Uranyl-peroxide nanocapsules in aqueous solution: Force field development and first applications

Pere Miró; Bess Vlaisavljevich; Allison L. Dzubak; Shuxian Hu; Peter C. Burns; Christopher J. Cramer; Riccardo Spezia; Laura Gagliardi

doi:10.1021/jp504147s

Uranyl-peroxide nanocapsules in aqueous solution: Force field development and first applications

Pere Miró, Bess Vlaisavljevich, Allison L. Dzubak, Shuxian Hu, Peter C. Burns, Christopher J. Cramer, Riccardo Spezia, Laura Gagliardi

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

20 Scopus citations

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 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 ([(U^VIO₂)]²⁺, [(U^VIO₂)₂(μ²-O₂)]²⁺, [(U^VIO₂)₅(μ²-O₂)₅], and [(U^VIO₂)₂₀(μ²-O₂)₃₀]^20-) were studied in aqueous solution. The largest studied system is predicted to encapsulate an ice-like water cluster.

Original language	English (US)
Pages (from-to)	24730-24740
Number of pages	11
Journal	Journal of Physical Chemistry C
Volume	118
Issue number	42
DOIs	https://doi.org/10.1021/jp504147s
State	Published - Oct 23 2014

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© 2014 American Chemical Society.

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title = "Uranyl-peroxide nanocapsules in aqueous solution: Force field development and first applications",

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 M{\o}ller-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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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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Uranyl-peroxide nanocapsules in aqueous solution: Force field development and first applications

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