Theoretical prediction of separation performance of minor-actinides by introducing carbonyl donors to TPEN ligand

Kaneko, Masashi   ; Watanabe, Masayuki   ; Matsumura, Tatsuro  

In Japan Atomic Energy Agency, the extraction reagents for the inter- and intragroup separation of mainor-actinides from lanthanides have been developed in order to construct the partitioning and transmutation process. We aim to reveal the separation mechanism using various extraction materials at a molecular level and to design the novel extraction reagents. In this study, we design a novel TPEN-type extraction reagent in which carbonyl donors are introduced and predict its separation performance of Am(III) from Eu(III) using density functional calculations. We modeled molecular complexes by referring single crystal structures and compared the stability between Eu(III) and Am(III) complexes. As a result, the relative stability of Am complex to Eu complex increased and its separation factor was improved by an order from five to twenty compared to the prediction value by non-substituent TPEN ligand.