Adsorption mechanisms of cesium at calcium-silicate-hydrate surfaces using molecular dynamics simulations

Bu, J.; Gonzalez Teresa, R.; Brown, K. G.; Sanchez, F.

doi:10.1016/j.jnucmat.2018.12.007

Adsorption mechanisms of cesium at calcium-silicate-hydrate surfaces using molecular dynamics simulations

Journal Article · Wed Dec 05 00:00:00 EST 2018 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2018.12.007· OSTI ID:1613755

Bu, J. ^[1]; Gonzalez Teresa, R. ^[2]; Brown, K. G. ^[2]; Sanchez, F. ^[2]

Vanderbilt University, Nashville, TN (United States); DOE/OSTI
Vanderbilt University, Nashville, TN (United States)

We report understanding the mechanisms of interactions and immobilization of radionuclides in cement systems at the molecular level is key to developing safe and novel solutions for the long-term storage of nuclear wastes. The molecular level adsorption mechanisms of cesium (Cs⁺) ions onto tobermorite 9 Å, tobermorite 14 Å, and jennite – three crystalline structural analogues for calcium-silicate-hydrates, the main components in cement-based materials, were investigated using molecular dynamics (MD) simulations. Convergence monitoring of the simulations, using the root mean square displacement with average correlation analysis, indicated that MD trajectories of 10–15 ns were needed given the size of the selected computational cell to properly capture the dynamic process of adsorption. Cs⁺ ions adsorbed as inner-sphere complexes at the tobermorite surfaces, while they showed lower affinity for jennite. The charge and structure of the surface layer strongly influenced the adsorption mechanisms of Cs⁺ ions. Strong association with the hexagonal cavities of the silica sites were seen at the tetrahedral SiO₄ surface of the tobermorite structures. Cs⁺ ion adsorption was attributed to co-ion adsorption at the octahedral CaO₆ surface of tobermorite 9 Å, cation exchange at that of tobermorite 14 Å, and electrostatic interaction with the surface hydroxyl groups for jennite. Distribution coefficients of Cs⁺ ions onto cement pastes derived from molecular dynamics by taking the surface structure and dynamics of Cs⁺ ions directly into account showed a range of overlap with experimental results.

View Accepted Manuscript (DOE)

Research Organization:: Vanderbilt University, Nashville, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FC01-06EW07053

OSTI ID:: 1613755

Alternate ID(s):: OSTI ID: 1635962
OSTI ID: 22886822

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Journal Issue: C Vol. 515; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Adsorption mechanisms of cesium at calcium-silicate-hydrate surfaces using molecular dynamics simulations

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