Aguila Briana, Sun Qi, Cassady Harper, Abney Carter W, Li Baiyan, Ma Shengqian
Department of Chemistry , University of South Florida , 4202 E Fowler Avenue , Tampa , Florida 33620 , United States.
ExxonMobil Research and Engineering Company , 1545 Route 22 East , Annandale , New Jersey 08801 , United States.
ACS Appl Mater Interfaces. 2019 Aug 28;11(34):30919-30926. doi: 10.1021/acsami.9b09532. Epub 2019 Aug 16.
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-the-art 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-CHNHAO and PAF-1-NH(CH)AO, with varying chain lengths and grafting degrees, were investigated for their uranium uptakes and kinetic efficiency. PAF-1-NH(CH)AO was found to outperform PAF-1-CHNHAO, 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(CH)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.
为了将核能作为主要能源,必须确保铀资源的供应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,人们已对吸附材料进行研究以回收这种重要的燃料来源。已发现偕胺肟(AO)是用于此目的的最先进官能团,然而,仍需改进以克服在海洋中如此低浓度下选择性捕获铀的问题。在此,我们报告PAF-1作为研究两种偕胺肟配体效果的平台。对合成的具有不同链长和接枝度的吸附剂PAF-1-CHNHAO和PAF-1-NH(CH)AO的铀吸附量和动力学效率进行了研究。发现PAF-1-NH(CH)AO的性能优于PAF-1-CHNHAO,其最大吸附容量为385 mg/g,并且能够在10分钟内将加标铀溶液降低到ppb水平。对PAF-1-NH(CH)AO的进一步研究表明,它在多次吸附循环中具有有效的洗脱能力,并且在加标海水溶液的不同组成中回收铀方面显示出有希望的结果。本文所展示的工作推进了偕胺肟官能化配体的设计原则,并为增强作为可持续核燃料源的铀捕获策略提供了空间。