Production of 89Zr via the 89Y(p,n)89Zr reaction in aqueous solution: Effect of solution composition on in-target chemistry

Mukesh K. Pandey, Hendrik P. Engelbrecht, John P. Byrne, Alan B. Packard, Timothy R. DeGrado

Research output: Contribution to journalArticle

27 Scopus citations

Abstract

Objective: The existing solid target production method of radiometals requires high capital and operational expenditures, which limit the production of radiometals to the small fraction of cyclotron facilities that are equipped with solid target systems. Our objective is to develop a robust solution target method, which can be applicable to a wide array of radiometals and would be simply and easily adopted by existing cyclotron facility for the routine production of radiometals. Method: We have developed a simplified, solution target approach for production of 89Zr using a niobium target by 14 MeV energy proton bombardment of aqueous solutions of yttrium salts via the 89Y(p,n)89Zr nuclear reaction. The production conditions were optimized, following a detailed mechanistic study of the gas evolution. Results: Although the solution target approach avoided the expense and complication of solid target processing, rapid radiolytic formation of gases in the target represents a major impediment in the success of solution target. To address this challenge we performed a systematic mechanistic study of gas evolution. Gas evolution was found to be predominantly due to decomposition of water to molecular hydrogen and oxygen. The rate of gas evolutions varied >40-fold depending on solution composition even under the same irradiation condition. With chloride salts, the rate of gas evolution increased in the order rank Na<Ca<Y. However, the trend was reversed with the corresponding nitrate salts, and further addition of nitric acid to the irradiating solution minimized gas evolution. At optimized condition, 89Zr was produced in moderate yield (4.36±0.48 MBq/μAh) and high effective specific activity (464±215 MBq/μg) using the solution target approach (2.75M yttrium nitrate, 1.5N HNO3, 2h irradiation at 20μA). Conclusion: The novel findings on substrate dependent, radiation-induced water decomposition provide fundamental data for the development and optimization of conditions for solution targets. The developed methodology of irradiation of nitrate salts in dilute nitric acid solutions can be translated to the production of a wide array of radiometals like 64Cu, 68Ga and 86Y, and is well suited for short-lived isotopes.

Original languageEnglish (US)
Pages (from-to)309-316
Number of pages8
JournalNuclear Medicine and Biology
Volume41
Issue number4
DOIs
StatePublished - Apr 2014

Keywords

  • Cyclotron targetry
  • Solution target

ASJC Scopus subject areas

  • Molecular Medicine
  • Radiology Nuclear Medicine and imaging
  • Cancer Research

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