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]

Dezerald, Lucile; Kohanoff, Jorge J.; Correa, Alfredo A.; Caro, Alfredo; Pellenq, Roland J. -M.; Ulm, Franz J.; Saul, Andres

doi:10.1021/acs.est.5b02609

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]

Journal Article · 28 October 2015 · Environmental Science and Technology

DOI: https://doi.org/10.1021/acs.est.5b02609 · OSTI ID:1377788

Dezerald, Lucile ^[1]; Kohanoff, Jorge J. ^[2]; Correa, Alfredo A. ^[3]; Caro, Alfredo ^[4]; Pellenq, Roland J. -M. ^[5]; Ulm, Franz J. ^[1]; Saul, Andres ^[5]

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)

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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Energy Dissipation to Defect Evolution (EDDE); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725; AC52-07NA27344

OSTI ID:: 1377788

Report Number(s):: LLNL-JRNL-736176

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 22 Vol. 49; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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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]