Search Results (40)

Composite hydrogels with improved mechanical and chemical properties can be formed by non-covalently decorating the nanofibrillar structures formed by the self-assembly of peptides with fucoidan. Nevertheless, the precise interactions, and the electrochemical and thermodynamic stability of these composite materials have not been determined. Here, we present a thermodynamic analysis of the interacting forces that drive the formation of a composite fucoidan/9-fluorenylmethoxycarbonyl-phenylalanine-arginine-glycine-aspartic acid-phenylalanine (Fmoc-FRGDF) hydrogel. The results showed that the co-assembly of fucoidan and Fmoc-FRGDF was spontaneous and exothermic. The melting point increased from 87.0 °C to 107.7 °C for Fmoc-FRGDF with 8 mg/mL of added fucoidan. A complex network of hydrogen bonds formed between the molecules of Fmoc-FRGDF, and electrostatic, hydrogen bond, and van der Waals interactions were the main interactions driving the co-assembly of fucoidan and Fmoc-FRGDF. Furthermore, the sulfate group of fucoidan formed a strong salt bridge with the arginine of Fmoc-FRGDF. This study provides useful biomedical engineering design parameters for the inclusion of other highly soluble biopolymers into these types of hydrogel vectors. Full article

The abundance of hyaluronic acid (HA) in human tissues attracts its thorough research in tissue regenerating scaffolds and 3D bioprintable hydrogel preparation. Though methacrylation of HA can lead to photo-crosslinkable hydrogels, the catalyst has toxicity concerns, and the hydrogel is not suitable for creating stable complex 3D structures using extrusion 3D bioprinting. In this study, a dual crosslinking on methacrylated HA is introduced, using cysteamine-grafted HA and varying concentrations of 2-hydroxy ethyl acrylate. The resultant hydrogel is suitable for extrusion 3D printing (or bioprinting), mechanically robust, self-standing, stable in phosphate-buffered saline at 37 °C for more than 42 days, has high water absorption capacity with a low swelling ratio (1.5), and exhibits self-healing and adhesive properties. Complex 3D structures like ears and pyramid shapes with more than 2 cm of height are 3D printed using the optimized composition. All the synthesized hydrogels have shown nontoxicity and cell-supportiveness. Loading of cells, tetracycline, and bovine serum albumin into the hydrogel led to better bioink properties such as cell attachment, growth, and proliferation for osteoblast cells. The test results suggest that this hydrogel is biocompatible and has potential for 3D bioprinting of self-standing structures in bioink form in tissue engineering and regenerative medicine. Full article

Currently, tissue engineering technologies are promising for the restoration of damaged organs and tissues. For regeneration of electrically conductive tissues or neural interfaces, it is necessary to provide electrical conductivity for the transmission of electrophysiological signals. The developed biocomposite structures presented in this article possess such properties. Their composition includes bovine serum albumin (BSA), gelatin, eosin-Y and single-walled carbon nanotubes (SWCNTs). For the first time, a biocomposite structure was formed from the proposed hydrogel using a nanosecond laser, and a two-photon absorption cross section value of 580 GM was achieved. Increased viscosity over 3 mPa∙s and self-focusing with a nonlinear refractive index of 42 × 10⁻¹² cm²/W make it possible to create a biocomposite structure over the entire specified area. The obtained electrical conductivity value was 19 mS∙cm⁻¹, due to the formation of effective electrically conductive networks. For a biocomposite with a concentration of gelatin 3 wt. %, formed by low-energy near-IR pulses, the survival of Neuro 2A nerve tissue cells was confirmed. The obtained results are important for the creation of new tissue engineering structures and neural interfaces from a biopolymer hydrogel based on the organic dye eosin-Y and carbon nanotubes by two-photon polymerization. Full article

The application of fish gelatin (FG) is limited due to its poor mechanical properties and thermal stability, both of which could be significantly improved by gellan gum (GG) found in previous research. However, the FG/GG composite hydrogel was brittle and easily damaged by external forces. It was found that the composite hydrogel with Fe₂(SO₄)₃ showed good flexibility and self-healing properties in the pre-experiment. Thus, the synergistic effect of FG, GG and Fe₂(SO₄)₃ on the mechanical properties of the composite hydrogel was investigated in this study. According to one-way experiments, response surface tests and Texture Profile Analysis, it was found that under the optimum condition of FG concentration 186.443 g/L, GG concentration 8.666 g/L and Fe₂(SO₄)₃ concentration 56.503 g/L, the springiness of the composite cylindrical hydrogel with the height of 25 mm formed in 25 mL beakers (bottom diameter 30 mm) was 7.602 mm. Determination of the rheological properties, compression performance, adhesive performance and self-healing properties showed that the composite hydrogel had good thermal stability, flexibility and self-healing properties with good adhesion, skin compliance and compressive strength, and it was easy to remove. The composite hydrogel showed strong antimicrobial activity against A. salmonicida and V. parahaemolyticus. All hydrogels showed a uniform and porous structure. The 3D structure of the composite hydrogel was much looser and more porous than the pure FG hydrogel. The flexible and self-healing composite hydrogel with some antimicrobial activity is suitable for the development of medical dressings, which broadens the applications of the composite hydrogel. Full article

Traditional anti-corrosion and anti-fouling coatings struggle against the harsh marine environment. Our study tackled this by introducing a novel dual-layer hydrogel (A-H DL) coating system. This system combined a Cu₂O–SiO₂–acrylic resin primer for anchoring and controlled copper ion release with a dissipative double-network double-anchored hydrogel (DNDAH) boasting superior mechanical strength and anti-biofouling performance. An acrylamide monomer was copolymerized and cross-linked with a coupling agent to form the first irreversible network and first anchoring, providing the DNDAH coating with mechanical strength and structural stability. Alginate gel microspheres (AGMs) grafted with the same coupling agent formed the second reversible network and second anchoring, while coordinating with Cu²⁺ released from the primer to form a system buffering Cu²⁺ release, enabling long-term antibacterial protection and self-healing capabilities. FTIR, SEM, TEM, and elemental analyses confirmed the composition, morphology, and copper distribution within the A-H DL coating. A marine simulation experiment demonstrated exceptional stability and anti-fouling efficacy. This unique combination of features makes A-H DL a promising solution for diverse marine applications, from ship hulls to aquaculture equipment. Full article

Mineralized materials are gaining increased interest recently in a number of fields, especially in bone tissue engineering as bone replacement materials as well as in the architecture-built environment as structural building materials. Until the moment, there has not been a unified sustainable approach that addresses this multi-scale application objective by developing a self-mineralized material with minimum consumption of materials and processes. Thus, in the current study, a hydrogel developed from sodium alginate, gelatine, and calcium phosphate dibasic (CPDB) was optimized in terms of rheological properties and mineralization capacity through the formation of hydroxyapatite crystals. The hydrogel composition process adopted a three-stage, thermally induced chemical cross-linking to achieve a stable and enhanced hydrogel. The 6% CPDB-modified SA–gelatine hydrogel achieved the best rheological properties in terms of elasticity and hardness. Different concentrations of epigallocatechin gallate were tested as well as a rheological enhancer to optimize the hydrogel and to boost its anti-microbial properties. However, the results from the addition of EPGCG were not considered significant; thus, the 6% CPDB-modified SA–gelatine hydrogel was further tested for mineralization by incubation in various media, without and with cells, for 7 and 14 days, respectively, using scanning electron microscopy. The results revealed significantly enhanced mineralization of the hydrogel by forming hydroxyapatite platelets of the air-incubated hydrogel (without cells) in non-sterile conditions, exhibiting antimicrobial properties as well. Similarly, the air-incubated bioink with osteosarcoma SaOs-2 cells exhibited dense mineralized topology with hydroxyapatite crystals in the form of faceted spheres. Finally, the FBS-incubated hydrogel and FBS-incubated bioink, incubated for 7 and 14 days, respectively, exhibited less densely mineralized topology and less distribution of the hydroxyapatite crystals. The degradation rate of the hydrogel and bioink incubated in FBS after 14 days was determined by the increase in dimensions of the 3D-printed samples, which was between 5 to 20%, with increase in the bioink samples dimensions in comparison to their dimensions post cross-linking. Meanwhile, after 14 days, the hydrogel and bioink samples incubated in air exhibited shrinkage: a 2% decrease in the dimensions of the 3D-printed samples in comparison to their dimensions post cross-linking. The results prove the capacity of the developed hydrogel in achieving mineralized material with anti-microbial properties and a slow-to-moderate degradation rate for application in bone tissue engineering as well as in the built environment as a structural material using a sustainable approach. Full article

Gas inflow control in oil wells is one of the most challenging types of repair and sealing operations, the success rate of which does not exceed, as a rule, 30%. Conventional shutoff methods are often ineffective for this purpose. For instance, cement solutions cannot be injected into wells in the required volumes, while gel screens can only temporarily block the breakthrough zones, as gas easily seeps through the gel, forming new channels for gas inflow. Technology for the two-stage injection of gas-insulating gel systems for gas control in horizontal wells was developed. At the first stage, a self-generating foam gel composition (FGC), consisting of gel-forming and gas-forming compositions, was used. A foam gel structure with enhanced rheological and flow characteristics was formed over a controlled time as a result of the interaction between the gel-forming and gas-forming compounds. A PAM-based hydrogel crosslinked with an organic crosslinker was added to the FGC at the second stage of treatment. The laboratory experiments substantiated the technology of well gas and water shutoff by the sequential injection of self-generating foam gel composition and hydrogel. Field tests confirmed the correctness of the chosen concept. It is very important to clearly identify the sources of gas inflow for the success of this well intervention and take into account the well design, as well as the reservoir geological structure and characteristics. The gas shutoff operation can be properly designed for each well only by comparing all these factors. The validity of the selected technology was tested through a series of laboratory experiments. Successful laboratory tests allowed for the application of the studied technology in a field setting, where the gas shutoff agent was injected into three horizontal wells. As a result of the field application, the gas inflow was successfully isolated in two wells. However, the application of the technology failed in the third well which gave an opportunity to revisit the technology’s design and to review the sources of gas inflow. Overall, the achieved success rate of 66% demonstrated the high efficiency of the studied technology and supported its wider application in the field. Full article

Hydrogel-based dressings can effectively heal wounds by providing multiple functions, such as antibacterial, anti-inflammatory, and preangiogenic bioactivities. The ability to spray the dressing is important for the rapid and effective coverage of the wound surface. In this study, we developed a sprayable hydrogel-based wound dressing using naturally derived materials: hyaluronic acid and gelatin. We introduced methacrylate groups (HAMA and GelMA) to these materials to enable controllable photocrosslinking and form a stable hydrogel on the wound surface. To achieve sprayability, we evaluated the concentration of GelMA within a range of 5–15% (w/v) and then incorporated 1% (w/v) HAMA. Additionally, we incorporated calcium peroxide into the hydrogel at concentrations ranging from 0 to 12 mg/mL to provide self-oxygenation and antibacterial properties. The results showed that the composite hydrogels were sprayable and could provide oxygen for up to two weeks. The released oxygen relieved metabolic stress in fibroblasts and reduced cell death under hypoxia in in vitro culture. Furthermore, calcium peroxide added antibacterial properties to the wound dressing. In conclusion, the developed sprayable hydrogel dressing has the potential to be advantageous for wound healing due to its practical and conformable application, as well as its self-oxygenating and antibacterial functions. Full article

We designed and characterized chitosan–caseinate fibers processed through wet spinning for biomedical applications such as drug delivery from knitted medical devices. Sodium caseinate was either incorporated directly into the chitosan dope or allowed to diffuse into the chitosan hydrogel from a coagulation bath containing sodium caseinate and sodium hydroxide (NaOH). The latter route, where caseinate was incorporated in the neutralization bath, produced fibers with better mechanical properties for textile applications than those formed by the chitosan–caseinate mixed collodion route. The latter processing method consists of enriching a pre-formed chitosan hydrogel with caseinate, preserving the structure of the semicrystalline hydrogel without drastically affecting interactions involved in the chitosan self-assembly. Thus, dried fibers, after coagulation in a NaOH/sodium caseinate aqueous bath, exhibited preserved ultimate mechanical properties. The crystallinity ratio of chitosan was not significantly impacted by the presence of caseinate. However, when caseinate was incorporated into the chitosan dope, chitosan–caseinate fibers exhibited lower ultimate mechanical properties, possibly due to a lower entanglement density in the amorphous phase of the chitosan matrix. A standpoint is to optimize the chitosan–caseinate composition ratio and processing route to find a good compromise between the preservation of fiber mechanical properties and appropriate fiber composition for potential application in drug release. Full article

In this study, a new strategy was adopted for obtaining polymer/protein hybrid hydrogels with shape stability and tunable mechanical or rheological characteristics by using non-toxic procedures. A chemical network was created using a poly(vinyl alcohol)(PVA)/bovine serum albumin (BSA) mixture in aqueous solution in the presence of genipin and reduced glutathione (GSH). Then, a second physical network was formed through PVA after applying freezing/thawing cycles. In addition, the protein macromolecules formed intermolecular disulfide bridges in the presence of GSH. In these conditions, multiple crosslinked networks were obtained, determining the strengthening and stiffening into relatively tough porous hydrogels with tunable viscoelasticity and a self-healing ability. A SEM analysis evidenced the formation of networks with interconnected pores of sizes between 20 μm and 50 μm. The mechanical or rheological investigations showed that the hydrogels’ strength and response in different conditions of deformation were influenced by the composition and crosslinking procedure. Thus, the dynamics of the hybrid hydrogels can be adjusted to mimic the viscoelastic properties of the native tissues. The dynamic water vapor-sorption ability, swelling behavior in an aqueous environment, and bioadhesive properties were also investigated and are discussed in this paper. The hybrid hydrogels with tunable viscoelasticity can be designed on request, and they are promising candidates for tissue engineering, bioinks, and wound dressing applications. Full article

The photoantibacterial properties of titania nanoparticles (TiO₂NPs) are attracting much interest, but the separation of their suspension limits their application. In this study, the encapsulation of commercial TiO₂NPs within self-assembling tripeptide hydrogels to form hgel-TiO₂NP composites with significant photoantibacterial properties is reported. The Fmoc-Phe₃ hydrogelator was synthesized via an enzymatic method. The resulting composite was characterized with DLS, ζ-potential, SAXS, FESEM-EDS and rheological measurements. Two different concentrations of TiO₂NPs were used. The results showed that, by increasing the TiO₂NP quantity from 5 to 10 mg, the value of the elastic modulus doubled, while the swelling ratio decreased from 63.6 to 45.5%. The antimicrobial efficacy of hgel-TiO₂NPs was tested against a laboratory Staphylococcus aureus (S. aureus) strain and two methicillin-resistant S. aureus (MRSA) clinical isolates. Results highlighted a concentration-dependent superior antibacterial activity of hgel-TiO₂NPs over TiO₂NPs in the dark and after UV photoactivation. Notably, UV light exposure substantially increased the biocidal action of hgel-TiO₂NPs compared to TiO₂NPs. Surprisingly, in the absence of UV light, both composites significantly increased S. aureus growth relative to control groups. These findings support the role of hgel-TiO₂NPs as promising biocidal agents in clinical and sanitation contexts. However, they also signal concerns about TiO₂NP exposure influencing S. aureus virulence. Full article

Aiming at developing a dermal formulation against melanoma, the synthesized imidazo-pyrazoles 2-phenyl-2,3-dihydro-1H-imidazo[1,2-b]pyrazole-7-carboxylic acid (3-methoxy-4-phenoxy-benzylidene)-hydrazide (4G) and 2-phenyl-2,3-dihydro-1H-imidazo[1,2-b]pyrazole-7-carboxylic acid (4-benzyloxy-3-methoxy-benzylidene)-hydrazide (4I) were screened on patient-isolated melanoma cells (MEOV NT) and on Vemurafenib (PLX4032)-resistant (MEOV PLX-R) ones. Since 4I on MEOV PLX-R cells was 1.4-fold more effective than PLX, a hydrogel formulation containing 4I (R4HG-4I) was prepared in parallel with an empty R4-based hydrogel (R4HG) using a synthesized antibacterial resin (R4) as gelling agent. Thanks to its high hydrophilicity, porosity (85%), and excellent swelling capability (552%), R4 allowed to achieve R4HG and R4HG-4I with high equilibrium degree of swelling (EDS) and equilibrium water content (EWC). Chemometric-assisted ATR-FTIR analyses confirmed the chemical structure of swollen and fully dried (R4HG-D and R4HG-4I-D) hydrogels. The morphology of R4HG-D and R4HG-4I-D was examined by optical microscopy and SEM, while UV–vis analyses were carried out to obtain the drug loading (DL%) and the encapsulation efficiency (EE%) of R4HG-4I. Potentiometric titrations were performed to determine the equivalents of NH₃⁺ in both R4HG and R4HG-4I. The swelling and water release profiles of both materials and related kinetics were assessed by equilibrium swelling rate and water loss studies, respectively, while their biodegradability over time was assessed by in vitro degradation experiments determining their mass loss. Rheological experiments established that both R4HG and R4HG-4I are shear-thinning Bingham pseudoplastic fluids with low yield stress, thus assuring easy spreadability in a future topical application. Release studies evidenced a sustained and quantitative release of 4I governed mainly by diffusion. Upon favorable results from further experiments in a more realistic 3D model of melanoma, R4HG-4I could represent a starting point to develop new topical therapeutic options to adjuvate the treatments of melanoma cells also when resistant to currently available drugs. Full article

Osteogenic scaffolds reproducing the natural bone composition, structures, and properties have represented the possible frontier of artificially orthopedic implants with the great potential to revolutionize surgical strategies against the bone-related diseases. However, it is difficult to achieve an all-in-one formula with the simultaneous requirement of favorable biocompatibility, flexible adhesion, high mechanical strength, and osteogenic effects. Here in this work, an osteogenic hydrogel scaffold fabricated by inorganic-in-organic integration between amine-modified bioactive glass (ABG) nanoparticles and poly(ethylene glycol) succinimidyl glutarate-polyethyleneimine (TSG-PEI) network was introduced as an all-in-one tool to flexibly adhere onto the defective tissue and subsequently accelerate the bone formation. Since the N-hydroxysuccinimide (NHS)-ester of tetra-PEG-SG polymer could quickly react with the NH₂-abundant polyethyleneimine (PEI) polymer and ABG moieties, the TSG-PEI@ABG hydrogel was rapidly formed with tailorable structures and properties. Relying on the dense integration between the TSG-PEI network and ABG moieties on a nano-scale level, this hydrogel expressed powerful adhesion to tissue as well as durable stability for the engineered scaffolds. Therefore, its self-endowed biocompatibility, high adhesive strength, compressive modulus, and osteogenic potency enabled the prominent capacities on modulation of bone marrow mesenchymal stem cell (BMSCs) proliferation and differentiation, which may propose a potential strategy on the simultaneous scaffold fixation and bone regeneration promotion for the tissue engineering fields. Full article

The design and production of biodegradable and sustainable non-toxic materials for solar-energy harvesting and conversion is a significant challenge. Here, our goal was to report the preparation of novel protein/lipid hydrogels and demonstrate their utility in two orthogonal fundamental studies—light harvesting and white-light emission. Our hydrogels contained up to 90% water, while also being self-standing and injectable with a syringe. In one application, we loaded these hydrogels with suitable organic donor-acceptor dyes and demonstrated the energy-transfer cascade among four different dyes, with the most red-emitting dye as the energy destination. We hypothesized that the dyes were embedded in the protein/lipid phase away from the water pools as monomeric entities and that the excitation of any of the four dyes resulted in intense emission from the lowest-energy acceptor. In contrast to the energy-transfer cascade, we demonstrate the use of these gels to form a white-light-emitting hydrogel dye assembly, in which excitation migration is severely constrained. By restricting the dye-to-dye energy transfer, the blue, green, and red dyes emit at their respective wavelengths, thereby producing the composite white-light emission. The CIE color coordinates of the emission were 0.336 and 0.339—nearly pure white-light emission. Thus, two related studies with opposite requirements could be accommodated in the same hydrogel, which was made from edible ingredients by a simple method. These gels are biodegradable when released into the environment, sustainable, and may be of interest for energy applications. Full article

The reduction of tissue cytotoxicity and the improvement of cell viability are of utmost significance, particularly in the realm of green chemistry. Despite substantial progress, the threat of local infections remains a concern. Therefore, hydrogel systems that provide mechanical support and a harmonious balance between antimicrobial efficacy and cell viability are greatly needed. Our study explores the preparation of physically crosslinked, injectable, and antimicrobial hydrogels using biocompatible hyaluronic acid (HA) and antimicrobial ε-polylysine (ε-PL) in different weight ratios (10 wt% to 90 wt%). The crosslinking was achieved by forming a polyelectrolyte complex between HA and ε-PL. The influence of HA content on the resulting HA/ε-PL hydrogel physicochemical, mechanical, morphological, rheological, and antimicrobial properties was evaluated, followed by an inspection of their in vitro cytotoxicity and hemocompatibility. Within the study, injectable, self-healing HA/ε-PL hydrogels were developed. All hydrogels showed antimicrobial properties against S. aureus, P. aeruginosa, E. coli, and C. albicans, where HA/ε-PL 30:70 (wt%) composition reached nearly 100% killing efficiency. The antimicrobial activity was directly proportional to ε-PL content in the HA/ε-PL hydrogels. A decrease in ε-PL content led to a reduction of antimicrobial efficacy against S. aureus and C. albicans. Conversely, this decrease in ε-PL content in HA/ε-PL hydrogels was favourable for Balb/c 3T3 cells, leading to the cell viability of 152.57% for HA/ε-PL 70:30 and 142.67% for HA/ε-PL 80:20. The obtained results provide essential insights into the composition of the appropriate hydrogel systems able to provide not only mechanical support but also the antibacterial effect, which can offer opportunities for developing new, patient-safe, and environmentally friendly biomaterials. Full article