ABSTRACT
In this work, the design of a new generation of functionalized large pore silica nanoparticles is addressed for the specific removal of iron from biological environments. Herein, mesoporous silica with a large pore stellate morphology, denoted STMS, were grafted with the highly specific iron chelating agent desferrioxamine B, DFoB. The challenge of this work was the step by step elaboration of the nanoplatform and the evaluation of its chelating efficiency and selectivity. Hence, the controlled covalent grafting of DFoB specific iron chelator, was successfully achieved ensuring a high grafting rate of chelating ligand of 730 nmol·mg-1 (i.e., 0.85 ligand·nm-2). Furthermore, these highly chelating STMS silica were able to capture iron(III) stabilized with nitrilotriacetic acid (NTA) in solution at physiological pH with a fast kinetics (less than 30 min). For a stoichiometry 0.85:1 (FeNTA : DFoB), the STMS-DFoB nanoparticles allowed reaching capture capacity and efficiency of 480 nmolFe3+/mg SiO2 and 78%, respectively. Regarding the selectivity features of the removal process, studies were performed with two different media composed of various metal ions: (i) an equimolar solution of various metal cations and (ii) a Barth's buffer mimicking the brain solution composition. In both cases, the chelating STMS-DFoB showed a high selectivity for iron versus other ions at the same (Al3+) or different valency (Na+, K+ ). Finally, this work paves the way for new nanosystems for metal overload treatments as well as for future highly chelating nanoplatforms that can be used at the interface between depollution and nanomedecine.
