The aim of the present work was to obtain drug-loaded hydrogels based on combinations of dextran, chitosan/gelatin/xanthan, and poly (acrylamide) as a sustained and controlled release vehicle of Doxorubicin, a drug used in skin cancer therapy that is associated with severe side effects. Hydrogels for use as 3D hydrophilic networks with good manipulation characteristics were produced using methacrylated biopolymer derivatives and the methacrylate group’s polymerization with synthetic monomers in the presence of a photo-initiator, under UV light stimulation (365 nm). Transformed infrared spectroscopy analysis (FT-IR) confirmed the hydrogels’ network structure (natural–synthetic composition and photocrosslinking), while scanning electron microscopy (SEM) analysis confirmed the microporous morphology. The hydrogels are swellable in simulated biological fluids and the material’s morphology regulates the swelling properties: the maximum swelling degree was obtained for dextran–chitosan-based hydrogels because of their higher porosity and pore distribution. The hydrogels are bioadhesive on a biological simulating membrane, and values for the force of detachment and work of adhesion are recommended for applications on skin tissue. The Doxorubicin was loaded into the hydrogels and the drug was released by diffusion for all the resulting hydrogels, with small contributions from the hydrogel networks’ relaxation. Doxorubicin-loaded hydrogels are efficient on keratinocytes tumor cells, the sustained released drug interrupting the cells’ division and inducing cell apoptosis; we recommend the obtained materials for the topical treatment of cutaneous squamous cell carcinoma.

Due to their indisputable biocompatibility and abundant source, biopolymers are widely used to prepare hydrogels for skin tissue engineering. Among them, cellulose is a great option for this challenging application due to its increased water retention capacity, mechanical strength, versatility and unlimited availability. Since algae are an unexploited source of cellulose, the novelty of this study is the decellularization of two different species, freshly collected from the Black Sea coast, using two different chemical surfactants (sodium dodecyl sulphate and Triton X-100), and characterisation of the resulted complex biopolymeric 3D matrices. The algae nature and decellularization agent significantly influenced the matrices porosity, while the values obtained for the hydration degree included them in hydrogel class. Moreover, their capacity to retain and then controllably release an anti-inflammatory drug, ibuprofen, led us to recommend the obtained structures as drug delivery systems. The decellularized macroalgae hydrogels are bioadhesive and cytocompatible in direct contact with human keratinocytes and represent a great support for cells. Finally, it was noticed that human keratinocytes (HaCaT cell line) adhered and populated the structures during a monitoring period of 14 days.

The study presents novel photocrosslinked hydrogels based on methacrylated chitosan and methacrylated gelatin/allyl-modified gelatin and compares their properties as drug delivery systems in wound healing applications. The polymers were selected due to their biocompatible, mucoadhesive, cell-interactive properties and flexibility in adjusting their structure, making them suitable candidates for applications that require tissue repair. A range of hydrogel formulations was obtained by modulating the ratio of modified chitosan to two distinct modified gelatins, with photocrosslinking performed using Irgacure 2959 as the photoinitiator. FT-IR analysis, SEM data, and swelling and mechanical properties confirmed the 3D networking and the compatibility between the hydrogel components. Allylic gelatin-based hydrogels present larger pores and a stronger pH-responsive swelling behaviour compared to methacrylated gelatin-based samples, reflecting the higher flexibility of allylic gelatin networks. The hydrogels release bacitracin during the first six hours, with a release profile that follows a non-Fickian diffusion mechanism. Cytocompatibility and wound healing potential were tested in the presence of human and mouse fibroblasts, cells with a pivotal role in the wound healing process. All formulated hydrogels exhibit antioxidant capacity and protein stabilization properties, which are attributed to the presence of chitosan in their composition. The cytocompatibility, in vitro wound healing, and biological properties of the obtained hydrogels, as well as the drug release results, confirm their suitability in wound healing applications.

This study describes, for the first time in the literature, a suitable approach to develop co-encapsulated magnetic nanoparticles based on fluorescent biotinylated N-palmitoyl chitosan, hydrophobic magnetite, Docetaxel and Verapamil. The multicomponent nanostructures were obtained using a two-step method: ultrasonication-induced self-assembly followed by ionic gelation. Structural composition was confirmed by infrared spectroscopy; the magnetic nanostructures displayed an average hydrodynamic diameter of 322.20 ± 2.50 nm, a positive surface charge (5.63 ± 0.16 mV), good magnetic saturation (13.35 emu/g) and superparamagnetic behavior. In vitro drug release studies revealed a pH-responsive behavior for both encapsulated agents, with an enhanced release of the Verapamil. Cytotoxicity evaluation using live/dead assays on MCF-7 tumor spheroids embedded in collagen-based hydrogels demonstrated a substantial therapeutic effect. Serum interleukin-8 (IL-8) levels were quantified to evaluate systemic inflammatory responses following intravenous administration of drug free magnetic nanoparticles. IL-8 concentrations were considerably increased at day 3, indicating an acute inflammatory response, decreased during the subacute phase (days 7 and 14) and returned to control levels by day 21, demonstrating good biocompatibility. No significant toxicity was observed for magnetic nanoparticles in the rats. Overall, these findings suggest that the developed magnetic nanoplatforms represents a promising candidate for breast cancer applications and merits further in vivo investigation to elucidate the action mechanism of encapsulated therapeutics and their pharmacologic activity.