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.
ASJC Scopus subject areas
- Physical and Theoretical Chemistry