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Evaluation of a chloride-based 89 Zr isolation strategy using a tributyl phosphate (TBP)-functionalized extraction resin.

INTRODUCTION: The remarkable stability of the 89 Zr-DOTA complex has been shown in recent literature. The formation of this complex appears to require 89 Zr-chloride as the complexation precursor rather than the more conventional 89 Zr-oxalate. In this work we present a method for the direct isolation of 89 Zr-chloride from irradiated nat Y foils.

METHODS: 89 Zr, 88 Zr, and 88 Y were prepared by 16 MeV proton irradiation of nat Y foils and used for batch-extraction based equilibrium coefficient measurements for TBP and UTEVA resin. Radionuclidically pure 89 Zr was prepared by 14 MeV proton-irradiation of nat Y foils. These foils were dissolved in concentrated HCl, trapped on columns of TBP or UTEVA resin, and 89 Zr-chloride was eluted in <1 mL of 0.1 M HCl. For purposes of comparison, conventionally-isolated 89 Zr-oxalate was converted to 89 Zr-chloride by trapping, rinsing, and elution from a QMA cartridge into 1 M HCl. Trace metal analysis was performed on the resulting 89 Zr products.

RESULTS: Equilibrium coefficients for Y and Zr were similar between UTEVA and TBP resins across all HCl concentrations. Kd values of <10-1  mL/g were observed for Y across all HCl concentrations. Kd values of >103  mL/g were observed at HCl concentrations >9 M for Zr, falling to Kd values of <100  mL/g at low HCl concentrations. 89 Zr-chloride was recovered from small columns of TBP in <1 mL of 0.1 M HCl with an overall recovery efficiency of 89 ± 3% (n = 3). An average Y/Zr separation factor of 1.5 × 105 (n = 3) was obtained. Trace metal impurities, notably Fe, were higher in TBP-isolated 89 Zr-chloride compared with 89 Zr-chloride prepared using the conventional two-step procedure.

CONCLUSION: TBP-functionalized resin appears promising for the direct isolation of 89 Zr-chloride from irradiated nat Y targets. Excellent 89 Zr recovery efficiencies were obtained, and chemical purity was sufficient for proof-of-concept chelation studies.

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