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 · Thu Oct 29 00:00:00 EDT 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:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Energy Dissipation to Defect Evolution (EDDE)

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

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

OSTI ID:: 1377788

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

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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References (47)

Radiation effects in crystalline ceramics for the immobilization of high-level nuclear waste and plutonium Weber, W. J.; Ewing, R. C.; Catlow, C. R. A. Journal of Materials Research, Vol. 13, Issue 6 https://doi.org/10.1557/JMR.1998.0205	journal	June 1998
Radiation effects in nuclear waste forms for high-level radioactive waste Ewing, R. C.; Weber, W. J.; Clinard, F. W. Progress in Nuclear Energy, Vol. 29, Issue 2 https://doi.org/10.1016/0149-1970(94)00016-Y	journal	January 1995
Assessment of individual radionuclide distributions from the Fukushima nuclear accident covering central-east Japan Kinoshita, N.; Sueki, K.; Sasa, K. Proceedings of the National Academy of Sciences, Vol. 108, Issue 49 https://doi.org/10.1073/pnas.1111724108	journal	November 2011
Preliminary Estimation of Release Amounts of ¹³¹ I and ¹³⁷ Cs Accidentally Discharged from the Fukushima Daiichi Nuclear Power Plant into the Atmosphere Chino, Masamichi; Nakayama, Hiromasa; Nagai, Haruyasu Journal of Nuclear Science and Technology, Vol. 48, Issue 7 https://doi.org/10.1080/18811248.2011.9711799	journal	July 2011
Verification of radiocesium decontamination from farmlands by plants in Fukushima Kobayashi, Daisuke; Okouchi, Toshiyasu; Yamagami, Mutsumi Journal of Plant Research, Vol. 127, Issue 1 https://doi.org/10.1007/s10265-013-0607-x	journal	November 2013
Disaster Waste Characteristics and Radiation Distribution as a Result of the Great East Japan Earthquake Shibata, Tomoyuki; Solo-Gabriele, Helena; Hata, Toshimitsu Environmental Science & Technology, Vol. 46, Issue 7 https://doi.org/10.1021/es300055m	journal	March 2012
Application of portland cement-based materials to radioactive waste immobilization Atkins, M.; Glasser, F. P. Waste Management, Vol. 12, Issue 2-3 https://doi.org/10.1016/0956-053X(92)90044-J	journal	January 1992
Radiation effects in nuclear waste glasses Weber, W. J. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 32, Issue 1-4 https://doi.org/10.1016/0168-583X(88)90257-1	journal	May 1988
The metamict transformation in alpha-quartz Pascucci, M. R.; Hutchison, J. L.; Hobbs, L. W. Radiation Effects, Vol. 74, Issue 1-4 https://doi.org/10.1080/00337578308218415	journal	January 1983
Chemical evolution via beta decay: a case study in strontium-90 Marks, N. A.; Carter, D. J.; Sassi, M. Journal of Physics: Condensed Matter, Vol. 25, Issue 6 https://doi.org/10.1088/0953-8984/25/6/065504	journal	January 2013
First-principles prediction of disordering tendencies in pyrochlore oxides Jiang, Chao; Stanek, C. R.; Sickafus, K. E. Physical Review B, Vol. 79, Issue 10 https://doi.org/10.1103/PhysRevB.79.104203	journal	March 2009
Using “radioparagenesis” to design robust nuclear waste forms Jiang, C.; Uberuaga, B. P.; Sickafus, K. E. Energy Environ. Sci., Vol. 3, Issue 1 https://doi.org/10.1039/B915493K	journal	January 2010
Gamma irradiation resistance of an early age slag-blended cement matrix for nuclear waste encapsulation Mobasher, Neda; Bernal, Susan A.; Kinoshita, Hajime Journal of Materials Research, Vol. 30, Issue 9 https://doi.org/10.1557/jmr.2014.404	journal	February 2015
Radioactive Waste-Portland Cement Systems: I, Radionuclide Distribution Jantzen, Cm.; Glasser, F. P.; Lachowski, E. E. Journal of the American Ceramic Society, Vol. 67, Issue 10 https://doi.org/10.1111/j.1151-2916.1984.tb19680.x	journal	October 1984
Radioactive Waste-Portland Cement Systems: II, Leaching Characteristics Jantzen, C. M. Journal of the American Ceramic Society, Vol. 67, Issue 10 https://doi.org/10.1111/j.1151-2916.1984.tb19681.x	journal	October 1984
Alternative Binders to Ordinary Portland Cement for Radwaste Solidification and Stabilization Cau-dit-Coumes, C. Cement-Based Materials for Nuclear Waste Storage https://doi.org/10.1007/978-1-4614-3445-0_16	book	June 2012
Assessment of the Performance of Cement-Based Composite Material for Radioactive Waste Immobilization Atkins, M.; Cowie, J.; Glasser, F. P. MRS Proceedings, Vol. 176 https://doi.org/10.1557/PROC-176-117	journal	January 1989
Accelerated Ageing of Blended OPC Cements Quilin, K. C.; Duerden, S. L.; Majumdar, A. J. MRS Proceedings, Vol. 333 https://doi.org/10.1557/PROC-333-341	journal	January 1993
Alkali-Activated Fly Ash-Slag Cement Based Nuclear Waste Forms Jiang, W.; Wu, X.; Roy, D. M. MRS Proceedings, Vol. 294 https://doi.org/10.1557/PROC-294-255	journal	January 1992
Strontium Uptake by Cementitious Materials Wieland, Erich; Tits, Jan; Kunz, Dominik Environmental Science & Technology, Vol. 42, Issue 2 https://doi.org/10.1021/es071227y	journal	January 2008
Strontium binding by calcium silicate hydrates Tits, J.; Wieland, E.; Müller, C. J. Journal of Colloid and Interface Science, Vol. 300, Issue 1 https://doi.org/10.1016/j.jcis.2006.03.043	journal	August 2006
Binding mechanisms of radionuclides to cement Evans, N. D. M. Cement and Concrete Research, Vol. 38, Issue 4 https://doi.org/10.1016/j.cemconres.2007.11.004	journal	April 2008
Docking 90Sr radionuclide in cement: An atomistic modeling study Youssef, Mostafa; Pellenq, Roland J. -M.; Yildiz, Bilge Physics and Chemistry of the Earth, Parts A/B/C, Vol. 70-71 https://doi.org/10.1016/j.pce.2013.11.007	journal	January 2014
Combinatorial molecular optimization of cement hydrates Abdolhosseini Qomi, M. J.; Krakowiak, K. J.; Bauchy, M. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5960	journal	September 2014
Anomalous composition-dependent dynamics of nanoconfined water in the interlayer of disordered calcium-silicates Qomi, Mohammad Javad Abdolhosseini; Bauchy, Mathieu; Ulm, Franz-Josef The Journal of Chemical Physics, Vol. 140, Issue 5 https://doi.org/10.1063/1.4864118	journal	February 2014
A realistic molecular model of cement hydrates Pellenq, R. J. -M.; Kushima, A.; Shahsavari, R. Proceedings of the National Academy of Sciences, Vol. 106, Issue 38 https://doi.org/10.1073/pnas.0902180106	journal	September 2009
Nanostructure of CSH: Current status Taylor, H. F. W. Advanced Cement Based Materials, Vol. 1, Issue 1 https://doi.org/10.1016/1065-7355(93)90006-A	journal	October 1993
The Crystal Structure of Tobermorite 14 A (Plombierite), a C-S-H Phase Bonaccorsi, Elena; Merlino, Stefano; Kampf, Anthony R. Journal of the American Ceramic Society, Vol. 88, Issue 3 https://doi.org/10.1111/j.1551-2916.2005.00116.x	journal	March 2005
The crystal structure of jennite, Ca9Si6O18(OH)6·8H2O Bonaccorsi, E.; Merlino, S.; Taylor, H. F. W. Cement and Concrete Research, Vol. 34, Issue 9 https://doi.org/10.1016/j.cemconres.2003.12.033	journal	September 2004
Tobermorite/jennite- and tobermorite/calcium hydroxide-based models for the structure of C-S-H: applicability to hardened pastes of tricalcium silicate, β-dicalcium silicate, Portland cement, and blends of Portland cement with blast-furnace slag, metakaolin, or silica fume Richardson, I. G. Cement and Concrete Research, Vol. 34, Issue 9 https://doi.org/10.1016/j.cemconres.2004.05.034	journal	September 2004
The calcium silicate hydrates Richardson, I. G. Cement and Concrete Research, Vol. 38, Issue 2 https://doi.org/10.1016/j.cemconres.2007.11.005	journal	February 2008
Composition and density of nanoscale calcium–silicate–hydrate in cement Allen, Andrew J.; Thomas, Jeffrey J.; Jennings, Hamlin M. Nature Materials, Vol. 6, Issue 4 https://doi.org/10.1038/nmat1871	journal	March 2007
The nature of C-S-H in hardened cements Richardson, I. G. Cement and Concrete Research, Vol. 29, Issue 8 https://doi.org/10.1016/S0008-8846(99)00168-4	journal	August 1999
Microstructure and microanalysis of hardened cement pastes involving ground granulated blast-furnace slag Richardson, I. G.; Groves, G. W. Journal of Materials Science, Vol. 27, Issue 22 https://doi.org/10.1007/BF01133772	journal	January 1992
Transmission Electron Microscopy and Microanalytical Studies of Ion-Beam-Thinned Sections of Tricalcium Silicate Paste Groves, G. W.; Sueur, P. J.; Sinclair, W. Journal of the American Ceramic Society, Vol. 69, Issue 4 https://doi.org/10.1111/j.1151-2916.1986.tb04746.x	journal	April 1986
Improving the structural consistency of C-S-H solid solution thermodynamic models Kulik, Dmitrii A. Cement and Concrete Research, Vol. 41, Issue 5 https://doi.org/10.1016/j.cemconres.2011.01.012	journal	May 2011
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Uptake of Cm(III) and Eu(III) by Calcium Silicate Hydrates: A Solution Chemistry and Time-Resolved Laser Fluorescence Spectroscopy Study Tits, Jan; Stumpf, Thorsten; Rabung, Thomas Environmental Science & Technology, Vol. 37, Issue 16 https://doi.org/10.1021/es030020b	journal	August 2003
Uptake of trivalent actinides (curium(III)) by hardened cement paste: a time-resolved laser fluorescence spectroscopy study Stumpf, Thorsten; Tits, Jan; Walther, Clemens Journal of Colloid and Interface Science, Vol. 276, Issue 1 https://doi.org/10.1016/j.jcis.2004.03.014	journal	August 2004
Macro- and Microspectroscopic Study of Nd (III) Uptake Mechanisms in Hardened Cement Paste Mandaliev, Peter; Dähn, Rainer; Wehrli, Bernhard Environmental Science & Technology, Vol. 43, Issue 21 https://doi.org/10.1021/es902016q	journal	November 2009
EXAFS study of Nd(III) uptake by amorphous calcium silicate hydrates (C–S–H) Mandaliev, P.; Dähn, R.; Tits, J. Journal of Colloid and Interface Science, Vol. 342, Issue 1 https://doi.org/10.1016/j.jcis.2009.06.011	journal	February 2010
Effective ionic radii in oxides and fluorides Shannon, R. D.; Prewitt, C. T. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 25, Issue 5 https://doi.org/10.1107/S0567740869003220	journal	May 1969
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides Shannon, R. D. Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767 https://doi.org/10.1107/S0567739476001551	journal	September 1976
Uptake of Np(IV) by C–S–H Phases and Cement Paste: An EXAFS Study Gaona, Xavier; Dähn, Rainer; Tits, Jan Environmental Science & Technology, Vol. 45, Issue 20 https://doi.org/10.1021/es2012897	journal	October 2011
EXAFS Study of Sn(IV) Immobilization by Hardened Cement Paste and Calcium Silicate Hydrates Bonhoure, Isabelle; Wieland, Erich; Scheidegger, André M. Environmental Science & Technology, Vol. 37, Issue 10 https://doi.org/10.1021/es020194d	journal	May 2003
A grid-based Bader analysis algorithm without lattice bias Tang, W.; Sanville, E.; Henkelman, G. Journal of Physics: Condensed Matter, Vol. 21, Issue 8 https://doi.org/10.1088/0953-8984/21/8/084204	journal	January 2009

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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]