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