Abstract
The Tulul Al Hammam area in central Jordan is an advantageous natural analogue site to study long-term U(VI) retention in ~ 1 Ma old U-bearing combustion metamorphic marbles with clinker-like mineralogy exposed to prolonged supergene alteration for at least ~ 100 kyr. The marbles contain abundant grains of high-temperature (ca. 800–850 °C) primary double Ca-U(VI) oxides (mainly Ca3UO6 and CaUO4), which are commonly replaced by hydrated calcium uranates with various impurities (Si, Fe, Al and F). A more hydrous natural analogue of X-phase (Ca2UO5·2-3H2O) occurs as a predominant secondary U compound after primary Ca-U(VI) oxides. The phase was studied by single-crystal XRD, SEM/EDX and electron microprobe (EPMA) analyses and Raman spectroscopy. It is a non-crystalline phase with a specific finger-like microtexture consisting of thin (no wider than 1–2 μm) lamellar particles. Its Raman spectrum shows a single strong band at 706–713 cm−1, sometimes coexisting with up to three weak diffuse bands (ν ~ 390, ~ 540 and 1355–1400 cm−1). The find of the natural X-phase (Ca2UO5·2-3H2O) is evidence of its long-term stability in a natural environment. It proves explicitly that the compound Ca2UO5·nH2O is a solubility-limiting phase in aged cements. The results have implications for geological disposal of radioactive wastes.
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Acknowledgments
The manuscript benefited much from the thoughtful review and valuable comments by Dr. Erica Bittarello and anonymous reviewer, as well as the helpful suggestions of Professor Abdullah M. Al-Amri, Editor-in-Chief of Arabian Journal of Geosciences. We greatly appreciate the assistance of Drs. N. Karmanov, E. Nigmatulina and M. Khlestov (Analytical Center for Multi-Elemental and Isotope Research, Novosibirsk) during the analytical work. T. Perepelova (IGM, Novosibirsk) is thanked for the helpful advice. The study was performed in accordance with the state assignment project No. 0330-2016-0004 as well as the Memorandum of Understanding on Academic Cooperation between the University of Jordan (Amman) and Sobolev Institute of Geology and Mineralogy Siberian Branch Russian Academy of Sciences (Novosibirsk).
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The Russian contribution was supported by grant 15-05-00760 from the Russian Foundation for Basic Research.
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Sokol, E., Kokh, S., Khoury, H. et al. Natural analogue approaches to prediction of long-term behaviour of Ca2UO5∙2-3H2O X-phase: case study from Tulul Al Hammam site, Jordan. Arab J Geosci 10, 512 (2017). https://doi.org/10.1007/s12517-017-3305-5
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DOI: https://doi.org/10.1007/s12517-017-3305-5