Design Strategies to Enhance Amidoxime Chelators for Uranium Recovery

Design Strategies to Enhance Amidoxime Chelators for Uranium Recovery
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DOI:
10.1021/acsami.9b09532
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发表时间:
2019-08-28
影响因子:
9.5
通讯作者:
Mai, Shengqian
Mai, Shengqian
中科院分区:
材料科学2区
文献类型:
--
作者:
Aguila, Briana;Sun, Qi;Mai, Shengqian

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为了将核能作为主要能源,铀资源的保障必须超出陆地储量所能提供的范围。鉴于海洋中天然存在大量铀,人们对吸附材料进行了研究,以回收这种重要的燃料来源。偕胺肟 (AO) 已被发现是用于此目的的最先进的官能团,但是,仍然必须进行改进以克服选择性捕获海洋中如此低浓度的铀的问题。在此,我们报告 PAF-1 作为研究两种偕胺肟配体作用的平台。研究了不同链长和接枝度的合成吸附剂PAF-1-CH(2)NHAO和PAF-1-NH(CH2)(2)AO的铀吸收和动力学效率。研究发现 PAF-1-NH(CH2)(2)AO 的性能优于 PAF-1-CH(2)NHAO,最大吸收能力为 385 mg/g,能够在 10 分钟内将加铀溶液降低至 ppb 水平。 PAF-1-NH(CH2)(2)AO 的进一步研究证明了多个吸附循环的有效洗脱,并显示了在不同成分的加标海水溶液中铀回收的有希望的结果。这里介绍的工作推进了偕胺肟功能化配体的设计原则,并为加强捕获铀作为可持续核燃料源的策略提供了空间。
To move nuclear as a primary energy source, uranium resources must be secured beyond what terrestrial reserves can provide. Given the vast quantity of uranium naturally found in the ocean, adsorbent materials have been investigated to recover this vital fuel source. Amidoxime (AO) has been found to be the state-of-theart functional group for this purpose, however, improvements must still be made to overcome the issues with selectively capturing uranium at such a low concentration found in the ocean. Herein, we report PAF-1 as a platform to study the effects of two amidoxime ligands. The synthesized adsorbents, PAF-1-CH(2)NHAO and PAF-1-NH(CH2)(2)AO, with varying chain lengths and grafting degrees, were investigated for their uranium uptakes and kinetic efficiency. PAF-1-NH(CH2)(2)AO was found to outperform PAF-1-CH(2)NHAO, with a maximum uptake capacity of 385 mg/g and able to reduce a uranium-spiked solution to ppb level within 10 min. Further studies with PAF-1-NH(CH2)(2)AO demonstrated effective elution for multiple adsorption cycles and showed promising results for uranium recovery in the diverse composition of a spiked seawater solution. The work presented here moves forward design principles for amidoxime-functionalized ligands and provides scope for strategies to enhance the capture of uranium as a sustainable nuclear fuel source.