Incorporation of Neptunium(V) and Iodate into a Uranyl Phosphate: Implications for Mitigating the Release of 237Np and 129I in Repositories

Abstract

Listen

Translate article

The simultaneous incorporation of IO3(-) and NpO2+ into Ba3(UO2)2(HPO4)2(PO4)2 (BaUP), which serves as a model for uranyl alteration phases, was investigated. LA-ICP-MS data demonstrate that the incorporation of both of these species is significantly enhanced when they are present together. The most probable explanation is that charge balance is obtained by the coupled substitutions of NpO2+ <--> UO2(2+) and IO3(-) <--> HPO4(2-). According to the LA-ICP-MS results, in the absence of iodate as much as 2.91 +/- 0.14 to 3.44 +/- 0.25% of the uranium in BaUP can be replaced by neptunium. When iodate is present in the reaction, the amount of uranium substitution by neptunium increases to 6.05 +/- 0.65% to 7.93 +/- 0.83%. The net increase for neptunium is 116 +/- 0.30% to 225 +/- 0.25%. Similarly, in the absence of NpO2+, iodate incorporation into BaUP reaches an I/U level of 0.0021 +/- 0.0004 to 0.0038 +/- 0.0005; whereas in its presence there is an increase to as much as 100 +/- 0.11% to 0.0042 +/- 0.0008.