Uranyl Peroxide Cage Cluster Solubility in Water and the Role of the Electrical Double Layer

Kathryn M. Peruski; Varinia Bernales; Mateusz Dembowski; Haylie L. Lobeck; Kristi L. Pellegrini; Ginger E. Sigmon; Sarah Hickam; Christine M. Wallace; Jennifer E.S. Szymanowski; Enrica Balboni; Laura Gagliardi; Peter C. Burns

doi:10.1021/acs.inorgchem.6b02435

Uranyl Peroxide Cage Cluster Solubility in Water and the Role of the Electrical Double Layer

Kathryn M. Peruski, Varinia Bernales, Mateusz Dembowski, Haylie L. Lobeck, Kristi L. Pellegrini, Ginger E. Sigmon, Sarah Hickam, Christine M. Wallace, Jennifer E.S. Szymanowski, Enrica Balboni, Laura Gagliardi, Peter C. Burns

Research output: Contribution to journal › Article › peer-review

28 Scopus citations

Abstract

Uranium concentrations as high as 2.94 × 10⁵ parts per million (1.82 mol of U/1 kg of H₂O) occur in water containing nanoscale uranyl cage clusters. The anionic cage clusters, with diameters of 1.5-2.5 nm, are charge-balanced by encapsulated cations, as well as cations within their electrical double layer in solution. The concentration of uranium in these systems is impacted by the countercations (K, Li, Na), and molecular dynamics simulations have predicted their distributions in selected cases. Formation of uranyl cages prevents hydrolysis reactions that would result in formation of insoluble uranyl solids under alkaline conditions, and these spherical clusters reach concentrations that require close packing in solution.

Original language	English
Pages (from-to)	1333-1339
Number of pages	7
Journal	Inorganic Chemistry
Volume	56
Issue number	3
DOIs	https://doi.org/10.1021/acs.inorgchem.6b02435
State	Published - Feb 6 2017
Externally published	Yes

Funding

This research is funded by the Office of Basic Energy Sciences of the U.S. Department of Energy as part of the Materials Science of Actinides Energy Frontier Research Center (DESC0001089).

Funders	Funder number
Office of Basic Energy Sciences
U.S. Department of Energy	DESC0001089

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10.1021/acs.inorgchem.6b02435

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Peruski, K. M., Bernales, V., Dembowski, M., Lobeck, H. L., Pellegrini, K. L., Sigmon, G. E., Hickam, S., Wallace, C. M., Szymanowski, J. E. S., Balboni, E., Gagliardi, L., & Burns, P. C. (2017). Uranyl Peroxide Cage Cluster Solubility in Water and the Role of the Electrical Double Layer. Inorganic Chemistry, 56(3), 1333-1339. https://doi.org/10.1021/acs.inorgchem.6b02435

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abstract = "Uranium concentrations as high as 2.94 × 105 parts per million (1.82 mol of U/1 kg of H2O) occur in water containing nanoscale uranyl cage clusters. The anionic cage clusters, with diameters of 1.5-2.5 nm, are charge-balanced by encapsulated cations, as well as cations within their electrical double layer in solution. The concentration of uranium in these systems is impacted by the countercations (K, Li, Na), and molecular dynamics simulations have predicted their distributions in selected cases. Formation of uranyl cages prevents hydrolysis reactions that would result in formation of insoluble uranyl solids under alkaline conditions, and these spherical clusters reach concentrations that require close packing in solution.",

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AU - Peruski, Kathryn M.

AU - Bernales, Varinia

AU - Dembowski, Mateusz

AU - Lobeck, Haylie L.

AU - Pellegrini, Kristi L.

AU - Sigmon, Ginger E.

AU - Hickam, Sarah

AU - Wallace, Christine M.

AU - Szymanowski, Jennifer E.S.

AU - Balboni, Enrica

AU - Gagliardi, Laura

AU - Burns, Peter C.

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AB - Uranium concentrations as high as 2.94 × 105 parts per million (1.82 mol of U/1 kg of H2O) occur in water containing nanoscale uranyl cage clusters. The anionic cage clusters, with diameters of 1.5-2.5 nm, are charge-balanced by encapsulated cations, as well as cations within their electrical double layer in solution. The concentration of uranium in these systems is impacted by the countercations (K, Li, Na), and molecular dynamics simulations have predicted their distributions in selected cases. Formation of uranyl cages prevents hydrolysis reactions that would result in formation of insoluble uranyl solids under alkaline conditions, and these spherical clusters reach concentrations that require close packing in solution.

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Uranyl Peroxide Cage Cluster Solubility in Water and the Role of the Electrical Double Layer

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