Journal article
Uranyl-Peroxide Nanocapsules in Aqueous Solution: Force Field Development and First Applications
Journal of physical chemistry. C, Vol.118(42), pp.24730-24740
10/23/2014
DOI: 10.1021/jp504147s
Abstract
The self-assembly of uranyl-peroxide nanocapsules in aqueous solution is unique in uranium chemistry and has potential applications in the fabrication and reprocessing of actinide-based materials. We present the first study of these species in aqueous solution by means of classical molecular dynamics simulations. To this end, we parametrized a uranyl-peroxide force field from interaction energies computed with second order MollerPlesset perturbation theory and fit to a BornHugginsMayer potential. Bonded parameters were fit from density functional theory calculations. The solvent and counterion structures surrounding four different systems ([((UO2)-O-VI)](2+), [((UO2)-O-VI)(2)(mu(2)-O-2)](2+), [((UO2)-O-VI)(5)(mu(2)-O-2)(5)], and [((UO2)-O-VI)(20)(mu 2-O-2)(30)](20-)) were studied in aqueous solution. The largest studied system is predicted to encapsulate an ice-like water cluster.
Details
- Title: Subtitle
- Uranyl-Peroxide Nanocapsules in Aqueous Solution: Force Field Development and First Applications
- Creators
- Pere Miro - University of Minnesota SystemBess Vlaisavljevich - University of Minnesota SystemAllison L. Dzubak - University of Minnesota SystemShuxian Hu - Guangzhou Institute of GeochemistryPeter C. Burns - University of Notre DameChristopher J. Cramer - University of Minnesota SystemRiccardo Spezia - Laboratoire Analyse et Modélisation pour la Biologie et l'EnvironnementLaura Gagliardi - University of Minnesota System
- Resource Type
- Journal article
- Publication Details
- Journal of physical chemistry. C, Vol.118(42), pp.24730-24740
- DOI
- 10.1021/jp504147s
- ISSN
- 1932-7447
- eISSN
- 1932-7455
- Publisher
- Amer Chemical Soc
- Number of pages
- 11
- Grant note
- DE-SC0001015 / US Department of Energy; United States Department of Energy (DOE) 2010 JCJC 080701 ACLASOLV / ANR; Agence Nationale de la Recherche (ANR) Materials Science of Actinides, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science; United States Department of Energy (DOE) DE-SC0001089 / Materials Science of Actinides, an Energy Frontier Research Center - U.S. Department of Energy, Office of Basic Energy Sciences; United States Department of Energy (DOE) University of Minnesota; University of Minnesota System CHE-0952054 / U.S. National Science Foundation; National Science Foundation (NSF)
- Language
- English
- Date published
- 10/23/2014
- Academic Unit
- Chemistry
- Record Identifier
- 9984618649502771
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