Safe and rapid development of capillary electrophoresis for ultratrace uranyl ions in radioactive samples from nuclear power facilities by way of fluorescent probe selection for actinide ions from a chemical library
Safe and rapid development of capillary electrophoresis for ultratrace uranyl ions in radioactive samples from nuclear power facilities by way of fluorescent probe selection for actinide ions from a chemical library
复制标题
通过从化学库中选择锕系离子的荧光探针，安全、快速地开发核电设施放射性样品中超痕量铀酰离子的毛细管电泳
DOI：
10.1016/j.aca.2018.05.077
复制
发表时间：
2018
影响因子：
6.2
通讯作者：
Shingo Saito
中科院分区：
文献类型：
--
作者：
Tomoko Haraga;Kazuki Ouchi;Yoshiyuki Sato;Hitoshi Hoshino;Rei Tanaka;Takashi Fujihara;Hideki Kurokawa;Masami Shibukawa;Ken-ichiro Ishimori;Yutaka Kameo;Shingo Saito
2011年东日本大地震引发的福岛第一核电站严重核事故发生后，开发可行、安全、高灵敏度（低水平辐射暴露和放射性废物产生）的放射性样品分析方法，特别是锕系元素（An）离子，是一个重要的挑战。在这里，我们提出了一种方法来选择合适的发射探针的离子具有非常低的消耗和发射的放射性的毛细管荧光激光诱导荧光检测（CE-LIF），使用一个小的化学库的探针与8个不同的螯合部分。结果表明，具有四齿螯合基团1，10-菲咯啉-2，9-二甲酸（PDA）的发射探针L1适合于检测铀酰离子。使用CE-LIF结合动态三元络合和毛细管浓缩技术测定的铀酰-L1络合物的检测限为2.9 × 10− 12 M（0.7 ppt）。未观察到大量过量基质金属离子的干扰。该方法已成功应用于从核设施（包括福岛第一核电站）采集的真实的放射性液体样品。这种策略不仅允许开发一种安全和快速的分析方法，而且还提供了深入了解的配位化学的离子络合物。具体而言，PDA结构提供了大量的动力学惰性，其铀酰络合物;形成的三元配合物之间的铀酰-L1和碳酸盐被揭示;和不寻常的相互作用之间的π-电子系统的铀酰和菲咯啉环，这稳定了铀酰PDA的相互作用。
After the serious nuclear accident at the Fukushima Daiichi Nuclear Power Plant caused by the Great East Japan Earthquake in 2011, the development of feasible, safe, and highly sensitive analytical methods (in terms of low levels of radiation exposure and radioactive waste generation) for radioactive samples, especially actinide (An) ions, represents an important challenge. Here we propose a methodology for selecting appropriate emissive probes for An ions with very low consumption and emission of radioactivity by capillary electrophoresis–laser-induced fluorescence detection (CE-LIF), using a small chemical library of probes with eight different chelating moieties. It was found that the emissive probe L1, which possesses the tetradentate chelating moiety 1,10-phenanthroline-2,9-dicarboxylic acid (PDA), was suitable for detecting uranyl ions. The detection limit for the uranyl–L1 complex using CE-LIF combined with dynamic ternary complexation and on-capillary concentration techniques was determined to be 2.9 × 10−12M (0.7 ppt). No interference from the large excess of matrix metal ions was observed. This method was successfully applied to real radioactive liquid samples collected from nuclear facilities, including the Fukushima Daiichi Nuclear Power Plant. This strategy not only permitted the development of a safe and rapid analytical method but also provided insight into the coordination chemistry of An ion complexes. Specifically, the PDA structure provided substantial kinetic inertness to its uranyl complex; the formation of a ternary complex between uranyl–L1 and carbonate was revealed; and unusual interactions were observed between the π-electron systems of uranyl and the phenanthroline ring, which stabilized the uranyl–PDA interaction.