skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Talanta
 [1];  [2];  [2];  [3];  [3];  [3];  [3];  [4];  [3];  [3];  [5];  [3];  [3];  [2];  [6];  [6];  [6];  [6];  [2];  [2] more »;  [3];  [2] « less
  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)
+ Show Author Affiliations

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.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Nuclear Physics (NP)
Grant/Contract Number:
AC52-06NA25396; AC05-00OR22725; AC52-06NA253996
OSTI ID:
1372800
Alternate ID(s):
OSTI ID: 1409769; OSTI ID: 1481648; OSTI ID: 1549645
Report Number(s):
LA-UR-17-22523; LA-UR-17-22508
Journal Information:
Talanta, Vol. 175, Issue C; ISSN 0039-9140
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science

References (33)

Targeted α-therapy: past, present, future? journal January 2007
Cancer Therapy with Alpha-Emitters Labeled Peptides journal May 2010
Realizing the potential of the Actinium-225 radionuclide generator in targeted alpha particle therapy applications journal September 2008
213Bi-DOTATOC receptor-targeted alpha-radionuclide therapy induces remission in neuroendocrine tumours refractory to beta radiation: a first-in-human experience journal July 2014
225Ac-PSMA-617 for PSMA-Targeted  -Radiation Therapy of Metastatic Castration-Resistant Prostate Cancer journal July 2016
Proton-induced cross sections relevant to production of 225Ac and 223Ra in natural thorium targets below 200MeV journal November 2012
Production of actinium-225 for alpha particle mediated radioimmunotherapy journal May 2005
Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes journal February 2015
Separation of actinides from Low Level Liquid Wastes (LLLW) by extraction chromatography using novel DMDOHEMA and TODGA impregnated resins journal January 2004
Novel Extraction of Chromatographic Resins Based on Tetraalkyldiglycolamides: Characterization and Potential Applications journal May 2005
Extraction chromatographic studies of metal ions using N,N,N′,N′-tetraoctyl diglycolamide as the stationary phase journal February 2006
An Improved Method for the Production of Ac‐225/Bi‐213 from Th‐229 for Targeted Alpha Therapy journal April 2007
Synergistic Enhancement of the Extraction of Trivalent Lanthanides and Actinides by Tetra‐( n ‐Octyl)Diglycolamide from Chloride Media journal January 2008
Extraction chromatography of lanthanides using N,N,N′,N′-tetraoctyl diglycolamide (TODGA) as the stationary phase journal September 2008
Rapid method for determination of 228Ra in water samples journal October 2012
Distribution coefficients of 60 elements on TODGA resin: Application to Ca, Lu, Hf, U and Th isotope geochemistry journal May 2010
Large scale accelerator production of 225Ac: Effective cross sections for 78–192 MeV protons incident on 232Th targets journal December 2016
Density‐functional thermochemistry. III. The role of exact exchange journal April 1993
The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals journal July 2007
Energy-adjusted pseudopotentials for the rare earth elements journal January 1989
Use of Solution-Phase Vibrational Frequencies in Continuum Models for the Free Energy of Solvation journal December 2011
Quantum Mechanical Continuum Solvation Models journal August 2005
Trivalent Actinide and Lanthanide Separations by Tetradentate Nitrogen Ligands: A Quantum Chemistry Study journal October 2011
An europium( iii ) diglycolamide complex: insights into the coordination chemistry of lanthanides in solvent extraction journal January 2015
Crystal Structures of Ln(III) (Ln = La, Pr, Nd, Sm, Eu, and Gd) Complexes with N , N , N ′, N ′-Tetraethyldiglycolamide Associated with Homoleptic [Ln(NO 3 ) 6 )] 3− journal February 2014
The separation mechanism of Am( iii ) from Eu( iii ) by diglycolamide and nitrilotriacetamide extraction reagents using DFT calculations journal January 2016
The selectivity of diglycolamide (TODGA) and bis-triazine-bipyridine (BTBP) ligands in actinide/lanthanide complexation and solvent extraction separation – a theoretical approach journal January 2015
Crystal Structures of Lanthanoid(III) (Ln(III), Ln = Tb, Dy, Ho, Er, Tm, Yb, and Lu) Nitrate Complexes with N , N , N ′, N ′-Tetraethyldiglycolamide journal October 2014
Ligand design for selective complexation of metal ions in aqueous solution journal December 1989
Separation of Am, Cm and Lanthanides by Solvent Extraction with Hydrophilic and Lipophilic Organic Ligands journal January 2011
Actinide Lanthanide Separation Process—ALSEP journal January 2014
A Computational Approach to Predicting Ligand Selectivity for the Size-Based Separation of Trivalent Lanthanides: A Computational Approach to Predicting Ligand Selectivity for the Size-Based Separation of Trivalent Lanthanides journal June 2016
“Straining” to Separate the Rare Earths: How the Lanthanide Contraction Impacts Chelation by Diglycolamide Ligands journal November 2016

Cited By (2)

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

Similar Records

The Coordination Chemistry and Stoichiometry of Extracted Diglycolamide Complexes of Lanthanides in Extraction Chromatography Materials
Journal Article · Mon Sep 06 00:00:00 EDT 2021 · Solvent Extraction and Ion Exchange · OSTI ID:1372800
+6 more
Structure Activity Relationship Approach toward the Improved Separation of Rare-Earth Elements Using Diglycolamides
Journal Article · Fri Nov 13 00:00:00 EST 2020 · Inorganic Chemistry · OSTI ID:1372800
+9 more
Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes
Journal Article · Thu Dec 18 00:00:00 EST 2014 · Journal of Chromatography · OSTI ID:1372800
+7 more

Related Subjects

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