Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids
Abstract
Understanding the parameters that control colloid-mediated transport of radionuclides is important for the safe disposal of used nuclear fuel. We report an experimental and reactive transport modeling examination of americium transport in a groundwater–bentonite–fracture fill material system. A series of batch sorption and column transport experiments were conducted to determine the role of desorption kinetics from bentonite colloids in the transport of americium through fracture materials. We used fracture fill material from a shear zone in altered granodiorite collected from the Grimsel Test Site (GTS) in Switzerland and colloidal suspensions generated from FEBEX bentonite, a potential repository backfill material. The colloidal suspension (100 mg L–1) was prepared in synthetic groundwater that matched the natural water chemistry at GTS and was spiked with 5.5 × 10–10 M241Am. Batch characterizations indicated that 97% of the americium in the stock suspension was adsorbed to the colloids. Breakthrough experiments conducted by injecting the americium colloidal suspension through three identical columns in series, each with mean residence times of 6 h, show that more than 95% of the bentonite colloids were transported through each of the columns, with modeled colloid filtration rates (kf) of 0.01–0.02 h–1. Am recoveries in each column were 55–60%, and Ammore »
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1247312
- Alternate Identifier(s):
- OSTI ID: 1249612
- Report Number(s):
- LA-UR-15-25173
Journal ID: ISSN 0265-931X; PII: S0265931X15300436
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Environmental Radioactivity
- Additional Journal Information:
- Journal Volume: 148; Journal Issue: C; Journal ID: ISSN 0265-931X
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 42 ENGINEERING; 54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; americium; granite/granodiorite; reactive transport; desorption kinetics; column experiments; bentonite colloids
Citation Formats
Dittrich, Timothy Mark, Boukhalfa, Hakim, Ware, Stuart Douglas, and Reimus, Paul William. Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids. United States: N. p., 2015.
Web. doi:10.1016/j.jenvrad.2015.07.001.
Dittrich, Timothy Mark, Boukhalfa, Hakim, Ware, Stuart Douglas, & Reimus, Paul William. Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids. United States. https://doi.org/10.1016/j.jenvrad.2015.07.001
Dittrich, Timothy Mark, Boukhalfa, Hakim, Ware, Stuart Douglas, and Reimus, Paul William. Mon .
"Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids". United States. https://doi.org/10.1016/j.jenvrad.2015.07.001. https://www.osti.gov/servlets/purl/1247312.
@article{osti_1247312,
title = {Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids},
author = {Dittrich, Timothy Mark and Boukhalfa, Hakim and Ware, Stuart Douglas and Reimus, Paul William},
abstractNote = {Understanding the parameters that control colloid-mediated transport of radionuclides is important for the safe disposal of used nuclear fuel. We report an experimental and reactive transport modeling examination of americium transport in a groundwater–bentonite–fracture fill material system. A series of batch sorption and column transport experiments were conducted to determine the role of desorption kinetics from bentonite colloids in the transport of americium through fracture materials. We used fracture fill material from a shear zone in altered granodiorite collected from the Grimsel Test Site (GTS) in Switzerland and colloidal suspensions generated from FEBEX bentonite, a potential repository backfill material. The colloidal suspension (100 mg L–1) was prepared in synthetic groundwater that matched the natural water chemistry at GTS and was spiked with 5.5 × 10–10 M241Am. Batch characterizations indicated that 97% of the americium in the stock suspension was adsorbed to the colloids. Breakthrough experiments conducted by injecting the americium colloidal suspension through three identical columns in series, each with mean residence times of 6 h, show that more than 95% of the bentonite colloids were transported through each of the columns, with modeled colloid filtration rates (kf) of 0.01–0.02 h–1. Am recoveries in each column were 55–60%, and Am desorption rate constants from the colloids, determined from 1-D transport modeling, were 0.96, 0.98, and 0.91 h–1 in the three columns, respectively. The consistency in Am recoveries and desorption rate constants in each column indicates that the Am was not associated with binding sites of widely-varying strengths on the colloids, as one binding site with fast kinetics represented the system accurately for all three sequential columns. As a result, our data suggest that colloid-mediated transport of Am in a bentonite-fracture fill material system is unlikely to result in transport over long distance scales because of the ability of the fracture materials to rapidly strip Am from the bentonite colloids and the apparent lack of a strong binding site that would keep a fraction of the Am strongly-associated with the colloids.},
doi = {10.1016/j.jenvrad.2015.07.001},
journal = {Journal of Environmental Radioactivity},
number = C,
volume = 148,
place = {United States},
year = {Mon Jul 13 00:00:00 EDT 2015},
month = {Mon Jul 13 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Sorption of Plutonium and Americium on Repository, Backfill and Geological Materials Relevant to The JNFL Low-Level Radioactive Waste Repository at Rokkasho-Mura
journal, January 1994
- Baston, G. M. N.; Berry, J. A.; Brownsword, M.
- MRS Proceedings, Vol. 353
Sorption modelling on illite. Part II: Actinide sorption and linear free energy relationships
journal, February 2009
- Bradbury, M. H.; Baeyens, B.
- Geochimica et Cosmochimica Acta, Vol. 73, Issue 4
Modelling the sorption of Mn(II), Co(II), Ni(II), Zn(II), Cd(II), Eu(III), Am(III), Sn(IV), Th(IV), Np(V) and U(VI) on montmorillonite: Linear free energy relationships and estimates of surface binding constants for some selected heavy metals and actinides
journal, February 2005
- Bradbury, Michael H.; Baeyens, Bart
- Geochimica et Cosmochimica Acta, Vol. 69, Issue 4
Experimental measurements and modeling of sorption competition on montmorillonite
journal, September 2005
- Bradbury, Michael H.; Baeyens, Bart
- Geochimica et Cosmochimica Acta, Vol. 69, Issue 17
Sorption of 241Am onto Montmorillonite, Illite and Hematite Colloids
journal, January 1994
- Degueldre, C.; Ulrich, H. J. .; Silby, H.
- Radiochimica Acta, Vol. 65, Issue 3
Sorption behaviour of Am on marl groundwater colloids
journal, January 2001
- Degueldre, C.; Bilewicz, A.; Hummel, W.
- Journal of Environmental Radioactivity, Vol. 55, Issue 3
Size dispersion and colloid mediated radionuclide transport in a synthetic porous media
journal, August 2008
- Delos, A.; Walther, C.; Schäfer, T.
- Journal of Colloid and Interface Science, Vol. 324, Issue 1-2
Colloid Movement in Unsaturated Porous Media: Recent Advances and Future Directions
journal, May 2004
- DeNovio, Nicole M.; Saiers, James E.; Ryan, Joseph N.
- Vadose Zone Journal, Vol. 3, Issue 2
Uranium transport in a crushed granodiorite: Experiments and reactive transport modeling
journal, April 2015
- Dittrich, T. M.; Reimus, P. W.
- Journal of Contaminant Hydrology, Vol. 175-176
Results of the colloid and radionuclide retention experiment (CRR) at the Grimsel Test Site (GTS), Switzerland – impact of reaction kinetics and speciation on radionuclide migration
journal, January 2004
- Geckeis, Horst; Schäfer, Thorsten; Hauser, W.
- Radiochimica Acta, Vol. 92, Issue 9-11
Sorption reversibility kinetics in the ternary system radionuclide–bentonite colloids/nanoparticles–granite fracture filling material
journal, December 2011
- Huber, F.; Kunze, P.; Geckeis, H.
- Applied Geochemistry, Vol. 26, Issue 12
Distribution of Cs and Am in the solution-bentonite colloids-granite ternary system: effect of addition order and sorption reversibility
journal, November 2010
- Iijima, Kazuki; Tomura, T.; Tobita, M.
- ract, Vol. 98, Issue 9-11
Sorption behavior of americium onto bentonite colloid
journal, November 2008
- Iijima, Kazuki; Shoji, Y.; Tomura, T.
- Radiochimica Acta, Vol. 96, Issue 9-11
Migration of plutonium in ground water at the Nevada Test Site
journal, January 1999
- Kersting, A. B.; Efurd, D. W.; Finnegan, D. L.
- Nature, Vol. 397, Issue 6714
The influence of colloid formation in a granite groundwater bentonite porewater mixing zone on radionuclide speciation
journal, December 2008
- Kunze, P.; Seher, H.; Hauser, W.
- Journal of Contaminant Hydrology, Vol. 102, Issue 3-4
Model analysis of the colloid and radionuclide retardation experiment at the Grimsel Test Site
journal, June 2006
- Kurosawa, Susumu; James, Scott C.; Yui, Mikazu
- Journal of Colloid and Interface Science, Vol. 298, Issue 1
Mechanism of Plutonium Transport in a Shallow Aquifer in Mortandad Canyon, Los Alamos National Laboratory, New Mexico
journal, July 1997
- Marty, Richard C.; Bennett, Deborah; Thullen, Philip
- Environmental Science & Technology, Vol. 31, Issue 7
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
Mobilization of Microspheres from a Fractured Soil during Intermittent Infiltration Events
journal, January 2015
- Mohanty, Sanjay K.; Bulicek, Mark C. D.; Metge, David W.
- Vadose Zone Journal, Vol. 14, Issue 1
Mobility of plutonium and americium through a shallow aquifer in a semiarid region
journal, February 1990
- Penrose, William R.; Polzer, Wilfred L.; Essington, Edward H.
- Environmental Science & Technology, Vol. 24, Issue 2
Seismic stress stimulation mobilizes colloids trapped in a porous rock
journal, July 2009
- Roberts, Peter M.; Abdel-Fattah, Amr I.
- Earth and Planetary Science Letters, Vol. 284, Issue 3-4
U, Th, Eu and colloid mobility in a granite fracture under near-natural flow conditions
journal, January 2004
- Schäfer, Thorsten; Geckeis, Horst; Bouby, Muriel
- Radiochimica Acta, Vol. 92, Issue 9-11
Nanoparticles and their influence on radionuclide mobility in deep geological formations
journal, February 2012
- Schäfer, Thorsten; Huber, Florian; Seher, Holger
- Applied Geochemistry, Vol. 27, Issue 2
Colloidal Particles at Solid–Liquid Interfaces: Mechanisms of Desorption Kinetics
journal, October 1998
- Weiss, Michael; Lüthi, Yves; Rička, Jaro
- Journal of Colloid and Interface Science, Vol. 206, Issue 1
Works referencing / citing this record:
Migration of polyethylene glycol coated gold nanoparticles in surrogate natural barriers
journal, April 2020
- Ordonez, Carlos; Watanabe, Naoko; Kozaki, Tamotsu
- Journal of Nuclear Science and Technology, Vol. 57, Issue 7
Migration of polyethylene glycol coated gold nanoparticles in surrogate natural barriers
text, January 2020
- Ordonez, Carlos; Watanabe, Naoko; Kozaki, Tamotsu
- Taylor & Francis