The use of electromigration as a qualitative technique to study the migration behaviour and speciation of uranium in the Boom Clay
-
N. Maes
Summary
Under the geochemical conditions prevailing in situ in the Boom Clay Formation (pH, Eh, …), calculations predict that U(OH)4 is the dominant uranium species present in the interstitial water and the concentration is solubility limited. However the boundary of the domain where the non solubility limited UO2(CO3)34− species dominates is very close. It is therefore of prime interest to know the correct speciation of uranium during the migration process.
Electromigration was used as technique with the advantage that it can provide information on the speciation because the movement of the species towards the electrodes depends on its charge and speciation. Electromigration experiments have been performed with preconditioned 233UO2(CO3)34− sources, starting from the hypothesis that this species should migrate without retardation towards the anode. Despite relatively long electromigration times, sufficient to displace strong retarded tracers, no displacement of the migration profile towards the anode was observed. All 233U remained near the source position, but the electropherograms clearly showed the presence of species moving towards the cathode. This indicates the presence of neutral or positively charged uranium species. These electropherograms are interpreted as a change in uranium valence state: reduction of UO2(CO3)34− and precipitation of U(IV) oxy-hydroxides near the source position. The solubility limited species, U(OH)4(aq), are carried with the pore water towards the cathode. The electromigration experiments indicate, in support of the speciation calculations, that the dominant migrating U-species is probably the solubility limited U(OH)4.
© Oldenbourg Wissenschaftsverlag, München
Artikel in diesem Heft
- Solubility of amorphous Th(IV) hydroxide – application of LIBD to determine the solubility product and EXAFS for aqueous speciation
- Thermodynamics of the U(VI)-Ca2+-Cl −-OH −-H2O system: Solubility product of becquerelite
- Control of plutonium dioxide solubility by amorphous tetrahydroxide: A critical review of the model
- Technetium migration in fluoroapatite during thermal annealing
- Uranium release from boom clay in bicarbonate media
- Coprecipitation of thorium with UO2
- Formation of secondary phases after long-term corrosion of simulated HLW glass in brine solutions at 190 °C
- Sorption behaviour of Am on precorroded HLW glass in water and brines
- Molecular fluorescence spectroscopy and mixture analysis for the evaluation of the complexation between humic acid and UO22+
- Investigation on uranyl interaction with bioactive ligands. Synthesis and structural studies of the uranyl complexes with glycine and N-(2-mercaptopropionyl)glycine
- Complex formation of calcium with humic acid and polyacrylic acid
- Complexation of americium with humic, fulvic and citric acids at high ionic strength
- Complex formation of Eu(III) with humic acid and polyacrylic acid
- XAS study of technetium(IV) polymer formation in mixed sulphate/chloride media
- Complexation of uranium(VI) with malonate at variable temperatures
- The hydrolysis of uranium(VI)
- Corrosion and dissolution studies of UO2 containing α-emitters
- The effects of alpha-radiolysis on UO2 dissolution determined from electrochemical experiments with 238Pu-doped UO2
- Radiolytic formation of Tc(IV) oxide colloids
- Radiation-chemical effects in the near-field of a final disposal site: role of bromine on the radiolytic processes in NaCl-solutions
- The reduction of U(VI) on corroded iron under anoxic conditions
- New selenium solution speciation method by ion chromatography + gamma counting and its application to FeS2-controlled reducing conditions
- Uptake of oxo-anions by cements through solid-solution formation: experimental evidence and modelling
- Iodine species uptake by cement and CSH studied by I K-edge X-ray absorption spectroscopy
- Structure of uranium sorption complexes at montmorillonite edge sites
- Sorption of several safety relevant radionuclides on granite and diorite – a potential repository host rock in the Taiwan area
- Sorption and reduction of neptunium(V) on the surface of iron oxides
- Uptake mechanism of IO3− to NO3−-hydrotalcite
- Structure alteration of C-S-H (calcium silicate hydrated phases) caused by sorption of caesium
- The effect of α-isosaccharinic acid on the stability of and Th(IV) uptake by hardened cement paste
- Complexation studies of Eu(III) with polyacrylic acid either free in solution or adsorbed onto alumina
- Sorption behaviour of caesium on a bentonite sample
- Specific interaction of cesium with the surface of calcium silicate hydrates
- Relationship of quantitative X-ray diffraction measurements of geologic materials to cesium sorption
- Instrumental development for spectroscopic speciation of f-elements in hydrothermal solutions: luminescence properties of lanthanide(III) ions
- Application of microprecipitation on membrane filters for Alpha Spectrometry, liquid scintillation counting and Mass Spectrometric determination of plutonium isotopes
- Characterization of aquatic colloids by a combination of LIBD and ICP-MS following the size fractionation
- Technetium behaviour in Boom Clay – a laboratory and field study
- The use of electromigration as a qualitative technique to study the migration behaviour and speciation of uranium in the Boom Clay
- Input contribution and vertical migration of plutonium, americium and cesium in lake sediments (Belham Tarn, Cumbria, UK)
- Diffusion of 22Na+, 85Sr2+, 134Cs+ and 57Co2+ in bentonite clay compacted to different densities: experiments and modeling
- U6+ phases in the weathering zone of the Bangombé U-deposit: observed and predicted mineralogy
- Precipitation of technetium by subsurface sulfate-reducing bacteria
- Spectroscopic studies on the interaction of U(VI) with Bacillus sphaericus
- Bio-sorption of neptunium(V) by Pseudomonas fluorescens
- Biotransformation of pertechnetate by Clostridia
- Solubility and hydrolysis of Zr oxides: a review and supplemental data
- Nagra/PSI Chemical Thermodynamic Data Base 01/01
- Sorption modelling by Gibbs energy minimisation: Towards a uniform thermodynamic database for surface complexes of radionuclides
Artikel in diesem Heft
- Solubility of amorphous Th(IV) hydroxide – application of LIBD to determine the solubility product and EXAFS for aqueous speciation
- Thermodynamics of the U(VI)-Ca2+-Cl −-OH −-H2O system: Solubility product of becquerelite
- Control of plutonium dioxide solubility by amorphous tetrahydroxide: A critical review of the model
- Technetium migration in fluoroapatite during thermal annealing
- Uranium release from boom clay in bicarbonate media
- Coprecipitation of thorium with UO2
- Formation of secondary phases after long-term corrosion of simulated HLW glass in brine solutions at 190 °C
- Sorption behaviour of Am on precorroded HLW glass in water and brines
- Molecular fluorescence spectroscopy and mixture analysis for the evaluation of the complexation between humic acid and UO22+
- Investigation on uranyl interaction with bioactive ligands. Synthesis and structural studies of the uranyl complexes with glycine and N-(2-mercaptopropionyl)glycine
- Complex formation of calcium with humic acid and polyacrylic acid
- Complexation of americium with humic, fulvic and citric acids at high ionic strength
- Complex formation of Eu(III) with humic acid and polyacrylic acid
- XAS study of technetium(IV) polymer formation in mixed sulphate/chloride media
- Complexation of uranium(VI) with malonate at variable temperatures
- The hydrolysis of uranium(VI)
- Corrosion and dissolution studies of UO2 containing α-emitters
- The effects of alpha-radiolysis on UO2 dissolution determined from electrochemical experiments with 238Pu-doped UO2
- Radiolytic formation of Tc(IV) oxide colloids
- Radiation-chemical effects in the near-field of a final disposal site: role of bromine on the radiolytic processes in NaCl-solutions
- The reduction of U(VI) on corroded iron under anoxic conditions
- New selenium solution speciation method by ion chromatography + gamma counting and its application to FeS2-controlled reducing conditions
- Uptake of oxo-anions by cements through solid-solution formation: experimental evidence and modelling
- Iodine species uptake by cement and CSH studied by I K-edge X-ray absorption spectroscopy
- Structure of uranium sorption complexes at montmorillonite edge sites
- Sorption of several safety relevant radionuclides on granite and diorite – a potential repository host rock in the Taiwan area
- Sorption and reduction of neptunium(V) on the surface of iron oxides
- Uptake mechanism of IO3− to NO3−-hydrotalcite
- Structure alteration of C-S-H (calcium silicate hydrated phases) caused by sorption of caesium
- The effect of α-isosaccharinic acid on the stability of and Th(IV) uptake by hardened cement paste
- Complexation studies of Eu(III) with polyacrylic acid either free in solution or adsorbed onto alumina
- Sorption behaviour of caesium on a bentonite sample
- Specific interaction of cesium with the surface of calcium silicate hydrates
- Relationship of quantitative X-ray diffraction measurements of geologic materials to cesium sorption
- Instrumental development for spectroscopic speciation of f-elements in hydrothermal solutions: luminescence properties of lanthanide(III) ions
- Application of microprecipitation on membrane filters for Alpha Spectrometry, liquid scintillation counting and Mass Spectrometric determination of plutonium isotopes
- Characterization of aquatic colloids by a combination of LIBD and ICP-MS following the size fractionation
- Technetium behaviour in Boom Clay – a laboratory and field study
- The use of electromigration as a qualitative technique to study the migration behaviour and speciation of uranium in the Boom Clay
- Input contribution and vertical migration of plutonium, americium and cesium in lake sediments (Belham Tarn, Cumbria, UK)
- Diffusion of 22Na+, 85Sr2+, 134Cs+ and 57Co2+ in bentonite clay compacted to different densities: experiments and modeling
- U6+ phases in the weathering zone of the Bangombé U-deposit: observed and predicted mineralogy
- Precipitation of technetium by subsurface sulfate-reducing bacteria
- Spectroscopic studies on the interaction of U(VI) with Bacillus sphaericus
- Bio-sorption of neptunium(V) by Pseudomonas fluorescens
- Biotransformation of pertechnetate by Clostridia
- Solubility and hydrolysis of Zr oxides: a review and supplemental data
- Nagra/PSI Chemical Thermodynamic Data Base 01/01
- Sorption modelling by Gibbs energy minimisation: Towards a uniform thermodynamic database for surface complexes of radionuclides