TY - JOUR
T1 - Radiometric evaluation of diglycolamide resins for the chromatographic separation of actinium from fission product lanthanides
AU - Radchenko, Valery
AU - Mastren, Tara
AU - Meyer, Catherine A.L.
AU - Ivanov, Alexander S.
AU - Bryantsev, Vyacheslav S.
AU - Copping, Roy
AU - Denton, David
AU - Engle, Jonathan W.
AU - Griswold, Justin R.
AU - Murphy, Karen
AU - Wilson, Justin J.
AU - Owens, Allison
AU - Wyant, Lance
AU - Birnbaum, Eva R.
AU - Fitzsimmons, Jonathan
AU - Medvedev, Dmitri
AU - Cutler, Cathy S.
AU - Mausner, Leonard F.
AU - Nortier, Meiring F.
AU - John, Kevin D.
AU - Mirzadeh, Saed
AU - Fassbender, Michael E.
N1 - Publisher Copyright:
© 2017 Elsevier B.V.
PY - 2017/12/1
Y1 - 2017/12/1
N2 - 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 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.
AB - 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 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.
KW - Ac
KW - Diglycolamide resins
KW - Distribution coefficients
KW - Extraction chromatography
KW - Gibbs sorption energy
KW - Lanthanide separation
UR - http://www.scopus.com/inward/record.url?scp=85025151364&partnerID=8YFLogxK
U2 - 10.1016/j.talanta.2017.07.057
DO - 10.1016/j.talanta.2017.07.057
M3 - Article
C2 - 28841997
AN - SCOPUS:85025151364
SN - 0039-9140
VL - 175
SP - 318
EP - 324
JO - Talanta
JF - Talanta
ER -