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Title: Laboratory column experiments and transport modeling to evaluate retardation of uranium in an aquifer downgradient of a uranium in-situ recovery site

Journal Article · · Applied Geochemistry

The purpose of this study was to determine the attenuation potential and retardation of uranium in sediments taken from boreholes at the Smith-Ranch Highland in-situ recovery (ISR) site. Five column experiments with four different sediments were conducted to study the effects of variable mineralogy and alkalinity on uranium breakthrough. Uranium transport was modeled with PHREEQC using a generalized composite surface complexation model (GC SCM) with one, two, and, three generic surfaces, respectively. Reactive surface areas were approximated with PEST using BET derived surface areas to constrain fitting parameters. Uranium breakthrough was delayed by a factor of 1.68, 1.69 and 1.47 relative to the non-reactive tracer for three of the 5 experiments at an alkalinity of 540 mg/l. A sediment containing smectite and kaolinite retained uranium by a factor of 2.80 despite a lower measured BET surface area. Decreasing alkalinity to 360 mg/l from 540 mg/l increased retardation by a factor of 4.26. Model fits correlated well to overall BET surface area in the three columns where clay content was less than 1%. For the sediment with clay, models consistently understated uranium retardation when reactive surface sites were restricted by BET results. Calcite saturation was shown to be a controlling factor for uranium desorption as the pH of the system changes. A pH of 6 during a secondary background water flush remobilized previously sorbed uranium resulting in a secondary uranium peak at twice the influent concentrations. Furthermore, this study demonstrates the potential of GC SCM models to predict uranium transport in sediments with homogenous mineral composition, but highlights the need for further research to understand the role of sediment clay composition and calcite saturation in uranium transport.

Research Organization:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
U.S. Environmental Protection Agency; USDOE
Grant/Contract Number:
AC52-06NA25396
OSTI ID:
1345947
Report Number(s):
LA-UR-16-29661
Journal Information:
Applied Geochemistry, Vol. 80, Issue C; ISSN 0883-2927
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 25 works
Citation information provided by
Web of Science

References (47)

Sorption of Uranium and Radium by Biotite, Muscovite, and Phlogopite journal January 1983
Sorption of uranium(VI) at the clay mineral–water interface journal October 2010
Characterization of U(VI)-carbonato ternary complexes on hematite: EXAFS and electrophoretic mobility measurements journal August 2000
U(VI) Adsorption to Heterogeneous Subsurface Media:  Application of a Surface Complexation Model journal March 2002
Competition between enzymatic and abiotic reduction of uranium(VI) under iron reducing conditions journal August 2005
Movement of tracers through dual-porosity media — Experiments and modelling in the Cretaceous Chalk, England journal April 1983
Determination of contaminant levels and remediation efficacy in groundwater at a former in situ recovery uranium mine journal January 2012
Standard Electrode Potentials and Temperature Coefficients in Water at 298.15 K journal January 1989
Modelling the migration of contaminants through variably saturated dual-porosity, dual-permeability chalk journal January 2006
Adsorption of Gases in Multimolecular Layers journal February 1938
Reactive transport of uranium(VI) and phosphate in a goethite-coated sand column: An experimental study journal July 2007
Coprecipitation of radionuclides with calcite: estimation of partition coefficients based on a review of laboratory investigations and geochemical data journal June 1999
Approaches to surface complexation modeling of Uranium(VI) adsorption on aquifer sediments journal September 2004
Influence of Calcite and Dissolved Calcium on Uranium(VI) Sorption to a Hanford Subsurface Sediment journal October 2005
Determination of the Formation Constants of Ternary Complexes of Uranyl and Carbonate with Alkaline Earth Metals (Mg 2+ , Ca 2+ , Sr 2+ , and Ba 2+ ) Using Anion Exchange Method journal August 2006
Formation of Aqueous MgUO 2 (CO 3 ) 3 2− Complex and Uranium Anion Exchange Mechanism onto an Exchange Resin journal March 2008
Uranium(VI) Adsorption and Surface Complexation Modeling onto Background Sediments from the F-Area Savannah River Site journal January 2012
Effect of pH on the sorption of uranium in soils journal March 2001
Influence of humic acid on the sorption of uranium(IV) to kaolin journal September 2009
The effect of calcium on aqueous uranium(VI) speciation and adsorption to ferrihydrite and quartz journal March 2006
Complex Formation between UO 2+ 2 and CO 2- 3 : Studied by Laser-Induced Photoacoustic Spectroscopy (LIPAS) journal December 1998
Thermodynamic Constraints on the Oxidation of Biogenic UO 2 by Fe(III) (Hydr)oxides journal June 2006
Enzymic uranium precipitation journal January 1992
Adsorption of uranyl species from bicarbonate solution onto hematite particles journal March 1986
Surface Complexation Modeling of U(VI) Adsorption by Aquifer Sediments from a Former Mill Tailings Site at Rifle, Colorado journal December 2009
Acid–base titration curves of solid humic acids journal January 2008
X-ray absorption spectroscopy identifies calcium-uranyl-carbonate complexes at environmental concentrations journal February 2007
The coprecipitation of uranium with calcium carbonate journal February 1971
Sorption of uranium (VI) on homoionic sodium smectite experimental study and surface complexation modeling journal September 2009
Determination of OH groups in humic acids using methylation with dimethylsulfate journal August 2008
Uranium(VI) sorption to hematite in the presence of humic acid journal October 1999
Surface catalysis of uranium(VI) reduction by iron(II) journal October 1999
A comparison of methods used to characterize the soil specific surface area of clays journal October 2013
Nuclear Energy and Uranium Resources journal June 2007
Uranyl Adsorption onto Hydrous Ferric Oxide—A Re-Evaluation for the Diffuse Layer Model Database journal December 2009
Migration of uranium(IV)/(VI) in the presence of humic acids in quartz sand: A laboratory column study journal January 2007
Kinetics and irreversibility of cesium and uranium sorption onto bentonite colloids in a deep granitic environment journal August 2004
Adsorption of uranium(VI) on amorphous ferric oxyhydroxide at high concentrations of dissolved carbon(IV) and sulfur(VI) journal February 1995
The future of Yellowcake: A global assessment of uranium resources and mining journal February 2014
Impact of Alkaline Earth Metals on Aqueous Speciation of Uranium(VI) and Sorption on Quartz journal February 2011
Factors Affecting Efficient Aquifer Restoration at In Situ Uranium Mine Sites journal May 1990
Surface complexation model of uranyl sorption on Georgia kaolinite journal August 2004
Coprecipitation of Uranium(VI) with Calcite: XAFS, micro-XAS, and luminescence characterization journal October 2001
Impact of Uranyl−Calcium−Carbonato Complexes on Uranium(VI) Adsorption to Synthetic and Natural Sediments journal February 2010
Interaction between aqueous uranium (VI) and sulfide minerals: Spectroscopic evidence for sorption and reduction journal July 1994
Determination of the surface area of smectite in water by ethylene oxide chain adsorption journal May 2005
Competitive complexation of metal ions with humic substances journal March 2005

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