Ultra-trace plutonium determination in small volume seawater by sector field inductively coupled plasma mass spectrometry with application to Fukushima seawater samples

Ultra-trace plutonium determination in small volume seawater by sector field inductively coupled plasma mass spectrometry with application to Fukushima seawater samples
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扇形场电感耦合等离子体质谱法测定小体积海水中的超痕量钚并应用于福岛海水样品

DOI:
10.1016/j.chroma.2014.02.066
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发表时间:
2014-04-11
影响因子:
4.1
通讯作者:
Yamada, Masatoshi
Yamada, Masatoshi
中科院分区:
化学2区
文献类型:
--
作者:
Bu, Wenting;Zheng, Jian;Yamada, Masatoshi

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为了评估福岛第一核电站事故对海洋环境的钚污染,需要对海水中的钚同位素进行长期监测。本研究建立了一种基于阴离子交换色谱和SF-ICP-MS的准确、精密的分析方法,该方法可用于小体积(20- 60 L)海水样品中钚同位素的测定。铀净化因子为3 × 10(7)~ 1 × 10(8),可充分去除海水样品中的干扰铀。(PU)-P-239和Pu-240的估计检测限分别为0.11 fgmL(-1)和0.08 fgmL(-1),当测量20 L体积的海水时,这对应于(PU)-P-239的0.01 mBq m(-3)和(240)pu的0.03 mBq m(-3)。在(PU)-P-239浓度为11 fg mL(-1)和Pu-240浓度为2.7 fg mL(-1)的标准Pu溶液中,我们获得了良好的精密度(2.9%)和准确度(0.8%),用于测量(PU)-P-240/2(39)PU原子比。海水参比物质用于方法验证,Pu-239 +240活性和Pu-240/Pu-239原子比与预期值一致。分析了2011年3月以来在北太平洋西部福岛海域采集的表层和底层海水样品。结果表明,与事故前相比,调查区域海水中钚的分布没有明显变化。(C)2014爱思唯尔有限公司版权所有。
Long-term monitoring of Pu isotopes in seawater is required for assessing Pu contamination in the marine environment from the Fukushima Dai-ichi Nuclear Power Plant accident. In this study, we established an accurate and precise analytical method based on anion-exchange chromatography and SF-ICP-MS. This method was able to determine Pu isotopes in seawater samples with small volumes (20-60L). The U decontamination factor was 3 x 10(7)-1 x 10(8), which provided sufficient removal of interfering U from the seawater samples. The estimated limits of detection for (PU)-P-239 and Pu-240 were 0.11 fgmL(-1) and 0.08 fg mL(-1), respectively, which corresponded to 0.01 mBq m(-3) for (PU)-P-239 and 0.03 mBq m(-3) for (240)pu when a 20 L volume of seawater was measured. We achieved good precision (2.9%) and accuracy (0.8%) for measurement of the (PU)-P-240/2(39)PU atom ratio in the standard Pu solution with a (PU)-P-239 concentration of 11 fg mL(-1) and Pu-240 concentration of 2.7 fg mL(-1). Seawater reference materials were used for the method validation and both the Pu239+240 activities and Pu-240/Pu-239 atom ratios agreed well with the expected values. Surface and bottom seawater samples collected off Fukushima in the western North Pacific since March 2011 were analyzed. Our results suggested that there was no significant variation of the Pu distribution in seawater in the investigated areas compared to the distribution before the accident. (C) 2014 Elsevier B.V. All rights reserved.