Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

Giant uranium deposits formed from exceptionally uranium-rich acidic brines

Abstract

Giant uranium deposits were formed during the Mesoproterozoic era, 1.6–1.0 Gyr ago, in both Canada and Australia. The deposits are thought to have formed from large-scale circulation of brines at temperatures of 120–200 °C that percolated between sedimentary basins and underlying crystalline basement rocks1,2,3. However, the precise conditions for transport of the uranium in these brines are poorly understood4,5,6,7. Here we use mass spectrometry to analyse the uranium content of brines preserved in naturally occurring fluid inclusions in ore deposits from the Athabasca Basin, Canada. We measure concentrations of uranium in the range 1.0×10−6–2.8×10−3 mol l−1. These concentrations are three orders of magnitude above any other common crustal fluids. Experimentally, we measure the solubility of uranium as a function of NaCl content and pH, in mixtures that are analogous to ore-forming brines at 155 °C. To account for the high uranium content observed in the Athabasca deposits, we find that the brines must have been acidic, with a pH between 2.5 and 4.5. Our results strongly suggest that the world’s richest uranium deposits formed from highly concentrated uranium-bearing acidic brines. We conclude that these conditions are a necessary requirement for the formation of giant uranium deposits in relatively short periods of time of about 0.1–1 Myr, similar to other world-class deposits of lead–zinc and gold8,9.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Quartz-vein and fluid-inclusion petrography.
Figure 2: LA–ICP–MS determination of U concentration in fluid inclusions.
Figure 3: U(VI) solubility in H2O–NaCl mixtures at 155 °C and Psat as a function of pH155 °C and Na concentration.
Figure 4: Comparison of U concentrations in Athabasca U ore fluids (this study) with U concentration in various crustal fluids.

Similar content being viewed by others

References

  1. Kyser, T. K. & Cuney, M. in Recent and Not-so-Recent Developments in Uranium Deposits and Implications for Exploration (eds Cuney, M. &Kyser, T. K.) 161–219 (Mineralogical Association of Canada, 2008).

    Google Scholar 

  2. Boiron, M. C., Cathelineau, M. & Richard, A. Fluid flows and metal deposition near basement/cover unconformity: Lessons and analogies from Pb–Zn–F–Ba systems for the understanding of Proterozoic U deposits. Geofluids 10, 270–292 (2010).

    Google Scholar 

  3. Morichon, E., Beaufort, D., Allard, T. & Quirt, D. Tracing past migrations of uranium in Paleoproterozoic basins: New insights from radiation-induced defects in clay minerals. Geology 38, 983–986 (2010).

    Article  Google Scholar 

  4. Raffensperger, J. P. & Garven, G. The formation of unconformity-type uranium ore deposits 2. Coupled hydrochemical modeling. Am. J. Sci. 295, 639–696 (1995).

    Article  Google Scholar 

  5. Komninou, A. & Sverjensky, D. A. Geochemical modeling on the formation of an unconformity-type uranium deposit. Econ. Geol. 91, 590–606 (1996).

    Article  Google Scholar 

  6. Kister, P., Vieillard, P., Cuney, M., Quirt, D. & Laverret, E. Thermodynamic constraints on the mineralogical and fluid composition evolution in a clastic sedimentary basin: The Athabasca Basin (Saskatchewan, Canada). Eur. J. Mineral. 17, 325–342 (2005).

    Article  Google Scholar 

  7. Richard, A. et al. Brine–rock interaction in the Athabasca basement (McArthur River U deposit, Canada): Consequences for fluid chemistry and uranium uptake. Terra Nova 22, 303–308 (2010).

    Google Scholar 

  8. Simmons, S. F. & Brown, K. L. Gold in magmatic hydrothermal solutions and the rapid formation of a giant ore deposit. Science 314, 288–291 (2006).

    Article  Google Scholar 

  9. Wilkinson, J. J., Stoffell, B., Wilkinson, C. C., Jeffries, T. E. & Appold, M. S. Anomalously metal-rich fluids form hydrothermal ore deposits. Science 323, 764–767 (2009).

    Article  Google Scholar 

  10. Yardley, B. W. D. Metal concentration in crustal fluids and their relationships to ore formation. Econ. Geol. 100, 613–632 (2005).

    Article  Google Scholar 

  11. Audétat, A., Günther, D. & Heinrich, C. A. Formation of a magmatic-hydrothermal ore deposit: Insights with LA–ICP–MS analysis of fluid inclusions. Science 279, 2091–2094 (1998).

    Article  Google Scholar 

  12. Loucks, R. R. & Mavrogenes, J. A. Gold solubility in supercritical hydrothermal brines measured in synthetic fluid inclusions. Science 284, 2159–2163 (1999).

    Article  Google Scholar 

  13. Ulrich, T., Günther, D. & Heinrich, C. A. Gold concentrations of magmatic brines and the metal budget of porphyry copper deposits. Nature 399, 676–679 (1999).

    Article  Google Scholar 

  14. Pokrovski, G. S. & Dubrovinsky, L. S. The S3 ion is stable in geological fluids at elevated temperatures and pressures. Science 331, 1052–2054 (2011).

    Article  Google Scholar 

  15. Cuney, M. Evolution of uranium fractionation processes through time: Driving the secular variation of uranium deposit types. Econ. Geol. 105, 553–569 (2010).

    Article  Google Scholar 

  16. Kotzer, T. G. & Kyser, T. K. Petrogenesis of the Proterozoic Athabasca Basin, northern Saskatchewan, Canada, and its relation to diagenesis, hydrothermal uranium mineralization and paleohydrogeology. Chem. Geol. 120, 45–89 (1995).

    Article  Google Scholar 

  17. Derome, D. et al. Mixing of sodic and calcic brines and uranium deposition at McArthur River, Saskatchewan, Canada: A Raman and laser-induced breakdown spectroscopic study of fluid inclusions. Econ. Geol. 100, 1529–1545 (2005).

    Article  Google Scholar 

  18. Richard, A. et al. An evaporated seawater origin for the ore-forming brines in unconformity-related uranium deposits (Athabasca Basin, Canada): Cl/Br and δ37Cl study of fluid inclusions. Geochim. Cosmochim. Acta 75, 2792–2810 (2011).

    Article  Google Scholar 

  19. Hecht, L. & Cuney, M. Hydrothermal alteration of monazite in the Precambrian crystalline basement of the Athabasca Basin (Saskatchewan, Canada): Implication for the formation of unconformity-related uranium deposits. Miner. Deposita 35, 791–795 (2000).

    Article  Google Scholar 

  20. Mercadier, J., Richard, A., Boiron, M. C., Cathelineau, M. & Cuney, M. Migration of brines in the basement rocks of the Athabasca Basin through microfracture networks (P-Patch U deposit, Canada). Lithos 115, 121–136 (2010).

    Article  Google Scholar 

  21. Hoeve, J. & Quirt, D. A stationary redox front as a critical factor in the formation of high-grade, unconformity-type uranium ores in the Athabasca Basin, Saskatchewan, Canada. Bull. Mineral. 110, 151–171 (1987).

    Google Scholar 

  22. Grenthe, I. et al. Chemical Thermodynamics of Uranium (Nuclear Energy Agency, 1992).

    Google Scholar 

  23. Guillaumont, R. et al. Update on the Chemical Thermodynamics of U, Np, Pu, Am and Tc (Nuclear Energy Agency, 2003).

    Google Scholar 

  24. Heinrich, C. A. et al. Quantitative multi-element analysis of minerals, fluid and melt inclusions by laser-ablation inductively-coupled-plasma mass-spectrometry. Geochim. Cosmochim. Acta 67, 3473–3497 (2003).

    Article  Google Scholar 

  25. Allan, M. M. et al. Validation of LA–ICP–MS fluid inclusion analysis with synthetic fluid inclusions. Am. Mineral. 90, 1767–1775 (2005).

    Article  Google Scholar 

  26. Pitzer, K. S. & Li, Y. G. Thermodynamics of aqueous sodium chloride to 823 K and 1 kilobar (100 MPa). Proc. Natl Acad. Sci. USA 80, 7689–7693 (1983).

    Article  Google Scholar 

  27. Anderson, G. M. & Crerar, D. A. Thermodynamics in Geochemistry: The Equilibrium Model (Oxford Univ. Press, 1993).

    Google Scholar 

  28. Yates, D. M. & Rosenberg, P. E. Formation and stability of endmember illite: I. Solution equilibration experiments at 100–250 °C and Pv,soln . Geochim. Cosmochim. Acta 60, 1873–1883 (1996).

    Article  Google Scholar 

  29. Benison, K. C., Goldstein, R. H., Wopenka, B., Burruss, R. C. & Pasteris, J. D. Extremely acid Permian lakes and ground waters in North America. Nature 392, 911–914 (1998).

    Article  Google Scholar 

  30. Bali, E., Audétat, A. & Keppler, H. The mobility of U and Th in subduction zone fluids: An indicator of oxygen fugacity and salinity. Contrib. Mineral. Petrol. 161, 597–613 (2011).

    Article  Google Scholar 

  31. Longerich, H. P., Jackson, S. E. & Günther, D. J. Laser ablation inductively coupled plasma mass spectrometric transient signal data acquisition and analyte concentration calculation. Anal. At. Spectrom. 11, 899–904 (1996).

    Article  Google Scholar 

  32. Guillong, M., Meier, D. L., Allan, M. M., Heinrich, C. A. & Yardley, B. W. D. in Laser Ablation ICP–MS in the Earth Sciences: Current Practices and Outstanding Issues (ed. Sylvestor, P.) 328–333 (Mineralogical Association of Canada, 2008).

    Google Scholar 

  33. Lodding, W. & Ojamaa, L. Dehydration and thermal decomposition of uranyl nitrates in the presence of steam. J. Inorg. Nucl. Chem. 27, 1261–1268 (1965).

    Article  Google Scholar 

Download references

Acknowledgements

We thank Centre national de la recherche scientifique and Areva NC for financial support; Areva NC and Cameco for sampling and scientific collaboration; J. Cortot for ICP–atomic emission spectroscopy analyses; J. Grausem for the access to the Raman spectrometer; J. Dubessy, J. L. Vigneresse and B. W. D. Yardley for discussions and T. Pettke for help on early LA–ICP–MS work.

Author information

Authors and Affiliations

Authors

Contributions

M. Cuney, M. Cathelineau and M-C.B. conceived the project. J.M., M. Cathelineau and M. Cuney collected samples used in this study. A.R., M-C.B. and J.M. did the petrographic and microthermometric analyses of fluid inclusions. D.A.B., A.R. and M-C.B. carried out the LA–ICP–MS analyses of fluid inclusions. C.R. did the experimental U solubility measurements and analyses. A.R. and C.R. wrote the manuscript with contributions from all co-authors. All co-authors contributed to the discussion and interpretation of the data.

Corresponding authors

Correspondence to Antonin Richard or Julien Mercadier.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

Supplementary Information (PDF 577 kb)

Rights and permissions

Reprints and permissions

About this article

Cite this article

Richard, A., Rozsypal, C., Mercadier, J. et al. Giant uranium deposits formed from exceptionally uranium-rich acidic brines. Nature Geosci 5, 142–146 (2012). https://doi.org/10.1038/ngeo1338

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/ngeo1338

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing