Uranyl-peroxide Nanocapsules in Aqueous Solution: Force Field Development and First Applications

Pere Mirò (1) , Vlaisavljevich Bess (1) , Allison L. Dzuback (1) , Hu Shuxian (2) , Peter C. Burns (3) , Christopher J. Cramer (1) , Riccardo Spezia (4) , Laura Gagliardi (1)

1 UMN - University of Minnesota System
2 Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, China
3 UND - University of Notre Dame [Indiana]
4 LAMBE - Laboratoire Analyse et Modélisation pour la Biologie et l'Environnement

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 Møller–Plesset perturbation theory and fit to a Born–Huggins–Mayer potential. Bonded parameters were fit from density functional theory calculations. The solvent and counterion structures surrounding four different systems ([(UVIO2)]2+, [(UVIO2)2(μ2-O2)]2+, [(UVIO2)5(μ2-O2)5], and [(UVIO2)20(μ2-O2)30]20-) were studied in aqueous solution. The largest studied system is predicted to encapsulate an ice-like water cluster.

Mots clés: Oxides; Counterions; Nanocapsules; Molecules; Cations

Domaines: Chimie-Physique [physics.chem-ph]

Pere Mirò, Vlaisavljevich Bess, Allison L. Dzuback, Hu Shuxian, Peter C. Burns, et al.. Uranyl-peroxide Nanocapsules in Aqueous Solution: Force Field Development and First Applications. Journal of Physical Chemistry C, 2014, 118 (42), pp.24730-24740. ⟨10.1021/jp504147s⟩. ⟨hal-01077293⟩