Radiometric evaluation of diglycolamide resins for the chromatographic separation of actinium from fission product lanthanides

TALANTA

卷:175

Article

Radchenko, Valery^1,2  Mastren, Tara¹  Meyer, Catherine A. L.¹  Ivanov, Alexander S.³  Bryantsev, Vyacheslav S.³  Copping, Roy⁴  Denton, David⁴  Engle, Jonathan W.^1,5  Griswold, Justin R.⁴  Murphy, Karen⁴  Wilson, Justin J.^1,6  Owens, Allison⁴  Wyant, Lance³  Birnbaum, Eva R.¹  Fitzsimmons, Jonathan⁷  Medvedev, Dmitri⁷  Cutler, Cathy S.⁷  Mausner, Leonard F.⁷  Nortier, Meiring F.¹  John, Kevin D.¹  Mirzadeh, Saed⁴  Fassbender, Michael E.¹ 

[1] Los Alamos Natl Lab, Div Chem, POB 1663, Los Alamos, NM 87545 USA

[2] TRIUMF, Div Life Sci, 4004 Wesbrook Mall, Vancouver, BC V6T 2A3, Canada

[3] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA

[4] Oak Ridge Natl Lab, Nucl Secur & Isotope Technol Div, Oak Ridge, TN 37831 USA

[5] Univ Wisconsin, Dept Med Phys, Madison, WI 53705 USA

[6] Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14853 USA

[7] Brookhaven Natl Lab, Collider Accelerator Dept, Bldg 801, Upton, NY 11973 USA

关键词: Ac-225;    Lanthanide separation;    Extraction chromatography;    Diglycolamide resins;    Distribution coefficients;    Gibbs sorption energy;   

DOI  :  10.1016/j.talanta.2017.07.057

来源: Elsevier

【 摘 要 】

Actinium-225 is a potential Targeted Alpha Therapy (TAT) isotope. It can be generated with high energy (>= 100 MeV) proton irradiation of thorium targets. The main challenge in the chemical recovery of Ac-225 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-225. 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 (Delta G(aq)) calculations confirm significantly higher selectivity of DGA based resins for Ln(III) over Ac-III in the presence of nitrate. DFT calculations and experimental results reveal that Ac chemistry cannot be predicted from lanthanide behavior under comparable circumstances.

【 授权许可】

Free