@article {37, title = {Docking 90 Sr radionuclide in cement: An atomistic modeling study}, journal = {Physics and Chemistry of the Earth, Parts A/B/C}, volume = {70{\textendash}71}, year = {2014}, month = {2014}, pages = {39{\textendash}44}, abstract = {

Cementitious materials are considered to be a waste form for the ultimate disposal of radioactive materials in geological repositories. We investigated by means of atomistic simulations the encapsulation of strontium-90, an important radionuclide, in calcium\–silicate\–hydrate (C\–S\–H) and its crystalline analog, the 9\ \Å-tobermorite. C\–S\–H is the major binding phase of cement. Strontium was shown to energetically favor substituting calcium in the interlayer sites in C\–S\–H and 9\ \Å-tobermorite with the trend more pronounced in the latter. The integrity of the silicate chains in both cementitious waste forms were not affected by strontium substitution within the time span of molecular dynamics simulation. Finally, we observed a limited degradation of the mechanical properties in the strontium-containing cementitious waste form with the increasing strontium concentration. These results suggest the cement hydrate as a good candidate for immobilizing radioactive strontium.

Image for unlabelled figure

}, doi = {10.1016/j.pce.2013.11.007}, author = {Youssef, Mostafa and Roland Jean-Marc Pellenq and Bilge Yildiz} } @article {97, title = {Docking Sr-90 radionuclide in cement: An atomistic modeling study}, journal = {Physics and Chemistry of the Earth}, volume = {70-71}, year = {2014}, month = {2014}, pages = {39-44}, type = {Article}, abstract = {

Cementitious materials are considered to be a waste form for the ultimate disposal of radioactive materials in geological repositories. We investigated by means of atomistic simulations the encapsulation of strontium-90, an important radionuclide, in calcium silicate hydrate (C-S-H) and its crystalline analog, the 9 angstrom-tobermorite. C-S-H is the major binding phase of cement. Strontium was shown to energetically favor substituting calcium in the interlayer sites in C-S-H and 9 angstrom-tobermorite with the trend more pronounced in the latter. The integrity of the silicate chains in both cementitious waste forms were not affected by strontium substitution within the time span of molecular dynamics simulation. Finally, we observed a limited degradation of the mechanical properties in the strontium-containing cementitious waste form with the increasing strontium concentration. These results suggest the cement hydrate as a good candidate for immobilizing radioactive strontium. (C) 2013 Elsevier Ltd. All rights reserved.

}, keywords = {Cement, mechanical properties, Molecular simulation, Nuclear waste storage}, issn = {1474-7065}, doi = {10.1016/j.pce.2013.11.007}, author = {Youssef, Mostafa and Roland Jean-Marc Pellenq and Bilge Yildiz} } @article {292, title = {Glassy Nature of Water in an Ultraconfining Disordered Material: The Case of Calcium-Silicate-Hydrate}, journal = {Journal of the American Chemical Society}, volume = {133}, year = {2011}, month = {Mar-02-2011}, pages = {2499 - 2510}, abstract = {
Abstract Image

We present the structural and dynamic nature of water ultraconfined in the quasi-two-dimensional nanopores of the highly disordered calcium\−silicate\−hydrate (C-S-H), the major binding phase in cement. Our approach is based on classical molecular simulations. We demonstrate that the C-S-H nanopore space is hydrophilic, particularly because of the nonbridging oxygen atoms on the disordered silicate chains which serve as hydrogen-bond acceptor sites, directionally orienting the hydrogen atoms of the interfacial water molecules toward the calcium\−silicate layers. The water in this interlayer space adopts a unique multirange structure: a distorted tetrahedral coordination at short range up to 2.7 \Å, a disordered structure similar to that of dense fluids and supercooled phases at intermediate range up to 4.2 \Å, and persisting spatial correlations through dipole\−dipole interactions up to 10 \Å. A three-stage dynamics governs the mean square displacement (MSD) of water molecules, with a clear cage stage characteristic of the dynamics in supercooled liquids and glasses, consistent with its intermediate-range structure identified here. At the intermediate time scales corresponding to the \β-relaxation of glassy materials, coincident with the cage stage in MSD, the non-Gaussian parameter indicates a significant heterogeneity in the translational dynamics. This dynamic heterogeneity is induced primarily because of the heterogeneity in the distribution of hydrogen bond strengths. The strongly attractive interactions of water molecules with the calcium silicate walls serve to constrain their motion. Our findings have important implications on describing the cohesion and mechanical behavior of cement from its setting to its aging.

}, issn = {0002-7863}, doi = {10.1021/ja107003a}, author = {Youssef, Mostafa and Roland Jean-Marc Pellenq and Bilge Yildiz} }