Uranium(VI) interaction with pyrite (FeS2): Chemical and spectroscopic studies

Abstract

The mechanism of uranium(VI) interaction with pyrite was studied by solution chemistry and X-ray Photoelectron Spectroscopy (XPS). Natural pyrite was characterized by X-Ray Diffraction (XRD) and Scanning Electron Microscopy (SEM). After equilibration in 10-2 mol L-1 NaNO3, pyrite was reacted with uranium(VI) by the batch method in an anoxic glove box (PO2 <1 ppm) at ambient temperature. The reaction products of uranium, iron and sulphur were characterized (oxidation state, chemical environment) by XPS. Quantitative analysis revealed that only a few atomic percent of uranium is retained at the pyrite surface. The U4f core level binding energies are consistent with the coexistence of an uranium(VI) species and of uranium in a reduced form. No sulphur oxidation products were observed by XPS, but spectral decomposition of the Fe2p lines revealed the presence of iron(III) oxide or (oxy)hydroxide. These results seem to point to a redox reaction between uranium(VI) and pyrite.