Solid-liquid separation of oxidized americium from fission product lanthanides

Abstract

The separation of americium from the lanthanides and curium is a requirement if transmutation of americium is to be performed in advanced nuclear fuel cycles. Oxidation of Am3+ to AmO2+ or AmO22+ may allow separation of Am from Ln and Cm in one step, since the lanthanides and curium do not have higher oxidation states as accessible. Two possible solid-liquid separation methods have been developed to address this difficult separation. Under acidic conditions using oxone or persulfate, the oxidation and retention of tracer Am in the aqueous phase has been observed with a separation factor of 11 ± 1. Most of these studies have been conducted using 237NpO2(NO3), 233UO2(NO3)2, 238Pu(NO3)4 and 241Am(NO3)3 at radiotracer concentrations. Lanthanides precipitate as the sodium or potassium europium double sulfate salt. Under basic conditions, ozone oxidation of Am(CO3)OH(s) solubilizes Am from a lanthanide carbonate hydroxide solid phase to the aqueous phase as the AmO2(CO3)34-or AmO2(CO3)35- species. For the ozone oxidation of the americium tracer a separation factor of 1.6 ± 0.8 and 47 ± 2 for the oxidation/separation in Na2CO3 and NaHCO3 respectively.