title: Production of 89Zr via the 89Y(p,n)89Zr reaction in aqueous solution: effect of solution composition on in-target chemistry.
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.
  
  
  METHODS
  We have developed a simplified, solution target approach for production of (89)Zr using a niobium target by 14 MeV energy proton bombardment of aqueous solutions of yttrium salts via the (89)Y(p,n)(89)Zr 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, (89)Zr was produced in moderate yield (4.36 ± 0.48 MBq/μA • h) and high effective specific activity (464 ± 215 MBq/μg) using the solution target approach (2.75 M yttrium nitrate, 1.5 N HNO3, 2h irradiation at 20 μA).
  
  
  CONCLUSIONS
  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 (64)Cu, (68)Ga and (86)Y, and is well suited for short-lived isotopes.
authors.affiliation: Department of Radiology, Mayo Clinic Rochester MN 55905; Brigham and Women's Hospital, Harvard Medical School Boston MA 02115. Electronic address: pandey.mukesh@mayo.edu.
authors.forename: Mukesh K
authors.initials: MK
authors.lastname: Pandey
authors.affiliation: Department of Radiology, Mayo Clinic Rochester MN 55905.
authors.forename: Hendrik P
authors.initials: HP
authors.lastname: Engelbrecht
authors.affiliation: Brigham and Women's Hospital, Harvard Medical School Boston MA 02115.
authors.forename: John P
authors.initials: JP
authors.lastname: Byrne
authors.affiliation: Boston Children's Hospital, Harvard Medical School Boston MA 02115.
authors.forename: Alan B
authors.initials: AB
authors.lastname: Packard
authors.affiliation: Department of Radiology, Mayo Clinic Rochester MN 55905; Brigham and Women's Hospital, Harvard Medical School Boston MA 02115. Electronic address: degrado.timothy@mayo.edu.
authors.forename: Timothy R
authors.initials: TR
authors.lastname: DeGrado
mesh_terms: D017357:Cyclotrons; D017942:Nitric Acid / Q000737:chemistry; D011522:Protons; D011854:Radiochemistry / Q000295:instrumentation / Q000379:methods*; D011868:Radioisotopes / Q000737:chemistry*; D012996:Solutions; D014867:Water / Q000737:chemistry*; D015019:Yttrium / Q000737:chemistry*; D015040:Zirconium / Q000737:chemistry*
chemical_list: D011522:Protons; D011868:Radioisotopes; D012996:Solutions; D014867:Water; D017942:Nitric Acid; D015019:Yttrium; D015040:Zirconium
keywords: (89)Zr; Cyclotron targetry; Solution target