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用于锕系元素钍、镤和铀色谱分离的二甘醇酰胺功能化介孔二氧化硅的合成及放射性评价

Synthesis and radiometric evaluation of diglycolamide functionalized mesoporous silica for the chromatographic separation of actinides Th, Pa and U.

作者信息

Hopkins Philip D, Mastren Tara, Florek Justyna, Copping Roy, Brugh Mark, John Kevin D, Nortier Meiring F, Birnbaum Eva R, Kleitz Freddy, Fassbender Michael E

机构信息

Chemistry Division, Los Alamos National Laboratory, P.O. Box 1663, Los Alamos, NM 87545, USA.

出版信息

Dalton Trans. 2018 Apr 17;47(15):5189-5195. doi: 10.1039/c8dt00404h.

DOI:10.1039/c8dt00404h
PMID:29528078
Abstract

The separation of Th, Pa, and U is of high importance in many applications including nuclear power, nuclear waste, environmental and geochemistry, nuclear forensics and nuclear medicine. Diglycolamide (DGA)-based resins have shown the ability to separate many elements, however, these resins consist of non-covalent impregnation of the DGA molecules on the resin backbone resulting in co-elution of the extraction molecule during separation cycles, therefore limiting their long-term and repeated use. Covalently binding the DGA molecules onto silica is one way to overcome this issue. Herein, measured equilibrium distribution coefficients of normal extraction chromatographic DGA resin and a covalently bound form (KIT-6-N-DGA sorbent) are reported. Several differences are observed between the two systems, the most significant being observed for uranium, which demonstrated significantly lower sorption behavior on KIT-6-N-DGA. These results indicate that U can effectively be separated from Th and Pa using KIT-6-N-DGA, a task that could not be completed with the use of normal DGA alone.

摘要

钍、镤和铀的分离在许多应用中具有高度重要性,包括核能、核废料、环境与地球化学、核法医学以及核医学等领域。基于二甘醇酰胺(DGA)的树脂已显示出分离多种元素的能力,然而,这些树脂由DGA分子在树脂主链上的非共价浸渍组成,导致在分离循环过程中萃取分子的共洗脱,因此限制了它们的长期和重复使用。将DGA分子共价结合到二氧化硅上是克服这一问题的一种方法。在此,报告了常规萃取色谱DGA树脂和共价结合形式(KIT-6-N-DGA吸附剂)的测量平衡分配系数。在这两个体系之间观察到了一些差异,其中最显著的是铀,它在KIT-6-N-DGA上表现出明显较低的吸附行为。这些结果表明,使用KIT-6-N-DGA可以有效地将铀与钍和镤分离,而仅使用常规DGA则无法完成这项任务。

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