Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel

Abstract

An investigation of molybdate melts containing sodium molybdate (Na2MoO4) and molybdenum trioxide (MoO3) to achieve the separation of uranium from fission products by crystallization has been performed. The separation is based on the difference in solubility of the fission product metal oxides compared to the uranium oxide or molybdate in the molybdate melt. The molybdate melt dissolves uranium dioxide at high temperatures, and upon cooling, uranium precipitates as uranium dioxide or molybdate, whereas the fission product metals remain soluble in the melt. Small-scale experiments using gram quantities of uranium dioxide have been performed to investigate the feasibility of UO2 purification from the fission products. The composition of the uranium precipitate as well as data for partitioning of several fission product surrogates between the uranium precipitate and molybdate melt for various melt compositions are presented and discussed. The fission products Cs, Sr, Ru and Rh all displayed very large distribution ratios. The fission products Zr, Pd, and the lanthanides also displayed good distribution ratios (D > 10). A melt consisting of 20 wt% MoO3- 50 wt% Na2MoO4-30 wt% UO2 heated to 1313 K and cooled to 1123 K for the physical separation of the UO2 product from the melt, and washed once with Na2MoO4 displays optimum conditions for separation of the UO2 from the fission products.