Evaluation of americium and curium-ligand complexation for liquid-based separation systems

In the research area of spent nuclear fuel reprocessing, the difficulties of extracting and separating the minor actinides Am and Cm from each other have been attributed to their similar chemical behaviors. However, the implementation of high-performance computing methods may greatly benefit research into Am/Cm separation based on interpolating data from reported bonds between these minor actinides and chelating ligands. An evaluation of Am- and Cm-containing compounds was conducted to determine preferential binding in liquid-liquid extraction systems. Gibbs free energies of reaction were calculated with electronic structure methods. The differences in Gibbs free energies of reaction between Am- and Cm-compounds with each ligand are used to determine the predicted efficiency of their use for extracting either actinide from the other. Results from level of theory evaluations, their significant impact on the chosen parameters of the environment and theoretical descriptions of the species, and preferential binding will be presented.