Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes

Radchenko, Valery; Engle, Jonathan W.; Wilson, Justin Jeff; Maassen, Joel Ryan; Nortier, Francois Meiring; Taylor, Wayne Allen; Birnbaum, Eva R.; Hudston, Lisa Ann; John, Kevin Dale; Fassbender, Michael Ernst

doi:10.1016/j.chroma.2014.12.045

Title: 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

DOI:https://doi.org/10.1016/j.chroma.2014.12.045· OSTI ID:1492639

Radchenko, Valery ^[1]; Engle, Jonathan W. ^[1]; Wilson, Justin Jeff ^[1];

^[1];

^[1]; Taylor, Wayne Allen ^[1];

^[1]; Hudston, Lisa Ann ^[1];

^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

We present that actinium-225 (t_1/2 = 9.92 d) is an α-emitting radionuclide with nuclear properties well-suited for use in targeted alpha therapy (TAT), a powerful treatment method for malignant tumors. Actinium-225 can also be utilized as a generator for ²¹³Bi (t_1/2 45.6 min), which is another valuable candidate for TAT. Actinium-225 can be produced via proton irradiation of thorium metal; however, long-lived ²²⁷Ac (t_1/2 = 21.8 a, 99% β^-, 1% α) is co-produced during this process and will impact the quality of the final product. Thus, accurate assays are needed to determine the ²²⁵Ac/²²⁷Ac ratio, which is dependent on beam energy, irradiation time and target design. Accurate actinium assays, in turn, require efficient separation of actinium isotopes from both the Th matrix and highly radioactive activation by-products, especially radiolanthanides formed from proton-induced fission. In this study, we introduce a novel, selective chromatographic technique for the recovery and purification of actinium isotopes from irradiated Th matrices. A two-step sequence of cation exchange and extraction chromatography was implemented. Radiolanthanides were quantitatively removed from Ac, and no non-Ac radionuclidic impurities were detected in the final Ac fraction. An ²²⁵Ac spike added prior to separation was recovered at ≥98%, and Ac decontamination from Th was found to be ≥10⁶. Finally, the purified actinium fraction allowed for highly accurate ²²⁷Ac determination at analytical scales, i.e., at ²²⁷Ac activities of 1–100 kBq (27 nCi to 2.7 μCi).

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Nuclear Physics (NP)

Grant/Contract Number:: 89233218CNA000001; AC52-06NA253996

OSTI ID:: 1492639

Alternate ID(s):: OSTI ID: 1244093

Report Number(s):: LA-UR-14-26567

Journal Information:: Journal of Chromatography, Vol. 1380, Issue C; ISSN 0021-9673

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 74 works

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References (20)

Radiometals for Combined Imaging and Therapy Cutler, Cathy S.; Hennkens, Heather M.; Sisay, Nebiat Chemical Reviews, Vol. 113, Issue 2, p. 858-883 https://doi.org/10.1021/cr3003104	journal	October 2012
Metallic radionuclides in the development of diagnostic and therapeutic radiopharmaceuticals Bhattacharyya, Sibaprasad; Dixit, Manish Dalton Transactions, Vol. 40, Issue 23 https://doi.org/10.1039/c1dt10379b	journal	January 2011
Generator-based PET radiopharmaceuticals for molecular imaging of tumours: on the way to THERANOSTICS Rösch, Frank; Baum, Richard P. Dalton Transactions, Vol. 40, Issue 23 https://doi.org/10.1039/c0dt01504k	journal	January 2011
Chemical and Radiochemical Considerations in Radiolabeling with α-Emitting Radionuclides Scott Wilbur, D. Current Radiopharmaceuticalse, Vol. 4, Issue 3 https://doi.org/10.2174/1874471011104030214	journal	July 2011
Bismuth-213 and Actinium-225 – Generator Performance and Evolving Therapeutic Applications of Two Generator-Derived Alpha-Emitting Radioisotopes Morgenstern, Alfred; Bruchertseifer, Frank; Apostolidis, Christos Current Radiopharmaceuticals, Vol. 5, Issue 3 https://doi.org/10.2174/1874471011205030221	journal	June 2012
Actinium-225 in Targeted Alpha-Particle Therapeutic Applications A. Scheinberg, David; R. McDevitt, Michael Current Radiopharmaceuticalse, Vol. 4, Issue 4 https://doi.org/10.2174/1874471011104040306	journal	October 2011
Production of actinium-225 for alpha particle mediated radioimmunotherapy Boll, Rose A.; Malkemus, Dairin; Mirzadeh, Saed Applied Radiation and Isotopes, Vol. 62, Issue 5 https://doi.org/10.1016/j.apradiso.2004.12.003	journal	May 2005
Production of ²²⁵Ac and ²²³Ra by irradiation of Th with accelerated protons Zhuikov, B. L.; Kalmykov, S. N.; Ermolaev, S. V. Radiochemistry, Vol. 53, Issue 1, p. 73-80 https://doi.org/10.1134/S1066362211010103	journal	February 2011
Cross sections from proton irradiation of thorium at 800 MeV Engle, Jonathan W.; Mashnik, Stepan G.; Weidner, John W. Physical Review C, Vol. 88, Issue 1 https://doi.org/10.1103/PhysRevC.88.014604	journal	July 2013
225Ac and 223Ra production via 800MeV proton irradiation of natural thorium targets Weidner, J. W.; Mashnik, S. G.; John, K. D. Applied Radiation and Isotopes, Vol. 70, Issue 11 https://doi.org/10.1016/j.apradiso.2012.07.003	journal	November 2012
Isolation of Medicine-Applicable Actinium-225 from Thorium Targets Irradiated by Medium-Energy Protons Aliev, R. A.; Ermolaev, S. V.; Vasiliev, A. N. Solvent Extraction and Ion Exchange, Vol. 32, Issue 5 https://doi.org/10.1080/07366299.2014.896582	journal	June 2014
Carrier-free separation of228Ac from aged thorium nitrate Sani, A. R. Journal of Radioanalytical Chemistry, Vol. 4, Issue 1 https://doi.org/10.1007/BF02513645	journal	January 1970
The Preparation of Carrier-Free Radium-228 Using Cation Exchange Columns Paige, C. R.; Kornicker, W. A.; Hileman, O. E. International Journal of Environmental Analytical Chemistry, Vol. 37, Issue 1 https://doi.org/10.1080/03067318908026882	journal	September 1989
Isolation of radionuclides from thorium targets irradiated with 300-MeV protons Filosofov, D. V.; Rakhimov, A. V.; Bozhikov, G. A. Radiochemistry, Vol. 55, Issue 4 https://doi.org/10.1134/S1066362213040127	journal	July 2013
Generator of actinium-225 Tsoupko-Sitnikov, V.; Norseev, Yu.; Khalkin, V. Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 205, Issue 1 https://doi.org/10.1007/BF02040552	journal	April 1996
Ion Exchange Method for the Separation of MsTh ₁ (Ra ²²⁸ ) MsTh ₂ (Ac ²²⁸ ) ThB(Pb ²¹² ) and ThC(Bi ²¹² ) from thorium nitrate Chen, Ying-Mao; Wong, Chiu-Ming Journal of the Chinese Chemical Society, Vol. 6, Issue 1 https://doi.org/10.1002/jccs.195900006	journal	September 1959
Ac, La, and Ce radioimpurities in 225Ac produced in 40–200 MeV proton irradiations of thorium Engle, Jonathan W.; Weidner, John W.; Ballard, Beau D. Radiochimica Acta, Vol. 102, Issue 7 https://doi.org/10.1515/ract-2013-2179	journal	January 2014
Selenium-72 formation via natBr(p,x) induced by 100MeV Protons: Steps towards a novel 72Se/72As generator system Ballard, B.; Wycoff, D.; Birnbaum, E. R. Applied Radiation and Isotopes, Vol. 70, Issue 4 https://doi.org/10.1016/j.apradiso.2012.01.018	journal	April 2012
An Improved Method for the Production of Ac‐225/Bi‐213 from Th‐229 for Targeted Alpha Therapy Zielinska, B.; Apostolidis, C.; Bruchertseifer, F. Solvent Extraction and Ion Exchange, Vol. 25, Issue 3 https://doi.org/10.1080/07366290701285108	journal	April 2007
Distribution coefficients of 60 elements on TODGA resin: Application to Ca, Lu, Hf, U and Th isotope geochemistry Pourmand, Ali; Dauphas, Nicolas Talanta, Vol. 81, Issue 3 https://doi.org/10.1016/j.talanta.2010.01.008	journal	May 2010

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Synthesis and Characterization of the Actinium Aquo Ion Ferrier, Maryline G.; Stein, Benjamin W.; Batista, Enrique R. ACS Central Science, Vol. 3, Issue 3 https://doi.org/10.1021/acscentsci.6b00356	journal	February 2017
Spectroscopic and computational investigation of actinium coordination chemistry Ferrier, Maryline G.; Batista, Enrique R.; Berg, John M. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12312	journal	August 2016
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Title: Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes

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