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Gels, Volume 6, Issue 1 (March 2020) – 10 articles

Cover Story (view full-size image): At present, in the field of drug delivery, great consideration is given to colloidal systems and especially to polymeric nanoparticles and nanogels because of their characteristics, such as biocompatibility, biodegradability, water solubility, and ability of incorporation and preservation of drugs. The great benefit of these devices is the possibility to functionalize their surface through proper coating agents to improve their ability in targeted drug delivery and be able to treat specific tissues of human body. Obviously, many strategies are available, and the choice is strictly case-dependent. In this review, we illustrate the most important techniques of nanoparticles’ surface functionalization. Moreover, a detailed focus on the use of polymers, cell membranes, proteins, antibodies, and hybridized DNA structures as coating strategies is provided, together with a comparison of their characteristics, [...] Read more.
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16 pages, 2937 KiB  
Article
Bioprinted Three-Dimensional Cell-Laden Hydrogels to Evaluate Adipocyte-Breast Cancer Cell Interactions
by Sarah Chaji, Jenna Al-Saleh and Cheryl T. Gomillion
Gels 2020, 6(1), 10; https://doi.org/10.3390/gels6010010 - 24 Mar 2020
Cited by 38 | Viewed by 5893
Abstract
Three-dimensional (3D) bioprinting, although still in its infancy as a fabrication tool, has the potential to effectively mimic many biological environments. Cell-laden 3D printed structures have demonstrated to be an improvement from the widely used monolayer platforms, largely because of recapitulation of native [...] Read more.
Three-dimensional (3D) bioprinting, although still in its infancy as a fabrication tool, has the potential to effectively mimic many biological environments. Cell-laden 3D printed structures have demonstrated to be an improvement from the widely used monolayer platforms, largely because of recapitulation of native tissue architecture with the 3D structures. Thus, 3D in vitro models have been increasingly investigated for improved modeling of cell and disease systems, such as for breast cancer. In the present work, multicellular cell-laden hydrogels comprised of adipocytes and breast cancer cells were bioprinted and evaluated. An ideal bioink of 3:2 5% alginate was determined to mimic the tissue stiffness observed in a physiological breast cancer tumor environment. Rheological characterization and degradation studies were performed to verify the stability of the artificial breast hydrogel environment. It was found that both the breast cancer cells and adipocytes remained viable directly after printing and throughout the 10-day culture period within the printed hydrogels. Direct printing of the cells in co-culture resulted in morphology changes and variations in cell localization within printed structures. Overall, the feasibility of efficiently fabricating multicellular cell-laden bioprinted models of the breast tumor microenvironment was established. Full article
(This article belongs to the Special Issue Hydrogels in Tissue Engineering 2.0)
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11 pages, 1958 KiB  
Article
Elucidating the Structure-Function Relationship of Solvent and Cross-Linker on Affinity-Based Release from Cyclodextrin Hydrogels
by Sean T. Zuckerman, Edgardo Rivera-Delgado, Rebecca M. Haley, Julius N. Korley and Horst A. von Recum
Gels 2020, 6(1), 9; https://doi.org/10.3390/gels6010009 - 22 Mar 2020
Cited by 8 | Viewed by 3194
Abstract
Minocycline (MNC) is a tetracycline antibiotic capable of associating with cyclodextrin (CD), and it is a frontline drug for many instances of implant infection. Due to its broad-spectrum activity and long half-life, MNC represents an ideal drug for localized delivery; however, classic polymer [...] Read more.
Minocycline (MNC) is a tetracycline antibiotic capable of associating with cyclodextrin (CD), and it is a frontline drug for many instances of implant infection. Due to its broad-spectrum activity and long half-life, MNC represents an ideal drug for localized delivery; however, classic polymer formulations, particularly hydrogels, result in biphasic release less suitable for sustained anti-microbial action. A polymer delivery system capable of sustained, steady drug delivery rates poses an attractive target to maximize the antimicrobial activity of MNC. Here, we formed insoluble hydrogels of polymerized CD (pCD) with a range of crosslinking densities, and then assessed loading, release, and antimicrobial activity of MNC. MNC loads between 5–12 wt % and releases from pCD hydrogels for >14 days. pCD loaded with MNC shows extended antimicrobial activity against S. aureus for >40 days and E. coli for >70 days. We evaluated a range of water/ethanol blends to test our hypothesis that solvent polarity will impact drug-CD association as a function of hydrogel swelling and crosslinking. Increased polymer crosslinking and decreased solvent polarity both reduced MNC loading, but solvent polarity showed a dramatic reduction independent of hydrogel swelling. Due to its high solubility and excellent delivery profile, MNC represents a unique drug to probe the structure-function relationship between drug, affinity group, and polymer crosslinking ratio. Full article
(This article belongs to the Special Issue Hydrogels for Drug Delivery 2020)
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14 pages, 1919 KiB  
Article
Effect of Aromatic Amines on the Properties of Formaldehyde-Based Xerogels
by David Martin, Martin Prostredný and Ashleigh J. Fletcher
Gels 2020, 6(1), 8; https://doi.org/10.3390/gels6010008 - 2 Mar 2020
Cited by 1 | Viewed by 3082
Abstract
This study investigates the synthesis of formaldehyde-based xerogels using alternative aromatic precursors, with comparison to traditional resorcinol-formaldehyde analogues, in order to alter the chemical composition of the resulting gels. By replacing resorcinol with aromatic amine molecules, i.e., ammeline, melamine and melem, each expected [...] Read more.
This study investigates the synthesis of formaldehyde-based xerogels using alternative aromatic precursors, with comparison to traditional resorcinol-formaldehyde analogues, in order to alter the chemical composition of the resulting gels. By replacing resorcinol with aromatic amine molecules, i.e., ammeline, melamine and melem, each expected to undergo similar reactions with formaldehyde as the substituted species, we found that for all substituted gels, at low additive contents, the gel structure was compromised and non-porous materials were formed, as opposed to the most abundant monomers, and therefore, these additives seem to act as impurities at low levels. Working towards higher additive contents, melem monomers exhibited low solubility (~5%), even at elevated temperatures, thereby limiting the range to which melem could act as a substitute, while melamine could be incorporated up to ~40% under acidic conditions, with enhanced microporosity over this range. Pure gels were successfully synthesised from ammeline, but their performance was inferior to resorcinol-formaldehyde gels, while melamine-formaldehyde analogues required acidic reaction conditions but shrank considerably on sub-critical drying, adversely affecting the gel properties and demonstrating their lack of potential as sorbents. This demonstrates the potential for the inclusion of aminated aromatics within resorcinol-based gel systems, however, only as partial substitutes and not complete replacements. Full article
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11 pages, 368 KiB  
Review
Construction of a Universal Gel Model with Volume Phase Transition
by Gerald S. Manning
Gels 2020, 6(1), 7; https://doi.org/10.3390/gels6010007 - 27 Feb 2020
Cited by 3 | Viewed by 3426
Abstract
The physical principle underlying the familiar condensation transition from vapor to liquid is the competition between the energetic tendency to condense owing to attractive forces among molecules of the fluid and the entropic tendency to disperse toward the maximum volume available as limited [...] Read more.
The physical principle underlying the familiar condensation transition from vapor to liquid is the competition between the energetic tendency to condense owing to attractive forces among molecules of the fluid and the entropic tendency to disperse toward the maximum volume available as limited only by the walls of the container. Van der Waals incorporated this principle into his equation of state and was thus able to explain the discontinuous nature of condensation as the result of instability of intermediate states. The volume phase transition of gels, also discontinuous in its sharpest manifestation, can be understood similarly, as a competition between net free energy attraction of polymer segments and purely entropic dissolution into a maximum allowed volume. Viewed in this way, the gel phase transition would require nothing more to describe it than van der Waals’ original equation of state (with osmotic pressure Π replacing pressure P). But the polymer segments in a gel are networked by cross-links, and a consequent restoring force prevents complete dissolution. Like a solid material, and unlike a van der Waals fluid, a fully swollen gel possesses an intrinsic volume of its own. Although all thermodynamic descriptions of gel behavior contain an elastic component, frequently in the form of Flory-style rubber theory, the resulting isotherms usually have the same general appearance as van der Waals isotherms for fluids, so it is not clear whether the solid-like aspect of gels, that is, their intrinsic volume and shape, adds any fundamental physics to the volume phase transition of gels beyond what van der Waals already knew. To address this question, we have constructed a universal chemical potential for gels that captures the volume transition while containing no quantities specific to any particular gel. In this sense, it is analogous to the van der Waals theory of fluids in its universal form, but although it incorporates the van der Waals universal equation of state, it also contains a network elasticity component, not based on Flory theory but instead on a nonlinear Langevin model, that restricts the radius of a fully swollen spherical gel to a solid-like finite universal value of unity, transitioning to a value less than unity when the gel collapses. A new family of isotherms arises, not present in a preponderately van der Waals analysis, namely, profiles of gel density as a function of location in the gel. There is an abrupt onset of large amplitude density fluctuations in the gel at a critical temperature. Then, at a second critical temperature, the entire swollen gel collapses to a high-density phase. Full article
(This article belongs to the Special Issue New Era in the Volume Phase Transition of Gels)
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16 pages, 2257 KiB  
Review
Coating and Functionalization Strategies for Nanogels and Nanoparticles for Selective Drug Delivery
by Filippo Pinelli, Giuseppe Perale and Filippo Rossi
Gels 2020, 6(1), 6; https://doi.org/10.3390/gels6010006 - 4 Feb 2020
Cited by 76 | Viewed by 8185
Abstract
Drug delivery is a fascinating research field with several development opportunities. Great attention is now focused on colloidal systems, nanoparticles, and nanogels and on the possibility of modifying them in order to obtain precise targeted drug delivery systems. The aim of this review [...] Read more.
Drug delivery is a fascinating research field with several development opportunities. Great attention is now focused on colloidal systems, nanoparticles, and nanogels and on the possibility of modifying them in order to obtain precise targeted drug delivery systems. The aim of this review is to give an overview of the main available surface functionalization and coating strategies that can be adopted in order to modify the selectivity of the nanoparticles in the delivery process and obtain a final system with great targeted drug delivery ability. We also highlight the most important fields of application of these kinds of delivery systems and we propose a comparison between the advantages and disadvantages of the described functionalization strategies. Full article
(This article belongs to the Special Issue Gels: 6th Anniversary)
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20 pages, 3478 KiB  
Article
Tailoring Properties of Mixed-Component Oleogels: Wax and Monoglyceride Interactions Towards Flaxseed Oil Structuring
by Noadia G. Barroso, Paula K. Okuro, Ana P. B. Ribeiro and Rosiane L. Cunha
Gels 2020, 6(1), 5; https://doi.org/10.3390/gels6010005 - 31 Jan 2020
Cited by 58 | Viewed by 7486
Abstract
The combination of oleogelators in oil structuring has an untapped potential, since effective pairs have usually been found by serendipity. The aim of this work was to evaluate the combination of berry (BEW) or sunflower wax (SHW) with glycerol monostearate (GMS) in flaxseed [...] Read more.
The combination of oleogelators in oil structuring has an untapped potential, since effective pairs have usually been found by serendipity. The aim of this work was to evaluate the combination of berry (BEW) or sunflower wax (SHW) with glycerol monostearate (GMS) in flaxseed oil (FXO) at 5 and 25 °C. The thermal and mechanical properties, microstructure, and stability of oleogels were investigated. Self-standing and translucent gels were obtained from BEW in FXO. However, the mixture BEW:GMS resulted in a decrease of dynamic moduli. Moreover, changes in the crystal network and a reduction of oil binding capacity were noticed. Thus, the GMS prevented the complete organization of BEW in polyunsaturated chains of FXO. Conversely, a positive interaction was found for GMS:SHW, since both alone were not able to impart the structure in FXO. Interestingly, gel was formed with improved properties, even with a small addition of GMS, although an ideal ratio of 1:1 (GMS50:50SHW) was found. Oxidative stability analysis showed that all gels resembled the behavior of liquid oil (~12.00 meqO2/kg) over 30 days storage. Therefore, semi-solid systems with nutritional and techno-functional claims were created by using waxes and fatty-acid derivative oleogelator in a rational fashion; this opened the opportunity to tailor oleogel properties. Full article
(This article belongs to the Special Issue Gels: 6th Anniversary)
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13 pages, 2968 KiB  
Article
Poly(Hydroxyethyl Methacrylate) Immunoaffinity Cryogel Column for the Purification of Human Immunoglobulin M
by Monireh Bakhshpour, Aykut Arif Topcu, Nilay Bereli, Huseyin Alkan and Adil Denizli
Gels 2020, 6(1), 4; https://doi.org/10.3390/gels6010004 - 29 Jan 2020
Cited by 13 | Viewed by 3867
Abstract
Human immunoglobulin M (hIgM) antibodies are considered as hopeful tools for diseases therapy. Therefore, chromatography approaches are used to purify hIgM with a single step. In this study, we prepared a poly(hydroxyethyl methacrylate) based immunoaffinity p(HEMA-I) cryogel column by using cyanamide to immobilize [...] Read more.
Human immunoglobulin M (hIgM) antibodies are considered as hopeful tools for diseases therapy. Therefore, chromatography approaches are used to purify hIgM with a single step. In this study, we prepared a poly(hydroxyethyl methacrylate) based immunoaffinity p(HEMA-I) cryogel column by using cyanamide to immobilize antihuman immunoglobulin on the p(HEMA) cryogel for purification of hIgM in aqueous solution and artificial human plasma. The characterization of the p(HEMA) cryogel column was performed by using a scanning electron microscope (SEM), micro-computerized tomography (µ-CT), Fourier transform infrared spectroscopy (FTIR), swelling degree and macro-porosity. Further, the optimizations of various parameters were performed such as, pH, ionic strength, temperature and concentration of hIgM in aqueous solutions. In addition, the Langmuir adsorption model was supported by experimental results. Maximum adsorbed amount of hIgM corresponded to 11.1 mg/g at pH 5.75 [morpholino ethanesulfonic acid (MES buffer)]. Our results indicated that the p(HEMA-I) cryogel column can be reused at least 10 times without significant loss in adsorption capacity. As a natural source, artificial human plasma was selected for hIgM adsorption and the purity of hIgM was evaluated using sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE). Full article
(This article belongs to the Special Issue Cryogelation and Cryogels)
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2 pages, 164 KiB  
Editorial
Acknowledgement to Reviewers of Gels in 2019
by Gels Editorial Office
Gels 2020, 6(1), 3; https://doi.org/10.3390/gels6010003 - 19 Jan 2020
Viewed by 1982
Abstract
The editorial team greatly appreciates the reviewers who have dedicated their considerable time and expertise to the journal’s rigorous editorial process over the past 12 months, regardless of whether the papers are finally published or not [...] Full article
10 pages, 2234 KiB  
Article
Crosslinker-Based Regulation of Swelling Behavior of Poly(N-isopropylacrylamide) Gels in a Post-Polymerization Crosslinking System
by Shohei Ida, Akimitsu Katsurada, Mitsuhiro Tsujio, Motoharu Nakamura and Yoshitsugu Hirokawa
Gels 2020, 6(1), 2; https://doi.org/10.3390/gels6010002 - 21 Dec 2019
Cited by 9 | Viewed by 4241
Abstract
A fundamental understanding of the effect of a crosslinker on gel properties is important for the design of novel soft materials because a crosslinking is a key component of polymer gels. We focused on post-polymerization crosslinking (PPC) system utilizing activated ester chemistry, which [...] Read more.
A fundamental understanding of the effect of a crosslinker on gel properties is important for the design of novel soft materials because a crosslinking is a key component of polymer gels. We focused on post-polymerization crosslinking (PPC) system utilizing activated ester chemistry, which is a powerful tool due to structural diversity of diamine crosslinkers and less susceptibility to solvent effect compared to conventional divinyl crosslinking system, to systematically evaluate the crosslinker effect on the gel properties. A variety of alkyldiamine crosslinkers was employed for the synthesis of poly(N-isopropylacrylamide) (PNIPAAm) gels and it was clarified that the length of alkyl chains of diamine crosslinkers strongly affected the gelation reaction and the swelling behavior. The longer crosslinker induced faster gelation and decreased the swelling degree and the response temperature in water, while the crosslinking density did not significantly change. In addition, we were able to modify the polymer chains in parallel with crosslinking by using a monoamine modifier along with a diamine crosslinker. This simultaneous chain modification during crosslinking (SMC) was demonstrated to be useful for the regulation of the crosslinking density and the swelling behavior of PNIPAAm gels. Full article
(This article belongs to the Special Issue New Era in the Volume Phase Transition of Gels)
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17 pages, 2984 KiB  
Article
Polyolefin-Supported Hydrogels for Selective Cleaning Treatments of Paintings
by Silvia Freese, Samar Diraoui, Anca Mateescu, Petra Frank, Charis Theodorakopoulos and Ulrich Jonas
Gels 2020, 6(1), 1; https://doi.org/10.3390/gels6010001 - 18 Dec 2019
Cited by 8 | Viewed by 7877
Abstract
Surface decontamination is of general concern in many technical fields including optics, electronics, medical environments, as well as art conservation. In this respect, we developed thin copolymer networks covalently bonded to flexible polyethylene (PE) sheets for hydrogel-based cleaning of varnished paintings. The syntheses [...] Read more.
Surface decontamination is of general concern in many technical fields including optics, electronics, medical environments, as well as art conservation. In this respect, we developed thin copolymer networks covalently bonded to flexible polyethylene (PE) sheets for hydrogel-based cleaning of varnished paintings. The syntheses of acrylates and methacrylates of the surfactants Triton X-100, Brij 35, and Ecosurf EH-3 or EH-9 and their incorporation into copolymers with acrylamide (PAM) and N-(4-benzoylphenyl)acrylamide are reported. Photocrosslinked polymer networks were prepared from these copolymers on corona-treated PE sheets, which can be swollen with aqueous solution to form hydrogel layers. The cleaning efficacy of these PE-PAM hydrogel systems, when swollen with appropriate cleaning solutions, was evaluated on painting surfaces in dependence of the PAM copolymer composition and degree of crosslinking. Specifically, soil and varnish removal and varnish surface solubilization were assessed on mock-ups as well as on paintings, indicating that even surfactant-free cleaning solutions were effective. Full article
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