Measurement and Surface Complexation Modeling of U(VI) Adsorption to Engineered Iron Oxide Nanoparticles.

Abstract

Surface-functionalized magnetite nanoparticles have high capacity for U(VI) adsorption and can be easily separated from the aqueous phase by applying a magnetic field. A surface-engineered bilayer structure enables the stabilization of nanoparticles in aqueous solution. Functional groups in stearic acid (SA), oleic acid (OA), and octadecylphosphonic acid (ODP) coatings led to different adsorption extents (SA≈ OA > ODP) under the same conditions. The impact of water chemistry (initial loading of U(VI), pH, and the presence of carbonate) has been systematically examined for U(VI) adsorption to OA-coated nanoparticles. A diffuse double layer surface complexation model was developed for surface-functionalized magnetite nanoparticles that could simulate both the measured surface charge and the U(VI) adsorption behavior at the same time. With a small set of adsorption reactions for uranyl hydroxide and uranyl carbonate complexes to surface sites, the model can successfully simulate the entire adsorption data set over all uranium loadings, pH values, and dissolved inorganic carbon concentrations. The results show that the adsorption behavior was related to the changing U(VI) species and properties of surface coatings on nanoparticles. The model could also fit pH-dependent surface potential values that are consistent with measured zeta potentials.