Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform

Anion exchange to hydroxamate resin columns

Matthew J. O'Hara, Nathaniel J. Murray, Jennifer C. Carter, Cynthia M. Kellogg, Jeanne Link

Research output: Contribution to journalArticle

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 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. 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.

Original languageEnglish (US)
Pages (from-to)37-46
Number of pages10
JournalJournal of Chromatography A
Volume1567
DOIs
StatePublished - Sep 14 2018

Fingerprint

Cyclotrons
Yttrium
Oxalates
Distillation columns
Fluidics
Anions
divinyl benzene
Resins
Metal foil
Purification
Anion Exchange Resins
Styrene
Deferoxamine
Titration
Radioisotopes
Effluents
Polymers
Salts
Metals
Recovery

Keywords

  • Zr
  • Anion exchange
  • Deferoxamine
  • Hydroxamate
  • Laboratory automation
  • Medical isotope
  • PET imaging

ASJC Scopus subject areas

  • Analytical Chemistry
  • Biochemistry
  • Organic Chemistry

Cite this

Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform : Anion exchange to hydroxamate resin columns. / O'Hara, Matthew J.; Murray, Nathaniel J.; Carter, Jennifer C.; Kellogg, Cynthia M.; Link, Jeanne.

In: Journal of Chromatography A, Vol. 1567, 14.09.2018, p. 37-46.

Research output: Contribution to journalArticle

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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 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. 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.",
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N2 - 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. 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.

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KW - Zr

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KW - Deferoxamine

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KW - Laboratory automation

KW - Medical isotope

KW - PET imaging

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