Plutonium and Americium Alpha Radiolysis of Nitric Acid Solutions

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• 作者：Gregory P. HorneColin R. Gregson ; Howard E. Sims ; Robin M. Orr ; Robin J. Taylor ; Simon M. Pimblott
• 刊名：Journal of Physical Chemistry B
• 出版年：2017
• 出版时间：February 2, 2017
• 年：2017
• 卷：121
• 期：4
• 页码：883-889
• 全文大小：368K
• ISSN：1520-5207

文摘

The yield of HNO₂, as a function of absorbed dose and HNO₃ concentration, from the α-radiolysis of aerated HNO₃ solutions containing plutonium or americium has been investigated. There are significant differences in the yields measured from solutions of the two different radionuclides. For 0.1 mol dm^–3 HNO₃ solutions, the radiolytic yield of HNO₂ produced by americium α-decay is below the detection limit, whereas for plutonium α-decay the yield is considerably greater than that found previously for γ-radiolysis. The differences between the solutions of the two radionuclides are a consequence of redox reactions involving plutonium and the products of aqueous HNO₃ radiolysis, in particular H₂O₂ and HNO₂ and its precursors. This radiation chemical behavior is HNO₃ concentration dependent with the differences between plutonium and americium α-radiolysis decreasing with increasing HNO₃ concentration. This change may be interpreted as a combination of α-radiolysis direct effects and acidity influencing the plutonium oxidation state distribution, which in turn affects the radiation chemistry of the system.