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采用放射化学分离结合放射性测量和质谱测量法测定环境样品中的钚同位素(238Pu、239Pu、240Pu、241Pu)

Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements.

作者信息

Xu Yihong, Qiao Jixin, Hou Xiaolin, Pan Shaoming, Roos Per

机构信息

The Key Laboratory of Coastal and Island Development of Ministry of Education, Nanjing University, Nanjing 210093, China; Center for Nuclear Technologies, Technical University of Denmark, Risø Campus, Roskilde 4000, Denmark.

Center for Nuclear Technologies, Technical University of Denmark, Risø Campus, Roskilde 4000, Denmark.

出版信息

Talanta. 2014 Feb;119:590-5. doi: 10.1016/j.talanta.2013.11.061. Epub 2013 Dec 1.

Abstract

This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation.

摘要

本文报道了一种用于测定环境样品中钚同位素((238)Pu、(239)Pu、(240)Pu、(241)Pu)的分析方法,该方法采用阴离子交换色谱结合萃取色谱对钚进行化学分离。采用放射性测量方法(液体闪烁计数法和α能谱法)以及电感耦合等离子体质谱法(ICP-MS)对钚同位素进行测量。与文献报道的水平相比,20 g土壤中铀的去污因子显著提高至7.5×105,这对于使用质谱技术测量钚同位素至关重要。尽管整个过程中钚的化学产率约为55%,但本工作中IAEA土壤6和IAEA - 367的分析结果与文献报道值或参考值吻合良好,表明所建立的环境样品中钚的测定方法可靠。α能谱法测定(239 + 240)Pu的结果与ICP-MS测定的(239)Pu和(240)Pu之和非常吻合。ICP-MS不仅可以分别测量(239)Pu和(240)Pu,还可以测量(241)Pu。然而,即使通过化学分离获得了高达106的铀去污因子,在环境样品中使用ICP-MS也无法测量(238)Pu。

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