基组功能化二胺作为在恶劣条件下Am(III) /Eu(III) 分离的高效掩饰剂
Yaoyang Liu1, Yu Kang2, Mingjie Bao2
1Institute of Nuclear and New Energy Technology, Tsinghua University, Haidian District, Beijing 100084, China.
Journal of hazardous materials
|October 22, 2023
概括
在酸性核废物中,基功能化二胺有效地将美洲 (III) 与欧洲 (III) 分离. 这些水友性联体具有高选择性和耐酸性,促进了核燃料循环的关闭.
科学领域:
- 放射化学和核化学的研究.
- 水合金和分离科学 水合金和分离科学
背景情况:
- 在高水平液体废物中将兰化物 (Ln) (III) (Lns) (III)) 与动化物 (Ans) (III) 分离,是核燃料回收和废物管理的关键挑战.
- 水友性联体对于先进的分离过程至关重要,但由于合成复杂性,性能和酸稳定性问题,其落后于脂友性对应物.
研究的目的:
- 开发高效,耐酸,易于合成的水友性联体,用于选择性Lns(III) /Ans(III) 分离.
- 为了研究基组功能化二胺作为美国 (III) /欧洲 (III) 分离在高酸度中的掩盖剂.
主要方法:
- 合成基组功能化类二胺.
- 在高酸度下进行液体液体提取实验 ( 1 M HNO3).
- 光谱技术 (紫外线吸收,NMR,时间分辨率激光光光谱 - TRLFS) 用于物种分析.
- 进行X射线晶体学和密度功能理论 (DFT) 计算,以获得结构和性能洞察力.
主要成果:
- 南二胺衍生物证明有效地掩盖了Am(III) / Eu(III).
- 用Phen-2DIC4OH在1.25M HNO3.3中获得了高达264的Eu (III) /Am (III) 的记录分离因子 (SF).
- 在提取条件下确认了占主导的1:1联体/金属物种形成.
- X射线数据和DFT计算阐明了优越的提取性能和选择性背后的机制.
结论:
- 氧基功能化二胺是Am (III) /Eu (III) 分离的高效和选择性的水友性联体.
- 这些配体易于合成,可扩展,耐酸,兼容CHON,使它们成为先进的核废物分离工艺的前景.
- 该研究促进了封闭核燃料循环的发展和现有核废物的有效管理.
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