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A Study of Uranyl (VI) Chloride Complexes in Aqueous Solutions under Hydrothermal Conditions using Raman Spectroscopy

MRS Advances volume 5, pages 2623–2629 (2020)Cite this article

Abstract

The transport and deposition of uranium under hydrothermal conditions in the Earth’s crust has been a subject of ongoing study but is yet to be completely understood. In addition, there is little known about the fate of nuclear waste, consisting of uranium from spent fuel and other radioactive materials, upon storage in repositories or in nuclear reactor facilities. Because the nuclear waste often comes in contact with aqueous fluids in storage environments, studies of uranyl complexation with chloride and other ligands in aqueous media, to high temperature and pressure conditions, are needed. The primary purpose of this study was to investigate the speciation of aqueous uranyl (VI) chloride complexes, in solutions having a 0.05 M uranyl concentration and [Cl] concentrations ranging from 0.2 M to 6 M, under hydrothermal conditions. The aqueous uranyl chloride complexes in the samples were studied using Raman spectroscopy and the hydrothermal diamond anvil cell (HDAC), at temperatures up to 500 °C and pressures up to ~ 0.5 GPa. The uranyl bond stretching band feature occurring in the ~810 to 870 cm-1 region was fitted using the Voigt peak shape to determine the speciation of the equilibrium uranyl chloride complexes present in the samples. As expected, the n integer value of the UO2Cln+2-n complex species increases with the increase in temperature and chloride concentration, generally trending toward charge neutrality at high temperatures.

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Acknowledgments

Research presented in this article was supported by the Laboratory Directed Research and Development program of Los Alamos National Laboratory (LANL) under project number 20180007DR. LANL, an affirmative action/equal opportunity employer, is managed by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract 89233218CNA000001. We thank an anonymous reviewer for their valuable comments which have improved the manuscript.

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Authors and Affiliations

  1. Department of Physics, Astronomy and Materials Science, Missouri State University, Springfield, Missouri, U.S.A.

    Diwash Dhakal, Nadib Akram & Robert A. Mayanovic

  2. Earth and Environmental Sciences Division, Los Alamos National Laboratory, Los Alamos, New Mexico, 87545, U.S.A.

    Hakim Boukhalfa & Hongwu Xu

Authors
  1. Diwash Dhakal
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  2. Nadib Akram
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  3. Robert A. Mayanovic
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  4. Hakim Boukhalfa
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  5. Hongwu Xu
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Dhakal, D., Akram, N., Mayanovic, R.A. et al. A Study of Uranyl (VI) Chloride Complexes in Aqueous Solutions under Hydrothermal Conditions using Raman Spectroscopy. MRS Advances 5, 2623–2629 (2020). https://doi.org/10.1557/adv.2020.195

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  • DOI: https://doi.org/10.1557/adv.2020.195