具有不同N/O捐赠模式的异环联体对Am (III) /Eu (III) 分离:一个理论观点
Ling-Ling Su1,2, Qun-Yan Wu2, Cong-Zhi Wang2
1School of Nuclear Science and Technology, University of South China, Hengyang 421001, China.
Inorganic chemistry
|December 6, 2023
概括
这项研究表明,异环联体中原子的数量显著影响三价乙烯酸与兰坦酸的分离. 更多的捐赠者提高了选择性,这对于核燃料再加工至关重要.
科学领域:
- 核化学 核化学 核化学
- 材料科学 材料科学 材料科学
- 计算化学计算化学
背景情况:
- 废核燃料的再加工需要有效地将三价乙化物 (An(III)) 与化物 (Ln(III)) 分离出来.
- 对于这种分离,研究了具有 (N) 和氧 (O) 捐赠者的异环配体.
- 与联体的An(III) 和Ln(III) 的协调化学作用影响了分离性能.
研究的目的:
- 调查四种衍生于类素的四联体的电子结构,协调模式和提取反应.
- 评估连接体供体原子 (N/O) 对美国 (Am(III)) 与欧洲 (Eu(III)) 的分离的影响.
- 为设计有效的连接物用于An(III) /Ln(III) 分离提供基本见解.
主要方法:
- 尺度相对论密度函数理论 (DFT) 用于研究四个四形形异环联体 (L1-L4).
- 评估了电子结构,粘合特性和与Am (III) 和Eu (III) 的协调模式.
- 提取反应和吉布斯自由能量变化计算以评估选择性.
主要成果:
- Am(III) / Eu(III) 的选择性受到连接体中协调原子的数量的影响.
- 与氧气捐赠者 (L2,L3) 相比,具有更多捐赠者 (L1) 的体具有更高的Am(III) /Eu(III) 选择性.
- 联体L4表现出强大的结合性,但由于结构预组织,选择性较低.
结论:
- heterocyclic 配体中协调的 N 和 O 原子的数量极大地影响了 An (III) /Ln (III) 的选择性.
- 增加的协调增加了分离Am(III) 和Eu(III) 的选择性.
- 这些发现为开发用于核废物管理的先进配体提供了有价值的指导.
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