Uranium Speciation - from mineral phases to mineral waters View Full Text


Ontology type: schema:Chapter     


Chapter Info

DATE

2008

AUTHORS

Gerhard Geipel , Gert Bernhard

ABSTRACT

Uranium ammunition can generate locally high concentrations of uranium in the environment. Weathering processes of the uranium metal lead in a first step to the formation of uranium minerals1. Depending on the composition of the soil the formation of several types of minerals can be estimated. Especially the content of phosphate from fertilizers and the aluminium from soil components are involved in the mineral formation. By use of time-resolved laser-induced fluorescence spectroscopy (TRLFS) the mineral type can be determined without any destruction. A large database of luminescence spectra, obtained from uranium minerals of the collection of the Technical University Mining Academy Freiberg, enables us to identify the formed uranium mineral2. It was found that mainly the mineral sabugalite was formed during weathering processes1. Other experiments with pure calcium and phosphate containing solution lead to the formation of the mineral meta-autunite3. In a second step the formed minerals than undergo further weathering processes, forming dissolved uranium species. In the former uranium mining areas of eastern Germany we could discover a new dissolved uranium carbonate species4,5. However, the uranium concentration of about 2 mg/L in these mining related waters is relatively high. Nevertheless the carbonate and calcium concentration are high enough to form a very stable discal-cium-uranyl-tricarbonate species. This species is of great importance, as its existence explains the uranium migration at the Hanford site6. In addition to the calcium species it can be stated that also the other alkaline earth elements form this type of alkaline earth uranyl carbonate species7,8,9,10. Following the uranium migration in the soil we could detect in the experiments that mainly carbonate species are formed. The pure carbonate species do not show any luminescence properties at room temperature. Therefore the samples have to be frozen to temperatures below 220 K11, in order to minimize the dynamic quench effect of the carbonate anion. This increases also the luminescence intensity and the luminescence lifetime of all carbonate containing species. Nevertheless, in one case of the soil experiment also hydroxo species were found. This may be connected to a non-equilibrium with atmospheric CO2 in this column. Following the possible transport of uranium under environmental conditions we may start with the weathering of uranium compounds in the soil or in a mining waste rock pile. The seepage water contains about 2 mg/L uranium and the speciation is mainly influenced be the formation of the dicalcium-uranyl-tricarbonate species. The input of these seepage water leads to a dilution of the uranium by about three orders of magnitude. Using the cryogenic technique in TRLFS12 we could also determine the uranium speciation in the river water nearby the former uranium mining area. The uranium concentration was about 2 μg/L uranium and in the river water mainly uranyl-tricarbonate species are formed. Despite this uranium can migrate down to the groundwater. In this case uranium may come back to the food chain by the production of mineral waters. We have studied the uranium speciation in several German mineral waters with uranium concentrations between 50 ng/L and 5 μg/L. In agreement with speciation calculations the sparkling and the calcium poor waters contain uranium as uranyltricarbonate species, whereas the non-sparkling waters if they are rich in calcium show clearly the formation of the dicalcium-uranyl-tricarbonate species. Using cryogenic TRLFS the detection limit for uranium species was estimated to be about 50 ng/L. Additionally a Hungarian medicinical water shows a uranium concentration of 150 μg/L. Due to the high mineralisation of this water also the dicalcium- uranyl-tricarbonate species was determined. Summarizing it can be concluded that the most natural waters contain uranium as tri-carbonate species. According to investigations of Carriere13 these uranium species are less hazardous than phosphate and citrate species. More... »

PAGES

599-602

Book

TITLE

Uranium, Mining and Hydrogeology

ISBN

978-3-540-87745-5
978-3-540-87746-2

Identifiers

URI

http://scigraph.springernature.com/pub.10.1007/978-3-540-87746-2_74

DOI

http://dx.doi.org/10.1007/978-3-540-87746-2_74

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1000087232


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