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Title: Cesium sorption reversibility and kinetics on illite, montmorillonite, and kaolinite

Abstract

Understanding sorption and desorption processes is essential to predicting the mobility of radionuclides in the environment. In this study, we investigate adsorption/desorption of cesium in both binary (Cs + one mineral) and ternary (Cs + two minerals) experiments to study component additivity and sorption reversibility over long time periods (500 days). Binary Cs sorption experiments were performed with illite, montmorillonite, and kaolinite in a 5 mM NaCl/0.7 mM NaHCO3 solution (pH 8) and Cs concentration range of 10 –3 to 10 –11 M. The binary sorption experiments were followed by batch desorption experiments. The sorption behavior was modeled with the FIT4FD code and the results used to predict desorption behavior. Sorption to montmorillonite and kaolinite was linear over the entire concentration range but sorption to illite was non-linear, indicating the presence of multiple sorption sites. Based on the 14 day batch desorption data, cesium sorption appeared irreversible at high surface loadings in the case of illite but reversible at all concentrations for montmorillonite and kaolinite. Additionally, a novel experimental approach, using a dialysis membrane, was adopted in the ternary experiments, allowing investigation of the effect of a second mineral on Cs desorption from the original mineral. Cs was first sorbedmore » to illite, montmorillonite or kaolinite, then a 3.5–5 kDalton Float-A-Lyzer® dialysis bag with 0.3 g of illite was introduced to each experiment inducing desorption. Nearly complete Cs desorption from kaolinite and montmorillonite was observed over the experiment, consistent with our equilibrium model, indicating complete Cs desorption from these minerals. Results from the long-term ternary experiments show significantly greater Cs desorption compared to the binary desorption experiments. Approximately ~ 45% of Cs desorbed from illite. However, our equilibrium model predicted ~ 65% desorption. Importantly, the data imply that in some cases, slow desorption kinetics rather than permanent fixation may play an important role in apparent irreversible Cs sorption.« less

Authors:
 [1];  [2];  [2];  [2]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Institute, Physical & Life Sciences; Pennsylvania State Univ., University Park, PA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Institute, Physical & Life Sciences
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1409965
Report Number(s):
LLNL-JRNL-733377
Journal ID: ISSN 0048-9697
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Science of the Total Environment
Additional Journal Information:
Journal Volume: 610-611; Journal Issue: C; Journal ID: ISSN 0048-9697
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Ternary system; Desorption; Irreversibility; Permeable membrane

Citation Formats

Durrant, Chad B., Begg, James D., Kersting, Annie B., and Zavarin, Mavrik. Cesium sorption reversibility and kinetics on illite, montmorillonite, and kaolinite. United States: N. p., 2017. Web. doi:10.1016/j.scitotenv.2017.08.122.
Durrant, Chad B., Begg, James D., Kersting, Annie B., & Zavarin, Mavrik. Cesium sorption reversibility and kinetics on illite, montmorillonite, and kaolinite. United States. doi:10.1016/j.scitotenv.2017.08.122.
Durrant, Chad B., Begg, James D., Kersting, Annie B., and Zavarin, Mavrik. Thu . "Cesium sorption reversibility and kinetics on illite, montmorillonite, and kaolinite". United States. doi:10.1016/j.scitotenv.2017.08.122. https://www.osti.gov/servlets/purl/1409965.
@article{osti_1409965,
title = {Cesium sorption reversibility and kinetics on illite, montmorillonite, and kaolinite},
author = {Durrant, Chad B. and Begg, James D. and Kersting, Annie B. and Zavarin, Mavrik},
abstractNote = {Understanding sorption and desorption processes is essential to predicting the mobility of radionuclides in the environment. In this study, we investigate adsorption/desorption of cesium in both binary (Cs + one mineral) and ternary (Cs + two minerals) experiments to study component additivity and sorption reversibility over long time periods (500 days). Binary Cs sorption experiments were performed with illite, montmorillonite, and kaolinite in a 5 mM NaCl/0.7 mM NaHCO3 solution (pH 8) and Cs concentration range of 10–3 to 10–11 M. The binary sorption experiments were followed by batch desorption experiments. The sorption behavior was modeled with the FIT4FD code and the results used to predict desorption behavior. Sorption to montmorillonite and kaolinite was linear over the entire concentration range but sorption to illite was non-linear, indicating the presence of multiple sorption sites. Based on the 14 day batch desorption data, cesium sorption appeared irreversible at high surface loadings in the case of illite but reversible at all concentrations for montmorillonite and kaolinite. Additionally, a novel experimental approach, using a dialysis membrane, was adopted in the ternary experiments, allowing investigation of the effect of a second mineral on Cs desorption from the original mineral. Cs was first sorbed to illite, montmorillonite or kaolinite, then a 3.5–5 kDalton Float-A-Lyzer® dialysis bag with 0.3 g of illite was introduced to each experiment inducing desorption. Nearly complete Cs desorption from kaolinite and montmorillonite was observed over the experiment, consistent with our equilibrium model, indicating complete Cs desorption from these minerals. Results from the long-term ternary experiments show significantly greater Cs desorption compared to the binary desorption experiments. Approximately ~ 45% of Cs desorbed from illite. However, our equilibrium model predicted ~ 65% desorption. Importantly, the data imply that in some cases, slow desorption kinetics rather than permanent fixation may play an important role in apparent irreversible Cs sorption.},
doi = {10.1016/j.scitotenv.2017.08.122},
journal = {Science of the Total Environment},
number = C,
volume = 610-611,
place = {United States},
year = {Thu Aug 17 00:00:00 EDT 2017},
month = {Thu Aug 17 00:00:00 EDT 2017}
}

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