sup>−1</sup> (<b>b</b>), 20 mg L<sup>−1</sup> (<b>c</b>) and 50 mg L<sup>−1</sup> (<b>d</b>). The data were normalized to the cell viability in the respective agarose hydrogels without DOX. Data are the means ± S.D. (<span class="html-italic">n</span> = 3). Significant differences: * <span class="html-italic">p</span> &lt; 0.1; ** <span class="html-italic">p</span> &lt; 0.01; *** <span class="html-italic">p</span> &lt; 0.001.</p>
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<p>Quantified viability of breast cancer cells after 12 (<b>a</b>), 24 (<b>b</b>), 36 (<b>c</b>), 48 (<b>d</b>) and 60 h (<b>e</b>) culture in 0.35%, 0.5%, 1%, 2%, 3% and 4% agarose hydrogels containing 10 mg L<sup>−1</sup> DOX. The data were normalized to the cell viability in the respective agarose hydrogels without DOX. Data are the means ± S.D. (<span class="html-italic">n</span> = 3). Significant differences: * <span class="html-italic">p</span> &lt; 0.1; ** <span class="html-italic">p</span> &lt; 0.01; *** <span class="html-italic">p</span> &lt; 0.001. n.s. = no significant difference.</p>
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<p>Quantified expression level of P-gP mRNA in breast cancer cells after 36 h culture in 0.35%, 0.5%, 1%, 2%, 3% and 4% agarose hydrogels without DOX (<b>a</b>) or with 10 mg L<sup>−1</sup> DOX (<b>b</b>). The data relative to GAPDH were normalized to the expression level in 0.35% agarose hydrogel. Data are the means ± S.D. (<span class="html-italic">n</span> = 3). Significant differences: * <span class="html-italic">p</span> &lt; 0.1; ** <span class="html-italic">p</span> &lt; 0.01. n.s. = no significant difference.</p>
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17 pages, 1365 KiB  
Article
Comparison of the Adsorption and Desorption Dynamics of Biological Molecules on Alginate Hydrogel Microcapsules—The Case of Sugars, Polyphenols, and Proteins
by Maja Benković, Izvorka Laljak, Davor Valinger, Tamara Jurina, Tea Sokač Cvetnić, Jasenka Gajdoš Kljusurić and Ana Jurinjak Tušek
Gels 2024, 10(3), 201; https://doi.org/10.3390/gels10030201 - 16 Mar 2024
Cited by 1 | Viewed by 1280
Abstract
The aim of this work was to analyze and compare the adsorption and desorption processes of carbohydrates (glucose as a model molecule), polyphenols (gallic acid as a model molecule), and proteins (bovine serum albumin, BSA as a model molecule) on alginate microcapsules. The [...] Read more.
The aim of this work was to analyze and compare the adsorption and desorption processes of carbohydrates (glucose as a model molecule), polyphenols (gallic acid as a model molecule), and proteins (bovine serum albumin, BSA as a model molecule) on alginate microcapsules. The adsorption and desorption processes were described by mathematical models (pseudo-first-order, pseudo-second-order, and Weber–Morris intraparticle diffusion model for adsorption, and first-order, Korsmeyer–Peppas, and the Higuchi model for desorption) in order to determine the dominant mechanisms responsible for both processes. By comparing the values of adsorption rate (k2) and initial adsorption rate (h0) based on the pseudo-first-order model, the lowest values were recorded for BSA (k1 = 0.124 ± 0.030 min−1), followed by glucose (k1 = 0.203 ± 0.041 min−1), while the model-obtained values for gallic acid were not considered significant at p < 0.05. For glucose and gallic acid, the limiting step of the adsorption process is the chemical sorption of substances, and the rate of adsorption does not depend on the adsorbate concentration, but depends on the capacity of the hydrogel adsorbent. Based on the desorption rates determined by the Korsmeyer–Peppas model (k), the highest values were recorded for gallic acid (k = 3.66236 ± 0.20776 g beads/mg gallic acid per min), followed by glucose (k = 2.55760 ± 0.16960 g beads/mg glucose per min) and BSA (k = 0.78881 ± 0.11872 g beads/mg BSA per min). The desorption process from alginate hydrogel microcapsules is characterized by the pseudo Fickian diffusion mechanism. Full article
(This article belongs to the Special Issue Physical and Mechanical Properties of Polymer Gels (2nd Edition))
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<p>(<b>a</b>) Changes in the relative (c<sub>t</sub>/c<sub>0</sub>) concentrations of the supernatant solutions during adsorption and the concentrations of the adsorbate in the alginate hydrogel beads (q<sub>t</sub>) during adsorption (experimental + model fitted data): (<b>b</b>) glucose containing alginate hydrogel beads; (<b>c</b>) gallic acid—alginate hydrogel beads; and (<b>d</b>) BSA—alginate hydrogel beads.</p>
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<p>(<b>a</b>) Changes in the relative (c<sub>t/</sub>c<sub>e</sub>) concentrations of the supernatant solutions during desorption and the concentrations of the adsorbate in the alginate hydrogel beads (M<sub>t</sub>) during desorption (experimental + model fitted data): glucose-containing alginate hydrogel beads (<b>b</b>); gallic acid–alginate hydrogel beads (<b>c</b>) and BSA–alginate hydrogel beads (<b>d</b>). Due to model fitting procedure, data for the first-order model are shown separately (secondary axis) to the Korsmeyer–Peppas and the Higuchi model.</p>
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<p>Images of the alginate beads: (<b>a</b>) plain alginate beads surface; (<b>b</b>) plain alginate beads surface with filter; (<b>c</b>) plain alginate beads cross-section; (<b>d</b>) BSA–alginate beads surface; (<b>e</b>) BSA–alginate beads surface with filter; (<b>f</b>) BSA–alginate beads cross-section; (<b>g</b>) glucose–alginate beads surface; (<b>h</b>) glucose–alginate beads surface with filter; (<b>i</b>) glucose–alginate beads cross-section; (<b>j</b>) gallic acid–alginate beads surface; (<b>k</b>) gallic acid–alginate beads surface with filter; (<b>l</b>) gallic acid–alginate beads cross-section.</p>
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20 pages, 4786 KiB  
Article
pH-Responsive Cellulose/Silk/Fe3O4 Hydrogel Microbeads Designed for Biomedical Applications
by Seung Hyeon Weon, Yuhyeon Na, Jiwoo Han, Jeong Woo Lee, Hyung Joo Kim, Saerom Park and Sang Hyun Lee
Gels 2024, 10(3), 200; https://doi.org/10.3390/gels10030200 - 16 Mar 2024
Cited by 1 | Viewed by 1716
Abstract
In this study, cellulose/Fe3O4 hydrogel microbeads were prepared through the sol–gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (TBAH) and 40% tetrabutylphosphonium hydroxide (TBPH) dissolved cellulose at room temperature [...] Read more.
In this study, cellulose/Fe3O4 hydrogel microbeads were prepared through the sol–gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (TBAH) and 40% tetrabutylphosphonium hydroxide (TBPH) dissolved cellulose at room temperature and effectively dispersed Fe3O4, forming cellulose/Fe3O4 microbeads with an average diameter of ~15 µm. Additionally, these solvents co-dissolved cellulose and silk, allowing for the manufacture of cellulose/silk/Fe3O4 hydrogel microbeads with altered surface characteristics. Owing to the negatively charged surface characteristics, the adsorption capacity of the cellulose/silk/Fe3O4 microbeads for the cationic dye crystal violet was >10 times higher than that of the cellulose/Fe3O4 microbeads. When prepared with TBAH, the initial adsorption rate of bovine serum albumin (BSA) on the cellulose/silk/Fe3O4 microbeads was 18.1 times higher than that on the cellulose/Fe3O4 microbeads. When preparing TBPH, the equilibrium adsorption capacity of the cellulose/silk/Fe3O4 microbeads for BSA (1.6 g/g) was 8.5 times higher than that of the cellulose/Fe3O4 microbeads. The pH-dependent BSA release from the cellulose/silk/Fe3O4 microbeads prepared with TBPH revealed 6.1-fold slower initial desorption rates and 5.2-fold lower desorption amounts at pH 2.2 than those at pH 7.4. Cytotoxicity tests on the cellulose and cellulose/silk composites regenerated with TBAH and TBPH yielded nontoxic results. Therefore, cellulose/silk/Fe3O4 microbeads are considered suitable pH-responsive supports for orally administered protein pharmaceuticals. Full article
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<p>Optical microscopic images of cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads prepared using TBAH (<b>a</b>) and TBPH (<b>b</b>). The contents of cellulose, silk, and Fe<sub>3</sub>O<sub>4</sub> in the microbead-preparing solution were 4, 1, and 0.5%, respectively. Hydrogel microbeads were stained with Congo red.</p>
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<p>FE-SEM images of cellulose-based microbeads: (<b>a</b>,<b>b</b>) cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared using TBAH; (<b>c</b>,<b>d</b>) cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared using TBAH; (<b>e</b>,<b>f</b>) cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared using TBPH; (<b>g</b>,<b>h</b>) cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared using TBPH. The contents of cellulose, silk, and Fe<sub>3</sub>O<sub>4</sub> in the microbead-preparing solution were 4, 1, and 0.5%, respectively.</p>
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<p>Swelling volumes (<b>a</b>) and swelling ratios (<b>b</b>) of cellulose-based hydrogel microbeads with same dry weight. The contents of cellulose, silk, and Fe<sub>3</sub>O<sub>4</sub> in the microbead-preparing solution were 4, 1, and 0.5%, respectively.</p>
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<p>Size distribution of cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads with various silk contents (●: 0%; ○: 0.25%; ▼: 0.5%; ∆: 1%; ■: 1.5%; and □: 2%) prepared using TBAH (<b>a</b>) and TBPH (<b>b</b>).</p>
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<p>Protein contents in cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads prepared with various silk contents. TBPH was used as the cellulose-dissolving solvent.</p>
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<p>The effect of silk content in cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads on the adsorption capacity for CV at pH 7. Black bars (TBAH) and gray bars (TBPH) represent the solvent used to prepare the microbeads. The initial concentration of CV for adsorption was 700 µg/mL. One-way analysis of variance (ANOVA) for silk content using Tukey’s test (<span class="html-italic">p</span> &lt; 0.05); inset letters suggest the group classified from Tukey’s test. The subscripts (1, 2) are in the same group for the ANOVA test. The same letter indicates that there is no significant difference between the data. Asterisks (*) indicate statistical significance by <span class="html-italic">t</span>-test analysis of variance for the solvent (<span class="html-italic">p</span> &lt; 0.05). N.S: not significant.</p>
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<p>Effect of contact time (<b>a</b>) and pseudo-second-order model fitting (<b>b</b>) for BSA adsorption on cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads. Filled and blanked symbols represent the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared with and without silk, respectively. Circle symbols (TBAH) and triangle symbols (TBPH) represent the solvent used to prepare the microbeads. The initial concentrations of BSA were 100 and 500 µg/mL for microbeads without and with silk, respectively.</p>
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<p>Effect of BSA concentration (<b>a</b>) and Langmuir model fitting as the best-fitted isotherm model (<b>b</b>) for BSA adsorption on cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads. Filled and blanked symbols represent cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared with and without silk, respectively. Circle symbols (TBAH) and triangle symbols (TBPH) represent the solvents used to prepare the microbeads.</p>
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<p>Cumulative release profiles of BSA from cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads at pH 2.2 and pH 7.4. Circle symbols (TBAH) and triangle symbols (TBPH) represent the solvents used to prepare the microbeads. Solid lines and dotted lines represent pH 2.2 and pH 7.4, respectively.</p>
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<p>Effects of regenerated cellulose and cellulose/silk film on HaCaT cell viability. Cell viability was determined using an NR assay. One-way analysis of variance with Tukey’s test (<span class="html-italic">p</span> &lt; 0.05); N.S: not significant.</p>
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14 pages, 5387 KiB  
Article
Synthesis and Properties of Polyvinylidene Fluoride-Hexafluoropropylene Copolymer/Li6PS5Cl Gel Composite Electrolyte for Lithium Solid-State Batteries
by Xinghua Liang, Xueli Shi, Lingxiao Lan, Yunmei Qing, Bing Zhang, Zhijie Fang and Yujiang Wang
Gels 2024, 10(3), 199; https://doi.org/10.3390/gels10030199 - 14 Mar 2024
Cited by 1 | Viewed by 1684
Abstract
Gel electrolytes for lithium-ion batteries continue to replace the organic liquid electrolytes in conventional batteries due to their advantages of being less prone to leakage and non-explosive and possessing a high modulus of elasticity. However, the development of gel electrolytes has been hindered [...] Read more.
Gel electrolytes for lithium-ion batteries continue to replace the organic liquid electrolytes in conventional batteries due to their advantages of being less prone to leakage and non-explosive and possessing a high modulus of elasticity. However, the development of gel electrolytes has been hindered by their generally low ionic conductivity at room temperature and high interfacial impedance with electrodes. In this paper, a poly (vinylidene fluoride)-hexafluoropropylene copolymer (PVdF-HFP) with a flexible structure, Li6PS5Cl (LPSCl) powder of the sulfur–silver–germanium ore type, and lithium perchlorate salt (LiClO4) were prepared into sulfide gel composite electrolyte films (GCEs) via a thermosetting process. The experimental results showed that the gel composite electrolyte with 1% LPSCl in the PVdF-HFP matrix exhibited an ionic conductivity as high as 1.27 × 10−3 S·cm−1 at 25 °C and a lithium ion transference number of 0.63. The assembled LiFePO4||GCEs||Li batteries have excellent rate (130 mAh·g−1 at 1 C and 54 mAh·g−1 at 5 C) and cycling (capacity retention was 93% after 100 cycles at 0.1 C and 80% after 150 cycles at 0.2 C) performance. This work provides new methods and strategies for the design and fabrication of solid-state batteries with high ionic conductivity and high specific energy. Full article
(This article belongs to the Section Gel Analysis and Characterization)
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<p>(<b>a</b>,<b>d</b>) Macroscopic picture of PVdF-HFP/LiClO<sub>4</sub> gel electrolyte film. (<b>b</b>) Moreover, 10 μm SEM image of the surface morphology of PVdF-HFP/LiClO<sub>4</sub>. (<b>c</b>) Furthermore, 5 μm SEM image of the surface morphology of PVdF-HFP/LiClO<sub>4</sub>. (<b>e</b>) Moreover, 20 μm SEM image of the cross-section morphology of PVdF-HFP/LiClO<sub>4</sub>. (<b>f</b>) Furthermore, 10 μm SEM image of the cross-section morphology of PVdF-HFP/LiClO<sub>4</sub>. (<b>g</b>) Moreover, 50 μm SEM image and EDS mappings of PVdF-HFP/LiClO<sub>4</sub>.</p>
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<p>(<b>a</b>,<b>d</b>) Macroscopic picture of PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte film. (<b>b</b>) Moreover, 10 μm SEM images of the surface morphology of PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte film. (<b>c</b>) Furthermore, 5 μm SEM images of the surface morphology of PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte film. (<b>e</b>) Moreover, 20 μm SEM images of the cross-sectional morphology of PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte film. (<b>f</b>) Furthermore, 10 μm SEM images of the cross-sectional morphology of PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte film. (<b>g</b>) Moreover, 50 μm SEM image and EDS mappings of PVdF-HFP/LiClO<sub>4</sub>/LPSCl distributions in the SCE membrane.</p>
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<p>(<b>a</b>) Impedance values of the battery electrolyte corresponding to the addition of different proportions of LPSCl for PVdF-HFP/LPSCl/LiClO<sub>4</sub>. (<b>b</b>) Ionic conductivity of the gel composite electrolyte film corresponding to the addition of different proportions of LPSCl. (<b>c</b>) Lithium-ion transference number of PVdF-HFP/LiClO<sub>4</sub> gel composite electrolyte. (<b>d</b>) Lithium-ion transference number of PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte.</p>
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<p>(<b>a</b>) DTG results of PVdF-HFP/LiClO<sub>4</sub> gel electrolyte film and PVdF-HFP/LPSCl/LiClO4 gel composite electrolyte film; (<b>b</b>) thermogravimetric analysis curves of PVdF-HFP, PVdF-HFP/LiClO<sub>4</sub>, and PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte films; (<b>c</b>) X-ray diffraction (XRD) patterns of PVdF-HFP, PVdF-HFP/LiClO<sub>4</sub> gel electrolyte film, and PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte film; (<b>d</b>) Fourier-transform infrared (FTIR) spectral curves of PVdF-HFP, PVdF-HFP/LiClO<sub>4</sub> gel electrolyte film, and PVdF-HFP/LPSCl/LiClO<sub>4</sub> gel composite electrolyte film.</p>
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<p>(<b>a</b>) Comparative cycling performance graphs of PVdF-HFP/LiClO<sub>4</sub> and PVdF-HFP/LPSCl/LiClO<sub>4</sub> solid-state batteries at 0.1 C; (<b>b</b>) graphs of current cycling performance of PVdF-HFP/LPSCl/LiClO<sub>4</sub> solid-state batteries at 0.2 C; (<b>c</b>) graphs of PVdF-HFP/LiClO<sub>4</sub> and PVdF-HFP/LPSCl/LiClO<sub>4</sub> solid-state battery performance from 0.1 C to 5 C multiplication rate; (<b>d</b>) charge–discharge curve of PVdF-HFP/LPSCl/LiCLlO<sub>4</sub> solid-state battery at 0.2 C.</p>
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<p>(<b>a</b>) CV curve of PVdF-HFP/LiClO<sub>4</sub> solid-state battery; (<b>b</b>) CV curve of PVdF-HFP/LPSCl/LiClO<sub>4</sub> solid-state battery.</p>
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<p>Flowchart of gel composite electrolyte film preparation.</p>
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27 pages, 1561 KiB  
Review
Cryogels and Monoliths: Promising Tools for Chromatographic Purification of Nucleic Acids
by João Ribeiro, Marco Â. Luís, Bruno Rodrigues, Fátima Milhano Santos, Joana Mesquita, Renato Boto and Cândida Teixeira Tomaz
Gels 2024, 10(3), 198; https://doi.org/10.3390/gels10030198 - 14 Mar 2024
Cited by 1 | Viewed by 1871
Abstract
The increasing demand for highly pure biopharmaceuticals has put significant pressure on the biotechnological industry to innovate in production and purification processes. Nucleic acid purification, crucial for gene therapy and vaccine production, presents challenges due to the unique physical and chemical properties of [...] Read more.
The increasing demand for highly pure biopharmaceuticals has put significant pressure on the biotechnological industry to innovate in production and purification processes. Nucleic acid purification, crucial for gene therapy and vaccine production, presents challenges due to the unique physical and chemical properties of these molecules. Meeting regulatory standards necessitates large quantities of biotherapeutic agents of high purity. While conventional chromatography offers versatility and efficiency, it suffers from drawbacks like low flow rates and binding capacity, as well as high mass transfer resistance. Recent advancements in continuous beds, including monoliths and cryogel-based systems, have emerged as promising solutions to overcome these limitations. This review explores and evaluates the latest progress in chromatography utilizing monolithic and cryogenic supports for nucleic acid purification. Full article
(This article belongs to the Section Gel Analysis and Characterization)
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<p>Mesopores and macropores in monoliths and cryogels are pivotal for nucleic acid purification via chromatography. Monoliths: mesopores amplify surface area for efficient molecule interaction, boosting purification efficacy and macropores serve as fluid conduits, easing solvent transport and minimizing mass transfer resistance. Cryogels: the interconnected macropores offer minimal pressure drop, short diffusion path, and retention time, facilitating rapid biomacromolecule enrichment and purification.</p>
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<p>Schematization of transport phenomena by diffusion in a packed-bed chromatography column (particulate support) and by convective flow in continuous beds (cryogels and monoliths). The diffusive mass transport is related to a slow process, lower resolution, and low capacity. In convective mass transport, the big channels allow laminar flow with no shear forces, leading to a flow-independent resolution and capacity.</p>
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<p>Cryogelation process. A solution of monomers and initiators is prepared in a cryogelation solvent and then is frozen (<b>A</b>), resulting in the formation of ice crystals (<b>B</b>). During freezing, an unfrozen liquid microphase (UFLMP) is formed, trapping polymer precursors, and allowing crystallization to progress, forming a network (<b>C</b>). Thawing the mixture at room temperature causes the ice to melt leaving behind macropores surrounded by a gel matrix and forming a supermacroporous interconnected structure (<b>D</b>).</p>
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13 pages, 4092 KiB  
Article
Flexible Composite Hydrogels Based on Polybenzoxazine for Supercapacitor Applications
by Shakila Parveen Asrafali, Thirukumaran Periyasamy, Gazi A. K. M. Rafiqul Bari and Seong-Cheol Kim
Gels 2024, 10(3), 197; https://doi.org/10.3390/gels10030197 - 13 Mar 2024
Cited by 1 | Viewed by 1302
Abstract
Polybenzoxazines (Pbzs) are advanced forms of phenolic resins that possess many attractive properties, including thermal-induced self-curing polymerization, void-free polymeric products and absence of by-product formation. They also possess high Tg (glass transition temperature) and thermal stability. But the produced materials are brittle [...] Read more.
Polybenzoxazines (Pbzs) are advanced forms of phenolic resins that possess many attractive properties, including thermal-induced self-curing polymerization, void-free polymeric products and absence of by-product formation. They also possess high Tg (glass transition temperature) and thermal stability. But the produced materials are brittle in nature. In this paper, we present our attempt to decrease the brittleness of Pbz by blending it with polyvinylalcohol (PVA). Benzoxazine monomer (Eu-Ed-Bzo) was synthesized by following a simple Mannich condensation reaction. The formation of a benzoxazine ring was confirmed by FT-IR and NMR spectroscopic analyses. The synthesized benzoxazine monomer was blended with PVA in order to produce composite films, PVA/Pbz, by varying the amount of benzoxazine monomer (1, 3 and 5 wt. % of PVA). The property of the composite films was studied using various characterization techniques, including DSC, TGA, water contact angle analysis (WCA) and SEM. WCA analysis proved that the hydrophobic nature of Pbz (value) was transformed to hydrophilic (WCA of PVA/Pbz5 is 35.5°). These composite films could play the same role as flexible electrolytes in supercapacitor applications. For this purpose, the composite films were immersed in a 1 M KOH solution for 12 h in order to analyze their swelling properties. Moreover, by using this swelled gel, a symmetric supercapacitor, AC//PVA/Pbz5//AC, was constructed, exhibiting a specific capacitance of 170 F g−1. Full article
(This article belongs to the Special Issue Gels for Energy Generation, Conversion and Storage Applications)
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<p>FT-IR spectrum of Eu-Ed-Bzo.</p>
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<p><sup>1</sup>H-NMR spectrum of Eu-Ed-Bzo.</p>
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<p>DSC profile of (<b>a</b>) Eu-Ed-Bzo, and (<b>b</b>) Eu-Ed-Bzo/PVA films [(i) PVA/Pbz1; (ii) PVA/Pbz3; and (iii) PVA/Pbz5].</p>
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<p>Water contact angle images of (<b>a</b>) PVA, (<b>b</b>) PVA/Pbz1, (<b>c</b>) PVA/Pbz3, and (<b>d</b>) PVA/Pbz5.</p>
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<p>FE-SEM images of (<b>a</b>) PVA, (<b>b</b>) PVA/Pbz1, (<b>c</b>) PVA/Pbz3 and (<b>d</b>) PVA/Pbz5.</p>
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<p>(<b>a</b>) TGA and (<b>b</b>) DTG graphs of (i) PVA/Pbz1, (ii) PVA/Pbz3 and (iii) PVA/Pbz5.</p>
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<p>Images of the composite films (<b>top</b>) and swelled gels (<b>bottom</b>) [(<b>i</b>) PVA/Pbz1, (<b>ii</b>) PVA/Pbz3, and (<b>iii</b>) PVA/Pbz5].</p>
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<p>(<b>a</b>) Tensile measurements and (<b>b</b>) XRD graphs of PVA and PVA/Pbz films.</p>
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<p>(<b>a</b>) CV curves of symmetric SCs at 50 mV s<sup>−1</sup>, (<b>b</b>) CV, (<b>c</b>) GCD, (<b>d</b>) EIS spectra, (<b>e</b>) cyclic stability and (<b>f</b>) capacitance retention of AC//PVA/PbzG5//AC.</p>
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<p>Synthesis of benzoxazine monomer (Eu-Ed-Bzo).</p>
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<p>Preparation of PVA/Pbz composite films.</p>
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17 pages, 2180 KiB  
Review
Hydrogels for Cardio and Vascular Tissue Repair and Regeneration
by Ilenia Motta, Michelina Soccio, Giulia Guidotti, Nadia Lotti and Gianandrea Pasquinelli
Gels 2024, 10(3), 196; https://doi.org/10.3390/gels10030196 - 13 Mar 2024
Cited by 1 | Viewed by 1844
Abstract
Cardiovascular disease (CVD), the leading cause of death globally, affects the heart and arteries with a variety of clinical manifestations, the most dramatic of which are myocardial infarction (MI), abdominal aortic aneurysm (AAA), and intracranial aneurysm (IA) rupture. In MI, necrosis of the [...] Read more.
Cardiovascular disease (CVD), the leading cause of death globally, affects the heart and arteries with a variety of clinical manifestations, the most dramatic of which are myocardial infarction (MI), abdominal aortic aneurysm (AAA), and intracranial aneurysm (IA) rupture. In MI, necrosis of the myocardium, scar formation, and loss of cardiomyocytes result from insufficient blood supply due to coronary artery occlusion. Beyond stenosis, the arteries that are structurally and functionally connected to the cardiac tissue can undergo pathological dilation, i.e., aneurysmal dilation, with high risk of rupture. Aneurysms of the intracranial arteries (IAs) are more commonly seen in young adults, whereas those of the abdominal aorta (AAA) are predominantly seen in the elderly. IAs, unpredictably, can undergo rupture and cause life-threatening hemorrhage, while AAAs can result in rupture, internal bleeding and high mortality rate. In this clinical context, hydrogels, three-dimensional networks of water-seizing polymers, have emerged as promising biomaterials for cardiovascular tissue repair or protection due to their biocompatibility, tunable properties, and ability to encapsulate and release bioactive molecules. This review provides an overview of the current state of research on the use of hydrogels as an innovative platform to promote cardiovascular-specific tissue repair in MI and functional recovery or protection in aneurysmal dilation. Full article
(This article belongs to the Special Issue Hydrogel for Tissue Regeneration)
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<p><b>Chemical structures of commonly used natural and synthetic materials</b>. PCL: polycaprolactone, PEG: poly(ethylene glycol), PHEMA: poly(2-hydroxyethyl methacrylate), PLA: poly(lactic acid), PVA: poly(vinyl alcohol).</p>
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<p><b>Hydrogel approaches for MI treatment.</b> In the figure, the different therapeutic approaches investigated to restore cardiac functions following MI are depicted. This figure was created by adapting a Servier Medical Art template [licensed under Creative Commons Attribution 3.0 Unported License <a href="http://www.smart.servier.com" target="_blank">www.smart.servier.com</a> (accessed on 12 December 2023)].</p>
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<p><b>Timeline of studies using hydrogel for the delivery of growth factors, cells, and exosomes for the treatment of MI [<a href="#B44-gels-10-00196" class="html-bibr">44</a>,<a href="#B47-gels-10-00196" class="html-bibr">47</a>,<a href="#B49-gels-10-00196" class="html-bibr">49</a>,<a href="#B50-gels-10-00196" class="html-bibr">50</a>,<a href="#B54-gels-10-00196" class="html-bibr">54</a>,<a href="#B56-gels-10-00196" class="html-bibr">56</a>,<a href="#B58-gels-10-00196" class="html-bibr">58</a>,<a href="#B60-gels-10-00196" class="html-bibr">60</a>,<a href="#B62-gels-10-00196" class="html-bibr">62</a>,<a href="#B63-gels-10-00196" class="html-bibr">63</a>,<a href="#B64-gels-10-00196" class="html-bibr">64</a>,<a href="#B65-gels-10-00196" class="html-bibr">65</a>,<a href="#B67-gels-10-00196" class="html-bibr">67</a>,<a href="#B68-gels-10-00196" class="html-bibr">68</a>,<a href="#B69-gels-10-00196" class="html-bibr">69</a>,<a href="#B70-gels-10-00196" class="html-bibr">70</a>,<a href="#B71-gels-10-00196" class="html-bibr">71</a>,<a href="#B73-gels-10-00196" class="html-bibr">73</a>,<a href="#B74-gels-10-00196" class="html-bibr">74</a>,<a href="#B75-gels-10-00196" class="html-bibr">75</a>,<a href="#B76-gels-10-00196" class="html-bibr">76</a>,<a href="#B81-gels-10-00196" class="html-bibr">81</a>,<a href="#B84-gels-10-00196" class="html-bibr">84</a>,<a href="#B85-gels-10-00196" class="html-bibr">85</a>,<a href="#B86-gels-10-00196" class="html-bibr">86</a>,<a href="#B88-gels-10-00196" class="html-bibr">88</a>].</b> </p>
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<p><b>EVAR complication and treatment approaches.</b> After treatment of AAA using EVAR, the occurrence of endoleaks can take place, resulting in the failure of the complete exclusion of an aneurysm from systemic circulation. The standard treatment for endoleaks is the use of metallic coils, which are injected into the aneurysm sac to induce coagulation and thus restore the exclusion of the aneurysm. However, the use of hydrogels could represent an effective approach for the treatment of endoleaks. This figure was created by adapting a Servier Medical Art templates [licensed under Creative Commons Attribution 3.0 Unported License <a href="http://www.smart.servier.com" target="_blank">www.smart.servier.com</a> (accessed on 12 December 2023)].</p>
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17 pages, 13462 KiB  
Article
Microstructure, Physical Properties, and Oxidative Stability of Olive Oil Oleogels Composed of Sunflower Wax and Monoglycerides
by Dafni Dimakopoulou-Papazoglou, Konstantina Zampouni, Prodromos Prodromidis, Thomas Moschakis and Eugenios Katsanidis
Gels 2024, 10(3), 195; https://doi.org/10.3390/gels10030195 - 13 Mar 2024
Cited by 1 | Viewed by 2010
Abstract
The utilization of natural waxes to form oleogels has emerged as a new and efficient technique for structuring liquid edible oil into solid-like structures for diverse food applications. The objective of this study was to investigate the interaction between sunflower wax (SW) and [...] Read more.
The utilization of natural waxes to form oleogels has emerged as a new and efficient technique for structuring liquid edible oil into solid-like structures for diverse food applications. The objective of this study was to investigate the interaction between sunflower wax (SW) and monoglycerides (MGs) in olive oil oleogels and assess their physical characteristics and storage stability. To achieve this, pure SW and a combination of SW with MGs in a 1:1 ratio were examined within a total concentration range of 6–12% w/w. The formed oleogels were characterized based on their microstructure, melting and crystallization properties, textural characteristics, and oxidative stability during storage. All the oleogels were self-standing, and, as the concentration increased, the hardness of the oleogels also increased. The crystals of SW oleogels were long needle-like, while the combination of SW and MGs led to the formation of crystal aggregates and rosette-like crystals. Differential scanning calorimetry and FTIR showed that the addition of MGs led to different crystal structures. The oxidation results revealed that oleogels had low peroxide and TBARS values throughout the 28-day storage period. These results provide useful insights about the utilization of SW and MGs oleogels for potential applications in the food industry. Full article
(This article belongs to the Special Issue Functionality of Oleogels and Bigels in Foods)
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<p>Visual appearance of oleogels created using sunflower wax (SW) and the monoglycerides (MGs) in olive oil.</p>
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<p>Polarized light micrographs of olive oil oleogels prepared with different concentrations of sunflower wax (SW) and sunflower wax with monoglycerides (SW + MGs) in a 1:1 ratio (scale 100 μm).</p>
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<p>Polarized light micrographs of olive oil oleogels prepared with 6 and 10% (<span class="html-italic">w</span>/<span class="html-italic">w</span>) of sunflower wax (SW) and sunflower wax with monoglycerides (SW + MGs) in a 1:1 ratio, stored at 5 °C for 1, 7, and 14 days (scale 100 μm).</p>
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<p>μDSC thermographs of olive oil oleogels prepared with 6 and 10% (<span class="html-italic">w</span>/<span class="html-italic">w</span>) of sunflower wax (SW) and sunflower wax with monoglycerides (SW + MGs) in a 1:1 ratio; (<b>a</b>) first heating run from 30 °C to 100 °C; (<b>b</b>) cooling from 100 °C to −10 °C; and (<b>c</b>) second heating run from −10 °C to 90 °C.</p>
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<p>μDSC thermographs of olive oil oleogels prepared with sunflower wax (SW) and sunflower wax with monoglycerides (SW + MGs, in a 1:1 ratio) stored at 5 °C for 1, 7, and 14 days; heating run from 30 °C to 100 °C; heating rate: 1 °C/min.</p>
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<p>FTIR spectra of olive oil oleogels created with a variety of concentrations of sunflower wax (SW) or sunflower wax with monoglycerides (SW + MGs) in a 1:1 ratio (spectral regions: (<b>a</b>) 4000–500 cm<sup>−1</sup>, (<b>b</b>) 3400–2800 cm<sup>−1</sup>, (<b>c</b>) 1800–1650 cm<sup>−1</sup>, and (<b>d</b>) 1450–900 cm<sup>−1</sup>).</p>
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<p>FTIR spectra of olive oil oleogels, prepared with 6 and 10% (<span class="html-italic">w</span>/<span class="html-italic">w</span>) of sunflower wax (SW) and sunflower wax with monoglycerides (SW + MGs) in a 1:1 ratio, stored at 5 °C for 1, 7, and 14 days (first raw: spectral region 1800–1650 cm<sup>−1</sup>, second raw: spectral region 1450–900 cm<sup>−1</sup>).</p>
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<p>Evolution of peroxide (<b>a</b>) and TBARS (<b>b</b>) values in liquid olive oil, SW-based oleogels, and SW plus MGs-based oleogels during storage at 25 and 35 °C over time.</p>
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21 pages, 3027 KiB  
Article
Characterization of Beeswax and Rice Bran Wax Oleogels Based on Different Types of Vegetable Oils and Their Impact on Wheat Flour Dough Technological Behavior during Bun Making
by Sorina Ropciuc, Florina Dranca, Mircea Adrian Oroian, Ana Leahu, Ancuţa Elena Prisacaru, Mariana Spinei and Georgiana Gabriela Codină
Gels 2024, 10(3), 194; https://doi.org/10.3390/gels10030194 - 12 Mar 2024
Cited by 2 | Viewed by 1788
Abstract
Five varieties of vegetable oil underwent oleogelation with two types of wax as follows: beeswax (BW) and rice bran wax (RW). The oleogels were analyzed for their physicochemical, thermal, and textural characteristics. The oleogels were used in the bun dough recipe at a [...] Read more.
Five varieties of vegetable oil underwent oleogelation with two types of wax as follows: beeswax (BW) and rice bran wax (RW). The oleogels were analyzed for their physicochemical, thermal, and textural characteristics. The oleogels were used in the bun dough recipe at a percentage level of 5%, and the textural and rheological properties of the oleogel doughs were analyzed using dynamic and empirical rheology devices such as the Haake rheometer, the Rheofermentometer, and Mixolab. The thermal properties of beeswax oleogels showed a melting peak at a lower temperature for all the oils used compared with that of the oleogels containing rice bran wax. Texturally, for both waxes, as the percentage of wax increased, the firmness of the oleogels increased proportionally, which indicates better technological characteristics for the food industry. The effect of the addition of oleogels on the viscoelastic properties of the dough was measured as a function of temperature. All dough samples showed higher values for G′ (storage modulus) than those of G″ (loss modulus) in the temperature range of 20–90 °C, suggesting a solid, elastic-like behavior of all dough samples with the addition of oleogels. The influence of the beeswax and rice bran oleogels based on different types of vegetable oils on the thermo-mechanical properties of wheat flour dough indicated that the addition of oleogels in dough recipes generally led to higher dough stability and lower values for the dough development time and those related to the dough’s starch characteristics. Therefore, the addition of oleogels in dough recipes inhibits the starch gelatinization process and increases the shelf life of bakery products. Full article
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<p>Visual appearance of vegetable oil oleogels with natural waxes.</p>
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<p>Effect of beeswax and rice bran concentrations on G′ and G″ with the angular frequency (<b>A</b>,<b>B</b>) and temperature (<b>C</b>,<b>D</b>). The red line represents the oleogel with grape seed oil (GO), the green line represents the oleogel with hemp seed oil (HO), the purple line represents the oleogel with olive oil (OL), the blue line represents the oleogel with sunflower oil (SO), and the orange line represents the oleogel with walnut oil (WO). Empty symbols represent the addition of 5% beeswax (BW) and solid symbols represent rice bran wax (RW). (<b>A</b>)—G′ angular frequency sweeps of oleogels with 5% wax; (<b>B</b>)—G″ angular frequency sweep of oleogels; (<b>C</b>)—oleogel modules G′ and G″ with 5% BW temperature sweep; (<b>D</b>)—oleogels modules G′ and G″ with 9% BW temperature sweep.</p>
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<p>Thermograms of oleogels, oils, and waxes for heating (→) and cooling (←) profiles: (<b>A</b>) oleogels with grape oil, (<b>B</b>) oils, and (<b>C</b>) beeswax and rice bran wax.</p>
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<p>Thermograms of oleogels, oils, and waxes for heating (→) and cooling (←) profiles: (<b>A</b>) oleogels with grape oil, (<b>B</b>) oils, and (<b>C</b>) beeswax and rice bran wax.</p>
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<p>Graphical representation of the viscoelastic modules for dough samples with the addition of oleogels. (<b>A</b>,<b>B</b>)—describe the viscoelastic modules for doughs obtained with oleogels with 5% and 9% BW; (<b>C</b>,<b>D</b>)—represent the viscoelastic modules for doughs with the addition of 5% and 9% RW. The red line represents the dough with oleogel from grape seed oil (GO), the green line represents the dough with oleogel from hemp seed oil (HO), the purple line represents the dough with oleogel from olive oil (OL), the blue line represents the dough with oleogel from sunflower oil (SO), and the orange line represents the dough with oleogel from walnut oil (WO). The empty symbols represent the module G′ and the filled symbols represent G″.</p>
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<p>Graphical representation of the viscoelastic modules for dough samples with the addition of oleogels. (<b>A</b>,<b>B</b>)—describe the viscoelastic modules for doughs obtained with oleogels with 5% and 9% BW; (<b>C</b>,<b>D</b>)—represent the viscoelastic modules for doughs with the addition of 5% and 9% RW. The red line represents the dough with oleogel from grape seed oil (GO), the green line represents the dough with oleogel from hemp seed oil (HO), the purple line represents the dough with oleogel from olive oil (OL), the blue line represents the dough with oleogel from sunflower oil (SO), and the orange line represents the dough with oleogel from walnut oil (WO). The empty symbols represent the module G′ and the filled symbols represent G″.</p>
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<p>PCA graph for thermal and rheological properties of oleogels.</p>
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13 pages, 2136 KiB  
Article
Thermosensitive In Situ Gelling Poloxamers/Hyaluronic Acid Gels for Hydrocortisone Ocular Delivery
by Fabrizio Villapiano, Teresa Silvestri, Camilla Lo Gatto, Danilo Aleo, Virginia Campani, Sossio Fabio Graziano, Concetta Giancola, Federica D’Aria, Giuseppe De Rosa, Marco Biondi and Laura Mayol
Gels 2024, 10(3), 193; https://doi.org/10.3390/gels10030193 - 12 Mar 2024
Viewed by 1919
Abstract
This study endeavored to overcome the physiological barriers hindering optimal bioavailability in ophthalmic therapeutics by devising drug delivery platforms that allow therapeutically effective drug concentrations in ocular tissues for prolonged times. Thermosensitive drug delivery platforms were formulated by blending poloxamers (F68 and F127) [...] Read more.
This study endeavored to overcome the physiological barriers hindering optimal bioavailability in ophthalmic therapeutics by devising drug delivery platforms that allow therapeutically effective drug concentrations in ocular tissues for prolonged times. Thermosensitive drug delivery platforms were formulated by blending poloxamers (F68 and F127) with low-molecular-weight hyaluronic acid (HA) in various concentrations and loaded with hydrocortisone (HC). Among the formulations examined, only three were deemed suitable based on their desirable gelling properties at a temperature close to the eye’s surface conditions while also ensuring minimal gelation time for swift ocular application. Rheological analyses unveiled the ability of the formulations to develop gels at suitable temperatures, elucidating the gel-like characteristics around the physiological temperature essential for sustained drug release. The differential scanning calorimetry findings elucidated intricate hydrogel–water interactions, indicating that HA affects the water–polymer interactions within the gel by increasing the platform hydrophilicity. Also, in vitro drug release studies demonstrated significant hydrocortisone release within 8 h, governed by an anomalous transport mechanism, prompting further investigation for optimized release kinetics. The produced platforms offer promising prospects for efficacious ocular drug delivery, addressing pivotal challenges in ocular therapeutics and heralding future advancements in the domain. Full article
(This article belongs to the Special Issue Gels in Medicine and Pharmacological Therapies (2nd Edition))
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<p>Fourier transform infrared spectra (FTIR) of raw materials and selected hydrogels (<b>left</b>). Scanning electron microscopy (SEM) micrographs of freeze-dried hydrogels with (<b>right</b>) or without HC (<b>left</b>).</p>
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<p>Mechanical spectra of unloaded pol/HA platforms at three different temperatures: 4 °C (<b>A</b>), 25 °C (<b>B</b>) and 37 °C (<b>C</b>).</p>
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<p>Elastic and viscous moduli as a function of temperature, at a fixed frequency of 1 Hz for formulations P3/0.1, P3/1 and P4/0.1, unloaded (<b>left</b>) and HC loaded (<b>right</b>). The error bars are omitted for clarity purpose.</p>
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<p>Thermograms of (<b>A</b>) P3/0.1; (<b>B</b>) P3/1; (<b>C</b>) P4/0.1.</p>
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<p>Swelling ratio of dried gel formulations.</p>
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<p>Hydrocortisone release curves from pol/HA gels.</p>
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16 pages, 4056 KiB  
Article
Chitosan–Silica Composite Aerogel for the Adsorption of Cupric Ions
by João P. Vareda, Pedro M. C. Matias, José A. Paixão, Dina Murtinho, Artur J. M. Valente and Luisa Durães
Gels 2024, 10(3), 192; https://doi.org/10.3390/gels10030192 - 11 Mar 2024
Cited by 3 | Viewed by 1706
Abstract
A chitosan–silica hybrid aerogel was synthesized and presented as a potential adsorbent for the purification of cupric ion-contaminated media. The combination of the organic polymer (chitosan), which can be obtained from fishery wastes, with silica produced a mostly macroporous material with an average [...] Read more.
A chitosan–silica hybrid aerogel was synthesized and presented as a potential adsorbent for the purification of cupric ion-contaminated media. The combination of the organic polymer (chitosan), which can be obtained from fishery wastes, with silica produced a mostly macroporous material with an average pore diameter of 33 µm. The obtained aerogel was extremely light (56 kg m−3), porous (96% porosity, 17 cm3 g−1 pore volume), and presented a Brunauer–Emmett–Teller surface area (SBET) of 2.05 m2 g−1. The effects of solution pH, aerogel and Cu(II) concentration, contact time, and counterion on cupric removal with the aerogel were studied. Results showed that the initial pH of the cation-containing aqueous solution had very little influence on the removal performance of this aerogel. According to Langmuir isotherm, this material can remove a maximum amount of ca. 40 mg of cupric ions per gram and the kinetic data showed that the surface reaction was the rate-limiting step and equilibrium was quickly reached (in less than one hour). Thus, the approach developed in this study enabled the recovery of waste for the preparation of a novel material, which can be efficiently reused in a new application, namely water remediation. Full article
(This article belongs to the Special Issue Gels for Water Treatment)
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<p>Aspect (<b>a</b>), and microstructure of the chitosan–silica aerogel at ×100 (<b>b</b>) and ×5 K (<b>c</b>) magnification. Inset detailing the sample’s microstructure across the height of the solid obtained at ×25 K magnification.</p>
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<p>FTIR spectra of chitosan–silica aerogel (solid blue line) and chitosan (solid black line) (<b>a</b>); thermogram (weight, %, solid blue line) and respective derivative (dTG, dotted blue line) (<b>b</b>); and XRD pattern (<b>c</b>) of the chitosan–silica aerogel.</p>
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<p>Cupric ion removal with the chitosan–silica aerogel from nitrate and sulfate salt solutions at pH = 4 (<b>a</b>) and pH = 5 (<b>b</b>), and cupric ions speciation diagram in the Cu<sup>2+</sup>-OH system (<b>c</b>).</p>
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<p>Kinetics (<b>a</b>) and isotherms (<b>b</b>) of cupric sorption. For the kinetics, a starting copper concentration of 100 mg L<sup>−1</sup> was used.</p>
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<p>Microstructure at 100× (<b>a</b>) and 2.5 K× (<b>b</b>), and EDX spectrum (<b>c</b>) of the copper-loaded chitosan–silica aerogel.</p>
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17 pages, 32541 KiB  
Article
Study on Carbonation of Porcine Blood Hydrogel in the Composite Mortar of Ancient Chinese Architectural Painting
by Cong Cheng, Wenhua Ma, Rui Chen, Yeting Zhu, Lizhen Zheng, Wei Li and Daodao Hu
Gels 2024, 10(3), 191; https://doi.org/10.3390/gels10030191 - 9 Mar 2024
Viewed by 1330
Abstract
In the ancient Chinese recipe for composite mortar used in the construction of ground layers for architectural painting, the mixture of porcine blood and lime water is one of the constituent materials. Herein, according to the traditional recipe, the interaction between porcine blood [...] Read more.
In the ancient Chinese recipe for composite mortar used in the construction of ground layers for architectural painting, the mixture of porcine blood and lime water is one of the constituent materials. Herein, according to the traditional recipe, the interaction between porcine blood and lime water was systematically and deeply investigated. The experimental investigation demonstrated that porcine blood mixed with lime water at the ratio found in the recipe can form a hydrogel with a hydrophobic surface. During air-drying, the lime water in porcine blood hydrogel can react with CO2 to form calcium carbonate. The crystal morphology of the formed calcium carbonate depends on the surrounding micro-environment of calcium ions in the porcine blood hydrogel. The formed morphology of calcium carbonate includes small calcite crystallites, small graininess calcite crystals with round features, calcite aggregates with layered ladder-like structures, and amorphous calcium carbonate (ACC). Interestingly, the calcium carbonate formed in the inner part of the porcine blood hydrogel exhibits lamellar distribution due to a Liesegang pattern formation. Based on the findings that the porcine blood hydrogel has surface hydrophobicity and brittleness, it can be predicted that in the preparation process of composite mortar for ancient building color painting base course, porcine blood used in the form of a hydrogel is not only easier to be dispersed in hydrophobic tung oil than in liquid porcine blood but also the affinity between porcine blood gel and tung oil is enhanced. As constituent material dispersed in the composite mortar, the layered distribution of calcium carbonate in the porcine blood hydrogel may presumably be beneficial to reduce the internal stress of the composite mortar material. Full article
(This article belongs to the Special Issue Advance in Composite Gels (2nd Edition))
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<p>Photos of porcine blood mixed with different additives after standing at the given condition (25–28 °C, 40–60% RH) for different times: (<b>A</b>) CaCl<sub>2</sub>, (<b>B</b>) NaOH, (<b>C</b>) mixture of CaCl<sub>2</sub> and NaOH, and (<b>D</b>) lime water.</p>
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<p>Contact angle images for water droplets on the surfaces of various samples. The powders from the products formed by the mixtures of porcine blood and different additives: (<b>A</b>) CaCl<sub>2</sub>, (<b>B</b>) NaOH, (<b>C</b>) mixture of CaCl<sub>2</sub> and NaOH, and (<b>D</b>) lime water.</p>
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<p>Cross-sectional SEM images (×100, ×1K) of the porcine blood hydrogel after freeze-drying at different times.</p>
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<p>Illustrations of the formation of calcite on the surface of the porcine blood hydrogel. (<b>A</b>) Photos of the porcine blood hydrogel after standing for different times. (<b>B</b>) XRD pattern of the surface substance of the dried porcine blood hydrogel. (<b>C</b>) Surface morphology (×1.5K) (d, e, f corresponding position in (<b>C</b>)) and (<b>D</b>) weightlessness curve of the porcine blood hydrogel after standing for 5 days.</p>
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<p>Diagram illustrating the different morphologies of calcite formed in different regions of the surface of the porcine blood hydrogel.</p>
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<p>Variation in the XRD patterns of the porcine blood hydrogel after standing exposed to the air for different times.</p>
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<p>SEM images (×100, ×1K) of the porcine blood hydrogels air-dried (<b>left</b> column) in a CO<sub>2</sub>-free atmosphere (<b>right</b> column). The surface morphology of the sample before (<b>A</b>,<b>A’</b>) and after (<b>B</b>,<b>B’</b>) saturation with water. The cross-sectional morphology of the sample before (<b>C</b>,<b>C’</b>) and after (<b>D</b>,<b>D’</b>) saturation with water.</p>
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<p>Surface (<b>A</b>–<b>C</b>) and cross-sectional (<b>D</b>–<b>F</b>) SEM images (×100, ×1K) of the air-dried porcine blood hydrogel before (<b>A</b>,<b>D</b>) and after (<b>B</b>,<b>C</b>,<b>E</b>,<b>F</b>) acid etching. The air-dried porcine blood hydrogel soaked with hydrochloric acid for 4 h.</p>
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<p>SEM images (×100, ×1K) and EDS spectrum as well as the corresponding Ca element mapping of the air-dried porcine blood hydrogel. a, b for the corresponding amplification in A.</p>
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<p>Cross-sectional SEM images (×100, ×200, ×1K) of the air-dried porcine blood hydrogel after standing in a humid atmosphere (<b>A</b>–<b>C</b>). (<b>B</b>,<b>C</b>) illustrate a local enlargement of (<b>A</b>,<b>B</b>), respectively; (<b>D</b>) illustrates the peeled lamellar surface; and (<b>E</b>) illustrates the local enlargement of (<b>D</b>).</p>
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<p>Diagram illustrating the formation principle of Liesegang patterns.</p>
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<p>Diagram illustrating the formation principle of the lamellar patterns of calcium carbonate formed in the porcine blood hydrogel.</p>
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29 pages, 5054 KiB  
Review
Injectable Hydrogels for Nervous Tissue Repair—A Brief Review
by Gladys Arline Politrón-Zepeda, Gabriela Fletes-Vargas and Rogelio Rodríguez-Rodríguez
Gels 2024, 10(3), 190; https://doi.org/10.3390/gels10030190 - 9 Mar 2024
Cited by 6 | Viewed by 2755
Abstract
The repair of nervous tissue is a critical research field in tissue engineering because of the degenerative process in the injured nervous system. In this review, we summarize the progress of injectable hydrogels using in vitro and in vivo studies for the regeneration [...] Read more.
The repair of nervous tissue is a critical research field in tissue engineering because of the degenerative process in the injured nervous system. In this review, we summarize the progress of injectable hydrogels using in vitro and in vivo studies for the regeneration and repair of nervous tissue. Traditional treatments have not been favorable for patients, as they are invasive and inefficient; therefore, injectable hydrogels are promising for the treatment of damaged tissue. This review will contribute to a better understanding of injectable hydrogels as potential scaffolds and drug delivery system for neural tissue engineering applications. Full article
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<p>Porous microstructure of the hydrogels in cell behavior. Reprinted from Ma et al. [<a href="#B21-gels-10-00190" class="html-bibr">21</a>].</p>
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<p>Structure of hydrogels where (<b>A</b>) ideal network, (<b>B</b>) entanglements, and (<b>C</b>) hydrogel network micro-structures. Reprinted from Solbu et al. [<a href="#B75-gels-10-00190" class="html-bibr">75</a>].</p>
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<p>Live–dead assay of hyaluronic acid (HA)–puramatrix (RADA) hydrogels at 7 days where (<b>a</b>) HA-1, (<b>b</b>) HA-1-RADA-1, (<b>c</b>) HA-1-RADA-5 and (<b>d</b>) HA-1-RADA-10. The green color indicates viable cells and the red color indicates dead cells. Reprinted from Abbasi Aval et al. [<a href="#B101-gels-10-00190" class="html-bibr">101</a>].</p>
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<p>(<b>a</b>) Scanning electron microscopy (SEM) images, (<b>b</b>) swelling ratio (%), and (<b>c</b>) enzymatic degradation (%) of chitosan/β-GP hydrogels. Data was analyzed by one-way ANOVA and Tukey’s test where <span class="html-italic">p</span> ≤ 0.01 **, <span class="html-italic">p</span> ≤ 0.001 ***, and <span class="html-italic">p</span> ≤ 0.001 ****. Reprinted from Bhuiyan et al. [<a href="#B103-gels-10-00190" class="html-bibr">103</a>], copyright 2023, with permission of Elsevier.</p>
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<p>(<b>A</b>) Cross-sections of regenerated nerves taken from nerve conduits implanted in rats after 1 and 3 months. Red arrows show nerve fibers. (<b>a</b>–<b>d</b>): Autograft group; (<b>e</b>–<b>h</b>): Poly(D, L-lactic acid)/β-tricalcium phosphate nerve conduits group; (<b>i</b>–<b>l</b>): Poly(D, L-lactic acid)/β-tricalcium phosphate nerve conduits/hyaluronic acid-chitosan group; (<b>m</b>–<b>p</b>): Poly(D, L-lactic acid)/β-tricalcium phosphate nerve conduits/hyaluronic acid-chitosan/ nerve growth factor group. (<b>B</b>) Axon diameters of regenerated myelinated nerve fibers. (<b>C</b>) Thicknesses of regenerated myelinated sheaths. (<b>D</b>) Diameters of regenerated nerve fibers. (<b>E</b>) Densities of regenerated myelinated nerve fibers. Data was analyzed by one-way ANOVA where <span class="html-italic">p</span> &lt; 0.05 *. Reprinted from Xu et al. [<a href="#B109-gels-10-00190" class="html-bibr">109</a>], copyright 2022, with permission of Elsevier.</p>
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<p>Middle cross-section of regenerated nerves at day 28 post-surgery. (<b>A</b>) Hematoxylin and eosin (HE) staining, (<b>B</b>) Luxol fast blue staining, (<b>C</b>) immunofluorescence staining of S100 and neurofilament-200, (<b>D</b>) immunofluorescence staining of myelin basic protein and beta III Tubulin, (<b>E</b>) TEM images of transverse sections of regenerated nerve fibers, (<b>F</b>) myelinated axons from TEM observation, (<b>G</b>) myelin thickness from TEM observation, and (<b>H</b>) axon-to-fiber diameter of regenerated nerves from TEM observation. <span class="html-italic">p</span> &lt; 0.01 **; <span class="html-italic">p</span> &lt; 0.001 ***. Reprinted from Xu et al. [<a href="#B110-gels-10-00190" class="html-bibr">110</a>], copyright 2023, with permission of Elsevier.</p>
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<p>Hydrogel implantation promotes nerve regeneration. (<b>A</b>) Immunohistofluorescence images of longitudinal spinal cord sections from rats. (<b>B</b>) Quantitative analysis of Nestin, (<b>C</b>) Quantitative analysis of MAP2, (<b>D</b>) Protein expression of VEGF and CD31 of different groups and (<b>E</b>) Scheme of hydrogel-releasing drug and conductive black phosphorus promoting vascular regeneration. * <span class="html-italic">p</span> &lt; 0.05, *** <span class="html-italic">p</span> &lt; 0.001, **** <span class="html-italic">p</span> &lt; 0.0001. Reprinted from Liu et al. [<a href="#B111-gels-10-00190" class="html-bibr">111</a>], copyright 2024, with permission of Elsevier.</p>
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<p>Promotion of angiogenesis process by hyaluronic acid-based hydrogels after spinal cord injury. (<b>a</b>) Laminectomy and injected the hydrogel in the lesion area, (<b>b</b>) behavior assay of BBB scores, (<b>c</b>) spinal sections staining CD31 (red) and DAPI (blue) from spinal cord injury and hydrogel-treated rats at 56 days post-injury, (<b>d</b>) luxol fast blue staining of longitudinal sections at 56 days post-injury, and (<b>e</b>) quantification of luxol fast blue staining ratio of the total spinal cord. * <span class="html-italic">p</span> &lt; 0.05 compared with Sham and # <span class="html-italic">p</span> &lt; 0.05 compared with spinal cord injury. Reprinted from Li et al. [<a href="#B124-gels-10-00190" class="html-bibr">124</a>], copyright 2022, with permission of Elsevier.</p>
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<p>Recovery of motor function after spinal cord injury in rats. (<b>A</b>) Rat left spinal cord hemisection injury model, (<b>B</b>) Left hindlimb locomotor recovery by the BBB scale. Rats treated with the GMEB hydrogel, (<b>C</b>) Footprints used to analyze the recovery of hindlimb motor function, (<b>D</b>) Quantification of the stride length, (<b>E</b>) print area, (<b>F</b>) and mean intensity (<b>F</b>) of the left hindlimb in each group 4 weeks after operation. <sup>+</sup>, * <span class="html-italic">p</span> &lt; 0.05, <sup>++</sup>, ##, ** <span class="html-italic">p</span> &lt; 0.01, <sup>+++</sup>, *** <span class="html-italic">p</span> &lt; 0.001, ####, **** <span class="html-italic">p</span> &lt; 0.0001, ns = not significant. Reprinted from Wang et al. [<a href="#B131-gels-10-00190" class="html-bibr">131</a>], copyright 2023, with permission of Elsevier.</p>
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<p>Recovery of motor function after spinal cord injury in rats. (<b>A</b>) Rat left spinal cord hemisection injury model, (<b>B</b>) Left hindlimb locomotor recovery by the BBB scale. Rats treated with the GMEB hydrogel, (<b>C</b>) Footprints used to analyze the recovery of hindlimb motor function, (<b>D</b>) Quantification of the stride length, (<b>E</b>) print area, (<b>F</b>) and mean intensity (<b>F</b>) of the left hindlimb in each group 4 weeks after operation. <sup>+</sup>, * <span class="html-italic">p</span> &lt; 0.05, <sup>++</sup>, ##, ** <span class="html-italic">p</span> &lt; 0.01, <sup>+++</sup>, *** <span class="html-italic">p</span> &lt; 0.001, ####, **** <span class="html-italic">p</span> &lt; 0.0001, ns = not significant. Reprinted from Wang et al. [<a href="#B131-gels-10-00190" class="html-bibr">131</a>], copyright 2023, with permission of Elsevier.</p>
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<p>Remyelination and functional recovery 2 months after implantation of hydrogel loaded with curcumin following spinal cord injury. (<b>A</b>) Remyelination in the graft, (<b>a</b>) nerve fibers, (<b>B</b>), (<b>b</b>) transversal section in the lesion, (<b>C</b>) regenerated tissues in cross sections of the lesion, (<b>F</b>) BBB open-field walking scale of rats, (<b>D</b>) amplitude and (<b>E</b>) latency of motor evoked potential. * <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; 0.001. Reprinted from Luo et al. [<a href="#B134-gels-10-00190" class="html-bibr">134</a>].</p>
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<p>Neurogenesis and brain tissue remodeling after treatment for 21 days. (<b>A</b>) Immunofluorescence staining of NeuN and Ki67, (<b>B</b>) western blot and (<b>C</b>) relative expression of β-III tubulin, NeuN, NSE and NFL, (<b>D</b>) H&amp;E staining and imaging of TBI mice brain, (<b>E</b>) brain lesion volume. *, # <span class="html-italic">p</span> &lt; 0.05. Reprinted from Zhang et al. [<a href="#B146-gels-10-00190" class="html-bibr">146</a>].</p>
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14 pages, 4068 KiB  
Article
Spray-Dried Chitosan Hydrogel Particles as a Potential Delivery System for Benzydamine Hydrochloride
by Sofia Milenkova, Rita Ambrus, Mahwash Mukhtar, Bissera Pilicheva and Maria Marudova
Gels 2024, 10(3), 189; https://doi.org/10.3390/gels10030189 - 8 Mar 2024
Cited by 1 | Viewed by 1746
Abstract
Chitosan, being a biocompatible and mucoadhesive polysaccharide, is one of the most preferred hydrogel-forming materials for drug delivery. The objectives of the present study are to obtain spray-dried microparticles based on low-molecular-weight chitosan and study their potential application as cargo systems for the [...] Read more.
Chitosan, being a biocompatible and mucoadhesive polysaccharide, is one of the most preferred hydrogel-forming materials for drug delivery. The objectives of the present study are to obtain spray-dried microparticles based on low-molecular-weight chitosan and study their potential application as cargo systems for the orally active drug benzydamine hydrochloride. Three types of particles are obtained: raw chitosan particles (at three different concentrations), cross-linked with sodium tripolyphosphate (NaTPP) particles (at three different chitosan:NaTPP ratios), and particles coated with mannitol (at three different chitosan:mannitol ratios), all of them in the size range between 1 and 10 µm. Based on the loading efficiency and the yields of the formulated hydrogel particles, one model of each type is chosen for further investigation of the effect of the cross-linker or the excipient on the properties of the gel structures. The morphology of both empty and benzydamine hydrochloride-loaded chitosan particles was examined by scanning electron microscopy, and it was quite regular and spherical. Interactions and composition in the samples are investigated by Fourier-transformed infrared spectroscopy. The thermal stability and phase state of the drug and drug-containing polymer matrixes were tested by differential scanning calorimetry and X-ray powdered diffraction, revealing that the drug underwent a phase transition. A drug release kinetics study of the chosen gel-based structures in simulated saliva buffer (pH = 6.8) and mathematical modeling of the process were performed, indicating the Weibull model as the most appropriate one. Full article
(This article belongs to the Special Issue Gel-Based Materials: Preparations and Characterization (2nd Edition))
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<p>Chitosan structure, properties, and potential biomedical applications.</p>
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<p>SEM images of (<b>a</b>) C2, (<b>b</b>) CN2, (<b>c</b>) CM2, (<b>d</b>) BC2, (<b>e</b>) BCN2, and (<b>f</b>) BCM2 (from left top to right down, magnification: 2500×).</p>
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<p>(<b>a</b>) FTIR spectra of blank particles, (<b>b</b>) FTIR spectra of BHCl-loaded particles.</p>
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<p>(<b>a</b>) DSC thermograms of empty particles, (<b>b</b>) drug-loaded particles and the drug itself.</p>
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<p>(<b>a</b>) Diffractograms of BHCl, BC2, BCN2, BCM2, C2, CN2, and CM2 (from top to down). (<b>b</b>) Diffractogram of different mannitol polymorphs and CM2.</p>
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<p>Drug release kinetics (points) and the Weibull model predicted values (lines).</p>
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46 pages, 5115 KiB  
Review
Hydrogels in Cutaneous Wound Healing: Insights into Characterization, Properties, Formulation and Therapeutic Potential
by Mariana Ribeiro, Marco Simões, Carla Vitorino and Filipa Mascarenhas-Melo
Gels 2024, 10(3), 188; https://doi.org/10.3390/gels10030188 - 8 Mar 2024
Cited by 8 | Viewed by 4472
Abstract
Hydrogels are polymeric materials that possess a set of characteristics meeting various requirements of an ideal wound dressing, making them promising for wound care. These features include, among others, the ability to absorb and retain large amounts of water and the capacity to [...] Read more.
Hydrogels are polymeric materials that possess a set of characteristics meeting various requirements of an ideal wound dressing, making them promising for wound care. These features include, among others, the ability to absorb and retain large amounts of water and the capacity to closely mimic native structures, such as the extracellular matrix, facilitating various cellular processes like proliferation and differentiation. The polymers used in hydrogel formulations exhibit a broad spectrum of properties, allowing them to be classified into two main categories: natural polymers like collagen and chitosan, and synthetic polymers such as polyurethane and polyethylene glycol. This review offers a comprehensive overview and critical analysis of the key polymers that can constitute hydrogels, beginning with a brief contextualization of the polymers. It delves into their function, origin, and chemical structure, highlighting key sources of extraction and obtaining. Additionally, this review encompasses the main intrinsic properties of these polymers and their roles in the wound healing process, accompanied, whenever available, by explanations of the underlying mechanisms of action. It also addresses limitations and describes some studies on the effectiveness of isolated polymers in promoting skin regeneration and wound healing. Subsequently, we briefly discuss some application strategies of hydrogels derived from their intrinsic potential to promote the wound healing process. This can be achieved due to their role in the stimulation of angiogenesis, for example, or through the incorporation of substances like growth factors or drugs, such as antimicrobials, imparting new properties to the hydrogels. In addition to substance incorporation, the potential of hydrogels is also related to their ability to serve as a three-dimensional matrix for cell culture, whether it involves loading cells into the hydrogel or recruiting cells to the wound site, where they proliferate on the scaffold to form new tissue. The latter strategy presupposes the incorporation of biosensors into the hydrogel for real-time monitoring of wound conditions, such as temperature and pH. Future prospects are then ultimately addressed. As far as we are aware, this manuscript represents the first comprehensive approach that brings together and critically analyzes fundamental aspects of both natural and synthetic polymers constituting hydrogels in the context of cutaneous wound healing. It will serve as a foundational point for future studies, aiming to contribute to the development of an effective and environmentally friendly dressing for wounds. Full article
(This article belongs to the Special Issue Hydrogel-Based Novel Biomaterials: Achievements and Prospects)
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<p>Representation of the chemical structures of some natural polymers classified into proteins (collagen, gelatin, and silk fibroin) and polysaccharides (alginate, hyaluronic acid, cellulose, dextran, and chitosan).</p>
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<p>Synthetic polymers and their respective chemical structures.</p>
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<p>Representation of some of the applications of hydrogels as wound dressings: intrinsic capacity to stimulate healing; drug delivery systems or transporters of other substances; support for cell growth; real-time monitoring of the state of wounds through the incorporation of biosensors.</p>
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<p>(<b>A</b>) Comparison of wound size over 21 days after treatment with hydrogels. (<b>B</b>) In vivo observation of burn wound healing over 21 days. (<b>C</b>) In vivo study on EGF delivery and wound healing promotion. (<b>D</b>) Schematic representation of EGF loaded in carboxymethyl chitosan and alginate hydrogel. (<b>E</b>) In vitro inhibition of <span class="html-italic">S. aureus</span> and <span class="html-italic">P. aeruginosa</span> growth after loading ciprofloxacin in SF hydrogel. (<b>F</b>) In vivo study on partial-thickness burns treatment with hydrogels loaded with keratinocytes and fibroblasts (* means significant difference (<span class="html-italic">p</span> &lt; 0.05) between the groups) (<b>G</b>) Schematic representation of the operation of a hydrogel incorporated with poly (N-isopropyl acrylamide) stimuli-responsive particles. Adapted from: [<a href="#B8-gels-10-00188" class="html-bibr">8</a>,<a href="#B109-gels-10-00188" class="html-bibr">109</a>,<a href="#B276-gels-10-00188" class="html-bibr">276</a>,<a href="#B277-gels-10-00188" class="html-bibr">277</a>,<a href="#B278-gels-10-00188" class="html-bibr">278</a>].</p>
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24 pages, 5683 KiB  
Review
Three-Dimensional Printing of Hydrogels for Flexible Sensors: A Review
by Suhail Ayoub Khan, Hamza Ahmad, Guoyin Zhu, Huan Pang and Yizhou Zhang
Gels 2024, 10(3), 187; https://doi.org/10.3390/gels10030187 - 8 Mar 2024
Cited by 3 | Viewed by 2253
Abstract
The remarkable flexibility and heightened sensitivity of flexible sensors have drawn significant attention, setting them apart from traditional sensor technology. Within this domain, hydrogels—3D crosslinked networks of hydrophilic polymers—emerge as a leading material for the new generation of flexible sensors, thanks to their [...] Read more.
The remarkable flexibility and heightened sensitivity of flexible sensors have drawn significant attention, setting them apart from traditional sensor technology. Within this domain, hydrogels—3D crosslinked networks of hydrophilic polymers—emerge as a leading material for the new generation of flexible sensors, thanks to their unique material properties. These include structural versatility, which imparts traits like adhesiveness and self-healing capabilities. Traditional templating-based methods fall short of tailor-made applications in crafting flexible sensors. In contrast, 3D printing technology stands out with its superior fabrication precision, cost-effectiveness, and satisfactory production efficiency, making it a more suitable approach than templating-based strategies. This review spotlights the latest hydrogel-based flexible sensors developed through 3D printing. It begins by categorizing hydrogels and outlining various 3D-printing techniques. It then focuses on a range of flexible sensors—including those for strain, pressure, pH, temperature, and biosensors—detailing their fabrication methods and applications. Furthermore, it explores the sensing mechanisms and concludes with an analysis of existing challenges and prospects for future research breakthroughs in this field. Full article
(This article belongs to the Special Issue Gels for Flexible Electronics and Energy Devices)
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<p>Representation of 3D printing by various approaches, inkjet (<b>a</b>) reproduced with permission [<a href="#B32-gels-10-00187" class="html-bibr">32</a>]. Copyright © 2020 American Chemical Society, Washington, DC. Direct ink (<b>b</b>) reproduced with permission [<a href="#B40-gels-10-00187" class="html-bibr">40</a>]. Copyright © 2019 Royal Society of Chemistry, London. Stereolithography (<b>c</b>) reproduced with permission [<a href="#B45-gels-10-00187" class="html-bibr">45</a>]. Copyright © 2014 Royal Society of Chemistry. Digital light processing (<b>d</b>) reproduced with permission [<a href="#B48-gels-10-00187" class="html-bibr">48</a>]. Copyright © 2023 American Chemical Society, and two-photon polymerization (<b>e</b>) reproduced with permission [<a href="#B52-gels-10-00187" class="html-bibr">52</a>]. Copyright © 2023 WILEY-VCH Verlag GmbH &amp; Co. KGaA, Weinheim, Germany.</p>
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<p>Schematic representation of ECHs using in situ polymerization, in which metal ions are reduced to metal nanoparticles (<b>a</b>), reproduced with permission [<a href="#B63-gels-10-00187" class="html-bibr">63</a>]. Copyright © 2011 WILEY-VCH Verlag GmbH &amp; Co. KGaA, Weinheim. Fabrication of conductive CNT-based hydrogels (<b>b</b>), reproduced with permission [<a href="#B66-gels-10-00187" class="html-bibr">66</a>]. Copyright © 2023 Elsevier Ltd, Amsterdam. Illustration of polypyrrole-based composited conductive hydrogel, in situ polymerization, and chain entanglement (<b>c</b>) reproduced with permission [<a href="#B73-gels-10-00187" class="html-bibr">73</a>]. Copyright © 2018, American Chemical Society. Schematic representation of ICHs, possible mechanism, and redox process to endorse free radical polymerization (<b>d</b>) reproduced with permission [<a href="#B74-gels-10-00187" class="html-bibr">74</a>]. Copyright © 2022 Elsevier B.V.</p>
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<p>Schematic representation of sensing mechanism of hydrogel-based sensors, piezoresistive (<b>a</b>), capacitive (<b>b</b>), piezoelectric (<b>c</b>), and triboelectric (<b>d</b>). Reproduced with permission [<a href="#B79-gels-10-00187" class="html-bibr">79</a>]. Copyright © 2023 WILEY-VCH Verlag GmbH &amp; Co. KGaA, Weinheim.</p>
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<p>Digital-light-processing approach for the fabrication of hydrogel strain sensor, kinetics of the ACMO slurry (<b>a</b>), digital photographs of 3D structures, representation of ion sputtering system (<b>b</b>), and electrical conductivity of poly (ACMO) components with various sputtering times (<b>c</b>). Reproduced with permission [<a href="#B91-gels-10-00187" class="html-bibr">91</a>]. Copyright © 2022 Published by Elsevier Ltd.</p>
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<p>Real-time variations in relative resistance during external compression, stretching, deep breathing, finger flexion, wrist movements, and changes in elbow motion using the B-PVA/kC<sub>1</sub> hydrogel sensor. Reproduced with permission [<a href="#B93-gels-10-00187" class="html-bibr">93</a>]. Copyright © 2023 Elsevier B.V.</p>
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<p>Electrical conductivity of Pul-SH/PDA/MoS<sub>2</sub> hydrogel sensor and its utility as an electronic skin for strain and pressure sensing (<b>a</b>). Electrical impedance spectroscopy plots (<b>b</b>). Relative change in resistance values (ΔR/R0) of the hydrogel Pul-SH/PDA/MoS<sub>2</sub> in reaction to external force, strain, and pressure variations and numerous cycles of compression (25 cycles), showing linearity in response (<b>c</b>). Vibrations recorded from the two different acts (<b>d</b>). Reproduced with permission [<a href="#B95-gels-10-00187" class="html-bibr">95</a>]. Copyright © 2024 Wiley-VCH GmbH.</p>
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<p>Shear rate as a function of viscosity (<b>a</b>). Strain sweep at a fixed frequency of 10 rad⋅s<sup>–1</sup> (<b>b</b>). Oscillatory frequency sweep at a fixed shear strain of 0.1%. G′ (<b>c</b>). Reproduced with permission [<a href="#B98-gels-10-00187" class="html-bibr">98</a>]. Copyright © 2022 Elsevier B.V.</p>
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<p>Schematic representation of GOx-loaded H/G4–PANI hydrogel sensor along with its optical images (<b>a</b>), cyclic voltammograms, UV–Vis absorption spectra, and potential and chronoamperometry curves (<b>b</b>). Reproduced with permission [<a href="#B102-gels-10-00187" class="html-bibr">102</a>]. Copyright © 2018 WILEY-VCH Verlag GmbH &amp; Co. KGaA, Weinheim.</p>
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<p>Sensory operations (<b>a</b>). Resistance alteration ratio of hydrogel sensor during stretching (<b>b</b>). Response time at 1% strain (<b>c</b>). Resistance alteration ratios under various strains (<b>d</b>). Compressive-pressure-sensing hydrogel sensor (<b>e</b>). At 600 Pa, the response time (<b>f</b>). Resistance alteration ratio at different compressive stresses (<b>g</b>). Resistance alteration ratio changes over 600 cycles (<b>h</b>). Resistance alteration when attached to human finger (<b>i</b>) and neck (<b>j</b>). Reproduced with permission [<a href="#B105-gels-10-00187" class="html-bibr">105</a>]. Copyright © 2023 Royal Society of Chemistry.</p>
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<p>The electrical response of the hydrogel sensor to the pH change from neutral to pH 3 (<b>a</b>), the correlation between resistance and pH of the solution for the hydrogel sensor (<b>b</b>), The arrows in (<b>a</b>,<b>b</b>) indicate the same data points. Schematic representation of the influence of pH on the molecular structure of hydrogel sensor (<b>c</b>). Reproduced with permission [<a href="#B108-gels-10-00187" class="html-bibr">108</a>]. Copyright © 2018 WILEY-VCH Verlag GmbH &amp; Co. KGaA, Weinheim.</p>
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<p>Photographs representing the thermo-responsive ionic skin attached to a prosthetic finger (<b>a</b>) and a human hand (<b>b</b>). Plots illustrating different grid structures at different temperatures (<b>c</b>). Reproduced with permission [<a href="#B113-gels-10-00187" class="html-bibr">113</a>]. Copyright © 2017 Royal Society of Chemistry.</p>
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15 pages, 4131 KiB  
Article
A Fully Integrated Microfluidic Device with Immobilized Dyes for Simultaneous Detection of Cell-Free DNA and Histones from Plasma Using Dehydrated Agarose Gates
by Shadi Shahriari and P. Ravi Selvaganapathy
Gels 2024, 10(3), 186; https://doi.org/10.3390/gels10030186 - 8 Mar 2024
Viewed by 1640
Abstract
Sepsis, a life-threatening condition resulting from a failing host response to infection, causes millions of deaths annually, necessitating rapid and simple prognostic assessments. A variety of genomic and proteomic biomarkers have been developed for sepsis. For example, it has been shown that the [...] Read more.
Sepsis, a life-threatening condition resulting from a failing host response to infection, causes millions of deaths annually, necessitating rapid and simple prognostic assessments. A variety of genomic and proteomic biomarkers have been developed for sepsis. For example, it has been shown that the level of plasma cell-free DNA (cfDNA) and circulating histones increases considerably during sepsis, and they are linked with sepsis severity and mortality. Developing a diagnostic tool that is capable of assessing such diverse biomarkers is challenging as the detection methodology is quite different for each. Here, a fully integrated microfluidic device capable of detecting a genomic biomarker (cfDNA) and a proteomic biomarker (total circulating histones) using a common detection platform has been demonstrated. The microfluidic device utilizes dehydrated agarose gates loaded with pH-specific agarose to electrophoretically trap cfDNA and histones at their respective isoelectric points. It also incorporates fluorescent dyes within the device, eliminating the need for off-chip sample preparation and allowing the direct testing of plasma samples without the need for labeling DNA and histones with fluorescent dyes beforehand. Xurography, which is a low-cost and rapid method for fabrication of microfluidics, is used in all the fabrication steps. Experimental results demonstrate the effective accumulation and separation of cfDNA and histones in the agarose gates in a total processing time of 20 min, employing 10 and 30 Volts for cfDNA and histone accumulation and detection, respectively. The device can potentially be used to distinguish between the survivors and non-survivors of sepsis. The integration of the detection of both biomarkers into a single device and dye immobilization enhances its clinical utility for rapid point-of-care assessment of sepsis prognosis. Full article
(This article belongs to the Special Issue Recent Progress of Hydrogel Sensors and Biosensors)
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<p>Working principle and steps of the device. (<b>a</b>) Filling the top channels with the corresponding buffers for agarose rehydration. (<b>b</b>) Filling the sample channels and waiting for labelling DNA and proteins with their corresponding dyes. (<b>c</b>) DNA accumulation by applying 10 V to the channels connected to agarose gate with pH 8.5. (<b>d</b>) Histone separation and detection by applying 30 V to the channels connected to the agarose gate with pH 11.</p>
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<p>Tagging and concentration of (<b>a</b>) histones and (<b>b</b>) 150 bp DNA in the devices with integrated dried fluorescent dyes.</p>
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<p>Trapping histones in the presence of 40 mg/mL BSA in the devices with immobilized Qubit. (<b>a</b>) Images captured at the time of filling the sample channel, at the time of applying voltage (0 min), and after 6 min for different samples. (<b>b</b>) Fluorescence intensity for each concentration of histone in the sample containing BSA (N = 3).</p>
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<p>Accumulation of DNA in the presence of histones. (<b>a</b>) Gel electrophoresis of DNA, histone, and mixture of DNA and histone. (<b>b</b>) Tagging and separating DNA in the presence of histone with different dilution ratios for immobilized GelGreen.</p>
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<p>Accumulation of 150 bp DNA spiked in plasma in the presence of histone in the devices with 30X GelGreen. (<b>a</b>) Images captured after agarose rehydration and after 5 min of applying 10 V for samples of healthy persons, survivors, and non-survivors. (<b>b</b>) Fluorescence intensity values for DNA concentrations corresponding to survivors and non-survivors (N = 3). Statistical significance for samples were calculated by the two-tailed <span class="html-italic">t</span>-test (n.s: not significant, ** <span class="html-italic">p</span> &lt; 0.01).</p>
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<p>Fluorescence saturation inside the channel for DNA detection due to interference from plasma proteins tagged with Qubit when both dyes are mixed with the sample.</p>
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<p>Trapping and concentrating 150 bp DNA and histones from spiked plasma samples in a fully integrated device. (<b>a</b>) Images captured after agarose rehydration and after 5 min of applying 10 V for DNA detection and 30 V for histone detection in the plasma samples of healthy persons, survivors, and non-survivors. (<b>b</b>) Plot showing changes in measured fluorescent intensity for DNA and histones for samples of healthy person, survivors, and non-survivors (N = 3). Statistical significance for samples calculated by the two-tailed <span class="html-italic">t</span>-test (** <span class="html-italic">p</span> &lt; 0.01, * <span class="html-italic">p</span> &lt; 0.05, # <span class="html-italic">p</span> &lt; 0.1).</p>
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<p>Fabrication steps of the final device. (<b>a</b>) Integration of agarose gates into the device using PTFE membranes and double-sided adhesives. (<b>b</b>) Steps for immobilization of the fluorescent dyes in the device. (<b>c</b>) Alignment and assembly of the layers. (<b>d</b>) Schematic view of the final device.</p>
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<p>Experimental setup for each part of experiment. (<b>a</b>) The setup for DNA detection part. (<b>b</b>) The setup for histone detection.</p>
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15 pages, 13251 KiB  
Article
The Controlled Release of Abscisic Acid (ABA) Utilizing Alginate–Chitosan Gel Blends: A Synergistic Approach for an Enhanced Small-Molecule Delivery Controller
by Oscar Valdes, Daniel Bustos, Luis Guzmán, Marcelo Muñoz-Vera, Gabriela Urra, Ricardo I. Castro and Luis Morales-Quintana
Gels 2024, 10(3), 185; https://doi.org/10.3390/gels10030185 - 8 Mar 2024
Cited by 1 | Viewed by 1303
Abstract
The integration of abscisic acid (ABA) into a chitosan–alginate gel blend unveils crucial insights into the formation and stability of these two substances. ABA, a key phytohormone in plant growth and stress responses, is strategically targeted for controlled release within these complexes. This [...] Read more.
The integration of abscisic acid (ABA) into a chitosan–alginate gel blend unveils crucial insights into the formation and stability of these two substances. ABA, a key phytohormone in plant growth and stress responses, is strategically targeted for controlled release within these complexes. This study investigates the design and characterization of this novel controlled-release system, showcasing the potential of alginate–chitosan gel blends in ABA delivery. Computational methods, including molecular dynamics simulations, are employed to analyze the structural effects of microencapsulation, offering valuable insights into complex behavior under varying conditions. This paper focuses on the controlled release of ABA from these complexes, highlighting its strategic importance in drug delivery systems and beyond. This controlled release enables targeted and regulated ABA delivery, with far-reaching implications for pharmaceuticals, agriculture, and plant stress response studies. While acknowledging context dependency, the paper suggests that the liberation or controlled release of ABA holds promise in applications, urging further research and experimentation to validate its utility across diverse fields. Overall, this work significantly contributes to understanding the characteristics and potential applications of chitosan–alginate complexes, marking a noteworthy advancement in the field of controlled-release systems. Full article
(This article belongs to the Special Issue Recent Advances in Biopolymer Gels)
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<p>SEM images of alginate–chitosan–ABA Ca<sup>2+</sup> blend: 100× magnification images of the cross-linked alginate–chitosan–abscisic acid blend gel for delivery system, with alginate/chitosan ratios of (<b>A</b>) 2:1, (<b>B</b>) 1:1, and (<b>C</b>) 1:2. Ratios of alginate/chitosan in the 500× magnification images are (<b>D</b>) 2:1, (<b>E</b>) 1:1, (<b>F</b>) 1:2.</p>
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<p>Thermogravimetric analysis (TGA) and the differential thermogravimetric analysis (DTG) thermogram for the polymer complexes: chitosan and alginate gel blends at different ratios (alginate/chitosan) of (<b>A</b>) 2:1, (<b>B</b>) 1:1, (<b>C</b>) 1:2.</p>
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<p>The vibrational frequencies (cm<sup>−1</sup>) obtained using FT-IR of the different complexes. (<b>A</b>) Spectra of different blends; (<b>B</b>) spectra range 4000 at 2600 cm<sup>−1</sup>; (<b>C</b>) spectra range 1800 at 1200 cm<sup>−1</sup>; and (<b>D</b>) spectra range 1200 at 800 cm<sup>−1</sup>.</p>
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<p>Cumulative release of model compounds from alginate–chitosan–ABA complex using different formulations in phosphate buffer solution at pH 7.4; alginate/chitosan ratios of (2:1 (black curve, system 1), 1:1 (red curve, system 2), 1:2 (blue curve, system 3). Data are presented as average ± SEM (n = 3).</p>
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<p>Fitting of appropriate experimental data (M<sub>t</sub>/M<sub>∞</sub> ≤ 0.6) to Peppas–Sahlin kinetic model for system 1 (<b>a</b>), system 2 (<b>b</b>), and system 3 (<b>c</b>).</p>
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<p>Stabilization of the nanoparticles over the simulation time: (<b>A</b>) radius of gyration of alginate and chitosan, (<b>B</b>) the number of hydrogen bonds between alginate and chitosan, and (<b>C</b>) the number of salt bridges between the ALG/CS complex and ABA.</p>
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<p>Alginate–chitosan–ABA nanoparticle formation. The initial (0 ns) and final (400 ns) time steps for each complex are depicted. Both types of alginate chains are colored in blue and cyan (in the core of the molecules), while chitosan chains and ABA molecules are in red and yellow colors, respectively.</p>
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<p>Molecular characterization of nanoparticles and ABA. The graph depicts (<b>A</b>) intermolecular hydrogen bond interactions between the alginate nanoparticles and ABA over the simulation period, and (<b>B</b>) the release profile of ABA molecules from the polymer. Statistical analyses for each molecular descriptor are included. In (<b>C</b>–<b>E</b>), the final states of nanoparticles are presented for the 1:1, 1:2, and 2:1 alginate/chitosan ratios, respectively, with white arrows indicating porosities formed by polymer composition ratios during simulation. Dark blue and light blue represent alginate monomers β-D-mannopyranuronate and α-L-gulopyranuronate, orange denotes chitosan chains, yellow signifies ABA, and green represents calcium ions. (<b>F</b>) The solvent accessible surface area (SASA) is illustrated across the simulation for the three studied proportions. The inset offers an approach to discerning SASA differences between the systems from ~25 ns onward.</p>
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<p>Approach to the intermolecular cavities of the ALG/CS nanoparticle where the ABA molecules are interacting with alginate/chitosan chains.</p>
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14 pages, 3868 KiB  
Article
pNIPAm-Based pH and Thermoresponsive Copolymer Hydrogel for Hydrophobic and Hydrophilic Drug Delivery
by Anandhu Mohan, Madhappan Santhamoorthy, Thi Tuong Vy Phan and Seong-Cheol Kim
Gels 2024, 10(3), 184; https://doi.org/10.3390/gels10030184 - 7 Mar 2024
Cited by 6 | Viewed by 2243
Abstract
The regulated and targeted administration of hydrophobic and hydrophilic drugs is both promising and challenging in the field of drug delivery. Developing a hydrogel which is responsive to dual stimuli is considered a promising and exciting research area of study. In this work, [...] Read more.
The regulated and targeted administration of hydrophobic and hydrophilic drugs is both promising and challenging in the field of drug delivery. Developing a hydrogel which is responsive to dual stimuli is considered a promising and exciting research area of study. In this work, melamine functionalized poly-N-isopropyl acrylamide-co-glycidyl methacrylate copolymer has been developed by copolymerizing glycidyl methacrylate (GMA) monomer with N-isopropyl acrylamide (NIPAm) and further functionalized with melamine units (pNIPAm-co-pGMA-Mela). The prepared pNIPAm-co-pGMA-Mela copolymer hydrogel was characterized using various characterization techniques, including 1H NMR, FTIR, SEM, zeta potential, and particle size analysis. A hydrophobic drug (ibuprofen, Ibu) and hydrophilic drug (5-fluorouracil, 5-Fu) were selected as model drugs. Dual pH and temperature stimuli-responsive drug release behavior of the pNIPAm-co-pGMA-Mela hydrogel was evaluated under different pH (pH 7.4 and 4.0) and temperature (25 °C, 37 °C, and 45 °C) conditions. Furthermore, the in vitro biocompatibility of the developed pNIPAm-co-pGMA-Mela copolymer hydrogel was determined on MDA-MB-231 cells. The pH and temperature-responsive drug delivery study results reveal that the pNIPAm-co-pGMA-Mela hydrogel system is responsive to both pH and temperature stimuli and exhibits about ~100% of Ibu and 5-Fu, respectively, released at pH 4.0/45 °C. Moreover, the MTT assay and hemocompatibility analysis results proved that the pNIPAm-co-pGMA-Mela hydrogel system is biocompatible and hemocompatible, suggesting that that it could be used for drug delivery applications. The experimental results suggest that the proposed pNIPAm-co-pGMA-Mela hydrogel system is responsive to dual pH and temperature stimuli, and could be a promising drug carrier system for both hydrophilic and hydrophobic drug delivery applications. Full article
(This article belongs to the Special Issue Biopolymer Gels as Smart Drug Delivery and Theranostic Systems)
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<p>(<b>A</b>) ¹H NMR spectra of pNIPAAm-co-pGMA copolymer and pNIPAAm-co-pGMA-Mela hydrogel; (<b>B</b>) FTIR analysis of (i) pNIPAAm-co-pGMA copolymer and (ii) pNIPAAm-co-pGMA-Mela hydrogel samples; (<b>C</b>) SEM images of (<b>i</b>) pNIPAAm-co-pGMA copolymer and (<b>ii</b>) pNIPAAm-co-pGMA-Mela hydrogel system.</p>
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<p>Zeta potential analysis of (<b>A</b>) pNIPAm-co-pGMA copolymer at (<b>i</b>) 25 °C and (<b>ii</b>) 45 °C and (<b>B</b>) pNIPAm-co-pGMA-Mela hydrogel at (<b>i</b>) 25 °C and (<b>ii</b>) 45 °C.</p>
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<p>Particle size analysis of (<b>A</b>) pNIPAm-co-pGMA copolymer and (<b>B</b>) pNIPAm-co-pGMA-Mela hydrogel at different temperature conditions; (<b>C</b>) particle size analysis of (i) pNIPAm-co-pGMA copolymer and (ii) pNIPAm-co-pGMA-Mela hydrogel at different pH conditions.</p>
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<p>Relative turbidity of (<b>A</b>) pNIPAm-co-pGMA copolymer and (<b>B</b>) pNIPAm-co-pGMA-Mela hydrogel samples at temperatures ranging from 25 °C to 55 °C; (<b>C</b>) schematic representation of the phase transition of the pNIPAm-co-pGMA-Mela hydrogel.</p>
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<p>Temperature-responsive swelling-deswelling behavior of (<b>A</b>) pNIPAm-co-pGMA copolymer and (<b>B</b>) pNIPAm-co-pGMA-Mela hydrogel at temperatures ranging from25 °C to 45 °C; (<b>C</b>) schematic representation of the sol–gel phase transition of pNIPAm-co-pGMA-Mela hydrogel.</p>
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<p>In vitro drug delivery efficiency of pNIPAAm-co-pGMA-Mela/Ibu hydrogel system: (<b>A</b>) Ibu release under various pH conditions, (<b>B</b>) Ibu release under various temperatures, and (<b>C</b>) Ibu release with different combinations of pH and temperature stimuli conditions.</p>
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<p>In vitro drug delivery efficiency of pNIPAAm-co-pGMA-Mela/5-Fu hydrogel system: (<b>A</b>) 5-Fu release at various pH conditions, (<b>B</b>) 5-Fu release at various temperatures, and (<b>C</b>) 5-Fu release with different combined pH and temperature conditions.</p>
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<p>(<b>A</b>) In vitro cytocompatibility of (i) pNIPAAm-co-pGMA-Mela hydrogel, (ii) 5-Fu drug-loaded pNIPAAm-co-pGMA-Mela/5-Fu hydrogel, and (iii) pure 5-Fu drug tested on MDA-MB-231 cells at different concentrations; (<b>B</b>) in vitro cytocompatibility of (i) pNIPAAm-co-pGMA-Mela hydrogel, (ii) Ibu drug-loaded pNIPAAm-co-pGMA-Mela/Ibu hydrogel, and (iii) pure Ibu drug tested on MDA-MB-231 cells at different concentrations; and (<b>C</b>) blood compatibility behavior of pNIPAAm-co-pGMA-Mela hydrogel at different sample concentrations. The inset image shows the in vitro blood compatibility of pNIPAAm-co-pGMA-Mela hydrogel by exposure of red blood cells to PBS, pNIPAAm-co-pGMA-Mela hydrogel sample, and Triton-X. Statistical significance refers to the cell toxicity with different samples (** significant <span class="html-italic">p</span> &lt; 0.05).</p>
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<p>In vitro fluorescence cell images of (<b>i</b>) control without cells and (<b>ii</b>) MDA-MB-231 cells after treatment with pNIPAAm-co-pGMA-Mela hydrogel.</p>
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<p>Illustration of the synthesis of pNIPAAm-co-pGMA copolymer (Step 1), melamine-functionalized pNIPAm-co-pGMA-Mela hydrogel (Step 2), and drug loading into the pNIPAAm-co-pGMA-Mela hydrogel system (Step 3).</p>
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24 pages, 1346 KiB  
Review
Gellan Gum as a Unique Microbial Polysaccharide: Its Characteristics, Synthesis, and Current Application Trends
by Raghad Abdl Karim Abdl Aali and Shayma Thyab Gddoa Al-Sahlany
Gels 2024, 10(3), 183; https://doi.org/10.3390/gels10030183 - 6 Mar 2024
Cited by 6 | Viewed by 2983
Abstract
Gellan gum (GG) is a linear, negatively charged exopolysaccharide that is biodegradable and non-toxic. When metallic ions are present, a hard and transparent gel is produced, which remains stable at a low pH. It exhibits high water solubility, can be easily bio-fabricated, demonstrates [...] Read more.
Gellan gum (GG) is a linear, negatively charged exopolysaccharide that is biodegradable and non-toxic. When metallic ions are present, a hard and transparent gel is produced, which remains stable at a low pH. It exhibits high water solubility, can be easily bio-fabricated, demonstrates excellent film/hydrogel formation, is biodegradable, and shows biocompatibility. These characteristics render GG a suitable option for use in food, biomedical, and cosmetic fields. Thus, this review paper offers a concise summary of microbial polysaccharides. Moreover, an in-depth investigation of trends in different facets of GG, such as biosynthesis, chemical composition, and physical and chemical properties, is emphasized. In addition, this paper highlights the process of extracting and purifying GG. Furthermore, an in-depth discussion of the advantages and disadvantages of GG concerning other polysaccharides is presented. Moreover, the utilization of GG across different industries, such as food, medicine, pharmaceuticals, cosmetics, etc., is thoroughly examined and will greatly benefit individuals involved in this field who are seeking fresh opportunities for innovative projects in the future. Full article
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<p>Chemical structures of gellan gum: (<b>A</b>) natural high-acyl gellan and (<b>B</b>) low-acyl gellan.</p>
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<p>Chemical structures of gellan gum: (<b>A</b>) natural high-acyl gellan and (<b>B</b>) low-acyl gellan.</p>
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<p>The metabolic pathway of <span class="html-italic">Sphingomonas</span> bacteria to produce gellan gum.</p>
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