Minor actinides found in spent nuclear fuel, such as Am and Cm, have isotopes with substantial radioactive half- lives that generate significant amounts of heat, which is detrimental to long-term waste storage. As a result, selective extraction of these actinides from spent reactor fuel is currently of great interest. The standard approach for selective separation of the species of interest is on the basis of liquid-liquid extraction processes where an extractant molecule preferentially binds to one of the ion. These extractant molecules typically have a non-polar tail that helps them migrate, through an organic-aqueous interface, carrying the ions and effectively separating them. Designing such extractants molecules is of high interest and it requires overcoming significant difficulties imposed by the similarity in chemical interactions between the lanthanides in solution and the late actinides, both of which tend to be in a +3 oxidation state. In this talk we will present a series of theoretical studies on the basis of electronic structure calculations to analyze potential extractant molecules based on N, O, S, and a combination of them. Our calculations aim at understanding the origin of the differences in their interactions with the intention to identify design principles and propose new ligands.

Electronic structure and chemical bonding of f-element coordination complexes with N,O,S-donor ligand

2019 Spring National Meeting

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