Behavior of Actinide Elements and Fission Products in Recovery of Uranyl Nitrate Hexahydrate Crystal by Cooling Crystallization Method

To elucidate various kinds of actinide element and fission product behavior, U crystallization experiments were carried out with a uranyl nitrate solution and with a solution in which irradiated fast reactor core fuel was dissolved. Insoluble residue simulating that found in actual reactor operation was not incorporated into the uranyl nitrate hexahydrate (UNH) crystal in the course of the U crystallization. However, the decontamination factors (DFs) were below 10 even when the UNH crystal was washed because the mother liquor containing the simulated insoluble residue occupied the interspaces of the agglutinated UNH crystal. In the U crystallization process, the DF of Pu was >40 when the UNH crystal was washed. But, Np was not removed from the UNH crystal because Np was oxidized to Np(VI) in the feed solution and thus was co-crystallized with U(VI). Cesium exhibited different behavior depending on whether Pu was present. Although a high DF of Cs was obtained in the case of uranyl nitrate solution without Pu, Cs was hardly separated at all from the UNH crystal formed from the dissolver solution of irradiated fast reactor core fuel. It is likely that crystals of a mixed salt of Pu and Cs, Cs₂Pu(NO₃)₆, precipitated from the dissolver solution. Since Ba precipitated as Ba(NO₃)₂ during the crystallization process, its DF was low after the UNH crystal was washed. On the other hand, Am, Cm, Rb, Sr, Zr, Nb, Ru, Sb, and rare earth elements remained in the mother liquor at the time of U crystallization. Therefore, portions of these elements in the mother liquor that was attached to the surface of the UNH crystal were washed away with HNO₃ solution.