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Radiation-Damage Resistance in Phyllosilicate Minerals from First Principles and Implications for Radiocesium and Strontium Retention in Soils

Published online by Cambridge University Press:  01 January 2024

Michel Sassi*
Affiliation:
Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99354, USA
Kevin M. Rosso
Affiliation:
Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99354, USA
Masahiko Okumura
Affiliation:
CCSE, Japan Atomic Energy Agency, Kashiwa, Chiba 277-8587, Japan
Masahiko Machida
Affiliation:
CCSE, Japan Atomic Energy Agency, Kashiwa, Chiba 277-8587, Japan
*
*E-mail address of corresponding author: [email protected]
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Abstract

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Accidental discharges of the hazardous nuclear fission products 137Cs+ and 90Sr2+ into the environment, such as during the Fukushima Dai-ichi nuclear accident, have occurred repeatedly throughout the ‘nuclear age.’ Numerous studies of the fate and transport of 137Cs+ and 90Sr2+ in soils and sediments have demonstrated their strong and selective binding to phyllosilicate clay minerals, primarily by means of cation exchange into interlayer sites. The locally concentrated amounts of these radioactive beta-emitters that can be found in these host minerals raise important questions regarding the long-term interplay and durability of radioisotope—clay associations, which is not well known. The present study goes beyond the usual short-term focus to address the permanence of radioisotope retention in clay minerals, by developing a general theoretical understanding of their resistance to the creation of defects. The present study reports ab initio molecular dynamics (AIMD) calculations of the threshold displacement energy (TDE) of each symmetry-unique atomic species comprising the unit cell of model vermiculite. The TDE values determined are material specific, radiation independent, and can be used to estimate the probability of Frenkel-pair creation by direct electron—ion collision, as could be induced by the passage of a high-energy electron emitted during the beta-decay of 137Cs, 90Sr, and daughter 90Y. For 137Cs and 90Sr, the calculated probability is ~36%, while for 90Y the probability is much greater at ~89%. The long-term retention picture that emerges is that decay will progressively alter the clay interlayer structure and charge, probably leading to delamination of the clay, and re-release of residual parent isotopes. Further work examining the effect of Frenkel defect accumulation on the binding energy of parent and daughter radionuclides in the interlayer is thus justified and potentially important for accurate long-term forecasting of radionuclide transport in the environment.

Type
Article
Copyright
Copyright © The Clay Minerals Society 2016

References

Blochl, P.E., 1994 Projector augmented-wave method Physical Review B 50 17953.CrossRefGoogle ScholarPubMed
Bortz, A.B. Kalos, M.H. and Lebowitz, J.L., 1975 A new algorithm for Monte Carlo simulation of Ising spin systems Journal of Computational Physics 17 1018.CrossRefGoogle Scholar
Hess, N.J. Espinosa, F.J. Conradson, S.D. and Weber, W.J., 2000 Beta radiation effects in 137Cs-substituted pollucite Journal of Nuclear Materials 281 2233.CrossRefGoogle Scholar
Hobbs, L.W. Clinard, F.W. Zinkle, S.J. and Ewing, R.C., 1994 Radiation effects in ceramics Journal of Nuclear Materials 216 291321.CrossRefGoogle Scholar
Kogure, T. Morimoto, K. Tamura, K. Sato, H. and Yamagishi, A., 2012 XRD and HRTEM evidences for fixation of cesium ions in vermiculite clay Chemistry Letters 41 380382.CrossRefGoogle Scholar
Kresse, G. and Furthmuller, J., 1996 Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Physical Review B 54 11169.CrossRefGoogle ScholarPubMed
Kresse, G. and Furthmuller, J., 1996 Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Computational Materials Science 6 1550.CrossRefGoogle Scholar
Lucas, G. and Pizzagalli, L., 2005 Ab initio molecular dynamics calculations of threshold displacement energies in silicon carbide Physical Review B 72 161202.CrossRefGoogle Scholar
Lucas, G. and Pizzagalli, L., 2005 Comparison of threshold displacement energies in b-SiC determined by classical potentials and ab initio calculations Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms 229 359366.CrossRefGoogle Scholar
McKinley, J.P. Zachara, J.M. Heald, S.M. Dohnalkova, A. Newville, M.G. and Sutton, S.R., 2004 Microscale distribution of cesium sorbed to biotite and muscovite Environmental Science & Technology 38 10171023.CrossRefGoogle ScholarPubMed
Perdew, J.P. Burke, K. and Ernzerhof, M., 1996 Generalized gradient approximation made simple Physical Review Letters 77 38653868.CrossRefGoogle ScholarPubMed
Sorensen, M.R. and Voter, A.F., 2000 Temperature-accelerated dynamics for simulation of infrequent events The Journal of Chemical Physics 112 95999606.CrossRefGoogle Scholar
Tamura, K. Kogure, T. Watanabe, Y. Nagai, C. and Yamada, H., 2014 Uptake of cesium and strontium ions by artificially altered phlogopite Environmental Science & Technology 48 58085815.CrossRefGoogle ScholarPubMed
Vosko, S.H. Wilk, L. and Nusair, M., 1980 Accurate spindependent electron liquid correlation energies for local spin density calculations: a critical analysis Canadian Journal of Physics 58 12001211.CrossRefGoogle Scholar
Wampler, J.M. Krogstad, E.J. Elliott, W.C. Kahn, B. and Kaplan, D.I., 2012 Long-term selective retention of natural Cs and Rb by highly weathered coastal plain soils Environmental Science & Technology 46 38373843.CrossRefGoogle ScholarPubMed
Weber, W.J. Ewing, R.C. Catlow, C.R.A. De La Rubia, T.D. Hobbs, L.W. Kinoshita, C. Matzke, H.J. Motta, A.T. Nastasi, M. Salje, E.K.H. Vance, E.R. and Zinkle, S.J., 1998 Radiation effects in crystalline ceramics for the immobilization of high-level nuclear waste and plutonium Journal of Materials Research 13 14341484.CrossRefGoogle Scholar
Xu, L. and Henkelman, G., 2008 Adaptive kinetic Monte Carlo for first-principles accelerated dynamics The Journal of Chemical Physics 129 114104.CrossRefGoogle ScholarPubMed
Ziegler, J.F. Ziegler, M.D. and Biersack, J.P., 2010 SRIM — the stopping and range of ions in matter Nuclear Instruments and Methods in Physics Research Section B 268 18181823.CrossRefGoogle Scholar