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

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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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ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

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