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 ([M_B]) of 13.5 and 16.7 nmole·g^-1. In conclusion, these ESA and [M_B] values infer that the ⁸⁹Zr(IV) oxalate product resulting from this tandem column isolation method has the highest purity reported to date.« less

Authors:

O?Hara, Matthew J.  ^[1];

• Search DOE PAGES for author "O?Hara, Matthew J."
• Search DOE PAGES for ORCID "0000-0003-3982-5897"
• Search orcid.org for ORCID "0000-0003-3982-5897"

Murray, Nathaniel J. ^[1]; Carter, Jennifer C. ^[1]; Kellogg, Cynthia M. ^[1]; Link, Jeanne M. ^[2]

---

+ Show Author Affiliations

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:

2018-07-24

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