Search Results (253)

This study focuses on the synthesis and characterization of thermoresponsive hydrogels of poly(lactic acid) (PLA) and poly(ethylene glycol) (PEG), PLA–PEG copolymers, aiming at the targeted and controlled release of deferoxamine (DFO), a clinically applied iron-chelating drug. Triblock (PLA-PEG-PLA) and diblock (mPEG-PLA) copolymers were synthesized using ring-opening polymerization (ROP) with five different PEGs with molecular weights of 1000, 1500, 2000, 4000, and 6000 g/mol and two types of lactide (L-lactide and D-lactide). Emulsions of the polymers in phosphate-buffered saline (PBS) were prepared at concentrations ranging from 10% to 50% w/w to study the sol–gel transition properties of the copolymers. Amongst the synthesized copolymers, only those that demonstrated thermoresponsive sol-to-gel transitions near physiological temperature (37 °C) were selected for further analysis. Structural and molecular confirmation was performed by Nuclear Magnetic Resonance (NMR) and Fourier-transform infrared spectroscopy (FTIR), while the molecular weights were determined via Gel Permeation Chromatography (GPC). The thermal transitions were studied by calorimetry (DSC) and crystallinity via X-ray diffraction (XRD) analysis. DFO-loaded hydrogels were prepared, and their drug release profiles were investigated under simulated physiological conditions (37 °C) for seven days using HPLC analysis. The thermoresponsive characteristics of these systems can offer a promising strategy for injectable drug delivery applications, where micelles serve as drug carriers and undergo in situ gelation, enabling controlled release. This alternative procedure may significantly improve the bioavailability of DFO and enhance patient compliance by addressing key limitations of conventional administration routes. Full article

Background/Objectives: This study presents the development and characterization of a novel thermoresponsive hydrogel composed of hyaluronic acid (HA), poloxamer 407, cannabidiol (CBD), and colloidal silver (Ag), designed for topical antimicrobial therapy. Methods: The Ag-CBD complex was first synthesized and subsequently incorporated into a HA–poloxamer gel matrix to produce a stable, sprayable formulation with suitable physicochemical properties for dermal applications. Results: The HA-Ag-CBD hybrid gel exhibited a physiological pH, a gelation temperature compatible with skin surface conditions, and favorable rheological behavior, including thixotropy and shear thinning—critical for uniform application and retention under dynamic conditions. Release studies confirmed a sustained delivery profile, supporting prolonged local activity of CBD and colloidal Ag. Antimicrobial assays demonstrated that the HA-Ag-CBD hybrid gel retained potent activity against Staphylococcus aureus and Candida albicans, with minimum inhibitory and bactericidal concentrations (MIC/MBC) statistically comparable to those of the unencapsulated Ag-CBD complex. Against E. coli, the HA-Ag-CBD hydrogel exhibited primarily bacteriostatic activity, with a low MIC (9.24 μg/mL) but a substantially higher MBC (387.35 μg/mL), consistent with the intrinsic structural resistance of Gram-negative bacteria. In contrast, bactericidal activity was more pronounced against Gram-positive strains, reflecting differential susceptibility related to bacterial envelope properties. CBD consistently demonstrated superior antimicrobial efficacy to colloidal Ag, while the Ag-CBD combination produced slightly enhanced, mainly additive effects, likely due to complementary membrane disruption and intracellular Ag⁺ ion activity. Cytotoxicity assays on normal human dermal fibroblasts confirmed that the HA-Ag-CBD hybrid gel maintained >70% cell viability at therapeutically relevant concentrations, in accordance with ISO 10993-5:2009 guidelines, and effectively mitigated the inherent cytotoxicity of the Ag-CBD complex. Conclusions: The HA-Ag-CBD hybrid gel demonstrates strong potential as a biocompatible, multifunctional topical formulation for the treatment of infected wounds and skin lesions. Future work will focus on in vivo evaluation, assessment of skin permeation, and further development to support translational applications. Full article

Poly(N-isopropylacrylamide) (PNIPAAm) hydrogels exhibit temperature-responsive volume changes near physiological temperature, but their low mechanical strength in the swollen state limits use in structurally demanding biomedical applications. In this study, we systematically investigated poly(NIPAAm-co-acrylamide), P(NIPAAm-co-AAm), hydrogels with varying AAm-to-NIPAAm ratios to explore the compositional trade-offs between thermal responsiveness and mechanical performance. Hydrogels were synthesized under fixed crosslinker and water content conditions, and evaluated through compressive mechanical testing, thermal swelling analysis, and crosslinking density estimation. Our results show that increasing AAm content enhances mechanical strength and stiffness but reduces the magnitude of temperature-induced volumetric shrinkage. An intermediate comonomer formulation demonstrated an optimal balance, maintaining both sufficient mechanical integrity for transdermal microneedle insertion and a reversible volume transition. This study highlights the potential of compositional tuning in hydrogel systems to meet the competing demands of responsiveness and durability in advanced biomedical applications. Full article

Thermoresponsive hydrogels that undergo reversible sol-gel transitions near physiological temperatures are highly attractive for biomedical applications, such as injectable drug delivery and embolization therapies. In this study, a library of polyurethane-based hydrogels was synthesized via step-growth polymerization using polyethylene glycol (PEG) of varying molecular weights, different diisocyanates, and a series of functional diols derived from diethanolamine with increasing hydrophobicity. The resulting polymers exhibited sol–gel transition behaviors without the need for external crosslinkers, relying solely on non-covalent interactions. The thermal responsiveness was systematically investigated using UV–Vis turbidimetry, and the cloud point temperature (T_CP) was found to be tunable within a range of 26–49 °C by modulating the monomer composition. Statistical modeling identified PEG molecular weight and diol structure as the primary determinants of T_CP, while diisocyanate type and diol-to-PEG ratio had negligible effects. Only diethanolamine (DEA)-based polymers formed stable hydrogels above a critical gelation temperature (LCGT), attributed to enhanced intermolecular interactions via free amine groups. In vitro degradation assays confirmed good hydrolytic stability under physiological conditions over four weeks, with degradation profiles strongly influenced by the PEG chain length and hydrophobic content. These findings establish a structure–property framework for the rational design of injectable, thermoresponsive polyurethane hydrogels with tailored sol–gel behavior for biomedical applications. Full article

Thermoresponsive Pluronic hydrogels offer a promising platform for localised antibiotic delivery. However, how drug loading affects the structural integrity and gelation of these systems remains underexplored. This study evaluates the impact of vancomycin on the physicochemical and self-assembly behaviour of Pluronic F127, F108, and F68 hydrogels. Rheological analysis revealed that vancomycin altered the critical micellisation and gelation temperatures (CMT and CGT, respectively), accelerating gelation in weak gel systems but disrupting network formation in stronger gels. Small-angle X-ray scattering (SAXS) showed that vancomycin suppressed micellar ordering, particularly along FCC (111) planes in F127, without inducing a phase transition. Scanning electron microscopy (SEM) imaging confirmed reduced pore integrity in vancomycin-loaded F127 and F108 gels, while 35% F68 gels failed to form stable structures at the tested concentrations despite enhanced drug solubility. F127 (18%) and F108 (22–23%) maintained gelation at 37 °C with reasonable mechanical strength and partial cubic ordering, making them suitable candidates for drug-eluting gels. These findings inform the design of thermoresponsive hydrogels for localised, implant-associated antibiotic delivery. Full article

Atmospheric water harvesting, as an emerging water collection technology, is expected to mitigate water resource crises. Adsorption-based atmospheric water harvesting technology offers distinct advantages, including geographical independence and reduced reliance on ambient humidity levels. Herein, a thermoresponsive gel (PNIPAM/TO-CNF) integrated with lithium chloride was constructed to achieve accelerated moisture sorption and rapid desorption capabilities. In the designated PNIPAM/TO-CNF/LiCl gel, PNIPAM provided a temperature-responsive hydrophilic–hydrophobic transition network; the hydrophilicity and structural strength were enhanced by TO-CNF, the moisture absorption capacity was dramatically elevated by hygroscopic salt LiCl, and pore-forming agent polyethylene glycol created a favorable porous structure. This synergistic design endows the gel with an optimized hydrophilic network, temperature-responsive behavior, and a porous architecture conducive to water vapor transportation, thereby achieving rapid moisture absorption and desorption. Under 60% relative humidity, the gel exhibited a water vapor adsorption capacity of 144% within 1 h, reaching its maximum absorption capacity of 178% after 140 min. The gel exhibited an even more superior desorption performance: when heated to 70 °C, its moisture content rapidly decreased to 16% of its initial weight within 1 h, corresponding to the desorption of 91% of the total absorbed water. A simplified pore-forming methodology that enables the integration of temperature-responsive properties with efficient moisture transfer channels was reported in this paper, providing a viable design pathway for achieving accelerated adsorption–desorption cycles in atmospheric water harvesting. Full article

Developing a rapidly gel-forming, in situ sprayable hydrogel with wound dressing functionality is essential for enhancing the wound healing process. In this study, a novel sprayable hydrogel-based wound dressing was developed by combining thermo- and pH- responsive polymers including Pluronic F127 (PF127) and N-succinyl chitosan (NSC). NSC was prepared by modifying chitosan with succinic anhydride, as confirmed by Fourier-transform infrared spectroscopy and nuclear magnetic resonance spectroscopy. The NSC synthesized using a succinic anhydride-to-chitosan molar ratio of 5:1 exhibited the highest degree of substitution, resulting in a water-soluble polymer effective over a broad pH range. The formulation process of the PF127:NSC sprayable hydrogel was optimized and evaluated based on its sol–gel phase transition behavior, clarity, gelation time, liquid and moisture management, stability, and cytotoxicity. These properties can be suitably tailored by adjusting the concentrations of PF127 and NSC. Moreover, the antioxidant capacity of the hydrogels was enhanced by incorporating Azadirachta indica (neem) extract, a bioactive compound, into the optimized sprayable hydrogel. Both neem release and antioxidant activity increased in a dose-dependent manner. Overall, the developed sprayable hydrogel exhibited favorable sprayability, appropriate gelation properties, controlled drug release, and antioxidant activity, underscoring its promising translational potential as a wound dressing. Full article

Periodontitis, a chronic inflammatory disease, causes alveolar bone loss. Current treatments show limitations in achieving dual antimicrobial and anti-inflammatory effects. We evaluated an emodin-loaded thermoresponsive hydrogel as a local drug delivery system for periodontitis treatment. Emodin itself demonstrated antibacterial activity against Porphyromonas gingivalis, with minimal inhibitory and minimal bactericidal concentrations of 50 μM. It also suppressed mRNA expression of proinflammatory cytokines [tumor necrosis factor alpha, interleukin (IL)-1β, and IL-6] in lipopolysaccharide-stimulated RAW 264.7 cells. The hydrogel, formulated with poloxamers and carboxymethylcellulose, remained in a liquid state at room temperature and formed a gel at 34 °C, providing sustained drug release for 96 h and demonstrating biocompatibility with human periodontal ligament stem cells while exhibiting antibacterial activity against P. gingivalis. In a rat model of periodontitis, the hydrogel significantly reduced alveolar bone loss and inflammatory responses, as confirmed by micro-computed tomography and reverse transcription quantitative polymerase chain reaction of gingival tissue. The dual antimicrobial and anti-inflammatory properties of emodin, combined with its thermoresponsive delivery system, provide advantages over conventional treatments by maintaining therapeutic concentrations in the periodontal pocket while minimizing systemic exposure. This shows the potential of emodin-loaded thermoresponsive hydrogels as effective local delivery systems for periodontitis treatment. Full article

Zwitterionic hydrogels have emerged as eco-friendly anti-fouling materials owing to their superior hydration-mediated resistance to biofouling. Nevertheless, their practical utility remains constrained by intrinsically poor mechanical robustness. Herein, this study proposes a novel strategy to develop novel tough zwitterionic hydrogels by freezing the gels’ polymer network. As a proof of concept, a zwitterionic hydrogel was synthesized via copolymerization of hydrophobic monomer phenyl methacrylate (PMA) and hydrophilic cationic monomer N-(3-dimethylaminopropyl) methacrylamide (DMAPMA), followed by post-oxidation to yield a zwitterionic structure. At service temperature, the rigid and hydrophobic PMA segments remain frozen, while the hydrophilic zwitterionic units maintain substantial water content by osmotic pressure. Synergistically, the zwitterionic hydrogel achieves robust toughness and adhesiveness, with high rigidity (66 MPa), strength (4.78 MPa), and toughness (2.53 MJ/m³). Moreover, the hydrogel exhibits a distinct temperature-dependent behavior by manifesting softer and more stretchable behavior after heating, since the thawing of the gel network at high temperatures increases segmental mobility. Therefore, it achieved satisfactory adhesiveness to substrates (80 kPa). Additionally, the hydrogel demonstrated remarkable anti-fouling performance, effectively suppressing biofilm formation and larval attachment. In summary, this work opens up promising prospects for the development of zwitterionic hydrogels with high application potential. Full article

In high-slope substrates, special requirements are imposed on sprayed ecological soil, which needs to exhibit high rheological properties before spraying and rapid curing after spraying. Traditional stabilizers are often unable to meet these demands. This study developed a thermo-responsive hydrogel stabilizer (HSZ) and applied it to ecological soil. The effects of HSZ on the rheological, mechanical, and vegetation performance of ecological soil were investigated, and the mechanism of the responsive carrier in the stabilizer was explored. The experimental results show that the ecological soil containing HSZ has high flowability before response, but its flowability rapidly decreases and consistency sharply increases after response. After the addition of HSZ, the 7 d unconfined compressive strength of the ecological soil reaches 1.55 MPa. The pH value of the ecological soil generally ranges from 6.5 to 8.0, and plant growth in a simulated vegetation box is favorable. Conductivity and viscosity tests demonstrate that the core–shell microcarriers, upon thermal response, release crosslinking components from the carrier, which rapidly react with the precursor solution components to form a curing system. This study provides a novel method for regulating ecological soil using a responsive stabilizer, further expanding its capacity to adapt to various complex scenarios. Full article

In this study, we present bi-layered hydrogel systems that incorporate different sizes and shapes of gold nanoparticles (nanospheres and nanorods) for potential use in areas such as photoactuators, soft robotics, artificial muscles, drug delivery and tissue engineering. The synthesized nano Au-PNiPAAm/PVA bi-layered hydrogel nanocomposites provide the unique ability to exhibit controlled motion upon light exposure, indicating that the above systems possess the capability of photo–thermal energy conversion. The chosen synthesis approach is a combination of chemical production of gold nanoparticles (AuNPs) followed by gamma radiation formation of crosslinked polymer networks around them, as the final step, which also allows for sterilization in a single technological step. According to the TEM analysis, the gold nanospheres (AuNSs) with mean diameters of around 17 and 30 nm, as well as nanorods (AuNRs) with an aspect ratio of around 4.5, were synthesized and used as nanofillers in the formation of nanocomposites. Their stability within the polymer matrix was confirmed by UV–Vis spectral studies, by the presence of local surface plasmon resonance (LSPR) bands, typical for nanoparticles of various shapes and sizes. Morphological studies (FE-SEM) of hydrogels revealed the formation of a porous structure with PNiPAAm hydrogel as an active layer and PVA hydrogel as a passive layer, as well as a stable interfacial layer with a thickness of around 80 μm. The synthesized bi-layered photoactuators showed a photo–thermal response upon exposure to irradiation of green lasers and lamps that simulate sunlight, resulting in bending motion. This bending response reveals the huge potential of the obtained materials as soft actuators, which are more flexible than rigid systems, making them effective for specific applications where controlled movement and flexibility are essential. Full article

In this paper, different poly((ethylene glycol)-(propylene glycol)) methacrylate (P(EGPG)MA) hydrogels were synthesized by gamma-radiation-induced polymerization and crosslinking from a monomer–bisolvent mixture using the following monomers: (ethylene glycol)₆ methacrylate (EG₆MA), ((ethylene glycol)₆-(propylene glycol)₃) methacrylate (EG₆PG₃MA), ((propylene glycol)₆-(ethylene glycol)₃) methacrylate (PG₆EG₃MA), and (propylene glycol)₅ methacrylate (PG₅MA), along with different water/ethanol compositions as the solvent. The monomer–bisolvent mixture was exposed to various radiation doses (5, 10, 15, 25, and 50 kGy). Considerable emphasis was placed on optimizing and tuning the reaction conditions necessary for the fabrication of methacrylic networks with pendant EGPG terminals. A further investigation was conducted on the effects of monomer composition, different preparation conditions, and radiation processing on thermal properties, microstructure, swelling behavior, and volume phase transition. Special attention was dedicated to PPG₆EG₃MA hydrogel, whose volume phase transition temperature is near physiological temperatures. This study identifies an optimal radiation dose and a water/ethanol solvent ratio for the synthesis of the radiation-induced hydrogels. Employing ionizing radiation within the sterilization dose range enables the simultaneous fabrication and sterilization of these hydrogels, offering an efficient production process. The findings provide new insights into the role of bisolvent composition on hydrogel formation and properties, and they present practical guidelines for optimizing hydrogel synthesis across a wide range of applications. Full article

Background/Objectives: The management of ocular tumours is faced with the challenge of developing a suitable treatment strategy with consideration of the anatomical and physiological protective barriers of the eye. Interferon alpha has been employed to treat patients with ocular tumours for decades; however, its short half-life and poor tolerability necessitate frequent administration. This study focuses on the design of an injectable pH-responsive and protective nanoparticle system dispersed into a thermo-responsive hydrogel for site-specific sustained delivery of interferon alpha (IFN-α2b) in the treatment of ocular surface tumours. Methods: The synthesis of a poly(ethylene glycol)-poly(caprolactone)-poly(ethylene glycol) (PEG-PCL-PEG) triblock copolymer (PECE) was undertaken. The IFN-α2b was encapsulated in poly(β-amino ester) (PBAE) nanoparticles (NP) with pH-responsive characteristics to proposedly release the IFNα-2b in response to the acidic nature of the tumour microenvironment. This was followed by characterisation via Fourier transform infrared spectroscopy (FT-IR), ¹H-nuclear magnetic resonance (¹H-NMR) analysis, differential scanning calorimetry (DSC), X-ray powder diffraction (XRPD) analysis, thermogravimetric analysis (TGA), and thermal-transition analysis of the PECE hydrogels. Results: Release studies demonstrated that the PBAE nanoparticulate PEG-PCL-PEG hydrogel was both pH-responsive, while providing controlled release of IFN-α2b, and thermo-responsive. Release analysis highlighted that IFN-α2b-loaded NP dispersed into the hydrogel (IFNH) further prolonged the release of IFN-α2b with a pH-responsive yet controlled release rate in an acidic environment simulating a tumour microenvironment. The developed system proved to be biocompatible with human retinal pigment epithelial cells and the released IFN-α demonstrated bioactivity in the presence of an A172 glioblastoma cell line. Conclusions: In conclusion, the PECE hydrogel has promising potential for application as an ocular drug delivery system for the treatment of ocular tumours and could potentially overcome and prevent the drawbacks associated with the commercially available IFN-α2b injection. Full article

Background: Spinal cord injury (SCI) is a devastating neurological condition with limited therapeutic options. Current clinical interventions predominantly rely on prolonged or high-dose pharmacological regimens, often causing systemic toxicity and adverse events. Although black phosphorus nanosheets (BPNSs) exhibit remarkable reactive oxygen species (ROS)-scavenging capacity to mitigate oxidative damage, their rapid degradation severely compromises their therapeutic efficacy. Methods: This study presents a thermosensitive hydrogel with rapid gelation properties by incorporating different proportions and concentrations of sodium alginate (SA) into a chitosan/β-glycerophosphate (CS/β-GP) hydrogel and loading it with BPNS for the treatment of SCI in rats. In vitro, the physical properties of the composite were characterized and the cytotoxicity and ROS scavenging abilities were assessed using PC12 cells; in vivo, behavioral tests, histopathological analysis, transcriptomics, immunohistochemistry, and Western blotting were performed to explore the therapeutic effects and mechanisms. Results: The results demonstrate that this hydrogel effectively slows BPNS degradation, exhibits a high ROS scavenging capacity, reduces lipid peroxidation, and thereby inhibits ferroptosis and apoptosis, offering neuroprotective effects and promoting motor function recovery. Conclusions: Our findings establish the CS/β-GP/SA-BPNS hydrogel as a multifunctional therapeutic platform for SCI, synergizing sustained drug release with ROS–ferroptosis–apoptosis axis modulation to achieve neuroprotection and functional restoration. This strategy provides a translatable paradigm for combining nanotechnology and biomaterial engineering in neural repair. Full article

Background/Objective: A clinical need exists for more effective therapeutics and sustained drug delivery systems to promote ocular surface healing. This study tested the hypothesis that a novel biodegradable, thermoresponsive hydrogel loaded with the human recombinant (rh)MG53 protein, which we have demonstrated to promote corneal healing without fibrosis, would exhibit safety and biocompatibility in vitro and in vivo. Methods: Hydrogel optimization was performed based on varying concentrations of poloxamer 407, poloxamer 188, and hydroxypropyl methylcellulose. Hydrogels were characterized and potential toxicity was evaluated in vitro in cultured corneal epithelium, fibroblasts, and endothelium. In vivo safety and tolerability were assessed in mice and hydrogels were used to evaluate corneal healing following alkali injury. Results: The optimized hydrogel formulation did not result in any detrimental changes to the corneal cells and released functional rhMG53 protein for at least 24 h. In vivo rhMG53-loaded hydrogels improved re-epithelialization, reduced stromal opacification and vascularization, and promoted corneal nerve density. Mechanistically, rhMG53 reduced vascular endothelial cell migration and tube formation by inhibiting pSTAT3 signaling. Conclusions: Taken together, our poloxamer-based thermoresponsive hydrogel effectively released rhMG53 protein and enhanced multiple corneal healing outcomes. Full article