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Title: Radiocesium interaction with clay minerals: Theory and simulation advances Post–Fukushima

Abstract

Insights at the microscopic level of the process of radiocesium adsorption and interaction with clay mineral particles have improved substantially over the past several years, triggered by pressing social issues such as management of huge amounts of waste soil accumulated after the Fukushima Dai-ichi nuclear power plant accident. In particular, computer-based molecular modeling supported by advanced hardware and algorithms has proven to be a powerful approach. Its application can now generally encompass the full complexity of clay particle adsorption sites from basal surfaces to interlayers with inserted water molecules, to edges including fresh and weathered frayed ones. On the other hand, its methodological schemes are now varied from traditional force-field molecular dynamics on large-scale realizations composed of many thousands of atoms including water molecules to first-principles methods on smaller models in rather exacting fashion. In this article, we overview new understanding enabled by simulations across methodological variations, focusing on recent insights that connect with experimental observations, namely: 1) the energy scale for cesium adsorption on the basal surface, 2) progress in understanding the structure of clay edges, which is difficult to probe experimentally, 3) cesium adsorption properties at hydrated interlayer sites, 4) the importance of the size relationship between themore » ionic radius of cesium and the interlayer distance at frayed edge sites, 5) the migration of cesium into deep interlayer sites, and 6) the effects of nuclear decay of radiocesium. Key experimental observations that motivate these simulation advances are also summarized. Furthermore, some directions toward future solutions of waste soil management are discussed based on the obtained microscopic insights.« less

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [5];  [2];  [2];  [1]
+ Show Author Affiliations
  1. Japan Atomic Energy Agency, Chiba (Japan)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Princeton Univ., Princeton, NJ (United States)
  4. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. National Institutes for Quantum and Radiological Science and Technology (QST), Sayo, Hyogo (Japan)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1580417
Grant/Contract Number:  
AC02-05CH11231; SC0018419
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Environmental Radioactivity
Additional Journal Information:
Journal Volume: 210; Journal Issue: C; Journal ID: ISSN 0265-931X
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Okumura, Masahiko, Kerisit, Sebastien, Bourg, Ian C., Lammers, Laura N., Ikeda, Takashi, Sassi, Michel, Rosso, Kevin M., and Machida, Masahiko. Radiocesium interaction with clay minerals: Theory and simulation advances Post–Fukushima. United States: N. p., 2018. Web. doi:10.1016/j.jenvrad.2018.09.007.
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Okumura, Masahiko, Kerisit, Sebastien, Bourg, Ian C., Lammers, Laura N., Ikeda, Takashi, Sassi, Michel, Rosso, Kevin M., & Machida, Masahiko. Radiocesium interaction with clay minerals: Theory and simulation advances Post–Fukushima. United States. https://doi.org/10.1016/j.jenvrad.2018.09.007
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Okumura, Masahiko, Kerisit, Sebastien, Bourg, Ian C., Lammers, Laura N., Ikeda, Takashi, Sassi, Michel, Rosso, Kevin M., and Machida, Masahiko. Tue . "Radiocesium interaction with clay minerals: Theory and simulation advances Post–Fukushima". United States. https://doi.org/10.1016/j.jenvrad.2018.09.007. https://www.osti.gov/servlets/purl/1580417.
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@article{osti_1580417,
title = {Radiocesium interaction with clay minerals: Theory and simulation advances Post–Fukushima},
author = {Okumura, Masahiko and Kerisit, Sebastien and Bourg, Ian C. and Lammers, Laura N. and Ikeda, Takashi and Sassi, Michel and Rosso, Kevin M. and Machida, Masahiko},
abstractNote = {Insights at the microscopic level of the process of radiocesium adsorption and interaction with clay mineral particles have improved substantially over the past several years, triggered by pressing social issues such as management of huge amounts of waste soil accumulated after the Fukushima Dai-ichi nuclear power plant accident. In particular, computer-based molecular modeling supported by advanced hardware and algorithms has proven to be a powerful approach. Its application can now generally encompass the full complexity of clay particle adsorption sites from basal surfaces to interlayers with inserted water molecules, to edges including fresh and weathered frayed ones. On the other hand, its methodological schemes are now varied from traditional force-field molecular dynamics on large-scale realizations composed of many thousands of atoms including water molecules to first-principles methods on smaller models in rather exacting fashion. In this article, we overview new understanding enabled by simulations across methodological variations, focusing on recent insights that connect with experimental observations, namely: 1) the energy scale for cesium adsorption on the basal surface, 2) progress in understanding the structure of clay edges, which is difficult to probe experimentally, 3) cesium adsorption properties at hydrated interlayer sites, 4) the importance of the size relationship between the ionic radius of cesium and the interlayer distance at frayed edge sites, 5) the migration of cesium into deep interlayer sites, and 6) the effects of nuclear decay of radiocesium. Key experimental observations that motivate these simulation advances are also summarized. Furthermore, some directions toward future solutions of waste soil management are discussed based on the obtained microscopic insights.},
doi = {10.1016/j.jenvrad.2018.09.007},
journal = {Journal of Environmental Radioactivity},
number = C,
volume = 210,
place = {United States},
year = {Tue Oct 16 00:00:00 EDT 2018},
month = {Tue Oct 16 00:00:00 EDT 2018}
}
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