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Solubility of ThO2·xH2O(am) and the formation of ternary Th(IV) hydroxide-carbonate complexes in NaHCO3-Na2CO3 solutions containing 0−4 M NaCl
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M. Altmaier
Published/Copyright:
September 25, 2009
The solubility of ThO2· x H2O(am) is studied at I=0.1−4.0 M (NaHCO3-Na2CO3-NaCl) and 22 °C. Several sets of closed system experiments are performed at total carbonate concentrations of Ctot=[HCO3-]+[CO32-]=0.02 and 0.1 M in the range pHc = 8−11. In our recent study at I=0.5 M, the simultaneous evaluation of solubility data at widely varied pHc and carbonate concentrations has shown that Th(OH)(CO3)45-, Th(OH)2(CO3)22- and Th(OH)4(CO3)2- are the most important ternary complexes. The present results at I=0.1−4.0 M are used to describe the ionic strength dependence of the equilibrium constants logKs, 1yz (for the reactions Th(OH)4(am)+zCO32-↔Th(OH)y(CO3)z4-y-2z+(4-y)OH-) with the SIT. EXAFS measurements in 0.1 and 1.0 M carbonate solutions support the calculated speciation. They show clearly different spectra for the predominant species Th(OH)(CO3)45- and Th(CO3)56-, respectively.
Keywords: Thorium(IV); Solubility; Carbonate solution; Hydroxide-carbonate complexes; Thermodynamic modelling; Ionic strength; SIT
Received: 2005-9-19
Accepted: 2006-3-26
Published Online: 2009-9-25
Published in Print: 2006-11-1
© Oldenbourg Wissenschaftsverlag
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Keywords for this article
Thorium(IV);
Solubility;
Carbonate solution;
Hydroxide-carbonate complexes;
Thermodynamic modelling;
Ionic strength;
SIT
Articles in the same Issue
- Preface Migration 2005
- Solubility measurement of zirconium(IV) hydrous oxide
- Solubility of ThO2·xH2O(am) and the formation of ternary Th(IV) hydroxide-carbonate complexes in NaHCO3-Na2CO3 solutions containing 0−4 M NaCl
- Ion interaction (SIT) coefficients for the Th4+ ion and trace activity coefficients in NaClO4, NaNO3 and NaCl solution determined by solvent extraction with TBP
- Leaching of neptunium from garnet- and murataite-based ceramics
- Coprecipitation of thorium and lanthanum with UO2+x(s) as host phase
- Rare Earth element (REE) incorporation in natural calcite: Upper limits for actinide uptake in a secondary phase
- Protonation of D-gluconate and its complexation with Np(V) in acidic to nearly neutral solutions
- Complexing properties of α-isosaccharinate: thorium
- Determination of the thermodynamic quantities of complexation between Eu(III) and carboxylic acids by microcalorimetry
- Potentiometric investigations on the interaction of humic acid with Cu(II) and Eu(III) ions
- Investigation of complexation of thorium by humic acid using chemically immobilized humic acid on silica gel
- Correlation between X-ray chemical shift and partial charge in Tc(IV) complexes: Determination of Tc partial charge in TcnOy(4n-2y)+
- Oxidation and dissolution rates of UO2(s) in carbonate-rich solutions under external alpha irradiation and initially reducing conditions
- On the stability of Pu(III) at different pH under non-inert conditions
- Reduction behavior of uranium in the presence of citric acid
- Leaching of zirconolite ceramics under H+ and He2+ irradiation
- Reduction of plutonium(VI) in brine under subsurface conditions
- Theoretical first step towards an understanding of the uranyl ion sorption on the rutile TiO2(110) face: A DFT periodic and cluster study
- Cm(III) sorption onto γ-Al2O3: New insight into sorption mechanisms by time-resolved laser fluorescence spectroscopy and extended X-ray absorption fine structure
- Modelling sorption data for the actinides Am(III), Np(V) and Pa(V) on montmorillonite
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- Np(V)O2+ sorption on hydroxyapatite-effect of calcium and phosphate anions
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- Biotransformation of plutonium complexed with citric acid
- Iodination of humic acid samples from different origins
- The fate of the epsilon phase (Mo-Ru-Pd-Tc-Rh) in the UO2 of the Oklo natural fission reactors
- Rhenium migration at the Maqarin natural analogue site (Jordan)
- Classic adsorption isotherms incorporated in modern surface complexation models: Implications for sorption of actinides
- Use of thermodynamic sorption models to derive radionuclide Kd values for performance assessment: selected results and recommendations of the NEA sorption project
- Modeling spent nuclear fuel alteration and radionuclide migration in disposal conditions
