Langmuir, Vol.22, No.5, 2141-2145, 2006
Modeling adsorption of the uranyl dication on the hydroxylated (alpha-Al2O3(0001) surface in an aqueous medium. Density functional study
As a first step toward modeling the interaction of dissolved actinide contaminants with mineral surfaces. we studied low-coverage adsorption of aqueous uranyl, UO22+, oil the hydroxylated alpha-Al2O3(0001) surface. We carried out density functional periodic slab model calculations and modeled solvation effects by explicit aqua ligands. We explored the formation of both inner- and outer-sphere complexes and estimated the Corresponding adsorption energies. Effects of solvation were accounted for by explicit consideration of the first hydration shell of uranyl and by means of a posteriori corrections for long-range solvent effect. With energetics described at the GGA-PW91 level and under the assumption of a fully protonated ideal surface, we predict a weakly bound outer-sphere adsorption complex.