PNNL

Abstract

Advanced concepts for closing the nuclear fuel cycle include separating Am and Cm from other fuel components. Separating these elements from the lanthanide elements at an industrial scale remains a significant technical challenge. We describe here a chemical system in which a neutral extractant--octyl(phenyl)-N,N-diisobutyl-carbamoylmethyl-phosphine oxide (CMPO)--is combined with an acidic extractant--bis-(2-ethylhexyl)phosphoric acid (HDEHP)--to form a single process solvent (with dodecane as the diluent) for separating Am and Cm from the other components of irradiated nuclear fuel. Continuous variation experiments in which the relative CMPO and HDEHP concentrations are varied indicate a synergistic relationship between the two extractants in the extraction of Am from buffered diethylenetriaminepentaacetic acid (DTPA) solutions. A solvent mixture consisting or 0.1 M CMPO + 1 M HDEHP in dodecane offers acceptable extraction efficiency for the trivalent lanthanides and actinides from 1 M HNO3 while maintaining good lanthanide/actinide separation factors in the stripping regime (buffered DTPA solutions with pH 3.5 to 4). Using citrate buffer instead of lactate buffer results in improved lanthanide/actinide separation factors.