Th(Ⅳ) and U(Ⅵ) removal by TODGA in ionic liquids:extraction behavior and mechanism,and radiation effect

摘要

Extraction behavior of thorium(Ⅳ) and uranium(Ⅵ) from nitric acid(HNO_3) was studied using N,N,N',N'-tetraoctyldiglycolamide(TODGA) as extractant in different ionic liquids, and isooctane as comparison.Slope analyses with varying HNO_3 concentrations and diluents revealed the extraction mechanism. With increasing length of alkyl chain and HNO_3 concentration, the extraction mechanism of TODGA/IL system changed from cation exchange to neutral complex and/or anion exchange,and the molar ratio between TODGA and metal ions varied gradually from 2:1 to 1:1 for Th(Ⅳ) and 3:1 to 1:1 for U(Ⅵ). The kinetics and thermodynamic studies of Th(Ⅳ)and U(Ⅵ) by the best TODGA/[C_2mim][NTf_2] system showed that the extraction equilibrium was reached within 2 h and extraction reactions were endothermic. Compared to TODGA/isooctane system, TODGA/[C_2mim][NTf_2]system presented higher radiation stability under c-irradiation. Therefore, it would have a promising application in spent fuel reprocessing.