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 sorbed to illite,more »
- Authors:
-
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Institute, Physical & Life Sciences; Pennsylvania State Univ., University Park, PA (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Institute, Physical & Life Sciences
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1409965
- Alternate Identifier(s):
- OSTI ID: 1549755
- Report Number(s):
- LLNL-JRNL-733377
Journal ID: ISSN 0048-9697
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- 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. https://doi.org/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. https://doi.org/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}
}
Web of Science
Works referenced in this record:
Interlayer Collapse Affects on Cesium Adsorption Onto Illite
journal, April 2014
- Benedicto, Ana; Missana, Tiziana; Fernández, Ana María
- Environmental Science & Technology, Vol. 48, Issue 9
A Study of the Equilibria Between Three Categories of Potassium in an Illitic Soil1
journal, January 1963
- Bolt, G. H.; Sumner, M. E.; Kamphorst, A.
- Soil Science Society of America Journal, Vol. 27, Issue 3
Cesium Adsorption on Clay Minerals: An EXAFS Spectroscopic Investigation
journal, June 2002
- Bostick, Benjamin C.; Vairavamurthy, Murthy A.; Karthikeyan, K. G.
- Environmental Science & Technology, Vol. 36, Issue 12
A generalised sorption model for the concentration dependent uptake of caesium by argillaceous rocks
journal, March 2000
- Bradbury, Michael H.; Baeyens, Bart
- Journal of Contaminant Hydrology, Vol. 42, Issue 2-4
Cesium and rubidium ion equilibriums in illite clay
journal, March 1983
- Brouwer, E.; Baeyens, B.; Maes, A.
- The Journal of Physical Chemistry, Vol. 87, Issue 7
Reassessment of 90 Sr, 137 Cs, and 134 Cs in the Coast off Japan Derived from the Fukushima Dai-ichi Nuclear Accident
journal, December 2015
- Castrillejo, Maxi; Casacuberta, Núria; Breier, Crystaline F.
- Environmental Science & Technology, Vol. 50, Issue 1
Kinetics of cesium sorption on illite
journal, March 1992
- Comans, Rob N. J.; Hockley, Daryl E.
- Geochimica et Cosmochimica Acta, Vol. 56, Issue 3
Sorption of cesium on illite: Non-equilibrium behaviour and reversibility
journal, February 1991
- N. J. Comans, Rob; Haller, Manuela; De Preter, Peter
- Geochimica et Cosmochimica Acta, Vol. 55, Issue 2
Adsorption of cesium on minerals: A review
journal, July 1993
- Cornell, R. M.
- Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 171, Issue 2
Application of the Surface Complexation Concept to Complex Mineral Assemblages
journal, October 1998
- Davis, J. A.; Coston, J. A.; Kent, D. B.
- Environmental Science & Technology, Vol. 32, Issue 19
Reversibility of radiocaesium sorption on illite
journal, July 2004
- de Koning, Arjan; Comans, Rob N. J.
- Geochimica et Cosmochimica Acta, Vol. 68, Issue 13
Prediction of Intrinsic Cesium Desorption from Na-Smectite in Mixed Cation Solutions
journal, August 2015
- Fukushi, Keisuke; Fukiage, Tomo
- Environmental Science & Technology, Vol. 49, Issue 17
Desorption of Intrinsic Cesium from Smectite: Inhibitive Effects of Clay Particle Organization on Cesium Desorption
journal, August 2014
- Fukushi, Keisuke; Sakai, Haruka; Itono, Taeko
- Environmental Science & Technology, Vol. 48, Issue 18
Ionic strength and pH dependent multi-site sorption of Cs onto a micaceous aquifer sediment
journal, January 2014
- Fuller, Adam J.; Shaw, Samuel; Peacock, Caroline L.
- Applied Geochemistry, Vol. 40
Caesium incorporation and retention in illite interlayers
journal, May 2015
- Fuller, Adam J.; Shaw, Samuel; Ward, Michael B.
- Applied Clay Science, Vol. 108
Standard Heats and Entropies of Exchange for Alkali Metal Cations on Wyoming Bentonite
journal, September 1969
- Gast, R. G.; Van Bladel, Robert; Deshpande, K. B.
- Soil Science Society of America Journal, Vol. 33, Issue 5
Total caesium-fixing potentials of acid organic soils
journal, January 1995
- Hird, Adine B.; Rimmer, David L.; Livens, Francis R.
- Journal of Environmental Radioactivity, Vol. 26, Issue 2
Study of Factors Dominating Sorption/Desorption of Cs in Soil
journal, January 1995
- Hsu, Chun-nan; Chang, Kwo-ping
- Radiochimica Acta, Vol. 68, Issue 2
Reversibility and modeling of adsorption behavior of cesium ions on colloidal montmorillonite particles
journal, July 2010
- Iijima, Kazuki; Tomura, Tsutomu; Shoji, Yoshiyuki
- Applied Clay Science, Vol. 49, Issue 3
Interlayering of Expansible Layer Silicates in Soils by Chemical Weathering
journal, January 1962
- Jackson, M. L.
- Clays and Clay Minerals, Vol. 11, Issue 1
133Cs NMR study of cesium on the surfaces of kaolinite and illite
journal, November 1996
- Kim, Yeongkyoo; James Kirkpatrick, R.; Cygan, Randall T.
- Geochimica et Cosmochimica Acta, Vol. 60, Issue 21
133Cs NMR and XPS investigation of cesium adsorbed on clay minerals and related phases
journal, March 1996
- Kim, Yeongkyoo; Cygan, Randall T.; Kirkpatrick, R. James
- Geochimica et Cosmochimica Acta, Vol. 60, Issue 6
Radioactive Fallout Phenomena and Mechanisms
journal, January 1965
- Klement, A. W.
- Health Physics, Vol. 11, Issue 12
Shale as a radioactive waste repository: the importance of vermiculite
journal, January 1979
- Komarneni, Sridhar; Roy, Della M.
- Journal of Inorganic and Nuclear Chemistry, Vol. 41, Issue 12
Hydrothermal Effects on Cesium Sorption and Fixation by Clay Minerals and Shales
journal, January 1980
- Komarneni, Sridhar
- Clays and Clay Minerals, Vol. 28, Issue 2
Distribution and Retention of 137 Cs in Sediments at the Hanford Site, Washington
journal, September 2001
- McKinley, James P.; Zeissler, Cynthia J.; Zachara, John M.
- Environmental Science & Technology, Vol. 35, Issue 17
Kinetics and irreversibility of cesium and uranium sorption onto bentonite colloids in a deep granitic environment
journal, August 2004
- Missana, T.; Garcı́a-Gutiérrez, M.; Alonso, Ú.
- Applied Clay Science, Vol. 26, Issue 1-4
Modelling of Cs sorption in natural mixed-clays and the effects of ion competition
journal, October 2014
- Missana, Tiziana; García-Gutiérrez, Miguel; Benedicto, Ana
- Applied Geochemistry, Vol. 49
Adsorption behavior of radioactive cesium by non-mica minerals
journal, April 2013
- Ohnuki, Toshihiko; Kozai, Naofumi
- Journal of Nuclear Science and Technology, Vol. 50, Issue 4
Experimental and modelling studies of caesium sorption on illite
journal, October 1999
- Poinssot, Christophe; Baeyens, Bart; Bradbury, Michael H.
- Geochimica et Cosmochimica Acta, Vol. 63, Issue 19-20
Sampling and Analysis of Kga-1B Well-Crystallized Kaolin Source Clay
journal, January 1993
- Pruett, Robert J.
- Clays and Clay Minerals, Vol. 41, Issue 4
Study of Major Ions Sorption Equilibria To Characterize the Ion Exchange Properties of Kaolinite
journal, October 2014
- Reinoso-Maset, Estela; Ly, Jacques
- Journal of Chemical & Engineering Data, Vol. 59, Issue 12
Pottasium Exchange as Affected by Cation Size, ph, and Mineral Structure
journal, January 1964
- Rich, C. I.; Black, W. R.
- Soil Science, Vol. 97, Issue 6
Potassium and Cesium Ion Selectivity in Relation to Clay Mineral Structure
journal, January 1970
- Sawhney, B. L.
- Clays and Clay Minerals, Vol. 18, Issue 1
Selective Sorption and Fixation of Cations by Clay Minerals: A Review
journal, January 1972
- Sawhney, B. L.
- Clays and Clay Minerals, Vol. 20, Issue 2
On the soil Chemistry of Cesium 137
journal, January 1960
- Schulz, R. K.; Overstreet, Roy; Barshad, I.
- Soil Science, Vol. 89, Issue 1
TOF-SIMS study of Cs + sorption on natural kaolinite
journal, February 1999
- Shahwan, T.; Erten, H. N.; Black, L.
- Science of The Total Environment, Vol. 226, Issue 2-3
Adsorption of 137Cs on Montmorillonite and Illite: Effect of Charge Compensating Cation, Ionic Strength, Concentration of Cs, K and Fulvic Acid
journal, January 1997
- Staunton, Siobhán
- Clays and Clay Minerals, Vol. 45, Issue 2
Post-Accident Sporadic Releases of Airborne Radionuclides from the Fukushima Daiichi Nuclear Power Plant Site
journal, November 2015
- Steinhauser, Georg; Niisoe, Tamon; Harada, Kouji H.
- Environmental Science & Technology, Vol. 49, Issue 24
Surface and colloid chemistry of clays
journal, June 1974
- Swartzen-Allen, S. Lee; Matijevic, Egon
- Chemical Reviews, Vol. 74, Issue 3
Effect of desorption kinetics on colloid-facilitated transport of contaminants: Cesium, strontium, and illite colloids: CESIUM AND STRONTIUM COLLOID-FACILITATED TRANSPORT
journal, December 2006
- Turner, Ned B.; Ryan, Joseph N.; Saiers, James E.
- Water Resources Research, Vol. 42, Issue 12
Equilibria of the Base-Exchange Reactions of Bentonites, Permutites, soil Colloids, and Zeolites
journal, January 1932
- Vanselow, Albert P.
- Soil Science, Vol. 33, Issue 2
Sorption of Cs+ to micaceous subsurface sediments from the Hanford site, USA
journal, January 2002
- Zachara, John M.; Smith, Steven C.; Liu, Chongxuan
- Geochimica et Cosmochimica Acta, Vol. 66, Issue 2
Eu(III), Sm(III), Np(V), Pu(V), and Pu(IV) sorption to calcite
journal, January 2005
- Zavarin, Mavrik; Roberts, S. K.; Hakem, N.
- Radiochimica Acta, Vol. 93, Issue 2
Np(V) and Pu(V) Ion Exchange and Surface-Mediated Reduction Mechanisms on Montmorillonite
journal, February 2012
- Zavarin, Mavrik; Powell, Brian A.; Bourbin, Mathilde
- Environmental Science & Technology, Vol. 46, Issue 5
Colloid-Facilitated Cs Transport through Water-Saturated Hanford Sediment and Ottawa Sand
journal, November 2003
- Zhuang, Jie; Flury, Markus; Jin, Yan
- Environmental Science & Technology, Vol. 37, Issue 21
Works referencing / citing this record:
Sorption capacity of cesium on different forest and agricultural soils
journal, July 2018
- Shao, Huijuan; Wei, Yongfen; Li, Fusheng
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 317, Issue 3
Fixation capability of recycling materials as potential additives for cesium immobilization in contaminated forest soil
journal, December 2018
- Shao, Huijuan; Wei, Yongfen; Li, Fusheng
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 319, Issue 1
Decontamination of radioactive cesium ions using ordered mesoporous monetite
journal, January 2018
- Tag El-Din, Ali F.; Elshehy, Emad A.; Abd El-Magied, Mahmoud O.
- RSC Advances, Vol. 8, Issue 34
Cesium Sorption and Desorption on Glauconite, Bentonite, Zeolite and Diatomite
journal, October 2019
- Belousov, Petr; Semenkova, Anna; Egorova, Tolganay
- Minerals, Vol. 9, Issue 10