羟肟酸盐基树脂分离纯化89Zr

    Purification of 89Zr by Hydroxamate-Based Resins

    • 摘要: 回旋加速器轰击89Y固体靶制备89Zr过程中,靶件存在Fe、Al、Zn、Mg等微量金属杂质元素及大量未反应的89Y,需要进行分离纯化才能应用于89Zr放射性药物的制备。本工作研究了羟肟酸盐基树脂在HCl溶液中对Zr4+、Y3+、Fe3+、Al3+、Mg2+、Zn2+等金属元素的吸附性能及Zr4+的洗脱条件。结果表明:羟肟酸盐基树脂在HCl中不吸附Y3+、Al3+、Zn2+、Mg2+;在2.0~4.0 mol/L的HCl溶液中,对Fe3+吸附效果较差;在2.0~6.0 mol/L HCl溶液中对于Zr4+吸附效果较好;在0.05 mol/L以上的草酸溶液中几乎不吸附Zr4+;采用羟肟酸盐基树脂柱,建立了在回旋加速器轰击后Y靶片中分离纯化89Zr高效快速的方法,即在含有Zr4+、Y3+、Fe3+ 、Al3+、Zn2+、Mg2+等元素的溶液通过羟肟酸盐基树脂柱后,依次使用2.0 mol/L HCl和去离子水过羟肟酸盐基树脂柱,最后用0.50 mol/L草酸洗脱吸附在树脂柱上的Zr4+,得到纯化后的草酸锆溶液。稳定核素和89Zr示踪的研究表明,采用羟肟酸盐基树脂纯化89ZrCl4溶液的工艺可行,羟肟酸盐基树脂可用于89ZrCl4溶液中Mg2+、Fe3+ 、Y3+、Zn2+等元素的去除。

       

      Abstract: In the preparation of 89Zr using a cyclotron to bombard a 89Y solid target, trace metal impurities such as Fe, Al, Zn, and Mg, along with unreacted 89Y, are present. Separation and purification are necessary for application in 89Zr-labeled radiopharmaceuticals. This study conducted the following work: the static distribution coefficients of Zr4+, Y3+, Fe3+, Mg2+, Zn2+ and Al3+ on hydroxamate-based resin were measured in hydrochloric acid and oxalic acid systems. The dynamic adsorption rates of these metal ions on the resin column were measured in hydrochloric acid. The breakthrough curves of Zr4+ in the hydroxamate-based resin were determined in hydrochloric acid. The elution of Zr4+ and Fe3+ from the resin using oxalic acid as an eluent was measured. The purification process conditions were validated using ZrCl4 simulated solution and trace amounts of 89Zr4+. The hydroxamate-based resin does not adsorb Y3+, Al3+, Zn2+, or Mg2+ in HCl. In 2.0 mol/L to 4.0 mol/L HCl solution, the adsorption of Fe3+ is poor, while the adsorption of Zr4+ is good in 2.0 mol/L to 6.0 mol/L HCl solution. The hydroxamate-based resin hardly adsorbs Zr4+ in oxalic acid solutions above 0.05 mol/L, and its adsorption capacity for Fe3+ first increases and then decreases with higher oxalic acid concentrations, reaching the strongest capacity at 0.5 mol/L. Zr4+ is adsorbed by the hydroxamate-based resin column in 2.0 mol/L to 6.0 mol/L HCl solution, with an adsorption rate exceeding 95%. As the HCl concentration increases to 8.0 mol/L, the adsorption rate drops to 61.42%. Y3+, Al3+, and Mg2+ are hardly adsorbed in 2.0 mol/L to 8.0 mol/L HCl. Fe3+ shows negligible adsorption in 2.0 mol/L to 4.0 mol/L HCl, but the adsorption rate increases to 15.69% at 8.0 mol/L HCl. Using 200 mg of hydroxamate-based resin meets the adsorption capacity requirements for Zr4+ in the purification of 89ZrCl4 solution. During Zr purification, a 0.10 mol/L to 1.00 mol/L oxalic acid solution can be chosen for elution, but it is difficult to wash off Fe with this solution. 89Zr mainly concentrates in the elution volume of 400 μL to 1200 μL, with a total recovery rate exceeding 85%. Y3+, Al3+, Zn2+, and Fe3+ remain in the adsorption effluent and washing solution, with no impurities adsorbed on the resin column. Zr is almost completely adsorbed on the resin column, and the elution liquid can effectively wash out Zr, with no overlap between Zr elution peaks and impurity peaks. Using hydroxamate-based resin columns, an efficient and rapid method is established for separating and purifying 89Zr from Y targets after cyclotron bombardment. Solutions containing Zr4+, Y3+, Fe3+, Al3+, Zn2+, and Mg2+ pass through the hydroxamate-based resin columns. Then, 2.0 mol/L HCl and deionized water are used sequentially to wash the columns, and finally, Zr4+ adsorbed on the resin is eluted with 0.50 mol/L oxalic acid, resulting in a purified oxalic zirconium solution. Studies with stable isotopes and 89Zr tracers indicate that the process for purifying 89ZrCl4 solution using hydroxamate-based resin is feasible, and the resin effectively removes Mg2+, Fe3+, Y3+, Al3+, and Zn2+ from the 89ZrCl4 solution.

       

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