U, Th, Eu and colloid mobility in a granite fracture under near-natural flow conditions
-
Thorsten Schäfer
Summary
Laboratory core migration experiments were performed in a granite fracture from the Grimsel Test Site (GTS, central Swiss Alps). The flow velocity was varied (46 m yr-1, 94 m yr-1, 187 m yr-1) and solutions with 10-6 mol L-1 U(VI), 10-8 mol L-1 Th(IV) and 10-8 mol L-1 Eu(III) without (cocktail I) and with addition of 2 mgL-1 bentonite colloids (cocktail II) have been injected. Results are compared with those obtained in a field study at the GTS. Flow field-flow fractionation and ultrafiltration measurements show that U(VI) is not colloid borne, different from Th(IV) and Eu(III) which are associated with colloids in both spiked natural groundwaters with and without bentonite colloid addition. The partly unretarded U(VI) migration observed at short contact times (1-2 h) diminished under near-natural groundwater velocities (∼46 m yr-1) and only a weak retardation (Rf=19.5) could be observed. Furthermore, the U(VI) mass recovery decreased with increasing contact time and was as expected unaffected by bentonite colloid addition. A groundwater colloid mediated Th(IV)/Eu(III) migration without bentonite colloid addition could be confirmed in the core experiments but only at fast groundwater flow rates. Experiments at a water flow rate of 94 m yr-1 with cocktail II demonstrated a partially bentonite colloid facilitated transport of Th(IV) and Eu(III) with 27% and 37% mass recovery, respectively. At long tracer residence times in the flow field, no breakthrough of colloidal Th(IV)/Eu(III) could be observed in both runs, indicating the strong dependence of reaction kinetics on their mobility. Reference colloid experiments using fluorescence dye labeled carboxylated polystyrene microspheres (25 nm, 50 nm and 100 nm) revealed in general a higher recovery of smaller colloid size classes increasing with groundwater velocity. Additionally, an earlier peak arrival time of colloids and colloid-associated Th(IV) and Eu(III) was observed with respect to the conservative tracer 3H in all experiments due to pore-size or charge exclusion effects. In general, the colloid recoveries found in the laboratory core experiments are lower than those obtained in the field studies. The decrease of colloid mobility with increasing residence time suggests the occurrence of colloid attachment to the rock surfaces even under the colloid stabilizing groundwater conditions.
© 2004 Oldenbourg Wissenschaftsverlag GmbH
Articles in the same Issue
- Preface: Migration Conference 2003
- Actinide chemistry: from weapons to remediation to stewardship
- Thermodynamics and solubility of (UxNp1-x)O2(am) solid solution in the carbonate system
- Solubility and colloid formation of Th(IV) in concentrated NaCl and MgCl2 solution
- Effect of reducing agents on the uranium concentration above uranium(IV) amorphous precipitate in Boom Clay pore water
- On Mo-Ru-Tc-Pd-Rh-Te alloy particles extracted from spent fuel and their leaching behavior under Ar and H2 atmospheres
- Modeling of the complex formation of metal ions with humic acids
- Application of the NICA-Donnan model for proton, copper and uranyl binding to humic acid
- Protonation and complexation of isosaccharinic acid with U(VI) and Fe(III) in acidic solutions: potentiometric and calorimetric studies
- Carbonate complexation of neptunium(IV) in highly basic solutions
- Fluorescence characteristics of complex formation of europium(III)-salicylate
- The reduction of U(VI) by near field hydrogen in the presence of UO2(s)
- Electrochemical aspects of radiolytically enhanced UO2 dissolution
- Effect of alpha radiolysis on doped UO2 dissolution under reducing conditions
- The redox behaviour of plutonium in humic rich groundwater
- The fate of radiolytic oxidants during spent fuel leaching in the presence of dissolved near field hydrogen
- Structural changes of uranyl moiety with reduction from U(VI) to U(V)
- Trivalent actinide coprecipitation with powellite (CaMoO4): Secondary solid solution formation during HLW borosilicate-glass dissolution
- Reproducibility of the uptake of U(VI) onto degraded cement pastes and calcium silicate hydrate phases
- Uranium adsorption on weathered schist – intercomparison of modelling approaches
- Contribution of minerals to the sorption of U(VI) on granite
- Distribution and geochemical association of actinides in a contaminated soil as a function of grain size
- Interactions between anionic complex species of actinides and negatively charged mineral surfaces
- Measurements and modelling of Pm sorption onto TiO2 and goethite
- Effect of humic acid on the sorption of Cm(III) onto γ-Al2O3 studied by the time-resolved laser fluorescence spectroscopy
- Am(III) and Eu(III) uptake on hematite in the presence of humic acid
- Luminescence properties of tetravalent uranium in aqueous solution
- Scanning transmission X-ray microscopy as a speciation tool for natural organic molecules
- Formation of hydroxyapatite in soils using calcium citrate and sodium phosphate for control of strontium migration
- Influence of humic substances on the 63Ni migration through crushed rock media
- U, Th, Eu and colloid mobility in a granite fracture under near-natural flow conditions
- Sorption behavior of europium(III) and curium(III) on the cell surfaces of microorganisms
- Interactions of trivalent and tetravalent heavy metal-siderophore complexes with Pseudomonas fluorescens
- In-situ diffusion of HTO, 22Na+, Cs+ and I- in Opalinus Clay at the Mont Terri underground rock laboratory
- 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
- Fracture flow and radionuclide transport in block-scale laboratory experiments
- Comparison between in situ and laboratory diffusion studies of HTO and halides in Opalinus Clay from the Mont Terri
- Solubility constraints on uranium concentrations in groundwaters of the Tono uranium deposit, Japan
- Mobility of uranium in tertiary argillaceous sediments – a natural analogue study
- Redistribution of U, Pb and REE in association with alteration of uranium minerals from the Koongarra deposit, Northern Territory, Australia
- Towards a common thermodynamic database for speciation models
- Geochemically derived non-gaseous radionuclide source term for the Asse salt mine – assessment for the use of a Mg(OH)2-based backfill material
- Simulation of remediation alternatives for a 137Cs contaminated soil
- Simulating reactive transport in time dependent multiphase flow problems
- Reactive transport modelling of a spent fuel repository in a stiff clay formation considering excavation damaged zones
- Coupled transport/reaction modelling of copper canister corrosion aided by microbial processes
Articles in the same Issue
- Preface: Migration Conference 2003
- Actinide chemistry: from weapons to remediation to stewardship
- Thermodynamics and solubility of (UxNp1-x)O2(am) solid solution in the carbonate system
- Solubility and colloid formation of Th(IV) in concentrated NaCl and MgCl2 solution
- Effect of reducing agents on the uranium concentration above uranium(IV) amorphous precipitate in Boom Clay pore water
- On Mo-Ru-Tc-Pd-Rh-Te alloy particles extracted from spent fuel and their leaching behavior under Ar and H2 atmospheres
- Modeling of the complex formation of metal ions with humic acids
- Application of the NICA-Donnan model for proton, copper and uranyl binding to humic acid
- Protonation and complexation of isosaccharinic acid with U(VI) and Fe(III) in acidic solutions: potentiometric and calorimetric studies
- Carbonate complexation of neptunium(IV) in highly basic solutions
- Fluorescence characteristics of complex formation of europium(III)-salicylate
- The reduction of U(VI) by near field hydrogen in the presence of UO2(s)
- Electrochemical aspects of radiolytically enhanced UO2 dissolution
- Effect of alpha radiolysis on doped UO2 dissolution under reducing conditions
- The redox behaviour of plutonium in humic rich groundwater
- The fate of radiolytic oxidants during spent fuel leaching in the presence of dissolved near field hydrogen
- Structural changes of uranyl moiety with reduction from U(VI) to U(V)
- Trivalent actinide coprecipitation with powellite (CaMoO4): Secondary solid solution formation during HLW borosilicate-glass dissolution
- Reproducibility of the uptake of U(VI) onto degraded cement pastes and calcium silicate hydrate phases
- Uranium adsorption on weathered schist – intercomparison of modelling approaches
- Contribution of minerals to the sorption of U(VI) on granite
- Distribution and geochemical association of actinides in a contaminated soil as a function of grain size
- Interactions between anionic complex species of actinides and negatively charged mineral surfaces
- Measurements and modelling of Pm sorption onto TiO2 and goethite
- Effect of humic acid on the sorption of Cm(III) onto γ-Al2O3 studied by the time-resolved laser fluorescence spectroscopy
- Am(III) and Eu(III) uptake on hematite in the presence of humic acid
- Luminescence properties of tetravalent uranium in aqueous solution
- Scanning transmission X-ray microscopy as a speciation tool for natural organic molecules
- Formation of hydroxyapatite in soils using calcium citrate and sodium phosphate for control of strontium migration
- Influence of humic substances on the 63Ni migration through crushed rock media
- U, Th, Eu and colloid mobility in a granite fracture under near-natural flow conditions
- Sorption behavior of europium(III) and curium(III) on the cell surfaces of microorganisms
- Interactions of trivalent and tetravalent heavy metal-siderophore complexes with Pseudomonas fluorescens
- In-situ diffusion of HTO, 22Na+, Cs+ and I- in Opalinus Clay at the Mont Terri underground rock laboratory
- 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
- Fracture flow and radionuclide transport in block-scale laboratory experiments
- Comparison between in situ and laboratory diffusion studies of HTO and halides in Opalinus Clay from the Mont Terri
- Solubility constraints on uranium concentrations in groundwaters of the Tono uranium deposit, Japan
- Mobility of uranium in tertiary argillaceous sediments – a natural analogue study
- Redistribution of U, Pb and REE in association with alteration of uranium minerals from the Koongarra deposit, Northern Territory, Australia
- Towards a common thermodynamic database for speciation models
- Geochemically derived non-gaseous radionuclide source term for the Asse salt mine – assessment for the use of a Mg(OH)2-based backfill material
- Simulation of remediation alternatives for a 137Cs contaminated soil
- Simulating reactive transport in time dependent multiphase flow problems
- Reactive transport modelling of a spent fuel repository in a stiff clay formation considering excavation damaged zones
- Coupled transport/reaction modelling of copper canister corrosion aided by microbial processes
