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The influence of carbonate complexation on lanthanide/actinide sorption on montmorillonite
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Maria Marques Fernandes
Veröffentlicht/Copyright:
25. September 2009
Abstract
The safety case for radioactive waste repositories is, to a large extend based on the physical and chemical retention of radionuclides on clay minerals which are important constituents in both the man-made engineered barriers and in argillaceous host rock formations. The presence of carbonate, one of the most important inorganic ligands for lanthanide and actinide ions in groundwaters and clay porewaters, can have a significant influence on their sorption behaviour on clay minerals. The sorption of Eu(III) on Na-montmorillonite in the absence and the presence of carbonate was investigated in batch sorption experiments. In the presence of carbonate two sets of experimental conditions were investigated. Eu(III) sorption measurements were performed as a function of pH in equilibrium with atmospheric pCO2 (=10−3.5 bar) and at a variable pCO2 (=10−1.4 to 10−3.4 bar). The sorption data were modelled using the 2 site protolysis non-electrostatic surface complexation and cation exchange model. Both experimental data sets in the presence of carbon could be quantitatively modelled by including in the sorption model two additional surface complexation reactions on the strong sites forming ≡SSOEuCO30 and ≡SSOEuOHCO3− surface complexes.
Keywords: Actinide surface complexation; Carbonate complexation; Montmorillonite; Sorption modelling
Published Online: 2009-09-25
Published in Print: 2008-11
© by Oldenbourg Wissenschaftsverlag, Villigen PSI, Germany
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Artikel in diesem Heft
- Preface
- Discrepancies in thorium oxide solubility values: a new experimental approach to improve understanding of oxide surface at solid/solution interface
- Modeling plutonium solubility for Yucca Mountain performance assessment
- Uranium/technetium separation for the UREX process – synthesis and characterization of solid reprocessing forms
- UO2 dissolution in the presence of hydrogen peroxide at pH>11
- Solubility of Zr(IV), Th(IV) and Pu(IV) hydrous oxides in CaCl2 solutions and the formation of ternary Ca-M(IV)-OH complexes
- A TRLFS study of Cm(III) hydroxide complexes in alkaline CaCl2 solutions
- Thermodynamic interpretation of neptunium coprecipitation in uranophane for application to the Yucca Mountain repository
- Structural investigation of coprecipitation of technetium-99 with iron phases
- Synthesis, crystallographic characterization, and conformational prediction of a structurally unique molecular mixed-ligand U(VI) solid, Na6[UO2(O2)2(OH)2](OH)2·14H2O
- Thermodynamic study on the U(VI) complexation with dicarboxylates by calorimetry
- A cryogenic fluorescence spectroscopic study of uranyl carbonate, phosphate and oxyhydroxide minerals
- A spectroscopic study of the effect of ligand complexation on the reduction of uranium(VI) by anthraquinone-2,6-disulfonate (AH2DS)
- The relationship of monodentate and bidentate coordinated uranium(VI) sulfate in aqueous solution
- Hydrolysis constants of tetravalent neptunium by using solvent extraction method
- Leaching of a zirconolite ceramic waste-form under proton and He2+ irradiation
- Oxidative dissolution of Tc(IV)O2·nH2O colloids by sonolysis
- Technetium reduction and reoxidation behaviour in Dounreay soils
- Effects of hydrogen and bromide on the corrosion of spent nuclear fuel and γ-irradiated UO2(s) in NaCl brine
- Sorption of selenium on Mg-Al and Mg-Al-Eu layered double hydroxides
- Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)
- Polarized EXAFS characterization of the sorption mechanism of yttrium on hectorite
- Measuring sorption coefficients and BET surface areas on intact drillcore and crushed granite samples
- Hydration and hydrolysys of Sm3+ and Eu3+ in a clay interlayer: a neutron diffraction study with isotopic substitution
- Sorption of neptunium onto goethite in the presence of humic acids with different hydroquinone group content
- The influence of carbonate complexation on lanthanide/actinide sorption on montmorillonite
- Sorption of radionuclides onto natural clay rocks
- The influence of natural organic matter on the speciation and solubility of Eu in Boom Clay porewater
- Sorption behavior of americium onto bentonite colloid
- Vertical distribution of 238Pu, 239(40)Pu, 241Am, 90Sr and 137Cs in Austrian soil profiles
- Pu(V) reduction and enhancement of particle-water partitioning by exopolymeric substances
- Laser ablation microprobe inductively coupled plasma mass spectrometry study on diffusion of uranium into cement materials
- Binding of Pu(IV) to galacturonic acid and extracellular polymeric substances (EPS) from Shewanella putrefaciens, Clostridium sp. and Pseudomonas fluorescens
Schlagwörter für diesen Artikel
Actinide surface complexation;
Carbonate complexation;
Montmorillonite;
Sorption modelling
Artikel in diesem Heft
- Preface
- Discrepancies in thorium oxide solubility values: a new experimental approach to improve understanding of oxide surface at solid/solution interface
- Modeling plutonium solubility for Yucca Mountain performance assessment
- Uranium/technetium separation for the UREX process – synthesis and characterization of solid reprocessing forms
- UO2 dissolution in the presence of hydrogen peroxide at pH>11
- Solubility of Zr(IV), Th(IV) and Pu(IV) hydrous oxides in CaCl2 solutions and the formation of ternary Ca-M(IV)-OH complexes
- A TRLFS study of Cm(III) hydroxide complexes in alkaline CaCl2 solutions
- Thermodynamic interpretation of neptunium coprecipitation in uranophane for application to the Yucca Mountain repository
- Structural investigation of coprecipitation of technetium-99 with iron phases
- Synthesis, crystallographic characterization, and conformational prediction of a structurally unique molecular mixed-ligand U(VI) solid, Na6[UO2(O2)2(OH)2](OH)2·14H2O
- Thermodynamic study on the U(VI) complexation with dicarboxylates by calorimetry
- A cryogenic fluorescence spectroscopic study of uranyl carbonate, phosphate and oxyhydroxide minerals
- A spectroscopic study of the effect of ligand complexation on the reduction of uranium(VI) by anthraquinone-2,6-disulfonate (AH2DS)
- The relationship of monodentate and bidentate coordinated uranium(VI) sulfate in aqueous solution
- Hydrolysis constants of tetravalent neptunium by using solvent extraction method
- Leaching of a zirconolite ceramic waste-form under proton and He2+ irradiation
- Oxidative dissolution of Tc(IV)O2·nH2O colloids by sonolysis
- Technetium reduction and reoxidation behaviour in Dounreay soils
- Effects of hydrogen and bromide on the corrosion of spent nuclear fuel and γ-irradiated UO2(s) in NaCl brine
- Sorption of selenium on Mg-Al and Mg-Al-Eu layered double hydroxides
- Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)
- Polarized EXAFS characterization of the sorption mechanism of yttrium on hectorite
- Measuring sorption coefficients and BET surface areas on intact drillcore and crushed granite samples
- Hydration and hydrolysys of Sm3+ and Eu3+ in a clay interlayer: a neutron diffraction study with isotopic substitution
- Sorption of neptunium onto goethite in the presence of humic acids with different hydroquinone group content
- The influence of carbonate complexation on lanthanide/actinide sorption on montmorillonite
- Sorption of radionuclides onto natural clay rocks
- The influence of natural organic matter on the speciation and solubility of Eu in Boom Clay porewater
- Sorption behavior of americium onto bentonite colloid
- Vertical distribution of 238Pu, 239(40)Pu, 241Am, 90Sr and 137Cs in Austrian soil profiles
- Pu(V) reduction and enhancement of particle-water partitioning by exopolymeric substances
- Laser ablation microprobe inductively coupled plasma mass spectrometry study on diffusion of uranium into cement materials
- Binding of Pu(IV) to galacturonic acid and extracellular polymeric substances (EPS) from Shewanella putrefaciens, Clostridium sp. and Pseudomonas fluorescens
