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Title: Speciation of technetium in carbonate media under helium ions and γ radiation

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 (NH 4) 2TcCl 6 salt was dissolved in 2 M KHCO 3. 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 [Tc 2(μ-O) 2] 4+ core coordinated to carbonate ligand. Concerning the electrochemical methods, the pertechnetate anion was electrochemically reduced in concentrated carbonate solution [(CO 3 2-)=5 M and (HCO 3 -)=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 themore » radiolytic reduction of pertechnetate is in the +IV oxidation state. The final structure of the reduced product by He 2+ 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.« less

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
FOREIGN
OSTI Identifier:
1493771
Resource Type:
Journal Article
Journal Name:
Radiochimica Acta
Additional Journal Information:
Journal Volume: 107; Journal Issue: 2; Journal ID: ISSN 0033-8230
Publisher:
de Gruyter
Country of Publication:
United States
Language:
ENGLISH

Citation Formats

Ghalei, Mohammad, Vandenborre, Johan, Poineau, Frederic, Blain, Guillaume, Solari, Pier-Lorenzo, Rôques, Jerome, Haddad, Ferid, and Fattahi, Massoud. Speciation of technetium in carbonate media under helium ions and γ radiation. United States: N. p., 2019. Web. doi:10.1515/ract-2018-2939.
Ghalei, Mohammad, Vandenborre, Johan, Poineau, Frederic, Blain, Guillaume, Solari, Pier-Lorenzo, Rôques, Jerome, Haddad, Ferid, & Fattahi, Massoud. Speciation of technetium in carbonate media under helium ions and γ radiation. United States. doi:10.1515/ract-2018-2939.
Ghalei, Mohammad, Vandenborre, Johan, Poineau, Frederic, Blain, Guillaume, Solari, Pier-Lorenzo, Rôques, Jerome, Haddad, Ferid, and Fattahi, Massoud. Mon . "Speciation of technetium in carbonate media under helium ions and γ radiation". United States. doi:10.1515/ract-2018-2939.
@article{osti_1493771,
title = {Speciation of technetium in carbonate media under helium ions and γ radiation},
author = {Ghalei, Mohammad and Vandenborre, Johan and Poineau, Frederic and Blain, Guillaume and Solari, Pier-Lorenzo and Rôques, Jerome and Haddad, Ferid and Fattahi, Massoud},
abstractNote = {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.},
doi = {10.1515/ract-2018-2939},
journal = {Radiochimica Acta},
issn = {0033-8230},
number = 2,
volume = 107,
place = {United States},
year = {2019},
month = {2}
}

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