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• W2013212102 abstract "Atomistic simulations were performed to study the diffusion and adsorption of Ca(2)UO(2)(CO3)3 and of some of its constituent species, i.e., UO(2)2+, CO(3)2–, and UO(2)CO3, in feldspar nanosized fractures. Feldspar is important to uranium remediation efforts at the U.S. Department of Energy Hanford site as it has been found in recent studies to host contaminants within its intragrain fractures. In addition, uranyl carbonate species are known to dominate U(VI) speciation in conditions relevant to the Hanford site. Molecular dynamics (MD) simulations showed that the presence of the feldspar surface diminishes the diffusion coefficients of all of the species considered in this work and that the diffusion coefficients do not reach their bulk aqueous solution values in the center of a 2.5 nm fracture. Moreover, the MD simulations showed that the rate of decrease in the diffusion coefficients with decreasing distance from the surface is greater for larger adsorbing species. Free energy profiles of the same species adsorbing on the feldspar surface revealed a large favorable free energy of adsorption for UO(2)2+ and UO(2)CO3, which are able to adsorb to the surface with their uranium atom directly bonded to a surface hydroxyl oxygen, whereas adsorption of CO(3)2– and Ca(2)UO(2)(CO3)3, which attach to the surface via hydrogen bonding from a surface hydroxyl group to a carbonate oxygen, was calculated to be either only slightly favorable or unfavorable." @default.
• W2013212102 created "2016-06-24" @default.
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• W2013212102 date "2012-01-13" @default.
• W2013212102 modified "2023-10-16" @default.
• W2013212102 title "Diffusion and Adsorption of Uranyl Carbonate Species in Nanosized Mineral Fractures" @default.
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• W2013212102 doi "https://doi.org/10.1021/es2027696" @default.
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