Plutonium and Americium Alpha Radiolysis of Nitric Acid Solutions.
Plutonium and Americium Alpha Radiolysis of Nitric Acid Solutions.
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DOI：
10.1021/acs.jpcb.6b12061
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发表时间：
2017-01
期刊：
影响因子：
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通讯作者：
Gregory P. Horne;C. Gregson;H. Sims;R. Orr;R. Taylor;S. Pimblott
中科院分区：
文献类型：
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作者：
Gregory P. Horne;C. Gregson;H. Sims;R. Orr;R. Taylor;S. Pimblott
本文研究了含钚或Am的曝气硝酸溶液α辐解过程中硝酸产率随吸收剂量和硝酸浓度的变化规律。从两种不同放射性核素的溶液中测得的产额有显著差异。对于0.1moldm~(-3)HNO_3溶液，Amα衰变产生的HNO_2的辐解产额低于检测下限，而钚α衰变的产额比以前的γ辐解产额高得多。这两种放射性核素溶液之间的差异是钚与硝酸水溶液辐射分解产物，特别是H_2O_2和HNO_2及其前体的氧化还原反应的结果。这种辐射化学行为依赖于HNO_3浓度，钚和Am之间的差值α-辐解随着HNO_3浓度的增加而减小。这种变化可能被解释为α-辐解直接效应和酸度影响钚的氧化态分布，进而影响体系的辐射化学。
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.