A study on selective precipitation ability of cyclic urea to U(VI) for developing reprocessing system based on precipitation method

Abstract

We have proposed a new reprocessing system based on precipitation method. In order to find out precipitants with high selectivity to U(VI) and to investigate factors controlling precipitation ability to U(VI) and U(IV), properties of 3,4,5,6-tetrahydro-1,3-dimethyl-2(1H)-pyrimidinone (DMPU) as a precipitant have been examined by using U(VI), U(IV) as a simulant of Pu(IV), and simulated fission products (FPs). We have evaluated precipitation ratios (P.R.) for U(VI) and U(IV), solubility of U(VI) precipitates to 3.0 mol dm−3 (M) HNO3 solution, melting points (MPs) of U(VI) precipitates, log P (distribution ratio of a substance in 1-octanol/water biphasic system, a measure of hydrophobicity) of precipitants, and decontamination factors (DFs) of FPs. The properties of DMPU were compared with those in systems using N-n-butyl-2-pyrrolidone (NBP), N-cyclohexyl-2-pyrrolidone (NCP), and other pyrrolidone derivatives as the precipitant. The P.R. values of DMPU to U(VI) and U(IV) in 3.0 M HNO3 solutions were around 99% at [DMPU]/[U(VI)] = 2.0 and 0% at [DMPU]/[U(IV)] = 5.0, respectively. In DMPU system, the DF values of the most of simulated FPs [Rb(I), Cs(I), Sr(II), Ba(II), Ru(III), Rh(III), La(III), Ce(III), Pr(III), Nd(III), and Sm(III)] used in the present study were found to be more than 100. Even in U(VI)–U(IV) coexisting system, the selectivity of DMPU to U(VI) was higher than those of NBP and NCP. This selective precipitation ability of DMPU to U(VI) was evaluated by the solubility of U(VI) precipitates on the basis of their MPs and the log P values of precipitants. As a result, it was found that the precipitants having low hydrophobicity and forming the U(VI) precipitates with high MPs have highly selective precipitation ability to U(VI).