Molecular dynamics simulations of uranyl adsorption and structure on the basal surface of muscovite
Abstract
Anthropogenic activities have led to an increased concentration of uranium on the Earth’s surface and potentially in the subsurface with the development of nuclear waste repositories. Uranium is soluble in groundwater, and its mobility is strongly affected by the presence of clay minerals in soils and in subsurface sediments. We use molecular dynamics simulations to probe the adsorption of aqueous uranyl (UO22+) ions onto the basal surface of muscovite, a suitable proxy for typically ultrafine-grained clay phases. Model systems include the competitive adsorption between potassium counterions and aqueous ions (0.1 M and 1.0 M UO2Cl2 , 0.1 M NaCl). We find that for systems with potassium and uranyl ions present, potassium ions dominate the adsorption phenomenon. Potassium ions adsorb entirely as inner-sphere complexes associated with the ditrigonal cavity of the basal surface. Uranyl ions adsorb in two configurations when it is the only ion species present, and in a single configuration in the presence of potassium. Finally, the majority of adsorbed uranyl ions are tilted less than 45° relative to the muscovite surface, and are associated with the Si4Al2 rings near aluminum substitution sites.
- Authors:
-
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Geochemistry Department
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1082222
- Report Number(s):
- SAND2013-4522J
Journal ID: ISSN 0892-7022; 456021
- Grant/Contract Number:
- AC04-94AL85000
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Molecular Simulation
- Additional Journal Information:
- Journal Volume: 40; Journal Issue: 7-9; Related Information: Proposed for publication in Molecular Simulation.; Journal ID: ISSN 0892-7022
- Publisher:
- Taylor & Francis
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; mica; uranium; surface charge; electrolyte
Citation Formats
Teich-McGoldrick, Stephanie L., Greathouse, Jeffery A., and Cygan, Randall T. Molecular dynamics simulations of uranyl adsorption and structure on the basal surface of muscovite. United States: N. p., 2014.
Web. doi:10.1080/08927022.2013.838675.
Teich-McGoldrick, Stephanie L., Greathouse, Jeffery A., & Cygan, Randall T. Molecular dynamics simulations of uranyl adsorption and structure on the basal surface of muscovite. United States. https://doi.org/10.1080/08927022.2013.838675
Teich-McGoldrick, Stephanie L., Greathouse, Jeffery A., and Cygan, Randall T. Wed .
"Molecular dynamics simulations of uranyl adsorption and structure on the basal surface of muscovite". United States. https://doi.org/10.1080/08927022.2013.838675. https://www.osti.gov/servlets/purl/1082222.
@article{osti_1082222,
title = {Molecular dynamics simulations of uranyl adsorption and structure on the basal surface of muscovite},
author = {Teich-McGoldrick, Stephanie L. and Greathouse, Jeffery A. and Cygan, Randall T.},
abstractNote = {Anthropogenic activities have led to an increased concentration of uranium on the Earth’s surface and potentially in the subsurface with the development of nuclear waste repositories. Uranium is soluble in groundwater, and its mobility is strongly affected by the presence of clay minerals in soils and in subsurface sediments. We use molecular dynamics simulations to probe the adsorption of aqueous uranyl (UO22+) ions onto the basal surface of muscovite, a suitable proxy for typically ultrafine-grained clay phases. Model systems include the competitive adsorption between potassium counterions and aqueous ions (0.1 M and 1.0 M UO2Cl2 , 0.1 M NaCl). We find that for systems with potassium and uranyl ions present, potassium ions dominate the adsorption phenomenon. Potassium ions adsorb entirely as inner-sphere complexes associated with the ditrigonal cavity of the basal surface. Uranyl ions adsorb in two configurations when it is the only ion species present, and in a single configuration in the presence of potassium. Finally, the majority of adsorbed uranyl ions are tilted less than 45° relative to the muscovite surface, and are associated with the Si4Al2 rings near aluminum substitution sites.},
doi = {10.1080/08927022.2013.838675},
journal = {Molecular Simulation},
number = 7-9,
volume = 40,
place = {United States},
year = {Wed Feb 05 00:00:00 EST 2014},
month = {Wed Feb 05 00:00:00 EST 2014}
}
Web of Science
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