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

Okumura, Masahiko; Kerisit, Sebastien; Bourg, Ian C.; Lammers, Laura N.; Ikeda, Takashi; Sassi, Michel; Rosso, Kevin M.; Machida, Masahiko

doi:10.1016/j.jenvrad.2018.03.011

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 »« less

Authors:

; Kerisit, Sebastien; Bourg, Ian C.;

;

; Sassi, Michel; Rosso, Kevin M.; Machida, Masahiko

Publication Date:: Sat Sep 01 00:00:00 EDT 2018

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Japan Atomic Energy Agency (JAEA), Kashiwa (Japan); Japan Society for the Promotion of Science (JSPS)

OSTI Identifier:: 1724299

Alternate Identifier(s):: OSTI ID: 1434652; OSTI ID: 1465469

Report Number(s):: PNNL-SA-137174
Journal ID: ISSN 0265-931X; S0265931X1730930X; PII: S0265931X1730930X

Grant/Contract Number:: SC0018419; 16H02437; AC05-76RL01830; AC02-05CH11231

Resource Type:: Published Article

Journal Name:: Journal of Environmental Radioactivity

Additional Journal Information:: Journal Name: Journal of Environmental Radioactivity Journal Volume: 189 Journal Issue: C; Journal ID: ISSN 0265-931X

Publisher:: Elsevier

Country of Publication:: United Kingdom

Language:: English

Subject:: 63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTANT EFFECTS ON LIVING ORGS. AND BIOL. MAT.

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 Kingdom: N. p., 2018. 
Web.  doi:10.1016/j.jenvrad.2018.03.011.

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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 Kingdom.  https://doi.org/10.1016/j.jenvrad.2018.03.011

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                    Okumura, Masahiko, Kerisit, Sebastien, Bourg, Ian C., Lammers, Laura N., Ikeda, Takashi, Sassi, Michel, Rosso, Kevin M., and Machida, Masahiko. Sat .  
"Radiocesium interaction with clay minerals: Theory and simulation advances Post–Fukushima".  United Kingdom.  https://doi.org/10.1016/j.jenvrad.2018.03.011.

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@article{osti_1724299,

  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.2018.03.011},

  journal      = {Journal of Environmental Radioactivity},

  number       = C,

  volume       = 189,

  place        = {United Kingdom},

  year         = {Sat Sep 01 00:00:00 EDT 2018},

  month        = {Sat Sep 01 00:00:00 EDT 2018}

}

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Cited by: 48 works

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Figures / Tables:

Fig. 1: Conceptual model of adsorption sites on an illite particle. This model contains (a) basal surface, (b) edge, (c) hydrated interlayer, (d) frayed edge, and (e) interlayer sites.

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Influence of land management on soil erosion, connectivity, and sediment delivery in agricultural catchments: Closing the sediment budget
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Title: Radiocesium interaction with clay minerals: Theory and simulation advances Post–Fukushima

Abstract

Citation Formats

Figures / Tables:

Influence of land management on soil erosion, connectivity, and sediment delivery in agricultural catchments: Closing the sediment budget journal, August 2019

Influence of land management on soil erosion, connectivity, and sediment delivery in agricultural catchments: Closing the sediment budget
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