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The mechanism of PuVI oxidation with ozone and other reagents in alkaline solutions

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Abstract

The analysis of reported data on the interaction of ozone with alkaline solutions of PuVI leads to the conclusion that the process of ozonation involves reactions O3 + OH– → HO -2 + O2, O3 + + HO -2 + OH– → O -3 + O -2 + H2O and O3 + O -2 → O -3 + O2. The O -3 radical ion oxidizes PuVI, the HO -2 and O -2 anions reduce PuVII and PuVI and react with O -3 . Using persulfate instead of O3 in aerated solution at 80—95 °C results in thermal decomposition of the S2O 2-8 anion into radical ions of SO -4 , oxidizing OH– to the O– ion, which in reaction with O2 forms O -3 . The oxidation of PuVI proceeds via the formation of an activated complex with O -3 . where charge transfer occurs with the simultaneous elimination of two H+ ions. A similar mechanism is operating in reactions of PuVI with BrO–, Fe(CN) 3–6 , AmVI, and AmVII. Upon the γ-radiolysis of alkaline solutions of PuVI saturated with N2O or containing S2O 2–8 , e –aq is converted into O– and then into O -3 ; F2 and XeF2 in alkaline solutions are decomposed with the formation of H2O2, which prevents producing PuVII.

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Authors and Affiliations

  1. A. N. Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences, Build. 4, 31 Leninsky prosp., 119071, Moscow, Russian Federation

    V. P. Shilov, A. V. Gogolev, A. M. Fedosseev & B. G. Ershov

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  1. V. P. Shilov
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  2. A. V. Gogolev
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  3. A. M. Fedosseev
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  4. B. G. Ershov
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Correspondence to A. V. Gogolev.

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Published in Russian in Izvestiya Akademii Nauk. Seriya Khimicheskaya, No. 10, pp. 2351—2354, October, 2016.

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Shilov, V.P., Gogolev, A.V., Fedosseev, A.M. et al. The mechanism of PuVI oxidation with ozone and other reagents in alkaline solutions. Russ Chem Bull 65, 2351–2354 (2016). https://doi.org/10.1007/s11172-016-1587-5

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  • DOI: https://doi.org/10.1007/s11172-016-1587-5

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