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The autoradiolytic oxidation of Pu(IV) and Am(III) has been investigated in saline solution of different NaCl concentrations, pH and specific α-activities. The high linear energy transfer (LET) property of α-radiation in solution enhances the oxidation of the Cl ion and thus increases the redox potential (Eh) of the NaCI solution system to a value of more than +1000 mV vs. NHE. Radiolytic reaction products are found as being comparable with those from the Cl2 saturated NaCl solution 'and create a metastable system consisting of C12/HCl0/Cl0−/Cl−. The oxidation of Pu(IV) and Am(III) in such solutions is dependent on the NaCl concentration, pH and specific a-activity involved. The quantitative oxidation to Pu(VI) and Am(V) is ob- served in the concentrated NaCl solution at pH > 7 with a moderately high specific activity (> 1 Ci/L).

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