Behavior of heptavalent technetium in sulfuric acid under α-irradiation

Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations

I. Denden, F. Poineau, M. L. Schlegel, J. Roques, P. Lorenzo Solari, G. Blain, K. R. Czerwinski, Rachid Essehli, J. Barbet, M. Fattahi

Research output: Contribution to journalArticle

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Abstract

The effect of α-radiolysis on the behavior of heptavalent technetium has been investigated in 13 and 18 M H2SO4. Irradiation experiments were performed using α-particles (4He2+, E = 68 MeV) generated by the ARRONAX cyclotron. UV-visible and X-ray absorption fine structure spectroscopic studies indicate that Tc(VII) is reduced to Tc(V) under α-irradiation. Extended X-ray absorption fine structure (EXAFS) spectroscopy measurements are consistent with the presence of mononuclear technetium sulfate complexes. Experimental results and density functional calculations show the formation of [TcO(HSO4)3(H 2O)(OH)]- and/or [TcO(HSO4)3(H 2O)2] and [Tc(HSO4)3(SO 4)(H2O)] and/or [Tc(HSO4)3(SO 4)(OH)]- for 13 and 18 M H2SO4, respectively.

Original languageEnglish
Pages (from-to)1568-1575
Number of pages8
JournalJournal of Physical Chemistry A
Volume118
Issue number9
DOIs
Publication statusPublished - 6 Mar 2014
Externally publishedYes

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X-Ray Absorption Spectroscopy
technetium
X ray absorption spectroscopy
Technetium
sulfuric acid
Sulfates
sulfates
absorption spectroscopy
fine structure
X-Rays
Irradiation
Extended X ray absorption fine structure spectroscopy
Cyclotrons
Radiolysis
irradiation
X ray absorption
radiolysis
Density functional theory
cyclotrons
Spectrum Analysis

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Behavior of heptavalent technetium in sulfuric acid under α-irradiation : Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations. / Denden, I.; Poineau, F.; Schlegel, M. L.; Roques, J.; Solari, P. Lorenzo; Blain, G.; Czerwinski, K. R.; Essehli, Rachid; Barbet, J.; Fattahi, M.

In: Journal of Physical Chemistry A, Vol. 118, No. 9, 06.03.2014, p. 1568-1575.

Research output: Contribution to journalArticle

Denden, I. ; Poineau, F. ; Schlegel, M. L. ; Roques, J. ; Solari, P. Lorenzo ; Blain, G. ; Czerwinski, K. R. ; Essehli, Rachid ; Barbet, J. ; Fattahi, M. / Behavior of heptavalent technetium in sulfuric acid under α-irradiation : Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations. In: Journal of Physical Chemistry A. 2014 ; Vol. 118, No. 9. pp. 1568-1575.
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AU - Solari, P. Lorenzo

AU - Blain, G.

AU - Czerwinski, K. R.

AU - Essehli, Rachid

AU - Barbet, J.

AU - Fattahi, M.

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