Radchenko Valery, Mastren Tara, Meyer Catherine A L, Ivanov Alexander S, Bryantsev Vyacheslav S, Copping Roy, Denton David, Engle Jonathan W, Griswold Justin R, Murphy Karen, Wilson Justin J, Owens Allison, Wyant Lance, Birnbaum Eva R, Fitzsimmons Jonathan, Medvedev Dmitri, Cutler Cathy S, Mausner Leonard F, Nortier Meiring F, John Kevin D, Mirzadeh Saed, Fassbender Michael E
Chemistry Division, Los Alamos National Laboratory, P.O. Box 1663, Los Alamos, NM 87545, USA; Life Science Division, TRIUMF, 4004 Wesbrook Mall, Vancouver, BC V6T 2A3, Canada.
Chemistry Division, Los Alamos National Laboratory, P.O. Box 1663, Los Alamos, NM 87545, USA.
Talanta. 2017 Dec 1;175:318-324. doi: 10.1016/j.talanta.2017.07.057. Epub 2017 Jul 20.
Actinium-225 is a potential Targeted Alpha Therapy (TAT) isotope. It can be generated with high energy (≥ 100MeV) proton irradiation of thorium targets. The main challenge in the chemical recovery of Ac lies in the separation from thorium and many fission by-products most importantly radiolanthanides. We recently developed a separation strategy based on a combination of cation exchange and extraction chromatography to isolate and purify Ac. In this study, actinium and lanthanide equilibrium distribution coefficients and column elution behavior for both TODGA (N,N,N',N'-tetra-n-octyldiglycolamide) and TEHDGA (N,N,N',N'-tetrakis-2-ethylhexyldiglycolamide) were determined. Density functional theory (DFT) calculations were performed and were in agreement with experimental observations providing the foundation for understanding of the selectivity for Ac and lanthanides on different DGA (diglycolamide) based resins. The results of Gibbs energy (ΔG) calculations confirm significantly higher selectivity of DGA based resins for Ln over Ac in the presence of nitrate. DFT calculations and experimental results reveal that Ac chemistry cannot be predicted from lanthanide behavior under comparable circumstances.
锕-225是一种潜在的靶向α治疗（TAT）同位素。它可以通过用高能（≥100MeV）质子辐照钍靶来产生。锕化学回收中的主要挑战在于从钍以及许多裂变副产物（最重要的是放射性镧系元素）中分离出来。我们最近开发了一种基于阳离子交换和萃取色谱相结合的分离策略来分离和纯化锕。在本研究中，测定了TODGA（N，N，N'，N'-四正辛基二甘醇酰胺）和TEHDGA（N，N，N'，N'-四-2-乙基己基二甘醇酰胺）的锕和镧系元素平衡分配系数以及柱洗脱行为。进行了密度泛函理论（DFT）计算，其与实验观察结果一致，为理解不同基于DGA（二甘醇酰胺）的树脂对锕和镧系元素的选择性提供了基础。吉布斯自由能（ΔG）计算结果证实，在硝酸盐存在下，基于DGA的树脂对镧系元素的选择性明显高于对锕的选择性。DFT计算和实验结果表明，在可比情况下，不能根据镧系元素的行为来预测锕的化学性质。
