TY - JOUR
T1 - Uranyl-peroxide nanocapsules in aqueous solution
T2 - Force field development and first applications
AU - Miró, Pere
AU - Vlaisavljevich, Bess
AU - Dzubak, Allison L.
AU - Hu, Shuxian
AU - Burns, Peter C.
AU - Cramer, Christopher J.
AU - Spezia, Riccardo
AU - Gagliardi, Laura
PY - 2014/10/23
Y1 - 2014/10/23
N2 - 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.
AB - 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.
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U2 - 10.1021/jp504147s
DO - 10.1021/jp504147s
M3 - Article
AN - SCOPUS:84908112335
VL - 118
SP - 24730
EP - 24740
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 42
ER -