Speciation of technetium in carbonate media under helium ions and γ radiation
-
Mohammad Ghalei
,
Frederic Poineau
Abstract
Technetium carbonates complexes produced by chemical, electrochemical and radiolytic methods have been studied by UV-Visible, X-ray Absorption Fine Structure (XAFS) and Density Functional Theory methods. The (NH4)2TcCl6 salt was dissolved in 2 M KHCO3. The resulting purple solution was analyzed by XAFS and UV-Visible spectroscopy. The UV-Visible spectra exhibits a band centered at 515 nm. The XAFS results were consistent with the presence of polymeric species containing the [Tc2(μ−O)2]4+ core coordinated to carbonate ligand. Concerning the electrochemical methods, the pertechnetate anion was electrochemically reduced in concentrated carbonate solution [(CO32−)=5 M and (HCO3−)=0.5 M]. For the radiolytic reduction, the speciation of Tc under Helium ions particle beam and γ radiation was examined by UV-Visible and XAFS spectroscopy in high concentrated carbonate media. In concentrated carbonate solutions, pertechnetate as Tc(VII), was not reduced under irradiation due to the formation of carbonate radical which is a strong oxidant. Then, the solution proposed was the addition of formate to the solution which can scavenge hydroxyl radical 10 times faster than carbonate and prevent re-oxidation of reduced technetium. The XANES and EXAFS spectroscopies, approved by theoretical methods, revealed that the final product of the radiolytic reduction of pertechnetate is in the +IV oxidation state. The final structure of the reduced product by He2+ radiolysis was the same as electrochemical reduction. From this complex determination and evolution vs. the dose, this study is reporting the solubility of the Tc(IV) complex.
Acknowledgment
The authors would like to thank the ARRONAX staff for the efficient performing of irradiation runs in the cyclotron facility. This work has been supported in part by a grant from the French National Agency for Research called “Investissements d’Avenir”, Equipex ArronaxPlus n°ANR-11-EQPX-0004. The authors would like to thank SOLEIL synchrotron for provision of beam time using MARS beamline. Use of the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.
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©2019 Walter de Gruyter GmbH, Berlin/Boston
Artikel in diesem Heft
- Frontmatter
- Electrochemical and thermodynamic properties of U4+ and U3+ on Mo electrode in LiCl-KCl eutectic
- Speciation of technetium in carbonate media under helium ions and γ radiation
- Effect of sulfate on sorption of Eu(III) by Na-montmorillonite
- Effect of grain size on radon emanation coefficient, surface and mass exhalation rates and the correlation coefficient between them in different masses of soil and phosphate fertilizer
- Ratio primary reference measurement procedure (RPRMP) for the certification of chromium content in biological reference materials
- Photon activation analysis of sand samples from Antalya in Turkey with a clinical electron linear accelerator
- 68Ga@pyridine-functionalized MCM-41 mesoporous silica: a novel radio labeled composite for diagnostic applications
- Kinetics of nonisothermal dehydration of unirradiated and γ-ray irradiated neodymium (III) acetate hydrate
- Investigation of radiation shielding properties for some ceramics
Artikel in diesem Heft
- Frontmatter
- Electrochemical and thermodynamic properties of U4+ and U3+ on Mo electrode in LiCl-KCl eutectic
- Speciation of technetium in carbonate media under helium ions and γ radiation
- Effect of sulfate on sorption of Eu(III) by Na-montmorillonite
- Effect of grain size on radon emanation coefficient, surface and mass exhalation rates and the correlation coefficient between them in different masses of soil and phosphate fertilizer
- Ratio primary reference measurement procedure (RPRMP) for the certification of chromium content in biological reference materials
- Photon activation analysis of sand samples from Antalya in Turkey with a clinical electron linear accelerator
- 68Ga@pyridine-functionalized MCM-41 mesoporous silica: a novel radio labeled composite for diagnostic applications
- Kinetics of nonisothermal dehydration of unirradiated and γ-ray irradiated neodymium (III) acetate hydrate
- Investigation of radiation shielding properties for some ceramics
