title: Uranyl Peroxide Cage Cluster Solubility in Water and the Role of the Electrical Double Layer.
abstract: Uranium concentrations as high as 2.94 × 105parts 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.
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Kathryn M
authors.initials: KM
authors.lastname: Peruski
authors.affiliation: Department of Chemistry, Minnesota Supercomputing Institute, University of Minnesota , Minneapolis, Minnesota 55455, United States.
authors.forename: Varinia
authors.initials: V
authors.lastname: Bernales
authors.affiliation: Department of Chemistry and Biochemistry, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Mateusz
authors.initials: M
authors.lastname: Dembowski
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Haylie L
authors.initials: HL
authors.lastname: Lobeck
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Kristi L
authors.initials: KL
authors.lastname: Pellegrini
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Ginger E
authors.initials: GE
authors.lastname: Sigmon
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Sarah
authors.initials: S
authors.lastname: Hickam
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Christine M
authors.initials: CM
authors.lastname: Wallace
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Jennifer E S
authors.initials: JE
authors.lastname: Szymanowski
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Enrica
authors.initials: E
authors.lastname: Balboni
authors.affiliation: Department of Chemistry, Minnesota Supercomputing Institute, University of Minnesota , Minneapolis, Minnesota 55455, United States.
authors.forename: Laura
authors.identifier: http://orcid.org/0000-0001-5227-1396
authors.initials: L
authors.lastname: Gagliardi
authors.affiliation: Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame , Notre Dame, Indiana 46556, United States.|Department of Chemistry and Biochemistry, University of Notre Dame , Notre Dame, Indiana 46556, United States.
authors.forename: Peter C
authors.identifier: http://orcid.org/0000-0002-2319-9628
authors.initials: PC
authors.lastname: Burns