Separation of Am from lanthanides and Cm using the ADAAM(EH)-DTBA extraction system and elucidation of its complexation with DTBA through DFT calculations

Sasaki, Yuji  ; Kaneko, Masashi   ; Kumagai, Yuta   ; Ban, Yasutoshi  

We developed a method called the alkyl-diamide amine (ADAAM(EH))-diethylenetriamine-triacetic acid-bis(diethylacetamide) (DTBA) technique for separating actinide (An) and lanthanide (Ln) elements from high-level liquid waste. ADAAM(EH) exhibits a high separation factor (SF) not only for Am/Cm but also for light/heavy Ln under acidic conditions (1.5 M HNO). Consequently, Am can be separated from Cm as well as from middle Ln (Sm, Eu, and Gd) using ADAAM(EH) as an extractant. DTBA enables the stripping of Am and potentially separates it from Ln in the organic phase at low pH ( 2). The lowest SF among the light Ln, observed for Nd/Am, exceeded 10, indicating that Am can be separated from light Ln by stripping using DTBA from the ADAAM(EH) extraction solvent. The density functional theory calculations for understanding the coordination bond properties of metal-DTBA complexes are performed, which supported higher affinity of DTBA toward Am than Nd.