@article {RADCHENKO2017318, title = {Radiometric evaluation of diglycolamide resins for the chromatographic separation of actinium from fission product lanthanides}, journal = {Talanta}, volume = {175}, year = {2017}, pages = {318 - 324}, abstract = {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 225Ac 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 225Ac. 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 (ΔGaq) calculations confirm significantly higher selectivity of DGA based resins for LnIII over AcIII in the presence of nitrate. DFT calculations and experimental results reveal that Ac chemistry cannot be predicted from lanthanide behavior under comparable circumstances.}, keywords = {Ac, Diglycolamide resins, Distribution coefficients, Extraction chromatography, Gibbs sorption energy, Lanthanide separation}, issn = {0039-9140}, doi = {https://doi.org/10.1016/j.talanta.2017.07.057}, url = {http://www.sciencedirect.com/science/article/pii/S0039914017307798}, author = {Valery Radchenko and Tara Mastren and Catherine A.L. Meyer and Alexander S. Ivanov and Vyacheslav S. Bryantsev and Roy Copping and David Denton and Jonathan W. Engle and Justin R. Griswold and Karen Murphy and Justin J. Wilson and Allison Owens and Lance Wyant and Eva R. Birnbaum and Jonathan Fitzsimmons and Dmitri Medvedev and Cathy S. Cutler and Leonard F. Mausner and Meiring F. Nortier and Kevin D. John and Saed Mirzadeh and Michael E. Fassbender} }