Molecular Hydrogen Yields from the α-Self-Radiolysis of Nitric Acid Solutions Containing Plutonium or Americium

The Journal of Physical Chemistry. B
Colin R GregsonKevin J Webb

Abstract

The yield of molecular hydrogen, as a function of nitric acid concentration, from the α-radiolysis of aerated nitric acid and its mixtures with sulfuric acid containing plutonium or americium has been investigated. Comparison of experimental measurements with predictions of a Monte Carlo radiation track chemistry model shows that, in addition to scavenging of the hydrated electron, its precursor, and the hydrogen atom, the quenching of excited state water is important in controlling the yield of molecular hydrogen. In addition, increases in solution acidity cause a significant change in the track reactions, which can be explained as resulting from scavenging of eaq- by Haq+ to form H•. Although plutonium has been shown to be an effective scavenger of precursors of molecular hydrogen below 0.1 mol dm-3 nitrate, previously reported effects of plutonium on G(H2)α between 1 and 10 mol dm-3 nitric acid were not reproduced. Modeling results suggest that plutonium is unlikely to effectively compete with nitrate ions in scavenging the precursors of molecular hydrogen at higher nitric acid concentrations, and this was confirmed by comparing molecular hydrogen yields from plutonium solutions with those from americium solutions. Finally, ...Continue Reading

References

Dec 16, 2016·The Journal of Physical Chemistry. B·G P HorneS P Mezyk
Jan 10, 2017·The Journal of Physical Chemistry. B·Gregory P HorneSimon M Pimblott
May 12, 2017·The Journal of Physical Chemistry. B·Gregory P HorneJay A LaVerne

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Citations

Jul 12, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Gregory P HorneBruce J Mincher
Mar 6, 2021·Journal of Computational Chemistry·Nikolai AndreadiVladimir Petrov

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