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Abstract

Hemochromatosis can be described as a medical condition with excessive iron accumulation in the body. There are two types of hemochromatosis, which include hereditary and acquired. Acquired hemochromatosis, as seen in patients with β-thalassemia and sickle cell disease, is due to transfusion-induced during the management of anaemia. When there is iron ++overload in the body, this can lead to the generation of reactive oxygen species, which can affect the heart, brain, liver, pancreas, joints, etc. One of the most established treatment strategies for hemochromatosis is iron chelation therapy, with deferoxamine being described clinically as the most successful in removing excess iron from the body. Deferoxamine is a clinically approved iron chelator and is a standard treatment in the management of hemochromatosis, but suffers from poor oral bioavailability, clinical toxicity, poor patient adherence, and suboptimal pharmacokinetics, necessitating prolonged intravenous infusion regimens. To address these issues, we developed two distinct: oral delivery strategies and which include:(1) self-assembled polymeric nanoparticles based on hyaluronic acid (HA, MW 15 kDa) conjugated with bile acids— deoxycholic acid (DOCA) or taurocholic acid (TCA)—and DFO, and (2) deferoxamine-loaded nanostructured lipid carriers (DFO-NLCs) engineered using glyceryl monooleate and oleic acid, with poloxamer 188 as surfactant and a chitosan-alginate coating to enhance stability in gastric environments and gastrointestinal permeation. In this dissertation, HA-BA-DFO conjugates were synthesized and formulated into self assembled nanoparticles. The structural integrity was investigated with NMR, FTIR, and UV-Vis spectroscopy. It was observed that TCA9-HA-DFO displayed superior in vitro permeability and lower cytotoxicity compared to free DFO, while maintaining effective iron-chelating activity. For the second strategy, a Quality by Design (QbD) framework with Design of Experiments (DOE) was applied to optimize DFO-NLC formulations. Physicochemical characterization showed that formulations (F2, F3, and F5) demonstrated desirable particle size, encapsulation efficiency, DFO loading, and controlled release profiles, with F2 exhibiting the most sustained DFO release. With these two approaches, it was observed that both highlighted promising strategies that can be exploited to overcome the limitations of current DFO therapy. This offers huge potential for the development of safe, effective, and patient-friendly oral formulations that enhance therapeutic outcomes in iron-overload disorders.

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