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

Abstract

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.

Authors:
 [1];  [2];  [2];  [3];  [3];  [3];  [3];  [4];  [3];  [3];  [5];  [3];  [3];  [2];  [6];  [6];  [6];  [6];  [2];  [2] more »;  [3];  [2] « less
+ Show Author Affiliations
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); TRIUMF, Vancouver, BC (Canada)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Wisconsin, Madison, WI (United States)
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Cornell Univ., Ithaca, NY (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Nuclear Physics (NP)
OSTI Identifier:
1372800
Alternate Identifier(s):
OSTI ID: 1409769; OSTI ID: 1481648; OSTI ID: 1549645
Report Number(s):
LA-UR-17-22523; LA-UR-17-22508
Journal ID: ISSN 0039-9140
Grant/Contract Number:  
AC52-06NA25396; AC05-00OR22725; AC52-06NA253996
Resource Type:
Accepted Manuscript
Journal Name:
Talanta
Additional Journal Information:
Journal Volume: 175; Journal Issue: C; Journal ID: ISSN 0039-9140
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 225Ac; lanthanide separation; extraction chromatography; diglycolamide resins; distribution coefficients; Gibbs sorption energy

Citation Formats

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, and Fassbender, Michael E. Radiometric evaluation of diglycolamide resins for the chromatographic separation of actinium from fission product lanthanides. United States: N. p., 2017. Web. doi:10.1016/j.talanta.2017.07.057.
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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. Radiometric evaluation of diglycolamide resins for the chromatographic separation of actinium from fission product lanthanides. United States. https://doi.org/10.1016/j.talanta.2017.07.057
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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, and Fassbender, Michael E. Thu . "Radiometric evaluation of diglycolamide resins for the chromatographic separation of actinium from fission product lanthanides". United States. https://doi.org/10.1016/j.talanta.2017.07.057. https://www.osti.gov/servlets/purl/1372800.
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@article{osti_1372800,
title = {Radiometric evaluation of diglycolamide resins for the chromatographic separation of actinium from fission product lanthanides},
author = {Radchenko, Valery and Mastren, Tara and Meyer, Catherine A. L. and Ivanov, Alexander S. and Bryantsev, Vyacheslav S. and Copping, Roy and Denton, David and Engle, Jonathan W. and Griswold, Justin R. and Murphy, Karen and Wilson, Justin J. and Owens, Allison and Wyant, Lance and Birnbaum, Eva R. and Fitzsimmons, Jonathan and Medvedev, Dmitri and Cutler, Cathy S. and Mausner, Leonard F. and Nortier, Meiring F. and John, Kevin D. and Mirzadeh, Saed and Fassbender, Michael E.},
abstractNote = {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.},
doi = {10.1016/j.talanta.2017.07.057},
journal = {Talanta},
number = C,
volume = 175,
place = {United States},
year = {Thu Jul 20 00:00:00 EDT 2017},
month = {Thu Jul 20 00:00:00 EDT 2017}
}
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    Works referencing / citing this record:

    Selective biosorption of thorium (IV) from aqueous solutions by ginkgo leaf
    journal, March 2018

    Development of 225 Ac Radiopharmaceuticals: TRIUMF Perspectives and Experiences
    journal, October 2018

    • Robertson, Andrew Kyle Henderson; Ramogida, Caterina Fortunata; Schaffer, Paul
    • Current Radiopharmaceuticals, Vol. 11, Issue 3
    • DOI: 10.2174/1874471011666180416161908
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