Characterizing Extraction Chromatography for Large-Scale Americium-241 Processing,Industrial & Engineering Chemistry Research

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Characterizing Extraction Chromatography for Large-Scale Americium-241 Processing
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2021-09-27 , DOI: 10.1021/acs.iecr.1c02360
Brian T. Arko _{1,

2} , David Dan ₁ , Sara L. Adelman ₁ , Daniel L. Huber ₁ , David B. Kimball ₁ , Stosh A. Kozimor ₁ , Mila Nhu Lam ₁ , Veronika Mocko ₁ , Jenifer C. Shafer ₂ , Benjamin W. Stein ₁ , Sara L. Thiemann ₁

Affiliation

The americium-241 (²⁴¹Am) radioisotope has valuable nuclear properties that find broad industrial usage. Ensuring stable supplies of ²⁴¹Am is critical for supporting (and expanding) the existing ²⁴¹Am-application space and enabling emerging ²⁴¹Am-technologies that are important for economic growth, energy, and national security. Unfortunately, the United States halted ²⁴¹Am production in 1984 and the existing inventory was depleted in the early 2000s. This situation recently changed when the U.S. Department of Energy Isotope Program established ²⁴¹Am recovery at Los Alamos National Laboratory. Today, large-scale quantities of ²⁴¹Am are now obtained using the Chloride Extraction and Actinide Recovery (CLEAR) process. This method uses a resin that has the di-(4-t-butylphenyl)-N,N-di-iso-butylcarbamoylmethylphosphine oxide (m-CMPO) extractant adsorbed on a resin bead to harvest ²⁴¹Am from plutonium-containing waste streams. To maintain and improve CLEAR processing of ²⁴¹Am, we have evaluated the extraction of ²⁴¹Am by m-CMPO as a function of three important processing relevant variables: (1) HCl concentration, (2) metal contaminant concentration, and (3) contact time. The performance of the m-CMPO resin was additionally compared against commercially available resins, namely, rare earth (RE) resin and a selected series of diglycolamide (DGA) resins. Our results suggested that the m-CMPO resin outperformed most of the commercially available alternatives. However, tetraoctyl-DGA (TODGA) and tetraethyl-hexyl-DGA (TEHDGA) prevailed on several fronts. The TODGA and TEHDGA resins quantitatively released ²⁴¹Am at low HCl concentrations (<0.5 M), were less susceptible to deleterious side effects from metal contaminants in the mobile phase and bound ²⁴¹Am faster. Based on these results, we concluded that ²⁴¹Am recovery yields have the potential to improve if TODGA or TEHDGA is used in place of m-CMPO for large-scale CLEAR processing of ²⁴¹Am.

中文翻译：

表征用于大规模 Americ-241 处理的萃取色谱

镅 241 ( ²⁴¹ Am) 放射性同位素具有宝贵的核特性，可在工业上广泛使用。确保²⁴¹ Am 的稳定供应对于支持（和扩展）现有的²⁴¹ Am 应用空间以及启用对经济增长、能源和国家安全至关重要的新兴²⁴¹ Am 技术至关重要。不幸的是，美国在 1984 年停止了²⁴¹ Am 的生产，现有库存在 2000 年代初耗尽。当美国能源部同位素计划在洛斯阿拉莫斯国家实验室建立²⁴¹ Am 恢复时，这种情况最近发生了变化。如今，^{241 件的}大批量Am 现在使用氯化物萃取和锕系元素回收 (CLEAR) 工艺获得。该方法使用具有吸附在树脂珠上的二-(4-叔丁基苯基) -N , N-二异丁基氨基甲酰基甲基氧化膦 ( m - CMPO) 萃取剂的树脂，以从含钚的废物流中收集²⁴¹ Am。为了维持和改进²⁴¹ Am 的CLEAR 处理，我们评估了m- CMPO对²⁴¹ Am的提取作为三个重要处理相关变量的函数：( 1 ) HCl 浓度，( 2 ) 金属污染物浓度，和 ( 3)) 联系时间。此外，还将m- CMPO 树脂的性能与市售树脂，即稀土 (RE) 树脂和选定系列的二甘醇酰胺 (DGA) 树脂进行了比较。我们的结果表明，m- CMPO 树脂的性能优于大多数市售替代品。然而，四辛基-DGA (TODGA) 和四乙基-己基-DGA (TEHDGA) 在几个方面占了上风。TODGA 和 TEHDGA 树脂在低 HCl 浓度 (<0.5 M) 下定量释放²⁴¹ Am，不易受到流动相中金属污染物的有害副作用的影响，并且结合²⁴¹ Am 的速度更快。基于这些结果，我们得出结论，²⁴¹如果使用 TODGA 或 TEHDGA 代替m -CMPO 进行²⁴¹ Am的大规模 CLEAR 处理，Am 回收率有可能提高。

更新日期：2021-10-06

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