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Uranium and Multi-element Release from Orthogneiss and Granite (Austria): Experimental Approach Versus Groundwater Composition

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Abstract

In this study, the release of elements and in particular U from five Austrian orthogneiss and granite samples into a CO2-bearing solution was investigated to describe the initial phase (24 h) of leaching focusing on the impact of ferrous (hydro)oxide formation. Experiments were conducted at ambient temperature by flushing CO2:N2 gas through the reactive solution (pHinitial ~ 4.3) at a liquid:solid ratio of 10:1 with and without a reducing agent. The chemical evolution of the leaching solution was dominated by incongruent dissolution of silicates showing a parabolic kinetic behavior due to protective surface formation most likely caused by precipitation of amorphous FeIII/Al hydroxides. However, the relative distribution of Ca, Mg and Sr in the leaching solution excellently traced the individual bulk rock composition. The mobilization of U was highly prevented under oxidizing conditions by sorption onto ferrous (hydro)oxides, which were precipitating through ongoing silicate leaching. Therefore, the leaching behavior of individual U-bearing minerals was less relevant for U release. At reducing conditions, the above elements were accumulated in the solution, although an oversaturation regarding UIVO2 was calculated. This indicates its inhibited formation within the experimental run time. The composition of experimental leaching solutions did not reflect analyzed groundwater compositions from investigated local rock-type aquifers indicating that reaction rate constants of siliceous rocks significantly differ between values found in nature and in the laboratory. Change in active mineral surface areas with ongoing weathering, accumulation of secondary precipitates, leached layer formation and given reaction time are key factors for distinct elemental release.

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Acknowledgements

Funding of this study was provided through a PhD program from the Austrian Institute of Technology. We would like to thank the personnel involved in analytics from the following institutions: Seibersdorf Labor GmbH (hydrochemical analyses and rock chemistry analyses), Austrian Institute of Technology, Geological Survey of Austria - Department of Geochemistry and Department of Hydrogeology and Geothermics (REM analyses, XRF-analyses, heavy liquid separation, radon and hydrochemical analysis), University of Salzburg - Department of Chemistry and Physics of Materials (REM analyses) and Graz University of Technology - Institute of Technology and Testing of Building Materials (BET analyses).

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Authors and Affiliations

  1. Center for Energy, Electric Energy Systems, Austrian Institute of Technology GmbH, Giefinggasse 6, 1210, Vienna, Austria

    Daniel Elster & Edith Haslinger

  2. Institute of Applied Geosciences, Graz University of Technology, Rechbauerstraße 12, 8010, Graz, Austria

    Daniel Elster & Martin Dietzel

  3. Department of Hydrogeology and Geothermal Energy, Geological Survey of Austria, Neulinggasse 38, 1030, Vienna, Austria

    Daniel Elster & Gerhard Schubert

  4. Seibersdorf Labor GmbH, 2444, Seibersdorf, Austria

    Heinz Fröschl

Authors
  1. Daniel Elster
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  2. Edith Haslinger
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  3. Martin Dietzel
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  4. Heinz Fröschl
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  5. Gerhard Schubert
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Corresponding author

Correspondence to Daniel Elster.

Appendices

Appendix 1

See Table 3.

Table 3 Geochemical analyses of bulk rocks
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Appendix 2

See Table 4.

Table 4 Heavy liquid separation
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Appendix 3

See Fig. 7.

Fig. 7
figure 7

Chemical composition of rocks used for the leaching experiments a distribution of major elements, b distribution of trace elements, c distribution of REEs, d concentration of REEs and U in the separated heavy (> 2.89 g mL−1) and light fraction compared to the whole rock chemistry

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Appendix 4

See Table 5.

Table 5 Hydrochemical analysis of natural groundwater
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Appendix 5

See Fig. 8.

Fig. 8
figure 8

Chemical composition of typical local groundwater associated with the investigated rocks a distribution of major and chosen trace elements, b distribution of REEs

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Appendix 6

See Table 6.

Table 6 Elemental distribution during water–rock interaction experiments with the five sampled rock types under oxidizing conditions (experiment WR2)
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Appendix 7

See Table 7.

Table 7 Water–rock interaction experiments under reducing followed by oxidizing conditions for rock type ROM (experiment WR3)
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Appendix 8

See Table 8.

Table 8 Preliminary batch water–rock interaction experiments with UHP water and rock powder
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Elster, D., Haslinger, E., Dietzel, M. et al. Uranium and Multi-element Release from Orthogneiss and Granite (Austria): Experimental Approach Versus Groundwater Composition. Aquat Geochem 24, 279–306 (2018). https://doi.org/10.1007/s10498-018-9344-z

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