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Identification of the uranium speciation in an underground acid mine drainage environment |
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| Authors: | Thuro Arnold Nils Baumann Sina Brockmann Udo Zimmermann Stephan Weiß |
| Institution: | a Helmholtz-Zentrum Dresden-Rossendorf, Institute of Radiochemistry, P.O. Box 510119, D-01314 Dresden, Germany b Technical University Dresden, Radiochemistry, D-01062 Dresden, Germany c Wismut GmbH, Jagdschänkenstraße 29, 09117 Chemnitz, Germany |
| Abstract: | The subsurface acid mine drainage (AMD) environment of an abandoned underground uranium mine in Königstein/Saxony/Germany, currently in the process of remediation, is characterized by low pH, high sulfate concentrations and elevated concentrations of heavy metals, in particular uranium. Acid streamers thrive in the mine drainage channels and are heavily coated with iron precipitates. These precipitates are biologically mediated iron precipitates and related to the presence of Fe-oxidizing microorganisms forming copious biofilms in and on the Fe-precipitates. Similar biomineralisations were also observed in stalactite-like dripstones, called snottites, growing on the gallery ceilings.The uranium speciation in these solutions of underground AMD waters flowing in mine galleries as well as dripping from the ceiling and forming stalactite-like dripstones were studied by time resolved laser-induced fluorescence spectroscopy (TRLFS). The fluorescence lifetime of uranium species in both AMD water environments were best described with a mono-exponential decay, indicating the presence of one major species. The detected positions of the emission bands and by comparing it in a fingerprinting procedure with spectra obtained for acid sulfate reference solutions, in particular Fe(III) - SO42− - UO22+ reference solutions, indicated that the uranium speciation in the AMD environment of Königstein is dominated in the pH range of 2.5-3.0 by the highly mobile aquatic uranium sulfate species UO2SO4(aq) and formation of uranium precipitates is rather unlikely as is retardation by sorption processes. The presence of iron in the AMD reduces the fluorescence lifetime of the UO2SO4(aq) species from 4.3 μs, found in iron-free uranium sulfate reference solutions, to 0.7 μs observed in both AMD waters of Königstein and also in the iron containing uranium sulfate reference solutions.Colloids were not observed in both drainage water and dripping snottite water as photon correlation spectroscopy analyses and centrifugation experiments at different centrifugal accelerations between 500g and 46000g revealed. Thus transport and uranium speciation at the investigated AMD sites is neither influenced by U(IV) or U(VI) eigencolloids nor by uranium adsorbed on colloidal particles.This study shows that TRLFS is a suitable spectroscopic technique to identify the uranium speciation in bulk solutions of AMD environments. |
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