Highly sensitive detection of neodymium ion

Highly sensitive detection of neodymium ion
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高灵敏检测钕离子

DOI:
10.1016/j.chroma.2011.11.032
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发表时间:
2012
影响因子:
4.1
通讯作者:
Shingo Saito et al.
Shingo Saito et al.
中科院分区:
化学2区
文献类型:
--
作者:
Shingo Saito;Yoshiyuki Sato;Tomoko Haraga;Yuta Nakano;Shiho Asai;Yutaka Kameo;Kuniaki Takahashi;Masami Shibukawa;Shingo Saito et al.

文献摘要

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由于总Nd离子的精确定量可以确定燃耗(燃料消耗程度),因此迫切需要一种快速、高灵敏度的检测方法来检测少量乏核燃料样品中Nd离子的总浓度(total Nd)。本文提出了一种毛细管电泳-激光诱导荧光检测方法(CE-LIF),用于分析乏燃料样品溶液中的总Nd,使用一种新合成的金属荧光探针,该探针具有荧光素和大环六齿酸螯合基团fcc - abnota,用于分析镧系(Ln)离子。Ln离子衍生与探针形成强荧光配合物,抑制配体中心发射的猝灭。CE-LIF中Ln复合物的检测表明,Ln离子与FTC-ABNOTA之间的相互作用足够强,在迁移过程中不会解离。CE-LIF中Ln-FTC-ABNOTA配合物通过pH控制实现了相互分离,并与氢氧离子形成动态三元络合(DTC)。采用DTC分离模式,成功地获得了Nd与其他Ln离子的高分辨率,高分辨率为1.3 ~ 1.9,理论板数为68000,极低的检出限为22pM (3.2ppt, 0.11原子量基础)。用该方法对含多种金属离子的模拟乏燃料样品进行了定量分析,结果表明,即使U含量大量超标,也能获得102.1%的回收率。
A rapid and high-sensitive detection method for the total concentration of Nd ion (total Nd) in a small amount of a spent nuclear fuel sample is urgently required since the precise quantification of total Nd ion makes it possible for burnup (degree of fuel consumption) to be determined. In this work, a capillary electrophoresis-laser-induced fluorescent detection method (CE-LIF) is proposed for the analysis of total Nd in a spent fuel sample solution, with the use of a newly synthesized metal fluorescent probe which has a fluorescein and a macrocylic hexadentate chelating group, FTC-ABNOTA, for lanthanide (Ln) ions. Ln ions were derivatized to form a strongly fluorescent complex with the probe to suppress the quenching of the ligand-centered emission. The detection of Ln complexes in the CE-LIF indicated that the interaction between Ln ions and the FTC-ABNOTA was strong enough not to dissociate during migration. The mutual separation among the Ln–FTC-ABNOTA complexes in CE-LIF was achieved by pH control providing a dynamic ternary complexation (DTC) with hydroxide ions. Using the DTC separation mode, a high resolution of Nd from other Ln ions with high resolution of 1.3–1.9 and a theoretical plate number of 68,000, and a very low detection limit of 22pM (3.2ppt, 0.11attomole amount basis) were successfully obtained. A simulated spent fuel sample containing various metal ions was examined in this method with a good quantification result of 102.1% recovery obtained even with a large excess of U.