Influence of plutonium oxidation state on the formation of molecular hydrogen, nitrous acid and nitrous oxide from alpha radiolysis of nitric acid solution

The study of the formation of radiolytic products, such as molecular hydrogen and nitrous acid, is of primary importance in the reprocessing of spent nuclear fuel and the storage of aqueous solutions containing radioactive materials. The radiolytic yields of molecular hydrogen, nitrous acid and nitrous oxide from alpha radiolysis of nitric acid solutions containing plutonium have been experimentally investigated. The results have shown that the yields of radiolytic products depends on the nitric acid concentration as well as the oxidation state of plutonium. However, the influence of plutonium oxidation state on radiolytic yields is less notable as the nitric acid concentration increases. Molecular hydrogen production decreases with increasing nitric acid concentration while nitrous acid and nitrous oxide productions increase. While radiolytic yields from plutonium(IV) nitric acid solutions have been previously investigated, this study provides radiolytic yields from alpha radiolysis of plutonium(III) and plutonium(VI) nitric acid solutions for molecular hydrogen, nitrous acid and nitrous oxide. These information provide insight into the role played by plutonium redox behaviour on the formation of radiolytic products.