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采用自动化流体制备平台从回旋加速器辐照的钇靶中串联柱分离 89Zr:阴离子交换到羟肟酸树脂柱。

Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform: Anion exchange to hydroxamate resin columns.

机构信息

Nuclear Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd., PO Box 999, Richland, WA 99352, United States.

Nuclear Sciences Division, Pacific Northwest National Laboratory, 902 Battelle Blvd., PO Box 999, Richland, WA 99352, United States.

出版信息

J Chromatogr A. 2018 Sep 14;1567:37-46. doi: 10.1016/j.chroma.2018.06.035. Epub 2018 Jul 24.

Abstract

The development of a tandem column purification method for the preparation of high-purity Zr(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 Zr eluent solution for the primary column is equivalent to the Zr load solution for the secondary column. The ability to transfer Zr from one column to the next allows two sequential column clean-up methods to be performed prior to the final elution of the Zr(IV) oxalate. This approach assures delivery of high purity Zr product and assures a Zr 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 Zr present in the foils was recovered in the secondary column elution fraction. Furthermore, elution peak analysis of several Zr elution profile radiochromatograms made possible the determination of Zr recovery as a function of volume; a Zr 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 Zr 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 Zr product elution volume, titrations of the Zr product with deferoxamine mesylate salt across two preparatory methods resulted in mean effective specific activity (ESA) values of 279 and 340 T Bq·mmole and mean bindable metals concentrations ([M]) of 13.5 and 16.7 nmole·g. These ESA and [M] values infer that the Zr(IV) oxalate product resulting from this tandem column isolation method has the highest purity reported to date.

摘要

本文介绍了一种串联柱纯化方法,用于制备高纯度 Zr(IV)草酸盐。第一根柱子是一种大孔强碱性阴离子交换树脂,由苯乙烯-二乙烯基苯共聚体制成。第二根柱子的内体积为 33μL,填充有羟肟酸树脂。开发了一种倒置选择性条件,其中第一根柱子的 Zr 洗脱液相当于第二根柱子的 Zr 负载溶液。将 Zr 从一根柱子转移到另一根柱子的能力允许在最后洗脱 Zr(IV)草酸盐之前进行两次连续的柱清洗方法。这种方法保证了高纯度 Zr 产品的交付,并保证了比传统使用单一羟肟酸树脂柱方法洗脱的 Zr 产品更小的洗脱体积。串联柱纯化过程已被引入到原型自动化流体系统中。该系统配置有在线伽马检测,因此可以实时监测柱流出物。自动化方法已通过 7 个回旋加速器轰炸的 Y 箔靶进行了测试。结果发现,箔片中 95.1±1.3%的 Zr 被回收在第二根柱子的洗脱部分。此外,对几个 Zr 洗脱轮廓放射性色谱图的洗脱峰分析,使得可以确定 Zr 回收率作为体积的函数;在 0.29±0.06mL 中可以获得包含 90%第二根柱子洗脱峰的 Zr 产物体积(代表靶中 86±5%的 Zr 活性)(代表靶中 86±5%的 Zr 活性)。与该领域中使用的主要方法相比,该产物体积代表放射性核素产物浓度的显著提高。除了减少 Zr 产物洗脱体积外,用甲磺酸去铁胺盐对两种制备方法的 Zr 产物进行滴定,得到平均有效比活度(ESA)值分别为 279 和 340 TBq·mmole 和平均结合金属浓度([M])分别为 13.5 和 16.7nmole·g。这些 ESA 和[M]值推断,该串联柱分离方法得到的 Zr(IV)草酸盐产物具有迄今为止报道的最高纯度。

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