Research

24 pages, 25012 KiB

Open AccessArticle

The Development and Characterisation of a P(3HB-co-4HB)–Bioactive Glass–Graphene Hydrogel as a Potential Formulation for Biomedical and Therapeutical Translation

by Nik S. A. N. Sharifulden, Lady V. Barrios Silva, Sean P. Nair, Amirul A. A. Abdullah, Siti N. F. M. Noor, Michael Sulu, Linh T. B. Nguyen and David Y. S. Chau

Gels 2024, 10(1), 85; https://doi.org/10.3390/gels10010085 - 22 Jan 2024

Viewed by 1282

Abstract

The clinical management of wounds is known to be a significant challenge: not only does the dressing need to ensure and provide the appropriate barrier and healing characteristics, but consideration of patient compliance concerning comfort, functionality, and practicality also needs to be included. [...] Read more.

The clinical management of wounds is known to be a significant challenge: not only does the dressing need to ensure and provide the appropriate barrier and healing characteristics, but consideration of patient compliance concerning comfort, functionality, and practicality also needs to be included. The poly(3-hydroxybutyrate-co-4-hydroxubutyrate) (P(3HB-co-4HB)) copolymer, isolated from Cupriavidus malaysiensis USM1020 (C. malaysiensis USM1020), was produced in the presence of excess carbon sources (1,4-butanediol and 1,6-hexanediol) using either a shake flask cultivation process or a bioreactor fermentation system. P(3HB-co-4HB) is widely known to be biodegradable and highly biocompatible and contains a tuneable 4HB monomer molar fraction, which is known to affect the final physicochemical properties of the intracellular copolymer. In this paper, we describe not only the fabrication of the polymeric gel but also its optimised profiling using a range of physical and mechanical techniques, i.e., SEM, FTIR, DMA, DSC, and WCA. The further enhancement of the gel through additional functionalisation with sol-gel-derived bioactive glass and liquid-exfoliated graphene was also investigated. The biocompatibility and biological characterisation of the substrates was assessed using murine osteoblasts (MC3T3), human primary dermal fibroblasts (HDFs), human fibroblast (BJ) cells, and standard cell culture assays (i.e., metabolic activity, LDH release, and live/dead staining). In short, P(3HB-co-4HB) was successfully isolated from the bacteria, with the defined physico-chemical profiles dependent on the culture substrate and culturing platform used. The additional enhancement of the copolymer with bioactive glass and/or graphene was also demonstrated by varying the combination loading of the materials, i.e., graphene resulted in an increase in tensile strength (~11 MPa) and the wettability increased following the incorporation of bioactive glass and 0.01 wt% graphene (WCA ~46.3°). No detrimental effects in terms of biocompatibility were noticed during the 7 days of culture in the primary and established cell lines. This study demonstrates the importance of optimising each of the individual components within the biocomposite and their relationship concerning the fine-tuning of the material’s properties, thus targeting and impacting the endpoint application. Full article

(This article belongs to the Special Issue Synthetic, Natural and Hybrid Gels Intended for Various Applications)

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15 pages, 2933 KiB

Open AccessArticle

Superfast Gelation of Spider Silk-Based Artificial Silk Protein

by Fan Wen, Yu Wang, Bowen Tu and Lun Cui

Gels 2024, 10(1), 69; https://doi.org/10.3390/gels10010069 - 17 Jan 2024

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Abstract

Spider silk proteins (spidroins) have garnered attention in biomaterials research due to their ability to self-assemble into hydrogels. However, reported spidroin hydrogels require high protein concentration and prolonged gelation time. Our study engineered an artificial spidroin that exhibits unprecedented rapid self-assembly into hydrogels [...] Read more.

Spider silk proteins (spidroins) have garnered attention in biomaterials research due to their ability to self-assemble into hydrogels. However, reported spidroin hydrogels require high protein concentration and prolonged gelation time. Our study engineered an artificial spidroin that exhibits unprecedented rapid self-assembly into hydrogels at physiologically relevant conditions, achieving gelation at a low concentration of 6 mg/mL at 37 °C without external additives. Remarkably, at a 30 mg/mL concentration, our engineered protein forms hydrogels within 30 s, a feature we termed “superfast gelation”. This rapid formation is modulated by ions, pH, and temperature, offering versatility in biomedical applications. The hydrogel’s capacity to encapsulate proteins and support E. coli growth while inducing RFP expression provides a novel platform for drug delivery and bioengineering applications. Our findings introduce a superfast, highly adaptable, and cytocompatible hydrogel that self-assembles under mild conditions, underscoring the practical implication of rapid gelation in biomedical research and clinical applications. Full article

(This article belongs to the Special Issue Synthetic, Natural and Hybrid Gels Intended for Various Applications)

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13 pages, 3178 KiB

Open AccessArticle

Graphene-Enhanced Methacrylated Alginate Gel Films for Sustainable Dye Removal in Water Purification

by Rubén Teijido, Qi Zhang, Miren Blanco, Leyre Pérez-Álvarez, Senentxu Lanceros-Méndez, José Luis Vilas-Vilela and Leire Ruiz-Rubio

Gels 2024, 10(1), 25; https://doi.org/10.3390/gels10010025 - 27 Dec 2023

Viewed by 1063

Abstract

Self-standing nanocomposite films were prepared by three-dimensional UV-induced radical copolymerization of methacrylated alginate (MALG) with acrylic acid (AA) and reinforced with graphene oxide (GO) to improve both mechanical strength and dye adsorption capacity in wastewater decontamination operations. Dynamic mechanical–thermal analysis revealed variations in [...] Read more.

Self-standing nanocomposite films were prepared by three-dimensional UV-induced radical copolymerization of methacrylated alginate (MALG) with acrylic acid (AA) and reinforced with graphene oxide (GO) to improve both mechanical strength and dye adsorption capacity in wastewater decontamination operations. Dynamic mechanical–thermal analysis revealed variations in storage modulus: the higher the GO content, the higher the storage modulus (E′) values. Also, the higher the temperature (associated with a lower and lower water content of films), the larger values of E′ for the films of the same composition (E′(25 °C) = 676.6–1538.7 MPa; E′(100 °C) = 886.9–2066.6 MPa), providing insights into the compatibility between GO and the MALG/AA matrix, as well as, assessing the improvement in the nanocomposite’s final mechanical properties. These crosslinked films in a dry state exhibited rapid water uptake and relatively short drying times (ca. 30 min at room temperature for the MALG/AA/GO composites) resulting from the swelling–drying studies and water contact angle measurements. The efficacy of methylene blue removal from water assessed via UV–VIS spectrometry revealed excellent results, expressed as an adsorption yield of 70–80% and 85–98% after 30 h and 258 h, respectively, of immersion time of films into an MB aqueous solution of 12.5 mg/L (as the contaminated water model). The reusability of the same films was evaluated by consecutive extraction processes of MB from the composite membranes when the content of desorbed dye was also spectrophotometrically monitored and conducted in acidic conditions (HCl aqueous solutions of pH 2). Overall, the introduction of GO in the developed self-standing MALG/AA nanocomposite films exhibited enhanced mechanical properties and increased efficiency for dye removal applications. Their great reutilization potential was highlighted by low drying times and a good ability to release the dye initially adsorbed. Thus, the prepared films could be suitable materials for sustainable and effective water treatment technologies. Full article

(This article belongs to the Special Issue Synthetic, Natural and Hybrid Gels Intended for Various Applications)

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13 pages, 3049 KiB

Open AccessArticle

Gel Polymer Electrolytes for Lithium-Ion Batteries Enabled by Photo Crosslinked Polymer Network

by Kyeongsik Kim, Wookil Chae, Jaehyeon Kim, Choongik Kim and Taeshik Earmme

Gels 2023, 9(12), 975; https://doi.org/10.3390/gels9120975 - 13 Dec 2023

Cited by 1 | Viewed by 1386

Abstract

We demonstrate a gel polymer electrolyte (GPE) featuring a crosslinked polymer matrix formed by poly(ethylene glycol) diacrylate (PEGDA) and dipentaerythritol hexaacrylate (DPHA) using the radical photo initiator via ultraviolet (UV) photopolymerization for lithium-ion batteries. The two monomers with acrylate functional groups undergo chemical [...] Read more.

We demonstrate a gel polymer electrolyte (GPE) featuring a crosslinked polymer matrix formed by poly(ethylene glycol) diacrylate (PEGDA) and dipentaerythritol hexaacrylate (DPHA) using the radical photo initiator via ultraviolet (UV) photopolymerization for lithium-ion batteries. The two monomers with acrylate functional groups undergo chemical crosslinking, resulting in a three-dimensional structure capable of absorbing liquid electrolytes to form a gel. The GPE system was strategically designed by varying the ratios between the main polymer backbone (PEGDA) and the crosslinker (DPHA) to achieve an optimal gel polymer electrolyte network. The resulting GPE exhibited enhanced thermal stability compared to conventional liquid electrolytes (LE) and demonstrated high ionic conductivity (1.40 mS/cm) with a high lithium transference number of 0.65. Moreover, the obtained GPE displayed exceptional cycle performance, maintaining a higher capacity retention (85.2%) comparable to the cell with LE (79.3%) after 200 cycles. Full article

(This article belongs to the Special Issue Synthetic, Natural and Hybrid Gels Intended for Various Applications)

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19 pages, 8026 KiB

Open AccessArticle

The Sustainable Bioactive Dyeing of Textiles: A Novel Strategy Using Bacterial Pigments, Natural Antibacterial Ingredients, and Deep Eutectic Solvents

by Cláudia Mouro, Ana P. Gomes, Rita V. Costa, Farzaneh Moghtader and Isabel C. Gouveia

Gels 2023, 9(10), 800; https://doi.org/10.3390/gels9100800 - 05 Oct 2023

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Abstract

The textile industry stands as a prominent contributor to global environmental pollution, primarily attributable to its extensive reliance on synthetic dyes, hazardous components, and solvents throughout the textile dyeing and treatment processes. Consequently, the pursuit of sustainable textile solutions becomes imperative, aimed at [...] Read more.

The textile industry stands as a prominent contributor to global environmental pollution, primarily attributable to its extensive reliance on synthetic dyes, hazardous components, and solvents throughout the textile dyeing and treatment processes. Consequently, the pursuit of sustainable textile solutions becomes imperative, aimed at replacing these environmentally unfriendly constituents with biobased and bioactive pigments, antibacterial agents, and, notably, natural solvents. Achieving this goal is a formidable yet indispensable challenge. In this study, the dyeing ability of the crude gel prodigiosin, produced by non-pathogenic bacteria Serratia plymuthica, was investigated on various multifiber fabrics at different conditions (temperature and pH) and by using salts and alternative mordants (the conventional Ferrous Sulphate (FeSO₄) and a new bio-mordant, L-Cysteine (L-Cys)). Additionally, a novel gel-based Choline chloride (ChCl)/Lactic acid (LA) (1:2) deep eutectic solvent (DES) dyeing medium was studied to replace the organic solvents. Nylon fabrics dyed with 3.0% over the weight of the fiber (owf) L-Cys at pH = 8.3 had improved color fastness to washing, while the gel-based ChCl/LA (1:2) DES dyebath provided a better color fastness to light. Moreover, nylon fabrics under these conditions exhibited remarkable antimicrobial activity against Staphylococcus aureus (S. aureus) and Pseudomonas aeruginosa (P. aeruginosa). In conclusion, the utilization of the crude gel-based prodigiosin pigment demonstrates a distinct advantage in dyeing textile materials, aligning with the growing consumer demand for more eco-friendly and sustainable products. Additionally, the application of the natural reducing agent L-Cys, previously untested as a bio-mordant, in conjunction with the use of gel-based DES as a dyeing medium, has showcased improved colorimetric and antibacterial properties when applied to nylon that is dyed with the crude gel prodigiosin pigment. Full article

(This article belongs to the Special Issue Synthetic, Natural and Hybrid Gels Intended for Various Applications)

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18 pages, 14324 KiB

Open AccessArticle

Transparent Sol–Gel-Based Coatings Reflecting Heat Radiation in the Near Infrared

by Thomas Mayer-Gall, Leonie Kamps, Thomas Straube, Jochen S. Gutmann and Torsten Textor

Gels 2023, 9(10), 795; https://doi.org/10.3390/gels9100795 - 02 Oct 2023

Viewed by 1106

Abstract

Thin, flat textile roofing offers negligible heat insulation. In warm areas, such roofing membranes are therefore equipped with metallized surfaces to reflect solar heat radiation, thus reducing the warming inside a textile building. Heat reflection effects achieved by metallic coatings are always accompanied [...] Read more.

Thin, flat textile roofing offers negligible heat insulation. In warm areas, such roofing membranes are therefore equipped with metallized surfaces to reflect solar heat radiation, thus reducing the warming inside a textile building. Heat reflection effects achieved by metallic coatings are always accompanied by shading effects as the metals are non-transparent for visible light (VIS). Transparent conductive oxides (TCOs) are transparent for VIS and are able to reflect heat radiation in the infrared. TCOs are, e.g., widely used in the display industry. To achieve the perfect coatings needed for electronic devices, these are commonly applied using costly vacuum processes at high temperatures. Vacuum processes, on account of the high costs involved and high processing temperatures, are obstructive for an application involving textiles. Accepting that heat-reflecting textile membranes demand less perfect coatings, a wet chemical approach has been followed here when producing transparent heat-reflecting coatings. Commercially available TCOs were employed as colloidal dispersions or nanopowders to prepare sol–gel-based coating systems. Such coatings were applied to textile membranes as used for architectural textiles using simple coating techniques and at moderate curing temperatures not exceeding 130 °C. The coatings achieved about 90% transmission in the VIS spectrum and reduced near-infrared transmission (at about 2.5 µm) to nearly zero while reflecting up to 25% of that radiation. Up to 35% reflection has been realized in the far infrared, and emissivity values down to ε = 0.5777 have been measured. Full article

(This article belongs to the Special Issue Synthetic, Natural and Hybrid Gels Intended for Various Applications)

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21 pages, 6605 KiB

Open AccessArticle

Liquid Crystalline and Gel Properties of Luminescent Cyclometalated Palladium Complexes with Benzoylthiourea Ligands

by Theodora A. Ilincă, Monica Iliș, Marin Micutz and Viorel Cîrcu

Gels 2023, 9(10), 777; https://doi.org/10.3390/gels9100777 - 25 Sep 2023

Viewed by 878

Abstract

The design and development of new luminescent metallogels formed by cyclometalated palladium(II) complexes in protic solvents were investigated by a combination of differential scanning calorimetry (DSC), polarized optical microscopy (POM), and rheology. Cyclometalated palladium(II) complexes based on imine ligand and ancillary benzoylthiourea (BTU) [...] Read more.

The design and development of new luminescent metallogels formed by cyclometalated palladium(II) complexes in protic solvents were investigated by a combination of differential scanning calorimetry (DSC), polarized optical microscopy (POM), and rheology. Cyclometalated palladium(II) complexes based on imine ligand and ancillary benzoylthiourea (BTU) ligand showed red emission in solid and gel states. The formation of a lyotropic liquid crystal phase was observed for the complex bearing shorter alkyl groups on the BTU ligand. This complex also behaved as a thermotropic liquid crystal that displays a monotropic smectic A phase (SmA). Dynamic rheology measurements (frequency sweep in the 5–90 °C range) of the 1-decanol solution of palladium(II) complexes highlighted their supramolecular self-association ability to generate 3D networks and form gels as a final result. Full article

(This article belongs to the Special Issue Synthetic, Natural and Hybrid Gels Intended for Various Applications)

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24 pages, 4293 KiB

Open AccessArticle

Nanomaterial-Doped Xerogels for Biosensing Measurements of Xanthine in Clinical and Industrial Applications

by Quang Minh Dang, Ann H. Wemple and Michael C. Leopold

Gels 2023, 9(6), 437; https://doi.org/10.3390/gels9060437 - 25 May 2023

Cited by 3 | Viewed by 1373

Abstract

First-generation amperometric xanthine (XAN) biosensors, assembled via layer-by-layer methodology and featuring xerogels doped with gold nanoparticles (Au-NPs), were the focus of this study and involved both fundamental exploration of the materials as well as demonstrated usage of the biosensor in both clinical (disease [...] Read more.

First-generation amperometric xanthine (XAN) biosensors, assembled via layer-by-layer methodology and featuring xerogels doped with gold nanoparticles (Au-NPs), were the focus of this study and involved both fundamental exploration of the materials as well as demonstrated usage of the biosensor in both clinical (disease diagnosis) and industrial (meat freshness) applications. Voltammetry and amperometry were used to characterize and optimize the functional layers of the biosensor design including a xerogel with and without embedded xanthine oxidase enzyme (XOx) and an outer, semi-permeable blended polyurethane (PU) layer. Specifically, the porosity/hydrophobicity of xerogels formed from silane precursors and different compositions of PU were examined for their impact on the XAN biosensing mechanism. Doping the xerogel layer with different alkanethiol protected Au-NPs was demonstrated as an effective means for enhancing biosensor performance including improved sensitivity, linear range, and response time, as well as stabilizing XAN sensitivity and discrimination against common interferent species (selectivity) over time—all attributes matching or exceeding most other reported XAN sensors. Part of the study focuses on deconvoluting the amperometric signal generated by the biosensor and determining the contribution from all of the possible electroactive species involved in natural purine metabolism (e.g., uric acid, hypoxanthine) as an important part of designing XAN sensors (schemes amenable to miniaturization, portability, or low production cost). Effective XAN sensors remain relevant as potential tools for both early diagnosis of diseases as well as for industrial food monitoring. Full article

(This article belongs to the Special Issue Synthetic, Natural and Hybrid Gels Intended for Various Applications)

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