Abstract
Residual solid-phase uranium from former mill tailings leachate can contribute to persistent concentrations of uranium in groundwater that exceed regulatory levels. Microscale characterization of uranium-contaminated sediment samples is lacking due to the challenges of detecting uranium at the parts-per-million level and identifying its associations with co-occurring elements. An emerging methodology, fission-track radiography, was applied to detect the low-level solid-phase uranium in sediments. Scanning electron microscopy and energy-dispersive X-ray spectroscopy were used to elucidate the uranium associations with co-occurring aluminum, and iron. Uranium-contaminated sediments were collected from upgradient source zone aquifer sediments in Riverton, Wyoming, USA, where the residual uranium was present. The combined microscopic analyses revealed that in the water-saturated layers, solid-phase uranium primarily co-occurred with amorphous aluminum (Al)-rich and iron (Fe)-rich coatings in the source zone. The unique geochemical associations of solid-phase uranium with the co-occurring Al-rich and Fe-rich coatings suggest that a select suite of equilibrium and kinetic reactions controls its persistence in groundwater. The identification of the uranium co-associations at a former uranium mill tailings site indicates that fission-track radiography with spectroscopic methods can be utilized in uranium-contaminated sites that contain trace-level solid-phase uranium and can inform conceptual and geochemical models for further mechanistic insight.
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Acknowledgements
Financial support was provided by the National Science Foundation (NSF) under award number 2229869, the 2022 Geological Society of America (GSA) Graduate Student Research Grant program under grant number 13597-22 and the U.S. Department of Energy Office of Legacy Management through contract number 89303020DLM000001, task order number 89303022FLM400039. The authors express their gratitude to Dr. Heather A. Owen, Director of Electron Microscope Laboratory at the Department of Biological Sciences, University of Wisconsin-Milwaukee, for her guidance on operating the electron microscope. The authors also thank the anonymous reviewers and Editors-in-Chief Olaf Kolditz and Yan Zheng for their invaluable comments that improved the manuscript from its previous version.
Funding
Financial support was provided by the National Science Foundation (NSF) under award number 2229869, the 2022 Geological Society of America (GSA) Graduate Student Research Grant program under grant number 13597-22 and the U.S. Department of Energy Office of Legacy Management through contract number 89303020DLM000001, task order number 89303022FLM400039.
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RS did spectroscopic and light microscopic lab data acquisition, performed data analysis, and wrote the manuscript. MAD reviewed and edited the manuscript critically. CJP reviewed and edited the manuscript critically. RHJ did fission-track radiography lab data acquisition, performed data analysis, and supervised the manuscript.
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Sultana, R., Dangelmayr, M.A., Paradis, C.J. et al. Combining fission-track radiography and scanning electron microscopy to identify uranium host phases. Environ Earth Sci 83, 56 (2024). https://doi.org/10.1007/s12665-023-11373-5
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DOI: https://doi.org/10.1007/s12665-023-11373-5