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Sorption of radionuclides onto natural clay rocks

  • E. Hartmann , H. Geckeis , Thomas Rabung , Johannes Lützenkirchen and Thomas Fanghänel
Published/Copyright: September 25, 2009
Radiochimica Acta
From the journal Radiochimica Acta Volume 96 Issue 9-11

Abstract

Reactions of U(VI) and Eu/Cm(III) with natural clay rock (Opalinus Clay, Switzerland, and Callovo-Oxfordian Clay, France) are investigated by batch and spectroscopic experiments as well as geochemical calculations. The aim of the studies is to identify those minerals in the heterogeneous multiphase systems with sometimes high calcite content which control lanthanide and actinide sorption. The outcome of batch sorption studies with natural clay rocks (2 g/L natural clay rock, 0.1 mol/L NaClO4, pH 3−11) and thermodynamic calculations is compared with experimental results using a synthetic mixture consisting of purified Na-montmorillonite and calcite (ratio 80:20[wt.]%). Our studies show that U(VI) sorption decreases at intermediate pH (6.5−9) where dissolved U(VI) carbonate species predominate. In the high pH region (>9) U(VI) sorption again increases by formation of ternary hydroxo surface complexes on the clay mineral fraction, whereby calculated U(VI) sorption overestimates experimental data for the natural rock. Complete sorption to natural clay rock and the synthetic clay/calcite mixture is observed for Eu(III) at pH>7 for the conditions studied. Model calculations again point to the predominance of clay-sorbed species even though calculated speciation underestimates the experimentally observed sorption at pH 6−9 slightly. Preliminary time-resolved laser-fluorescence spectroscopy (TRLFS) studies using Cm(III) as fluorescent probe reveal the appearance of several Cm(III)-clay surface species in the pH range 5−11, but give no indications for the presence of calcite-bound Cm(III). We conclude that the clay minerals in the multiphasic clay rock act as main sorbents for tri- and hexavalent actinides.

Keywords: Sorption; Clays; Eu(III); U(VI); TRLFS
* Correspondence address: Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, P.O. Box 3640, 76021 Karlsruhe, Deutschland,
Published Online: 2009-09-25
Published in Print: 2008-11

© by Oldenbourg Wissenschaftsverlag, Karlsruhe, Germany

Articles in the same Issue

  1. Preface
  2. Discrepancies in thorium oxide solubility values: a new experimental approach to improve understanding of oxide surface at solid/solution interface
  3. Modeling plutonium solubility for Yucca Mountain performance assessment
  4. Uranium/technetium separation for the UREX process – synthesis and characterization of solid reprocessing forms
  5. UO2 dissolution in the presence of hydrogen peroxide at pH>11
  6. Solubility of Zr(IV), Th(IV) and Pu(IV) hydrous oxides in CaCl2 solutions and the formation of ternary Ca-M(IV)-OH complexes
  7. A TRLFS study of Cm(III) hydroxide complexes in alkaline CaCl2 solutions
  8. Thermodynamic interpretation of neptunium coprecipitation in uranophane for application to the Yucca Mountain repository
  9. Structural investigation of coprecipitation of technetium-99 with iron phases
  10. 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
  11. Thermodynamic study on the U(VI) complexation with dicarboxylates by calorimetry
  12. A cryogenic fluorescence spectroscopic study of uranyl carbonate, phosphate and oxyhydroxide minerals
  13. A spectroscopic study of the effect of ligand complexation on the reduction of uranium(VI) by anthraquinone-2,6-disulfonate (AH2DS)
  14. The relationship of monodentate and bidentate coordinated uranium(VI) sulfate in aqueous solution
  15. Hydrolysis constants of tetravalent neptunium by using solvent extraction method
  16. Leaching of a zirconolite ceramic waste-form under proton and He2+ irradiation
  17. Oxidative dissolution of Tc(IV)O2·nH2O colloids by sonolysis
  18. Technetium reduction and reoxidation behaviour in Dounreay soils
  19. Effects of hydrogen and bromide on the corrosion of spent nuclear fuel and γ-irradiated UO2(s) in NaCl brine
  20. Sorption of selenium on Mg-Al and Mg-Al-Eu layered double hydroxides
  21. Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)
  22. Polarized EXAFS characterization of the sorption mechanism of yttrium on hectorite
  23. Measuring sorption coefficients and BET surface areas on intact drillcore and crushed granite samples
  24. Hydration and hydrolysys of Sm3+ and Eu3+ in a clay interlayer: a neutron diffraction study with isotopic substitution
  25. Sorption of neptunium onto goethite in the presence of humic acids with different hydroquinone group content
  26. The influence of carbonate complexation on lanthanide/actinide sorption on montmorillonite
  27. Sorption of radionuclides onto natural clay rocks
  28. The influence of natural organic matter on the speciation and solubility of Eu in Boom Clay porewater
  29. Sorption behavior of americium onto bentonite colloid
  30. Vertical distribution of 238Pu, 239(40)Pu, 241Am, 90Sr and 137Cs in Austrian soil profiles
  31. Pu(V) reduction and enhancement of particle-water partitioning by exopolymeric substances
  32. Laser ablation microprobe inductively coupled plasma mass spectrometry study on diffusion of uranium into cement materials
  33. Binding of Pu(IV) to galacturonic acid and extracellular polymeric substances (EPS) from Shewanella putrefaciens, Clostridium sp. and Pseudomonas fluorescens
https://doi.org/10.1524/ract.2008.1556
Keywords for this article
Sorption; Clays; Eu(III); U(VI); TRLFS

Articles in the same Issue

  1. Preface
  2. Discrepancies in thorium oxide solubility values: a new experimental approach to improve understanding of oxide surface at solid/solution interface
  3. Modeling plutonium solubility for Yucca Mountain performance assessment
  4. Uranium/technetium separation for the UREX process – synthesis and characterization of solid reprocessing forms
  5. UO2 dissolution in the presence of hydrogen peroxide at pH>11
  6. Solubility of Zr(IV), Th(IV) and Pu(IV) hydrous oxides in CaCl2 solutions and the formation of ternary Ca-M(IV)-OH complexes
  7. A TRLFS study of Cm(III) hydroxide complexes in alkaline CaCl2 solutions
  8. Thermodynamic interpretation of neptunium coprecipitation in uranophane for application to the Yucca Mountain repository
  9. Structural investigation of coprecipitation of technetium-99 with iron phases
  10. 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
  11. Thermodynamic study on the U(VI) complexation with dicarboxylates by calorimetry
  12. A cryogenic fluorescence spectroscopic study of uranyl carbonate, phosphate and oxyhydroxide minerals
  13. A spectroscopic study of the effect of ligand complexation on the reduction of uranium(VI) by anthraquinone-2,6-disulfonate (AH2DS)
  14. The relationship of monodentate and bidentate coordinated uranium(VI) sulfate in aqueous solution
  15. Hydrolysis constants of tetravalent neptunium by using solvent extraction method
  16. Leaching of a zirconolite ceramic waste-form under proton and He2+ irradiation
  17. Oxidative dissolution of Tc(IV)O2·nH2O colloids by sonolysis
  18. Technetium reduction and reoxidation behaviour in Dounreay soils
  19. Effects of hydrogen and bromide on the corrosion of spent nuclear fuel and γ-irradiated UO2(s) in NaCl brine
  20. Sorption of selenium on Mg-Al and Mg-Al-Eu layered double hydroxides
  21. Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)
  22. Polarized EXAFS characterization of the sorption mechanism of yttrium on hectorite
  23. Measuring sorption coefficients and BET surface areas on intact drillcore and crushed granite samples
  24. Hydration and hydrolysys of Sm3+ and Eu3+ in a clay interlayer: a neutron diffraction study with isotopic substitution
  25. Sorption of neptunium onto goethite in the presence of humic acids with different hydroquinone group content
  26. The influence of carbonate complexation on lanthanide/actinide sorption on montmorillonite
  27. Sorption of radionuclides onto natural clay rocks
  28. The influence of natural organic matter on the speciation and solubility of Eu in Boom Clay porewater
  29. Sorption behavior of americium onto bentonite colloid
  30. Vertical distribution of 238Pu, 239(40)Pu, 241Am, 90Sr and 137Cs in Austrian soil profiles
  31. Pu(V) reduction and enhancement of particle-water partitioning by exopolymeric substances
  32. Laser ablation microprobe inductively coupled plasma mass spectrometry study on diffusion of uranium into cement materials
  33. Binding of Pu(IV) to galacturonic acid and extracellular polymeric substances (EPS) from Shewanella putrefaciens, Clostridium sp. and Pseudomonas fluorescens
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