Uranyl鈥揚eroxide Nanocapsules in Aqueous Solution: Force Field Development and First Applications
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- 作者：Pere Mir贸 ; Bess Vlaisavljevich ; Allison L. Dzubak ; Shuxian Hu ; Peter C. Burns ; Christopher J. Cramer ; Riccardo Spezia ; Laura Gagliardi
- 刊名：Journal of Physical Chemistry C
- 出版年：2014
- 出版时间：October 23, 2014
- 年：2014
- 卷：118
- 期：42
- 页码：24730-24740
- 全文大小：478K
- ISSN：1932-7455
文摘
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酶ller鈥揚lesset perturbation theory and fit to a Born鈥揌uggins鈥揗ayer potential. Bonded parameters were fit from density functional theory calculations. The solvent and counterion structures surrounding four different systems ([(UVIO2)]2+, [(UVIO2)2(渭2-O2)]2+, [(UVIO2)5(渭2-O2)5], and [(UVIO2)20(渭2-O2)30]20-) were studied in aqueous solution. The largest studied system is predicted to encapsulate an ice-like water cluster.