Rapid determination of Pu isotopes and atom ratios in small amounts of environmental samples by an on-line sample pre-treatment system and isotope dilution high resolution inductively coupled plasma mass spectrometry
Rapid determination of Pu isotopes and atom ratios in small amounts of environmental samples by an on-line sample pre-treatment system and isotope dilution high resolution inductively coupled plasma mass spectrometry
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DOI：
10.1039/a907739a
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发表时间：
2000
影响因子：
3.4
通讯作者：
Cheol-Su Kim;Chang-Kyu Kim;Jong-In Lee;Kunjai Lee
中科院分区：
文献类型：
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作者：
Cheol-Su Kim;Chang-Kyu Kim;Jong-In Lee;Kunjai Lee
采用同位素稀释（ID）高分辨电感耦合等离子体质谱（HR-ICP-MS）结合在线样品前处理技术，对少量环境样品中痕量239 Pu、240 Pu和240 Pu/239 Pu比值进行了测定。为了减少238 U的干扰效应，使用微同心雾化器（MCN-6000®）作为样品引入方法，其显示出比常规气动雾化器低5倍的UH+/U+比率。在两种萃取树脂Sr-Spec®和TEVA-Spec®上依次进行钚的238 U分离和预浓缩，这两种树脂依次组合在集成液体处理系统PrepLabTM中。通过将最终样品体积减少到2.4 ml，将其注入HR-ICP-MS系统并使用MCN-6000，在具有Pu环境水平的1 g土壤和沉积物中进行Pu同位素分析是可行的。该方法对239 Pu、240 Pu和242 Pu的检测限分别约为4 fg ml−1（9.2 µBq ml−1）、3 fg ml−1（25 µBq ml−1）和6 fg ml−1（0.87 µBq ml−1）。这些代表最终样品体积中239 Pu、240 Pu和242 Pu的总量分别为9.6、7.2和14 fg。样品消化后，238 U消除和钚预浓缩程序完全自动化。因此，样品制备更加简单，整个样品分析过程可在约5小时内完成。使用几种经认证或标准参比物质（NIST SRM-4350 b、IAEA-6、IAEA-300、IAEA-367、IAEA-368、IAEA-375）确认了分析可靠性。
Isotope dilution (ID) high resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) combined with an on-line sample pre-treatment method was applied to the trace determination of 239Pu, 240Pu and 240Pu/239Pu ratios in small amounts of environmental samples. To reduce the interference effect of 238U, a microconcentric nebulizer, MCN-6000®, was used as a sample introduction method, which showed a 5-fold lower UH+/U+ ratio than the conventional pneumatic nebulizer. 238U separation and preconcentration of Pu were performed sequentially on two extraction resins, Sr-Spec® and TEVA-Spec®, which were sequentially combined in PrepLabTM, an integrated liquid handing system. By reducing the final sample volume to 2.4 ml, injecting it into the HR-ICP-MS system and employing the MCN-6000, the analysis of Pu isotopes is feasible in 1 g of soil and sediment having the environmental level of Pu. The detection limits for 239Pu, 240Pu and 242Pu by this method were about 4 fg ml−1 (9.2 µBq ml−1), 3 fg ml−1 (25 µBq ml−1) and 6 fg ml−1 (0.87 µBq ml−1), respectively. These represent total amounts of 9.6, 7.2 and 14 fg for 239Pu, 240Pu and 242Pu in a final sample volume. After digestion of the sample, the 238U elimination and Pu preconcentration procedures were fully automated. Sample preparation is therefore far simpler and the full sample analysis process can be achieved within about 5 h. The analytical reliability was confirmed using several certified or standard reference materials (NIST SRM-4350b, IAEA-6, IAEA-300, IAEA-367, IAEA-368, IAEA-375).