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Title: Radionuclide transport in fractured chalk under abrupt changes in salinity

Journal Article · · Science of the Total Environment
 [1];  [1];  [2];  [2];  [2];  [3];  [1];  [1];  [1];  [1];  [4]
  1. Ben Gurion University of the Negev, Beer Sheva (Israel)
  2. Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
  3. Geological Survey of Israel, Jerusalem (Israel)
  4. Nuclear Research Center of the Negev, Beersheva (Israel); Ben Gurion University of the Negev, Beer Sheva (Israel)

Internationally, it has been agreed that geologic repositories for spent fuel and radioactive waste are considered the internationally agreed upon solution for intermediate and long-term disposal. In countries where traditional nuclear waste repository host rocks (e.g., clay, salt, granite) are not available, other low permeability lithologies must be studied. Here, chalk is considered to determine its viability for disposal. Despite chalk's low bulk permeability, it may contain fracture networks that can facilitate radionuclide transport. In arid areas, groundwater salinity may change seasonally due to the mixing between brackish groundwater and fresh meteoric water. Such salinity changes may impact the radionuclides' mobility. In this study, radioactive U(VI) and radionuclide simulant tracers (Sr, Ce and Re) were injected into a naturally fractured chalk core. The mobility of tracers was investigated under abrupt salinity variations. Two solutions were used: a low ionic strength (IS) artificial rainwater (ARW; IS ~0.002) and a high IS artificial groundwater (AGW; IS ~0.2). During the experiments, the tracers were added to ARW, then the carrier was changed to AGW, and vice versa. Ce was mobile only in colloidal form, while Re was transported as a conservative tracer. Both Re and Ce demonstrated no change in mobility due to salinity changes. In contrast, U and Sr showed increased mobility when AGW was introduced and decreased mobility when ARW was introduced into the core. These experimental results, supported by reactive transport modeling, suggest that saline groundwater solutions promote U and Sr release via ion-exchange and enhance their migration in fractured chalk. Here the study emphasizes the impact of salinity variations near spent fuel repositories and their possible impact on radionuclide mobility.

Research Organization:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); Israel Science Foundation (ISF); PAZY Foundation
Grant/Contract Number:
AC52-07NA27344
OSTI ID:
2337572
Report Number(s):
LLNL-JRNL-862943; 1095696
Journal Information:
Science of the Total Environment, Journal Name: Science of the Total Environment Journal Issue: N/A Vol. 912; ISSN 0048-9697
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (47)

Neptunium, plutonium and 137Cs sorption by bentonite clays and their speciation in pore waters journal November 2006
Coupled Effects of Ionic Strength, Particle Size, and Flow Velocity on Transport and Deposition of Suspended Particles in Saturated Porous Media journal April 2017
Chemical Compositions in Modified Salinity Waterflooding of Calcium Carbonate Reservoirs: Experiment journal January 2022
Study on speciation and salinity-induced mobility of uranium from soil journal February 2015
A Basin-Scale Groundwater Flow Model of the Columbia Plateau Regional Aquifer System in the Palouse (USA): Insights for Aquifer Vulnerability Assessment journal February 2021
The adsorption of plutonium IV and V on goethite journal November 1985
Sorption of divalent metals on calcite journal June 1991
Rhenium in seawater: Confirmation of generally conservative behavior journal November 1992
Rhenium, molybdenum, and uranium in groundwater from the southern Great Basin, USA: Evidence for conservative behavior journal September 1996
Characterisation of hydrogeologically significant fracture distributions in the Chalk: an example from the Upper Chalk of southern England journal October 1996
A study of the interaction of strontium ions in aqueous solution with the surfaces of calcite and kaolinite journal May 1998
Characterizing flow and transport in fractured geological media: A review journal August 2002
Salinity increases mobility of heavy metals in soils journal November 2011
Evaluation of high fluoride contaminated fractured rock aquifer in South Africa – Geochemical and chemometric approaches journal November 2019
Colloid-facilitated transport of lead in natural discrete fractures journal August 2009
Uncertainty quantification of radionuclide migration in fractured granite journal September 2022
A review of model applications for structured soils: a) Water flow and tracer transport journal February 2009
Colloid-associated plutonium transport in the vadose zone sediments at Lop Nor journal February 2013
Radionuclide transport in multi-scale fractured rocks: A review journal February 2022
The significance of flow in the matrix of the Chalk unsaturated zone journal August 2005
Transient simulations of flow and transport in the Chalk unsaturated zone journal October 2006
Impact of environmental conditions on the sorption behavior of radionuclide 90 Sr(II) on Na-montmorillonite journal March 2015
Adsorption of bivalent ions (Ca(II), Sr(II) and Co(II)) onto FEBEX bentonite journal January 2007
The significance of colloids in the transport of pesticides through Chalk journal October 2007
Uranium facilitated transport by water-dispersible colloids in field and soil columns journal April 2010
Uranium and Cesium sorption to bentonite colloids under carbonate-rich environments: Implications for radionuclide transport journal December 2018
Co-transport of U(VI) and gibbsite colloid in saturated granite particle column: Role of pH, U(VI) concentration and humic acid journal October 2019
Colloid-facilitated transport of 238Pu, 233U and 137Cs through fractured chalk: Laboratory experiments, modelling, and implications for nuclear waste disposal journal February 2021
New insights into U(VI) sorption onto montmorillonite from batch sorption and spectroscopic studies at increased ionic strength journal February 2022
Influence of heteroaggregation processes between intrinsic colloids and carrier colloids on cerium(III) mobility through fractured carbonate rocks journal September 2016
Radionuclide transport in brackish water through chalk fractures journal October 2019
Mobility of Radionuclides in Fractured Carbonate Rocks: Lessons from a Field-Scale Transport Experiment journal August 2020
Influence of Intrinsic Colloid Formation on Migration of Cerium through Fractured Carbonate Rock journal October 2015
Field Scale Mobility and Transport Manipulation of Carbon-Supported Nanoscale Zerovalent Iron in Fractured Media journal June 2018
Oil Recovery Mechanism(s) by Low Salinity Brines and Their Interaction with Chalk journal October 2014
Plutonium Transport in the Environment journal June 2012
Impact of intermittent rainwater and wastewater flow on coated and uncoated fractures in chalk journal November 1999
Impact of particle size on colloid transport in discrete fractures: COLLOID TRANSPORT IN DISCRETE FRACTURES journal November 2006
Water Recharge and Solute Transport Through the Vadose Zone of Fractured Chalk Under Desert Conditions journal February 1995
Long-term storage of spent nuclear fuel journal February 2015
Characterization of the Hydraulic Properties of Fractures in Chalk journal July 2003
Contaminant Transport in Fractured Chalk: Laboratory and Field Experiments journal November 2003
Sorption kinetics and impact of temperature, ionic strength and colloid concentration on the adsorption of plutonium-239 by inorganic colloids journal January 2003
Geological Disposal of Nuclear Waste: a Primer journal July 2016
Immobilization of Cesium-137 and Uranium in Contaminated Sediments Using Soil Amendments journal January 2001
Geochemical Processes Controlling Migration of Tank Wastes in Hanford's Vadose Zone journal January 2007
Reactive transport simulations of uranium migration in the Opalinus Clay depend on ion speciation governed by underlying thermodynamic data journal October 2022