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Title: Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform: Anion exchange to hydroxamate resin columns

Abstract

The development of a tandem column purification method for the preparation of high-purity 89Zr(IV) oxalate is presented. The primary column was a macroporous strongly basic anion exchange resin on styrene divinylbenzene co-polymer. The secondary column, with an internal volume of 33 μL, was packed with hydroxamate resin. A condition of inverted selectivity was developed, whereby the 89Zr eluent solution for the primary column is equivalent to the 89Zr load solution for the secondary column. The ability to transfer 89Zr from one column to the next allows two sequential column clean-up methods to be performed prior to the final elution of the 89Zr(IV) oxalate. This approach assures delivery of high purity 89Zr product and assures a 89Zr product that is eluted in a substantially smaller volume than is possible when using the traditionally-employed single hydroxamate resin column method. The tandem column purification process has been implemented into a prototype automated fluidic system. The system is configured with on-line gamma detection so column effluents can be monitored in near-real time. The automated method was tested using seven cyclotron bombarded Y foil targets. It was found that 95.1 ± 1.3% of the 89Zr present in the foils was recovered in the secondary columnmore » elution fraction. Furthermore, elution peak analysis of several 89Zr elution profile radiochromatograms made possible the determination of 89Zr recovery as a function of volume; a 89Zr product volume that contains 90% of the mean secondary column elution peak can be obtained in 0.29 ± 0.06 mL (representing 86 ± 5% of the 89Zr activity in the target). This product volume represents a significant improvement in radionuclide product concentration over the predominant method used in the field. In addition to the reduced 89Zr product elution volume, titrations of the 89Zr product with deferoxamine mesylate salt across two preparatory methods resulted in mean effective specific activity (ESA) values of 279 and 340 T Bq·mmole-1 and mean bindable metals concentrations ([MB]) of 13.5 and 16.7 nmole·g-1. In conclusion, these ESA and [MB] values infer that the 89Zr(IV) oxalate product resulting from this tandem column isolation method has the highest purity reported to date.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [2]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Nuclear Sciences Division
  2. Oregon Health & Science Univ., Portland, OR (United States). Center for Radiochemistry Research, Department of Diagnostic Radiology
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1463331
Alternate Identifier(s):
OSTI ID: 1702371
Report Number(s):
PNNL-SA-134266
Journal ID: ISSN 0021-9673; PII: S002196731830791X
Grant/Contract Number:  
S10-RR017229; AC0576RL01830; AC06-67RLO 1830
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chromatography
Additional Journal Information:
Journal Volume: 1567; Journal Issue: C; Journal ID: ISSN 0021-9673
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 89Zr; PET imaging; Medical isotope; Laboratory automation; Hydroxamate; Anion exchange; Deferoxamine

Citation Formats

O?Hara, Matthew J., Murray, Nathaniel J., Carter, Jennifer C., Kellogg, Cynthia M., and Link, Jeanne M.. Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform: Anion exchange to hydroxamate resin columns. United States: N. p., 2018. Web. https://doi.org/10.1016/J.CHROMA.2018.06.035.
O?Hara, Matthew J., Murray, Nathaniel J., Carter, Jennifer C., Kellogg, Cynthia M., & Link, Jeanne M.. Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform: Anion exchange to hydroxamate resin columns. United States. https://doi.org/10.1016/J.CHROMA.2018.06.035
O?Hara, Matthew J., Murray, Nathaniel J., Carter, Jennifer C., Kellogg, Cynthia M., and Link, Jeanne M.. Tue . "Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform: Anion exchange to hydroxamate resin columns". United States. https://doi.org/10.1016/J.CHROMA.2018.06.035. https://www.osti.gov/servlets/purl/1463331.
@article{osti_1463331,
title = {Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform: Anion exchange to hydroxamate resin columns},
author = {O?Hara, Matthew J. and Murray, Nathaniel J. and Carter, Jennifer C. and Kellogg, Cynthia M. and Link, Jeanne M.},
abstractNote = {The development of a tandem column purification method for the preparation of high-purity 89Zr(IV) oxalate is presented. The primary column was a macroporous strongly basic anion exchange resin on styrene divinylbenzene co-polymer. The secondary column, with an internal volume of 33 μL, was packed with hydroxamate resin. A condition of inverted selectivity was developed, whereby the 89Zr eluent solution for the primary column is equivalent to the 89Zr load solution for the secondary column. The ability to transfer 89Zr from one column to the next allows two sequential column clean-up methods to be performed prior to the final elution of the 89Zr(IV) oxalate. This approach assures delivery of high purity 89Zr product and assures a 89Zr product that is eluted in a substantially smaller volume than is possible when using the traditionally-employed single hydroxamate resin column method. The tandem column purification process has been implemented into a prototype automated fluidic system. The system is configured with on-line gamma detection so column effluents can be monitored in near-real time. The automated method was tested using seven cyclotron bombarded Y foil targets. It was found that 95.1 ± 1.3% of the 89Zr present in the foils was recovered in the secondary column elution fraction. Furthermore, elution peak analysis of several 89Zr elution profile radiochromatograms made possible the determination of 89Zr recovery as a function of volume; a 89Zr product volume that contains 90% of the mean secondary column elution peak can be obtained in 0.29 ± 0.06 mL (representing 86 ± 5% of the 89Zr activity in the target). This product volume represents a significant improvement in radionuclide product concentration over the predominant method used in the field. In addition to the reduced 89Zr product elution volume, titrations of the 89Zr product with deferoxamine mesylate salt across two preparatory methods resulted in mean effective specific activity (ESA) values of 279 and 340 T Bq·mmole-1 and mean bindable metals concentrations ([MB]) of 13.5 and 16.7 nmole·g-1. In conclusion, these ESA and [MB] values infer that the 89Zr(IV) oxalate product resulting from this tandem column isolation method has the highest purity reported to date.},
doi = {10.1016/J.CHROMA.2018.06.035},
journal = {Journal of Chromatography},
number = C,
volume = 1567,
place = {United States},
year = {2018},
month = {7}
}

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    journal, December 2019

    • O’Hara, Matthew J.; Krzysko, Anthony J.; Hamlin, Donald K.
    • Scientific Reports, Vol. 9, Issue 1
    • DOI: 10.1038/s41598-019-56272-7