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Leaching of zirconolite ceramics under H+ and He2+ irradiation
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M. Tribet
Published/Copyright:
September 25, 2009
Zirconolite is a candidate host material for conditioning minor tri- and tetra-valent actinides arising from enhanced nuclear spent fuel reprocessing and partitioning, which can be disposed in a geological repository for nuclear waste. Its chemical durability has been studied here under charged particle-induced radiolysis (He2+ and proton external beams) to identify possible effects on dissolution rates and mechanisms in pure water. Two geometries of experiments have been used to evaluate the influence of the following parameters: solid irradiation, Linear Energy Transfer (LET) at the interface and total deposited energy. Preliminary results on the elemental releases due to the enhanced dissolution of the zirconolite surface during charged particle-induced irradiation are first presented. Then, we focus on H2O2 production which is one of the major molecular species, created under water radiolysis, and likely to interact with the zirconolite surface. In presence of zirconolite, first results indicate an apparent consumption of the radiolytic hydrogen peroxide or its precursors compared to the production in pure water calculated from the primary yield GH2O2. The measured H2O2 concentration varies linearly with the total deposited energy in water over the irradiation duration (between 1 h and 6 h) and in the conditions of our experiments. Moreover, the H2O2 concentration decreases when the local density of the deposited energy close to the interface increases. Thus, we suggest that the mechanism(s) leading to the consumption of H2O2 or its precursors involve zirconolite surface reactions.
Keywords: Zirconolite; Radiolysis; Hydrogen Peroxide; Leaching; Irradiation; Linear Transfer Energy (LET)
Received: 2005-10-26
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
Zirconolite;
Radiolysis;
Hydrogen Peroxide;
Leaching;
Irradiation;
Linear Transfer Energy (LET)
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
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- Np(V)O2+ sorption on hydroxyapatite-effect of calcium and phosphate anions
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- Comparative study of cesium sorption on crushed and intact sedimentary rock
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- Biotransformation of plutonium complexed with citric acid
- Iodination of humic acid samples from different origins
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- 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
