Cement As a Waste Form for Nuclear Fission Products: The Case of 90Sr and Its Daughters [Cement As a Container for Nuclear Fission Products: The Case of 90Sr and Its Daughters]
Abstract
One of the main challenges faced by the nuclear industry is the long-term confinement of nuclear waste. Because it is inexpensive and easy to manufacture, cement is the material of choice to store large volumes of radioactive materials, in particular the low-level medium-lived fission products. It is therefore of utmost importance to assess the chemical and structural stability of cement containing radioactive species. Here, we use ab initio calculations based on density functional theory (DFT) to study the effects of 90Sr insertion and decay in C–S–H (calcium-silicate-hydrate) in order to test the ability of cement to trap and hold this radioactive fission product and to investigate the consequences of its β-decay on the cement paste structure. We show that 90Sr is stable when it substitutes the Ca2+ ions in C–S–H, and so is its daughter nucleus 90Y after β-decay. Interestingly, 90Zr, daughter of 90Y and final product in the decay sequence, is found to be unstable compared to the bulk phase of the element at zero K but stable when compared to the solvated ion in water. Furthermore, cement appears as a suitable waste form for 90Sr storage.
- Authors:
-
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); MultiScale Material Science for Energy and Environment, Cambridge, MA (United States)
- Queen's Univ. Belfast, Belfast (United Kingdom)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); MultiScale Material Science for Energy and Environment, Cambridge, MA (United States); Aix-Marseille Univ., Marseille cedex (France)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Energy Dissipation to Defect Evolution (EDDE)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1377788
- Report Number(s):
- LLNL-JRNL-736176
Journal ID: ISSN 0013-936X
- Grant/Contract Number:
- AC52-07NA27344; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 49; Journal Issue: 22; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES
Citation Formats
Dezerald, Lucile, Kohanoff, Jorge J., Correa, Alfredo A., Caro, Alfredo, Pellenq, Roland J. -M., Ulm, Franz J., and Saul, Andres. Cement As a Waste Form for Nuclear Fission Products: The Case of 90Sr and Its Daughters [Cement As a Container for Nuclear Fission Products: The Case of 90Sr and Its Daughters]. United States: N. p., 2015.
Web. doi:10.1021/acs.est.5b02609.
Dezerald, Lucile, Kohanoff, Jorge J., Correa, Alfredo A., Caro, Alfredo, Pellenq, Roland J. -M., Ulm, Franz J., & Saul, Andres. Cement As a Waste Form for Nuclear Fission Products: The Case of 90Sr and Its Daughters [Cement As a Container for Nuclear Fission Products: The Case of 90Sr and Its Daughters]. United States. https://doi.org/10.1021/acs.est.5b02609
Dezerald, Lucile, Kohanoff, Jorge J., Correa, Alfredo A., Caro, Alfredo, Pellenq, Roland J. -M., Ulm, Franz J., and Saul, Andres. Thu .
"Cement As a Waste Form for Nuclear Fission Products: The Case of 90Sr and Its Daughters [Cement As a Container for Nuclear Fission Products: The Case of 90Sr and Its Daughters]". United States. https://doi.org/10.1021/acs.est.5b02609. https://www.osti.gov/servlets/purl/1377788.
@article{osti_1377788,
title = {Cement As a Waste Form for Nuclear Fission Products: The Case of 90Sr and Its Daughters [Cement As a Container for Nuclear Fission Products: The Case of 90Sr and Its Daughters]},
author = {Dezerald, Lucile and Kohanoff, Jorge J. and Correa, Alfredo A. and Caro, Alfredo and Pellenq, Roland J. -M. and Ulm, Franz J. and Saul, Andres},
abstractNote = {One of the main challenges faced by the nuclear industry is the long-term confinement of nuclear waste. Because it is inexpensive and easy to manufacture, cement is the material of choice to store large volumes of radioactive materials, in particular the low-level medium-lived fission products. It is therefore of utmost importance to assess the chemical and structural stability of cement containing radioactive species. Here, we use ab initio calculations based on density functional theory (DFT) to study the effects of 90Sr insertion and decay in C–S–H (calcium-silicate-hydrate) in order to test the ability of cement to trap and hold this radioactive fission product and to investigate the consequences of its β-decay on the cement paste structure. We show that 90Sr is stable when it substitutes the Ca2+ ions in C–S–H, and so is its daughter nucleus 90Y after β-decay. Interestingly, 90Zr, daughter of 90Y and final product in the decay sequence, is found to be unstable compared to the bulk phase of the element at zero K but stable when compared to the solvated ion in water. Furthermore, cement appears as a suitable waste form for 90Sr storage.},
doi = {10.1021/acs.est.5b02609},
journal = {Environmental Science and Technology},
number = 22,
volume = 49,
place = {United States},
year = {Thu Oct 29 00:00:00 EDT 2015},
month = {Thu Oct 29 00:00:00 EDT 2015}
}
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