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Ion interaction (SIT) coefficients for the Th4+ ion and trace activity coefficients in NaClO4, NaNO3 and NaCl solution determined by solvent extraction with TBP
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Volker Neck
Veröffentlicht/Copyright:
25. September 2009
Trace activity coefficients of the Th4+ ion in dilute to concentrated NaClO4, NaNO3 and NaCl solutions ([H+]=0.01−0.02 M) have been determined at 22 °C from liquid-liquid phase equilibria with 10−50 vol.% TBP in n-dodecane. Using the specific ion interaction theory (SIT) to describe these equilibria as a function of the medium electrolyte concentration, the following ion interaction coefficients are calculated: ε(Th4+, ClO4-)=0.70±0.06 kg/mol and ε(Th4+, NO3-) = 0.31±0.12 kg/mol. The latter value differs considerably from ε(Th4+, NO3-) = 0.11±0.02 kg/mol used in the NEA-TDB. The low distribution coefficients at mNaCl<3 mol/kg do not allow the linear SIT extrapolation to I=0, but the equilibrium constants in 2.5−5.0 m NaCl are compatible with the NEA-TDB value of ε(Th4+, Cl-)=0.25±0.03 kg/mol.
The SIT coefficients determined for the Th4+ ion follow the linear correlations between known values of ε(MZ+, NO3-), ε(MZ+, Cl-) and ε(MZ+, ClO4-) for non-complexed cations MZ+ with Z=1−4, including ε(Pu4+, ClO4-)=0.82±0.07 kg/mol and ε(Pu4+, Cl-)=0.37±0.05 kg/mol calculated from data accepted in the NEA-TDB. The interaction coefficients in the series of the tetravalent actinide ions show a slight systematic dependence on the ionic radius.
Keywords: Thorium; TBP; Extraction; Activity coefficients; SIT; Ion interaction coefficients; Th4+; Pu4+
Received: 2005-2-17
Accepted: 2006-3-26
Published Online: 2009-9-25
Published in Print: 2006-11-1
© Oldenbourg Wissenschaftsverlag
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Artikel in diesem Heft
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Schlagwörter für diesen Artikel
Thorium;
TBP;
Extraction;
Activity coefficients;
SIT;
Ion interaction coefficients;
Th4+;
Pu4+
Artikel in diesem Heft
- 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
- Sorption of Cs, Ni, Pb, Eu(III), Am(III), Cm, Ac(III), Tc(IV), Th, Zr, and U(IV) on MX 80 bentonite: An experimental approach to assess model uncertainty
- The uptake of radium by calcium silicate hydrates and hardened cement paste
- Np(V)O2+ sorption on hydroxyapatite-effect of calcium and phosphate anions
- Uranium(VI) interaction with pyrite (FeS2): Chemical and spectroscopic studies
- Interaction of U(VI) with pyrite, galena and their mixtures: a theoretical and multitechnique approach
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- Mechanisms of cesium sorption onto magnetite
- Sorption of cesium on granite under aerobic and anaerobic conditions
- Comparative study of cesium sorption on crushed and intact sedimentary rock
- The INE-Beamline for actinide research at ANKA
- Evaluation of the reversibility of iodide uptake by argillaceous rocks by the radial diffusion method
- Thermal diffusion of chlorine in uranium dioxide
- Effects of ionic strength on the coordination of Eu(III) and Cm(III) to a Gram-negative bacterium, Paracoccus denitrificans
- Interaction mechanisms of bacterial strains isolated from extreme habitats with uranium
- 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
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