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Title: First-principles molecular dynamics simulation of the Ca2UO2(CO3)3 complex in water

Abstract

Recent experiments have shown that the neutral Ca2UO2(CO3)3 complex is the dominant species of uranium in many uranyl-containing streams. However, the structure and solvation of such a species in water has not been investigated from first principles. Herein we present a first principles molecular dynamics perspective of the Ca2UO2(CO3)3 complex in water based on density functional theory and Born–Oppenheimer approximation. We find that the Ca2UO2(CO3)3 complex is very stable in our simulation timeframe for three different concentrations considered and that the key distances from our simulation are in good agreement with the experimental data from extended X-ray absorption fine structure (EXAFS) spectroscopy. More important, we find that the two Ca ions bind differently in the complex, as a result of the hydrogen-bonding network around the whole complex. Furthermore, this finding invites confirmation from time-resolved EXAFS and has implications in understanding the dissociative equilibrium of the Ca2UO2(CO3)3 complex in water.

Authors:
 [1];  [1];  [1]
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  1. Univ. of California, Riverside, CA (United States)
Publication Date:
Research Org.:
Univ. of California, Riverside, CA (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1435625
Grant/Contract Number:  
NE0008397
Resource Type:
Accepted Manuscript
Journal Name:
Dalton Transactions
Additional Journal Information:
Journal Volume: 45; Journal Issue: 24; Journal ID: ISSN 1477-9226
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Priest, Chad, Tian, Ziqi, and Jiang, De-en. First-principles molecular dynamics simulation of the Ca2UO2(CO3)3 complex in water. United States: N. p., 2016. Web. doi:10.1039/c5dt04576b.
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Priest, Chad, Tian, Ziqi, & Jiang, De-en. First-principles molecular dynamics simulation of the Ca2UO2(CO3)3 complex in water. United States. https://doi.org/10.1039/c5dt04576b
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Priest, Chad, Tian, Ziqi, and Jiang, De-en. Fri . "First-principles molecular dynamics simulation of the Ca2UO2(CO3)3 complex in water". United States. https://doi.org/10.1039/c5dt04576b. https://www.osti.gov/servlets/purl/1435625.
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@article{osti_1435625,
title = {First-principles molecular dynamics simulation of the Ca2UO2(CO3)3 complex in water},
author = {Priest, Chad and Tian, Ziqi and Jiang, De-en},
abstractNote = {Recent experiments have shown that the neutral Ca2UO2(CO3)3 complex is the dominant species of uranium in many uranyl-containing streams. However, the structure and solvation of such a species in water has not been investigated from first principles. Herein we present a first principles molecular dynamics perspective of the Ca2UO2(CO3)3 complex in water based on density functional theory and Born–Oppenheimer approximation. We find that the Ca2UO2(CO3)3 complex is very stable in our simulation timeframe for three different concentrations considered and that the key distances from our simulation are in good agreement with the experimental data from extended X-ray absorption fine structure (EXAFS) spectroscopy. More important, we find that the two Ca ions bind differently in the complex, as a result of the hydrogen-bonding network around the whole complex. Furthermore, this finding invites confirmation from time-resolved EXAFS and has implications in understanding the dissociative equilibrium of the Ca2UO2(CO3)3 complex in water.},
doi = {10.1039/c5dt04576b},
journal = {Dalton Transactions},
number = 24,
volume = 45,
place = {United States},
year = {Fri Jan 22 00:00:00 EST 2016},
month = {Fri Jan 22 00:00:00 EST 2016}
}
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Journal Article:
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https://doi.org/10.1039/c5dt04576b
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Cited by: 23 works
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Figures / Tables:

Table 1 Table 1: Three concentrations of Ca2UO2(CO3)3, the corresponding water molecules in the simulation boxes, the box sizes, and the densities, examined in the present work
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    Works referencing / citing this record:

    X-Ray crystallographic and computational study on uranyl–salophen complexes bearing nitro groups
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